Hydrogenated Bismuth Molybdate Nanoframe for Efficient Sunlight-Driven Nitrogen Fixation from Air

摘要

Sunlight-driven dinitrogen fixation can lead to a novel concept for the production of ammonia under mild conditions. However, the efficient artificial photosynthesis of ammonia from ordinary air (instead of high pure N-2) has never been implemented. Here, we report for the first time the intrinsic catalytic activity of Bi2MoO6 catalyst for direct ammonia synthesis under light irradiation. The edge-exposed coordinatively unsaturated Mo atoms in an Mo-O coordination polyhedron can act as activation centers to achieve the chemisorption, activation, and photoreduction of dinitrogen efficiently. Using that insight as a starting point, through rational structure and defect engineering, the optimized Bi2MoO6 sunlight-driven nitrogen fixation system, which simultaneously possesses robust nitrogen activation ability, excellent light-harvesting performance, and efficient charge transmission was successfully constructed. As a surprising achievement, this photocatalytic system demonstrated for the first time ultra-efficient (1.3 mmolg g(-1) h(-1)) and stable sunlight-driven nitro-gen fixation from air in the absence of any organic scavengers.