Enhanced Li‐ion conductivity of polymer electrolytes with selective introduction of hydrogen in 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). 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 remain still low (Li‐ion transference number, ~ 0.2). In this work, we report new H‐containing anions, conceived on the basis of theoretical considerations, as an electrolyte salt for SPEs. SPEs comprising H‐containing anions achieve higher Li‐ion conductivities than the TFSI‐based ones, and those anions are electrochemically stable for various kinds of ASSLMBs (Li‐LiFePO4, Li‐S and Li‐O2 batteries). This opens a new avenue for designing safe and high‐performance ASSLMBs in the future.

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