Nitrogen activation and surface charge regulation for enhancing the visible-light-driven N2 fixation over MoS2/UiO-66(SH)2

Abstract

A series of dehydrated MoS2/UiO-66(SH)2 (MS/UiS) composites has been prepared as photocatalysts for N2 fixation. Typically, 10% MS/UiS exhibits the best performance with an NH4+ yield rate of 54.08 μmol∙g−1∙h−1. 15N isotope test confirmed that the sample 10% MS/UiS was most effective for reducing N2 to ammonia. Such enhanced activity was due to the presence of abundant unsaturated Zr and Mo sites which would synergistically promote the adsorption and activation of N2. The photogenerated electrons would transfer to the unsaturated Zr-O clusters while part of photogenerated electrons at the interface migrate to MS via MoVI-O interactions between MS and UiS. These two electron transfer pathways effectively promote the separation of photogenerated carriers. The activated N2 is reduced to ammonia by the synergistic effect of protonated hydrogen and photogenerated electrons. Finally, a possible N2 fixation mechanism is proposed which emphasizes the significant roles of nitrogen activation and interface interaction in composites photocatalyst for improving photocatalytic performance.