High-Performance Photocatalytic Reduction of Nitrogen to Ammonia Driven by Oxygen Vacancy and Ferroelectric Polarization Field of SrBi4Ti4O15 Nanosheets

被引:69
|
作者
Gao, Shuai [1 ,2 ,3 ]
Ji, Haodong [4 ]
Yang, Peng [5 ]
Guo, Ming [1 ,2 ,3 ]
Tressel, John [6 ]
Chen, Shaowei [6 ]
Wang, Qiang [1 ,2 ,3 ]
机构
[1] Capital Normal Univ, Lab Microsized Funct Mat, Beijing 100048, Peoples R China
[2] Normal Univ Beijing, Coll Elementary Educ, Beijing 100048, Peoples R China
[3] Capital Normal Univ, Dept Chem, Beijing 100048, Peoples R China
[4] Peking Univ, Shenzhen Grad Sch, Sch Environm & Energy, Shenzhen 518055, Peoples R China
[5] Northwest Univ, Coll Chem & Mat Sci, Key Lab Synthet & Nat Funct Mol Chem, 1 Xuefu Ave, Xian 710127, Peoples R China
[6] Univ Calif, Dept Chem & Biochem, 1156 High St, Santa Cruz, CA 95064 USA
基金
美国国家科学基金会;
关键词
charge separation; ferroelectric polarization; nitrogen adsorption; oxygen vacancy; photocatalytic nitrogen fixation; BI4TI3O12; NANOCRYSTALS; CO2; PHOTOREDUCTION; BIOBR NANOSHEETS; FIXATION; OXIDATION; WATER; RAMAN;
D O I
10.1002/smll.202206114
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Photo-responsive semiconductors can facilitate nitrogen activation and ammonia production, but the high recombination rate of photogenerated carriers represents a significant barrier. Ferroelectric photocatalysts show great promise in overcoming this challenge. Herein, by adopting a low-temperature hydrothermal procedure with varying concentrations of glyoxal as the reducing agent, oxygen vacancies (Vo) are effectively produced on the surface of ferroelectric SrBi4Ti4O15 (SBTO) nanosheets, which leads to a considerable increase in photocatalytic activity toward nitrogen fixation under simulated solar light with an ammonia production rate of 53.41 mu mol g(-1) h(-1), without the need of sacrificial agents or photosensitizers. This is ascribed to oxygen vacancies that markedly enhance the self-polarization and internal electric field of ferroelectric SBTO, and hence, facilitate the separation of photogenerated charge carriers and light trapping as well as N-2 adsorption and activation, as compared to pristine SBTO. Consistent results are obtained in theoretical studies. Results from this study highlight the significance of surface oxygen vacancies in enhancing the performance of photocatalytic nitrogen fixation by ferroelectric catalysts.
引用
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页数:13
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