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

A series of dehydrated MoS 2 /UiO-66(SH) 2 (MS/UiS) composites has been prepared as photocatalysts for N 2 fixation. Typically, 10% MS/UiS exhibits the best performance with an NH 4 + yield rate of 54.08 μmol∙g −1 ∙h −1 . 15 N isotope test confirmed that the sample 10% MS/UiS was most effective for reducing N 2 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 N 2 . The photogenerated electrons would transfer to the unsaturated Zr-O clusters while part of photogenerated electrons at the interface migrate to MS via Mo VI -O interactions between MS and UiS. These two electron transfer pathways effectively promote the separation of photogenerated carriers. The activated N 2 is reduced to ammonia by the synergistic effect of protonated hydrogen and photogenerated electrons. Finally, a possible N 2 fixation mechanism is proposed which emphasizes the significant roles of nitrogen activation and interface interaction in composites photocatalyst for improving photocatalytic performance.