4.6 Article

Designing Advanced Electrolytes for Lithium Secondary Batteries Based on the Coordination Number Rule

Journal

ACS ENERGY LETTERS
Volume 6, Issue 12, Pages 4282-4290

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c02194

Keywords

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Funding

  1. International Science and Technology Cooperation of China [2019YFE0100200]
  2. National Nature Science Foundation of China [U20A20249, 21972108]
  3. Key R&D Plan of Hubei Province [2020BAA030]
  4. supercomputing system in the Supercomputing Center of Wuhan University

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This work presents a new concept of the coordination number (CN) rule to tune electrochemical compatibility of electrolytes, enabling reversible lithiation/delithiation of the graphite anode by introducing low-coordination-number solvents (LCNSs) into high-coordination-number solvent (HCNS) electrolytes. Infrared analysis and theoretical calculations confirm the working mechanism of the electrochemical compatibility based on the CN rule.
Advanced electrolytes play a key role in the development of next-generation lithium secondary batteries. However, many strong polar solvents, as a major component of the electrolyte, are incompatible with the commercialized graphite anode in Li-ion batteries. In this work, we propose a new concept of the coordination number (CN) rule to tune electrochemical compatibility of electrolytes by regulating the ion-solvent-coordinated (ISC) structure. Based on this rule, we introduced the low-coordination-number solvents (LCNSs) into the high-coordination-number solvent (HCNS) electrolytes to induce anions into the first solvation shell of Li+, forming the anion-induced ISC (AI-ISC) structure. The HCNS-LCNS electrolytes with the AI-ISC structure show enhanced reduction stability, enabling reversible lithiation/delithiation of the graphite anode. Infrared analysis and theoretical calculations confirm the working mechanism of the electrochemical compatibility in the HCNS-LCNS electrolytes based on the CN rule. Therefore, the CN rule provides guidance for the design of highly stable and multifunctional electrolytes to develop next-generation lithium secondary batteries.

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