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Published: 25 May 2024

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1

Hoffman, Zach J., Alec S. Ho, Saheli Chakraborty, and Nitash P. Balsara. "Limiting Current Density in Single-Ion-Conducting and Conventional Block Copolymer Electrolytes." Journal of The Electrochemical Society 169, no. 4 (April 1, 2022): 043502. http://dx.doi.org/10.1149/1945-7111/ac613b.

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The limiting current density of a conventional polymer electrolyte (PS-PEO/LiTFSI) and a single-ion-conducting polymer electrolyte (PSLiTFSI-PEO) was measured using a new approach based on the fitted slopes of the potential obtained from lithium-polymer-lithium symmetric cells at a constant current density. The results of this method were consistent with those of an alternative framework for identifying the limiting current density taken from the literature. We found the limiting current density of the conventional electrolyte is inversely proportional to electrolyte thickness as expected from theory. The limiting current density of the single-ion-conducting electrolyte was found to be independent of thickness. There are no theories that address the dependence of the limiting current density on thickness for single-ion-conducting electrolytes.
2

Issa, Sébastien, Roselyne Jeanne-Brou, Sumit Mehan, Didier Devaux, Fabrice Cousin, Didier Gigmes, Renaud Bouchet, and Trang N. T. Phan. "New Crosslinked Single-Ion Silica-PEO Hybrid Electrolytes." Polymers 14, no. 23 (December 6, 2022): 5328. http://dx.doi.org/10.3390/polym14235328.

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New single-ion hybrid electrolytes have been synthetized via an original and simple synthetic approach combining Michael addition, epoxidation, and sol–gel polycondensation. We designed an organic PEO network as a matrix for the lithium transport, mechanically reinforced thanks to crosslinking inorganic (SiO1.5) sites, while highly delocalized anions based on lithium vinyl sulfonyl(trifluoromethane sulfonyl)imide (VSTFSILi) were grafted onto the inorganic sites to produce single-ion hybrid electrolytes (HySI). The influence of the electrolyte composition in terms of the inorganic/organic ratio and the grafted VSTFSILi content on the local structural organization, the thermal, mechanical, and ionic transport properties (ionic conductivity, transference number) are studied by a variety of techniques including SAXS, DSC, rheometry, and electrochemical impedance spectroscopy. SAXS measurements at 25 °C and 60 °C reveal that HySI electrolyte films display locally a spatial phase separation with domains composed of PEO rich phase and silica/VSTFSILi clusters. The size of these clusters increases with the silica and VSTFSILi content. A maximum ionic conductivity of 2.1 × 10−5 S·cm−1 at 80 °C has been obtained with HySI having an EO/Li ratio of 20. The Li+ ion transfer number of HySI electrolytes is high, as expected for a single-ion electrolyte, and comprises between 0.80 and 0.92.
3

Dong, Xu, Dominik Steinle, and Dominic Bresser. "Single-Ion Conducting Polymer Electrolytes for Sodium Batteries." ECS Meeting Abstracts MA2023-01, no. 5 (August 28, 2023): 954. http://dx.doi.org/10.1149/ma2023-015954mtgabs.

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Sodium-ion batteries have attracted extensive attention recently owing to the announcements of several companies to commercialize this technology in the (very) near future. Just like commercial lithium-ion batteries, though, these batteries are comprising and/or will comprise a liquid electrolyte – with all its advantages and challenges. Thinking one step ahead (as also done by a few companies already), the next step might be the transition to (“zero-excess”) sodium-metal batteries, which will require fundamentally new electrolyte solutions, and just like for lithium-metal batteries, these might be based, e.g., on polymers. Herein, we present our latest results on single-ion conducting polymer electrolytes for sodium-metal batteries. These polymer electrolytes do not only show higher ionic conductivity than its lithium analogues (>2.5 mS cm-1 at 40 °C), but moreover the same beneficial properties in terms of high electrochemical stability towards oxidation, highly reversible sodium plating and stripping, and excellent cycling stability of Na‖Na3V2(PO4)3 cells for more than 500 cycles. The results thus show that single-ion conducting polymer electrolytes are very promising candidates for high-performance sodium batteries.
4

Ghorbanzade, Pedram, Laura C. Loaiza, and Patrik Johansson. "Plasticized and salt-doped single-ion conducting polymer electrolytes for lithium batteries." RSC Advances 12, no. 28 (2022): 18164–67. http://dx.doi.org/10.1039/d2ra03249j.

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5

Park, Habin, Anthony Engler, Nian Liu, and Paul Kohl. "Dynamic Anion Delocalization of Single-Ion Conducting Polymer Electrolyte for High-Performance of Solid-State Lithium Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 3 (October 9, 2022): 227. http://dx.doi.org/10.1149/ma2022-023227mtgabs.

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Lithium metal batteries (LMBs) have been considered as next-generation energy storages due to their extremely high theoretical specific capacity (3860 mAh g-1). However, current LMBs, using conventional liquid electrolytes, still could not fulfill the demand of soaring expansion of energy era, such as electrical vehicles, because of their safety issues, originated by uncontrollable electrolytic side reaction on the lithium, resulting unstable solid-electrolyte interphase (SEI) and vicious lithium dendritic growth [1]. Also, carbonate-based liquid electrolytes have an intrinsic flammability, and the lithium dendrite, which short-circuits a cell, can lead to severe safety hazard with the unfavorable flammability of current liquid system when they are ignited. Therefore, solid-state electrolytes have been spotlighted recently for a pathway for safe, and high energy and power LMBs, due to their superior thermal stability and low vapor pressure, while maintaining suitable electrolytic performances. In this study, solid-state single-ion conducting polymer electrolytes (SICPEs), utilizing dynamic anion delocalization (DAD), realizing high ionic conductivity and dimensional stability for high-performance LMB, are studied. The SICPEs enable superior lithium transference number, resulting in highly reduced concentration gradient of lithium cation along the electrolyte to suppress the undesirable lithium dendritic growth. However, SICPEs have prominently lower ionic conductivity than dual-ion conducting polymer electrolyte (DICPEs), which is a critical issue to make a slower charge/discharge for SICPEs [2]. Although an approach utilizing gel polymer electrolyte (GPE), using a liquid solvent as a plasticizer, has been exploited to increase the ionic conductivity of SICPEs, GPEs have struggled with lower mechanical stability, compared to solid state, and still existing flammability issue with the plasticizer. The novel plasticizer, which is described here, can interact with bulky anionic polymer matrix, so that the negative charge can be dispersed onto the whole complex by DAD. Once the bulky complex is formed by DAD, the dissociation of lithium cation from anionic matrix can be easier with the decreased activation energy and higher ionic conduction. While increasing the ionic conductivity with DAD, the nature of polymeric plasticizer will highly suppress flammability. DAD allows the membrane endure more tensile strength due to the dynamic structural change in crosslinking state, so that the polymer electrolyte can tolerate dendritic growth of lithium by morphological change on an electrode surface. The obvious advantages of DAD-induced solid polymer electrolytes in this study for a high energy and power, and ultra-safe LMB can present a novel approach of polymer electrolyte design to the astronomical demand of energy storages. [1] F. Ahmed, I. Choi, M.M. Rahman, H. Jang, T. Ryu, S. Yoon, L. Jin, Y. Jin, W. Kim, ACS Appl. Mater. Interfaces 2019, 11, 34930-34938. [2] D.-M. Shin, J.E. Bachman, M.K. Taylor, J. Kamcev, J.G. Park, M.E. Ziebel, E. Velasquez, N.N. Jarenwattananon, G.K. Sethi, Y. Cui, J.R. Long, Adv. Mater. 2020, 32, 1905771.
6

Ock, Jiyoung, Anisur Rahman, Catalin Gainaru, Alexei Sokolov, and Xi Chen. "Ion Transport in Polymer/Inorganic Composite Electrolytes – a Comparison between Broadband Dielectric Spectroscopy and Impedance Spectroscopy." ECS Meeting Abstracts MA2023-01, no. 7 (August 28, 2023): 2886. http://dx.doi.org/10.1149/ma2023-0172886mtgabs.

