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Highly Energy‐Dissipative, Fast Self‐Healing Binder for Stable Si Anode in Lithium‐Ion Batteries

A double‐wrapped binder has been rationally designed with high Young's modulus polyacrylic acid (PAA) inside and low Young's modulus bifunctional polyurethane (BFPU) outside to address the large inner stress of silicon anode with drastic volume changes during cycling. Harnessing the “hard to soft” gradient distribution strategy, the rigid PAA acts as a protective layer to dissipate the inner stress first during lithiation, while the elastic binder BFPU serves as a buffer layer to disperse residual stress, and thus avoids structural damage of rigid PAA. Moreover, the introduction of BFPU with fast self‐healing ability can dynamically recover the microcracks arising from large stress, further ensuring the integrity of silicon anode. This multifunctional binder with smart design of double‐wrapped structure provides enlightenment on enlarging the cycling life of high‐energy‐density lithium‐ion batteries that suffer enormous volume change during the cycling process.