To see the other types of publications on this topic, follow the link: Polymer Electrolytes - Ion Dynamics.
Journal articles on the topic 'Polymer Electrolytes - Ion Dynamics'
Create a spot-on reference in APA, MLA, Chicago, Harvard, and other styles
Consult the top 50 journal articles for your research on the topic 'Polymer Electrolytes - Ion Dynamics.'
Next to every source in the list of references, there is an 'Add to bibliography' button. Press on it, and we will generate automatically the bibliographic reference to the chosen work in the citation style you need: APA, MLA, Harvard, Chicago, Vancouver, etc.
You can also download the full text of the academic publication as pdf and read online its abstract whenever available in the metadata.
Browse journal articles on a wide variety of disciplines and organise your bibliography correctly.
1
Mabuchi, Takuya, Koki Nakajima, and Takashi Tokumasu. "Molecular Dynamics Study of Ion Transport in Polymer Electrolytes of All-Solid-State Li-Ion Batteries." Micromachines 12, no. 9 (2021): 1012. http://dx.doi.org/10.3390/mi12091012.
Full textAbstract:
Atomistic analysis of the ion transport in polymer electrolytes for all-solid-state Li-ion batteries was performed using molecular dynamics simulations to investigate the relationship between Li-ion transport and polymer morphology. Polyethylene oxide (PEO) and poly(diethylene oxide-alt-oxymethylene), P(2EO-MO), were used as the electrolyte materials, and the effects of salt concentrations and polymer types on the ion transport properties were explored. The size and number of LiTFSI clusters were found to increase with increasing salt concentrations, leading to a decrease in ion diffusivity at high salt concentrations. The Li-ion transport mechanisms were further analyzed by calculating the inter/intra-hopping rate and distance at various ion concentrations in PEO and P(2EO-MO) polymers. While the balance between the rate and distance of inter-hopping was comparable for both PEO and P(2EO-MO), the intra-hopping rate and distance were found to be higher in PEO than in P(2EO-MO), leading to a higher diffusivity in PEO. The results of this study provide insights into the correlation between the nanoscopic structures of ion solvation and the dynamics of Li-ion transport in polymer electrolytes.
2
Kim, Dokyung, So Jung Seo, Ji-Hun Seo, and Young Joo Lee. "Exploring the Relationship between Ion Diffusion and Molecular Structure of Gel Polymer Electrolytes Using NMR Spectroscopy." ECS Meeting Abstracts MA2024-02, no. 7 (2024): 964. https://doi.org/10.1149/ma2024-027964mtgabs.
Full textAbstract:
Lithium rechargeable batteries are widely used as energy sources for portable electronic devices, automobile, and wearable electronics. However, concerns regarding fire hazards have prompted efforts to transition from liquid to solid electrolytes. Gel polymer electrolytes (GPEs) have emerged as promising alternatives for enhancing the safety of lithium batteries. The ion conduction mechanism in GPEs can be conceptualized in two distinct modes: a liquid-like mechanism and a solid-like mechanism. We focus on the investigation of the liquid-like mechanism, which relies on polymer segmental motion. Various factors can influence ionic conduction of gel polymer electrolytes such as the structure of the sidechain, interaction between sidechain and ionic species etc. We utilize PFG NMR and nuclear relaxation time measurements to explore the correlation between the ionic motion and the structure of polymers and ionic liquids. Chain length of polymer sidechain will be varied and structurally isomeric ionic liquids will be utilized. We will demonstrate that NMR spectroscopy is a good indicator to examine the dynamics of the gel polymer electrolyte. Understanding of the structure-dynamics relation from our study will serve as a design principle to develop new gel polymer electrolyte with desired properties.
3
Zhang, Chao. "(Invited) Understanding Ion-Ion Correlations: From Liquid Electrolytes to Polymer Electrolytes." ECS Meeting Abstracts MA2023-01, no. 45 (2023): 2455. http://dx.doi.org/10.1149/ma2023-01452455mtgabs.
Full textAbstract:
Mass transport in electrolytes is one of the most important design focuses of electrochemical devices such as batteries, fuel cells, and supercapacitors. Compared to the infinitely dilute solution, ion-ion correlations play a central role in determining the structure-property relationships in the concentrated solution. Therefore, disentangling ion-ion correlations and establishing their impact on transport coefficients is a fundamental and pressing issue in the field of electrolyte materials. In this talk, I will present the recent works of my group and collaborators on using molecular dynamics simulations to understand ion-ion correlations. In particular, we looked into this issue by exploring the synergy between liquid electrolytes and polymer electrolytes following the physical chemistry route started by Onsager. This has led to a number of interesting results on the relationship between the ion-pairing and the deviation from the Nernst-Einstein relation [1-3], and shed light on resolving the controversy of the negative transference number found in polymer electrolytes [4]. References: [1] Y. Shao, M. Hellström, A. Yllö, J. Mindemark, K. Hermansson, J. Behler, and C. Zhang, “Temperature effects on the ionic conductivity in concentrated alkaline electrolyte solutions”, Phys. Chem. Chem. Phys. 2020, 22: 10426. [2] Y. Shao, K. Shigenobu, M. Watanabe, and C. Zhang, “Role of viscosity in deviations from the Nernst–Einstein relation”, J. Phys. Chem. B, 2020, 124: 4774. [3] H. Gudla, Y. Shao, S. Phunnarungsi, D. Brandell, and C. Zhang, “Importance of the ion-pair lifetime in polymer electrolytes”, J. Phys. Chem. Lett., 2021, 12: 8460. [4] Y. Shao, H. Gudla, D. Brandell, and C. Zhang, “Transference number in polymer electrolytes: mind the reference-frame gap”, J. Am. Chem. Soc., 2022, 144: 7583.
4
Chen, Xi. "(Invited) Ion Transport and Interface Resistance in Polymer-Based Composite Electrolytes and Composite Cathode." ECS Meeting Abstracts MA2023-01, no. 6 (2023): 983. http://dx.doi.org/10.1149/ma2023-016983mtgabs.
Full textAbstract:
Solid-state electrolytes are promising to enable the next generation batteries with higher energy density and improved safety. However, each major class of solid electrolytes has intrinsic weaknesses. By combining different classes of solid electrolytes, such as a polymer electrolyte and an oxide ceramic electrolyte, one can potentially overcome the intrinsic weaknesses of each component and develop a composite electrolyte to achieve high ionic conductivity, good mechanical properties, good chemical stability, and adhesion with the electrodes. In this presentation, we show that the interfacial resistance strongly affects the ionic conductivity of polymer/oxide ceramic composite electrolytes, in both the ceramic-in-polymer design where ceramic particles are dispersed within the polymer electrolyte matrix as well as the polymer-in-ceramic design where a three dimensionally interconnected ceramic scaffold is developed. The quantification of the interfacial resistance, the origin of this resistance, as well as the strategies to minimize it are discussed. In a second case, we examine the effect of interfaces on ion transport in a polymer based composite cathode consisting of LiFePO4 (LFP), carbon and poly(ethylene oxide) (PEO) with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). The structure and dynamics of PEO and lithium ion mobility are studied by small angle neutron scattering and quasi-elastic neutron scattering. The results show that Li ion mobility in PEO/LiTFSI in the composite cathode is only 30% of the bulk electrolyte. This suggests a key bottleneck that limits the rate performance of polymer-based solid-state batteries originates from the sluggish ion transport in the polymer electrolyte confined in the cathode.
5
Chae, Somin, and Sangheon Lee. "Theoretical Study on the Dynamics of Lithium-Ion Transport in PPS-Based Polymer Electrolytes." ECS Meeting Abstracts MA2024-01, no. 2 (2024): 465. http://dx.doi.org/10.1149/ma2024-012465mtgabs.
Full textAbstract:
The development of solid-state lithium-ion batteries (LIBs) is a key advancement in energy storage technology. Solid electrolytes are important in this development because they are safer and more stable than liquid electrolytes, and they have higher energy density. Among the various types of solid electrolytes, Polyphenylene Sulfide (PPS)-based solid-state polymer electrolytes (SPEs) are notable for their ability to conduct ions as well as liquid electrolytes across a wide range of temperatures. This ability is particularly important because other solid polymer electrolytes, like those based on polyethylene oxide (PEO), struggle with ion conduction at different temperatures. PPS-based SPEs are different because their ion transport does not depend on the movement of the polymer chains, which means their ion conduction remains steady from high to low temperatures. The previous study conducted a series of first-principle calculations, revealing that the introduction of neutral molecules, referred to as agent molecules, can significantly enhance the movement of lithium ions within a solid matrix when these are mixed with lithium salts. This is because the intermolecular interactions within a binary system comprising an agent molecule and lithium salt are governed by a strong bond formation between lithium and oxygen atoms. When these agent molecules are introduced, they replace the anionic species around lithium in the salts, leading to a weakened Coulomb force between lithium and oxygen. This reduction is essential for rapid lithium-ion movement through the easy separation of lithium salts and the subsequent generation of ion-hopping sites characterized as lithium-free oxygen cages. According to the previous study, the strategic selection of neutral molecules with functional groups that bolster chemical resonance is imperative. Such molecules have been identified as promising candidates for agent molecules. Our study builds upon previous research by directly incorporating PPS polymers into our computational simulations. We utilized molecular dynamics and quantum mechanics to examine the role of neutral molecules in PPS in facilitating lithium-ion mobility. We parameterized our system with quantum mechanics calculations, which were crucial in informing our molecular dynamics simulations. Using VASP program for interaction assessment and LAMMPS program for energy and structure analysis, we refined our models to understand the interactions between PPS polymers, Li+ ions, TFSI- ions, and Chloranil molecules. Our simulations explored the structural dynamics and the effects of fillers and PPS polymer layers on ion transport. Our work enhances the basic understanding of SPEs and helps in the creation of new lithium-ion batteries that perform better and are safer. We've pinpointed important factors that control how lithium ions move in PPS-based electrolytes, laying the groundwork for future improvements in solid-state electrolytes and leading to lithium-ion batteries that are more effective and safer. Reference: [1] Jiwon Yu, Myungsuk Lee, Yeonseo Kim, Hyung-Kyu Lim, Jonghyun Chae, Gyeong S. Hwang, Sangheon Lee, “Agent molecule modulated low-temperature activation of solid-state lithium-ion transport for polymer electrolytes”, Journal of Power Sources 505, 229917 (2021).
6
Kagawa, Yuta, Masaya Miyagawa, and Hiromitsu Takaba. "Important Structural Features to Enhance Na-Ionic Conductivity in Single-Ion-Conducting Polymer Electrolytes." ECS Meeting Abstracts MA2024-02, no. 3 (2024): 349. https://doi.org/10.1149/ma2024-023349mtgabs.
