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Adelhelm, Philipp. "From Lithium-Ion to Sodium-Ion Batteries." Diffusion fundamentals 21 (2014) 5, S.1, 2014. https://ul.qucosa.de/id/qucosa%3A32397.
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Nwafornso, Tochukwu. "Bismuth anode for sodium-ion batteries." Thesis, Uppsala universitet, Strukturkemi, 2021. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-449075.
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It is imperative to develop alternative battery technologies based on naturally abundant elements, with competitive performance as lithium-ion batteries. Sodium has a natural abundance 1000 times more than lithium with both lithium and sodium-ion batteries having similar chemistry. Sodium-ion batteries are potentially an alternative that can achieve such competitive performance, given that electrode and electrolyte materials of high rate and long-term electrochemical performance are being developed. This thesis investigates the rate capability and long-term performance of bulk bismuth electrodes containing varying carbon content. The electrodes were cycled in cells with glyme-based electrolytes: diglyme and tetraglyme. Scanning electron microscopy and energy dispersive spectroscopy showed the morphology and elemental mapping of pristine and cycled bismuth electrodes. The result demonstrates the evolving porosity as the electrode cycled. The galvanostatic cycling of half-cells showed two plateaus each for sodiation and desodiation. Also, two peaks are seen in cyclic voltammetry suggesting a two-phase reaction. When cycled between -0.6 to 0.6 V in a symmetrical cell, the bismuth electrode showed an appreciable rate capability at a current rate of 770 mA/g in diglyme. In tetraglyme, it showed a poor rate capability, even at a current rate of 308 mA/g. The rate performance in a full cell cycled between 0.1 to 3.2 V also showed a good rate capability at a current rate of 770 mA/g in diglyme. Tetraglyme showed poor rate capability at the same current rate. The capacity retention was higher in the symmetrical cells, with 79 % and 78 % capacity retention relative to the initial charge capacity after 100 cycles for diglyme and tetraglyme. At the same current rate and more than 70 cycles, the full cells showed capacity retention of 58 % in diglyme and 44.8 % in tetraglyme. The capacity retention varied slightly for the two different electrode composites. The superior performance in the symmetrical cell is due to the narrow voltage window. Evaluating the stability of the solid electrolyte interphase via galvanostatic cycling suggests some stability issues. The full cells showed growing resistance with an increasing number of cycles.
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Simone, Virginie. "Développement d'accumulateurs sodium-ion." Thesis, Université Grenoble Alpes (ComUE), 2016. http://www.theses.fr/2016GREAI092/document.
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Au vu d’une demande croissante pour un stockage d’énergie à grande échelle, il est préférable de se tourner vers des matériaux peu coûteux et répandus. De ce point de vue, le sodium, qui présente des caractéristiques très proches de celles du lithium, présente également l’avantage d’être peu coûteux, abondant et réparti uniformément dans le monde. Cette thèse porte sur l’étude d’un système complet Na-ion constitué d’un carbone dur à l’électrode négative et d’un oxyde lamellaire à l’électrode positive. Un volet sur l’électrolyte a également été abordé.Concernant l’électrode négative, l’influence de la température de pyrolyse de la cellulose sur la structure des carbones durs et sur les performances électrochimiques a été étudiée. Une graphitisation localisée, une fermeture des pores et une évolution de la porosité interne avec la température de pyrolyse ont pu être observées. Les meilleures performances électrochimiques ont été obtenues pour le matériau synthétisé à 1600 °C : une capacité réversible d’environ 300 mAh.g-1 stable sur 200 cycles est atteinte à 37,2 mA.g-1 avec une efficacité coulombique initiale de 84 %. Pour mieux comprendre les mécanismes d’insertion du sodium dans ces matériaux, des études par spectroscopie d’impédance, SAXS et EDX ont été réalisées sur des carbones durs cyclés à différents potentiels.Le matériau d’électrode positive choisi est l’oxyde lamellaire Na0,6Ni0,25Mn0,75O2. L’influence de la température de calcination a permis de faire varier le nombre de défauts d’empilement de type P3 au profit d’une phase P2 plus cristalline. Après avoir optimisé l’électrolyte à base de carbonates pour garantir la reproductibilité des tests oxyde lamellaire//sodium métal, une capacité d’oxydation de 130 mAh.g-1 a pu être atteinte au premier cycle avant de chuter fortement sur les 40 cycles suivants. Cette perte de capacité a pu être en partie expliquée par des études de DRX operando. Enfin, ces travaux ont permis d’aboutir à des systèmes complets Na-ion dont les premiers résultats sont prometteursBecause of the development of renewable energy and electric vehicles, the need for a large scale energy storage has increased. This type of storage requires a large amount of raw materials. Therefore low cost and abundant resources are necessary. Consequently the use of sodium batteries is of interest because sodium’s low cost, high abundance, and worldwide availability. This PhD thesis deals with the study of a full Na-ion cell containing a hard carbon negative electrode, and a layered oxide positive electrode. A shorter part concerns the electrolyte.Concerning the negative electrode, the first objective was to understand in detail the influence of the pyrolysis temperature of a hard carbon precursor, cellulose, on the final structure of the material and its consequences on the electrochemical performance. Many techniques were used to characterize the hard carbon structure as a function of the pyrolysis temperature. Localized graphitization, pore closure, and an increase in micropore size have been observed with increasing temperature. The best electrochemical performance has been reached with the hard carbon synthesized at 1600°C: a reversible capacity of around 300 mAh.g-1 stable over 200 cycles is obtained at 37.2 mA.g-1 with an initial coulombic efficiency of 84%. To deeper understand sodium insertion mechanisms in hard carbon structures impedance spectroscopy, SAXS and EDX were carried out on hard carbon electrodes cycled at different voltages.The layered oxide Na0.6Ni0.25Mn0.75O2 was investigated as the positive electrode. It was observed that with increasing calcination temperature the number of P3-type stacking faults decreases in favor of a more crystalline P2 phase. Then, the carbonate-based electrolyte has been optimized to guarantee the reproducibility of the electrochemical tests performed in a layered oxide//sodium metal configuration. A first oxidation capacity of around 130 mAh.g-1 is reached. However this value drops quickly after 40 cycles. Operando XRD analysis did partially explain the capacity decrease. Finally, the results of these investigations were used to design an optimized full cell which demonstrated promising performance during initial testing
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Toigo, Christina Verena <1986>. "Towards eco-friendly batteries: concepts for lithium and sodium ion batteries." Doctoral thesis, Alma Mater Studiorum - Università di Bologna, 2022. http://amsdottorato.unibo.it/10067/1/Thesis%20CT_final.pdf.
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Several possibilities are arising aiming the development of “greener”, more sustainable energy storage systems. One point is the completely water-based processing of battery electrodes, thus being able to renounce the use of toxic solvents in the preparation process. Despite its advantage of lower cost and eco-friendlyness, there is the need of similar mechanical and electrochemichal behavior for boosting this preparation mode.
Another point – accompanying the water-based processing - is the replacement of solvent-based polymer binders by water-based ones. These binders can be based on fluorinated, crude-oil based polymers on the one side, but also on naturally abundant and economic friendly biopolymers.
The most common anode materials, graphite and lithium titanate (LTO), have been subjected a water-based preparation route with different binder systems. LTO is a promising anode material for lithium ion batteries (LIBs), as it shows excellent safety characteristics, does not form a significant SEI and its volume change upon intercalation of lithium ions is negligible. Unfortunately, this material suffers from a rather low electric conductivity - that is why an intensive study on improved current collector surfaces for LTO electrodes was performed.
In order to go one step ahead towards sustainable energy storage, anode and cathode active materials for a sodium ion battery were synthesized. Anode active material resulted in a successful product which was then subjected to further electrochemical tests.
In this PhD work the development of “greener” energy storage possibilities is tested under several aspects. The ecological impact of raw materials and required battery components is examined in detail.
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Nose, Masafumi. "Studies on Sodium-containing Transition Metal Phosphates for Sodium-ion Batteries." 京都大学 (Kyoto University), 2016. http://hdl.handle.net/2433/215565.
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Naqash, Sahir Verfasser], Olivier [Akademischer Betreuer] Guillon, and Jochen M. [Akademischer Betreuer] [Schneider. "Sodium ion conducting ceramics for sodium ion batteries / Sahir Naqash ; Olivier Guillon, Jochen Michael Schneider." Aachen : Universitätsbibliothek der RWTH Aachen, 2019. http://d-nb.info/1190040611/34.
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Naqash, Sahir [Verfasser], Olivier Akademischer Betreuer] Guillon, and Jochen M. [Akademischer Betreuer] [Schneider. "Sodium ion conducting ceramics for sodium ion batteries / Sahir Naqash ; Olivier Guillon, Jochen Michael Schneider." Aachen : Universitätsbibliothek der RWTH Aachen, 2019. http://nbn-resolving.de/urn:nbn:de:101:1-2019070807164971884045.
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Wu, Di Ph D. Massachusetts Institute of Technology. "A layered sodium titanate as promising anode material for sodium ion batteries." Thesis, Massachusetts Institute of Technology, 2014. http://hdl.handle.net/1721.1/93004.
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Thesis: S.M., Massachusetts Institute of Technology, Department of Mechanical Engineering, 2014.Cataloged from PDF version of thesis.
Includes bibliographical references (pages 58-60).
Sodium ion batteries have recently received great attention for large-scale energy applications because of the abundance and low cost of sodium source. Although some cathode materials with desirable electrochemical properties have been proposed, it's quite challenging to develop suitable anode materials with high energy density and good cyclability for sodium ion batteries. Herein, we report a layered material, 03-NaTiO2, that delivers 130mAhg-1 of reversible capacity and presents excellent cyclability with capacity retention over 97.5% after 40 cycles and high rate capability. Furthermore, by coupling the electrochemical process with in situ X-ray diffraction, the structure evolution and variation of cell parameters corresponding to an 03-03' phase transition during sodium deintercalation is investigated. Unusual lattice parameter variation was observed by in situ XRD, which can be related to the structure modulation with varying Na vacancy ordering. An irreversible structural modification upon overcharging is also confirmed by in situ XRD. In summary, our work demonstrates that 03-NaTiO2 is a very promising anode material for sodium ion batteries with high energy density.
by Di Wu.
S.M.
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Cesetti, Lorenzo. "Systematic study of in-situ sodium plating/stripping on anode free substrates for sodium ion batteries." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2018.
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Gli oggetti di studio di questo lavoro di tesi sono le batterie agli ioni-sodio, in particolare una loro variante ancora in fase di sviluppo denominata “anode-free”.
Seppur questi accumulatori al sodio non siano nuovi ma conosciuti da tempo, è solamente dal 2010 che gli studi al riguardo si sono intensificati, tanto da portare alla realizzazione di diversi prototipi in pochi anni.
Le maggiori difficoltà nel loro sviluppo sono state riscontrate nella scelta del materiale costituente l’anodo.
Per ovviare al problema sono state ideate le batterie agli ioni-sodio “anode-free”: l’anodo è rappresentato da un semplice collettore di corrente, generalmente alluminio o rame, dove gli ioni-sodio si depositano, riducendosi e formando sodio metallico in situ durante la carica; al contrario, durante la scarica, è il sodio metallico che si ossida tornando ione e migrando verso il catodo.
Il lavoro di tesi ivi proposto è stato sviluppato presso l’Energy Storage Group del College of Engineering della Swansea University di Swansea (UK).
Sono stati esaminati tre substrati differenti valutando l’idoneità di ciascuno di essi ad un’applicazione come anodo in un accumulatore agli ioni-sodio “anode-free”, attraverso tecniche di caratterizzazione standard quali Galvanostatic Cycling (GC), Cyclic Voltammetry (CV) ed analisi al microscopio.
I materiali presi in esame sono stati: acciaio inossidabile, acciaio inossidabile rivestito di nichel ed un substrato di nichel chiamato nichel foam.
Dopo aver visto che l’acciaio inossidabile è il substrato in grado di garantire prestazioni migliori, lo step successivo è stato quello di realizzare una vera e propria batteria agli ioni-sodio “anode-free” utilizzando un catodo composto da pirite presodiata.
Le performance della batteria proposta in questa tesi sono state infine confrontate con quelle di un modello di riferimento che impiega un collettore di corrente in alluminio rivestito da carbon black come anodo.