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Significant efforts have been made to develop composite electrolytes combining polymer matrix with Li-ion conducting inorganic solids for feasible construction of solid-state batteries. However, the Li-ion transfer kinetics at the interface between polymer/inorganic electrolyte is unfavorable for Li-ion conduction in the composite electrolyte because of the interfacial resistance and the activation energy barrier for interfacial Li-ion transfer. The activation energy barrier for the Li-ion transfer reaction at the interface is correlated with the interaction between Li-ion and polymer matrix in the polymer electrolyte, interaction between Li-ion and anions in inorganic electrolytes and the interaction between polymer and inorganic electrolytes, therefore, the electrolyte composition significantly affects the interfacial charge transfer kinetics in composites. In this work, Li-ion transport properties in the composite electrolytes are investigated by using broadband dielectric spectroscopy (BDS) and impedance spectroscopy (IS). We particularly focus on Li-ion charge transfer at the polymer/inorganic interface from the dual ion conducting polymer to the single ion conducting polymer electrolytes with different Li-ion conducting salts such as LiN(SO2CF3)2 (LiTFSI) and (LiMTFSI) in vinyl ethylene carbonate (VEC) or polymerized vinyl ethylene carbonate (PVEC). The interfacial resistances of inorganic electrolytes Li0.34La0.56TiO3 (LLTO) in polymer electrolytes are elucidated. To further evaluate the polymer/inorganic electrolyte interfaces, various types of cell are assembled in a glove box filled with argon gas and characterized by a series of techniques such as BDS and IS. The Li-ion transfer kinetics at the interface significantly affects the Li-ion flux through the composite electrolytes and will be presented. In addition, we will present a systematic comparison between BDS and IS results in order to build connections between the two communities. Acknowledgements This work was supported as part of the Fast and Cooperative Ion Transport in Polymer-Based Materials (FaCT), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences at Oak Ridge National Laboratory under contract DE-AC05-00OR22725.
7

Badi, Nacer, Azemtsop Manfo Theodore, Saleh A. Alghamdi, Hatem A. Al-Aoh, Abderrahim Lakhouit, Pramod K. Singh, Mohd Nor Faiz Norrrahim, and Gaurav Nath. "The Impact of Polymer Electrolyte Properties on Lithium-Ion Batteries." Polymers 14, no. 15 (July 30, 2022): 3101. http://dx.doi.org/10.3390/polym14153101.

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In recent decades, the enhancement of the properties of electrolytes and electrodes resulted in the development of efficient electrochemical energy storage devices. We herein reported the impact of the different polymer electrolytes in terms of physicochemical, thermal, electrical, and mechanical properties of lithium-ion batteries (LIBs). Since LIBs use many groups of electrolytes, such as liquid electrolytes, quasi-solid electrolytes, and solid electrolytes, the efficiency of the full device relies on the type of electrolyte used. A good electrolyte is the one that, when used in Li-ion batteries, exhibits high Li+ diffusion between electrodes, the lowest resistance during cycling at the interfaces, a high capacity of retention, a very good cycle-life, high thermal stability, high specific capacitance, and high energy density. The impact of various polymer electrolytes and their components has been reported in this work, which helps to understand their effect on battery performance. Although, single-electrolyte material cannot be sufficient to fulfill the requirements of a good LIB. This review is aimed to lead toward an appropriate choice of polymer electrolyte for LIBs.
8

Ma, Peiyuan, Priyadarshini Mirmira, and Chibueze Amanchukwu. "Co-Intercalation-Free Fluorinated Ether Electrolytes for Lithium-Ion Batteries." ECS Meeting Abstracts MA2023-01, no. 2 (August 28, 2023): 550. http://dx.doi.org/10.1149/ma2023-012550mtgabs.

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Lithium-ion batteries are widely used to power portable electronics because of their high energy densities and have shown great promise in enabling the electrification of transport. However, the commercially used carbonate-based electrolytes are limited by a narrow operating temperature window and suffer against next generation lithium-ion battery chemistries such as silicon-containing anodes. The lack of non-carbonate electrolyte alternatives such as ether-based electrolytes is due to undesired solvent co-intercalation that occurs with graphitic anodes. Recently, fluorinated ether solvents have become promising electrolyte solvent candidates for lithium metal batteries but their applications in other battery chemistries have not been studied. In this work, we synthesize a group of novel fluorinated ether solvents and study them as electrolyte solvents for lithium-ion batteries. Using X-ray diffraction (XRD) and solid-state nuclear magnetic resonance (ssNMR), we show that fluorinated ether electrolytes support reversible lithium-ion intercalation into graphite without solvent co-intercalation at conventional salt concentrations. To the best of our knowledge, they are the first class of ether solvents that intrinsically suppress solvent co-intercalation without the need for high or locally high salt concentration. In full cells using graphite anode, fluorinated ether electrolytes enable much higher energy densities compared to conventional glyme ethers, and better thermal stability over carbonate electrolytes (operation up to 60°C). As single-solvent-single-salt electrolytes, they remarkably outperform carbonate electrolytes with fluoroethylene carbonate (FEC) and vinylene carbonate (VC) additives when cycled with graphite-silicon composite anodes. Using X-ray photoelectron spectroscopy (XPS), NMR and density functional theory (DFT) calculations, we show that fluorinated ethers produce a solvent-derived solid electrolyte interphase, which is likely the key to suppressing solvent co-intercalation. Rational molecular design of fluorinated ether solvents will produce novel electrolytes that enable next generation lithium-ion batteries with higher energy density and wider working temperature window.
9

Zhang, Heng, Chunmei Li, Michal Piszcz, Estibaliz Coya, Teofilo Rojo, Lide M. Rodriguez-Martinez, Michel Armand, and Zhibin Zhou. "Single lithium-ion conducting solid polymer electrolytes: advances and perspectives." Chemical Society Reviews 46, no. 3 (2017): 797–815. http://dx.doi.org/10.1039/c6cs00491a.

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Single lithium-ion conducting solid polymer electrolytes (SLIC-SPEs), with a high lithium-ion transference number, the absence of the detrimental effect of anion polarization, and low dendrite growth rate, could be an excellent choice of safe electrolyte materials for lithium batteries in the future.
10

Villaluenga, Irune, Kevin H. Wujcik, Wei Tong, Didier Devaux, Dominica H. C. Wong, Joseph M. DeSimone, and Nitash P. Balsara. "Compliant glass–polymer hybrid single ion-conducting electrolytes for lithium batteries." Proceedings of the National Academy of Sciences 113, no. 1 (December 22, 2015): 52–57. http://dx.doi.org/10.1073/pnas.1520394112.

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Despite high ionic conductivities, current inorganic solid electrolytes cannot be used in lithium batteries because of a lack of compliance and adhesion to active particles in battery electrodes as they are discharged and charged. We have successfully developed a compliant, nonflammable, hybrid single ion-conducting electrolyte comprising inorganic sulfide glass particles covalently bonded to a perfluoropolyether polymer. The hybrid with 23 wt% perfluoropolyether exhibits low shear modulus relative to neat glass electrolytes, ionic conductivity of 10−4 S/cm at room temperature, a cation transference number close to unity, and an electrochemical stability window up to 5 V relative to Li+/Li. X-ray absorption spectroscopy indicates that the hybrid electrolyte limits lithium polysulfide dissolution and is, thus, ideally suited for Li-S cells. Our work opens a previously unidentified route for developing compliant solid electrolytes that will address the challenges of lithium batteries.
11

Engler, Anthony, Habin Park, Nian Liu, and Paul Kohl. "Cyclic Carbonate-Based, Single-Ion Conducting Polymer Electrolytes for Li-Ion Batteries: Electrolyte Design." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 2437. http://dx.doi.org/10.1149/ma2022-0122437mtgabs.

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Solid polymer electrolytes (SPEs) have been the focus of study to address Li-ion battery issues including thermal runaway by mitigating the danger from volatile solvents. A single ion conductor has a high transference number which eliminates uncontrolled mass transport by immobilizing the anion to the polymer matrix. Problems with undesired side reactions and lithium dendrite growth can also be improved by providing a mechanical barrier. Unfortunately, single-ion conducting SPEs suffer from poor lithium-ion mobility and conductivity due to the immobilized nature of the anions, poor ion-pair dissociation, and the slower time scale diffusion in a polymer matrix compared to liquid electrolytes. In this study, cyclic carbonate-based polymer electrolytes were synthesized to mimic the beneficial properties of conventional carbonate-based liquid electrolytes, such as high level of ion dissociation and solid electrolyte interphase (SEI) formation. A series of copolymers were synthesized varying the structure and composition of the anionic monomer and polar cyclic carbonate containing monomer. The tertiary hydrogen on these carbonate monomers can act as a crosslinking point in free radical polymerizations or UV curing processes to provide robust mechanical properties to the SPEs at elevated temperatures. Although the inherent conductivities of the single-ion SPEs are on the order of 10-7 mS/cm, the addition of plasticizers can improve these conductivities to 0.1 mS/cm.
12

Hong, Da Young, Da-ae Lim, Young-Kyeong Shin, Jinhong Seok, and Dong-Won Kim. "In-Situ Crosslinked Single-Ion Conducting Gel Polymer Electrolyte for Lithium Metal Batteries." ECS Meeting Abstracts MA2023-01, no. 2 (August 28, 2023): 592. http://dx.doi.org/10.1149/ma2023-012592mtgabs.

