调节Co3O4的价电子结构提高硝酸根还原制氨的催化活性

Electrochemical conversion of NO3− to NH3via the nitrate reduction reaction (NO3−RR) is a promising approach for ammonia production and storage “green hydrogen”. Co3O4 has shown satisfactory Faradaic efficiency toward $${\rm{N}}{{\rm{H}}_3}\,({\rm{F}}{{\rm{E}}_{{\rm{N}}{{\rm{H}}_3}}})$$ stability, making it potential electrocatalyst NO3−-to-NH3 conversion. However, high overpotential required triggering NO3−RR on limits its efficiency. In this study, we synthesized Cu-doped porous hollow nanospheres (Cu−Co3O4 PHNSs) NO3−RR. Cu-doping effectively reduced improved NH3 yield rate matrix without reducing $${\rm{F}}{{\rm{E}}_{{\rm{N}}{{\rm{H}}_3}}}$$ stability. Both experimental theoretical analyses demonstrated that up-shifted highest occupied state (HOS) Co3O4, narrowed energy barrier between HOS lowest unoccupied molecular orbital NO3−, thus electron transfer from thereby endowing as-prepared Cu−Co3O4 PHNSs with outstanding electrocatalytic activity durability This study provides novel perspective regulation electrochemical performance.