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Toumar, Alexandra Jeanne. "Phase transformations in layered electrode materials for sodium ion batteries." Thesis, Massachusetts Institute of Technology, 2017. http://hdl.handle.net/1721.1/111255.
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Thesis: Ph. D., Massachusetts Institute of Technology, Department of Materials Science and Engineering, 2017.This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.
Cataloged from student-submitted PDF version of thesis.
Includes bibliographical references (pages 118-130).
In this thesis, I investigate sodium ion intercalation in layered electrode materials for sodium ion batteries. Layered metal oxides have been at the forefront of rechargeable lithium ion battery technology for decades, and are currently the state of the art materials for sodium ion battery cathodes in line for commercialization. Sodium ion intercalated layered oxides exist in several different host phases depending on sodium content and temperature at synthesis. Unlike their lithium ion counterparts, seven first row layered TM oxides can intercalate Na ions reversibly. Their voltage curves indicate significant and numerous reversible phase transformations during electrochemical cycling. These transformations arise from Na-ion vacancy ordering and metal oxide slab glide but are not well understood and difficult to characterize experimentally. In this thesis, I explain the nature of these lattice differences and phase transformations for O and P-type single-transition-metal layered systems with regards to the active ion and transition metal at hand. This thesis first investigates the nature of vacancy ordering within the O3 host lattice framework, which is currently the most widely synthesized framework for sodium ion intercalating oxides. I generate predicted electrochemical voltage curves for each of the Na-ion intercalating layered TM oxides using a high-throughput framework of density functional theory (DFT) calculations and determine a set of vacancy ordered phases appearing as ground states in all NaxMO₂ systems, and investigate the energy effect of stacking of adjacent layers. I also examine the influence of transition metal mixing and transition metal migration on the materials' thermodynamic properties. Recent work has established the P2 framework as a better electrode candidate structure type than O3, because its slightly larger interlayer spacing allows for faster sodium ion diffusion due to lower diffusion barriers. However, little has been resolved in explaining what stabilizing mechanisms allow for the formation of P-type materials and their synthesis. This work therefore also investigates what stabilizes P2, P3 and O3 materials and what makes them synthesizable at given synthesis conditions, both for the optimization of synthesis techniques and for better-guided material design. It is of further interest to understand why some transition metal oxide systems readily form P2 or P3 compounds while others do not. I investigate several possible stabilizing mechanisms that allow P-type layered sodium metal oxides to by synthesized, and relate these to the choice of transition metal in the metal oxide structure. Finally, this work examines the difficulty of sodium ion intercalation into graphite, which is a commonly used anode material for lithium ion batteries, proposing possible reasons for why graphite does not reversibly intercalate sodium ions and why cointercalation with other compounds is unlikely. This thesis concludes that complex stabilizing mechanisms that go beyond simple electrostatics govern the intercalation of sodium ions into layered systems, giving it advantages and disadvantages over lithium ion batteries and outlining design principles to improve full-cell sodium ion battery materials.
by Alexandra Jeanne Toumar.
Ph. D.
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Li, Xianji. "Metal nitrides as negative electrode materials for sodium-ion batteries." Thesis, University of Southampton, 2015. https://eprints.soton.ac.uk/374787/.
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Han, Ruixin. "SYNTHESIS, AND STRUCTURAL, ELECTROCHEMICAL, AND MAGNETIC PROPERTY CHARACTERIZATION OF PROMISING ELECTRODE MATERIALS FOR LITHIUM-ION BATTERIES AND SODIUM-ION BATTERIES." UKnowledge, 2018. https://uknowledge.uky.edu/chemistry_etds/90.
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Iron oxides, have been widely studied as promising anode materials in lithium-ion batteries (LIBs) for their high capacity (≈ 1000 mA h g-1 for Fe2O3 and Fe3O4,), non-toxicity, and low cost. In this work, β-FeOOH has been evaluated within a LIB half-cell showing an excellent capacity of ≈ 1500 mA h g-1 , superior to Fe2O3 or Fe3O4. Reaction mechanism has been proposed with the assistance of X-ray photoelectron spectroscopy (XPS). Various magnetic properties have been suggested for β-FeOOH such as superparamagnetism, antiferromagnetism and complex magnetism, for which, size of the material is believed to play a critical role. Here, we present a size-controlled synthesis of β-FeOOH nanorods. Co-existing superparamagnetism and antiferromagnetism have been revealed in β-FeOOH by using a Physical Property Measurement System (PPMS).
Compared with the high price of lithium in LIBs, sodium-ion batteries (SIBs) have attracted increasing attentions for lower cost. Recent studies have reported Na0.44MnO2 to be a promising candidate for cathode material of SIBs. This thesis has approached a novel solid-state synthesis of Na0.44MnO2 whiskers and a nano-scaled open cell for in situ TEM study. Preliminary results show the first-stage fabrication of the cell on a biasing protochip.
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Murphy, Denissa Tjiadarma. "Structural Investigation of Electrodes for Rechargeable Alkali Ion Batteries." Thesis, The University of Sydney, 2017. http://hdl.handle.net/2123/17699.
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This thesis describes the in-depth characterisation of the structure, including detailed cation distributions, of positive electrode materials for lithium and sodium ion batteries. As the crystal chemistry influences the mobility of lithium and sodium ions, the structure and electrochemical property relationships for select compounds have been established. The majority of this thesis is focused on the structural characterisation of LiMn2-xTixO4 (0.2 ≤ x ≤ 1.5). A combination of X-ray and neutron powder diffraction studies along with spectroscopic techniques and physical property measurements were employed to elucidate the complex metal ion ordering of the spinel electrodes. It was found that the synthesis conditions, particularly cooling regimes, play an important part in the final structures of LiMn1.8Ti0.2O4 and LiMnTiO4. The bulk substitution of 10% and 50% manganese with titanium heavily influenced the cation distribution and consequently, the electrochemistry of these compounds. In situ diffraction studies revealed the contrasting structural evolutions of LiMn1.8Ti0.2O4 and LiMnTiO4 during charge and discharge cycles. The potential of sodium silicate materials as positive electrodes for sodium ion batteries was explored. The fundamental crystal chemistry of Na2MnSiO4 and Na2CoSiO4 was established prior to electrochemical cycling. The as prepared Na2CoSiO4 exhibited better conductivity than the manganese analogue. Improvement of the conductivity of Na2MnSiO4 was achieved through carbon coating of the material. Finally, the addition of Li2RuO3 to form the lithium rich 0.5Li2RuO3∙0.5LiMO2 (M = Co and Ni) electrodes has resulted in the increased the stability of the layered structures of the compounds. The electrochemically active Li2RuO3 contributed to the excellent specific capacity and rate capability of the cobalt compound. Overall superior electrochemical performance was achieved by the nickel analogue.
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David, Lamuel Abraham. "Van der Waals sheets for rechargeable metal-ion batteries." Diss., Kansas State University, 2015. http://hdl.handle.net/2097/32796.
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Doctor of PhilosophyDepartment of Mechanical and Nuclear Engineering
Gurpreet Singh
The inevitable depletion of fossil fuels and related environmental issues has led to exploration of alternative energy sources and storage technologies. Among various energy storage technologies, rechargeable metal-ion batteries (MIB) are at the forefront. One dominant factor affecting the performance of MIB is the choice of electrode material. This thesis reports synthesis of paper like electrodes composed for three representative layered materials (van der Waals sheets) namely reduced graphene oxide (rGO), molybdenum disulfide (MoS₂) and hexagonal boron nitride (BN) and their use as a flexible negative electrode for Li and Na-ion batteries. Additionally, layered or sandwiched structures of vdW sheets with precursor-derived ceramics (PDCs) were explored as high C-rate electrode materials. Electrochemical performance of rGO paper electrodes depended upon its reduction temperature, with maximum Li charge capacity of 325 mAh.g⁻¹ observed for specimen annealed at 900°C. However, a sharp decline in Na charge capacity was noted for rGO annealed above 500 °C. More importantly, annealing of GO in NH₃ at 500 °C showed negligible cyclability for Na-ions while there was improvement in electrode's Li-ion cycling performance. This is due to increased level of ordering in graphene sheets and decreased interlayer spacing with increasing annealing temperatures in Ar or reduction at moderate temperatures in NH₃. Further enhancement in rGO electrodes was achieved by interfacing exfoliated MoS₂ with rGO in 8:2 wt. ratios. Such papers showed good Na cycling ability with charge capacity of approx. 225.mAh.g⁻¹ and coulombic efficiency reaching 99%. Composite paper electrode of rGO and silicon oxycarbide SiOC (a type of PDC) was tested as high power-high energy anode material. Owing to this unique structure, the SiOC/rGO composite electrode exhibited stable Li-ion charge capacity of 543.mAh.g⁻¹ at 2400 mA.g⁻¹ with nearly 100% average cycling efficiency. Further, mechanical characterization of composite papers revealed difference in fracture mechanism between rGO and 60SiOC composite freestanding paper. This work demonstrates the first high power density silicon based PDC/rGO composite with high cyclic stability. Composite paper electrodes of exfoliated MoS₂ sheets and silicon carbonitride (another type of PDC material) were prepared by chemical interfacing of MoS₂ with polysilazane followed by pyrolysis . Microscopic and spectroscopic techniques confirmed ceramization of polymer to ceramic phase on surfaces on MoS₂. The electrode showed classical three-phase behavior characteristics of a conversion reaction. Excellent C-rate performance and Li capacity of 530 mAh.g⁻¹ which is approximately 3 times higher than bulk MoS₂ was observed. Composite papers of BN sheets with SiCN (SiCN/BN) showed improved electrical conductivity, high-temperature oxidation resistance (at 1000 °C), and high electrochemical activity (~517 mAh g⁻¹ at 100 mA g⁻¹) toward Li-ions generally not observed in SiCN or B-doped SiCN. Chemical characterization of the composite suggests increased free-carbon content in the SiCN phase, which may have exceeded the percolation limit, leading to the improved conductivity and Li-reversible capacity. The novel approach to synthesis of van der Waals sheets and its PDC composites along with battery cyclic performance testing offers a starting point to further explore the cyclic performance of other van der Waals sheets functionalized with various other PDC chemistries.
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Wood, Stephen. "Computer modelling studies of new electrode materials for rechargeable batteries." Thesis, University of Bath, 2015. https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.687357.
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Developing a sustainable energy infrastructure for the 21st century requires the large scale development of renewable energy resources. Fully exploiting these inherently intermittent supplies will require advanced energy storage technologies, with rechargeable Li-ion and Na-ion batteries considered highly promising for both vehicle electrification and grid storage applications. However, the performance required of battery materials has not been achieved, and significant improvements are needed. Modern computational techniques allow the elucidation of structure-property relationships at the atomic level and are valuable tools in providing fundamental insights into novel materials. Therefore, in this thesis a combination of atomistic simulation and ab initio density functional theory (DFT) techniques have been used to study a number of potential battery cathode materials. Firstly, Na2FePO4F and NaFePO4 are interesting materials that have been reported recently as attractive positive electrodes for Na-ion batteries. Here, we report their Na-ion conduction behaviour and intrinsic defect properties using atomistic simulation methods. Na+ ion conduction in Na2FePO4F is predicted to be two-dimensional (2D) in the interlayer plane. Na ion migration in NaFePO4 is restricted to the [010] direction along a curved trajectory, leading to quasi-1D Na+ diffusion. Furthermore, Na/Fe antisite defects are predicted to have a lower formation energy in NaFePO4 than Na2FePO4F. The higher probability of tunnel occupation with a relatively immobile Fe2+ cation - along with a greater volume change on redox cycling - contributes to the poor electrochemical performance of NaFePO4. Secondly, work on the Na2FePO4F system is extended to include investigation of the surface structures and energetics. The equilibrium morphology is found to be essentially octagonal, compressed slightly along the [010] direction, and is dominated by the (010), (021), (122) and (110) surfaces. The calculated growth morphology is a more ``rod-like'' nanoparticle, with the (021), (023), (110) and (112) planes predominant. The (010) surface lies parallel to the Na layers in the ac plane and is unlikely to facilitate Na+ intercalation. As such, its prominence in the equilibrium morphology, and absence from the growth morphology, suggests nanoparticles synthesised in a kinetically limited regime should provide higher rate performance than those synthesised in close to equilibrium conditions. Surface redox potentials for Na2FePO4F derived using DFT vary between 2.76 - 3.37 V, in comparison to a calculated bulk cell voltage of 2.91 V. Most significantly, the lowest energy potentials are found for the (130) and (001) planes suggesting that upon charging Na+ will first be extracted from these surfaces, and inserted lastly upon discharging. Thirdly, the mixed phosphates Na4M3(PO4)2P2O7 (M=Fe, Mn, Co, Ni) are explored as a fascinating new class of materials reported to be attractive Na-ion cathodes, displaying low volume changes upon cycling indicative of long lifetime operation. Key issues surrounding intrinsic defects, Na-ion migration mechanisms and voltage trends have been investigated through a combination of atomistic energy minimisation, molecular dynamics and DFT simulations. The MD results suggest Na+ diffusion extends across a 3D network of migration pathways with an activation barrier of 0.20-0.24 eV, and diffusion coefficients (DNa) of 10-10-10-11 cm2s-1 at 325 K, suggesting high rate capability. The cell voltage trends, explored using DFT methods, indicate that doping the Fe-based cathode with Ni can significantly increase the voltage, and hence energy density. Finally, DFT simulations of K+-stabilised α-MnO2 have been combined with aberration corrected-STEM techniques to study the surface energetics, particle morphologies and growth mechanism. α-K0.25MnO2 grown through a hydrothermal synthesis method is found to produce primary nanowires with preferential growth along the [001] direction. Primary nanowires attach through a shared (110) interface to form larger secondary nanowires. This is in agreement with DFT simulations with the {100}, {110} and {211} surfaces displaying the lowest surface energies. The ranking of surface energies is driven by Mn coordination environments and surface relaxation. The calculated equilibrium morphology of α-K0.25MnO2 is consistent with the observed primary nanowires from high resolution electron microscopy images.
