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Magnetic‐Field‐Stimulated Efficient Photocatalytic N<sub>2</sub> Fixation over Defective BaTiO<sub>3</sub> Perovskites

Zhao Zhao, Dandan Wang, Rui Gao, Guobin Wen, Ming Feng, Guangxin Song, Jianbing Zhu, Dan Luo, Huaqiao Tan, Xin Ge, Wei Zhang, Yujun Zhang, Lirong Zheng, Haibo Li, Zhongwei Chen

2021Angewandte Chemie International Edition236 citationsDOI

Abstract

Abstract Efficient coupling solar energy conversion and N 2 fixation by photocatalysis has been shown promising potentials. However, the unsatisfied yield rate of NH 3 curbs its forward application. Defective typical perovskite, BaTiO 3 , shows remarkable activity under an applied magnetic field for photocatalytic N 2 fixation with an NH 3 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.

Topics & Concepts

PhotocatalysisMaterials sciencePerovskite (structure)OxygenDensity functional theoryPhotochemistryAdsorptionCharge carrierChemistryCatalysisOptoelectronicsPhysical chemistryComputational chemistryCrystallographyBiochemistryOrganic chemistryAdvanced Photocatalysis TechniquesAmmonia Synthesis and Nitrogen ReductionPerovskite Materials and Applications