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1
Qiao, Mo. "Electrochemical ion pumping." Nature Chemical Engineering 1, no. 11 (2024): 673. http://dx.doi.org/10.1038/s44286-024-00157-8.
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Zhou, Guolang, Linlin Chen, Yanhong Chao, Xiaowei Li, Guiling Luo, and Wenshuai Zhu. "Progress in electrochemical lithium ion pumping for lithium recovery." Journal of Energy Chemistry 59 (August 2021): 431–45. http://dx.doi.org/10.1016/j.jechem.2020.11.012.
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Lado, Julio J., Alba Fombona-Pascual, Daniel Pérez-Antolín, Enrique Garcia - Quismondo, Jesus Palma, and Edgar Ventosa. "Electrochemical Ion Separations By Recyclable Electrode Cell." ECS Meeting Abstracts MA2023-02, no. 25 (2023): 1373. http://dx.doi.org/10.1149/ma2023-02251373mtgabs.
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Electrochemical separations using Faradaic electrodes are able to exceed the ion adsorption values as well as selectivity when compared to capacitive electrodes, which is due to the bulk reactions for the former vs. surface confined for the latter. However, the cyclability of battery/faradaic electrodes is constrained to hundreds or a few thousands of cycles. This work proposes an electrochemical ion pumping design with the unique feature of using injectable electrodes to overcome the ciclability issue and easily control the areal capacity. The idea consists on using injectable electrodes with the intention of recycling the active material once the end-of-life of the device is reached due to active material degradation. In this fashion, the active material is replaced in a straightforward deinjecting-injecting process allowing direct reuse of the inactive components of the device, thus contributing to reducing the replacement cost. This device is called Ion Pumping Injectable Cell (IPIC). Moreover, the IPIC system is a tremendously versatile technology due to the simple and easy methodology employed to replace the electrodes. In this fashion, the system was tested using different types of lithium intercalation materials (LFP and LMO), different ion capturing such as potassium (Prussian Blue Analogs, PBA´s), sodium (NMO) or more conventional activated carbon electrodes (capacitive non-selective electrode). In addition to this feature, it is important to remark that the IPIC could be used in a symmetric (e.g. LFP-LFP) or asymmetric configuration (e.g. LFP-LMO). The main difference is that the asymmetric system has the ability of storing energy while capturing ions and deliver that energy in the subsequent step. This is so due to the different electrode potential. The selectivity toward specific ions is achieved by using a chemical ion-selective separator such as an ion exchange membrane (LFP-LFP or LFP-LMO systems), or by using ion selective intercalation materials such as LFP and PBA´s without the need of selective membranes. In this work, the benefits of the injectable electrode cell architecture will be examined, the performance of different cell configurations will be discussed and the electrochemical ion separation mechanism will be analyzed for different applications. Acknowledgements : J.J. Lado and Alba Fombona-Pascual acknowledge Comunidad de Madrid for the fellowship (2020-T1/AMB-19799).
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Salazar-Avalos, Sebastian, Alvaro Soliz, Luis Cáceres, et al. "Metal Recovery from Natural Saline Brines with an Electrochemical Ion Pumping Method Using Hexacyanoferrate Materials as Electrodes." Nanomaterials 13, no. 18 (2023): 2557. http://dx.doi.org/10.3390/nano13182557.
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The electrochemical ion pumping device is a promising alternative for the development of the industry of recovering metals from natural sources—such as seawater, geothermal water, well brine, or reverse osmosis brine—using electrochemical systems, which is considered a non-evaporative process. This technology is potentially used for metals like Li, Cu, Ca, Mg, Na, K, Sr, and others that are mostly obtained from natural brine sources through a combination of pumping, solar evaporation, and solvent extraction steps. As the future demand for metals for the electronic industry increases, new forms of marine mining processing alternatives are being implemented. Unfortunately, both land and marine mining, such as off-shore and deep sea types, have great potential for severe environmental disruption. In this context, a green alternative is the mixing entropy battery, which is a promising technique whereby the ions are captured from a saline natural source and released into a recovery solution with low ionic force using intercalation materials such as Prussian Blue Analogue (PBA) to store cations inside its crystal structure. This new technique, called “electrochemical ion pumping”, has been proposed for water desalination, lithium concentration, and blue energy recovery using the difference in salt concentration. The raw material for this technology is a saline solution containing ions of interest, such as seawater, natural brines, or industrial waste. In particular, six main ions of interest—Na+, K+, Mg2+, Ca2+, Cl−, and SO42−—are found in seawater, and they constitute 99.5% of the world’s total dissolved salts. This manuscript provides relevant information about this new non-evaporative process for recovering metals from aqueous salty solutions using hexacianometals such as CuHCF, NiHCF, and CoHCF as electrodes, among others, for selective ion removal.
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Galleguillos, Felipe, Luis Cáceres, Lindley Maxwell, and Álvaro Soliz. "Electrochemical Ion Pumping Device for Blue Energy Recovery: Mixing Entropy Battery." Applied Sciences 10, no. 16 (2020): 5537. http://dx.doi.org/10.3390/app10165537.
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In the process of finding new forms of energy extraction or recovery, the use of various natural systems as potential clean and renewable energy sources has been examined. Blue energy is an interesting energy alternative based on chemical energy that is spontaneously released when mixing water solutions with different salt concentrations. This occurs naturally in the discharge of rivers into ocean basins on such a scale that it justifies efforts for detailed research. This article collects the most relevant information from the latest publications on the topic, focusing on the use of the mixing entropy battery (MEB) as an electrochemical ion pumping device and the different technological means that have been developed for the conditions of this process. In addition, it describes various practices and advances achieved by various researchers in the optimization of this device, in relation to the most important redox reactions and the cathode and anodic materials used for the recovery of blue energy or salinity gradient energy.
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Raven, John A., and John Beardall. "Energizing the plasmalemma of marine photosynthetic organisms: the role of primary active transport." Journal of the Marine Biological Association of the United Kingdom 100, no. 3 (2020): 333–46. http://dx.doi.org/10.1017/s0025315420000211.
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AbstractGeneration of ion electrochemical potential differences by primary active transport can involve energy inputs from light, from exergonic redox reactions and from exergonic ATP hydrolysis. These electrochemical potential differences are important for homoeostasis, for signalling, and for energizing nutrient influx. The three main ions involved are H+, Na+ (efflux) and Cl− (influx). In prokaryotes, fluxes of all three of these ions are energized by ion-pumping rhodopsins, with one archaeal rhodopsin pumping H+into the cells; among eukaryotes there is also an H+ influx rhodopsin in Acetabularia and (probably) H+ efflux in diatoms. Bacteriochlorophyll-based photoreactions export H+ from the cytosol in some anoxygenic photosynthetic bacteria, but chlorophyll-based photoreactions in marine cyanobacteria do not lead to export of H+. Exergonic redox reactions export H+ and Na+ in photosynthetic bacteria, and possibly H+ in eukaryotic algae. P-type H+- and/or Na+-ATPases occur in almost all of the photosynthetic marine organisms examined. P-type H+-efflux ATPases occur in charophycean marine algae and flowering plants whereas P-type Na+-ATPases predominate in other marine green algae and non-green algae, possibly with H+-ATPases in some cases. An F-type Cl−-ATPase is known to occur in Acetabularia. Some assignments, on the basis of genomic evidence, of P-type ATPases to H+ or Na+ as the pumped ion are inconclusive.
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Calvo, Ernesto Julio. "Direct Lithium Recovery from Aqueous Electrolytes with Electrochemical Ion Pumping and Lithium Intercalation." ACS Omega 6, no. 51 (2021): 35213–20. http://dx.doi.org/10.1021/acsomega.1c05516.
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Fu, Lin, Yunfei Teng, Pei Liu, et al. "Electrochemical ion-pumping-assisted transfer system featuring a heterogeneous membrane for lithium recovery." Chemical Engineering Journal 435 (May 2022): 134955. http://dx.doi.org/10.1016/j.cej.2022.134955.
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Elmakki, Tasneem, Sifani Zavahir, Umme Hafsa, et al. "Novel LiAlO2 Material for Scalable and Facile Lithium Recovery Using Electrochemical Ion Pumping." Nanomaterials 13, no. 5 (2023): 895. http://dx.doi.org/10.3390/nano13050895.
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In this study, α-LiAlO2 was investigated for the first time as a Li-capturing positive electrode material to recover Li from aqueous Li resources. The material was synthesized using hydrothermal synthesis and air annealing, which is a low-cost and low-energy fabrication process. The physical characterization showed that the material formed an α-LiAlO2 phase, and electrochemical activation revealed the presence of AlO2* as a Li deficient form that can intercalate Li+. The AlO2*/activated carbon electrode pair showed selective capture of Li+ ions when the concentrations were between 100 mM and 25 mM. In mono salt solution comprising 25 mM LiCl, the adsorption capacity was 8.25 mg g−1, and the energy consumption was 27.98 Wh mol Li−1. The system can also handle complex solutions such as first-pass seawater reverse osmosis brine, which has a slightly higher concentration of Li than seawater at 0.34 ppm.
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Habeeb Dolapo Salaudeen, Tajudeen Ayinde Salaudeen, Yahya Onaopemipo, and Olubunmi Samuel. "Review of methods for lithium extraction from geothermal brines." World Journal of Advanced Research and Reviews 24, no. 1 (2024): 948–55. http://dx.doi.org/10.30574/wjarr.2024.24.1.2475.
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Lithium, a highly reactive and valuable metal, is essential for the clean energy transition, powering electronic devices, electric cars, and energy storage systems. With demand for lithium surging, environmentally responsible and economically viable extraction methods are crucial. Traditional sources include brines and mineral clays, but lithium-ion batteries have become a significant secondary source due to their high consumption of lithium. This review explores various extraction methods from geothermal brines, focusing on conventional techniques like solar evaporation, precipitation, and solvent extraction, highlighting their efficiency and limitations. Advanced electrochemical methods are also discussed, including the use of electrochemical ion pumping and electrodialysis, showcasing their potential for high-purity lithium recovery. Direct Lithium Extraction (DLE) technology, which offers over 90% recovery and reduces impurities by over 99%, is identified as a promising approach. The review underscores the need for large-scale field experiments and the development of new lithium sources to meet growing demand.
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Habeeb, Dolapo Salaudeen, Ayinde Salaudeen Tajudeen, Onaopemipo Yahya, and Samuel Olubunmi. "Review of methods for lithium extraction from geothermal brines." World Journal of Advanced Research and Reviews 24, no. 1 (2024): 948–55. https://doi.org/10.5281/zenodo.15016176.
