Abstract

Graphene-based electrodes with high gravimetric and high volumetric capacity simultaneously are crucial to the realization of high energy storage density, but still proved to be challenging to prepare. Herein, we report a three-dimensional porous graphene/Co aerogel with hierarchical porous structure and compressible features as a high-performance binder-free lithium-ion battery anode. In this composite aerogel, graphene nanosheets interconnect to form continuous macropores, and cobalt nanoparticles stemming from decomposition of cobalt salt not only react with carbon atoms of graphene to form nanopores on the graphene nanosheets, but also increase the conductivity of the aerogel. With efficient ion and electron transport pathways as well as high packing density, the compressed porous graphene/Co electrode exhibits significantly improved electrochemical performance including high gravimetric and volumetric capacity, excellent rate capability, and superior cycling stability. After compression, such a porous graphene/Co nanocomposite can deliver a gravimetric capacity of 900 mA h g−1 and a volumetric capacity of 358 mA h cm−3 at a current density of 0.05 A g−1. Furthermore, after 300 discharge/charge cycles at 1 A g−1, the specific capacity still remains at 163 mA h cm−3, corresponding to 90.5% retention of its initial capacity.

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