期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 21, 页码 11910-11918出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202100726
关键词
BaTiO3; defect engineering; N-2 fixation; photocatalysis
资金
- National Natural Science Foundation of China [21978110, 51772126, 21801092]
- Program for the Development of Science and Technology of Jilin province [20190101009JH, 20190103100JH, 20190201309JC, 20200801040GH, 20200201187JC]
- Project of Development and Reform Commission of Jilin Province [2019C042-1, 2020C026-3]
- Graduate Innovation Project of Jilin Normal University [201941]
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Waterloo Institute for Nanotechnology
- University of Waterloo
Efficient photocatalytic nitrogen fixation with high NH3 yield rate was achieved under an applied magnetic field using defective BaTiO3 perovskite. Manipulation of surface spin states and oxygen vacancies stimulated an electromagnetic synergistic effect between internal and external fields, suppressing carrier recombination and promoting N-2 adsorption and activation.
Efficient coupling solar energy conversion and N-2 fixation by photocatalysis has been shown promising potentials. However, the unsatisfied yield rate of NH3 curbs its forward application. Defective typical perovskite, BaTiO3, shows remarkable activity under an applied magnetic field for photocatalytic N-2 fixation with an NH3 yield rate exceeding 1.93 mg L-1 h(-1). Through steered surface spin states and oxygen vacancies, the electromagnetic synergistic effect between the internal electric field and an external magnetic field is stimulated. X-ray absorption spectroscopy and density functional theory calculations reveal the regulation of electronic and magnetic properties through manipulation of oxygen vacancies and inducement of Lorentz force and spin selectivity effect. The electromagnetic effect suppresses the recombination of photoexcited carriers in semiconducting nanomaterials, which acts synergistically to promote N-2 adsorption and activation while facilitating fast charge separation under UV-vis irradiation.
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