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Lithium, a highly reactive and valuable metal, is essential for the clean energy transition, powering electronic devices, electric cars, and energy storage systems. With demand for lithium surging, environmentally responsible and economically viable extraction methods are crucial. Traditional sources include brines and mineral clays, but lithium-ion batteries have become a significant secondary source due to their high consumption of lithium. This review explores various extraction methods from geothermal brines, focusing on conventional techniques like solar evaporation, precipitation, and solvent extraction, highlighting their efficiency and limitations. Advanced electrochemical methods are also discussed, including the use of electrochemical ion pumping and electrodialysis, showcasing their potential for high-purity lithium recovery. Direct Lithium Extraction (DLE) technology, which offers over 90% recovery and reduces impurities by over 99%, is identified as a promising approach. The review underscores the need for large-scale field experiments and the development of new lithium sources to meet growing demand.
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Perez-Antolin, Daniel, Cristina Irastorza, Sara Gonzalez, et al. "Regenerative electrochemical ion pumping cell based on semi-solid electrodes for sustainable Li recovery." Desalination 533 (July 2022): 115764. http://dx.doi.org/10.1016/j.desal.2022.115764.
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Palagonia, Maria Sofia, Doriano Brogioli, and Fabio La Mantia. "Influence of Hydrodynamics on the Lithium Recovery Efficiency in an Electrochemical Ion Pumping Separation Process." Journal of The Electrochemical Society 164, no. 14 (2017): E586—E595. http://dx.doi.org/10.1149/2.1531714jes.
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Hososhima, Shoko, Hideki Kandori, and Satoshi P. Tsunoda. "Ion transport activity and optogenetics capability of light-driven Na+-pump KR2." PLOS ONE 16, no. 9 (2021): e0256728. http://dx.doi.org/10.1371/journal.pone.0256728.
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KR2 from marine bacteria Krokinobacter eikastus is a light-driven Na+ pumping rhodopsin family (NaRs) member that actively transports Na+ and/or H+ depending on the ionic state. We here report electrophysiological studies on KR2 to address ion-transport properties under various electrochemical potentials of Δ[Na+], ΔpH, membrane voltage and light quality, because the contributions of these on the pumping activity were less understood so far. After transient expression of KR2 in mammalian cultured cells (ND7/23 cells), photocurrents were measured by whole-cell patch clamp under various intracellular Na+ and pH conditions. When KR2 was continuously illuminated with LED light, two distinct time constants were obtained depending on the Na+ concentration. KR2 exhibited slow ion transport (τoff of 28 ms) below 1.1 mM NaCl and rapid transport (τoff of 11 ms) above 11 mM NaCl. This indicates distinct transporting kinetics of H+ and Na+. Photocurrent amplitude (current density) depends on the intracellular Na+ concentration, as is expected for a Na+ pump. The M-intermediate in the photocycle of KR2 could be transferred into the dark state without net ion transport by blue light illumination on top of green light. The M intermediate was stabilized by higher membrane voltage. Furthermore, we assessed the optogenetic silencing effect of rat cortical neurons after expressing KR2. Light power dependency revealed that action potential was profoundly inhibited by 1.5 mW/mm2 green light illumination, confirming the ability to apply KR2 as an optogenetics silencer.
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Nelson, N. "The vacuolar H(+)-ATPase--one of the most fundamental ion pumps in nature." Journal of Experimental Biology 172, no. 1 (1992): 19–27. http://dx.doi.org/10.1242/jeb.172.1.19.
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An electrochemical gradient of protons (PMF) is a universal high-energy intermediate in biological systems. Two related families of proton pumps, denoted F- and V-ATPases, are among the principal generators of a PMF from ATP and can form ATP at the expense of a PMF. The enzymes of these two families share a similar structure and subunit composition; some subunits in the two families evolved from common ancestors. Other subunits having no common ancestry were added independently to the various enzymes and defined the two separate families. The general mechanism for the proton pumping activity is similar in the two families. However, whereas F-ATPases can act in both proton pumping and ATP formation, the V-ATPases of eukaryotes function exclusively as ATP-dependent proton pumps. The catalytic and membrane sectors of F-ATPases and archaebacterial V-ATPases can separately catalyze their specific partial activities of ATPase and proton conduction. The catalytic and membrane sectors of the eukaryotic V-ATPases cannot act separately. This property is correlated with the presence of a large proteolipid that traverses the membrane four times. The gene duplication of the smaller proteolipid in the formation of the large proteolipid was one of the most important events in the evolution of the V-ATPases of eukaryotic cells.
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Kautz, Rylan, Ethan J. Heffernan, Alon Herman, Joel Ager, Gideon Segev, and Shane Ardo. "Continuous Ion Separations Using Non-Faradaic Capacitive AC Ratcheting." ECS Meeting Abstracts MA2022-02, no. 27 (2022): 1052. http://dx.doi.org/10.1149/ma2022-02271052mtgabs.
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Traditional electrochemical separations processes require Faradaic reactions for sustained currents. We discovered that this limitation can be overcome by oscillating the applied potential across an ion-permeable material that has an asymmetric electric potential profile. We demonstrated this phenomenon for the first time using a flashing ratchet consisting of a nanoporous anodized aluminum oxide membrane infiltrated with salt water and containing metallic contacts on either side. When a symmetric +/-300 mV square-wave potential was applied to the metallic contacts at a frequency of ~100 Hz, an open-circuit potential as large as ~50 mV was observed between Ag/AgCl electrodes immersed in the chloride-containing electrolyte and positioned across the membrane. While this open-circuit potential was determined to be a consequence of net ionic polarization, additional electrochemical data were also consistent with transport of neutral salt across the membrane via a proposed ambipolar transport mechanism. In comparison, application of a DC potential bias resulted in non-Faradaic charging, and a near-zero long-time open-circuit potential. Moreover, high ionic strengths and large pore sizes diminished ratcheting behavior, consistent will more complete screening of surface charges in the nanopores. Collectively, this work represents a new paradigm for direct ion pumping and salt separations that requires no Faradaic reactions or additional transport pathway for ions or electrons.
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Trocoli, Rafael, Ghoncheh Kasiri Bidhendi, and Fabio La Mantia. "Lithium recovery by means of electrochemical ion pumping: a comparison between salt capturing and selective exchange." Journal of Physics: Condensed Matter 28, no. 11 (2016): 114005. http://dx.doi.org/10.1088/0953-8984/28/11/114005.
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Bronner, F., and W. D. Stein. "CaBPr facilitates intracellular diffusion for Ca pumping in distal convoluted tubule." American Journal of Physiology-Renal Physiology 255, no. 3 (1988): F558—F562. http://dx.doi.org/10.1152/ajprenal.1988.255.3.f558.
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The system of renal Ca transport in the rat is modeled in terms of two classes of processes: a nonsaturable flux that predominates in the proximal tubule, and an active, vitamin D-dependent flux with major expression in the distal convoluted tubule. There transport is against an electrochemical gradient, with much of the efflux probably mediated by the Ca/Mg-ATPase. Calculations of the rate of free Ca diffusion in tubular cells indicate that an unaided flux would be only one-seventy-seventh of that found experimentally. It is suggested that the vitamin D-induced renal calcium binding protein, CaBPr, Mr approximately 28,000, in raising total cellular calcium by three orders of magnitude, increases the transcellular Ca flux and thus the free intracellular Ca ion concentration at the basolateral pole, allowing the Ca/Mg-ATPase to function near its maximum. Analysis of the rate of nonsaturable Ca flux throughout the kidney tubule suggests a paracellular pathway via bulk flow, following water that is driven osmotically. Evaluation of whole animal data in terms of these two classes of calcium fluxes indicates that our model is consistent with experimental observations and assigns a functional role to active calcium transport.
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Shapovalov, Yuriy, Lyazzat Gumarova, and Arailym Massuadin. "Electro-enzymatic processes in mitochondria." BIO Web of Conferences 100 (2024): 01016. http://dx.doi.org/10.1051/bioconf/202410001016.
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Four enzymatic complexes form the electron transport chain of the mitochondrion. Complexes I and II are current generator half-elements, that create electron flows with the participation of the enzymes NADH dehydrogenase and Succinate dehydrogenase, oxidizing NADH·H into NAD+, and succinate into fumarate, respectively. Electrons are transferred throw the iron-sulfur clusters system, participate reduction enzymatic reaction of CoQ10 into CoQ10Н2. The proton pumping into the mitochondrial intermembrane space, as well as the regeneration of CoQ10 occur when electrons transferred by ubiquinone-cytochrome-c-oxidoreductase enzyme to the Riske iron-sulfur protein (Fe2S2). The Riske protein regulates electron flows: it transfers one electron to the bL,bН (III) complex, and the other to cytochrome c. Cytochrome c directs electrons to the ΙV complex electrolysis system. The binuclear copper center [CuA-CuB] of the ΙV complex is the anode, where oxygen is formed. Electrons along the galvanic pair chain from paired copper Cu2++ e- ↔ Cu+ and iron Fe2+- е- ↔Fe3+ are transferred to the cathode, copper ion (Сu+), where the electrochemical reaction occurs O2 + 4e- + 4H+ → 2H2O, with the pumping of 4 protons into the mitochondrial intermembrane space.
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Arges, Christopher G., Gokul Venugopalan, and Deepra Bhattacharya. "(Invited) Electrochemical Pumping for Hydrogen Storage and Distribution in the Natural Gas Pipeline." ECS Meeting Abstracts MA2022-01, no. 39 (2022): 1786. http://dx.doi.org/10.1149/ma2022-01391786mtgabs.
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Over the next decade, the production and use of hydrogen in various sectors of the global economy is anticipated to grow significantly. It is an already important feedstock in the production of ammonia and desulfurization of fuels in addition to being used in metals refining and as a coolant in thermal electric power plants. More recently, hydrogen is being considered for long-term seasonal energy storage for energy derived from renewables like solar and wind. To alleviate the severe costs of building out completely new infrastructure, the U.S. natural gas pipeline represents an enticing proposition for hydrogen storage and a potential distribution network from centralized production facilities. Embrittlement concerns of the pipeline with hydrogen limit the hydrogen partial pressure/concentration of hydrogen to be stored. Because many end use applications often require high purity hydrogen, it is necessary to separate/de-blend hydrogen from natural gas and compress it at the point-of-use. This talk presents high-temperature polymer electrolyte membrane (HT-PEM) electrochemical hydrogen pumps for separating hydrogen from gas mixtures. Hydrogen purification to +99% from syngas (25mol% hydrogen and 40mol% carbon monoxide (CO)) at 1 A cm-2 and cell voltage of 0.4 V with an electrochemical hydrogen pump was demonstrated. About 90% of hydrogen used in the United States today derives from steam-reformed natural gas that contains large concentrations of CO – which is a potent platinum electrocatalyst poison at temperatures below 100 °C. The hydrogen purification from syngas was possible with an electrochemical hydrogen pump operated at 220 °C and by using: i.) an ion pair HT-PEM that exploits electrostatic interactions to prevent phosphoric acid leaching at elevated temperatures from the membrane matrix and in the presence of water and ii.) a phosphonic acid ionomer electrode binder. The membrane electrode assembly (MEA) with the said materials and platinum on carbon (Pt/C) electrocatalyst was also effective for purifying hydrogen from other types of reformed hydrocarbons with different CO and hydrogen concentrations. Unexpectedly, operating the HT-PEM hydrogen pump at 220 °C minimized CO impact on cell polarization. At this temperature, cell polarization was governed by the hydrogen concentration in the gas feed. These observations motivate future work to develop new electrodes and electrode binders that can extract, purify, and compress hydrogen with feed streams that have low hydrogen content and contain other constituents in natural gas (methane, ethane, t-butyl mercaptan, etc).