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Dall'Agnese, Yohan. "Study of early transition metal carbides for energy storage applications." Thesis, Toulouse 3, 2016. http://www.theses.fr/2016TOU30025/document.
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La demande urgente d'innovations dans le domaine du stockage de l'énergie est liée au développement récent de la production d'énergie renouvelable ainsi qu'à la diversification des produits électroniques portables qui consomment de plus en plus d'énergie. Il existe plusieurs technologies pour le stockage et la conversion électrochimique de l'énergie, les plus notables étant les batteries aux ions lithium, les piles à combustible et les supercondensateurs. Ces systèmes sont utilisés de façon complémentaire des uns aux autres dans des applications différentes. Par exemple, les batteries sont plus facilement transportables que les piles à combustible et ont de bonne densité d'énergie alors que les supercondensateurs ont des densités de puissance plus élevés et une meilleure durée de vie. L'objectif principal de ces travaux est d'étudier les performances électrochimiques d'une nouvelle famille de matériaux bidimensionnel appelée MXène, en vue de proposer de nouvelles solutions pour le stockage de l'énergie. Pour y arriver, plusieurs directions ont été explorées. Dans un premier temps, la thèse se concentre sur les supercondensateurs dans des électrolytes aqueux et aux effets des groupes de surface. La seconde partie se concentre sur les systèmes de batterie et de capacités à ions sodium. Une cellule complète comportant une anode en carbone et une cathode de MXène a été développées. La dernière partie de la thèse présente l'étude des MXènes pour les supercondensateur en milieu organique. Une attention particulière est apportée à l'étude du mécanisme d'intercalation des ions entre les feuillets de MXène. Différentes techniques de caractérisations ont été utilisées, en particulier la voltampérométrie cyclique, le cyclage galvanostatique, la spectroscopie d'impédance, la microscopie électronique et la diffraction des rayons XAn increase in energy and power densities is needed to match the growing energy storage demands linked with the development of renewable energy production and portable electronics. Several energy storage technologies exist including lithium ion batteries, sodium ion batteries, fuel cells and electrochemical capacitors. These systems are complementary to each other. For example, electrochemical capacitors (ECs) can deliver high power densities whereas batteries are used for high energy densities applications. The first objective of this work is to investigate the electrochemical performances of a new family of 2-D material called MXene and propose new solutions to tackle the energy storage concern. To achieve this goal, several directions have been explored. The first part of the research focuses on MXene behavior as electrode material for electrochemical capacitors in aqueous electrolytes. The next part starts with sodium-ion batteries, and a new hybrid system of sodium ion capacitor is proposed. The last part is the study of MXene electrodes for supercapacitors is organic electrolytes. The energy storage mechanisms are thoroughly investigated. Different characterization techniques were used in this work, such as cyclic voltammetry, galvanostatic charge-discharge, electrochemical impedance spectroscopy, scanning electron microscopy and X-ray diffraction
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FIORE, MICHELE. "Nanostructured Materials for secondary alkaline ion batteries." Doctoral thesis, Università degli Studi di Milano-Bicocca, 2020. http://hdl.handle.net/10281/262348.
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Thanks to their superior energy and power density, lithium-ion batteries (LIBs) currently dominate the market of power sources for portable devices. The economy of scale and engineering optimizations have driven the cost of LIBs below the 200 $/KWh at the pack level. This catalyzed the market penetration of electric vehicles and made them a viable candidate for stationary energy storage. However, the rapid market expansion of LIBs raised growing concerns about the future sustainability of this technology. In particular, lithium and cobalt supplies are considered vulnerable, primarily because of the geopolitical implications of their high concentration in only a few countries. In the search for the next generation secondary batteries, known as post-lithium ion batteries, candidates that do not use rare metals have been extensively investigated in the last 10 years. Sodium-ion batteries (SIBs) attracted considerable attention thanks to the high abundance of the precursors and wide distribution of sodium on the earth's crust. As a matter of fact, as it will be pointed out during the dissertation, it is not straightforward to allocate the reduction of the price of the alkaline ion precursors to the reduction of the battery price. However, the difficulties in the supply of raw materials for LIBs, such as shortages in lithium carbonates and cobalt ores, could make lithium and cobalt-free systems, such as SIBs, attractive and cost-competitive alternatives. Compared to other, more exotic chemistries including Ca2+, Mg2+ and Al3+ batteries, SIBs are nowadays considered one as the most promising alternative to LIBs. Despite the extensive research, anode materials for SIBs still represent a serious problem for the commercial exploitation of this technology. Accordingly, the doctoral research on SIBs has been focused on anode materials. In particular, the attention was directed towards conversion oxides. Compared to intercalation materials, conversion-based ones have higher capacities but are more challenging to deal with because of the high volume variation during cycling. This challenge was addressed by material's nanostructuring and morphology control which proved to significantly reduce the pulverization of the active material. Different anode candidates have been studied during the doctoral work. Cobalt oxide nanofibers have been here explored as a first prototype for conversion materials in sodium ion batteries. The sodiation-desodiation mechanism is analyzed by means of ex situ XRD which led to a deeper understanding of the conversion reaction in SIBs. A cost-effective and environmentally benign alternative based on iron oxide is then considered. The limits of iron (III) oxide are tackled by combining the advantages of the nanostructuring and the doping with an aliovalent element. Si-doped Fe2O3 nanofibers are synthesized via an easy scalable process based on the electrospinning method. It is found that Si-addition improves the transport properties as well as induces changes in the crystal structure and morphology. In the final section of the thesis, potassium-ion batteries (KIBs) are examined as a promising alternative to sodium ion batteries. KIBs exhibit all the benefits of SIBs, with the additional advantage that graphite, can reversibly accommodate K-ions. On the positive side, Potassium manganese hexacyanoferrate (KMnHCF), has been reported to provide high operating voltages and satisfactory capacity retention. The proposed research activity presents the use of an ionic liquid based electrolyte compatible with the most promising anode and cathode for KIBs. In addition, a high-throughput optimization of the KMnHCF synthesis is reported. The selected candidates are then fully characterized, and their electrochemical properties investigated. The optimized material exhibits the highest ever reported coulombic efficiency for the KMHCF. This find, opens up the possibility of highly efficient, high energy potassium ion batteries.Thanks to their superior energy and power density, lithium-ion batteries (LIBs) currently dominate the market of power sources for portable devices. The economy of scale and engineering optimizations have driven the cost of LIBs below the 200 $/KWh at the pack level. This catalyzed the market penetration of electric vehicles and made them a viable candidate for stationary energy storage. However, the rapid market expansion of LIBs raised growing concerns about the future sustainability of this technology. In particular, lithium and cobalt supplies are considered vulnerable, primarily because of the geopolitical implications of their high concentration in only a few countries. In the search for the next generation secondary batteries, known as post-lithium ion batteries, candidates that do not use rare metals have been extensively investigated in the last 10 years. Sodium-ion batteries (SIBs) attracted considerable attention thanks to the high abundance of the precursors and wide distribution of sodium on the earth's crust. As a matter of fact, as it will be pointed out during the dissertation, it is not straightforward to allocate the reduction of the price of the alkaline ion precursors to the reduction of the battery price. However, the difficulties in the supply of raw materials for LIBs, such as shortages in lithium carbonates and cobalt ores, could make lithium and cobalt-free systems, such as SIBs, attractive and cost-competitive alternatives. Compared to other, more exotic chemistries including Ca2+, Mg2+ and Al3+ batteries, SIBs are nowadays considered one as the most promising alternative to LIBs. Despite the extensive research, anode materials for SIBs still represent a serious problem for the commercial exploitation of this technology. Accordingly, the doctoral research on SIBs has been focused on anode materials. In particular, the attention was directed towards conversion oxides. Compared to intercalation materials, conversion-based ones have higher capacities but are more challenging to deal with because of the high volume variation during cycling. This challenge was addressed by material's nanostructuring and morphology control which proved to significantly reduce the pulverization of the active material. Different anode candidates have been studied during the doctoral work. Cobalt oxide nanofibers have been here explored as a first prototype for conversion materials in sodium ion batteries. The sodiation-desodiation mechanism is analyzed by means of ex situ XRD which led to a deeper understanding of the conversion reaction in SIBs. A cost-effective and environmentally benign alternative based on iron oxide is then considered. The limits of iron (III) oxide are tackled by combining the advantages of the nanostructuring and the doping with an aliovalent element. Si-doped Fe2O3 nanofibers are synthesized via an easy scalable process based on the electrospinning method. It is found that Si-addition improves the transport properties as well as induces changes in the crystal structure and morphology. In the final section of the thesis, potassium-ion batteries (KIBs) are examined as a promising alternative to sodium ion batteries. KIBs exhibit all the benefits of SIBs, with the additional advantage that graphite, can reversibly accommodate K-ions. On the positive side, Potassium manganese hexacyanoferrate (KMnHCF), has been reported to provide high operating voltages and satisfactory capacity retention. The proposed research activity presents the use of an ionic liquid based electrolyte compatible with the most promising anode and cathode for KIBs. In addition, a high-throughput optimization of the KMnHCF synthesis is reported. The selected candidates are then fully characterized, and their electrochemical properties investigated. The optimized material exhibits the highest ever reported coulombic efficiency for the KMHCF. This find, opens up the possibility of highly efficient, high energy potassium ion batteries.
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Zhang, Huang [Verfasser], and S. [Akademischer Betreuer] Passerini. "Polyanionic cathode materials for sodium-ion batteries / Huang Zhang ; Betreuer: S. Passerini." Karlsruhe : KIT-Bibliothek, 2019. http://d-nb.info/1178528162/34.
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Richards, William D. (William Davidson). "Ab initio investigations of solid electrolytes for lithium- and Sodium-ion batteries." Thesis, Massachusetts Institute of Technology, 2017. http://hdl.handle.net/1721.1/108967.
Full textAbstract:
Thesis: Ph. D., Massachusetts Institute of Technology, Department of Materials Science and Engineering, 2017.Cataloged from PDF version of thesis.
Includes bibliographical references (pages 119-127).