Full textAbstract:
Polymeric solid electrolytes (SPEs) have excellent properties such as high safety and long life and are expected to be put to practical use as next-generation all-solid-state lithium secondary battery electrolyte. Single ion-conducting polymer electrolytes (SICPEs) are one of SPEs and have a structure in which the anion is covalently bonded to the polymer. They therefore have the advantage of high cation transference number, and a long lifetime because ionic polarization is less likely to occur. However, as the ionic conductivity is comparable to that of conventional SPE, it is necessary to clarify the structure that facilitates ion diffusion to further improve ionic conductivity. In this study, machine-learning combined with first-principles calculations and molecular dynamics (MD) were used to elucidate the important features for high Na-ionic conductivity in SICPEs. The diffusion of ions within the polymer is related to the desorption rate of ions from the strong interaction site in the polymer. Therefore, the adsorption energies (Eads) for thirteen different SICPEs monomer structures were firstly evaluated by a density functional theory (DFT) calculation. Among of the investigated SICPEs, the monomer structure of poly [lithium malonato oligo (ethylene glycolato) orthoborate] (MEGB) is explained as an example. In this polymer model, cations coordinate near anions with weak interaction to surrounding ether oxygen atoms. To consider multiple possible adsorption structure, DFT calculations were performed for several adsorption configurations and the one with the most stable energy was adopted. In addition, a bulk model of the electrolyte was prepared for SICPEs to perform MD simulations at 298 K to investigated 3D level structural features. The correlation between calculated Eads and literature values of their ionic conductivity (σ) is summarized and a reasonable correlation between Eads and σ was observed, indicating that the desorption process of ions from strong polymer interaction is dominant for diffusion dynamics. A high interaction energy between ions and polymers would suppress ion diffusion, resulting in a low ionic conductivity. Adsorption energy correlates with the distance between the anion atom and Na ion. The electronic structure of polymers such as HOMO/ LUMO was also investigated, however, there was no significant correlation has been observed. The free volumes of polymers were also estimated using the structure obtained by MD. The ratio of free volume against the total volume of the polymer was between 20 – 30 %. That free volume has no relation with the Na-ion conductivity. These results indicate that the Na-ionic conductivity is mainly governed by the interaction with the polymer chains, and the dynamics of Na-ion diffusion through the polymer chains and adsorption process to the strong interaction site are not significant in determining the Na-ionic conductivity. In the presentation, based on these results, novel polymer structures to enhance the Na-ionic conductivity will be presented with some validation data.
7
Kumar, Asheesh, Raghunandan Sharma, M. Suresh, Malay K. Das, and Kamal K. Kar. "Structural and ion transport properties of lithium triflate/poly(vinylidene fluoride-co-hexafluoropropylene)-based polymer electrolytes." Journal of Elastomers & Plastics 49, no. 6 (2016): 513–26. http://dx.doi.org/10.1177/0095244316676512.
Full textAbstract:
Polymer electrolytes consisting of poly(vinylidene fluoride-co-hexafluoropropylene) in combination with lithium triflate (LiCF3SO3) salt of varying concentration have been prepared using the conventional solution casting technique in the argon atmosphere. Structural electrical characterizations of the synthesized electrolytes have been performed using various imaging and spectroscopic techniques. The DC conductivities determined by complex impedance plots reveal gradual increase with increase in salt concentration up to a particular limit and decrease subsequently. The maximum DC conductivity obtained at 300 K is 1.64 × 10−4 Scm−1 for the electrolyte with a polymer to salt weight ratio of 1:1.8. The temperature-dependent conductivity followed a mixed Arrhenius and Vogel–Tamman–Fulcher type behaviour for the polymer electrolytes. From the Summerfield master curve plot, the conductivity of the solid polymer electrolytes is found to depend not only on ion dynamics but also on the segmental mobility of the polymer chains.
8
Choi, U. Hyeok, Ji Hyang Je, Seon Min Park, Puji Lestari Handayani, Dawoon Lee, and Jaekyun Kim. "(Invited) Tailoring Molecular Interaction in Solid-State Polymer Electrolytes for High-Performance Supercapacitors." ECS Meeting Abstracts MA2024-02, no. 6 (2024): 753. https://doi.org/10.1149/ma2024-026753mtgabs.
Full textAbstract:
In the development of the next-generation safe solid-state supercapacitors with high energy density, durability, and flexibility, the synthesis of high ion-conducting solid-state electrolytes with electrochemical and mechanical stabilities is a great challenge. Solid-state polymer electrolytes (SSPEs) are of great interest as materials in energy storage devices because ion-conducting SSPEs enable good adherence to electrodes and excellent processability for being made into a thin film. The key challenge facing the SSPE development for all-solid-state supercapacitors is to achieve high mechanical performance without sacrificing the requisite ionic conductivity. To overcome the issue, we synthesized networked polymer electrolytes in both aqueous- and non-aqueous forms, using UV or thermal cross-linking methods. The aqueous versions comprise nanohybrid polymer electrolytes (NPEs), salt-in-polyampholoytes (SIPAs), and triple-network polymer electrolytes (TNPEs). Meanwhile, the non-aqueous type features branched network structures endowed with hierarchical nano-canyon characteristics. To tune and understand the SSPE physical and electrochemical properties, the effects of electrolyte type and concentration on morphologic, dielectric, and mechanical properties were thoroughly explored by microstructural, dielectric relaxation, and mechanical measurements. We found that intermolecular interactions within the electrolyte play a vital role in the formation of a nanoscale ion channel confined in the polymer matrix, allowing for a simultaneous increase in the ionic conductivity and mechanical modulus. Tuning the SSPE morphology can also control the microscopic ion migration rate as well as the macroscopic flexibility of the SSPE. To further introduce multifunctional properties, nanocomposite SSPEs were also prepared by combining aqueous SSPEs with inorganic nanoparticles, and their physical properties were investigated using dielectric relaxation spectroscopy, oscillatory shear, and DFT calculation. The principal focus of this presentation is on the insight about our understanding of ion and polymer dynamics of the SSPEs for high-performance supercapacitors.
9
Lee, Young Joo, Dokyung KIM, Yoonju Shin, et al. "Conduction Mechanism Study of Argyrodite-Type and Polymer-Ceramic Composite Electrolyte By Solid-State and PFG NMR Spectroscopy." ECS Meeting Abstracts MA2024-02, no. 4 (2024): 416. https://doi.org/10.1149/ma2024-024416mtgabs.
Full textAbstract:
Solid-state electrolytes including inorganic ceramics, polymer, and composite polymer electrolytes have been intensively investigated as a key component for next-generation rechargeable batteries due to their low risk of fire and high energy density. Several criteria are required such as high ionic conductivity, electrochemical stability, compatibility and ductility with electrodes, and processability. Our focus relies on understanding the effect of the structural changes on the ion transport properties of various solid electrolytes by utilizing solid-state NMR and PFG NMR spectroscopy. Among various inorganic electrolytes, argyrodite-type sulfide electrolyte exhibits advantages owing to the relatively high ionic conductivity and flexibility. Thus, many attempts have been made to increase the ionic conductivity such as cation and anion doping. In particular, we investigate the effect of the anion substitution on the ion transport. By tuning the type and the size of the anion, the ionic conductivity can be enhanced. There have been controversies about the ion transport mechanism, i.e., rotation of anion influencing ion transport (paddle wheel effect), altered electronic interaction between anion and Li+, and increased defects, etc. On the one hand, polymer electrolyte has the advantages of high processability and the possibility to make good interfaces with electrodes, but, the ionic conduction is still limited by the segmental motion of the polymer. By incorporating ceramic particles into the polymer, both conductivity and mechanical strength can be improved. The conduction path can be only through a polymer network or by exchanging between the polymer network and particles. To increase the Li-ion conduction of polymer composite electrolytes, understanding the Li+ ion conduction pathway is important. In this work, we will present 1D and 2D solid-state NMR and PFG NMR spectroscopic studies to investigate the transport mechanism of anion-substituted argyrodite-type electrolyte and polymer composite electrolyte. We prepared various anion-substituted argyrodite-type electrolytes and compared spin-lattice relaxation times (T1) at various temperatures, revealing information about Li-ion conduction and anion rotation. By 2D 7Li-7Li NMR experiments, the conduction path involving both polymer matrix and solid ceramic particles and exchange between these two phases will be investigated. In contrast to the solid-state NMR which is sensitive to the localized motion, PFG NMR results show long-range transport motion of Li cations of various electrolytes. Our work will demonstrate that structural and dynamic knowledge about the materials obtained by various NMR techniques can help develop new materials for all solid-state batteries.
10
Yusof, S. Z., H. J. Woo, and A. K. Arof. "Ion dynamics in methylcellulose–LiBOB solid polymer electrolytes." Ionics 22, no. 11 (2016): 2113–21. http://dx.doi.org/10.1007/s11581-016-1733-y.
Full text
11
Peters, Brandon L., Zhou Yu, Paul C. Redfern, Larry A. Curtiss, and Lei Cheng. "Effects of Salt Aggregation in Perfluoroether Electrolytes." Journal of The Electrochemical Society 169, no. 2 (2022): 020506. http://dx.doi.org/10.1149/1945-7111/ac4c7a.
Full textAbstract:
Electrolytes comprised of polymers mixed with salts have great potential for enabling the use of Li metal anodes in batteries for increased safety. Ionic conductivity is one of the key performance metrics of these polymer electrolytes and achieving high room-temperature conductivity remains a challenge to date. For a bottom-up design of the polymer electrolytes, we must first understand how the structure of polyelectrolytes on a molecular level determines their properties. Here, we use classical molecular dynamics to study the solvation structure and ion diffusion in electrolytes composed of a short-chain perfluoroether with LiFSI or LiTFSI salts. Density functional theory is also used to provide some insights into the structures and energies of the salt interactions with the perfluoroether. We observe the formation of aggregates of salts in the fluorinated systems even at low salt concentrations. The fluorine-fluorine attraction in the solvent is the governing factor for creating the salt aggregates. The aggregates’ size and lifetime change with concentration and anion. These simulations provide an insight into the structure and dynamics of perfluoroether based electrolytes that can be used to improve Li-ion batteries.
12
Garaga, Mounesha N., Sahana Bhattacharyya, and Steve G. Greenbaum. "Achieving Enhanced Mobility of Ions in Ionic Liquid-Based Gel Polymer Electrolytes By Incorporating Inorganic Nanofibers for Li-Ion Battery." ECS Meeting Abstracts MA2022-02, no. 2 (2022): 160. http://dx.doi.org/10.1149/ma2022-022160mtgabs.