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Xu, Helin. "Advanced Electrode Materials in Capacitive Deionization for Lithium Recovery." Highlights in Science, Engineering and Technology 26 (December 30, 2022): 270–78. http://dx.doi.org/10.54097/hset.v26i.3984.
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Demand for lithium batteries and lithium resources is growing because of the fast development of electric vehicles which will reach 900,000 metric tons per year by 2025. But the available lithium supplies are running out, and the future utilization of lithium resources will depend on strong productivity and resource recovery. However, current methods of extracting lithium ion resources still have the disadvantages of slow rates, unstable system outputs, and low purity. These methods can hardly compensate for the huge market demand in the future. The alternative technology, capacitive deionization (CDI) technology based on electrochemical ion pumping, provides a high capacity and rate of lithium resource recovery, which uses renewable electrode materials, reduces system waste generation, and has high lithium ion purity in the extract, which is sufficient to meet the future market demand. This mini-review analyzes the electrode materials used in CDI technology with a particular emphasis on the development of three materials, Olivine LiFePO4/FePO4, Spinel LiMn2O4/λ-MnO2, and Spinel LiNi0.5Mn1.5O4. The advantages and disadvantages of the current advanced materials are evaluated from various perspectives, and the feasibility of different electrodes is analyzed.
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Rico-Zavala, A., J. L. Pineda-Delgado, A. Carbone, et al. "Composite Sulfonated Polyether-Ether Ketone Membranes with SBA-15 for Electrochemical Energy Systems." Materials 13, no. 7 (2020): 1570. http://dx.doi.org/10.3390/ma13071570.
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The aim of this work is the evaluation of a Sulfonated Poly Ether-Ether Ketone (S-PEEK) polymer modified by the addition of pure Santa Barbara Amorphous-15 (SBA-15, mesoporous silica) and SBA-15 previously impregnated with phosphotungstic acid (PWA) fillers (PWA/SBA-15) in order to prepare composite membranes as an alternative to conventional Nafion® membranes. This component is intended to be used as an electrolyte in electrochemical energy systems such as hydrogen and methanol Proton Exchange Membrane Fuel Cell (PEMFC) and Electrochemical Hydrogen Pumping (EHP). The common requirements for all the applications are high proton conductivity, thermomechanical stability, and fuel and oxidant impermeability. The morphology of the composite membranes was investigated by Scanning Electron Microscopy- Energy Dispersive X-ray Spectroscopy (SEM-EDS) analysis. Water Uptake (Wup), Ion Exchange Capacity (IEC), proton conductivity, methanol permeability and other physicochemical properties were evaluated. In PEMFC tests, the S-PEEK membrane with a 10 wt.% SBA-15 loading showed the highest performance. For EHP, the inclusion of inorganic materials led to a back-diffusion, limiting the compression capacity. Concerning methanol permeability, the lowest methanol crossover corresponded to the composites containing 5 wt.% and 10 wt.% SBA-15.
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Raja, Shilpa N., Jessica G. Swallow, Sean R. Bishop, et al. "Analysis of Electrochemomechanical Coupling in Non-Stoichiometric Oxide Thin Films." ECS Meeting Abstracts MA2018-01, no. 32 (2018): 1933. http://dx.doi.org/10.1149/ma2018-01/32/1933.
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Non-stoichiometric oxides are used in a wide variety of applications including solid oxide fuel cells (SOFCs), lithium ion batteries (LIBs), gas sensors, and catalysis. Through the capacity of such materials to support large point defect concentrations, these functional oxides can readily store, transport, and exchange ions. An important consequence of this non-stoichiometry is a tendency toward chemomechanical coupling, particularly in the form of chemical expansion, or the coupling between material volume and defect concentration. Thin films of non-stoichiometric oxides are of particular interest in such device designs, given the potential for strain engineering. For example, it has been shown for several materials that tensile strain can increase the ionic conductivity or gas exchange reactivity for oxygen by up to an order of magnitude, potentially enabling enhanced device efficiency or decreased operating temperatures1. In electrochemical devices, chemical expansion can generate stress or strain that can lead to mechanical failure, and/or changes in mechanical properties including elastic moduli. Given the extreme environments and range of non-stoichiometric oxides in which chemical expansion can be expected, robust device design requires accurate, flexible, and rapid characterization of environmental conditions and materials that maximize (or minimize) chemical expansion in situ. However, methods used at present for characterizing chemomechanical expansion, such as dilatometry, synchrotron techniques, reflectometry, and others, are not amenable to thin films or are difficult to implement in standard laboratory settings. Recently, Swallow et al. described an approach for characterizing thin film non-stoichiometric oxide chemical expansion at high temperatures by way of electrochemically induced actuation that addresses the above needs2. That work characterized volume change within a fluorite film of PrxCe1-xO2-δ (PCO) and structural deflection of the PCO/YSZ (yttria-stablized zirconia) bilayer during electrochemical pumping of oxygen ions into the PCO film. It also demonstrated a positive attribute of such chemical expansion in the form of high temperature oxide actuators, which harness electrochemically generated chemical strain to produce measurable, nanoscale device deflections. The actuation produced ranged between 5-15 nm of displacement amplitude depending on the experimental conditions2. Here, we provide an extended and graphically rich analysis of electrical and mechanical response data from such experiments. We model the current and mechanical response of PCO to an electrochemical driving force using previously established defect equilibria and kinetic relationships for that oxide, demonstrating the contributions that material properties and sample geometries make to device deflection and electrochemical pumping. We also extend the measurement approach to an additional material system, the perovskite-structured oxide SrTi0.65Fe0,35O3-δ (STF) used as part of magnetic memory devices, gas transport membranes, and fuel cells. This case study demonstrates the broad applicability of this measurement method, as well as means to leverage chemical expansion effects at elevated temperatures for diverse actuating and functional devices. Yildiz, B. ‘Stretching’ the energy landscape of oxides—Effects on electrocatalysis and diffusion. MRS Bull. 39, 147–156 (2014). Swallow, J. G. et al. Dynamic chemical expansion of thin-film non-stoichiometric oxides at extreme temperatures. Nat Mater (2017). doi:10.1038/nmat4898
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Trócoli, Rafael, Collins Erinmwingbovo та Fabio La Mantia. "Optimized Lithium Recovery from Brines by using an Electrochemical Ion-Pumping Process Based on λ-MnO2 and Nickel Hexacyanoferrate". ChemElectroChem 4, № 1 (2016): 143–49. http://dx.doi.org/10.1002/celc.201600509.
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Kaliaperumal, Muthukrishnan, and Ramesh Kumar Chidambaram. "Thermal Management of Lithium-Ion Battery Pack Using Equivalent Circuit Model." Vehicles 6, no. 3 (2024): 1200–1215. http://dx.doi.org/10.3390/vehicles6030057.
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The design of an efficient thermal management system for a lithium-ion battery pack hinges on a deep understanding of the cells’ thermal behavior. This understanding can be gained through theoretical or experimental methods. While the theoretical study of the cells using electrochemical and numerical methods requires expensive computing facilities and time, the Equivalent Circuit Model (ECM) offers a more direct approach. However, upfront experimental cell characterization is needed to determine the ECM parameters. In this study, the behavior of a cell is characterized experimentally, and the results are used to build a second-order equivalent electrical circuit model of the cell. This model is then integrated with the cooling system of the battery pack for effective thermal management. The Equivalent Circuit Model estimates the internal heat generation inside the cell using instantaneous load current, terminal voltage, and temperature data. By extrapolating the heat generation data of a single cell, we can determine the heat generation of the cells in the pack. With the implementation of the ECM in the cooling system, the coolant flow rate can be adjusted to ensure the attainment of a safe operating cell temperature. Our study confirms that 14% of pumping power can be reduced when compared to the conventional constant flow rate cooling system, while still maintaining the temperature of the cells within safe limits.
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Herman, Alon, Dafna Meltser, Eden Grossman, Karen Shushan, and Gideon Segev. "(Invited) Ratchet Based Ion Pumps for Selective Ion Separations." ECS Meeting Abstracts MA2023-02, no. 18 (2023): 1204. http://dx.doi.org/10.1149/ma2023-02181204mtgabs.
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Even though highly selective ion pumps are found in the membrane of every living cell, artificial ion selective separation is a longstanding unmet challenge in science and engineering. The development of a membrane-based ion separation technology can drive a dramatic progress in a wide range of applications such as: water treatment, bio-medical devices, extraction of precious metals from sea water, chemical sensors, solar fuels and more. In this contribution we report the experimental demonstration of ion pumps based on a electronic ratchet mechanism. Electronic ratchets are devices that utilize a temporal modulation of a spatially asymmetric electric field to drive steady state current. Like peristaltic pumps, where the pump mechanism is not in direct contact with the pumped fluid, electronic ratchets induce a net current with no direct charge transport between the power source and the pumped charge carriers. Thus, electronic ratchets can be used to pump ions in steady state with no electrochemical reactions between the power source and the pumped ions resulting in an 'all-electric' ion pump. Ratchet-based ion pumps (RBIPs) were fabricated by coating the two surfaces of nano-porous alumina wafers with gold, thus forming nano-porous capacitor-like devices. The electric field within the nano-pores is modulated by oscillating the capacitor voltage. Thus, when immersed in a solution, ions within the pores experience a modulating electric field resulting in ratchet-based ion pumping. The RBIPs performance was studied for various input signals, geometries, and solutions. RBIPs were shown to drive ionic current densities of several uA/cm^2 even when opposed by an electrostatic force. A significant ratchet action was observed with input signal amplitudes as low as 0.1V thus demonstrating that RBIPs can drive an ionic current with no associated redox reactions. An important hallmark of ratchets is the ability to invert the direction of particle flow with a change in the input signal frequency. The stopping frequency, which is the frequency at which the particle flux changes its direction, is determined by the potential distribution and particles transport properties. As a result, for a given ratchet, there can be a frequency at which particles with the same charge, but different diffusion coefficients, are transported in opposite directions. This concept, that was never applied to ion separations, can enable the extraction of ions with extremely low relative concentrations if their diffusion coefficient is even slightly different from the main ions in the solution. We show by simulation, that for the prevalent ions in water, ions with a relative diffusion coefficient difference as small as 1% can be driven to opposite directions with a velocity difference as high as 1.2 mm/s. Since the direction of ion transport is determined by the input signal frequency, the sorting properties can be tuned in real time providing a simple fit-to-purpose solution for a variety of ion separations applications. Figure 1
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Sinclair, Paul. "The Through-Flow Electrochemical Cell - a Breakthrough Technology." ECS Meeting Abstracts MA2023-02, no. 1 (2023): 107. http://dx.doi.org/10.1149/ma2023-021107mtgabs.
