Magnetic-Field-Stimulated Efficient Photocatalytic N-2 Fixation Over Defective Batio3 Perovskites

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION(2021)

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摘要
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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关键词
BaTiO3, defect engineering, N-2 fixation, photocatalysis
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