Full textAbstract:
Polymer electrolytes have received much attention in Li-ion battery research because of their unique properties, such as, high ionic conductivity, high mechanical strength including good electrode-electrolyte contact. A major research has been focused on improving the conductivity while retaining the mechanical stability of polymer electrolytes. In this context, ionic liquid-based gel polymer electrolytes are an excellent candidate. A detailed NMR investigation of PMMA-ILs gels electrolytes probing the structure and dynamics of ions was recently reported.[1] The presence of ILs in polymer matrix not only improves the conductivity but also enhances the self-healing capability. In another study, self-healing capability that reduces the dendrite formation at the interface has been discovered, for example, in PVDF-HFP-ILs electrolyte.[2] In this regard, this work reports the possible ways to enhance the ionic conductivity of such polymer electrolyte further by adding Al2O3 nanofibers. A series of PVDF-HFP-ILs with 1M LiTFSI in EMIMTFSI at different ratios of Al2O3nanofibers were prepared through solution cast technique. The dynamics of ions confined within polymer-Al2O3 matrix was explored through Impedence and PFG NMR spectroscopy. The amorphocity and the distribution of Al2O3 nanofibers are studied through XRD and SEM-EDX analyses. Lastly, the local structure of ions and their interaction with polymer and Al2O3 nanofibers were established through a detailed solid-state NMR analyses detecting 1H, 27Al, 13C, 19F, 7Li nuclei including 2D 13C{1H} HETCOR experiments. A reasonable enhancement in terms of ionic conductivity was observed with the addition of Al2O3 nanofibers, which improves the conducting pathways within the polymer network. [1] M. N. Garaga, N. Jayakody, C. C. Fraenza, B. Itin, and S. Greenbaum, Journal of Molecular Liquids 329, 115454 (2021). [2] T. Chen, W. Kong, Z. Zhang, L. Wang, Y. Hu, G. Zhu, R. Chen, L. Ma, W. Yan, Y. Wang, J. Liu, and Z. Jin, Nano Energy 54, 17 (2018).
13
Dennis, John Ojur, Abdullahi Abbas Adam, M. K. M. Ali, et al. "Substantial Proton Ion Conduction in Methylcellulose/Pectin/Ammonium Chloride Based Solid Nanocomposite Polymer Electrolytes: Effect of ZnO Nanofiller." Membranes 12, no. 7 (2022): 706. http://dx.doi.org/10.3390/membranes12070706.
Full textAbstract:
In this research, nanocomposite solid polymer electrolytes (NCSPEs) comprising methylcellulose/pectin (MC/PC) blend as host polymer, ammonium chloride (NH4Cl) as an ion source, and zinc oxide nanoparticles (ZnO NPs) as nanofillers were synthesized via a solution cast methodology. Techniques such as Fourier transform infrared (FTIR), electrical impedance spectroscopy (EIS), and linear sweep voltammetry (LSV) were employed to characterize the electrolyte. FTIR confirmed that the polymers, NH4Cl salt, and ZnO nanofiller interact with one another appreciably. EIS demonstrated the feasibility of achieving a conductivity of 3.13 × 10−4 Scm−1 for the optimum electrolyte at room temperature. Using the dielectric formalism technique, the dielectric properties, energy modulus, and relaxation time of NH4Cl in MC/PC/NH4Cl and MC/PC/NH4Cl/ZnO systems were determined. The contribution of chain dynamics and ion mobility was acknowledged by the presence of a peak in the imaginary portion of the modulus study. The LSV measurement yielded 4.55 V for the comparatively highest conductivity NCSPE.
14
Park, Habin, Anthony Engler, Nian Liu, and Paul Kohl. "Dynamic Anion Delocalization of Single-Ion Conducting Polymer Electrolyte for High-Performance of Solid-State Lithium Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (2022): 227. http://dx.doi.org/10.1149/ma2022-023227mtgabs.
Full textAbstract:
Lithium metal batteries (LMBs) have been considered as next-generation energy storages due to their extremely high theoretical specific capacity (3860 mAh g-1). However, current LMBs, using conventional liquid electrolytes, still could not fulfill the demand of soaring expansion of energy era, such as electrical vehicles, because of their safety issues, originated by uncontrollable electrolytic side reaction on the lithium, resulting unstable solid-electrolyte interphase (SEI) and vicious lithium dendritic growth [1]. Also, carbonate-based liquid electrolytes have an intrinsic flammability, and the lithium dendrite, which short-circuits a cell, can lead to severe safety hazard with the unfavorable flammability of current liquid system when they are ignited. Therefore, solid-state electrolytes have been spotlighted recently for a pathway for safe, and high energy and power LMBs, due to their superior thermal stability and low vapor pressure, while maintaining suitable electrolytic performances. In this study, solid-state single-ion conducting polymer electrolytes (SICPEs), utilizing dynamic anion delocalization (DAD), realizing high ionic conductivity and dimensional stability for high-performance LMB, are studied. The SICPEs enable superior lithium transference number, resulting in highly reduced concentration gradient of lithium cation along the electrolyte to suppress the undesirable lithium dendritic growth. However, SICPEs have prominently lower ionic conductivity than dual-ion conducting polymer electrolyte (DICPEs), which is a critical issue to make a slower charge/discharge for SICPEs [2]. Although an approach utilizing gel polymer electrolyte (GPE), using a liquid solvent as a plasticizer, has been exploited to increase the ionic conductivity of SICPEs, GPEs have struggled with lower mechanical stability, compared to solid state, and still existing flammability issue with the plasticizer. The novel plasticizer, which is described here, can interact with bulky anionic polymer matrix, so that the negative charge can be dispersed onto the whole complex by DAD. Once the bulky complex is formed by DAD, the dissociation of lithium cation from anionic matrix can be easier with the decreased activation energy and higher ionic conduction. While increasing the ionic conductivity with DAD, the nature of polymeric plasticizer will highly suppress flammability. DAD allows the membrane endure more tensile strength due to the dynamic structural change in crosslinking state, so that the polymer electrolyte can tolerate dendritic growth of lithium by morphological change on an electrode surface. The obvious advantages of DAD-induced solid polymer electrolytes in this study for a high energy and power, and ultra-safe LMB can present a novel approach of polymer electrolyte design to the astronomical demand of energy storages. [1] F. Ahmed, I. Choi, M.M. Rahman, H. Jang, T. Ryu, S. Yoon, L. Jin, Y. Jin, W. Kim, ACS Appl. Mater. Interfaces 2019, 11, 34930-34938. [2] D.-M. Shin, J.E. Bachman, M.K. Taylor, J. Kamcev, J.G. Park, M.E. Ziebel, E. Velasquez, N.N. Jarenwattananon, G.K. Sethi, Y. Cui, J.R. Long, Adv. Mater. 2020, 32, 1905771.
15
George, Sweta Mariam, Debalina Deb, Haijin Zhu, S. Sampath, and Aninda J. Bhattacharyya. "Spectroscopic investigations of solvent assisted Li-ion transport decoupled from polymer in a gel polymer electrolyte." Applied Physics Letters 121, no. 22 (2022): 223903. http://dx.doi.org/10.1063/5.0112647.
Full textAbstract:
We present here a gel polymer electrolyte, where the Li+-ion transport is completely decoupled from the polymer host solvation and dynamics. A free-standing gel polymer electrolyte with a high volume content (nearly 60%) of xM LiTFSI in G4 (tetraglyme) ( x = 1–7; Li+:G4 = 0.2–1.5) liquid electrolyte confined inside the PAN (polyacrylonitrile)-PEGMEMA [poly (ethylene glycol) methyl ether methacrylate oligomer] based polymer matrix is synthesized using a one-pot free radical polymerization process. For LiTFSI concentrations, x = 1–7 (Li+:G4 = 0.2–1.5), Raman and vibrational spectroscopies reveal that like in the liquid electrolyte, the designed gel polymer electrolytes (GPEs) also show direct coordination of Li+-ions with the tetraglyme leading to the formation of [Li(G4)]+. Coupled with the spectroscopic studies, impedance and nuclear magnetic resonance investigations also show that the ion transport is independent of the polymer segmental motion and is governed by the solvated species {[Li(G4)]+}, very similar to the scenario in ionic liquids. As a result, the magnitude of ionic conductivity and activation energies of the gel polymer electrolyte are very similar to that of the liquid electrolyte. The Li+-ion transport number for the GPE varied from 0.44 ( x = 1) to 0.5 ( x = 7) with the maximum being 0.52 at x = 5.
16
Caradant, Lea, Nina Verdier, Gabrielle Foran, et al. "The Influence of Polar Functional Groups in Hot-Melt Extruded Polymer Blend Electrolytes for Solid-State Lithium Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (2022): 210. http://dx.doi.org/10.1149/ma2022-012210mtgabs.
