Hierarchically Interpenetrated and Reentrant Microcellular Frameworks for Stretchable Lithium Metal Batteries

Abstract

With the rapid development of human-friendly wearable devices, energy storage components are required to have skin-like stretchability or free-form to fit closer and more comfortably to the human body. This study introduces a hierarchically interpenetrated reentrant microcellular structure combined with 2D cellular graphene/MXene/carbon nanotubes (CNTs) and 3D cellular melamine foam. This composite structure works as a stretchable framework of lithium metal composite electrodes to provide stretchability for lithium metal electrodes, which are promising as next-generation energy storage systems. The interpenetrated but independent cellular structures successfully obtain stable structural deformability from the nonconductive and deformable melamine foam, while at the same time, high electrical conductivity, lithiophilicity, and mechanical stability of the graphene/CNT/MXene network serve as a lithium deposition support during the electrodeposition of lithium. The reentrant structure is fabricated by radial compressing the hierarchical cellular structures to take advantage of the structural stretchability of the accordion-like reentrant frameworks. The lithium-deposited composite electrodes exhibit much lower overpotential during Li stripping and plating than lithium metal foil anodes and show stable electrochemical performances under 30% of mechanical strain. The reentrant microcellular electrodes offer great potential for advanced designs of lithium metal electrodes for stretchable batteries with high energy density. Hierarchically interpenetrating reentrant structures of 2D cellular graphene/carbon nanotubes (CNT)/MXene networks and 3D open-cell melamine foam can be fabricated by sequential directional freezing, electroplating, and radial compression. Therefore, stretchable lithium metal electrodes can be implemented in a form in which independent lithium plating occurs only on the electrical skeleton, while the melamine foam is responsible for stretchability.image