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Lithium metal batteries (LMBs) have been considered as promising candidates for energy storage device due to their high energy density. However, high reactivity of lithium metal with liquid electrolyte and continuous growth of dendrite lead to degradation of cycle performance and cell failure. To overcome these problems, the strategy of employing gel polymer electrolytes (GPE) was investigated. GPE can effectively encapsulate organic solvents and facilitate uniform contact with electrodes. Both cations and anions migrate in conventional GPE, which gives rise to low Li+ ion transference number (tLi+). Low tLi+ causes inhomogeneous Li+ ion flux and continuous dendrite growth. Compared to conventional GPE, single-ion conducting gel polymer electrolytes (SIC-GPE) have superior tLi+ value close to unity, since the movement of anions is suppressed. In this work, we synthesized a novel sulfonamide based single-ion conductor and prepared the chemically crosslinked SIC-GPE. The electrolyte was obtained by a facile in-situ crosslinking that further improves interfacial contact with electrodes. The resulting SIC-GPE exhibited high tLi+, which led to homogeneous deposition of Li+ ion and enhanced electrochemical stability. The LMB cell employing SIC-GPE exhibited stable cycle performance, proving ability to suppress the growth of lithium dendrite.
13

Chen, Kang, Bin Xu, Linyu Shen, Danhong Shen, Minjie Li, and Liang-Hong Guo. "Functions and performance of ionic liquids in enhancing electrocatalytic hydrogen evolution reactions: a comprehensive review." RSC Advances 12, no. 30 (2022): 19452–69. http://dx.doi.org/10.1039/d2ra02547g.

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Ionic liquids play multi-functions in synthesizing catalysts for HER such as electrolytes/electrolyte additives, reaction solvents, precursors, single/dual ion sources, binders, or morphological structure/phase structure directing agents.
14

Park, Habin, Anthony Engler, Nian Liu, and Paul Kohl. "Cyclic Carbonate-Based, Single-Ion Conducting Polymer Electrolytes for Li-Ion Batteries: Battery Performance." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 329. http://dx.doi.org/10.1149/ma2022-012329mtgabs.

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Solid polymer electrolytes (SPEs) are a pathway for safe, and high energy and power lithium batteries due to their thermal stability and low vapor pressure. Although polymers can be flexible and dimensional stability, it is lithium dendritic suppression can be a challenge for any electrolyte. Conventional SPEs have both mobile cations and anions, which migrate and cause concentration polarization. The low transference number for lithium ions in an electrolyte contributes lithium concentration gradients causing concentration polarization and lithium dendrites [1,2]. Single-ion conducting SPEs have been reported to demonstrate lithium ion only conduction in the electrolyte as well as retain their high mechanical stability during cycling. However, their low ionic conductivity is due to stationary phase of the tethered anion in the polymer matrix and cation-anion complexation [3]. In this study, a cyclic carbonate neutral moiety was included in the SPE to help dissociate the lithium cation from the tethered anion matrix to increase the ionic conductivity and help form the solid electrolyte interphase (SEI) layer. The cyclic carbonate unit in the SPE is similar to the cyclic carbonate solvent in a conventional lithium ion battery and could participate in the solvation of the lithium cation in the SPE. The cyclic carbonate monomer in the SPE can participate in SEI-forming electrochemical reactions on the electrode surface and suppress undesirable side reactions and lithium dendritic growth. Satisfactory level of rate and cycling performance was achieved with the novel neutral monomers in the single-ion conducting SPEs. [1] H. Zhang, C. Li, M. Piszcz, E. Coya, T. Rojo, L.M. Rodriguez-Martinez, M. Armand, Z. Zhou, Chem. Soc. Rev. 2017, 46, 797-815. [2] F. Ahmed, I. Choi, M.M. Rahman, H. Jang, T. Ryu, S. Yoon, L. Jin, Y. Jin, W. Kim, ACS Appl. Mater. Interfaces 2019, 11, 34930-34938. [3] D.-M. Shin, J.E. Bachman, M.K. Taylor, J. Kamcev, J.G. Park, M.E. Ziebel, E. Velasquez, N.N. Jarenwattananon, G.K. Sethi, Y. Cui, J.R. Long, Adv. Mater. 2020, 32, 1905771.
15

Carmona, Eric A., Yueming Song, and Paul Albertus. "(Digital Presentation) Electrochemical-Mechanical Coupling between Single-Ion Conducting Electrolytes and Metal Electrodes." ECS Meeting Abstracts MA2022-01, no. 37 (July 7, 2022): 1641. http://dx.doi.org/10.1149/ma2022-01371641mtgabs.

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Solid-state metal batteries provide increased gravimetric and volumetric energy density compared to conventional Li-ion batteries and their development is essential for meeting performance and cost targets for consumer applications. Conventional liquid electrolytes exhibit reactivity with pure Li and undergo significant dendrite formation, thus single-ion conducting solid electrolytes have been explored to prevent and mitigate dendrite formation as they possess high modulus, high room temperature ionic conductivity, and the potential to improve safety compared to organic liquid electrolytes. Unfortunately, ceramic single-ion conducting electrolytes such as LLZO have been demonstrated to form dendrites above critical current densities. Understanding the electrochemical-mechanical coupling between the electrolyte and electrode can help elucidate the mechanisms of dendrite formation and propagation in solid-state metal batteries as well as methods for prevention and mitigation. Mechanical stresses arise during battery operation due to external stack pressure, expansion and contraction of intercalation electrodes, and the deposition and stripping of metal electrodes. As we demonstrated in a previous work1, the thermodynamic state of the electrode is affected by its mechanical state, therefore, applied stresses alter the equilibrium potential of metal electrodes. Additionally, the mechanical state of the electrode can influence the metal electrode plating and stripping kinetics. Previous studies in the literature have examined the effect of mechanics on the current distribution; however, careful attention is required when coupling electrochemistry and mechanics as well as consideration as to the importance of the mechanical state of the electrolyte. This talk will focus on the effects of mechanical stresses on the current distribution at the metal electrode/single-ion conducting electrolyte interface and the implications on dendrite formation and mitigation. References: (1) Carmona, E. A.; Wang, M. J.; Song, Y.; Sakamoto, J.; Albertus, P. The Effect of Mechanical State on the Equilibrium Potential of Alkali Metal/Ceramic Single-Ion Conductor Systems. Advanced Energy Materials 2021, 11 (29), 2101355. https://doi.org/10.1002/AENM.202101355.
16

Li, Ruihe, Simon E. J. O'Kane, Andrew Wang, Taeho Jung, Monica Marinescu, Charles W. Monroe, and Gregory James Offer. "Effect of Solvent Segregation on the Performance of Lithium-Ion Batteries." ECS Meeting Abstracts MA2023-02, no. 7 (December 22, 2023): 975. http://dx.doi.org/10.1149/ma2023-027975mtgabs.