Full textAbstract:
Following the COP26 Summit in November 2021, more than hundred countries pledged to reach zero-emission by 2070 at the latest and the major car manufacturers committed to selling only electric vehicles by 2040. Currently, lithium-ion batteries (LIBs) are among the most widely used storage systems because of their high energy and power densities and long lifespan.1 The early LIBs are composed of intercalation electrodes, electronically isolated by an ion-conducting organic liquid electrolyte. However, the use of liquid electrolytes presents some disadvantages – especially in regard to consumer safety – related to short-circuits and potential leakages of the flammable liquid solvent. Moreover, in the case of lithium metal batteries, the combination of a liquid electrolyte and a high-capacity lithium metal anode leads to the uncontrolled deposition of lithium during the reduction, forming dendrites between the electrodes. A promising way to avoid this instability and improve battery safety is to replace the liquid electrolyte with an ion-conducting solid electrolyte.2 Among them, solid polymer electrolytes (SPEs) represent one of the most attractive alternatives due to their capacity to effectively conduct ions and higher mechanical resistance than their liquid counterparts.3 An important criterion for selecting polymers for use in SPEs is their ability to dissolve lithium salts through polar functional groups. Salt dissolution results in the replacement of ion-ion interactions in the lithium salt, with ion-dipole interactions in the polymer. The transport mechanisms of these ion-conducting materials differ from those of liquid electrolytes. Cation transport in polymer involves two steps which are considered to be dissociated or not, depending on the model chosen (Arrhenius or Vogel-Fulcher-Tammann, respectively). The application of one of these models provides interesting information on the ionic mobility dynamics in SPEs and, in particular, on the interplay between ionic jumps and polymer chain mobility. In the Arrhenius model, ionic jumps occur between coordinating sites, without taking into account the influence of segmental relaxation. Conversely, the VTF equation implies a strong relationship between these parameters. According to previous studies, higher segmental motions in the amorphous phase of polymers mainly provide ionic transport, which explains the limited ionic conductivity of SPEs at ambient temperature (less than 10-5 S/cm). Another major limitation of SPEs is primarily related to their dual role as electrolyte and binder in composite electrodes, which requires contradictory requirements to be met. Indeed, SPEs must have both sufficient flexibility to allow good interfacial contact between the electrode components and sufficient rigidity to limit short circuits. Polymer blending has emerged as an economic and effective technique to develop new SPEs which may simultaneously combine properties of each polymer and control the intrinsic properties of the resulting blend by adjusting the formulation.4 Moreover, polymer blends can be obtained by a solvent-free processing method, which reduce SPE toxicity and production time (no solvent evaporation). However, polymer blending makes both the salt dissociation processes and the ionic transport more difficult to understand as both polymers can dissolve lithium salts with their polar functional groups. Each polymer has different ionic transport properties depending on its architecture and thermal properties. Currently, no systematic survey comparing the ability of polymers with various functional groups to dissolve lithium salts in blends has thus far been conducted. In this presentation, we will discuss the salt dissociation ability of polar functional groups in various polymer blend SPEs. These groups are limited to those that are most commonly present in SPEs : ether, nitrile, carbonate, ester, alcohol and amide.5 The blends presented have been obtained by extrusion, which allows the effect of solvents on salt/polymer interactions to be neglected. In this work, coupled FTIR, EDX and 7Li NMR analyses allow the interactions between LiTFSI and the polymer blends to be determined with a good degree of certainty. Our original study combines experimental and theoretical approaches to determine effects of polymers’ lithium salt solvating ability on polymer blend electrolyte properties and represents an advancement in understanding and optimizing polymer selection for SPEs, used in lithium-ion batteries. References Xie, W., Liu, X., He, R., Li, Y., Gao, X., Li, X., Peng, Z., Feng, S., Feng, X. and Yang, S. Journal of Energy Storage 2020, 32, 101837. Chen, R., Qu, W., Guo, X., Li, L. and Wu, F. Materials Horizons 2016, 3, 487-516. Gray, F. M. Solid polymer electrolytes, VCH New Tork 1991. Caradant, L., Lepage, D., Nicolle, P., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2020, 4943-4951. Caradant, L., Verdier, N., Foran, G., Lepage, D., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2021. Figure 1
17
AL-Hamdani, Nasser, Paula V. Saravia, Javier Luque Di Salvo, Sergio A. Paz, and Giorgio De Luca. "Unravelling Lithium Interactions in Non-Flammable Gel Polymer Electrolytes: A Density Functional Theory and Molecular Dynamics Study." Batteries 11, no. 1 (2025): 27. https://doi.org/10.3390/batteries11010027.
Full textAbstract:
Lithium metal batteries (LiMBs) have emerged as extremely viable options for next-generation energy storage owing to their elevated energy density and improved theoretical specific capacity relative to traditional lithium batteries. However, safety concerns, such as the flammability of organic liquid electrolytes, have limited their extensive application. In the present study, we utilize molecular dynamics and Density Functional Theory based simulations to investigate the Li interactions in gel polymer electrolytes (GPEs), composed of a 3D cross-linked polymer matrix combined with two different non-flammable electrolytes: 1 M lithium hexafluorophosphate (LiPF6) in ethylene carbonate (EC)/dimethyl carbonate (DMC) and 1 M lithium bis(fluorosulfonyl)imide (LiFSI) in trimethyl phosphate (TMP) solvents. The findings derived from radial distribution functions, coordination numbers, and interaction energy calculations indicate that Li⁺ exhibits an affinity with solvent molecules and counter-anions over the functional groups on the polymer matrix, highlighting the preeminent influence of electrolyte components in Li⁺ solvation and transport. Furthermore, the second electrolyte demonstrated enhanced binding energies, implying greater ionic stability and conductivity relative to the first system. These findings offer insights into the Li+ transport mechanism at the molecular scale in the GPE by suggesting that lithium-ion transport does not occur by hopping between polymer functional groups but by diffusion into the solvent/counter anion system. The information provided in the work allows for the improvement of the design of electrolytes in LiMBs to augment both safety and efficiency.
18
Butnicu, Dan, Daniela Ionescu, and Maria Kovaci. "Structure Optimization of Some Single-Ion Conducting Polymer Electrolytes with Increased Conductivity Used in “Beyond Lithium-Ion” Batteries." Polymers 16, no. 3 (2024): 368. http://dx.doi.org/10.3390/polym16030368.
Full textAbstract:
Simulation techniques implemented with the HFSS program were used for structure optimization from the point of view of increasing the conductivity of the batteries’ electrolytes. Our analysis was focused on reliable “beyond lithium-ion” batteries, using single-ion conducting polymer electrolytes, in a gel variant. Their conductivity can be increased by tuning and correlating the internal parameters of the structure. Materials in the battery system were modeled at the nanoscale with HFSS: electrodes–electrolyte–moving ions. Some new materials reported in the literature were studied, like poly(ethylene glycol) dimethacrylate-x-styrene sulfonate (PEGDMA-SS) or PU-TFMSI for the electrolyte; p-dopable polytriphenyl amine for cathodes in Na-ion batteries or sulfur cathodes in Mg-ion or Al-ion batteries. The coarse-grained molecular dynamics model combined with the atomistic model were both considered for structural simulation at the molecular level. Issues like interaction forces at the nanoscopic scale, charge carrier mobility, conductivity in the cell, and energy density of the electrodes were implied in the analysis. The results were compared to the reported experimental data, to confirm the method and for error analysis. For the real structures of gel polymer electrolytes, this method can indicate that their conductivity increases up to 15%, and even up to 26% in the resonant cases, via parameter correlation. The tuning and control of material properties becomes a problem of structure optimization, solved with non-invasive simulation methods, in agreement with the experiment.
19
Nti, Frederick, George W. Greene, Haijin Zhu, Patrick C. Howlett, Maria Forsyth, and Xiaoen Wang. "Anion effects on the properties of OIPC/PVDF composites." Materials Advances 2, no. 5 (2021): 1683–94. http://dx.doi.org/10.1039/d0ma00992j.
Full text
20
Caradant, Lea, Nina Verdier, Gabrielle Foran, et al. "The Influence of Polar Functional Groups in Melt-Blended Polymers Used As New Solid Electrolytes for Lithium Batteries." ECS Meeting Abstracts MA2022-02, no. 7 (2022): 2423. http://dx.doi.org/10.1149/ma2022-0272423mtgabs.
Full textAbstract:
Following the COP26 Summit in November 2021, more than hundred countries pledged to reach zero-emission by 2070 at the latest and the major car manufacturers committed to selling only electric vehicles by 2040. Currently, lithium-ion batteries (LIBs) are among the most widely used storage systems because of their high energy and power densities and long lifespan.1 The early LIBs are composed of intercalation electrodes, electronically isolated by an ion-conducting organic liquid electrolyte. However, the use of liquid electrolytes presents some disadvantages – especially in regard to consumer safety – related to short-circuits and potential leakages of the flammable liquid solvent. Moreover, in the case of lithium metal batteries, the combination of a liquid electrolyte and a high-capacity lithium metal anode leads to the uncontrolled deposition of lithium during the reduction, forming dendrites between the electrodes. A promising way to avoid this instability and improve battery safety is to replace the liquid electrolyte with an ion-conducting solid electrolyte.2 Among them, solid polymer electrolytes (SPEs) represent one of the most attractive alternatives due to their capacity to effectively conduct ions and higher mechanical resistance than their liquid counterparts.3 An important criterion for selecting polymers for use in SPEs is their ability to dissolve lithium salts through polar functional groups. Salt dissolution results in the replacement of ion-ion interactions in the lithium salt, with ion-dipole interactions in the polymer. The transport mechanisms of these ion-conducting materials differ from those of liquid electrolytes. Cation transport in polymer involves two steps which are considered to be dissociated or not, depending on the model chosen (Arrhenius or Vogel-Tamman-Fulcher, respectively). The application of one of these models provides interesting information on the ionic mobility dynamics in SPEs and, in particular, on the interplay between ionic jumps and polymer chain mobility. According to previous studies, higher segmental motions in the amorphous phase of polymers mainly provide ionic transport, which explains the limited ionic conductivity of SPEs at ambient temperature (less than 10-5 S/cm). Another major limitation of SPEs is primarily related to their dual role as electrolyte and binder in composite electrodes, which requires contradictory requirements to be met. Indeed, SPEs must have both sufficient flexibility to allow good interfacial contact between the electrode components and sufficient rigidity to limit short circuits. Polymer blending has emerged as an economic and effective technique to develop new SPEs which may simultaneously combine properties of each polymer and control the intrinsic properties of the resulting blend by adjusting the formulation.4 Moreover, polymer blends can be obtained by a solvent-free processing method, which reduce SPE toxicity and production time and cost. However, polymer blending makes both the salt dissociation processes and the ionic transport more difficult to understand as both polymers can dissolve lithium salts with their polar groups. Each polymer has different ionic transport properties depending on its architecture and thermal properties. Currently, no systematic survey comparing the ability of polymers with various functional groups to dissolve lithium salts in blends has thus far been conducted. In this presentation, we will discuss the salt dissociation ability of polar functional groups in various polymer blend SPEs. These groups are limited to those that are most commonly present in SPEs : ether, nitrile, carbonate, ester, alcohol and amide.5 The blends presented have been obtained by extrusion, which allows the effect of solvents on salt/polymer interactions to be neglected. Coupled FTIR, EDX and 7Li NMR analyses allow the interactions between LiTFSI and the polymer blends to be determined with a good degree of certainty. Our original study combines experimental and theoretical approaches to determine effects of polymers’ lithium salt solvating ability on blend electrolyte properties. Finally, this survey highlights an ideal polymer couple with the most promising and complementary properties, usable as SPE for LIBs. Indeed, this blend presents encouraging properties, compared to single-polymer SPEs, such as higher ionic conductivities over a wide temperature range, as well as improved mechanical and thermal stability properties and cycling performances. References Xie, W., Liu, X., He, R., Li, Y., Gao, X., Li, X., Peng, Z., Feng, S., Feng, X. and Yang, S. Journal of Energy Storage 2020, 32, 101837. Chen, R., Qu, W., Guo, X., Li, L. and Wu, F. Materials Horizons 2016, 3, 487-516. Gray, F. M. Solid polymer electrolytes, VCH New Tork 1991. Caradant, L., Lepage, D., Nicolle, P., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2020, 4943-4951. Caradant, L., Verdier, N., Foran, G., Lepage, D., Prébé, A., Aymé-Perrot, D. and Dollé, M. ACS Applied Polymer Materials 2021. Figure 1
21
Weber, Ryan L., and Mahesh K. Mahanthappa. "Thiol–ene synthesis and characterization of lithium bis(malonato)borate single-ion conducting gel polymer electrolytes." Soft Matter 13, no. 41 (2017): 7633–43. http://dx.doi.org/10.1039/c7sm01738c.
