Chemically Binding Scaffolded Anodes with 3D Graphene Architectures Realizing Fast and Stable Lithium Storage

Three-dimensional (3D) graphene has emerged as an ideal platform to hybridize with electrochemically active materials for improved performances. However, for lithium storage, current anodic guests often exist in the form of nanoparticles, physically attached to graphene hosts, and therefore tend to detach from graphene matrices and aggregate into large congeries, causing considerable capacity fading upon repeated cycling. Herein, we develop a facile double-network hydrogel-enabled methodology for chemically binding anodic scaffolds with 3D graphene architectures. Taking tin-based alloy anodes as an example, the double-network hydrogel, containing interpenetrated cyano-bridged coordination polymer hydrogel and graphene oxide hydrogel, is directly converted to a physical-intertwined and chemical-bonded Sn−Ni alloy scaffold and graphene architecture (Sn−Ni/G) dual framework. The unique dual framework structure, with remarkable structural stability and charge-transport capability, enables the Sn−Ni/G anode to exhibit long-term cyclic life (701 mA h g−1 after 200 cycles at 0.1 A g−1) and high rate performance (497 and 390 mA h g−1 at 1 and 2 A g−1, respectively). This work provides a new perspective towards chemically binding scaffolded low-cost electrode and electrocatalyst materials with 3D graphene architectures for boosting energy storage and conversion.