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The paper describes a new approach to energy-storage electrochemical cells that is “chemistry-agnostic” and promises to solve several problems of existing batteries. These problems include: Charging rates are too slow Intrinsic failure-mechanisms compromise safety Energy Density is inadequate for mobile applications Lifetime is too short for large-scale permanent installations The key idea of the “Through-Flow Cell” is that the electrolyte is pumped continuously in a closed loop through a porous anode, porous separator, and porous cathode, in a direction aiding the active ionic flow. Although the idea of moving a liquid electrolyte is not new, there have not been any successful commercial products until now. It should not be confused with the “Flow-Battery”, an entirely different concept where two different fluids flow separately within anode and cathode. Previous attempts to develop a reliable Through-Flow Cell foundered on the difficulty of immobilizing active materials on the anode and cathode collectors while fluid flows freely through surrounding pore-spaces. I describe a new active-material encapsulation method to achieve that crucial objective, and a new more convenient cell configuration. Applications will include large grid-scale installations and could include high-power transportation vehicles such as trains and buses. The basic cell is configured as a stack-able, de-mountable, and repairable module. It is a completely self-contained package incorporating an adaptive electrolyte pumping system with optional heating and/or cooling to optimize efficiency in a wide range of environmental conditions. In grid-scale systems the ability to easily remove a low-performing cell from a stack, repair, and replace it is a very desirable feature that extends the life of a high-CAPEX installation almost indefinitely. The new cell design has a conservative capacity rating of 3000 Amp.hr (using 300 mA.hr/gm active materials) and a continuous current rating of 2000 Amps, with the cell voltage being determined by the chemistry employed. For the Lithium-ion chemistry with a nominal voltage of 3.7v it has 10 KW.hr energy capacity @ 90% discharge. A linear stack of 100 cells makes a battery storing 1 MW.hr on a rack 9 meters in length; easily accommodated in an enclosure the size of a shipping container that could contain up to eight such racks. For some people the idea of a battery with moving parts runs counter to notions of simplicity found in the standard sealed cylindrical cells. In practice, however, large assemblies of such cells require complex external liquid cooling and possibly fire-suppression systems. When individual cells fail, they are usually disconnected by blowing fuses, resulting in a steady degradation that is not easily repairable. In contrast to sealed cells, some unique advantages of the electrolyte circulation technique can be summarized as follows: Effective Mobility of active-species ions is dramatically boosted by the flow velocity, translating into reduced series resistance between electrodes. Peak charging or discharging currents can be ten times higher without overheating or loss of charge capacity when the flow velocity is only one centimeter per second. Flow direction is reversed when switching from charging to discharging, which reverses dendrite growth that is a potential source of catastrophic failure. The interior temperature of the cell can be directly controlled and excess heat removed from the electrolyte by an external heat-exchanger, or added in cold climates. The Anode and Cathode, being 3-Dimensional porous structures, incorporate greatly increased volumes of active material compared to typical 2-Dimensional foil electrodes. Electrolyte flowing across the surface of active material inside porous electrodes efficiently sweeps away ion-deficient liquid from within the Slipping-Plane near the Solid-Electrolyte Interface (SEI), reducing the parasitic Zeta-Potential. Results from a proof-of-principle laboratory cell using the Nickel Metal-Hydride chemistry will be briefly described, and a full-scale commercial cell design presented in more detail. The very important active-material encapsulation technique is also described along with its unique ability to tolerate large changes in volume of the active material without degradation. Current cylindrical “jelly-roll” format cells cannot tolerate significant volume change caused by ion-intercalation inside active materials without physical destruction. The new technology may enable complete replacement of Graphite by Silicon in the Anodes of Lithium-ion cells. Silicon has a charge capacity almost four times greater than Graphite, but expands up to 400%. In another example, Cathodes in the Lithium-Sulfur chemistry may tolerate far higher Sulfur loading with corresponding increased energy density. In summary, this new focus on the mechanics of energy-storage cells shows promise for a step-change increase in power-density, reliability, and safety. As described, the idea can be applied to any new improvement in chemistry that uses a liquid electrolyte as soon as it achieves maturity. Figure 1
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Kołacz, Angelika Monika, Monika Wiśnik-Sawka, Mirosław Maziejuk, et al. "Air Pollution and Radiation Monitoring in Collective Protection Facilities." Sensors 23, no. 2 (2023): 706. http://dx.doi.org/10.3390/s23020706.
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It has become increasingly important to monitor environment contamination by such chemicals as chemical warfare agents (CWAs) and industrial toxic chemicals (TICs), as well as radiation hazards around and inside collective protection facilities. This is especially important given the increased risk of terrorist or military attacks. The Military Institute of Chemistry and Radiometry (MICR) has constructed and developed the ALERT device for the effective monitoring of these threats. This device uses sensors that detect chemical and radiological contaminations in the air. The CWA detector is an ion mobility spectrometer, TICs are detected by electrochemical sensors, and radiation hazards are detected via Geiger–Muller tubes. The system was designed to protect the crew from contamination. When chemical or radioactive contamination is detected at the air inlet for the shelter, air filtration through a carbon filter is activated. At this time, the air test procedure at the filter outlet is started to test the condition of the filter on an ongoing basis. After detecting contamination at the filter outlet, the system turns off the air pumping and the service can start the procedure of replacing the damaged carbon filter. This paper presents the results of laboratory testing of the ALERT gas alarm detector, which showed high measurements for important parameters, including sensitivity, repeatability, accuracy, and speed.
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Yesilyurt, Muhammed Samil, and Huseyin Ayhan Yavasoglu. "An All-Vanadium Redox Flow Battery: A Comprehensive Equivalent Circuit Model." Energies 16, no. 4 (2023): 2040. http://dx.doi.org/10.3390/en16042040.
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In this paper, we propose a sophisticated battery model for vanadium redox flow batteries (VRFBs), which are a promising energy storage technology due to their design flexibility, low manufacturing costs on a large scale, indefinite lifetime, and recyclable electrolytes. Primarily, fluid distribution is analysed using computational fluid dynamics (CFD) considering only half-cells. Based on the analysis results, a novel model is developed in the MATLAB Simulink environment which is capable of identifying both the steady-state and dynamic characteristics of VRFBs. Unlike the majority of published studies, the inherent characteristics of the flow battery, such as shunt current, ion diffusion, and pumping energy consumption, are considered. Furthermore, simplified charge transfer resistance (CTR) is taken into account based on electrochemical impedance spectroscopy (EIS) measurement results. The accuracy of the model was determined by comparing the simulation results generated by the equivalent circuit battery model developed in this study with real datasets. The obtained results indicate that the developed model has an accuracy of 3% under the sample operating conditions selected. This study can also be used to fill the gap left by the absence of the VRFB battery model in commonly used programs for renewable energy systems, such as TRNSYS.
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Thangadurai, Venkataraman, Oanh Hoang Nguyen, Muhammad Shoaib, and Prathap Iyapazham Vaigunda Suba. "(Invited) Redox Flow Batteries – Exploring Electrolyte Additives and Hybrid Organic/Inorganic Redox Pairs." ECS Meeting Abstracts MA2024-01, no. 1 (2024): 87. http://dx.doi.org/10.1149/ma2024-01187mtgabs.
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Renewable energy sources are intermittent and thus require provision to store the energy when available using energy storage devices. These energy storage devices should be safe, efficient, and have a long life cycle for use in grid-scale energy storage systems. Lead-acid, Li-ion, and Redox Flow Batteries (RFBs) are examples of such energy storage devices. Among these energy storage systems, RFBs have unique advantages that make them attractive for large-scale energy storage applications, like a high cycle life of about 10,000 cycles.[1] The current generation of commercial RFBs use vanadium solution in different oxidation states as electrolytes (anolyte and catholyte), carbon-based electrodes and Nafion as the ion-exchange membrane. High cost, risk of electrolyte crossover, low volumetric energy density, and pumping losses limit the vanadium redox flow batteries (VRFBs).[2] Also, the Nafion membrane accounts for about 40% of the system's total cost.[3] To ensure high cycle life, the electrolytes must be stable (active material must remain dissolved in the supporting electrolyte), and vanadium ions should not crossover the Nafion membrane. The VRFBs tend to lose vanadium from electrolyte solutions due to the precipitation of V2O5 during charging, resulting in a significant loss of energy density. Additives help in maintaining the long-term stability of vanadium electrolytes. In this work, we have monitored the solubility and electrochemical characteristics of vanadium electrolyte solutions with V2O5 in the presence of different additives, namely HCl and MSA (methanesulfonic acid), for over three months.[4] The findings of this study provide insight into using these additives for VRFBs. Further research in RFBs has recently shifted towards redox-active aqueous-organic-based electrolytes consisting of Earth-abundant elements (C, H, O, N, S), accommodating the need for green, safe, and low-cost energy storage. We have studied the feasibility of using quinone-based organic electrolytes for RFBs. A proof-of-concept membrane-free two-compartment cell with an auxiliary electrode in each compartment was also demonstrated. In the conventional design, the hydrogen ions move through the Nafion membrane to balance charges but in the auxiliary electrode-based membrane-free setup, the auxiliary electrode in each compartment undergoes redox reactions opposite to the primary electrodes to balance charges.[5] References [1] Y.E. Durmus, H. Zhang, F. Baakes, G. Desmaizieres, H. Hayun, L. Yang, M. Kolek, V. Küpers, J. Janek, D. Mandler, S. Passerini, Y. Ein‐Eli, Side by Side Battery Technologies with Lithium‐Ion Based Batteries, Adv. Energy Mater. 10 (2020). https://doi.org/10.1002/aenm.202000089. [2] B. Turker, S. Arroyo Klein, E.M. Hammer, B. Lenz, L. Komsiyska, Modeling a vanadium redox flow battery system for large scale applications, Energy Convers. Manag. 66 (2013) 26–32. https://doi.org/10.1016/j.enconman.2012.09.009. [3] J. Ye, D. Yuan, M. Ding, Y. Long, T. Long, L. Sun, C. Jia, A cost-effective nafion/lignin composite membrane with low vanadium ion permeation for high performance vanadium redox flow battery, J. Power Sources. 482 (2021) 229023. https://doi.org/10.1016/j.jpowsour.2020.229023. [4] O.H. Nguyen, P. Iyapazham Vaigunda Suba, M. Shoaib, V. Thangadurai, Investigating the Electro-Kinetics and Long-Term Solubility of Vanadium Electrolyte in the Presence of Inorganic Additives, J. Electrochem. Soc. 170 (2023) 110523. https://doi.org/10.1149/1945-7111/ad0a75. [5] S.V. Venkatesan, K. Karan, S.R. Larter, V. Thangadurai, An auxiliary electrode mediated membrane-free redox electrochemical cell for energy storage, Sustain. Energy Fuels. 4 (2020) 2149–2152. https://doi.org/10.1039/c9se00734b.