Solid-state electrolytes have the potential to dramatically improve the safety and longevity of state-of-the-art battery technology by replacing the flammable organic electrolytes currently employed in Li-ion batteries. Recent advances in the development of new thiophosphate electrolytes have reenergized the field by achieving room temperature conductivities exceeding those liquid electrolytes, but a number of practical challenges to their widespread adoption still exist. This thesis applies ab initio computational methods based on density functional theory to investigate the structural origins of high conductivity in ionic conductor materials and provides a thermodynamic explanation of why the integration of these newly developed thiophosphates into high-rate cells has proven difficult in practice, often resulting in high interfacial resistance. As a result of these computational investigations, we report the prediction and synthesis of a new high performance sodium-ion conducting material: NaioSnP 2S 12, with room temperature ionic conductivity of 0.4 mS cm-1, which rivals the conductivity of the best sodium sulfide solid electrolytes to date. We computationally investigate the variants of this compound where Sn is substituted by Ge or Si and find that the latter may achieve even higher conductivity. We then investigate the relationship between anion packing and ionic transport in fast Li-ion conductors, finding that a bcc-like anion framework is desirable for achieving high ionic conductivity, and that this anion arrangement is present in a disproportionately high number of known Li-conducting materials, including Na10SnP2S12 and its structural analog Li10GeP2S2 . Using this bcc anion lattice as a screening criterion, we show that the I4 material LiZnPS4 also contains such a framework and has the potential for very high ionic conductivity. While the stoichiometric material has poor ionic conductivity, engineering of its composition to introduce interstitial lithium defects is able to exploit the low migration barrier of the bcc anion structure. Thermodynamic calculations predict a solid-solution regime in this system that extends to x = 0.5 in Li1+2xZn-xPS 4 , thus it may yield a new ionic conductor with exceptionally high lithium-ion conductivity, potentially exceeding 50 mS cm- 1 at room temperature. Finally, we develop a computational methodology to examine the thermodynamics of formation of resistive interfacial phases through mixing of the electrode and electrolyte. The results of the thermodynamic model of interfacial phase formation are well correlated with experimental observations and battery performance, and predict that thiophosphate electrolytes have especially high reactivity with high voltage oxide cathodes and a narrow electrochemical stability window. We also find that a number of known electrolytes are not inherently stable, but react in situ with the electrode to form passivating but ionically conducting barrier layers.
by William D. Richards.
Ph. D.
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LI, TAO. "The Study of Various Anode Materials for Sodium (or Lithium)-Ion Batteries." Doctoral thesis, Università degli studi di Genova, 2019. http://hdl.handle.net/11567/939856.
Full textAbstract:
room-temperature sodium-ion batteries (NIBs or SIBs) have raised a great deal of attention for grid-level applications considering the sustainability advantages of NIBs. Significant progress has been made for NIB cathodes by adapting the knowledge learned on lithium-ion batteries (LIBs). Simultaneously, numerous attempts have been made to find suitable anodes for NIBs, however, the research to improve NIB technologies rema ns a challenge. This thesis presents fundamental studies of various anode materials for NIBs from different aspects.
Surface and interface engineering of nanostructured anatase TiO2 anode through Al2O3 surface modification and wise electrolyte selection is conducted. The results show that Al2O3 coating provides beneficial effects to the TiO2-based anodes and the modified TiO2 exhibits significant improvements in cycling performance using electrolyte with binary ethylene carbonate (EC) and propylene carbonate (PC) solvent mixture without the need of the commonly used fluoroethylene carbonate (FEC) additive. The achieved excellent electrochemical performance (a high reversible capacity of 188.1 mAh g−1 at 0.1C after 50 cycles, good rate capability up to 5C, and long-term cycling performance for 650 cycles at a high rate of 1C) can be ascribed to the synergistic effects of surface and interface engineering enabling the formation of a stable and highly ionic conductive interface layer in EC:PC based electrolyte which combines the native SEI film and an ‘artificial’ SEI layer of irreversibly formed Na−Al−O.
A dual-modification approach of Mo doping combined with AlF3 coating is also introduced to enhance the sodium storage activity of anatase TiO2. The Mo-doped anatase TiO2 synthesized by a simple co-precipitation method delivers an enhanced reversible capacity compare to pristine TiO2 (139.8 vs. 100.7 mAh g−1 at 0.1C after 50 cycles) due to enhanced electronic/ionic conductivity. Via further coating AlF3 using a modified solid-state method, a much higher reversible capacity of 178.9 mAh g−1 with good cycle stability and excellent rate capabilities up to 10C can be finally obtained.
The experimental results indicate that AlF3 surface coating could effectively reduce solid electrolyte interfacial resistance, enhance electrochemical reactivity at the surface/interface region, and lower polarization during cycling.
As for alloy-type anode of Sn with high theoretical capacity of 847 mAh g−1 but experiences a high volume expansion of 420% upon sodiation, we carry out a fundamental study of the degradation mechanisms that occur in Sn during sodiation-desodiation by employing a Sn thick film as the anode. Electron microscopy reveals new deformation mechanisms, as multiple Sn whiskers nucleate on the surface of the Sn, while pores form within the Sn (over the Na-ion penetration distance) after electrochemical cycling. These mechanisms are in addition to the dry lake-bed fracture that is also observed. Such whiskers and pores may be more-subtle at the nanoscale, and therefore have not been reported for sub-micron Sn particles in porous electrodes. The simplified planar geometry of the Sn sheet allows to dispense with the influence of the binder and carbon additives that are required in porous electrodes and the implementation of the Randles-Sevick equation provides a first experimental estimate for the diffusion coefficient of Na+ in Sn as 6.45×10−12 cm2 s−1.
Finally, we explore facile synthesis of carbon materials from low cost carbon source of CaC2 using a novel sulfur-based thermo-chemical etching technique.
Comprehensive analysis using X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and N2 adsorption−desorption isotherms, reveals a highly graphitized mesoporous structure for the CaC2-derived carbon with a specific surface area of 159.5 m2 g−1. Microscopic analysis displays micron-scale mesoporous
frameworks (4–20 μm) with a distinct layered structure along with agglomerates of highly graphitized nanosheets (about 10 nm in thickness and 1–10 μm of lateral size).
The application of the as-prepared carbon materials as anode for NIBs and LIBs is also preliminarily studied.
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Huynh, Le Thanh Nguyen. "Les accumulateurs au sodium et sodium-ion, une nouvelle génération d’accumulateurs électrochimiques : synthèse et électrochimie de nouveaux matériaux d’électrodes performants." Thesis, Paris Est, 2016. http://www.theses.fr/2016PESC1123/document.
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Les accumulateurs au lithium jouent un rôle important comme source d'alimentation pour les appareils électroniques portables en raison de leur forte capacité gravimétrique et volumétrique et leur haute tension. En outre, la technologie lithium-ion est la mieux placée pour une application à grande échelle, telle que le véhicule électrique, ce qui pose un problème de ressource et à terme, de coût. Une des réponses envisagées sur le plan économique et environnemental est le développement d’accumulateurs sodium-ion. Dans tous les cas, le problème scientifique consiste à proposer des matériaux d’insertion des ions sodium avec un caractère réversible de la réaction électrochimique, et une durée de vie compétitive par rapport aux systèmes au lithium. Le travail présenté se situe dans cet effort de recherche. Les potentialités de matériaux dérivés du pentoxyde de vanadium, de structure 2D, sont étudiées comme composés d’intercalation du sodium: le composé de référence V2O5, le bronze performant dérivé de V2O5 de formule K0,5V2O5, ε’-V2O5, ainsi que le composé au manganèse de type lamellaire : la birnessite sol-gel et sa forme dopée au cobalt. Les relations structure-électrochimie sont élucidées à travers une étude combinant propriétés électrochimiques, diffraction des Rayons X et spectroscopie Raman des matériaux à différents taux d’insertion, en fin de réaction et après cyclages galvanostatiques. De nouvelles phases sont obtenues et des capacités spécifiques comprises entre 100 et 160 mAh/g dans le domaine de potentiel 4V-1V peuvent être obtenues avec parfois une stabilité remarquable comme dans le cas de NaV2O5 et ε’-V2O5Since commercialization, Li-ion batteries have been playing an important role as power source for portable electronic devices because of high gravimetric, volumetric capacity and high voltage. Furthermore, the lithium-ion technology is best suited for large-scale application, such as electric vehicles, which poses a resource problem and ultimately cost. On the contrary, sodium is a most abundant element, inexpensive and similarly properties as lithium. In order to solve the problem of lithium raw resource, sodium is proposed as a solution for next generation power source storage. This work investigates the potential derivative vanadium pentoxide materials as sodium intercalation compounds: the V2O5 reference compound, the promizing potassium bronze K0,5V2O5, ε'-V2O5, as well as a lamellar manganese oxide: the sol-gel birnessite and its doped cobalt form. The structure-electrochemistry relationships are clarified through a study combining electrochemical properties, X-ray diffraction and Raman spectroscopy of materials at different insertion rate, end of the reaction and after galvanostatic cycling. New phases are highlighted and specific capacities between 100 and 160 mAh / g in the field of 4V-1V potential can be obtained with sometimes remarkably stable as in the case of NaV2O5 and ε'-V2O5
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Dou, Xinwei [Verfasser], and S. [Akademischer Betreuer] Passerini. "Hard Carbon Anode Materials for Sodium-ion Batteries / Xinwei Dou ; Betreuer: S. Passerini." Karlsruhe : KIT-Bibliothek, 2019. http://d-nb.info/1179963695/34.
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Posch, P., P. Bottke, M. Wilkening, and I. Hanzu. "Hydrothermally Synthesized Nanostructured Sodium Titanates as Negative Electrode Materials for Na-Ion Batteries." Diffusion fundamentals 21 (2014) 22, S.1, 2014. https://ul.qucosa.de/id/qucosa%3A32432.
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CHEN, LIN. "Investigation of inorganic nanocrystals as electrode material for lithium and sodium ion batteries." Doctoral thesis, Università degli studi di Genova, 2018. http://hdl.handle.net/11567/929837.
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The worldwide demand for a clean, safe, high specific capacity and high energy rechargeable batteries systems keeps increasing. Li-ion batteries (LIBs) and Na-ion batteries (NIBs) have been proved to be reliable technologies, for a large variety of applications, ranging from portable high-end electronics, stationary.
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Wang, Luyuan Paul. "Matériaux à hautes performance à base d'oxydes métalliques pour applications de stockage de l'énergie." Thesis, Université Grenoble Alpes (ComUE), 2017. http://www.theses.fr/2017GREAI031/document.
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Le cœur de technologie d'une batterie réside principalement dans les matériaux actifs des électrodes, qui est fondamental pour pouvoir stocker une grande quantité de charge et garantir une bonne durée de vie. Le dioxyde d'étain (SnO₂) a été étudié en tant que matériau d'anode dans les batteries Li-ion (LIB) et Na-ion (NIB), en raison de sa capacité spécifique élevée et sa bonne tenue en régimes de puissance élevés. Cependant, lors du processus de charge/décharge, ce matériau souffre d'une grande expansion volumique qui entraîne une mauvaise cyclabilité, ce qui empêche la mise en oeuvre de SnO₂ dans des accumulateurs commerciaux. Aussi, pour contourner ces problèmes, des solutions pour surmonter les limites de SnO₂ en tant qu'anode dans LIB / NIB seront présentées dans cette thèse. La partie initiale de la thèse est dédié à la production de SnO₂ et de RGO (oxyde de graphène réduit)/SnO₂ par pyrolyse laser puis à sa mise en oeuvre en tant qu'anode. La deuxième partie s'attarde à étudier l'effet du dopage de l'azote sur les performances et permet de démontrer l'effet positif sur le SnO₂ dans les LIB, mais un effet néfaste sur les NIB. La partie finale de la thèse étudie l'effet de l'ingénierie matricielle à travers la production d'un composé ZnSnO₃. Enfin, les résultats obtenus sont comparés avec l'état de l'art et permettent de mettre en perspectives ces travauxThe heart of battery technology lies primarily in the electrode material, which is fundamental to how much charge can be stored and how long the battery can be cycled. Tin dioxide (SnO₂) has received tremendous attention as an anode material in both Li-ion (LIB) and Na-ion (NIB) batteries, owing to benefits such as high specific capacity and rate capability. However, large volume expansion accompanying charging/discharging process results in poor cycleability that hinders the utilization of SnO₂ in commercial batteries. To this end, engineering solutions to surmount the limitations facing SnO₂ as an anode in LIB/NIB will be presented in this thesis. The initial part of the thesis focuses on producing SnO₂ and rGO (reduced graphene oxide)/SnO₂ through laser pyrolysis and its application as an anode. The following segment studies the effect of nitrogen doping, where it was found to have a positive effect on SnO₂ in LIB, but a detrimental effect in NIB. The final part of the thesis investigates the effect of matrix engineering through the production of a ZnSnO₃ compound. Finally, the obtained results will be compared and to understand the implications that they may possess
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Lu, Xiaoxiao. "The improvement of electrochemical performance of SnO2-based nanocomposites as anodes for lithium ion and sodium ion batteries." Thesis, University of Manchester, 2015. https://www.research.manchester.ac.uk/portal/en/theses/the-improvement-of-electrochemical-performance-of-sno2based-nanocomposites-as-anodes-for-lithium-ion-and-sodium-ion-batteries(d0d78e2a-2ed4-4274-b3fe-9c018992e15a).html.
