Hetero-phase zirconia encapsulated with Au nanoparticles for boosting electrocatalytic nitrogen reduction

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 accelerating 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 strategy 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 adjusted 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 heterogeneous structures and the exploration of hetero-phase nanostructures in boosting the electrocatalytic NRR.