期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 311, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121372
关键词
Plasma treatment; Amorphous carbon nitride (ACN); H2O2 production; Hierarchical nanostructure; N-2C-site vacancy; First-principles calculations
资金
- Jiangsu Key Science and Technology project [BE2019108]
- National Natural Science Foundation of China [21173041]
- Opening Project of Jiangsu Key Laboratory of Advanced Metallic Materials, China
Amorphous carbon nitride (ACN) with two nitrogen vacancy sites in one CN unit has been successfully prepared using a one-step H2 plasma approach. The ACN material exhibits a stable network structure, high specific surface area, and enhanced photocatalytic H2O2 production. The presence of an electrostatic potential drop and a new strong band tail in ACN contribute to improved charge carrier separation and enhanced visible-light absorption.
Carbon nitride (CN) with nitrogen vacancy is a robust photocatalyst with proven enhancing H2O2 production ability. However, nitrogen vacancy control is extremely challenging with the majority of reports representing it as a few vacancies. Herein, for the first time, the amorphous CN (ACN) with two N-2 C-site vacancies in one CN unit is prepared by a one-step H-2 plasma approach. First-principles calculations , experimental results provide consistent evidence that two N-2 C vacancies are located in one CN unit structure after amorphous transformation. Plasma-induced ACN is stable with a hierarchical continuous nanosheet network structure and exhibits an ul-trahigh specific surface area of ~405.76 m(2)g(-1), which is 83 times higher than that of pristine CN (4.89 m(2)g(-1)) and significantly enhanced photocatalytic H2O2 production, yielding 1874 mu molg(-1)h(-1). Besides, the existence potential drop of 2.61 eV for the electrostatic potential in ACN is key to charge carrier separation. Moreover, the amorphous transformation leads to a new strong band tail, which remarkably enhances the absorbance edge of ACN up to 593 nm, resulting in a wider range of visible-light absorption to enhance H2O2 production. The results have provided an effective approach for promoting the practical application of ACN in photocatalytic H2O2 production.
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