▎ 摘　　要

Graphene papers are widely studied as stable hosts to suppress lithium dendrite growth and accommodate the volumetric expansion for lithium metal anodes. Designing and constructing flexible graphene-based films with unique structures as stable hosts in large scales for lithium metal anodes is challenging in terms of their realistic applications. Herein, scalable three-dimensional (3D) holey reduced graphene oxide (HrGO) films with abundant as-tailored oxygen functional groups on hole defects of graphene nanosheets are successfully constructed as stable hosts for lithium metal anodes. The as-designed anodes deliver a stable voltage of 11 mV for 1900 h at a current density of 0.2 mA cm(-2). The achieved cycling times of the optimized Li-HrGO-4 film anodes are over 1000 and 800 h at current densities of 0.5 and 1.0 mA cm(-2), respectively. Simultaneously, the Li-HrGO-4 composite film anodes also exhibit superior rate performance as compared to pure lithium and Li-rGO film anodes when utilized in symmetric cells. The as-assembled LiFePO4/Li-HrGO-4 full cells show superior rate performance and retain capacity after 300 cycles at the rate of 1 C. Furthermore, first-principles calculations indicate that C-O and O-C=O groups on defects of HrGO surfaces lead to excellent lithium affinity and uniform deposition. Above all, the unique 3D holey structure with as-tailored oxygen defects and its design strategy holds a significant potential for the development of high energy-dense and stable metal batteries.