Synergy of modulating in-plane pores and zincophilic sites on the flexible graphene paper for efficient and dendrite-free hosted Zn anode

The practical advancement of Zn-ion batteries (ZIBs) in the portable/wearable electronics field is still hindered by the notorious Zn dendrites formation and the lack of an appropriate host to construct a highly effective flexible Zn anode. Herein, we present a three-dimensional (3D) N-doped graphene paper framework with abundant in-plane pores (rHGP-N) as an efficient Zn plating/stripping scaffold. Remarkably, the rHGP-N paper electrode exhibits an unprecedentedly low Zn nucleation overpotential of 5.2 mV and maintains a high average Coulombic efficiency (∼99.3%) over a superior long Zn plating/stripping cycling of 1400 h. DFT calculation results demonstrate that pyrrolic-nitrogen on graphene possesses the strongest adsorption energy for Zn2+, serving as zincophilic sites to guide Zn uniform nucleation. Moreover, the finite elements simulation results illustrate that flexible graphene paper with abundant in-plane pores can mitigate structural stress and inhibit the formation of Zn dendrites by spatially homogenizing Zn2+ ions flux throughout the entire electrode. The assembled ZIBs full cell (rHGP-N@Zn//rHGP-N@Mn3(PO4)2) demonstrates an impressive volumetric energy density of 77 mWh/cm3, as well as excellent flexibility and mechanical stability with negligible capacity decay under harsh deformation conditions. Our approach can be potentially utilized in designing dendrite-free metal-based flexible anodes for Mg, Ca, or Al-ion batteries. [Display omitted] •3D N-doped graphene paper with abundant in-plane pores was applied for Zn plating.•N-doped sites of pyrrolic-N as zincophilic sites facilitate uniform Zn nucleation.•3D porous graphene paper frameworks spatially homogenizing the flux of Zn2+ ions.•Flexible and bendable of rHGP-N@Zn//rHGP-N@Mn3(PO4)2 ZIBs full cell was fabricated.