Full text
22
Asha, Aysha Siddika, Benjoe Rey B. Visayas, Maricris L. Mayes, and Caiwei Shen. "Understanding the Effect of Trace Solvent Content on Properties of Polymer Electrolytes through Molecular Dynamics Simulations." ECS Meeting Abstracts MA2023-01, no. 4 (2023): 862. http://dx.doi.org/10.1149/ma2023-014862mtgabs.
Full textAbstract:
The rapid growth of mobile, portable, wearable and flexible electronics leads to the increasing demand for energy storage devices using solid-state polymer electrolytes (PEs), which outperform liquid electrolytes in terms of safety, mechanical properties, and simplicity of device fabrication and packaging. However, processing PEs will always introduce solvent molecules that greatly affect the ionic conductivity and mechanical properties. For example, PEs prepared through solution-casting methods always have solvent residues. A trace amount of water molecules absorbed from the air is also inevitable. Recently, we demonstrated the controlled introduction of solvent molecules to PEs to balance the ionic conductivity and mechanical stiffness for structural energy storage applications. To better understand how solvent molecules behave and interact with other components in PEs, here we present the molecular dynamics simulation of a representative polymer electrolyte system with various water content. We use simulation results to determine the effect of trace water content before forming a liquid phase on ionic conductivity and mechanical properties. The insights into the molecular interactions in the PE system will help us design and optimize Pes’ composition and processing for practical applications. The simulation model of polymer electrolyte is built with polyethylene oxide (PEO) and lithium perchlorate (LiClO4) with various water contents, in which the water molecule to lithium-ion ratio ranges from 0 to 3. The electrolyte with each water content is simulated between two graphene electrodes to determine its ionic conductivity. Uniaxial deformation has been performed on the electrolyte to obtain the mechanical properties. All simulations were performed using the molecular dynamics simulation code LAMMPS with the CHARMM force field. The results show that the ionic conductivity of the polymer electrolyte system increases significantly (up to one order of magnitude) with the increase of water content (up to 3 water molecules per lithium ion), even when the added water does not form a continuous liquid phase. The change of ionic conductivity with water content is correlated to the degree of association between different types of ions or molecules in the system, as evidenced by the evaluation of the radial distribution functions. As the association between polymer molecules and lithium ions reduces with increasing water, it becomes easier for the lithium ions to diffuse and resulting in higher ionic conductivity. It is also observed that the perchlorate ions’ interactions with polymer molecules remain the same with different water contents, which shows different roles of lithium ions and perchlorate ions in ion conduction in this system. On the other hand, the modulus of elasticity of the polymer electrolyte does not change much with the increase of water, which agrees with the previous experimental work of our group. This means that the trace amount of water is strongly associated with other solid molecules or ions and is not affecting the stiffness of the system as long as no liquid phase is formed. The results will lead to novel strategies to design polymer electrolytes with both high ionic conductivity and good mechanical properties for flexible or multifunctional energy storage applications.
23
Rushing, Jeramie C., Anit Gurung, and Daniel G. Kuroda. "Relation between microscopic structure and macroscopic properties in polyacrylonitrile-based lithium-ion polymer gel electrolytes." Journal of Chemical Physics 158, no. 14 (2023): 144705. http://dx.doi.org/10.1063/5.0135631.
Full textAbstract:
Polymer gel electrolytes (PGE) have seen a renewed interest in their development because they have high ionic conductivities but low electrochemical degradation and flammability. PGEs are formed by mixing a liquid lithium-ion electrolyte with a polymer at a sufficiently large concentration to form a gel. PGEs have been extensively studied, but the direct connection between their microscopic structure and macroscopic properties remains controversial. For example, it is still unknown whether the polymer in the PGE acts as an inert, stabilizing scaffold for the electrolyte or it interacts with the ionic components. Here, a PGE composed of a prototypical lithium-carbonate electrolyte and polyacrylonitrile (PAN) is pursued at both microscopic and macroscopic levels. Specifically, this study focused on describing the microscopic and macroscopic changes in the PGE at different polymer concentrations. The results indicated that the polymer-ion and polymer–polymer interactions are strongly dependent on the concentration of the polymer and the lithium salt. In particular, the polymer interacts with itself at very high PAN concentrations (10% weight) resulting in a viscous gel. However, the conductivity and dynamics of the electrolyte liquid components are significantly less affected by the addition of the polymer. The observations are explained in terms of the PGE structure, which transitions from a polymer solution to a gel, containing a polymer matrix and disperse electrolyte, at low and high PAN concentrations, respectively. The results highlight the critical role that the polymer concentration plays in determining both the macroscopic properties of the system and the molecular structure of the PGE.
24
Eriksson, Therese, Harish Gudla, Yumehiro Manabe, et al. "Carbonyl-Containing Solid Polymer Electrolyte Host Materials: Conduction and Coordination in Polyketone, Polyester, and Polycarbonate Systems." Macromolecules 55, no. 24 (2022): 10940–49. https://doi.org/10.1021/acs.macromol.2c01683.
Full textAbstract:
Research on solid polymer electrolytes (SPEs) is now moving beyond the realm of polyethers that have dominated the field for several decades. A promising alternative group of candidates for SPE host materials is carbonyl-containing polymers. In this work, SPE properties of three different types of carbonyl-coordinating polymers are compared: polycarbonates, polyesters, and polyketones. The investigated polymers were chosen to be as structurally similar as possible, with only the functional group being different, thereby giving direct insights into the role of the noncoordinating main-chain oxygens. As revealed by experimental measurements as well as molecular dynamics simulations, the polyketone possesses the lowest glass transition temperature, but the ion transport is limited by a high degree of crystallinity. The polycarbonate, on the other hand, displays a relatively low coordination strength but is instead limited by its low molecular flexibility. The polyester performs generally as an intermediate between the other two, which is reasonable when considering its structural relation to the alternatives. This work demonstrates that local changes in the coordinating environment of carbonyl-containing polymers can have a large effect on the overall ion conduction, thereby also showing that desired transport properties can be achieved by fine-tuning the polymer chemistry of carbonyl-containing systems.
25
Bhandary, Rajesh, and Monika Schönhoff. "Polymer effect on lithium ion dynamics in gel polymer electrolytes: Cationic versus acrylate polymer." Electrochimica Acta 174 (August 2015): 753–61. http://dx.doi.org/10.1016/j.electacta.2015.05.145.
Full text
26
Kim, Young C., Brian L. Chaloux, Debra R. Rolison, Michelle D. Johannes, and Megan B. Sassin. "Molecular dynamics study of hydroxide ion diffusion in polymer electrolytes." Electrochemistry Communications 140 (July 2022): 107334. http://dx.doi.org/10.1016/j.elecom.2022.107334.
Full text
27
Ramya, C. S., and S. Selvasekarapandian. "Spectroscopic studies on ion dynamics of PVP–NH4SCN polymer electrolytes." Ionics 20, no. 12 (2014): 1681–86. http://dx.doi.org/10.1007/s11581-014-1130-3.
Full text
28
Ford, Hunter O., Ramsay Nuwayhid, Brian Chaloux, et al. "Accelerating Development of Submicron-Thick Initiated Chemical Vapor Deposition (iCVD)-Derived Polymer Electrolytes for All Solid-State Batteries Via Pre-Screening Bulk Surrogates." ECS Meeting Abstracts MA2024-02, no. 48 (2024): 3483. https://doi.org/10.1149/ma2024-02483483mtgabs.
Full textAbstract:
Initiated chemical vapor deposition (iCVD) is an emerging method for generating submicron-thick, conformal polymer coatings on structurally complex substrates, including those of interest to all solid-state 3D batteries, fuel cells, and capacitive deionization devices. From the perspective of the energy-storage community, the utility of iCVD arises from the ability to create conformal polymer anion- or cation-conducting solid-state electrolytes, artificial solid-electrolyte interphase (SEI) layers, and surface property-modifying coatings. Expanding the library of polymer chemistries and structures beyond those obtained using standard vinyl-containing iCVD monomers is essential to address the challenges facing next-generation, advanced energy storage (e.g., cycle life, suppression of unwanted ion transport). However, opening up this synthetic property-performance space for iCVD-generated materials challenges the throughput of iCVD and greatly increases the number of characterization experiments. To circumvent this challenge, we previously reported that bulk poly(dimethylaminomethylstyrene), pDMAMS, synthesized using bulk solution polymerization serves as a surrogate for iCVD-derived pDMAMS.1,2 We now extend the viability of bulk polymer surrogates to other polymer chemistries as a pre-screening option to accelerate the design and evaluation of iCVD-derived solid-state polymer electrolytes. For a selected test case involving single-anion conducting alkaline polymer electrolytes, we demonstrate how trends observed in polymer design regarding ion/mass transport and morphology on traditional bulk-synthesized polymers translate to iCVD-prepared analogs of the same systems. For example, we show that for a co-polymer system comprising divinylbenzene (DVB) and quaternized dimethylaminomethylstyrene (p[DVB-DMAMS+], increasing the crosslinking DVB content decreases ionic conductivity and restricts dynamic freedom. Using this understanding, we formulate an appropriate pre-optimized iCVD-derived p[DVB-DMAMS+] electrolyte and verify that its performance trend aligns with that of the bulk copolymer. 1. Ford, Hunter O., et al. Non-line-of-sight synthesis and characterization of a conformal submicron-thick cationic polymer deposited on 2D and 3D substrates. RSC Applied Interfaces (2024); doi: 1039/d3lf00256j. 2. Ford, Hunter O., et al. Submicron-thick single anion-conducting polymer electrolytes. RSC Applied Interfaces (2024); doi: 10.1039/d3lf00257h.
29
Chen, X. Chelsea, Robert L. Sacci, Naresh C. Osti, et al. "Correction: Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering." Molecular Systems Design & Engineering 4, no. 4 (2019): 983. http://dx.doi.org/10.1039/c9me90023c.
Full textAbstract:
Correction for ‘Study of segmental dynamics and ion transport in polymer–ceramic composite electrolytes by quasi-elastic neutron scattering’ by X. Chelsea Chen et al., Mol. Syst. Des. Eng., 2019, 4, 379–385.
