Abstract
Electrocatalytic nitrogen reduction reaction(NRR)is considered as an attractive approach for ammonia synthesis under mild conditions.A bottleneck of NRR is the exploration of efficient catalysts for accel-erating reaction kinetics,among which heterogeneous structures possessing distinct atomic arrangement could modify electronic structure,and therefore altering their NRR activity.Here,we report a facile strat-egy for fabricating hetero-phase metal oxides derived from metal organic framework that are further integrated with Au nanoparticles as NRR catalysts.The phase composition of zirconia can be easily ad-justed by simply changing the reaction temperature,where the monoclinic and tetragonal phases with the roughly close proportions have a distinct interface,leading to a strong interaction between Au and ZrO2.The enhanced interaction renders Au to be more electropositive and facilitates stronger binding to N2.As a result,a remarkable ammonia yield of 22.32 μg h-1 mgcat.-1 and a Faradaic efficiency of 31.92％can be achieved at low overpotential.This work is expected to pave the way for the design of hetero-geneous structures and the exploration of hetero-phase nanostructures in boosting the electrocatalytic NRR.
维普
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