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Nowadays, low carbon economy becomes a significant topic over the world. Due to the decreasing amount of fossil energy source and the worsening environmental pollution, traditional energy sources should be transferred to renewable energy sources. A transition to renewable energy will require radical changes to systems and technologies for energy storage. Lithium ion (Li-ion) batteries are now considered as the most important electrochemical energy source for portable devices, electrical vehicles and expected to be used in grid electrical energy storage. Beside on Li-ion batteries, sodium ion (Na-ion) batteries are another promising energy source, which have the advantages in cost, safety and environmental factors, and they could be used for stationary energy storage systems and large vehicles. Tin-based nanocomposites are promising to replace the traditional graphite for Li-ion batteries to achieve a higher battery performance. In 2005, Sony Corporation launched the first Sn-based anode Li-ion batteries (Nexelion) to obtain a 50% increase in volumetric capacity over the conventional battery, which marked Li-ion batteries to enter into a new cutting edge. However, Sn-based materials faced with challenges. The battery performance was limited by a low cycling life and low rate performance, and methods should be devised to overcome these shortcomings. In this thesis, SnO2-based nanocomposites, including the graphene-SnO2, the carbon-coated graphene-SnO2 and the carbon-coated nanostructured SnO2 have been prepared and investigated as anodes for Li-ion and Na-ion batteries. The microstructure, electrochemical performances and even the degradation mechanisms have been investigated as the effects for different composite materials. Chapter 4 reports an amorphous carbon coated graphene-SnO2 composite which exhibited an enhanced cycling stability. In previous researches, the performance enhancements of that type of materials were commonly attributed to the carbon coating enhancing the electronic conductivity. However, it is found that the carbon coating deeply relates to the microstructure stability of the active materials, the performance enhancement can be attributed to the enhancement of structural stability. Chapter 5 reports same composites with various graphene to amorphous carbon mass ratios. In this chapter, we try to find out the optimized composition and understanding the different roles of graphene and amorphous carbon in that type of composites. It is found that an optimised graphene to carbon mass ratio can effectively enhance the structural stability and the electrode conductivity. Chapter 6 reports a carbon-coated flower-like nanostructured SnO2 for Na-ion battery application, which has been demonstrated to have a high reversible capacity and high rate performance. The carbon coating is found to help in the formation of a high quality solid electrolyte interface (SEI) layer on the surface of the active materials. These researches focus on modifying SnO2 and SnO2-based materials by carbon coating technologies, which aim to develop novel electrode materials to obtain a better battery performance for Li-ion and Na-ion batteries.
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Castro, Alexandre. "Développement de batteries tout solide sodium ion à base d’électrolyte en verre de chalcogénures." Thesis, Rennes 1, 2018. http://www.theses.fr/2018REN1S126/document.
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L'évolution des consommations énergétiques au cours des dernières décennies entraîne des modifications majeures dans la conception des systèmes électriques autonomes à fournir, que ce soit pour des applications électriques ou électroniques. La nécessité présente de réaliser des générateurs capables de délivrer l'énergie suffisante, avec une garantie de sûreté maximale, impose à la recherche l'exploration de nouvelles voies de stockage. Les voies actuelles par accumulateurs au lithium tendent à montrer leurs limites, tant stratégiques qu'environnementales. Dans ce cadre, la construction de nouveaux systèmes électrochimiques mettant en œuvre le sodium ouvre une possibilité de réalisation d'accumulateurs sans lithium. Le besoin de batteries toujours plus performantes oblige à des conceptions innovantes, abandonnant la voie liquide au profit de systèmes tout solide plus sécuritaires. De plus, la miniaturisation de l'électronique conduit à revoir le dimensionnement des batteries, vers des batteries de type micro, pour lesquelles l'intérêt d'un empilement tout solide n'est plus à démontrer. Aujourd'hui, des verres de chalcogénures au soufre permettent l'accès à des conductivités ioniques qui laissent entrevoir la possibilité d'une réalisation de batteries tout solide, à la fois sous forme de micro batteries ou de batteries massives. Un effort de recherche a été porté à la formulation de ces verres de chalcogénures afin d'obtenir des conductivités ioniques maximales et des propriétés autorisant leur utilisation comme électrolyte. La modification de ces verres met alors en lumière l'intérêt des différents éléments les composant. L'étude de la mise en forme de l'électrolyte par dépôts de type couches minces (obtenues par Radio Fréquence Magnétron Sputering, RFMS) prouve la faisabilité de ces micro batteries tout solide au sodium. Par la suite, la réalisation de batteries massives tout solide a demandé la synthèse de deux matériaux de cathode (NaCrO2 et Na[Ni0,25Fe0,5Mn0,25]O2) et de deux matériaux d'anode (Na15Sn4 et Na) permettant ainsi la mise en œuvre de quatre empilements électrochimiques, tous caractérisés comme accumulateurs. Enfin, l'amélioration des interfaces grâce à un gel-polymère a permis de perfectionner les propriétés des assemblages avec notamment une augmentation des vitesses de charge/décharge et une mobilisation accrue des matériaux actifs de cathodeThe evolution of energy consumption in recent decades has led to major changes in the design of autonomous electrical systems dedicated to either electrical or electronic applications. The present demand to build generators capable of delivering sufficient energy, with a guarantee of maximum safety, requires to explore new storage routes. The current lithium battery routes tend to show their limits, both strategic and environmental. In this context, the construction of new electrochemical systems implementing sodium opens the way of the lithium-free accumulators production. The need for ever more efficient batteries requires innovative designs, giving up the liquid path in favor of stronger solid systems. In addition, the miniaturization of electronics leads to a review of the size of the batteries, to micro-type batteries, for which the interest of a solid stack is no longer to demonstrate. Today, sulfur chalcogenide glasses allow access to ionic conductivities that suggest the possibility of a realization of all solid batteries, both in the form of micro batteries or massive batteries. A research effort has been made to formulate these chalcogenide glasses in order to obtain a maximum of ionic conductivity and properties allowing their use as electrolytes. The composition of these glasses highlights the interest of the different elements for such properties. The study of the electrolyte shaping by thin-film deposition (obtained by Radio Frequency Magnetron Sputering, RFMS) proves the feasibility of these all-solid sodium micro-batteries. Subsequently, the realization of massive all solid batteries required the synthesis of two cathode materials (NaCrO2 and Na [Ni0.25Fe0.5Mn0.25]O2) and two anode materials (Na15Sn4 and Na) thus allowing the implementation of four electrochemical stacks, all characterized as accumulators. Finally, the improvement of the interfaces thanks to a gel-polymer made it possible to improve the properties of the assemblies with notably an increase of the speeds of charge / discharge and an enhanced mobilization of the cathode active materials
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Saavedra, Rios Carolina del Mar. "Etude des carbones durs issus de la biomasse pour l’application dans les batteries Sodium-ion." Thesis, Université Grenoble Alpes, 2020. https://thares.univ-grenoble-alpes.fr/2020GRALI072.pdf.
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La demande croissante en batteries Lithium-ion a suscité une certaine inquiétude concernant l'approvisionnement en matières premières critiques nécessaires à leur production, en particulier les ressources en Li, Co, Ni et Cu. La technologie Sodium-ion apparait comme une alternative pouvant utiliser des ressources abondantes et uniformément réparties, et qui pourrait réduire le coût des batteries par rapport au Lithium-ion. Toutefois, le débouché commercial des batteries Sodium-ion est encore limité par le développement de matériaux d'électrode négative à haute performance et bas coût. L'option la plus prometteuse est un matériau carboné désordonné appelé carbone dur, obtenu par traitement thermique à haute température de précurseurs organiques. Malgré ses bonnes performances, le carbone dur est toujours plus cher que le graphite utilisé dans les batteries Lithium-ion, étant donné le coût élevé de ses précurseurs synthétiques. La biomasse lignocellulosique a récemment attiré l'attention en tant que précurseur du carbone dur, étant donné sa nature renouvelable, son accessibilité et son faible coût. Cependant, la grande variabilité des matières premières de la biomasse ainsi que le faible rendement de la réaction de pyrolyse, rendent leur application commerciale plutôt difficile. De plus, le rôle de la composition de la biomasse sur les propriétés du carbone dur n’est pas complètement compris. Le travail de recherche présenté ici est une approche interdisciplinaire, visant à élucider l'impact de la composition de la biomasse sur les propriétés physico-chimiques et électrochimiques des carbones durs résultants ainsi que le rendement de leur synthèse. Un ensemble de 25 précurseurs ont été sélectionnés pour cette étude. La composition de chaque précurseur, telles que le contenu organique et inorganique élémentaire, et le contenu macromoléculaire, ont été évaluées. Les carbones durs synthétisés ont été caractérisés par des techniques de XRD, Raman, SEM, TEM, SAXS, XPS et de cyclage galvanostatique. Le contenu et la composition inorganique du précurseur, en particulier la présence de composés de Si, Ca et K, ont semblé jouer un rôle essentiel dans le développement de la structure et de la surface du carbone dur. Par conséquent, ils ont un impact négatif important sur les performances du carbone dur, en produisant des irréversibilités élevées. Compte tenu de leur faible teneur en cendres couplé à leur faible cout et leur faible impact environnemental, les résidus forestiers et certain résidus agricoles, semblent être le meilleur compromis pour l'application du carbone durThe ever-increasing demand for Lithium-ion batteries has raised some concern regarding the supply of the critical raw materials needed for their production, especially the Li, Co, Ni and Cu resources. The Sodium-ion technology appears to be an alternative which potentially uses abundant, and evenly distributed resources, that is able to reduce the cost of the batteries compared to Lithium-ion. However, the commercial intrusion of Sodium-ion batteries is still limited by the development of low-cost and high-performance negative electrode material. The most promising option is a disordered carbonaceous material called hard carbon obtained from high-temperature thermal treatment of organic precursors. Despite its good performance, hard carbon is still more expensive than the graphite used in Lithium-ion batteries, given the high cost of the synthetic precursors. Lignocellulosic biomass has recently attracted attention as a hard carbon precursor, given its renewable nature, accessibility, and low cost. However, the high variability of biomass feedstock, together with the poor yield of the pyrolysis reaction, make their commercial application rather difficult. Moreover, there is no clear understanding of the biomass composition role on the hard carbon properties. The research work presented here is an interdisciplinary approach, aiming to elucidate the biomass composition's impact on the physicochemical and electrochemical properties of the derived hard carbons as well as their synthesis yield. A set of 25 lignocellulosic biomass precursors have been selected for this study. The composition of each biomass precursor, such as the elemental organic and inorganic content, and the macromolecular contents were evaluated in detail. The synthesised hard carbons were characterised by XRD, Raman, SEM, TEM, SAXS, XPS, and galvanostatic cycling techniques. The inorganic content and composition of the precursor, particularly the presence of Si, Ca, and K compounds, was observed to play a critical role in developing the hard carbon structure and surface. Therefore, they have a strong negative impact on hard carbon performances, producing high irreversibility. Because of their low ash-content, coupled with their low cost and environmental impact, precursors such as forestry residues, and some agricultural residues, appeared to be the best compromise for hard carbon application
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Brown, James Emery. "Advances in electrical energy storage using core-shell structures and relaxor-ferroelectric materials." Diss., Kansas State University, 2018. http://hdl.handle.net/2097/38779.