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The pseudo two-dimensional (P2D) model is one of the most powerful tools in modelling lithium-ion batteries (LIBs) 1, in that it can describe the complex electrochemical and thermal behaviours of LIBs with high fidelity yet maintain relatively high computing efficiency. To achieve that, many assumptions have been made, one of which is the single solvent assumption. However, most electrolytes used in LIBs uses multiple solvents to balance the requirements of conductivity, diffusivity and viscosity 2. Therefore, the single solvent assumption indicates that all solvents move as a single entity. However, previous experimental studies have shown that Li+ preferentially attracts cyclic carbonates (like ethylene carbonate, EC) rather than linear carbonates (such as ethyl-methyl carbonate, EMC) to form ion-solvent clusters 3. During charge/discharge, ion-solvent clusters move between the positive and negative electrodes to constitute ionic current. At the electrolyte-electrolyte interface, Li+ de-solvates from the clusters and intercalates into the electrode, or vice versa. Such process will induce concentration gradients of both solvents and lithium ions; the solvent concentration has been ignored in the P2D model. The simplification means the current P2D model fails to capture two important phenomena: (1) many electrolyte properties - including conductivity, diffusivity, and thermodynamic factors - are sensitive to the solvent concentration 4; (2) the solvent components in the ion-solvent clusters are preferentially consumed by interfacial side reactions such as the growth of solid-electrolyte interface (SEI) 3. To fill this gap, we add an extra governing equation for the solvent concentration (in our case, EC) which allows us to describe an electrolyte with two solvents and one salt. We also include a cross diffusion term to consider the dragging effect between the working solvent (EC) and lithium ions. For the charge conservation equation, we directly use measured liquid junction potential as a function of both solvent and lithium-ion concentration, which avoids possible errors brought by identifying the thermodynamic factors. To elucidate the effect of solvent segregation, we compare the overpotential and concentration profile of Li ion and EC at the end of 3C discharge of the normal DFN (single case) and our revised model (double case). The revised model predicts opposite EC concentration compared with Li+, which has been observed by Wang et al. 5 For a high value of , the dragging effect between Li+ and EC is more significant, inducing high concentration gradients of both species. The EC overpotential can be as high as 10 mV and further affects the rate performance of LIBs. This revised model captures more complicated transport mechanisms in the electrolyte and opens the chance of linking the microscopic understanding on solvation structure to a continuum level model. Reference: (1) Newman, J.; Thomas-Alyea, K. E. Electrochemical Systems; 2004. (2) Xu, K. Electrolytes and interphases in Li-ion batteries and beyond. Chem Rev 2014, 114 (23), 11503-11618. DOI: 10.1021/cr500003w. (3) Xu, K. Solvation Sheath of Li+ in Nonaqueous Electrolytes and Its Implication of Graphite/ Electrolyte Interface Chemistry. J. Phys. Chem. C 2007. (4) Ding, M. S.; Xu, K.; Zhang, S. S.; Amine, K.; Henriksen, G. L.; Jow, T. R. Change of Conductivity with Salt Content, Solvent Composition, and Temperature for Electrolytes of LiPF6 in Ethylene Carbonate-Ethyl Methyl Carbonate. Journal of The Electrochemical Society 2001, 148 (10). DOI: 10.1149/1.1403730. (5) Wang, A. A.; Greenbank, S.; Li, G.; Howey, D. A.; Monroe, C. W. Current-driven solvent segregation in lithium-ion electrolytes. Cell Reports Physical Science 2022, 3 (9). DOI: 10.1016/j.xcrp.2022.101047. Figure 1
17

Butnicu, Dan, Daniela Ionescu, and Maria Kovaci. "Structure Optimization of Some Single-Ion Conducting Polymer Electrolytes with Increased Conductivity Used in “Beyond Lithium-Ion” Batteries." Polymers 16, no. 3 (January 29, 2024): 368. http://dx.doi.org/10.3390/polym16030368.

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Simulation techniques implemented with the HFSS program were used for structure optimization from the point of view of increasing the conductivity of the batteries’ electrolytes. Our analysis was focused on reliable “beyond lithium-ion” batteries, using single-ion conducting polymer electrolytes, in a gel variant. Their conductivity can be increased by tuning and correlating the internal parameters of the structure. Materials in the battery system were modeled at the nanoscale with HFSS: electrodes–electrolyte–moving ions. Some new materials reported in the literature were studied, like poly(ethylene glycol) dimethacrylate-x-styrene sulfonate (PEGDMA-SS) or PU-TFMSI for the electrolyte; p-dopable polytriphenyl amine for cathodes in Na-ion batteries or sulfur cathodes in Mg-ion or Al-ion batteries. The coarse-grained molecular dynamics model combined with the atomistic model were both considered for structural simulation at the molecular level. Issues like interaction forces at the nanoscopic scale, charge carrier mobility, conductivity in the cell, and energy density of the electrodes were implied in the analysis. The results were compared to the reported experimental data, to confirm the method and for error analysis. For the real structures of gel polymer electrolytes, this method can indicate that their conductivity increases up to 15%, and even up to 26% in the resonant cases, via parameter correlation. The tuning and control of material properties becomes a problem of structure optimization, solved with non-invasive simulation methods, in agreement with the experiment.
18

von Aspern, Natascha, Christian Wölke, Markus Börner, Martin Winter, and Isidora Cekic-Laskovic. "Impact of single vs. blended functional electrolyte additives on interphase formation and overall lithium ion battery performance." Journal of Solid State Electrochemistry 24, no. 11-12 (September 26, 2020): 3145–56. http://dx.doi.org/10.1007/s10008-020-04781-1.

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Abstract Two functional high-voltage additives, namely 2-(2,2,3,3,3-pentafluoropropoxy)-1,3,2-dioxaphospholane (PFPOEPi) and 1-methyl-3,5-bis(trifluoromethyl)-1H-pyrazole (MBTFMP) were combined as functional additive mixture in organic carbonate–based electrolyte formulation for high-voltage lithium battery application. Their impact on the overall performance in NMC111 cathode-based cells was compared with the single-additive–containing electrolyte counterpart. The obtained results point to similar cycling performance of the additive mixture containing electrolyte formulation compared with the MBTFMP-containing cells, whereas the single PFPOEPi-containing cells displayed the best cycling performance in NMC111||graphite cells. With regard to the cathode electrolyte interphase (CEI), characterized and analyzed by means of scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS), both the MBTFMP and the PFPOEPi functional additives decompose on the NMC111 surface in single-additive–containing electrolyte formulations. However, the thickness of the CEI formed in the additive mixture–containing electrolyte formulation is determined by the MBTFMP additive, whereas the PFPOEPi additive impacts a change in the composition of the CEI. Furthermore, the MBTFMP additive decomposes prior to the PFPOEPi and, therefore, dominates the cycling performance of NMC111||graphite cells containing functional additive mixture–based electrolyte. This systematic approach allows us to understand the synergistic impact of each functional additive in an electrolyte formulation containing an additive mixture and helps to identify the right additive combination for advanced electrolyte formulation as well as to elucidate whether the single-additive or the additive mixture approach is more effective for the development of advanced functional electrolytes for lithium-based cell chemistries. Graphical abstract
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Corradini, Fulvio, Luigi Marcheselli, Lorenzo Tassi, Giuseppe Tosi, and Salvatore Fanali. "Thermodynamic behaviour of some electrolytes in ethane-1,2-diol from −10 to +80 °C." Canadian Journal of Chemistry 71, no. 8 (August 1, 1993): 1265–72. http://dx.doi.org/10.1139/v93-163.

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Conductivities of the electrolytes NaBr, NaPi, HPi, NaBPh4, and Ph4PBr in ethane- 1,2-diol were determined in the −10 ≤ t ≤ +80 °C temperature range. The experimental data were analyzed by the Fuoss–Hsia equation, which provides further informative parameters such as the dissociation constant (K) of the ion pairs formed in solution, the limiting equivalent conductivity (Λ0), and the ion-size parameter (å). Thermodynamic behaviour of these electrolytes was derived from analysis of the K values. Single-ion conductivities were evaluated on the basis of the assumption of Ph4PBPh4 as reference electrolyte.
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Temprano, Israel, Wesley M. Dose, Michael F. L. De Volder, and Clare P. Grey. "Solvent-Driven Degradation of Ni-Rich Cathodes Probed by Operando Gas Analysis." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 348. http://dx.doi.org/10.1149/ma2023-022348mtgabs.

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High-capacity Ni-rich layered metal oxide cathodes are highly desirable to increase the energy density of lithium-ion batteries. However, these materials suffer from poor cycling stability, which is exacerbated by increased cell voltage due to higher interfacial reactivity than their lower Ni-content analogues. Here, we study the pivotal role of electrolyte solvents in determining the interfacial reactivity at charged LiNi0.33Mn0.33Co0.33O2 (NMC111) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes by using both single-solvent model electrolytes and the mixed solvents used in commercial cells (1, 2). Operando gas analysis reveals that the solvent-dependent reactivity for Ni-rich cathodes is related to the extent of lattice oxygen release and accompanying electrolyte oxidation. We demonstrate here the detrimental effect of ethylene carbonate (EC), a core component in conventional electrolytes, when NMC811 is charged above 4.3 V vs Li/Li+ - the observed onset potential for lattice oxygen release. Oxygen loss is enhanced by EC-containing electrolytes and correlates with more electrolyte oxidation/breakdown and cathode surface degradation, which increase concurrently above 4.4 V. The gas analysis also reveals the crosstalk effect caused by the products of the nascent oxygen from the NMC811 lattice and the electrolyte solvent, showing anodic reactivity. In contrast, NMC111, which does not release oxygen up to 4.6 V, shows a similar extent of degradation irrespective of the electrolyte. Higher lattice oxygen release with EC-containing electrolytes is coupled with higher interfacial impedance, a thicker oxygen-deficient rock-salt surface reconstruction layer, more electrolyte solvent and salt breakdown. Oxygen loss is suppressed in the EC-free electrolyte, highlighting the incompatibility between Ni-rich cathodes and conventional electrolyte solvents. W. M. Dose et al., Onset Potential for Electrolyte Oxidation and Ni-Rich Cathode Degradation in Lithium-Ion Batteries. ACS Energy Letters 7, 3524-3530 (2022). W. M. Dose et al., Electrolyte Reactivity at the Charged Ni-Rich Cathode Interface and Degradation in Li-Ion Batteries. ACS Applied Materials & Interfaces 14, 13206-13222 (2022). Figure 1
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Hakin, Andrew W., and Colin L. Beswick. "Single-ion enthalpies and entropies of transfer from water to aqueous urea solutions at 298.15 K." Canadian Journal of Chemistry 70, no. 6 (June 1, 1992): 1666–70. http://dx.doi.org/10.1139/v92-209.

