光催化
固氮
催化作用
氮气
材料科学
环境科学
环境化学
化学
化学工程
工程类
有机化学
作者
Xin Huang,Rui Du,Jingyu Ren,Xiang Li,Meng-Xi Fu,Shu-Ping Fu,Taoxia Ma,Li Guo,Razium Ali Soomro,Chunming Yang,Danjun Wang
标识
DOI:10.1021/acscatal.4c03183
摘要
The aerobic photocatalytic nitrogen reduction reaction (pNRR) is the photocatalytic synthesis of ammonia with air (N2/O2) instead of a high-purity nitrogen source, which can avoid the use of high-cost air separation equipment, thus reducing the production cost of synthetic ammonia. Nevertheless, the mechanism of the effect of oxygen (O2) on the structure and catalytic performance of photocatalysts in the aerobic pNRR is still unclear. Herein, a trace Bi0 loaded Bi2MO6 (M = Mo, W) was ingeniously synthesized by a solvothermal strategy, which demonstrated a superior aerobic pNRR performance. The mechanism of the aerobic pNRR was elucidated by quasi in situ X-ray photoelectron spectroscopy, in situ electron spin resonance and density functional theory calculation. The presence of O2 inhibited the formation of excess Bi0 by competing for photogenerated electrons and generating ·O2–, which dynamically renovated the structure of the catalyst. The polarization dipole field induced by an appropriate amount of Bi0 boosted the photocarrier spatial separation/transfer of the aerobic pNRR.
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