Enhanced Lithium‐Ion Conductivity of Polymer Electrolytes by Selective Introduction of Hydrogen into the Anion

The anion chemistry of lithium salts plays a pivotal role in dictating the physicochemical and electrochemical performance of solid polymer electrolytes (SPEs), thus affecting the cyclability of all‐solid‐state lithium metal batteries (ASSLMBs). The bis(trifluoromethanesulfonyl)imide anion (TFSI−) h...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2019-06, Vol.58 (23), p.7829-7834
Main Authors: Zhang, Heng, Oteo, Uxue, Zhu, Haijin, Judez, Xabier, Martinez‐Ibañez, Maria, Aldalur, Itziar, Sanchez‐Diez, Eduardo, Li, Chunmei, Carrasco, Javier, Forsyth, Maria, Armand, Michel
Format: Article
Language:English
Subjects:
Anions
Batteries
Conductivity
Electrochemical analysis
Electrochemistry
Electrolytes
Hydrogen
hydrogen-containing anions
Li-ion conductivity
Lithium
Lithium batteries
Molten salt electrolytes
Organic chemistry
Polymers
Salts
Solid electrolytes
sulfonimide
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Summary:The anion chemistry of lithium salts plays a pivotal role in dictating the physicochemical and electrochemical performance of solid polymer electrolytes (SPEs), thus affecting the cyclability of all‐solid‐state lithium metal batteries (ASSLMBs). The bis(trifluoromethanesulfonyl)imide anion (TFSI−) has long been studied as the most promising candidate for SPEs; however, the Li‐ion conductivities of the TFSI‐based SPEs still remain low (Li‐ion transference number: ca. 0.2). In this work, we report new hydrogen‐containing anions, conceived based on theoretical considerations, as an electrolyte salt for SPEs. SPEs comprising hydrogen‐containing anions achieve higher Li‐ion conductivities than TFSI‐based ones, and those anions are electrochemically stable for various kinds of ASSLMBs (Li–LiFePO4, Li–S, and Li–O2 batteries). This opens up a new avenue for designing safe and high‐performance ASSLMBs in the future. Substituted for success: A selective introduction of hydrogen into sulfonimide anions can improve the Li‐ion conductivity of polymer electrolytes by their interaction with the polymer matrices. This makes them promising building blocks for high‐performance all‐solid‐state lithium metal batteries.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201813700