An alternative route to single ion conductivity using multi-ionic salts

Chereddy, Sumanth; Chinnam, Parameswara Rao; Chatare, Vijay K.; DiLuzio, Stephen; Gobet, Mallory; Greenbaum, Steven; Wunder, Stephanie L.

doi:10.1039/c7mh01130j

Cited by 27 publications

(24 citation statements)

References 51 publications

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“…This applies not only to polyelectrolyte systems but also to those which tether the anions together through other means, for example, in polyoligomeric silsesquioxanes (POSS) functionalized with anionic moieties. 85…”

Section: Resultsmentioning

confidence: 99%

Ion Transport and the True Transference Number in Nonaqueous Polyelectrolyte Solutions for Lithium Ion Batteries

et al. 2019

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Nonaqueous polyelectrolyte solutions have been recently proposed as high Li + transference number electrolytes for lithium ion batteries. However, the atomistic phenomena governing ion diffusion and migration in polyelectrolytes are poorly understood, particularly in nonaqueous solvents. Here, the structural and transport properties of a model polyelectrolyte solution, poly(allyl glycidyl ether-lithium sulfonate) in dimethyl sulfoxide, are studied using all-atom molecular dynamics simulations. We find that the static structural analysis of Li + ion pairing is insufficient to fully explain the overall conductivity trend, necessitating a dynamic analysis of the diffusion mechanism, in which we observe a shift from largely vehicular transport to more structural diffusion as the Li + concentration increases. Furthermore, we demonstrate that despite the significantly higher diffusion coefficient of the lithium ion, the negatively charged polyion is responsible for the majority of the solution conductivity at all concentrations, corresponding to Li + transference numbers much lower than previously estimated experimentally. We quantify the ion–ion correlations unique to polyelectrolyte systems that are responsible for this surprising behavior. These results highlight the need to reconsider the approximations typically made for transport in polyelectrolyte solutions.

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Section: Resultsmentioning

confidence: 99%

Ion Transport and the True Transference Number in Nonaqueous Polyelectrolyte Solutions for Lithium Ion Batteries

et al. 2019

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“…[96][97][98][99] POSS is a cage-like organic-inorganic hybrid material (formula R 8 Si 8 O 12 ) with SiOSi as the internal inorganic framework and the substituted organic groups at eight vertices (Figure 2). POSS has attracted great attention due to its special nanostructure and easy modification, showing great potentials in separators, [100][101][102] liquid, [103,104] and solid state electrolytes [105] for batteries. Separators and electrolytes involving POSS and functionalized POSS are usually endowed with better thermal stability and higher safety.…”

Section: Macromolecule Polysiloxane and Possmentioning

confidence: 99%

Organosilicon‐Based Functional Electrolytes for High‐Performance Lithium Batteries

Wang

Chen

et al. 2021

Advanced Energy Materials

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Nowadays excessive consumption of fossil fuels due to population growth and industrial development induced serious energy and environmental crisis. To alleviate the ecological crisis and comply with the ever-increasing energy demand, developingThe electrolyte has been considered as a key factor toward higher energy density for Li-ion and Li-metal batteries. However, conventional electrolytes suffer from uncontrolled interfacial reactions and irreversible decomposition causing performance deterioration and potential safety hazard. Organosilicon compounds have attracted great interest as promising electrolyte components due to facile chemical modifications, low glass transition temperatures (T g ), superior chemical, and thermal stabilities. Considerable investigation efforts have been devoted to developing better overall performance of organosilicon-based electrolytes in the past few years. Herein, the recent research progress of organosilicon-based functional electrolytes for the development of liquid, gel, and solid state electrolytes in Li-ion and Li-metal batteries is summarized. Attention is devoted to various types of organosilicon such as silane, siloxane, polysiloxane, and polyhedral oligomeric silsesquioxanes in terms of molecular design, ionic conductivity, functions shown in batteries, thermal, chemical, electrochemical stability, safety, etc. The feasible strategies are also discussed that may promote the comprehensive electrochemical performances of organosilicon-based electrolytes in different types of electrolytes and batteries. Finally, the challenges facing organosilicon-based electrolytes and proposed their possible solutions are presented alongside promising development directions.

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“…Enlightened from the successful case of the graphite anode, which employs certain specific electrolyte additives such as vinyl carbonate, [361] allylethyl carbonate, [362] and lithium bis(oxalate) borate (LiBOB) [363] to form a protective nanosized coating film at the interface between the graphite anode and electrolytes, researchers have recently made great efforts to develop feasible strategy based on electrolyte additives to introduce protective interphases for Ni-based cathodes, that is, the CEI. [227][228][229][230][231][364][365][366][367][368][369][370] The facile and cost-effective approach can maximumly reduce the capacity loss when compared to other aforementioned methods including surface coating and/or doping, which generally need the complicated synthetic processes.…”

Section: Electrolyte Additives To Tune the Ceimentioning

confidence: 99%

Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies

Liang

Zhang

Zhao

et al. 2019

Adv Materials Inter

151

111

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Nickel‐rich layered transition‐metal oxides with high‐capacity and high‐power capabilities are established as the principal cathode candidates for next‐generation lithium‐ion batteries. However, several intractable issues such as the poor thermal stability and rapid capacity fade as well as the air‐sensitivity particularly for the Ni content over 80% have seriously restricted their broadly practical applications. The properties and nature of the stable surface/interface, where the Li+ shuttles back and forth between the cathode and electrolyte, play a significant role in their ultimate lithium‐storage performance and industrial processability. Thus, tremendous efforts are made to in‐depth understanding of the essential origins of surface/interface structure degradation and efficient surface modification methodologies are intensively explored. The purpose of the contribution is first to provide a comprehensive review of the up‐to‐date mechanisms proposed to rationally elucidate the surface/interface behaviors, and then, focus on recent developed strategies to optimize the surface/interface structure and chemistry including synthetic condition regulation, surface doping, surface coating, dual doping‐coating modification, and concentration‐gradient structure as well as electrolyte additives. Finally, the perspective on future research trends and feasible approaches toward advanced Ni‐rich cathodes with stable surface/interface is presented briefly.

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An alternative route to single ion conductivity using multi-ionic salts

Cited by 27 publications

References 51 publications

Ion Transport and the True Transference Number in Nonaqueous Polyelectrolyte Solutions for Lithium Ion Batteries

Ion Transport and the True Transference Number in Nonaqueous Polyelectrolyte Solutions for Lithium Ion Batteries

Organosilicon‐Based Functional Electrolytes for High‐Performance Lithium Batteries

Surface/Interface Structure Degradation of Ni‐Rich Layered Oxide Cathodes toward Lithium‐Ion Batteries: Fundamental Mechanisms and Remedying Strategies

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