30
Chavan, Kanchan, Pallab Barai, Hong-Keun Kim, and Venkat Srinivasan. "Decoding the Ceramics Influence in the Composite Electrolytes." ECS Meeting Abstracts MA2022-02, no. 4 (2022): 494. http://dx.doi.org/10.1149/ma2022-024494mtgabs.
Full textAbstract:
As Lithium-Ion Batteries (LIBs) becomes an essential part of the everyday life, fireproof electrolytes have become an important component of the next generation battery design without compromising the performance of the battery. Composite electrolytes (CEs), consist of polymer electrolytes with highly conducting ceramic particles are promising candidates to substitute currently commercialized LIBs with liquid electrolytes. So far, experiments with CEs have discovered positive and negative effect on the overall conductivity of the CEs in the presence of ceramic particles.1–4 Therefore, exists the conflict weather the CEs are the solution to overcome the disadvantages of all-liquid and all-solid electrolytes. In this work, a 2-Dimensional CE with a uniform ceramic particle size distribution is studied via continuum modeling. we analyze the effect of interface between polymer and ceramic particle on the overall conductivity and transference number of the CEs to guide experimentalist to fabricate these interfaces carefully. It is concluded that the interplay between ohmic resistance and polymer conductivity at the polymer and ceramic particle interfaces can explain the conflicts observed in the literature. The Ohmic resistance at the interface is a critical parameter that determines whether ceramic particles enhance the overall conductivity or not. Finally, CEs does meet the criteria of the conductivity and transference number requirement in order to use in the EVs.5 References: (1) Cheng, S. H.-S.; He, K.-Q.; Liu, Y.; Zha, J.-W.; Kamruzzaman, M.; Ma, R. L.-W.; Dang, Z.-M.; Li, R. K. Y.; Chung, C. Y. Electrochemical Performance of All-Solid-State Lithium Batteries Using Inorganic Lithium Garnets Particulate Reinforced PEO/LiClO4 Electrolyte. Electrochimica Acta 2017, 253, 430–438. (2) Zagórski, J.; López del Amo, J. M.; Cordill, M. J.; Aguesse, F.; Buannic, L.; Llordés, A. Garnet–Polymer Composite Electrolytes: New Insights on Local Li-Ion Dynamics and Electrodeposition Stability with Li Metal Anodes. ACS Appl. Energy Mater. 2019, 2 (3), 1734–1746. (3) Bonilla, M. R.; García Daza, F. A.; Ranque, P.; Aguesse, F.; Carrasco, J.; Akhmatskaya, E. Unveiling Interfacial Li-Ion Dynamics in Li 7 La 3 Zr 2 O 12 /PEO(LiTFSI) Composite Polymer-Ceramic Solid Electrolytes for All-Solid-State Lithium Batteries. ACS Appl. Mater. Interfaces 2021, 13 (26), 30653–30667. (4) Choi, J.-H.; Lee, C.-H.; Yu, J.-H.; Doh, C.-H.; Lee, S.-M. Enhancement of Ionic Conductivity of Composite Membranes for All-Solid-State Lithium Rechargeable Batteries Incorporating Tetragonal Li7La3Zr2O12 into a Polyethylene Oxide Matrix. J. Power Sources 2015, 274, 458–463. (5) Kim, H.-K.; Srinivasan, V. Status and Targets for Polymer-Based Solid-State Batteries for Electric Vehicle Applications. J. Electrochem. Soc. 2020, 167 (13), 130520.
31
Li, Guan Min. "Mathematical Model of Transmission Mechanism from Multiphase Composite System." Advanced Materials Research 850-851 (December 2013): 300–303. http://dx.doi.org/10.4028/www.scientific.net/amr.850-851.300.
Full textAbstract:
As part of the weak electrolyte, Multiphase Composite System’s structure is more complex. So the conductive electrolyte ion transport has some difficulty to understanding the mechanism. And the present study has not yet reached a consensus, but through the ion conduction mechanism in-depth research on polymer electrolytes Preparation of important guiding significance. Current theories include ionic conductivity effective medium theory (EMT), MN law, WFL equation, NE equation, dynamic bonding penetration model.
32
Brinkkötter, M., M. Gouverneur, P. J. Sebastião, F. Vaca Chávez, and M. Schönhoff. "Spin relaxation studies of Li+ ion dynamics in polymer gel electrolytes." Physical Chemistry Chemical Physics 19, no. 10 (2017): 7390–98. http://dx.doi.org/10.1039/c6cp08756f.
Full text
33
Gao, Yuqing, Yankui Mo, Shengguang Qi, Mianrui Li, Tongmei Ma, and Li Du. "Enhancing Ion Transport in Polymer Electrolytes by Regulating Solvation Structure via Hydrogen Bond Networks." Molecules 30, no. 11 (2025): 2474. https://doi.org/10.3390/molecules30112474.
Full textAbstract:
Polymer electrolytes (PEs) provide enhanced safety for high–energy–density lithium metal batteries (LMBs), yet their practical application is hampered by intrinsically low ionic conductivity and insufficient electrochemical stability, primarily stemming from suboptimal Li+ solvation environments and transport pathways coupled with slow polymer dynamics. Herein, we demonstrate a molecular design strategy to overcome these limitations by regulating the Li+ solvation structure through the synergistic interplay of conventional Lewis acid–base coordination and engineered hydrogen bond (H–bond) networks, achieved by incorporating specific H–bond donor functionalities (N,N′–methylenebis(acrylamide), MBA) into the polymer architecture. Computational modeling confirms that the introduced H–bonds effectively modulate the Li+ coordination environment, promote salt dissociation, and create favorable pathways for faster ion transport decoupled from polymer chain motion. Experimentally, the resultant polymer electrolyte (MFE, based on MBA) enables exceptionally stable Li metal cycling in symmetric cells (>4000 h at 0.1 mA cm−2), endows LFP|MFE|Li cells with long–term stability, achieving 81.0% capacity retention after 1400 cycles, and confers NCM622|MFE|Li cells with cycling endurance, maintaining 81.0% capacity retention after 800 cycles under a high voltage of 4.3 V at room temperature. This study underscores a potent molecular engineering strategy, leveraging synergistic hydrogen bonding and Lewis acid–base interactions to rationally tailor the Li+ solvation structure and unlock efficient ion transport in polymer electrolytes, paving a promising path towards high–performance solid–state lithium metal batteries.
34
Oh, Kyeong-Seok, Ji Eun Lee, Yong-Hyeok Lee, et al. "Elucidating Ion Transport Phenomena in Sulfide/Polymer Composite Electrolytes for Practical Solid-State Batteries." ECS Meeting Abstracts MA2024-02, no. 8 (2024): 1095. https://doi.org/10.1149/ma2024-0281095mtgabs.
Full textAbstract:
Solid-state batteries (SSBs) are emerging as a safer, higher-energy alternative to traditional lithium-ion batteries, driven by the demand for advanced energy storage solutions. Despite the potential of inorganic/polymer composite solid-state electrolytes (CSEs) to enhance SSB performance, the mechanisms of ion transport in these systems remain poorly understood. This study aims to elucidate these mechanisms by exploring the formation of bi-percolating ion channels and ion conduction at the interfaces between inorganic and polymer electrolytes in CSEs. We selected a model CSE composed of argyrodite-type Li6PS5Cl (LPSCl) and a gel polymer electrolyte (GPE) containing a Li+-glyme complex for ion conduction and a crosslinked ethoxylated trimethylolpropane triacrylate (ETPTA) polymer for structural support. Our findings reveal that the percolation threshold of the LPSCl phase within the CSE is significantly influenced by the elasticity of the GPE phase. Moreover, by modulating the solvation/desolvation dynamics of the Li+-glyme complex within the GPE, we achieved enhanced ion conduction across the LPSCl-GPE interface. The optimized CSE, incorporating a balance of material chemistry and composition, was integrated with an aramid nonwoven porous substrate to achieve scalability and flexibility in manufacturing. The resultant CSE, with dimensions of 8 × 6 (cm × cm) and a thickness of approximately 40 μm, was paired with a high-mass-loading LiNi0.7Co0.15Mn0.15O2 cathode and a graphite anode to construct an SSB full cell. This assembly, characterized by a bi-cell configuration and a negative (N)/positive (P) capacity ratio of 1.1, exhibited a remarkable volumetric energy density of 480 Wh Lcell -1 and stable cyclability at 25 °C. This study not only advances our understanding of ion transport phenomena in CSEs but also presents a pragmatic approach to the design and fabrication of SSBs with superior performance metrics. By integrating insights into ion channel formation and interfacial conduction with innovative materials engineering, we present a scalable and effective strategy for the development of high-performance SSBs. This research underscores the critical role of CSE design in overcoming the limitations associated with both inorganic and polymer electrolytes, paving the way for the next generation of energy storage technologies. Figure 1
35
Zhan, Yu-Ting, Santhanamoorthi Nachimuthu, and Jyh-Chiang Jiang. "Ab Initio Molecular Dynamics Study on Self-Healing Solid Polymer Electrolyte for Lithium Metal Batteries." ECS Meeting Abstracts MA2023-02, no. 65 (2023): 3110. http://dx.doi.org/10.1149/ma2023-02653110mtgabs.
Full textAbstract:
Lithium metal batteries (LMBs) have generally become potential candidates for energy storage devices because of their high energy density. However, the practical applications of LMBs have been limited due to the low safety of liquid electrolytes. Compared to liquid electrolytes, solid-state polymer electrolytes (SPEs) have excellent mechanical strength. However, there is room for improvement because traditional PEO-based SPEs need more mechanical properties and electrode contacts for flexible energy device applications. Self-healing solid polymer electrolytes (SHSPEs) have excellent flexibility and healing ability and can also suppress dendrite formation to increase the safety of LMBs. In this study, a novel SHSPE is designed by a combination of the zwitterionic copolymer, SBMA ([2-(methacryloyloxy) ethyl] dimethyl-(3-sulfopropyl) ammonium hydroxide)-co-BA (Butyl Acrylate), and a lithium salt, LiTFSI. We explored their solvation structures and reactivity on the Li metal anode using Density functional theory (DFT) and ab initio molecular dynamics (AIMD) methods. Besides, we also studied the reactivity of the considered SHSPE on the Cu (100) surface to explore the SEI formation mechanisms. The cationic NR4 + and anionic SO3 - groups of SBMA interact electrostatically and form cross-linked network structures within the electrolyte framework, providing the designed SHSPE with prominent self-healing capacity. The decomposition reactions of SHSPE on the Li metal anode are explored, and the resultant decomposition products that contribute to the formation of the solid electrolyte interphase (SEI) are identified. Furthermore, AIMD results indicate that highly concentrated SO3 - groups in the SHSPE promote Li ion diffusion, which increases Li ionic conductivity. The present findings provide design criteria for developing highly conductive self-healing SPEs.