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Doctor of PhilosophyDepartment of Chemistry
Jun Li
Electrical energy storage (EES) is crucial in todays’ society owing to the advances in electric cars, microelectronics, portable electronics and grid storage backup for renewable energy utilization. Lithium ion batteries (LIBs) have dominated the EES market owing to their wide use in portable electronics. Despite the success, low specific capacity and low power rates still need to be addressed to meet the increasing demands. Particularly, the low specific capacity of cathode materials is currently limiting the energy storage capability of LIBs. Vanadium pentoxide (V₂O₅) has been an emerging cathode material owing to its low cost, high electrode potential in lithium-extracted state (up to 4.0 V), and high specific capacities of 294 mAh g⁻¹ (for a 2 Li⁺/V₂O₅ insertion process) and 441 mAh g⁻¹ (for a 3 Li⁺/V₂O₅ insertion process). However, the low electrical conductivities and slow Li⁺ ion diffusion still limit the power rate of V₂O₅. To enhance the power-rate capability we construct two core-shell structures that can achieve stable 2 and 3 Li⁺ insertion at high rates. In the first approach, uniform coaxial V₂O₅ shells are coated onto electrospun carbon nanofiber (CNF) cores via pulsed electrodeposition. The materials analyses confirm that the V₂O₅ shell after 4 hours of thermal annealing at 300 °C is a partially hydrated amorphous structure. SEM and TEM images indicate that the uniform 30 to 50 nm thick V₂O₅ shell forms an intimate interface with the CNF core. Lithium insertion capacities up to 291 and 429 mAh g⁻¹ are achieved in the voltage ranges of 4.0 – 2.0 V and 4.0 – 1.5 V, respectively, which are in good agreement with the theoretical values for 2 and 3 Li⁺/V₂O₅ insertion. Moreover, after 100 cycles, remarkable retention rates of 97% and 70% are obtained for 2 and 3 Li⁺/V₂O₅ insertion, respectively. In the second approach, we implement a three-dimensional (3D) core-shell structure consisting of coaxial V₂O₅ shells sputter-coated on vertically aligned carbon nanofiber (VACNF) cores. The hydrated amorphous microporous structure in the “as-deposited” V₂O₅ shells and the particulated nano-crystalline V₂O₅ structure formed by thermal annealing are compared. The former provides remarkably high capacity of 360 and 547 mAh g⁻¹ in the voltage range of 4.0 – 2.0 V and 4.0 – 1.5 V, respectively, far exceeding the theoretical values for 2 and 3 Li⁺/V₂O₅ insertion, respectively. After 100 cycles of 3 Li⁺/V₂O₅ insertion/extraction at 0.20 A g⁻¹ (~ C/3), ~ 84% of the initial capacity is retained. After thermal annealing, the core-shell structure presents a capacity of 294 and 390 mAh g⁻¹, matching well with the theoretical values for 2 and 3 Li⁺/V₂O₅ insertion. The annealed sample shows further improved stability, with remarkable capacity retention of ~100% and ~88% for 2 and 3 Li⁺/V₂O₅ insertion/extraction. However, due to the high cost of Li. alternative approaches are currently being pursued for large scale production. Sodium ion batteries (SIB) have been at the forefront of this endeavor. Here we investigate the sodium insertion in the hydrate amorphous V₂O₅ using the VACNF core-shell structure. Electrochemical characterization was carried out in the potential ranges of 3.5 – 1.0, 4.0 – 1.5, and 4.0 – 1.0 (vs Na/Na⁺). An insertion capacity of 196 mAh g-1 is achieved in the potential range of 3.5 – 1.0 V (vs Na/Na⁺) at a rate of 250 mA g⁻¹. When the potential window is shifted upwards to 4.0 – 1.5 V (vs Na/Na⁺) an insertion capacity of 145 mAh g⁻¹ is achieved. Moreover, a coulombic efficiency of ~98% is attained at a rate of 1500 mA g⁻¹. To enhance the energy density of the VACNF-V₂O₅ core-shell structures, the potential window is expanded to 4.0 – 1.0 V (vs Na/Na⁺) which achieved an initial insertion capacity of 277 mAh g⁻¹. The results demonstrate that amorphous V₂O₅ could serve as a cathode material in future SIBs.
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Pfeifer, Kristina [Verfasser], and H. [Akademischer Betreuer] Ehrenberg. "Reactivity and Interplay of Critical Components in Sodium-Ion Batteries / Kristina Pfeifer ; Betreuer: H. Ehrenberg." Karlsruhe : KIT-Bibliothek, 2021. http://d-nb.info/1227451318/34.
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Difi, Siham. "Phosphates de type NASICON comme matériaux d'électrode pour batteries sodium-ion à haute densité d'énergie." Thesis, Montpellier, 2016. http://www.theses.fr/2016MONTT212/document.
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Ce mémoire est consacré à l’étude des composites à base de phosphates de type NASICON comme matériaux d’électrode pour batteries sodium-ion : Na1+xFexTi2-x(PO4)3/C et Na1+xFexSn2-x(PO4)3/C avec 0 ≤ x ≤ 1. Ces composites ont été synthétisés par voie solide suivie d’une pyrolyse avec le saccharose. Ils sont constitués de particules ayant une porosité élevée et enrobées par du carbone conférant à l’électrode une bonne conductivité ionique et électronique. Les mécanismes réactionnels se produisant lors des cycles de charge-décharge ont été analysés en mode operando par diffraction des rayons X, spectroscopies Mössbauer du 57Fe et de 119Sn et spectroscopie d’absorption X. Pour les composites fer-titane, ces mécanismes sont essentiellement basés sur la diffusion des ions Na+ dans les canaux des phases cristallisées avec changements d’état d’oxydation des métaux. Pour les composites fer-étain, les mécanismes sont plus complexes incluant insertion, conversion conduisant à la destruction des phases NASICON, puis formation d’alliages NaxSn. Les meilleures performances électrochimiques ont été obtenues pour Na1,5Fe0,5Ti1,5(PO4)3/C avec un potentiel de fonctionnement de 2,2 V vs Na+/Na0. Même si ces deux familles de matériaux peuvent être utilisées à plus bas potentiel, les performances doivent être améliorées pour envisager leur application comme électrode négativeThis thesis is devoted to the study of phosphate based composites with NASICON type structure, that are used as electrode materials for sodium-ion batteries: Na1+xFexTi2-x (PO4)3/C et Na1+xFexSn2-x(PO4)3/C with 0 ≤ x ≤ 1. These composites were synthesized by solid state route followed by a pyrolysis reaction with sucrose. They consist of particles having high porosity and coated with carbon giving to the electrode good ionic and electronic conductivity. The reaction mechanisms occurring during charge-discharge cycles were analyzed in operando mode, by X-ray diffraction, 57Fe and 119Sn Mössbauer spectroscopies and X-ray absorption spectroscopy. For the iron-titanium composites, the mechanisms are essentially based on the diffusion of Na+ in the channels of the crystalline phases with changes of transition metal oxidation state. For iron-tin composites, the mechanisms are more complex including insertion, conversion leading to the destruction of the NASICON phases and then reversible formation of NaxSn alloys. The best electrochemical performances were obtained for Na1,5Fe0,5Ti1,5(PO4)3/C with an operating potential of 2.2 V vs. Na+/Na0. Although these two types of materials can be used at lower potential, the performances must be improved to consider their application as the negative electrode
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Göktaş, Mustafa [Verfasser], Philipp [Gutachter] Adelhelm, and Andrea [Gutachter] Balducci. "Graphite as co-intercalation host for sodium ion batteries / Mustafa Göktaş ; Gutachter: Philipp Adelhelm, Andrea Balducci." Jena : Friedrich-Schiller-Universität Jena, 2019. http://d-nb.info/1207271713/34.
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GENTILE, ANTONIO. "MXene-based materials for alkaline-ion batteries: synthesis, properties, applications." Doctoral thesis, Università degli Studi di Milano-Bicocca, 2022. http://hdl.handle.net/10281/382748.
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La produzione sempre maggiore di dispositivi portatili e auto elettriche chiede al mercato di produrre dispositivi efficienti in grado di poter accumulare l’energia elettrica. Per questo tipo di tecnologie in cui la miniaturizzazione del dispositivo è essenziale, le batterie litio ione (LIBs) sono diventate il mezzo di accumulare energia. La ricerca su queste batterie è focalizzata ad ottenere dispositivi sempre più performanti con materiali elettrodici ad alte capacità gravimetriche e volumetriche. Accanto all’aspetto tecnologico, legato alla ottimizzazione dei materiali, vi è anche quello dell’approvvigionamento dei componenti attivi della batteria, tra tutti il litio.
La problematica attualmente è affrontata studiando batterie con altri metalli alcalini (Na e K). Di questi dispositivi non esistono però materiali già standardizzati malgrado la ricerca, specialmente sulle batterie sodio ione (SIB), sia partita solo qualche anno più tardi rispetto quella delle LIB; per cui queste tecnologie oggi sono destinate ad affiancare quelle delle LIB per sopperire all’enorme richiesta di mercato di batterie per i veicoli del futuro.
L’obbiettivo del presente lavoro è stato quello di sviluppare materiali anodici a base di MXene per ottenere efficienti anodi per batterie sodio e litio ione. I MXenes sono una famiglia di carburi di metalli di transizione con una struttura 2D che sembrerebbe promettente per l’intercalazione di diversi ioni grazie ad una grande flessibilità ed adattabilità strutturale nei confronti del tipo di ione intercalante. L’intercalazione degli ioni avviene con un meccanismo pseudocapacitivo per cui i materiali hanno capacità limitate, ma hanno grande stabilità elettrochimica su migliaia di cicli ed efficienze coulombiche prossime al 100%.
La produzione di questo materiale avviene per etching in HF di un precursore chiamato MAX phase. Questo è il metodo più facile e veloce per ottenere il materiale in scala di laboratorio ma presenta numerose criticità quando i volumi vengono rapportati su scala industriale. Una gran parte del lavoro è stata dedicata allo studio della tecnica sintetica per ottenere MXenes per SIB riducendo o sostituendo HF nella sintesi chimica. I materiali sono stati caratterizzati con varie tecniche di caratterizzazioni strutturali, morfologiche ed elettrochimiche.
Data la struttura 2D, che ricorda quella del grafene, un uso frequente in letteratura è quello della realizzazioni di nanocompositi per SIB e LIB, al fine di produrre materiali ad alta capacità, come richiesto nel mercato delle batterie. Sono stati quindi ottenuti dei nanocompositi a base di antimonio-MXene e ossido di stagno-MXene testati rispettivamente in SIB e LIB. Antimonio e ossido di stagno sono due materiale dalla elevata capacità teorica, quando usati come anodi in batterie, ma allo stesso tempo sono estremamente fragili e tendono a polverizzarsi nei processi di carica e scarica. Il MXene è servito da buffer per limitare o evitare la frattura e distacco delle leghe dalla superficie elettrodicaThe ever-increasing production of portable devices and electric cars asks to the market to produce efficient devices that can store electrical energy. For these types of technologies, where device miniaturization is essential, lithium-ion batteries (LIBs) have become leaders as energy storage systems. The research on the lithium-ion batteries is focused to obtain more performing devices with high gravimetric and volumetric capacities of the electrode materials. In addition to the technological aspect, related to the optimization of materials, there is the supply chain of active components of the battery to consider, starting from lithium. At the moment, the problem is tackled by studying batteries with other alkaline metal ions, i.e. Na+ and K+. However, there are no standardized active materials for these devices, especially on sodium-ion batteries (SIBs), started only a few years later than that of LIBs; therefore, today these technologies are intended to support the LIBs in order to satisfy the enormous market demand of the batteries for the future vehicles. The goal of this work was to develop MXene-based anode materials to obtain efficient anodes for sodium and lithium-ion batteries. MXenes are a family of inorganic transition metal carbides, nitrides, and carbonitrides with a 2D structure that would seem promising for the intercalation of different ions due to a great flexibility and adaptability towards several intercalating ions. The ion intercalations occur by a pseudocapacitive mechanism whereby the materials have limited capacity, but they have great electrochemical stability over thousands of cycles and coulombic efficiencies near to 100%. The production of this material was done by HF etching of a precursor called MAX phase. This is the easiest and fastest method to obtain the material in laboratory scale, but it has many criticalities when the process has to be scale-up to industrial scale. A large part of this work was spent studying the synthetic technique to obtain MXenes for SIB by reducing or replacing HF in the chemical synthesis. The materials have been characterized by various techniques such as X-ray diffractometry, electron microscopy, X-ray photoelectron spectroscopy, etc., and by electrochemical tests, such as cyclic voltammetry and galvanostatic cycling. Thanks to the 2D structure, a common use of MXene in the literature is in nanocomposite syntheses for SIBs and LIBs, in order to produce high-capacity materials, as required in the battery market. Therefore, two nanocomposites based on antimony-MXene and tin oxide-MXene tested for SIB and for LIB respectively, were synthesized. Antimony and tin oxide are two materials with high theoretical capacity when used as anodes in batteries, but at the same time, they are extremely fragile and tend to pulverize during charging and discharging processes. MXene is used as a buffer to limit or prevent cracking and separation of alloys from the electrode surface.