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In this paper we report enthalpies of solution at infinite dilution [Formula: see text] at 298.15 K for tetraphenylarsonium chloride (Ph4AsCl), sodium tetraphenylborate (NaBPh4), sodium chloride (NaCl), sodium bromide (NaBr), and sodium iodide (NaI) in water and aqueous solutions containing 5, 10, 20, and 30% urea by weight. Enthalpies of transfer from water to aqueous urea solutions are reported. Single-ion enthalpies of transfer [Formula: see text] have been calculated using the tetraphenylarsonium tetraphenylborate, (TATB) reference electrolyte assumption. These single-ion enthalpy data have been combined with single-ion Gibbs functions of transfer [Formula: see text] reported in the literature to obtain single-ion entropies of transfer [Formula: see text] for the urea + water mixed solvent system. The results of this single-ion analysis are discussed in terms of the impact of electrolytes on the structure of aqueous urea solutions.
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Liang, Hai-Peng, Maider Zarrabeitia, Zhen Chen, Sven Jovanovic, Steffen Merz, Josef Granwehr, Stefano Passerini, and Dominic Bresser. "Polysiloxane-Based Single-Ion Conducting Polymer Electrolyte for High-Performance Li‖NMC811 Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 326. http://dx.doi.org/10.1149/ma2022-012326mtgabs.

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The ongoing electrification of the transportation sector is triggering a continuous search for batteries with higher energy density. One approach to achieve this goal is the transition to lithium-metal anodes. However, the practical implementation brings about severe safety issues such as the dendritic deposition and growth of metallic lithium and the consequent risk of accidental short circuiting of the cell, resulting in a thermal runaway.1 Solid-state electrolytes such as polymers are considered a viable strategy to overcome this issue, especially single-ion conducting polymers, owing to the absence of the detrimental reversed cell polarization, the uniform Li+ flux, and frequently higher limiting current densities.2,3 In fact, the latter is of utmost importance for the fast charging of battery cells as well as the eventual power density. So far, however, the cycling performance at high dis-/charge rates and high current densities for battery cells comprising a polymer electrolyte remained little investigated and commonly non-satisfactory. Here, we report the development of a polysiloxane-based single-ion conducting polymer electrolyte (PSiOM) with a Li+ conductivity exceeding 10−4 S cm−1 at ambient temperature and excellent stability towards both lithium metal and high-energy LiNi0.8Co0.1Mn0.1O2 (NMC811) as the active material for the positive electrode. This new polymer electrolyte enables dendrite-free lithium deposition, thanks to the formation of a suitable electrode|electrolyte interface and interphase and the uniform Li+ flux. Moreover, PSiOM allows for an outstanding capacity retention of, e.g., 90% at 1C and 86% at 2C after 300 cycles and rapid charging and discharging at C rates as high as 5C. It is important to note that we used reasonable active material mass loadings for these tests (>7 mg cm-2), which means that the current densities applied were up to 7.20 mA cm−2 at 40 °C and 2.88 mA cm−2 at 20 °C. To the best of our knowledge, these current densities are among the highest reported so far for polymer-based electrolytes. References (1) Kalhoff, J.; Eshetu, G. G.; Bresser, D.; Passerini, S. Safer Electrolytes for Lithium-Ion Batteries: State of the Art and Perspectives. ChemSusChem 2015, 8 (13), 2154–2175. (2) Zhang, H.; Li, C.; Piszcz, M.; Coya, E.; Rojo, T.; Rodriguez-Martinez, L. M.; Armand, M.; Zhou, Z. Single Lithium-Ion Conducting Solid Polymer Electrolytes: Advances and Perspectives. Chemical Society Reviews 2017, 46 (3), 797–815. (3) Nguyen, H.-D.; Kim, G.-T.; Shi, J.; Paillard, E.; Judeinstein, P.; Lyonnard, S.; Bresser, D.; Iojoiu, C. Nanostructured Multi-Block Copolymer Single-Ion Conductors for Safer High-Performance Lithium Batteries. Energy & Environmental Science 2018, 11 (11), 3298–3309.
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Wittig, Marina, and Bernhard Rieger. "Synthesis of a Conceptual New Single-Ion Conducting Polymer Electrolyte for All-Solid-State Batteries." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 289. http://dx.doi.org/10.1149/ma2023-022289mtgabs.

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The increasing global population and the rapid change in climatic conditions strengthens the demand for a more efficient handling of energy consumption and energy storage technologies. In this context, all-solid-state batteries (ASSBs) as next-generation rechargeable lithium-ion batteries offer an improved energy and power density based on the integration of novel separators and electrode materials. In comparison to their liquid representatives, ASSBs provide a higher intrinsic safety via non-flammable components and in addition greater long-term durability. In relation to common electrolyte classes, solid polymers stand out due to their good mechanical flexibility, easy film-formation ability, good contact supply between cell components, and lower production costs, favoring the application as electrolytes, protective coatings, as well as additives in cathode composites. Among a variety of polymers, poly(ethylene oxide) (PEO) is a well-studied and established host polymer due to its great ability to dissolve lithium salts like LiBH4, LiPF6 or LiTFSI. Based on a low glass transition temperature (Tg) of about - 60 to - 50 °C, PEO shows a high degree of polymer chain flexibility which facilitates the migration of the lithium cations through the solid electrolyte. Nevertheless, its semi-crystalline character often leads to low conductivities below its melting point (Tm) of around 60 °C, making pure PEO unattractive as solid electrolyte. Copolymerization, the addition of a small amount of solvent to produce so called gel polymer electrolytes, the addition of some plasticizers, or the interplay of polymer and inorganic fillers try to counteract this trend. The synthetical concept behind this work is aiming to benefit from the flexible nature of PEO, and at the same time to improve the ionic conductivities and especially the lithium migration by structural realignment away from a dual-ion towards a single-ion conducting polymer electrolyte (SICPE). The polar PEO-backbone ensures polymer chain mobility, whereas a rigid aromatic structure unit as side chain bears the fixed anionic group. The immobilization of the anionic charges on the polyether backbone tends to guide the electrolyte to higher lithium transference numbers, fewer polarization effects, and the suppression of dendrite growth, resulting in an overall improved cell performance. Synthesis steps via the novel SICPE are characterized with the help of nuclear magnetic resonance spectroscopy (NMR), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC). Thermal analyses of the homopolymer already show the positive influence of the flexible PEO-backbone by lowering the Tg from 100 to 150 °C for related aliphatic derivatives down to 60 to 80 °C in our case. On the basis of electrochemical impedance spectroscopy (EIS) measurements, the interplay of chemical, thermal, and electrochemical key properties is investigated. The gained results tend to open a discussion panel concerning occurring challenges for solid-state polymer electrolytes and the interdependencies between electrolyte constitution and polymer characteristics.
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Sutton, Preston, Martino Airoldi, Luca Porcarelli, Jorge L. Olmedo-Martínez, Clément Mugemana, Nico Bruns, David Mecerreyes, Ullrich Steiner, and Ilja Gunkel. "Tuning the Properties of a UV-Polymerized, Cross-Linked Solid Polymer Electrolyte for Lithium Batteries." Polymers 12, no. 3 (March 5, 2020): 595. http://dx.doi.org/10.3390/polym12030595.

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Lithium metal anodes have been pursued for decades as a way to significantly increase the energy density of lithium-ion batteries. However, safety risks caused by flammable liquid electrolytes and short circuits due to lithium dendrite formation during cell cycling have so far prevented the use of lithium metal in commercial batteries. Solid polymer electrolytes (SPEs) offer a potential solution if their mechanical properties and ionic conductivity can be simultaneously engineered. Here, we introduce a family of SPEs that are scalable and easy to prepare with a photopolymerization process, synthesized from amphiphilic acrylic polymer conetworks based on poly(ethylene glycol), 2-hydroxy-ethylacrylate, norbornyl acrylate, and either lithium bis (trifluoromethanesulfonyl) imide (LiTFSI) or a single-ion polymethacrylate as lithium-ion source. Several conetworks were synthesized and cycled, and their ionic conductivity, mechanical properties, and lithium transference number were characterized. A single-ion-conducting polymer electrolyte shows the best compromise between the different properties and extends the calendar life of the cell.
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Voropaeva, Daria, Svetlana Novikova, Nikolay Trofimenko, and Andrey Yaroslavtsev. "Polystyrene-Based Single-Ion Conducting Polymer Electrolyte for Lithium Metal Batteries." Processes 10, no. 12 (November 25, 2022): 2509. http://dx.doi.org/10.3390/pr10122509.

