An oxygen-vacancy-rich polyoxometalate-aided Ag-based heterojunction electrocatalyst for nitrogen fixation
Polyoxometalates (POMs) with well-defined molecular structures are sustainable and promising catalysts for reducing nitrogen to ammonia under ambient conditions.In this study,oxy-gen-vacancy-rich AgPW11/Ag nanocube catalysts were synthesized via a one-pot method using POMs,reductants,and inducers.The oxygen-vacancy-rich AgPW11/Ag heterojunction catalyst ex-hibited a significant ammonia yield as high as 46.02±1.03 μg h-1 mg-1cat.and faradaic efficiency of 34.07±0.16％ at a potential of-0.2 V (vs.RHE),maintaining stable catalysis for 32 h without decay and greatly outperforming the Ag catalyst.The excellent catalytic performance and mechanism were established using density functional theory calculations.The robust interaction between the d orbitals of the Ag atom in AgPW1112e and π* orbitals of N2 activates the adsorbed N2 and promotes the conversion of the first protonation process *N2 to *N-NH (the potential determination step).This study provides a new avenue for designing stable Ag-based catalysts for nitrogen fixation.
万方数据
维普