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Seidl, Lukas [Verfasser], Ulrich [Akademischer Betreuer] Stimming, Aliaksandr [Gutachter] Bandarenka, and Ulrich [Gutachter] Stimming. "Sodium Ion Batteries - from Fundamentals to Application / Lukas Seidl ; Gutachter: Aliaksandr Bandarenka, Ulrich Stimming ; Betreuer: Ulrich Stimming." München : Universitätsbibliothek der TU München, 2018. http://d-nb.info/1175582468/34.
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Li, Sheng. "Graphene-based Composites as Anode Materials for Rechargeable Batteries." Thesis, Griffith University, 2015. http://hdl.handle.net/10072/367790.
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With increasing demand for low cost and high performance energy resources, rechargeable batteries, such as lithium ion batteries (LIBs) and sodium ion batteries (SIBs), have been intensively studied in recent years. The performance of existing anode materials for both LIBs and SIBs need substantial improvements in terms of energy capacity, rate capability, stability, safety and manufacturing cost to modernize the battery applications in electric vehicles (EV) and energy-saving smart electric grids.
Graphene is considered an effective additive in fabricating composites for anode materials since it possesses high electrical conductivity, large surface area and excellent mechanical properties. Therefore, this thesis attempts to synthesize a series of graphene-based composites as anode materials for LIBs and SIBs, to address the aforementioned concerns.
To date, numerous methods have been developed for the fabrication of graphene composites; however, most of them are sophisticated, complex, not scalable and therefore expensive. A wet-mechanochemical (wet ball-milling) method that is simple, rapid, facile, economic and most importantly, can be up-scaled for mass production is proposed to address these issues.Thesis (PhD Doctorate)
Doctor of Philosophy (PhD)
Griffith School of Environment
Science, Environment, Engineering and Technology
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Liu, Xinye. "Binary metal organic framework derived hierarchical hollow Ni3S2/Co9S8/N-doped carbon composite with superior sodium storage performance." University of Akron / OhioLINK, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=akron1489784678856585.
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Sgarbi, Stabellini Francesca. "Synthesis and surface characterization of metal (Mn, Ti) hexacyanoferrate electrodes." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2021. http://amslaurea.unibo.it/24378/.
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Due to the limited resources of lithium, new chemistries based on the abundant and cheap sodium and even zinc have been proposed for the battery market. Prussian Blue Analogues (PBAs) are a class of compounds which have been explored for many different applications because of their intriguing electrochemical and magnetic properties. Manganese and titanium hexacyanoferrate (MnHCF and TiHCF) belong to the class of PBAs. In this work, MnHCF and TiHCF electrodes were synthetized, cycled with cyclic voltammetry (CV) in different setups and subsequently, the surfaces were characterized with X-ray Photoelectron Spectroscopy (XPS). The setups chosen for CVs were coin cell with zinc aqueous solution for the MnHCF series, three-electrode cell and symmetric coin cell with sodium aqueous solution for the TiHCF series. The electrodes were treated with different number of cycles to evaluate the chemical changes and alterations in oxidation states during cycling.
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Soares, Adrien. "Batteries Lithium-ion innovantes, spécifiques pour le stockage de l'énergie photovoltaïque." Thesis, Montpellier 2, 2012. http://www.theses.fr/2012MON20206/document.
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Le travail de thèse, présenté dans ce mémoire, est consacré à l'étude de nouveaux matériaux d'électrode pour batterie lithium-ion pour le stockage d'énergie photovoltaïque. Ce type de production d'énergie impose de nombreuses intermittences de charge, des non synchronisations entre les périodes de production et de consommation, etc. L'objectif est d'évaluer le comportement de différents types de matériau d'électrode dans des batteries soumises à des profils de charge photovoltaïque pour ensuite sélectionner les plus adaptés à ce stockage spécifique d'énergie. Les matériaux choisis, Li4Ti5O12, Li2Ti3O7, NiP3, TiSnSb, présentent tous des mécanismes de réaction vis-à-vis du lithium très différents. Afin d'améliorer la durée de vie de ces matériaux d'électrodes, un travail d'optimisation des performances électrochimiques a été effectué en travaillant sur leur synthèse puis sur la formulation des électrodes. La formulation d'électrode en utilisant la carboxymethylcellulose sodique a notamment donné d'excellents résultats. La caractérisation de leurs propriétés physico-chimiques a été réalisée par diffraction des rayons X, in situ et en température, MEB, ATD, cyclage galvanostatique, etc.). Afin de reproduire des profils représentatifs de la production photovoltaïque à l'échelle des accumulateurs expérimentaux de laboratoire, un banc de simulation a été élaboré et validé avec un accumulateur de référence à base de Li4Ti5O12. Après cette étape de validation, les différents matériaux d'électrode ont été testés en condition photovoltaïque. Cette étude a permis de montrer que les intermittences de courte de durée (passages nuageux) et les régimes variables qu'impose ce type de production n'ont pas que peu d'influence sur les propriétés électrochimiques de l'ensemble de ces matériaux. Cependant, les périodes d'absence de production (nuit, journée pluvieuse, etc.) correspondant à une relaxation pour le matériau peuvent avoir un impact important. Les matériaux de conversion (NiP3, TiSnSb) ont montré de surprenants bons résultats. Enfin, les observations montrent que chaque type de matériau (mécanisme électrochimique différent) pourrait convenir i) à un type de production photovoltaïque, c'est à dire à une zone géographique et ii) à un type d'application particulièreThe thesis work, presented in this manuscript, is devoted to the study of new materials for lithium-ion battery for storing solar energy. This type of energy production imposes intermittent loading, non-synchronization between periods of production and consumption, etc. The objective is to evaluate the behavior of different types of electrode material in batteries under photovoltaic (PV) charge profiles and then to select the most suitable for this specific energy storage. The chosen materials, Li4Ti5O12, Li2Ti3O7, NiP3, TiSnSb, follow all very different reaction mechanisms versus lithium. To improve the cycling life of these electrode materials, a work on electrochemical performance optimization was performed by working on the synthesis and the electrode formulation. The electrode formulation, using in particular carboxymethyl cellulose, presented excellent results. Characterization of their physico-chemical properties was carried out by X-ray diffraction, in situ and as function of temperature, SEM, DTA, galvanostatic cycling, etc.). To reproduce representative profiles of the photovoltaic production at the experimental batteries scale, a test bench has been developed and validated with reference batteries (Li4Ti5O12). After this step of validation, different electrode materials were tested under photovoltaic conditions. This study shows that both intermittences with short duration (clouds) and variable rates of current imposed by this type of production don't strong influence on the electrochemical properties of all these materials. However, periods of no production (night, rainy day, etc.), corresponding to a relaxation for the material, can impact significantly. Materials following conversion mechanism (NiP3, TiSnSb) showed surprising good results. Finally, the observations indicated that each type of material (with different electrochemical mechanism) could be adapted to i) a type of photovoltaic production, ie to a geographical area and ii) a type of application
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Thanaweera, Achchige Dumindu P. "Design and characterisation of layered transition metal oxide cathode materials for Na-ion batteries." Thesis, Queensland University of Technology, 2022. https://eprints.qut.edu.au/228445/1/Dumindu_Thanaweera%20Achchige_Thesis.pdf.
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Owing to the scarcity of lithium, discovering alternatives for lithium in rechargeable batteries is a critical requirement. Sodium is an ideal candidate for this purpose. The absence of exceptional cathode materials in sodium-ion batteries is a bottleneck in realizing the above objective. This study focused on synthesizing novel transition metal oxide cathode materials for sodium-ion batteries and improving their electrochemical properties. The outcomes of this study emphasized the importance of novel material compositions as well as the role of smart cation substitution, anion redox reaction, electrochemical activation and the effect of the combination of strategies in achieving next-generation high-capacity cathodes.
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Fischer, Pauline Josephine [Verfasser], Fritz E. [Akademischer Betreuer] Kühn, Fritz E. [Gutachter] Kühn, and Tom [Gutachter] Nilges. "Room Temperature Ionic Liquids as Electrolytes for Sodium Ion Batteries / Pauline Josephine Fischer ; Gutachter: Fritz E. Kühn, Tom Nilges ; Betreuer: Fritz E. Kühn." München : Universitätsbibliothek der TU München, 2019. http://d-nb.info/1189815613/34.
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Zhang, Li [Verfasser], John [Akademischer Betreuer] Banhart, John [Gutachter] Banhart, and Martin [Gutachter] Winter. "Electrochemical performance and structural changes of Na0.67Mn0.67Ni0.33O2 as cathode for sodium ion batteries / Li Zhang ; Gutachter: John Banhart, Martin Winter ; Betreuer: John Banhart." Berlin : Technische Universität Berlin, 2019. http://d-nb.info/1201725054/34.
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Mattsson, Agnes-Matilda, Towa Eriksson, Caroline Löwnertz, and Marielle Holmbom. "Recycling of Prussian White." Thesis, Uppsala universitet, Institutionen för kemi - Ångström, 2021. http://urn.kb.se/resolve?urn=urn:nbn:se:uu:diva-445281.
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The aim of this project was to find a recycling route for Prussian white. During the experimental part, one recycling method was tested using sodium hydroxide and from this a method for re-synthesis of Prussian white was conducted as well as a method for re-crystallisation of sodium ferrocyanide. The method that proved most successful was the re-crystallisation of sodium ferrocyanide. Furthermore, the conditions needed to conduct a proper re-synthesis of Prussian white was not available during this research. Therefore, it was not possible to produce Prussian white of the right structure. The analysis was performed through XRD analysis and it was concluded that it is possible to re-crystallise sodium ferrocyanide from Prussian white.
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Liang, Liying [Verfasser], Yong Akademischer Betreuer] Lei, Martin [Gutachter] [Hoffmann, and Pu-Xian [Gutachter] Gao. "Rational design of antimony nanostructures toward high-performance anode materials for sodium-ion batteries / Liying Liang ; Gutachter: Martin Hoffmann, Pu-Xian Gao ; Betreuer: Yong Lei." Ilmenau : TU Ilmenau, 2017. http://d-nb.info/1178140784/34.
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Liang, Liying [Verfasser], Yong [Akademischer Betreuer] Lei, Martin [Gutachter] Hoffmann, and Pu-Xian [Gutachter] Gao. "Rational design of antimony nanostructures toward high-performance anode materials for sodium-ion batteries / Liying Liang ; Gutachter: Martin Hoffmann, Pu-Xian Gao ; Betreuer: Yong Lei." Ilmenau : TU Ilmenau, 2017. http://nbn-resolving.de/urn:nbn:de:gbv:ilm1-2017000445.
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Amaral, Ian Rodrigues do. "Propriedades estruturais e vibracionais de carbonatos fosfatos isoestruturados (sidorenkiktas)." Universidade Federal do CearÃ, 2017. http://www.teses.ufc.br/tde_busca/arquivo.php?codArquivo=18566.
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Carbonatos fosfatos isoestruturados do tipo sidorenkitas sÃo materiais com alto potencial de aplicaÃÃo em cÃtodos dos mais modernos tipos de baterias de sÃdio. Sua estrutura lamelar permite a inserÃÃo e extraÃÃo dos Ãons de sÃdio, que sÃo a principal fonte de forÃa eletromotriz da bateria. Utilizando um elemento muito mais abundante na crosta terrestre, esses dispositivos sÃo a grande promessa para substituiÃÃo da, jà bastante difundida, bateria de Ãons de lÃtio. PorÃm, o cÃtodo que contÃm as caracterÃsticas ideais para produzir o melhor desempenho, propiciando alta densidade de energia e estabilidade quÃmica, ainda està em desenvolvimento. A espectroscopia Raman continua sendo o melhor mÃtodo para caracterizar as propriedades destes compostos, pois contÃm a grande vantagem de ser altamente sensÃvel ao ambiente molecular das ligaÃÃes do oxigÃnio com os metais de transiÃÃo, o fÃsforo e o carbono. Nesta linha, realizamos um estudo de espectroscopia Raman em um conjunto de carbonatos fosfatos do tipo Na3MCO3PO4 (M = Mn, Fe, Co e Ni), obtidos por sÃntese hidrotÃrmica em microondas a 210 ÂC por 30 minutos. O sucesso na inserÃÃo de variados metais no interior de octaedros MO6, com raios iÃnicos distintos, produz uma alteraÃÃo no volume da cÃlula unitÃria do arranjo cristalino, modificando a distÃncia de equilÃbrio das ligaÃÃes atÃmicas, provocando uma alteraÃÃo substancial no nÃmero de onda dos seus modos normais de vibraÃÃo. Por isso, visto que informaÃÃes essenciais das propriedades quÃmicas e estruturais dos mais variados tipos de carbonatos fosfatos sÃo reveladas pela tÃcnica da espectroscopia Raman de forma confiÃvel, sua utilizaÃÃo se torna indispensÃvel para o desenvolvimento de mÃtodos e o planejamento de um material eficiente e comercialmente viÃvel para as inovadoras baterias de Ãons de sÃdio.
