Zhao Zhao, Wang Dandan, Gao Rui, Wen Guobin, Feng Ming, Song Guangxin, Zhu Jianbing, Luo Dan, Tan Huaqiao, Ge Xin, Zhang Wei, Zhang Yujun, Zheng Lirong, Li Haibo, Chen Zhongwei
Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education, Jilin Normal University, Changchun, 130103, China.
Department of Chemical Engineering, University of Waterloo, 200 University Avenue West, Waterloo, Ontario, N2L 3G1, Canada.
Angew Chem Int Ed Engl. 2021 May 17;60(21):11910-11918. doi: 10.1002/anie.202100726. Epub 2021 Apr 9.
Efficient coupling solar energy conversion and N fixation by photocatalysis has been shown promising potentials. However, the unsatisfied yield rate of NH curbs its forward application. Defective typical perovskite, BaTiO , shows remarkable activity under an applied magnetic field for photocatalytic N fixation with an NH yield rate exceeding 1.93 mg L h . 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 adsorption and activation while facilitating fast charge separation under UV-vis irradiation.
通过光催化实现高效耦合太阳能转换和固氮已显示出有前景的潜力。然而，氨产率不尽人意限制了其进一步应用。有缺陷的典型钙钛矿BaTiO₃在施加磁场下对光催化固氮表现出显著活性，氨产率超过1.93 mg L⁻¹ h⁻¹。通过调控表面自旋态和氧空位，激发了内电场和外磁场之间的电磁协同效应。X射线吸收光谱和密度泛函理论计算揭示了通过操纵氧空位以及诱导洛伦兹力和自旋选择性效应来调节电子和磁性性质。电磁效应抑制了半导体纳米材料中光激发载流子的复合，在紫外-可见光照射下协同促进氮的吸附和活化，同时促进快速电荷分离。