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Lithium metal batteries are one of the more promising replacements for lithium-ion batteries owing to their ability to reach high energy densities. The main problem limiting their commercial application is the formation of dendrites, which significantly reduces their durability and renders the batteries unsafe. In the present work, we used a single-ion conducting gel polymer electrolyte based on a poly(ethylene-ran-butylene)-block-polystyrene (SEBS) block copolymer, which was functionalized with benzenesulfonylimide anions and plasticized by a mixture of ethylene carbonate and dimethylacetamide (SSEBS-Ph-EC-DMA), with a solvent uptake of 160% (~12 solvent molecules per one functional group of the membrane). The SSEBS-Ph-EC-DMA electrolyte exhibits an ionic conductivity of 0.6 mSm∙cm−1 at 25 °C and appears to be a cationic conductor (TLi+ = 0.72). SSEBS-Ph-EC-DMA is electrochemically stable up to 4.1 V. Symmetrical Li|Li cells; further, with regard to SSEBS-Ph-EC-DMA membrane electrolytes, it showed a good performance (~0.10 V at first cycles and <0.23 V after 700 h of cycling at ±0.1 mA∙cm−2 and ±0.05 mAh∙cm−2). The LiFePO4|SSEBS-Ph-EC-DMA|Li battery showed discharge capacity values of 100 mAh∙g−1 and a 100% Coulomb efficiency, at a cycling rate of 0.1C.
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Alexander, George, and Eric Wachsman. "(Invited) Achieving High Areal Capacity and Extreme Critical Current Densities through Tailored Garnet Solid Electrolyte Structures." ECS Meeting Abstracts MA2023-01, no. 6 (August 28, 2023): 1026. http://dx.doi.org/10.1149/ma2023-0161026mtgabs.

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Garnet structured electrolytes are an exceptional candidate to substitute for organic liquid electrolytes owing to its high ionic conductivity and safety.[1] One of the main issues preventing the commercialization of this electrolyte is limited lithium plating capacity and lithium dendrite shorting.[2] To address this, we invented new single-phase mixed ion electron conducting (MIEC) garnet with comparable lithium-ion and electron conductivity at room temperature. We demonstrate that in a trilayer architecture, with a porous MIEC framework supporting a thin dense garnet solid electrolyte, the critical current density can be as high as 100 mA/cm2, with no dendrite-induced shorting at room temperature and without any stack pressure. The single-phase MIEC conductor spreads the potential uniformly across the material surface preventing dendrite propagation through the dense garnet solid electrolyte layer. Additionally, high lithium stripping capacity and impressive cycling stability were observed at commercial level current densities of well over 10 mA/cm2. The role of the porous MIEC garnet structure is elucidated using various electrochemical and electron microscopy techniques. Wang, C. et al. Garnet-Type Solid-State Electrolytes: Materials, Interfaces, and Batteries. Chem. Rev. 120, 4257–4300 (2020). Albertus, P., Babinec, S., Litzelman, S. & Newman, A. Status and challenges in enabling the lithium metal electrode for high-energy and low-cost rechargeable batteries. Nat. Energy 2017 31 3, 16–21 (2017).
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Wolf, A., N. Reber, P. Yu Apel, B. E. Fischer, and R. Spohr. "Electrolyte transport in charged single ion track capillaries." Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms 105, no. 1-4 (November 1995): 291–93. http://dx.doi.org/10.1016/0168-583x(95)00577-3.

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Park, Sodam, Imanuel Kristanto, Gwan Yeong Jung, David B. Ahn, Kihun Jeong, Sang Kyu Kwak, and Sang-Young Lee. "A single-ion conducting covalent organic framework for aqueous rechargeable Zn-ion batteries." Chemical Science 11, no. 43 (2020): 11692–98. http://dx.doi.org/10.1039/d0sc02785e.

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Cui, Wei Wei, Dong Yan Tang, and Li Li Guan. "A Single Ion Conducting Gel Polymer Electrolyte Based on Poly(lithium 2-Acrylamido-2-Methylpropanesulfonic Acid-Co-Vinyl Triethoxysilane) and its Electrochemical Properties." Advanced Materials Research 535-537 (June 2012): 2053–56. http://dx.doi.org/10.4028/www.scientific.net/amr.535-537.2053.

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Single ion conducting polymer electrolytes synthesized through a copolymer poly(lithium 2-acrylamido-2-methylpropanesulfonic acid-co-vinyl triethoxysilane) and a crosslinker poly(etheylene glycol) dimethacrylate (PEGDMA) were prepared. Scanning electron microscope (SEM) was used to observe the morphology of the surface and cross-section of the polymer electrolyte membrane. AC impedance and linear sweep voltammetry were used to investigate the electrochemical properties of the polymer electrolytes. It was found that the obtained membrane had a typical amorphous structure and possessed a smooth surface. The bulk resistance of the polymer electrolyte increased with the increase in the plasticizer uptake. The electrochemical stability increased with the increase in the content of VTES.
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Pandey, Kamlesh, Nidhi Asthana, Mrigank Mauli Dwivedi, and S. K. Chaturvedi. "Effect of Plasticizers on Structural and Dielectric Behaviour of [PEO + (NH4)2C4H8(COO)2] Polymer Electrolyte." Journal of Polymers 2013 (August 6, 2013): 1–12. http://dx.doi.org/10.1155/2013/752596.

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Improvements in ion transport property of polyethylene-oxide- (PEO-) based polymer electrolytes have been investigated, using different types of plasticizers. The effects of single and coupled plasticizers [i.e., EC, (EC + PC), and (EC + PEG)] on structural and electrical behavior of pristine electrolyte were studied by XRD, SEM technique, and impedance spectroscopy. The electrical conductivity of the best plasticized system was found to be 4 × 10−6 S/cm. Argand plots show dispersive nature of relaxation time or inhomogeneous space charge polarization of plasticized polymer electrolyte.
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Rohan, Rupesh, Kapil Pareek, Weiwei Cai, Yunfeng Zhang, Guodong Xu, Zhongxin Chen, Zhiqiang Gao, Zhao Dan, and Hansong Cheng. "Melamine–terephthalaldehyde–lithium complex: a porous organic network based single ion electrolyte for lithium ion batteries." Journal of Materials Chemistry A 3, no. 9 (2015): 5132–39. http://dx.doi.org/10.1039/c4ta06855f.

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Perez-Tejeda, P., A. Maestre, P. Delgado-Cobos, and J. Burgess. "Single-ion Setschenow coefficients for several hydrophobic non-electrolytes in aqueous electrolyte solutions." Canadian Journal of Chemistry 68, no. 2 (February 1, 1990): 243–46. http://dx.doi.org/10.1139/v90-032.

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Setschenow coefficients have been derived from solubility measurements on cyclohexane, benzene, naphthalene, 1-naphthol, 1,5-dihydroxynaphthalene, and anthracene in alkali halide, tetraalkylammonium bromide, and tetraphenylarsonium chloride aqueous solutions at 298.2 K. Single ion Setschenow coefficients have thence been obtained by an assumption involving extrapolation of the tetraalkylammonium bromide results to zero cation volume. Setschenow coefficients for the tetraalkylammonium cations correlate well with a hydrophobicity parameter based on their transfer chemical potentials from water into 1,2-dichloroethane. Keywords: solubilities, aqueous salt solutions, Setschenow coefficients.
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Xu, Guodong, Rupesh Rohan, Jing Li, and Hansong Cheng. "A novel sp3Al-based porous single-ion polymer electrolyte for lithium ion batteries." RSC Advances 5, no. 41 (2015): 32343–49. http://dx.doi.org/10.1039/c5ra01126d.

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We report synthesis of an Al-based porous gel single-ion polymer electrolyte, lithium poly (glutaric acid aluminate) (LiPGAA), using glutaric acid and lithium tetramethanolatoaluminate as the precursors.
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Zhang, Yunfeng, Corina Anrou Lim, Weiwei Cai, Rupesh Rohan, Guodong Xu, Yubao Sun, and Hansong Cheng. "Design and synthesis of a single ion conducting block copolymer electrolyte with multifunctionality for lithium ion batteries." RSC Adv. 4, no. 83 (2014): 43857–64. http://dx.doi.org/10.1039/c4ra08709g.