36
Lee, Youngju, and Peng Bai. "Overlimiting Currents and Sand’s Time Behaviors in Solid Polymer Electrolytes." ECS Meeting Abstracts MA2022-02, no. 4 (2022): 485. http://dx.doi.org/10.1149/ma2022-024485mtgabs.
Full textAbstract:
Dendrite growth in solid polymer electrolytes has been frequently analyzed since it was the critical issue that limited its applications. For the liquid electrolyte systems, the dilute solution theory and the classic Nernst-Planck equation have been proven to be useful tools for analysis of ion transport dynamics and especially the dendrite initiation at Sand’s time. However, characterization of the Sand’s time in solid polymer electrolyte systems is challenging and also seldomly performed. From the experimental perspective, operando observations have been done, but the true local current density was different from the geometrical average current density since there was always heterogeneous current distribution for millimeter-scale electrolytes. From the theoretical perspective, the dendrite initiation time followed the trend predicted by Sand’s equation, but discrepancies were found such as dendrites observed at under-limiting currents or the order-of-magnitude extended Sand’s time compared to theoretical predictions. Here, we use transparent microcapillary cells for solid polymer electrolyte systems to overcome these challenges. These specialized cells allow direct operando optical observations, while the micron-scale cross-sectional area minimizes the discrepancy between true local and averaged geometrical current densities. Comparison between operando image and voltage response during constant current polarization shows that, unlike liquid electrolyte cases, the dendrite initiation for solid polymer electrolytes doesn’t always trigger a voltage spike. We also derived transport parameters from the measured Sand’s time, limiting current density, and conductivity and the cross-validated transport parameters were used to calculate theoretical Sand’s time that can be compared with the experimental values. Using the analytical solution from the Nernst-Planck equation and numerical calculations using Newman’s concentrated solution model and COMSOL Multiphysics, the predicted Sand’s time for the dilute and concentrated solution theory both matched closely with our experimental values. This work demonstrates that while the polarization process and the onset of lithium dendritic growths in solid polymer electrolytes can be still accurately predicted by the dilute solution theory, it may not always result in voltage responses similar to that of the liquid electrolyte cases. It’s also suggested that ensuring the homogenous distribution of lithium flux and avoiding the localized overlimiting current density is the key to realizing the dendrite-free polymer electrolytes.
37
Wang, Hui, Naresh C. Osti, Jürgen Allgaier, et al. "Dynamics of polymer electrolyte with LiTFSI via Quasi-Elastic Neutron Scattering." EPJ Web of Conferences 286 (2023): 04005. http://dx.doi.org/10.1051/epjconf/202328604005.
Full textAbstract:
Most lithium batteries offer a wide range of applications. However, safety issues are still an unresolved issue for several applications. To solve the safety issue of Li-ion batteries, solid polymer electrolyte is a promising candidate to replace commercial liquid electrolyte. A 4-arm star poly(ethylene oxide) polymer with LiTFSI salt as an electrolyte was studied. The dynamics of this polymer were explored with the Quasi-Elastic Neutron Scattering technique. Furthermore, the influence of temperature and Li salt concentration on the polymer dynamics was investigated. The dynamics of the polymer ends of the arm show much higher flexibility than the core parts making those types of polymers attractive for further studies in battery research.
38
Aziz, B. Marif, Brza, Hamsan, and Kadir. "Employing of Trukhan Model to Estimate Ion Transport Parameters in PVA Based Solid Polymer Electrolyte." Polymers 11, no. 10 (2019): 1694. http://dx.doi.org/10.3390/polym11101694.
Full textAbstract:
In the current paper, ion transport parameters in poly (vinyl alcohol) (PVA) based solid polymer electrolyte were examined using Trukhan model successfully. The desired amount of lithium trifluoromethanesulfonate (LiCF3SO3) was dissolved in PVA host polymer to synthesis of solid polymer electrolytes (SPEs). Ion transport parameters such as mobility (μ), diffusion coefficient (D), and charge carrier number density (n) are investigated in detail using impedance spectroscopy. The data results from impedance plots illustrated a decrement of bulk resistance with an increase in temperature. Using electrical equivalent circuits (EEC), electrical impedance plots (ZivsZr) are fitted at various temperatures. The results of impedance study demonstrated that the resistivity of the sample decreases with increasing temperature. The decrease of resistance or impedance with increasing temperature distinguished from Bode plots. The dielectric constant and dielectric loss values increased with an increase in temperature. The loss tangent peaks shifted to higher frequency region and the intensity increased with an increase in temperature. In this contribution, ion transport as a complicated subject in polymer physics is studied. The conductivity versus reciprocal of temperature was found to obey Arrhenius behavior type. The ion transport mechanism is discussed from the tanδ spectra. The ion transport parameters at ambient temperature are found to be 9 × 10−8 cm2/s, 0.8 × 1017 cm−3, and 3 × 10−6 cm2/Vs for D, n, andμ respectively. All these parameters have shown increasing as temperature increased. The electric modulus parameters are studied in an attempt to understand the relaxation dynamics and to clarify the relaxation process and ion dynamics relationship.
39
Gerhardt, Michael Robert, Alejandro O. Barnett, Thulile Khoza, et al. "An Open-Source Continuum Model for Anion-Exchange Membrane Water Electrolysis." ECS Meeting Abstracts MA2023-01, no. 36 (2023): 2002. http://dx.doi.org/10.1149/ma2023-01362002mtgabs.
Full textAbstract:
Anion-exchange membrane (AEM) electrolysis has the potential to produce green hydrogen at low cost by combining the advantages of conventional alkaline electrolysis and proton-exchange membrane electrolysis. The alkaline environment in AEM electrolysis enables the use of less expensive catalysts such as nickel, whereas the use of a solid polymer electrolyte enables differential pressure operation. Recent advancements in AEM performance and lifetime have spurred interest in AEM electrolysis, but many open research areas remain, such as understanding the impacts of water transport in the membrane and salt content in the electrolyte on cell performance and degradation. Furthermore, integrating electrolyser systems into renewable energy grids necessitates dynamic operation of the electrolyser cell, which introduces additional challenges. Computational modelling of AEM electrolysis is ideally suited to tackle many of these open questions by providing insight into the transport processes and electrochemical reactions occurring in the cell under dynamic conditions. In this work, an open-source, transient continuum modelling framework for anion-exchange membrane (AEM) electrolysis is presented and applied to study electrolyzer cell dynamic performance. The one-dimensional cell model contains coupled equations for multiphase flow in the porous transport layers, a parameterized solution property model for potassium hydroxide electrolytes, and coupled ion and water transport equations to account for water activity gradients within the AEM. The model is validated with experimental results from an AEM electrolyser cell. We find that pH gradients develop within the electrolyte due to the production and consumption of hydroxide, which can lead to voltage losses and cell degradation. The influence of these pH gradients on potential catalyst dissolution mechanisms is explored and discussed. Finally, initial studies of transient operation will be presented. This work has been performed in the frame of the CHANNEL project. This project has received funding from the Fuel Cells and Hydrogen 2 Joint Undertaking (now Clean Hydrogen Partnership) under grant agreement No 875088. This Joint undertaking receives support from the European Union's Horizon 2020 Research and Innovation program, Hydrogen Europe and Hydrogen Europe Research. Some of this work has been performed within the MODELYS project "Electrolyzer 2030 – Cell and stack designs" financially supported by the Research Council of Norway under project number 326809.
40
Xue, Xiaoyuan, Long Wan, Wenwen Li, Xueling Tan, Xiaoyu Du, and Yongfen Tong. "A Self-Healing Gel Polymer Electrolyte, Based on a Macromolecule Cross-Linked Chitosan for Flexible Supercapacitors." Gels 9, no. 1 (2022): 8. http://dx.doi.org/10.3390/gels9010008.
Full textAbstract:
Gel polymer electrolytes with a satisfied ionic conductivity have attracted interest in flexible energy storage technologies, such as supercapacitors and rechargeable batteries. However, the poor mechanical strength inhibits its widespread application. One of the most significant ways to avoid the drawbacks of the gel polymer electrolytes without compromising their ion transportation capabilities is to create a self−healing structure with the cross−linking segment. Herein, a new kind of macromolecule chemical cross−linked network ionic gel polymer electrolyte (MCIGPE) with superior electrochemical characteristics, a high flexibility, and an excellent self−healing ability were designed, based on chitosan and dibenzaldehyde−terminated poly (ethylene glycol) (PEGDA) via dynamic imine bonds. The ionic conductivity of the MCIGPE−65 can achieve 2.75 × 10−2 S cm−1. A symmetric all−solid−state supercapacitor employing carbon cloth as current collectors, activated a carbon film as electrodes, and MCIGPE−65 as a gel polymer electrolyte exhibits a high specific capacitance of 51.1 F g−1 at 1 A g−1, and the energy density of 7.1 Wh kg−1 at a power density of 500.2 W kg−1. This research proves the enormous potential of incorporating, environmentally and economically, chitosan into gel polymer electrolytes for supercapacitors.
41
Liu, Jie, Lifang Zhang, Yufeng Cao, et al. "Water-tolerant solid polymer electrolyte with high ion-conductivity for simplified battery manufacturing in air surroundings." Applied Physics Letters 121, no. 15 (2022): 153905. http://dx.doi.org/10.1063/5.0106897.
Full textAbstract:
The humidity-sensitive electrolytes necessitate the stringent conditions of lithium battery manufacturing and, thus, increase the fabrication complexity and cost. We herein report a water-tolerant solid polymer electrolyte (WT-SPE) with high Li+ conductivity (2.08 × 10−4 S cm−1 at room temperature) and electrochemically stable window (up to 4.7 V vs Li/Li+), which utilizes moisture to initiate rapid polymerization and form dense structures to achieve a facile battery manufacturing in humid air without the need of a glovebox. Molecular dynamics simulations attribute this hydrophobic behavior to the hindered transfer of a water molecule in dense WT-SPE. A stable SEI layer composed of a polymeric framework and other organic/inorganic small molecular compounds contributes to the sustainable operation of batteries. As a result, the Li|WT-SPE|LiCoO2 cells manufactured in the air exhibit a high initial capacity of 192 mA h g−1 at 0.1C and an excellent capacity retention for 300 cycles at 1C. The great advantage significantly simplifies the battery assembly process in air environment and can also maintain good interfacial contact between an electrolyte and electrodes thanks to in situ initiated polymerization, which shows great superiority and promise in the alternatives of traditional liquid and polymer electrolytes for low-cost and facile fabrication of batteries in ambient atmosphere.
