Self-adaptive strain-relaxation optimization for high-energy lithium storage material through crumpling of graphene

High-energy lithium battery materials based on conversion/alloying reactions have tremendous potential applications in new generation energy storage devices. However, these applications are limited by inherent large volume variations and sluggish kinetics. Here we report a self-adaptive strain-relaxed electrode through crumpling of graphene to serve as high-stretchy protective shells on metal framework, to overcome these limitations. The graphene sheets are self-assembled and deeply crumpled into pinecone-like structure through a contraction-strain-driven crumpling method. The as-prepared electrode exhibits high specific capacity (2,165 mAh g−1), fast charge-discharge rate (20 A g−1) with no capacity fading in 1,000 cycles. This kind of crumpled graphene has self-adaptive behaviour of spontaneous unfolding–folding synchronized with cyclic expansion–contraction volumetric variation of core materials, which can release strain and maintain good electric contact simultaneously. It is expected that such findings will facilitate the applications of crumpled graphene and the self-adaptive materials.