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Roenigk, Samantha, and James McKone. "CO2 Hydrogenation through Electrochemical Hydrogen Activation in a Gas-Vapor Fed Reactor." ECS Meeting Abstracts MA2024-02, no. 62 (2024): 4169. https://doi.org/10.1149/ma2024-02624169mtgabs.
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An attractive concept in the chemical manufacturing industry is the adoption of a circular carbon economy, which can include continuous capture and conversion of CO2 into industrially relevant chemical feedstocks. This has driven considerable research interest in electrochemical CO2 reduction.1 Despite this popularity, major challenges remain even for the most advanced CO2 reduction reactors, including low conversion rates and energy efficiencies; moreover, in many cases, multiple carbon-containing products are generated, which add to costs for downstream separation.2 By contrast, thermochemical CO2 hydrogenation is well established and typically demonstrates higher energy efficiency and selectivity compared to electrochemical CO2 reduction.3,4 This notable contrast drives our interest in better understanding the physics that governs differences in reactivity between thermocatalytic and electrocatalytic CO2 reduction reactors. To address these questions, we are pursuing a unique approach that involves feeding humidified CO2 and H2, respectively, to the cathode and anode of an electrochemical membrane-electrode assembly (MEA). This presentation will cover initial work we have undertaken to design and validate this reactor for the study CO2 electro-reduction. The overall design of our reactor resembles a hydrogen fuel cell fed with humidified H2 and CO2. Thus, it was initially benchmarked through operation as an electrochemical hydrogen pump, wherein humidified Ar was fed to the cathode and humidified H2 was fed to the anode with Pt/C as the catalyst on each side of the membrane. Under these conditions, a cation exchange membrane (CEM) readily generated current densities in excess of 1 A/cm2 with monotonic decreases in polarization with increased temperature at fixed current. We then undertook analogous hydrogen pumping experiments using anion exchange membranes (AEM) that had been ion-exchanged with hydroxide, carbonate, and bicarbonate anions. We observed net proton transport between the anode and cathode chambers in each case, albeit with higher ionic resistance for AEMs in the bicarbonate form. We then undertook further studies to demonstrate the ability to reduce CO2 using H2 fed to the anode. This operating mode eliminates the need for a liquid anode feed, which dramatically reduces the driving force for CO2 crossover via bicarbonate formation. Moreover, the Pt/C anode catalyst is expected to oxidize hydrogen with minimal polarization, allowing the total cell polarization to be interpreted simply as the cathode potential on the RHE scale. CO2 reduction experiments were carried out using commercial Cu/C catalyst with online gas chromatography and NMR for product analysis of volatile and condensable products, respectively. Operation with a CEM yielded only H2(g) at the cathode, but initial experiments with an AEM in the carbonate/bicarbonate form gave high selectivity to ethanol at 70 oC. References: Sebastian-Pascual,P; Mezzavilla,S; Stephens,I,; Escudero-Escribano,M. Structure-Sensitivity and Electrolyte Effects in CO2 electroreduction: Fom Model Studies to Applications, ChemCatChem 2019,11,16,3626-3645. Higgins.D.; Hahn,C.; Xiang,C.; Jaramillo, T.F.; Weber, A. Z. Gas-Diffusion Electrodes for Carbon Dioxide Reduction: A New Paradigm. ACS Energy Letters 2019, 4, 1, 317-324. Gao, J.; Choo Sze Shiong, S.; Liu,Y.Reduction of CO2 to chemicals and Fuels: Thermocatalysis versus electrocatalysis, Chemical Engineering Journal 2023, 472, 145033 Alli, Y. A.; Oladoye, P. O.; Ejeromedoghene, O.; Bankole, O. M.; Alimi, O. A.; Omotola, E. O.; Olanrewaju, C. A.; Philippot, K.; Adeleye, A. S.; Ogunlaja, A. S. Nanomaterials as Catalysts for CO2 Transformation into Value-Added Products: A Review. Science of The Total Environment 2023, 868, 161547.
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Bhuiyan, Shaikh Al Mahmud, Aman Preet Kaur, Chad M. Risko, and Christine A. Trinkle. "A 3D Printed Pumpless Nonaqueous Organic Redox Flow Cell." ECS Meeting Abstracts MA2024-01, no. 5 (2024): 768. http://dx.doi.org/10.1149/ma2024-015768mtgabs.
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Redox flow batteries (RFBs) have considerable promise in addressing the ever-increasing demands for robust energy storage devices. The nature of these devices makes it possible to create storage with potential applicability at multiple size scales1. However, conventional RFBs require energy to pump the liquid electrolyte, reducing the overall system efficiency, and limiting its viability to mid- and large-scale operations only2. Eliminating the pumping load can improve overall efficiency and create opportunities for mobile applications. In this work, we demonstrate a 3D printed prototype of a pumpless non-aqueous organic RFB that induces flow in the electrolyte from sinusoidal rocking motion. The body of the flow cell was created using 3D printing, allowing us to modify and adapt geometry easily during testing. First, the compatibility of the 3D-printed material was studied by testing the chemical stability of widely available additive manufacturing materials under RFB conditions. Then, we evaluated the performance of this pumpless system using an easily scalable, soluble, and stable one electron donor phenothiazine derivative, N-(2-(2-methoxyethoxy)ethyl)phenothiazine (MEEPT) which has been widely studied for RFB applications3. We used 0.25 M MEEPT and its bis(trifluoromethanesulfonyl)imide radical cation salt (MEEPT-TFSI) as a redox-active couple in 0.5 M tetraethylammonium bis(trifluoromethanesulfonyl)imide (TEATFSI)/acetonitrile (MeCN). Our results suggest an inversely proportional empirical relationship between limiting current density and the frequency of sinusoidal motion due to varying mass transfer rates. After 100 cycles in this symmetric cell with an area specific resistance of 2.62 Ωcm2, we achieved a capacity retention of 63% and an average Coulombic efficiency of 96%, with minimal sign of decomposition of the redox couple when analyzed post-cell cycling. The results of this study can be used for 3D printing material selection in numerous electrochemical devices that use organic solvents, including flow cells, supercapacitors, and lithium-ion batteries. Using sinusoidal motion to drive electrolytes instead of a pump can increase the theoretical efficiency and decrease the overall size of a flow cell. This makes it attractive in wearable applications where biomechanical motion can be harnessed. 1 Wang, W. et al. Recent Progress in Redox Flow Battery Research and Development. Advanced Functional Materials 23, 970-986 (2013). https://doi.org:10.1002/adfm.201200694 2 Tian, C. H., Chein, R., Hsueh, K. L., Wu, C. H. & Tsau, F. H. Design and modeling of electrolyte pumping power reduction in redox flow cells. Rare Metals 30, 16-21 (2011). https://doi.org:10.1007/s12598-011-0229-1 3 Milshtein, J. D. et al. High current density, long duration cycling of soluble organic active species for non-aqueous redox flow batteries. Energy & Environmental Science 9, 3531-3543 (2016). https://doi.org:10.1039/C6EE02027E
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Arunagiri, Karthik, Andrew Jark-Wah Wong, Luis A. Briceno-Mena, Michael John Janik, Jose A. Romagnoli, and Christopher G. Arges. "Deconvolution of Charge-Transfer, Mass Transfer, and Ohmic Resistances of Phosphonic Acid-Sulfonic Acid Ionomer Binders in Electrochemical Hydrogen Pumps." ECS Meeting Abstracts MA2023-02, no. 39 (2023): 1928. http://dx.doi.org/10.1149/ma2023-02391928mtgabs.
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Ion-pair high-temperature polymer electrolyte membranes (HT-PEMs) paired with phosphonic acid ionomer electrode binders have substantially improved the performance of HT-PEM electrochemical hydrogen pumps (EHPs)1, 2 and fuel cells3. Recently, blending poly(pentafluorstyrene-co-tetrafluorostyrene phosphonic acid) (PTFSPA) with NafionTM improved ionomer conductivity under anhydrous conditions in the temperature range of 100 °C to 250 °C. Using the said polymer blend as an electrode binder resulted in a 2 W.cm-2 peak power density of fuel cells4 at 240 °C (a HT-PEM fuel cell record). However, much is still unknown about how phosphonic acid ionomers blended with perfluorosulfonic acid (PFSA) materials affect electrode kinetics and gas transport in porous electrodes. In this work, we studied the ionic conductivity, electrode kinetics, and gas transport resistance of 3 types of phosphonic acid ionomers, poly(vinyl phosphonic acid), poly(vinyl benzyl phosphonic acid) by themselves and when blended with Aquivion®. These studies were performed in the context of an EHP platform – both membrane electrode assemblies (MEAs) and interdigitated electrode arrays (IDAs) decorated with nanoscale platinum electrocatalysts with thin film ionomer electrolytes. For all phosphoric acid ionomer types, the addition of Aquivion® promoted ionic conductivity, hydrogen oxidation/evolution reaction kinetics (HOR/HER), and hydrogen gas permeability. Solid-state 31P NMR revealed that the addition of Aquivion® significantly reduced phosphate ester formation in phosphoric acid ionomers and this played a vital role in enhancing ionomer blend conductivity. Using the best blend variant, PTFSPA-Aquivion®, a remarkable EHP performance of 5.1 A.cm-2 at 0.4 V at T = 200 °C was attained. Density functional theory (DFT) simulations identified that phosphonic acids with electron-withdrawing moieties reduced the propensity of the phosphonic acid to adsorb to platinum electrocatalyst surfaces. All phosphonic acid ionomers are anticipated to have a greater affinity for adsorption on platinum when compared to sulphonic acid ionomers (PFSAs). The relative adsorption affiliation of the various phosphoric acid ionomers from DFT is consistent with an explanation that stronger anion-specific adsorption has a detrimental impact and is commensurate with experimentally obtained MEA charge-transfer kinetics. A machine learning-aided compositional model5 revealed that the addition of Aquivion® reduced activation and concentration overpotentials in EHP MEAs and improved exchange current density and diffusivity in EHP IDAs. Future work involves employing the EHPs in a real-world application for separating and compressing hydrogen from the natural gas mixture. References Venugopalan, G.; Bhattacharya, D.; Andrews, E.; Briceno-Mena, L.; Romagnoli, J.; Flake, J.; Arges, C. G., Electrochemical Pumping for Challenging Hydrogen Separations. ACS Energy Letters 2022, 7 (4), 1322-1329. Venugopalan, G.; Bhattacharya, D.; Kole, S.; Ysidron, C.; Angelopoulou, P. P.; Sakellariou, G.; Arges, C. G., Correlating high temperature thin film ionomer electrode binder properties to hydrogen pump polarization. Materials Advances 2021, 2 (13), 4228-4234. Atanasov, V.; Lee, A. S.; Park, E. J.; Maurya, S.; Baca, E. D.; Fujimoto, C.; Hibbs, M.; Matanovic, I.; Kerres, J.; Kim, Y. S., Synergistically integrated phosphonated poly(pentafluorostyrene) for fuel cells. Nat Mater 2021, 20 (3), 370-377. Lim, K. H.; Lee, A. S.; Atanasov, V.; Kerres, J.; Park, E. J.; Adhikari, S.; Maurya, S.; Manriquez, L. D.; Jung, J.; Fujimoto, C.; Matanovic, I.; Jankovic, J.; Hu, Z.; Jia, H.; Kim, Y. S., Protonated phosphonic acid electrodes for high power heavy-duty vehicle fuel cells. Nature Energy 2022, 7 (3), 248-259. Briceno-Mena, L. A.; Venugopalan, G.; Romagnoli, J. A.; Arges, C. G., Machine learning for guiding high-temperature PEM fuel cells with greater power density. Patterns 2021, 2 (2), 100187. Figure 1
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Otomo, Junichiro, Moe Okazaki, and Julián Andrés Ortiz Corrales. "Influence of Ionic and Electronic Transport Properties on Ammonia Electrochemical Synthesis in Protonic Ceramic Fuel Cells." ECS Meeting Abstracts MA2024-02, no. 48 (2024): 3475. https://doi.org/10.1149/ma2024-02483475mtgabs.