42
Marinow, Anja, Zviadi Katcharava, and Wolfgang H. Binder. "Self‐Healing Polymer Electrolytes for Next‐Generation Lithium Batteries." Polymers 15, no. 5 (2023): 1145. https://doi.org/10.3390/polym15051145.
Full textAbstract:
Abstract The integration of polymer materials with self-healing features into advanced lithium batteries is a promising and attractive approach to mitigate degradation and, thus, improve the performance and reliability of batteries. Polymeric materials with an ability to autonomously repair themselves after damage may compensate for the mechanical rupture of an electrolyte, prevent the cracking and pulverization of electrodes or stabilize a solid electrolyte interface (SEI), thus prolonging the cycling lifetime of a battery while simultaneously tackling financial and safety issues. This paper comprehensively reviews various categories of self-healing polymer materials for application as electrolytes and adaptive coatings for electrodes in lithium-ion (LIBs) and lithium metal batteries (LMBs). We discuss the opportunities and current challenges in the development of self-healable polymeric materials for lithium batteries in terms of their synthesis, characterization and underlying self-healing mechanism, as well as performance, validation and optimization.
43
Sundari, C. D. D., P. Fitriani, I. M. Arcana, and F. Iskandar. "Correlation between lithium-ion diffusion and coordination environment in solid polymer electrolytes: a molecular dynamics study." Journal of Physics: Conference Series 2734, no. 1 (2024): 012051. http://dx.doi.org/10.1088/1742-6596/2734/1/012051.
Full textAbstract:
Abstract Lithium-ion diffusion in solid polymer electrolytes (SPEs) is a pivotal characteristic that significantly influences overall lithium-ion battery performance. This characteristic can be affected by the coordination environment of lithium ions within the polymer matrix. However, the correlation between lithium-ion diffusion and its coordination environment in biopolymer-based SPEs such as carboxymethyl chitosan (CMCS) remains understudied. In this study, we used molecular dynamics (MD) simulations to investigate this correlation. Lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) was used as the lithium salt in the simulated systems. All MD simulations were conducted using the GROMACS package with the general AMBER force field (GAFF). The coordination structures around Li+ were successfully estimated using the radial distribution function obtained from the MD simulations. These results indicate a preference for Li+ coordination with oxygen atoms, both from the CMCS polymer chains (OCMCS) and TFSI− ions (OTFSI-). The coordination number between Li+ and OCMCS decreases as the concentration of LiTFSI increases. The diffusion coefficients of Li+ varied depending on the concentration of LiTFSI and demonstrated a sensitivity to the coordination structure of Li+. A high diffusion coefficient of Li+ ions was observed at low LiTFSI concentrations, where Li+ was primarily coordinated with oxygen atoms from the CMCS polymer chains.
44
Möller, Julia. "Solid-State NMR Revealing the Impact of Polymer Additives on Li-Ion Motions in Plastic-Crystalline Succinonitrile Electrolytes." ECS Meeting Abstracts MA2023-02, no. 56 (2023): 2726. http://dx.doi.org/10.1149/ma2023-02562726mtgabs.
Full textAbstract:
To enhance the safety of lithium-ion batteries (LIBs), alternatives to liquid electrolytes are widely studied. One of them is the plastic-crystal succinonitrile (SN) which can solvate various Li salts.[1] This system can be further extended by inserting polymers, bringing additional advantages such as higher melting points and the possibility of adjusting thermo-mechanical and electrochemical properties.[2] The plastic-crystalline electrolyte consisting of the Li salt lithium bis(trifluoro-methanesulfonyl)imide (LiTFSI) dissolved in SN was extended by adding various thermoplastic polymers, namely, polyacrylonitrile (PAN), poly(ethylene oxide) (PEO), polyethylene carbonate (PEC), and polyvinylpyrrolidone (PVP). Even small amounts (10 wt %) of added polymer to the SN-base were found to impact the Li-ion mobility. Variable temperature investigations on structure and ion dynamics were performed using static and magic angle spinning (MAS) solid-state NMR and various relaxometry measurements. Influence of the Li-concentration and the polymers’ functional groups on the structure of SN and the resulting Li-ion mobility was elaborated. Activation energies and jump rates of the Li-ions were determined. As a result, the PAN containing system stands out to be a promising candidate for application in future LIBs as it shows high ion mobility, low activation energy, and a high potential for further modifications. Solid-state NMR turned out to be a reliable method and a good alternative to impedance spectroscopy measurements for investigating ion mobility behaviour providing even more information.[3] Literature: [1] S. Long, D. R. MacFarlane, M. Forsyth, Solid State Ionics 2004, 175, 733. [2] N. Voigt, L. van Wüllen, Solid State Ionics 2014, 260, 65. [3] J. Möller, V. van Laack, K. Koschek, P. Bottke, M. Wark, J. Phys. Chem. C 2023, 127, 1464.
45
Ahmad, Shahzada, та S. A. Agnihotry. "Effect of nano γ-Al2O3 addition on ion dynamics in polymer electrolytes". Current Applied Physics 9, № 1 (2009): 108–14. http://dx.doi.org/10.1016/j.cap.2007.12.003.
Full text
46
Selter, Philipp, Stefanie Grote, and Gunther Brunklaus. "Synthesis and7Li Ion Dynamics in Polyarylene-Ethersulfone-Phenylene-Oxide-Based Polymer Electrolytes." Macromolecular Chemistry and Physics 217, no. 23 (2016): 2584–94. http://dx.doi.org/10.1002/macp.201600211.
Full text
47
Tiwari, Tuhina, Neelam Srivastava, and P. C. Srivastava. "Ion Dynamics Study of Potato Starch + Sodium Salts Electrolyte System." International Journal of Electrochemistry 2013 (2013): 1–8. http://dx.doi.org/10.1155/2013/670914.
Full textAbstract:
The effect of different anions, namely,SCN−,I−, andClO4−, on the electrical properties of starch-based polymer electrolytes has been studied. Anion size and conductivity are having an inverse trend indicating systems to be predominantly anionic conductor. Impact of anion size and multiplet forming tendency is reflected in number of charge carriers and mobility, respectively. Ion dynamics study reveals the presence of different mechanisms in different frequency ranges. Interestingly, superlinear power law (SLPL) is found to be present at <5 MHz frequency, which is further confirmed by dielectric data.
48
Srivastava, Neelam, and Manindra Kumar. "Ion dynamics behavior in solid polymer electrolyte." Solid State Ionics 262 (September 2014): 806–10. http://dx.doi.org/10.1016/j.ssi.2013.10.026.
Full text
49
Sadiq, Niyaz M., Shujahadeen B. Aziz, and Mohd F. Z. Kadir. "Development of Flexible Plasticized Ion Conducting Polymer Blend Electrolytes Based on Polyvinyl Alcohol (PVA): Chitosan (CS) with High Ion Transport Parameters Close to Gel Based Electrolytes." Gels 8, no. 3 (2022): 153. http://dx.doi.org/10.3390/gels8030153.
Full textAbstract:
In the current study, flexible films of polyvinyl alcohol (PVA): chitosan (CS) solid polymer blend electrolytes (PBEs) with high ion transport property close enough to gel based electrolytes were prepared with the aid of casting methodology. Glycerol (GL) as a plasticizer and sodium bromide (NaBr) as an ionic source provider are added to PBEs. The flexible films have been examined for their structural and electrical properties. The GL content changed the brittle and solid behavior of the films to a soft manner. X-ray diffraction (XRD) and Fourier transform infrared (FTIR) methods were used to examine the structural behavior of the electrolyte films. X-ray diffraction investigation revealed that the crystalline character of PVA:CS:NaBr declined with increasing GL concentration. The FTIR investigation hypothesized the interaction between polymer mix salt systems and added plasticizer. Infrared (FTIR) band shifts and fluctuations in intensity have been found. The ion transport characteristics such as mobility, carrier density, and diffusion were successfully calculated using the experimental impedance data that had been fitted with EEC components and dielectric parameters. CS:PVA at ambient temperature has the highest ionic conductivity of 3.8 × 10 S/cm for 35 wt.% of NaBr loaded with 55 wt.% of GL. The high ionic conductivity and improved transport properties revealed the suitableness of the films for energy storage device applications. The dielectric constant and dielectric loss were higher at lower frequencies. The relaxation nature of the samples was investigated using loss tangent and electric modulus plots. The peak detected in the spectra of tanδ and M” plots and the distribution of data points are asymmetric besides the peak positions. The movements of ions are not free from the polymer chain dynamics due to viscoelastic relaxation being dominant. The distorted arcs in the Argand plot have confirmed the viscoelastic relaxation in all the prepared films.
50
Tamire, Worku, and Tsiye Hailemariam. "Advancements in Solid-State Batteries Overcoming Challenges in Energy Density and Safety - Review." American Journal of Applied Chemistry 13, no. 2 (2025): 39–46. https://doi.org/10.11648/j.ajac.20251302.12.
Full textAbstract:
Solid-state batteries (SSBs) have emerged as a promising alternative to conventional lithium-ion batteries (LIBs), offering higher energy density, improved safety, and longer cycle life. This review explores recent advancements in SSB technology, focusing on the development of solid electrolytes, electrode materials, and interface engineering. Solid electrolytes, including oxide-based (Li7La3Zr2O12), sulfide-based (Li10GeP2S12), and polymer-based (PEO-LiTFSI) materials, are critical to SSB performance. While oxide-based electrolytes provide high ionic conductivity and stability, sulfide-based electrolytes offer ultra-high conductivity but suffer from air sensitivity. Polymer-based electrolytes are flexible and easy to process but exhibit low conductivity at room temperature. Key challenges such as high interfacial resistance, dendrite formation, and volume changes are addressed through strategies like surface modification, composite electrodes, and 3D architectures. Advanced characterization techniques, including in situ transmission electron microscopy (TEM) and X-ray tomography, provide insights into structural and chemical changes during operation. Computational modeling, such as density functional theory (DFT) and molecular dynamics (MD), accelerates material discovery and interface optimization. Despite significant progress, challenges remain in scalability, performance, and safety. Future research should focus on developing scalable fabrication methods, optimizing electrode-electrolyte interfaces, and integrating SSBs with renewable energy systems for grid storage and electric vehicles. SSBs have the potential to revolutionize energy storage, enabling the widespread adoption of renewable energy and reducing greenhouse gas emissions. Continued innovation and collaboration across disciplines will be essential to overcome remaining challenges and unlock the full potential of SSBs.