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Liu, Kewei, Yingying Xie, Zhenzhen Yang, Hong-Keun Kim, Trevor L. Dzwiniel, Jianzhong Yang, Hui Xiong, and Chen Liao. "Design of a Single-Ion Conducting Polymer Electrolyte for Sodium-Ion Batteries." Journal of The Electrochemical Society 168, no. 12 (December 1, 2021): 120543. http://dx.doi.org/10.1149/1945-7111/ac42f2.

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A sodium bis(fluoroallyl)malonato borate salt (NaBFMB) is synthesized. Using a Click thiol-ene reaction, NaBFMB can be photo-crosslinked with a tri-thiol (trimethylolpropane tris(3-mercapto propionate), TMPT) to create a single-ion conducting electrolyte (NaSIE), with all negative charges residing on the borate moieties and anions immobilized through the 3-D crosslinked network. The NaSIE can be prepared either as a free-standing film or through a drop-cast method followed by a photo crosslinking method for an in-situ formation on top of the electrodes. The free-standing film of NaSIE has a high ionic conductivity of 2 × 10−3 S cm−1 at 30 °C, and a high transference number (tNa +) of 0.91 as measured through the Bruce-Vincent method. The electrochemical stability of NaSIE polymer electrolyte is demonstrated via cyclic voltammetry (CV) to be stable up to 5 V vs Na/Na+. When tested inside a symmetrical Na//Na cell, the NaSIE shows a critical current density (CCD) of 0.4 mA cm−2. The stability of NaSIE is further demonstrated via a long cycling of the stripping/plating test with a current density of 0.1 mA cm−2 at five-minute intervals for over 10,000 min. Using the in-situ method, NaSIE is used as the electrolyte for a sodium metal battery using P2 (Na resides at prismatic sites with with ABBAAB stacking)-cathode of Na0.67Ni0.33Mn0.67O2 (NNMO) and is cycled between the cut-off voltages of 2.0–4.0 V. A high initial specific capacity (85.7 mAh g−1) with a capacity retention of 86.79% after 150 cycles is obtained.
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Yik, Jackie, Leiting Zhang, Jens Sjölund, Xu Hou, Per Svensson, Kristina Edström, and Erik J. Berg. "Automated Electrolyte Formulation and Coin Cell Assembly for High-Throughput Lithium-Ion Battery Research." ECS Meeting Abstracts MA2023-02, no. 4 (December 22, 2023): 572. http://dx.doi.org/10.1149/ma2023-024572mtgabs.

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Battery research involving performance evaluation by battery cycling is a time-consuming process with sometimes large cell-to-cell variations. To enhance the rate of testing and reproducibility, automation is one accelerator that can be used. In this study, we introduce ODACell1 (Figure 1), an automated system for high-throughput electrolyte screening and Li-ion cell assembly. ODACell enables the assembly of Li-ion battery cells in ambient atmosphere. We use LiFePO4||Li4Ti5O12-based full cells with a dimethyl sulfoxide-based model electrolyte for demonstrating the automated system. We investigate the reproducibility of the automated system on this system as well as the influence of water on the performance of the model electrolyte when exposed to ambient air. Our system is uniquely equipped for combinatorial experimentation, combining electrolyte formulation, batch coin cell assembly, and cycling into a single system. The integration of multiple setups into a single unit is made possible, overcoming the incompatibility issues with integrating multiple, different automated systems together. While there are several other robotic systems besides ODACell for battery material acceleration, ODACell’s unique combination of robots incorporated in the robotic setup allow a broader set of tasks to be automated. For example, Clio by Dave et al. 2 focus on electrolyte formulation and characterization, lacking assembly of battery cells; AutoBASS by Zhang et al. 3 only automates battery assembly; and Poseidon by Svensson et al. 4 can automate electrolyte formulation, characterization, and coin cell assembly, but lack high-throughput batch processing. ODACell ensures high reproducibility, which is needed to establish robust models and determine accurate electrochemical and physical properties. The system assembled 131 coin cells, with a conservative fail rate of only 5%. The relative standard deviation of the discharge capacity after 10 cycles was 2% for the studied system. The investigation into the influence of water on cycling performance show overlapping performance trends between coin cells with 2 vol% and 4 vol% of water in the electrolyte highlighting the nontrivial relationship between water and cycling performance. In conclusion, ODACell is a promising tool for high-throughput electrolyte screening and Li-ion cell assembly. It builds upon previously published robotic setups by automating more of the research workflow. Our study highlights the importance of reproducibility in battery research and the complex relationship between water contaminants in electrolytes and cycling performance. ODACell has the potential to be a useful tool for advancing battery research by enhancing the rate of testing and reducing the variation of results. References: [1]J. T. Yik, et al., Automated electrolyte formulation and coin cell assembly for high-throughput lithium-ion battery research, ChemRxiv, 2022. This content is a preprint and has not been peer-reviewed. [2] A. Dave, et al., Autonomous Discovery of Battery Electrolytes with Robotic Experimentation and Machine Learning, Cell Reports Physical Science, 2020, 1, 100264. [3] B. Zhang, et al., Robotic cell assembly to accelerate battery research, Digital Discovery, 2022, 1, 755–762. [4] P. H. Svensson, et al., Robotised screening and characterisation for accelerated discovery of novel Lithium ion battery electrolytes: Building a platform and proof of principle studies, Chemical Engineering Journal, 2023, 455, 140955. Figure 1
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Gerstenberg, Jessica, Dominik Steckermeier, Arno Kwade, and Peter Michalowski. "Effect of Mixing Intensity on Electrochemical Performance of Oxide/Sulfide Composite Electrolytes." Batteries 10, no. 3 (March 7, 2024): 95. http://dx.doi.org/10.3390/batteries10030095.

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Despite the variety of solid electrolytes available, no single solid electrolyte has been found that meets all the requirements of the successor technology of lithium-ion batteries in an optimum way. However, composite hybrid electrolytes that combine the desired properties such as high ionic conductivity or stability against lithium are promising. The addition of conductive oxide fillers to sulfide solid electrolytes has been reported to increase ionic conductivity and improve stability relative to the individual electrolytes, but the influence of the mixing process to create composite electrolytes has not been investigated. Here, we investigate Li3PS4 (LPS) and Li7La3Zr2O12 (LLZO) composite electrolytes using electrochemical impedance spectroscopy and distribution of relaxation times. The distinction between sulfide bulk and grain boundary polarization processes is possible with the methods used at temperatures below 10 °C. We propose lithium transport through the space-charge layer within the sulfide electrolyte, which increases the conductivity. With increasing mixing intensities in a high-energy ball mill, we show an overlay of the enhanced lithium-ion transport with the structural change of the sulfide matrix component, which increases the ionic conductivity of LPS from 4.1 × 10−5 S cm−1 to 1.7 × 10−4 S cm−1.
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Deng, Jie, Jing Li, Shuang Song, Yanping Zhou, and Luming Li. "Electrolyte-Dependent Supercapacitor Performance on Nitrogen-Doped Porous Bio-Carbon from Gelatin." Nanomaterials 10, no. 2 (February 18, 2020): 353. http://dx.doi.org/10.3390/nano10020353.

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The carbon supercapacitance strongly relies upon the electrolyte’s nature, but the clear-cut structure–performance nexus remains elusive. Herein, a series of bio-carbons with gradually varied pore structure and surface chemistry are derived using a new salt template protocol (with eco-benign KNO3 as the template, activator, and porogen, and cheap gelatin as the carbon precursor), and are used as model systems to probe the dependence of the electrochemical mechanism of such nanocarbons on two typical electrolytes (KOH and EMIBF4). By only adjusting the KNO3 dosage, two pivotal figures of merit of biochar—multiscale porosity and surface functionalization—were finely modulated to construct electric double layers. Electrochemical data clarify that the combined porosity and doping effects all contribute to enhanced supercapacitance, but with only one of the two factors playing the leading role in different electrolytes. Kinetic analysis corroborates the fact that ample heteroatom doping can effectively compensate capacitance by intensive surface redox insertion in KOH, while a suitable pore size dispersion plays a preponderant part in self-amplifying the ion partitioning, and thus dictating a good charge separation in EMIBF4. A quasi-quantitative model of performance–structure relevance in EMIBF4 is judiciously conjectured to hint at a superb ion–pore-size compatibility, in which the bi- and mono-layer ion confinement coupling in integrated single and double ion-sized pores is found to be more useful for curbing notorious over-screening effects and for changing the coordination number, Coulombic ordering, and phase conformation of EMIBF4 in several nm-sized nanopores. This unique energy storage fashion in ion-matching pores promotes the energy density of optimal samples to a novel level of 88.3 Wh kg−1 at 1 kW kg−1, which rivals the overwhelming majority of the reported carbon materials. In short, the comparison case study here reveals a valuable correlation of carbon’s figure of merit and electrolyte type, which may act as a vital rudder to design electrolyte-contingent state-of-the-art supercapacitor materials.
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Dai, Kuan, Cheng Ma, Yiming Feng, Liangjun Zhou, Guichao Kuang, Yun Zhang, Yanqing Lai, Xinwei Cui, and Weifeng Wei. "A borate-rich, cross-linked gel polymer electrolyte with near-single ion conduction for lithium metal batteries." Journal of Materials Chemistry A 7, no. 31 (2019): 18547–57. http://dx.doi.org/10.1039/c9ta05938e.