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Energy carriers play an important role in chemical energy storage and transport technology for effective hydrogen utilization. Ammonia is a carbon-free fuel and a promising energy carrier in terms of high energy density and easy liquefaction. Electrochemical synthesis provides an efficient method, and protonic ceramic fuel cells (PCFCs) can be applied to ammonia production (N2 + 3H2O → 2NH3 + 1.5O2). We reported that Fe-based electrode catalysts with a proton-conducting solid electrolyte improved the ammonia formation rate by the electrochemical promotion of catalysis (EPOC) (1-3). Ionic and electronic transports in PCFCs can affect the ammonia formation reaction. In this study, we investigate the correlation between the electrochemical synthesis of ammonia and the transport properties of proton, oxide ion, and hole in the PCFCs to clarify the ammonia formation reaction. BaCe0.9Y0.1O3−δ (BCY10) electrolyte-supported cells were used for all experiments. A Fe cathode was deposited as the ammonia-forming electrode. For hydrogen pumping mode, Pt was used as the anode, while for water electrolysis mode, an electrode based on BaCo0.4Fe0.4Zr0.1Y0.1O3−δ (BCFZY) was used instead due to its triple-conducting properties (4). Electrochemical testing was conducted at 600 °C in a double-chamber reactor with the cathodic atmosphere fixed as dry 50% H2/N2. The ammonia produced bubbled into a dilute sulfuric acid solution and was quantified using liquid chromatography. With all cells, both the ammonia formation rates and current densities were shown to increase with applied voltage (Fig.1a). Under the dry H2 condition in the anode, the ammonia formation rate was shown to exhibit a strong dependence on the applied voltage, reaching 10−8 mol s−1 cm−2. Meanwhile, the ammonia formation rates were comparatively lower for hydrated conditions, i.e., wet H2 and wet air with 3%H2O. On the contrary, the current density was found to be lowest for dry H2 and highest for wet air, with a six-fold difference between the two conditions. The Nernst–Planck–Poisson (NPP) model was used to investigate the defect transport across the electrolyte and elucidate the experimental results. The NPP model was discretized and numerically calculated by improving our previous work (5). However, due to the unavailability of required thermodynamic and transport parameters for BCY10, a set of parameters reported for BaZr0.8Y0.2O3−δ (BZY20) was used instead (6). The fluxes of protons, oxygen vacancies, and holes were calculated at 600 °C with an applied voltage of 1 V under varying atmospheres (Fig. 1b). The cathodic atmosphere was fixed as dry 50% H2/N2, while three anodic atmospheres were considered, dry H2, wet H2, and wet air, considering the experimental conditions in this study. It was observed that under wet H2 conditions, proton flux significantly dominated the defect transport, showing an increase with rising voltage. In contrast, both hole and oxygen vacancy fluxes remained relatively insignificant compared to the proton flux regardless of applied voltage. However, under dry conditions, the oxygen vacancy flux became notable in relation to the total current and increased with higher voltages. Furthermore, higher current densities were observed under wet H2 compared to those under dry H2, indicating that total current might not be the most important factor in ammonia production. The NPP-model predictions imply that a higher oxygen vacancy flux toward the cathode could promote ammonia formation as well as proton flux. Under wet air, the proton transport number considerably decreases on the anode side due to the formation of holes. Even though the current density is significantly high, most of it consists of leakage current, as holes are the dominant charge carriers. Acknowledgments This work was supported by JSPS KAKENHI Grant Numbers JP21H04938. References F. Kosaka, T. Nakamura, A. Oikawa, J. Otomo, ACS Sustainable Chem. Eng., 5(11), 10439-10446 (2017). C.-I. Li, H. Matsuo, J. Otomo, Sustainable Energy & Fuels, 5, 188-198 (2021). M. Okazaki, J. Otomo, ACS Omega, 8 (43), 40299-40308 (2023). C. Duan, J. Tong, M. Shang, S. Nikodemski, M. Sanders, S. Ricote, A. Almansoori, R. O’Hayre. Science, 349 (6254), 1321–1326 (2015). J. A. Ortiz Corrales, H. Matsuo, J. Otomo, ECS Trans., 103 (1) 1763-1777 (2021). H. Zhu, S. Ricote, C. Duan, R. P. O’Hayre, D. S. Tsvetkov, and R. J. Kee, J. Electrochem. Soc., 165(9), F581–F588 (2018). Figure 1
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Dogan, Deniz, Burkhard Hecker, Hermann Tempel, and Rüdiger-A. Eichel. "Experimental and Theoretical Investigations of Shunt Currents between Alkaline Water Electrolyzers." ECS Meeting Abstracts MA2023-02, no. 24 (2023): 1331. http://dx.doi.org/10.1149/ma2023-02241331mtgabs.
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A pivotal component of national climate strategies is the transition of the energy sector from fossil fuels to green energy. In this context, electrochemical processes will play a significant role in the future, requiring electrochemical systems with high efficiency and maximum system life cycles.1,2 For industrial electrochemical systems capital and operating costs are often reduced by a system design with a shared and circulating electrolyte supply providing ionically conductive cell-to-cell pathways. Under such conditions, parasitic ion migration occurs between adjacent cells, known as shunt currents.3,4 Shunt currents can have severe implications, such as decrease in faraday efficiency, material corrosion or interferences with instrumentation 3,5,6. To ensure high efficiency and maximum system life cycle, shunt current estimation is of high importance for the design of electrochemical multi-cell systems. A widely used approach in the literature is the theoretical, model-based approach using equivalent circuit models for shunt current determination7–9. Only a few publications demonstrate experimental determination methods 10,11. Furthermore, most shunt current studies in the field of electrochemistry focus on redox flow batteries. This work shows an innovative experimental approach for direct shunt current measurements between two alkaline water electrolysis cells with shared and circulating electrolyte feed under various conditions. The flow field design enables the insertion of reference electrodes into the flow cells for direct measurement of the potential differences between adjacent electrodes. Combined with the experimental data of the ionic tube resistances, the cell-to-cell shunt currents were accurately determined. Furthermore, an equivalent circuit model was created, fed with experimental data and validated with measured results. After successful validation the model was extended to electrolysis systems with more than two cells. Experimental data and simulations are in good agreement. The conducted experiments show the impact of temperature, cell voltage and tube manifold geometry on shunt current formation between alkaline water electrolyzers. Simulations performed are carried out to calculate shunt currents as a function of these parameters in large multi-cell systems. Furthermore, efficiency losses and corrosion processes as a result of shunt currents are estimated based on the results of this work. Literature Baños R, Manzano-Agugliaro F, Montoya FG, Gil C, Alcayde A, Gómez J. Optimization methods applied to renewable and sustainable energy: A review. Renew Sustain Energy Rev. 2011;15(4):1753-1766. doi:10.1016/j.rser.2010.12.008 Yan Z, Hitt JL, Turner JA, Mallouk TE. Renewable electricity storage using electrolysis. Proc Natl Acad Sci U S A. 2020;117(23):12558-12563. doi:10.1073/pnas.1821686116 Delgado NM, Monteiro R, Cruz J, Bentien A, Mendes A. Shunt currents in vanadium redox flow batteries – a parametric and optimization study. Electrochim Acta. 2022;403:139667. doi:10.1016/j.electacta.2021.139667 Kaminski EA, Savinell RF. A Technique for Calculating Shunt Leakage and Cell Currents in Bipolar Stacks Having Divided or Undivided Cells. J Electrochem Soc. 1983;130(5):1103-1107. doi:10.1149/1.2119891 Yin C, Guo S, Fang H, Liu J, Li Y, Tang H. Numerical and experimental studies of stack shunt current for vanadium redox flow battery. Appl Energy. 2015;151:237-248. doi:10.1016/j.apenergy.2015.04.080 Pletcher D, Walsh FC. Industrial Electrochemistry. Springer Science & Business Media; 2012. Schaeffer JA, Chen L Der, Seaba JP. Shunt current calculation of fuel cell stack using Simulink®. J Power Sources. 2008;182(2):599-602. doi:10.1016/j.jpowsour.2008.04.014 Wandschneider FT, Röhm S, Fischer P, Pinkwart K, Tübke J, Nirschl H. A multi-stack simulation of shunt currents in vanadium redox flow batteries. J Power Sources. 2014;261:64-74. doi:10.1016/j.jpowsour.2014.03.054 Ye Q, Hu J, Cheng P, Ma Z. Design trade-offs among shunt current, pumping loss and compactness in the piping system of a multi-stack vanadium flow battery. J Power Sources. 2015;296:352-364. doi:10.1016/j.jpowsour.2015.06.138 Rous̆ar I, Cezner V. Experimental Determination and Calculation of Parasitic Currents in Bipolar Electrolyzers with Application to Chlorate Electrolyzer. J Electrochem Soc. 1974;121(5):648. doi:10.1149/1.2401878 Fink H, Remy M. Shunt currents in vanadium flow batteries: Measurement, modelling and implications for efficiency. J Power Sources. 2015;284:547-553. doi:10.1016/j.jpowsour.2015.03.057
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Qiao, Jixin. "Dynamic Flow Approaches for Automated Radiochemical Analysis in Environmental, Nuclear and Medical Applications." Molecules 25, no. 6 (2020): 1462. http://dx.doi.org/10.3390/molecules25061462.
