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Alleviating large stress is critical for high‐energy batteries with large volume change upon cycling, yet this still presents a challenge. Here, a gradient hydrogen‐bonding binder is reported for high‐capacity silicon‐based anodes that are highly desirable for the next‐generation lithium‐ion batteries. The well‐defined gradient hydrogen bonds, with a successive bond energy of −2.88– −10.04 kcal mol...
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