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Cao, Chen, Yu Li, Yiyu Feng, Peng Long, Haoran An, Chengqun Qin, Junkai Han, Shuangwen Li, and Wei Feng. "A sulfonimide-based alternating copolymer as a single-ion polymer electrolyte for high-performance lithium-ion batteries." Journal of Materials Chemistry A 5, no. 43 (2017): 22519–26. http://dx.doi.org/10.1039/c7ta05787c.

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Sen, Sudeshna, Rudresha B. Jayappa, Haijin Zhu, Maria Forsyth, and Aninda J. Bhattacharyya. "A single cation or anion dendrimer-based liquid electrolyte." Chemical Science 7, no. 5 (2016): 3390–98. http://dx.doi.org/10.1039/c5sc04584c.

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The proposed dendrimer based liquid electrolyte is a single-ion conductor where ion transport is altered by the nature of the chemical functionalities leading to large variations in anion diffusion and hence ionic transference number.
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Zhu, Y. S., X. W. Gao, X. J. Wang, Y. Y. Hou, L. L. Liu, and Y. P. Wu. "A single-ion polymer electrolyte based on boronate for lithium ion batteries." Electrochemistry Communications 22 (August 2012): 29–32. http://dx.doi.org/10.1016/j.elecom.2012.05.022.

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Sun, Yubao, Rupesh Rohan, Weiwei Cai, Xifei Wan, Kapil Pareek, An Lin, Zhang Yunfeng, and Hansong Cheng. "A Polyamide Single-Ion Electrolyte Membrane for Application in Lithium-Ion Batteries." Energy Technology 2, no. 8 (July 23, 2014): 698–704. http://dx.doi.org/10.1002/ente.201402041.

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Aissou, Karim, Muhammad Mumtaz, Özlem Usluer, Gilles Pécastaings, Giuseppe Portale, Guillaume Fleury, Eric Cloutet, and Georges Hadziioannou. "Anisotropic Lithium Ion Conductivity in Single-Ion Diblock Copolymer Electrolyte Thin Films." Macromolecular Rapid Communications 37, no. 3 (November 30, 2015): 221–26. http://dx.doi.org/10.1002/marc.201500562.

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45

Yin, Hang, Jie Tang, Kun Zhang, Shiqi Lin, Guangxu Xu, and Lu-Chang Qin. "Achieving High-Energy-Density Graphene/Single-Walled Carbon Nanotube Lithium-Ion Capacitors from Organic-Based Electrolytes." Nanomaterials 14, no. 1 (December 22, 2023): 45. http://dx.doi.org/10.3390/nano14010045.

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Developing electrode materials with high voltage and high specific capacity has always been an important strategy for increasing the energy density of lithium-ion capacitors (LICs). However, organic-based electrolytes with lithium salts limit their potential for application in LICs to voltages below 3.8 V in terms of polarization reactions. In this work, we introduce Li[N(C2F5SO2)2] (lithium Bis (pentafluoroethanesulfonyl)imide or LiBETI), an electrolyte with high conductivity and superior electrochemical and mechanical stability, to construct a three-electrode LIC system. After graphite anode pre-lithiation, the anode potential was stabilized in the three-electrode LIC system, and a stable solid electrolyte interface (SEI) film formed on the anode surface as expected. Meanwhile, the LIC device using LiBETI as the electrolyte, and a self-synthesized graphene/single-walled carbon nanotube (SWCNT) composite as the cathode, showed a high voltage window, allowing the LIC to achieve an operating voltage of 4.5 V. As a result, the LIC device has a high energy density of up to 182 Wh kg−1 and a 2678 W kg−1 power density at 4.5 V. At a current density of 2 A g−1, the capacity retention rate is 72.7% after 10,000 cycles.
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Golodnitsky, D., R. Kovarsky, H. Mazor, Yu Rosenberg, I. Lapides, E. Peled, W. Wieczorek, et al. "Host-Guest Interactions in Single-Ion Lithium Polymer Electrolyte." Journal of The Electrochemical Society 154, no. 6 (2007): A547. http://dx.doi.org/10.1149/1.2722538.

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47

Lee, Yan Ying, and Andre Weber. "Harmonization of Testing Procedures for All Solid State Batteries." ECS Meeting Abstracts MA2023-02, no. 2 (December 22, 2023): 340. http://dx.doi.org/10.1149/ma2023-022340mtgabs.

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All Solid State Batteries (ASSBs) with lithium-ion based conducting solid state electrolytes are considered the next generation high performance batteries. They enable high power densities due to their single ion conducting solid electrolyte, eliminating salt concentration gradients and related polarization losses in the cell, and ensuring an unrivalled level of safety due to their non-combustibility. Currently, a variety of ASSBs based on different solid state electrolytes such as polymers, thiophosphates, oxides and combinations thereof are being developed. One general problem with ASSBs is establishing and maintaining contact between the solid electrolyte and the active material phase during production and cycling, respectively. In conventional lithium-ion batteries (LiBs), this contact is ensured by the liquid state of the electrolyte, but in ASSBs, chemical expansion and contraction of the active material during lithiation and delithiation can detach this contact, resulting in decreased capacity due to the loss of active material. As a consequence, ASSBs are often operated under pressurized conditions, applying pressures significantly exceeding those in conventional LiBs. The same holds for the operating temperature window. Especially for polymer electrolyte-based ASSBs, they are often operated at higher temperatures to compensate for the low ionic conductivity of polymers at room temperature. With respect to cell testing, such operating requirements must be considered, and testing protocols are designed according to the individual requirements of the tested cell. This contribution aims to provide an overview of testing protocols for various types of ASSBs applied to different cells with polymer-, thiophosphate-, oxide-, and hybrid-electrolytes. These protocols will be compared with standardized testing routines for conventional LiBs. Based on this compilation, a harmonized testing procedure that covers the special requirements of the individual cell types and enables a fair comparison of different ASSBs is suggested. Additionally, examples of ASSB testing results will be discussed, taking into consideration the harmonization of different testing parameters.
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Rohan, Rupesh, Kapil Pareek, Weiwei Cai, Yunfeng Zhang, Guodong Xu, Zhongxin Chen, Zhiqiang Gao, Dan Zhao, and Hansong Cheng. "Correction: Melamine–terephthalaldehyde–lithium complex: a porous organic network based single ion electrolyte for lithium ion batteries." Journal of Materials Chemistry A 5, no. 44 (2017): 23382. http://dx.doi.org/10.1039/c7ta90241g.

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Correction for ‘Melamine–terephthalaldehyde–lithium complex: a porous organic network based single ion electrolyte for lithium ion batteries’ by Rupesh Rohan et al., J. Mater. Chem. A, 2015, 3, 5132–5139.
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M. Ramasekhara Reddy, Et al. "Comparative Performance Analysis of Different Cathode materials of Solid State Lithium ion Battery." International Journal on Recent and Innovation Trends in Computing and Communication 11, no. 11 (November 30, 2023): 465–78. http://dx.doi.org/10.17762/ijritcc.v11i11.9903.

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In this paper , a single dimensional solid state lithium(Li)-ion batteries are simulated at different C-rates to analyze the characteristics like discharge curves, electrolyte potential along the thickness of electrolyte and variation of concentration along the electrolyte and positive electrode by using multi-physics simulation software tool, COMSOL. Li-ion batteries can be designed with different cathode materials but every material has its own advantages and disadvantages along with their applications. So, the main focus of this paper is to compare the characteristics of different cathode materials of Li-ion battery at different C-rates with similar design operating parameters.
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Duignan, Timothy T., Marcel D. Baer, Gregory K. Schenter, and Christopher J. Mundy. "Real single ion solvation free energies with quantum mechanical simulation." Chemical Science 8, no. 9 (2017): 6131–40. http://dx.doi.org/10.1039/c7sc02138k.

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Single ion solvation free energies are one of the most important properties of electrolyte solutions and yet there is ongoing debate about what these values are. Only the values for neutral ion pairs are known.

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