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Automated sample processing techniques are desirable in radiochemical analysis for environmental radioactivity monitoring, nuclear emergency preparedness, nuclear waste characterization and management during operation and decommissioning of nuclear facilities, as well as medical isotope production, to achieve fast and cost-effective analysis. Dynamic flow based approaches including flow injection (FI), sequential injection (SI), multi-commuted flow injection (MCFI), multi-syringe flow injection (MSFI), multi-pumping flow system (MPFS), lab-on-valve (LOV) and lab-in-syringe (LIS) techniques have been developed and applied to meet the analytical criteria under different situations. Herein an overall review and discussion on these techniques and methodologies developed for radiochemical separation and measurement of various radionuclides is presented. Different designs of flow systems with combinations of radiochemical separation techniques, such as liquid–liquid extraction (LLE), liquid–liquid microextraction (LLME), solid phase extraction chromatography (SPEC), ion exchange chromatography (IEC), electrochemically modulated separations (EMS), capillary electrophoresis (CE), molecularly imprinted polymer (MIP) separation and online sensing and detection systems, are summarized and reviewed systematically.
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Tanzharikov, P. A., Zh M. Omirzak, and Zh O. Abu. "ASSESSMENT OF CORROSION DAMAGE TO OIL-WELL TUBING IN MINERAL ENVIRONMENTS." ТЕХНИКА ҒЫЛЫМДАРЫ ЖӘНЕ ТЕХНОЛОГИЯ 3 (2023): 26–34. http://dx.doi.org/10.52081/tst.2023.v03.i3.022.
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The state of oil production technology and engineering, especially in the conditions of well operation with complex aggressive environment, requires solutions that allow to improve productivity processes without maximising costs. One of the reasons reducing effective well performance can be attributed to the formation of a corrosion layer formed on the surface of oilfield equipment. Mineral salts in formation waters together with other non-carbons form electrochemical corrosion activity on the surface structure of metal. As a result, there is a decrease in the strength of the metal of the tubing pipes in the well, the formation of cracks in the threads, as well as a decrease or complete loss of productivity. The effects of corrosion on pumping units can lead to emergency situations at oil production facilities. Currently, at the Kumkol oil field, the issue of increasing the strength of production equipment when working in conditions with high water content and mineral salt content in the composition has not lost its relevance. The purpose of this article is to determine a method for carrying out a set of anti-corrosion measures in the region with the destruction of metal tubing pipes and well pumps based on monitoring technological processes at oil enterprises.
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Hsu, Po Ching (Eric), Bo Yang, G. K. Surya G. K. Prakash, and Sri Narayan. "All Organic Quinone Solid State Batteries for Environmentally Friendly and Chemical Robust Alternatives Beyond Lithium-Ion Batteries." ECS Meeting Abstracts MA2024-01, no. 1 (2024): 37. http://dx.doi.org/10.1149/ma2024-01137mtgabs.
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Introduction: Organic solid-state quinone batteries have unparalleled properties that can meet the most urgent challenges the industry faces. It can create an energy system that is environmentally friendly and electrochemically robust, while being cost efficient enough for industry to adopt and invest in. The inspiration for fully organic solid-state batteries came from extended studies on our all-organic aqueous redox flow batteries, where much of the science of organic redox coupling molecules were understood. Like redox flow batteries, organic solid state quinone batteries utilizes the breaking and reforming of bonds to generate electrical energy. However, it doesn’t require the constant flow of charge carrier solution like the flow batteries. Consequently, this avoids the cost of an extra pumping system and significantly reduce the size of the batteries compared to flow battery systems. Furthermore, the downsized battery system allows for the cell to be implemented into applications such as EV and portable devices. The redox species are directly deposited onto the electrodes. This deposition of active material on carbon paper enables higher surface area for charge transfer, which increases the capacity for fast charge and discharge compared to flow batteries. Additionally, the active materials are of organic quinone nature providing great robustness that other battery systems like lithium-ion batteries don’t allow. The redox chemistry of these quinones still happens in aqueous system, which allows us to use very small amount of aqueous electrolyte instead of the combustible organic solvent used in lithium batteries. Results and discussion: The appropriate quinone species for this solid-state battery must be electrochemically stable and dissolution free in the aqueous system. Various quinones with different substituents were tested. One of the promising redox couples discovered is 2-methylanthraquinone (MAQ) and duroquinone (DQ). The couple displayed a cell voltage of 400 mV (0.4 V) as shown in Figure 1. This value was found to correspond to the redox potential difference between DQ and MAQ. New methods of deposition of active materials onto the electrodes were developed. High conductivity was achieved by introducing CNT with appropriate binder, which resulted in improvements to the cell’s charge and discharge performance (Figure 2). Figure 1. Cyclic voltammetry study of 10 mM 2-Methylanthraquinone (MAQ) and 10 mM Duroquinone (DQ) in 1 M sulfuric acid with 20% ethanol, MSE reference electrode, glassy carbon, 50 mV/s. (Refer to image file) Figure 2: Charge and discharge of solid-state batteries of 2-Methylanthraquinone (MAQ) and Duroquinone (DQ) at 10 mA. (Refer to image file) For the positive side, 0.164 g of duroquinone was deposited on 25 cm2 carbon paper with 0.05 g of CNT. Correspondingly, 0.222 g of 2-Methylantroquinone was deposited for the negative side. The cell was assembled with Nafion 117 as separator and small amount of 1 M sulfuric acid as the supporting electrolyte. The initial charge and discharge curve of this cell showed 97% columbic efficiency. Long-term cycling to test the stability was performed and other redox couples also showed higher cell voltage with high efficiency. The next step for this study is to explore different redox couples that might have better compatibility and higher cell voltage compared to the current redox couple. This will be done through studying the large library of organic compounds including quinones and other redox active organic compounds. Figure 1
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Cleis, Santos, and La Mantia Fabio. "Recent advances in reactor design and control for lithium recovery by means of electrochemical ion pumping." July 17, 2022. https://doi.org/10.1016/j.coelec.2022.101089.
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The necessity to tap new natural lithium sources worldwide has pushed in recent years the research in alternative methods for lithium recovery. Among them, electrochemical ion pumping is showing interesting performances, especially when addressing diluted sources. In this review, we summarize the recent advances in materials' and reactors’ design for lithium recovery by means of electrochemical ion pumping. We discuss simulations and modeling studies as a tool to study limitations and to provide improved engineering designs. In addition, we provide parameters based on lithium removal and energy consumption for a fair comparison among different ion pumping strategies. Accordingly, we stress the importance to report not only on lithium removal metrics, but also purity and energy-related parameters to provide an optimal assessment of this technology. Finally, remaining challenges and perspectives guidelines are included for future ion-pumping developments.
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Sasaki, Kazuya, Kiyoto Shin-mura, Shunsuke Honda, Hirofumi Tazoe, and Eiki Niwa. "A three-electrode dual-power-supply electrochemical pumping system for fast and energy efficient lithium extraction and recovery from solutions." Communications Engineering 3, no. 1 (2024). http://dx.doi.org/10.1038/s44172-024-00174-8.
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AbstractThe demand for Li-ion batteries (LIBs) for use in electric vehicles, which is key to realizing a decarbonized society, is accelerating. However, the supply of Li resources has recently become a major issue, thereby necessitating the development of economical and sustainable technologies of brine/seawater-based Li extraction and recycling Li from spent LIBs. This paper presents an innovative electrochemical pumping technology based on a new cell structure for Li extraction/recovery. This system can provide large electrochemical driving forces while preventing the occurrence of electronic conduction due to electrolyte reduction. This electrochemical pumping system allows extraction/recovery of Li ions from the anode side to the cathode side, rather than the diffusion of other ions, due to the ion-diffusion-bottleneck size of the electrolyte material. Using this system, high-purity Li can be collected with high energy efficiency and at least 464 times faster than that via conventional electrochemical pumping, even with a commercially available Li-ion electrolyte plate.
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Pérez-Antolín, Daniel, Cristina Irastorza, Sara González, et al. "Regenerative electrochemical ion pumping cell based on semi-solid electrodes for sustainable Li recovery." Desalination 533 (April 12, 2022). https://doi.org/10.1016/j.desal.2022.115764.
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Demand of lithium is expected to increase drastically in coming years driven by the market penetration of electric vehicles powered by Li-ion batteries, which will require faster and more efficient Li extraction technologies than conventional ones (evaporation in brines). The Electrochemical Ion Pumping Cell (EIPC) technology based on the use of Faradaic materials is one of the most promising approaches. However, its relatively short lifespan prevents its commercial deployment. Herein, a new EIPC concept based on the use of semi-solid electrodes is proposed for the first time, which takes advantage of the rheological characteristics of semi-solid electrodes that enable simple and cheap regeneration of the Regenerative Electrochemical Ion Pumping Cell (REIPC) systems after reaching its end-of-life. A proof-of-concept for REIPC is accomplished by simple replacement of the semi-solid electrode demonstrating a remarkable electrochemical performance (e.g. 99.87%cycle−1, 99.98%h−1, 3–4 mAh cm−2) along with a competitive ion separation (e.g. 16.2 mgLi·gNiHCF−1, 4 gLi m−2 and 15.6 Wh·mol−1). The use of semi-solid electrode offers other unique features such as a significant cost reduction of 95% for every regeneration regarding conventional EIPC, proving that REIPC concept successfully addresses the issues associated to the sustainability and recyclability of the conventional EIPC's for lithium capturing.
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Xu, Longqian, Weifan Liu, Xudong Zhang, et al. "Pseudo-continuous and scalable electrochemical ion pumping with circuit-switching-induced ion shuttling." Nature Water, October 1, 2024. http://dx.doi.org/10.1038/s44221-024-00312-8.
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Kumar, Anuj, Jennifer Roth, Hyunho Kim, et al. "Molecular principles of redox-coupled sodium pumping of the ancient Rnf machinery." Nature Communications 16, no. 1 (2025). https://doi.org/10.1038/s41467-025-57375-8.
