Catalytic photo-redox of simulated air into ammonia over bimetallic MOFs nanosheets with oxygen vacancies

催化作用 氧气 氧化还原 双金属片 化学 光化学 化学工程 无机化学 材料科学 有机化学 工程类
作者
Wenjun Zhao,Jiangzhou Qin,Wei Teng,Jincheng Mu,Chang Chen,Jun Ke,J.C. Huang,Baojun Liu,Shaobin Wang
出处
期刊:Applied Catalysis B-environmental [Elsevier BV]
卷期号:305: 121046-121046 被引量:43
标识
DOI:10.1016/j.apcatb.2021.121046
摘要

Solar-driven conversion of nitrogen (N 2 ) into ammonia (NH 3 ) is a promising alternative to the Haber-Bosch process, while still suffers from low conversion efficiency due to inactive N N bond. Herein, a novel pathway of photocatalytic air redox reaction (ARR) to ammonia via NO is proposed and tested over an effective catalyst of oxygen-vacancy-rich bimetallic Cu-Co organic framework ultrathin nanosheets (O VR -CuCo-MOFs NS) under visible light. The catalyst with unique oxygen defective sites shows an excellent NH 3 synthesis rate from air (287.76 ± 7.02 μmol g -1 ·h -1 ), which is 5.4-fold higher than that from pure N 2 . Moreover, experiments and theoretical calculations indicate that the transformation of air mainly follows a redox pathway, in which N 2 and O 2 can be trapped at the oxygen vacancies to generate nitric oxide (*NO) and further be reduced to ammonia by visible light. The ARR process shows a lower barrier of free energies in the onset activation step (*N 2 → *N-NO, −0.08 eV) and rate-limiting step (*NO → *NHO, 1.23 eV) compared with those of traditional nitrogen reduction (*N 2 → *N-NH, 1.48 eV and H 2 N-NH 2 → *NH 2 , 1.29 eV, respectively). This work provides a new and sustainable pathway for photo-driven ammonia synthesis. • Photocatalytic ammonia synthesis was achieved by a redox process of air. • Rich oxygen vacancies can promote the ammonia synthesis and photo/electro superiorities. • Experiment and theoretical calculation show less kinetic barrier of the redox possess. • The redox reaction provides a new strategy for green ammonia production.
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