Critical factors to inhibit water-splitting side reaction in carbon-based electrode materials for zinc metal anodes

Zinc metal anodes(ZMA)have high theoretical capacities(820 mAh g−1 and 5855 mAh cm−3)and redox potential(−0.76 V vs.standard hydrogen electrode),similar to the electrochemical voltage window of the hydrogen evolution reaction(HER)in a mild acidic electrolyte system,facilitating aqueous zinc batteries competitive in next-generation energy storage devices.However,the HER and byproduct formation effectuated by water-splitting deteriorate the electrochemical performance of ZMA,limiting their application.In this study,a key factor in promoting the HER in carbon-based electrode materials(CEMs),which can provide a larger active surface area and guide uniform zinc metal deposition,was investigated using a series of threedimensional structured templating carbon electrodes(3D-TCEs)with different local graphitic orderings,pore structures,and surface properties.The ultramicropores of CEMs are the determining critical factors in initiating HER and clogging active surfaces by Zn(OH)2 byproduct formation,through a systematic comparative study based on the 3D-TCE series samples.When the 3D-TCEs had a proper graphitic structure with few ultramicropores,they showed highly stable cycling performances over 2000 cycles with average Coulombic efficiencies of≥99%.These results suggest that a well-designed CEM can lead to high-performance ZMA in aqueous zinc batteries.