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Abstract The Rnf complex is the primary respiratory enzyme of several anaerobic prokaryotes that transfers electrons from ferredoxin to NAD+ and pumps ions (Na+ or H+) across a membrane, powering ATP synthesis. Rnf is widespread in primordial organisms and the evolutionary predecessor of the Na+-pumping NADH-quinone oxidoreductase (Nqr). By running in reverse, Rnf uses the electrochemical ion gradient to drive ferredoxin reduction with NADH, providing low potential electrons for nitrogenases and CO2 reductases. Yet, the molecular principles that couple the long-range electron transfer to Na+ translocation remain elusive. Here, we resolve key functional states along the electron transfer pathway in the Na+-pumping Rnf complex from Acetobacterium woodii using redox-controlled cryo-electron microscopy that, in combination with biochemical functional assays and atomistic molecular simulations, provide key insight into the redox-driven Na+ pumping mechanism. We show that the reduction of the unique membrane-embedded [2Fe2S] cluster electrostatically attracts Na+, and in turn, triggers an inward/outward transition with alternating membrane access driving the Na+ pump and the reduction of NAD+. Our study unveils an ancient mechanism for redox-driven ion pumping, and provides key understanding of the fundamental principles governing energy conversion in biological systems.
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Hau, Jann-Louis, Susann Kaltwasser, Valentin Muras, et al. "Conformational coupling of redox-driven Na+-translocation in Vibrio cholerae NADH:quinone oxidoreductase." Nature Structural & Molecular Biology, September 14, 2023. http://dx.doi.org/10.1038/s41594-023-01099-0.
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AbstractIn the respiratory chain, NADH oxidation is coupled to ion translocation across the membrane to build up an electrochemical gradient. In the human pathogen Vibrio cholerae, the sodium-pumping NADH:quinone oxidoreductase (Na+-NQR) generates a sodium gradient by a so far unknown mechanism. Here we show that ion pumping in Na+-NQR is driven by large conformational changes coupling electron transfer to ion translocation. We have determined a series of cryo-EM and X-ray structures of the Na+-NQR that represent snapshots of the catalytic cycle. The six subunits NqrA, B, C, D, E, and F of Na+-NQR harbor a unique set of cofactors that shuttle the electrons from NADH twice across the membrane to quinone. The redox state of a unique intramembranous [2Fe-2S] cluster orchestrates the movements of subunit NqrC, which acts as an electron transfer switch. We propose that this switching movement controls the release of Na+ from a binding site localized in subunit NqrB.
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Row, Hyeongjoo, Joshua B. Fernandes, Kranthi K. Mandadapu, and Karthik Shekhar. "Spatiotemporal dynamics of ionic reorganization near biological membrane interfaces." Physical Review Research 7, no. 1 (2025). https://doi.org/10.1103/physrevresearch.7.013185.
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Electrical signals in excitable cells involve spatially localized ionic fluxes through ion channels and pumps on cellular lipid membranes. Common approaches to understand how these fluxes spread assume that the membrane and the surrounding electrolyte comprise an equivalent circuit of capacitors and resistors, which ignores the localized nature of transmembrane ion transport, the resulting ionic gradients and electric fields, and their spatiotemporal relaxation. Here, we consider a model of localized ion pumping across a lipid membrane, and use theory and simulation to investigate how the electrochemical signal propagates spatiotemporally in and out of plane along the membrane. The localized pumping generates long-ranged electric fields with three distinct scaling regimes along the membrane: a constant potential near-field region, an intermediate monopolar region, and a far-field dipolar region. Upon sustained pumping, the monopolar region expands radially in plane with a steady speed that is enhanced by the dielectric mismatch and the finite thickness of the lipid membrane. For unmyelinated lipid membranes in physiological settings, we find remarkably fast propagation speeds of ∼40m/s, allowing faster ionic reorganization compared to bare diffusion. Together, our paper shows that transmembrane ionic fluxes induce transient long-ranged electric fields in electrolyte solutions, which may play hitherto unappreciated roles in biological signaling. Published by the American Physical Society 2025
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Chen, Wei, Yin Hu, Weiqiang Lv, et al. "Lithiophilic montmorillonite serves as lithium ion reservoir to facilitate uniform lithium deposition." Nature Communications 10, no. 1 (2019). http://dx.doi.org/10.1038/s41467-019-12952-6.
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Abstract The growing demand for lithium batteries with higher energy densities requires new electrode chemistries. Lithium metal is a promising candidate as the anode material due to its high theoretical specific capacity, negative electrochemical potential and favorable density. However, during cycling, low and uneven lithium ion concentration on the surface of anode usually results in uncontrolled dendrite growth, especially at high current densities. Here we tackle this issue by using lithiophilic montmorillonite as an additive in the ether-based electrolyte to regulate the lithium ion concentration on the anode surface and thus facilitate the uniform lithium deposition. The lithiophilic montmorillonite demonstrates a pumping feature that improves the self-concentrating kinetics of the lithium ion and thus accelerates the lithium ion transfer at the deposition/electrolyte interface. The signal intensity of TFSI− shows negligible changes via in situ Raman tracking of the ion flux at the electrochemical interface, indicating homogeneous ion distribution, which can lead to a stable and uniform lithium deposition on the anode surface. Our study indicates that the interfacial engineering induced by the lithiophilic montmorillonite could be a promising strategy to optimize the lithium deposition for next-generation lithium metal batteries.
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"A NMR Study of Sodium/Potassium Pumping System in the Node of Ranvier Myelin-Sheath." Biointerface Research in Applied Chemistry 11, no. 6 (2021): 14260–77. http://dx.doi.org/10.33263/briac116.1426014277.
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The QM/MM calculation has been applied to generalize the node of Ranvier results for computing action potentials and electrochemical behavior of membranes that agree with clusters of voltage-gated ion sodium and potassium channels. Ranvier complexes' node is an accurate organization of membrane-bound aqueous boxes. The model applied here shows an electrophysiological phenomenon with simulated structural and physiological data. The quantum effects of various thicknesses in a selected membrane of Galc /DMPC and Galc/NPGS have also been specifically investigated. This allows introducing a capacitive susceptibility that can resonate with the self-induction of helical coils or ion channels, the resonance of which is the main reason for various biological pulses.
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Xiong, Ningxin, Wenqiang Luo, Quan Lan, and Qixing Wu. "Slurry Based Lithium-Ion Flow Battery with a Flow Field Design." Journal of The Electrochemical Society, June 9, 2023. http://dx.doi.org/10.1149/1945-7111/acdd23.
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Abstract Slurry based lithium-ion flow batteries have been regarded as an emerging electrochemical system to obtain a high energy density and design flexibility for energy storage. The coupling nature of electrode thickness and flow resistance in previous slurry flow cell designs demands a nuanced balance between power output and auxiliary pumping. To address this issue, a slurry based lithium-ion flow battery featuring a serpentine flow field and a stationary porous carbon felt current collector is proposed. The carbon felt serves to provide a stable and efficient pathway for electron transport, while the flow field helps distribute active slurry onto the felt for electrochemical reactions. With such a design, the LiFePO4 (LFP) slurry-based flow battery shows a low flow resistance and good flow stability without forming severe filter cakes on the felt surface, similar to cross-flow filtration. A maximum power density of 84.5 mW cm-2 and a stable coulombic efficiency of ~98% under intermittent flow, and a specific capacity of 164.87 mAh g-1 (based on the total LFP in the tank) in continuous flow are successfully demonstrated. These preliminary yet encouraging results may put forward new avenues for future structural design and optimization of slurry based flow batteries.
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Zhao, Rui, Jie Liu, and Fai Ma. "Cathode Chemistries and Electrode Parameters Affecting the Fast Charging Performance of Li-Ion Batteries." Journal of Electrochemical Energy Conversion and Storage 17, no. 2 (2020). http://dx.doi.org/10.1115/1.4045567.
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Abstract Li-ion battery fast-charging technology plays an important role in popularizing electric vehicles (EV), which critically need a charging process that is as simple and quick as pumping fuel for conventional internal combustion engine vehicles. To ensure stable and safe fast charging of Li-ion battery, understanding the electrochemical and thermal behaviors of battery electrodes under high rate charges is crucial, since it provides insight into the limiting factors that restrict the battery from acquiring energy at high rates. In this work, charging simulations are performed on Li-ion batteries that use the LiCoO2 (LCO), LiMn2O4 (LMO), and LiFePO4 (LFP) as the cathodes. An electrochemical-thermal coupling model is first developed and experimentally validated on a 2.6Ah LCO based Li-ion battery and is then adjusted to study the LMO and LFP based batteries. LCO, LMO, and LFP based Li-ion batteries exhibited different thermal responses during charges due to their different entropy profiles, and results show that the entropy change of the LCO battery plays a positive role in alleviating its temperature rise during charges. Among the batteries, the LFP battery is difficult to be charged at high rates due to the charge transfer limitation caused by the low electrical conductivity of the LFP cathode, which, however, can be improved through doping or adding conductive additives. A parametric study is also performed by considering different electrode thicknesses and secondary particle sizes. It reveals that the concentration polarization at the electrode and particle levels can be weaken by using thin electrodes and small solid particles, respectively. These changes are helpful to mitigate the diffusion limitation and improve the performance of Li-ion batteries during high rate charges, but careful consideration should be taken when applying these changes since they can reduce the energy density of the batteries.
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Manoj, Kelath Murali, Laurent Jaeken, Nikolai Mikhailovich Bazhin, Hirohisa Tamagawa, Mahendra Kavdia, and Afsal Manekkathodi. "Murburn concept in cellular function and bioenergetics, Part 1: Understanding murzymes at the molecular level." AIP Advances 13, no. 12 (2023). http://dx.doi.org/10.1063/5.0171857.
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Bioenergetics is the study of how life-activities are powered within the cell. This also deals with the interactive exchange of matter/radiation between cellular components and their environment, and the accompanying changes thereof. The acclaimed bioenergetics paradigm has relied on “electron transport chains” and selective/stoichiometric electrogenic “ion-pumping” mediated by vectorial protein-embedded membranes. Therein, an electrochemical gradient was deemed to be the driving force for chemical reactions leading to ATP production, physical thermogenesis by uncoupling proteins, and complex electromechanical processes like information relay along the axon. On one hand, this vitally deterministic perception requires the membrane proteins to “intelligently” manipulate ion-fluxes and generate/harness an electrochemical gradient by a gambit-type logic. At the other hand, it also seeks that the same gradient should cyclically control the membrane-proteins’ activity. Our recent pursuits have questioned such traditional perspectives and advocated the alternate explanation of murburn concept, leading to a revamping of the macroscopic treatments of overall thermodynamic, kinetic, mechanistic, and evolutionary (probability) considerations. The current review aims to consolidate the murburn paradigm of bioenergetics, wherein murzymes initiate redox processes by effective charge separation and diffusible reactive species formation, enabling cells to work as simple chemical engines. Herein, we discuss the reaction chemistry of some simple enzyme systems and also delve into protein complex arrays mediated powering routines like mitochondrial respiration-thermogenesis and chloroplast-centered photosynthesis. Furthermore, we remark that the “water–ion–molecules” phase continuum is actually discretized into dynamically fluctuating coacervates and express concern over the marginalization of sound chemico-physical ideas by the bioenergetics community.