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Khan, Anastassiya. "Synthesis and characterization of defective PBAs electrode material." Master's thesis, Alma Mater Studiorum - Università di Bologna, 2020. http://amslaurea.unibo.it/21015/.
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Sodium manganese hexacyanoferrate (NaMnHCF) and its derivatives have been synthesized by simple co-precipitation method with addition of the citric and ascorbic acids respectively. The correspondent crystal structure, water content, chemical formula and a deep structural investigation of prepared samples have been performed by means of the combination of the laboratory and synchrotron techniques (PXRD, FT-IR, TGA, MP-AES and XAS). Electrochemical tests have been done using three-electrode system in sodium nitrate solution at different concentration. From cyclic voltammetry curves, Fe3+/2+ redox peak has been observed, whereas Mn3+/2+ peak was not always evident. Structural stability of the cycled samples has then been tested using 2D XRF imaging and Transmission X-ray microscopy (TXM) techniques. The intercalation of NaMnHCF after 20 cycles has been found by micro-XANES analysis of the highlighted spots which have been found in the XRF images. TXM has also confirmed the appearance of the intercalated particles after 50 cycles comparing the spectra between charged and discharged materials at three different edges (Mn, Fe and N). However, by comparison with lithium samples, it seems obvious that sodium samples are more homogeneous and intercalation is at the very beginning indicating the relative structural stability of sodium manganese hexacyanoferrate electrode material.
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Hartung, Steffen Uwe [Verfasser], Maria-Elisabeth [Akademischer Betreuer] Michel-Beyerle, Madhavi [Akademischer Betreuer] Srinivasan, and Fritz Elmar [Akademischer Betreuer] Kühn. "Vanadium-Based Materials as Electrode Materials in Sodium-Ion Batteries / Steffen Uwe Hartung. Betreuer: Maria-Elisabeth Michel-Beyerle. Gutachter: Madhavi Srinivasan ; Maria-Elisabeth Michel-Beyerle ; Fritz Elmar Kühn." München : Universitätsbibliothek der TU München, 2016. http://d-nb.info/1096458934/34.
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Gao, Suning [Verfasser], Rudolf [Gutachter] Holze, Rudolf [Akademischer Betreuer] Holze, and Qunting [Gutachter] Qu. "Layered transition metal sulfide- based negative electrode materials for lithium and sodium ion batteries and their mechanistic studies / Suning Gao ; Gutachter: Rudolf Holze, Qunting Qu ; Betreuer: Rudolf Holze." Chemnitz : Technische Universität Chemnitz, 2020. http://d-nb.info/1219910309/34.
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Bhatti, Asif Iqbal. "Calculs ab-initio et simulations atomistiques des propriétés thermodynamiques et cinétiques de complexes de métaux de transition utilisés comme batteries." Thesis, Université Grenoble Alpes (ComUE), 2018. http://www.theses.fr/2018GREAI092/document.
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Ce travail théorique vise à étudier, via les méthodes Premiers Principes, les propriétés des complexes de métaux de transitions, left[Mleft(dmbpyright)_{3}right]^{n+}nCi^{-} pour un usage en batterie. Pour cette étude ab-initio, les composés mono et bi-nucléaires ont été retenus. La pertinance de notre modélisation a été validée sur les composés mononucléaires. Nous nous sommes interessé au complexes de Fe, Ru et Cu pour lesquels une validation expérimentale était possible. Notre étude a principalement consisté à faire varier les degrés de liberté que nous possédons pour optimiser le voltage et la cinétique de chargement des batteries. Pour cela, nous avons fait varier le TM = Fe, Ru, et Cu, la nature des contre-ions Ci^{-}=PF_{6}^{-}, TFSI^{-} et ClO_{4}^{-} en interaction avec le polymère lors du processus de charge, ainsi que la longeur de la chaîne alkyl qui sépare les deux monomers dans le cas des composés binucléaires. Le composé à base de Fe avec une chaîne -left(CH_{2}right)_{n=6}- a été retenu comme le meilleur candidat pour une application batterie. Le composé à base Ru montre un comportement proche de celui du Fe, quant-au complexe de Cu, il présente des changements de géométrie locale sous chargement trop importants, le rendant peu apte à conduire à une cinétique efficace. Cette étude nous a permis de déterminer que l'approximation PBE était le meilleur choix possible pour modéliser nos complexes dans les conditions de fonctionnement en batterie (dans le champ créé par les contre-ions) et que l'approximation PBE0, généralement utilisée dans la littérature, ne pouvait rendre compte de la physico-chimie de nos composés dans de telles conditions.De surcroît, nous avons dévelopé pour le complexe de Fe, un potentiel atomistique de type “Champ de forces” de manière à pouvoir aborder les aspects dynamiques impliquant de plus grandes tailles de boîte de simulation. Ici, nous modélisons une structure 3D, totalement réticulée à partir de nos monomères à base de Fe. Nous nous sommes servi de la base de donnés DFT que nous avions généré (énergies, géométries, état de spin et fréquences vibrationnelles calculées) pour ajuster les paramètres entrant dans l'écriture du modèle. La construction de la géométrie initiale du polymère 3D a nécessité l'écriture d'un code de calcul visant à produire un arrangement complétement réticulé et à assigner les charges effectives issues des calculs DFT. Ce modèle nous a permis de déterminer les coefficients de diffusion des contre-ions pour les états totalement chargé et non-chargé. Un calcul plus ambitieux vise à déterminer les chemins de diffusion des contre-ions lors d'un processus de chargement en considérant un seul centre de degré d'oxydation 3+ au centre du polymère 3D, pour lequel les centres actifs possèdent un degré d'oxidation 2+. Les contre-ions assurent la neutralité globale.Keyword: Polymer, Electrochemistry, Li-ion Battery, DFT, Force Field development, 3D structure, Atomistic modelingAbstract Standard redox potentials for mono and bi-nuclear transition metal (TM) complexes left[Mleft(dmbpyright)_{3}right]^{n+}nCi^{-}, have been investigated using First Principles Calculation. Three metal centers are investigated: Fe, Ru, and Cu. Our modeling is validated on mono-nuclear compounds. This approach consists in determining the best small polymer (bi-nuclear) made out of these monomers for a battery application. For that, we varied the three available degrees of freedom i.e., the nature of the central TM atom (Fe, Ru, and Cu), counter-ions Ci=PF_{6}^{-}, TFSI^{-} and ClO_{4}^{-} in interaction with the polymer, and the alkyl chain -left(CH_{2}right)_{n}- of length n that connects both mono-nuclear in the bi-nuclear compound. The Iron compound with -left(CH_{2}right)_{n=6}- is found to be the best candidate. The left[Culeft(dmbpyright)_{2}right]^{n+}nCi^{-} complex shows too much structure deformation upon loading, making it less reliable for cathode material. Moreover, we studied two XC functional, PBE and PBE0 and found, for three complexes PBE approximation retains the ligand field picture whereas PBE0 functional induces an exaggerated and unexpected band dispersion by dissolving the ligand field picture expected for the octahedral environment of the TM in the studied complexes. These findings validate that hybrid functional for which it was designed to localize and cancel self-interaction error does not work for all system. More particularly, the PBE0 approximation fails to model the three complexes (Fe, Ru, and Cu) in functional conditions (in the field made by the counter-ions).Abstract Further, we have developed an atomistic potential relying on the Force Field scheme for the Iron complex in order to study the dynamical properties of this compound at larger simulation scale (3D reticulated polymerization made of our Fe complex monomers). We made an intensive use of our DFT data (energies, geometries, spin-state configurations and calculated vibrational properties) to develop the required parameters entering the model. Moreover, computational techniques (written python language) were developed specifically to create a 3D structure of transition metal complexes satisfying the condition to be fully reticulated. Bounding conditions had to be designed and a procedure aiming at fixing reliable and physical effective charges on each atom of the simulation cell (compatible with DFT results) were developed. Our first simulations have been attached to calculate the diffusion coefficients of the counter-ions in both the fully loaded and unloaded states. A more ambitious and realistic calculation aims at investigating the paths of the counter-ions when one single center starts to be loaded in an unloaded environment.Abstract Keyword: Polymer, Electrochemistry, Li-ion Battery, DFT, Force Field development, 3D structure, Atomistic modeling
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Nguyen, Long Hoang Bao. "Cristallochimie d’oxyphosphates fluorés de vanadium : De l’étude de leur structure à leurs performances en batteries Na-ion." Thesis, Bordeaux, 2019. http://www.theses.fr/2019BORD0356.
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Les batteries Na-ion se développent comme une nouvelle alternative aux batteries Li-ion. Parmi le grand nombre de matériaux déjà étudiés à l’électrode positive, Na3V2(PO4)2F3 et Na3(VO)2(PO4)2F sont les plus performants grâce à des capacités théoriques élevées, des potentiels d’extraction des ions Na+ élevés, et la stabilité de la structure lors de cyclages longues durées. De plus, la structure et les propriétés électrochimiques des matériaux Na3V2(PO4)2F3 et Na3(VO)2(PO4)2F peuvent être modulées par un effet de substitution cationique ou anionique. Ce travail de thèse a pour but d’explorer la cristallochimie de nouveaux matériaux dérivés de Na3V2(PO4)2F3 et Na3(VO)2(PO4)2F. Dans un premier temps, différentes modes de synthèse (voies tout solide, céramique assistée par sol-gel, et broyage mécanique) sont explorées pour réaliser des substitutions cationiques et anioniques. La structure tridimensionnelle à longue distance de ces matériaux est déterminée par diffraction des rayons X synchrotron, tandis que les environnements locaux sont ensuite décrits finement en combinant des techniques de spectroscopies (résonance magnétique nucléaire à l’état solide, absorption des rayons X, et infra-rouge) dont l’interprétation est appuyée par des calculs théoriques. Les diagrammes de phases et les processus d’oxydoréduction impliqués lors des réactions de dés-intercalation et de ré-intercalation des ions Na+ de la structure hôte sont étudiés pour chacune des compositions, operando (cad. lors du fonctionnement de la batterie) en diffraction et absorption des rayons X synchrotron. Une compréhension des mécanismes structuraux et redox impliqués au cours du cyclage permet d’identifier les limitations de ces phases et de nous guider pour proposer des nouveaux matériaux dérivés présentant de meilleures performancesNa-ion batteries are currently developed as a future alternative to the conventional Li-ion batteries. Among all the polyanion materials studied as positive electrodes for Na-ion batteries, Na3V2(PO4)2F3 and Na3(VO)2(PO4)2F are the two promising compositions thanks to their high theoretical capacity, high Na+-extraction voltage, and especially the high stability of their structural framework upon long-term cycling. Furthermore, the crystal structure and the electrochemical properties of these materials can be greatly modulated through an effect of cationic or anionic substitution. This PhD work aims at exploring the diversity in crystal chemistry of Na3V2(PO4)2F3, Na3(VO)2(PO4)2F and their derivatives obtained through different synthesis methods. The three-dimensional long range crystal structure of these phases is determined by the use of high resolution synchrotron X-ray powder diffraction whereas their local atomic and electronic structures are investigated through a combination of solid-state nuclear magnetic resonance supported by first-principles theoretical calculations, synchrotron X-ray absorption spectroscopy and infrared spectroscopy. Thereafter, the phase diagram and the redox processes involved in the Na+ de-intercalation and intercalation are established thanks to operando synchrotron X-ray diffraction and absorption. An in-depth understanding on the crystal structure as well as the involved redox couples for each composition helps us to determine the limitations of these vanadium fluorinated oxy-phosphates and sheds light to the development of new materials with better performance based on their structure