Amorphous Carbon Nitride with Three Coordinate Nitrogen (N3C) Vacancies for Exceptional NOx Abatement in Visible Light

被引:136
作者
Duan, Youyu [1 ,2 ]
Wang, Yang [1 ,2 ]
Gan, Liyong [1 ,2 ,3 ]
Meng, Jiazhi [1 ,2 ]
Feng, Yajie [1 ,2 ]
Wang, Kaiwen [4 ]
Zhou, Kai [5 ]
Wang, Cong [4 ]
Han, Xiaodong [4 ]
Zhou, Xiaoyuan [1 ,2 ,3 ,5 ]
机构
[1] Chongqing Univ, Coll Phys, Chongqing 401331, Peoples R China
[2] Chongqing Univ, Inst Adv Interdisciplinary Studies, Chongqing 401331, Peoples R China
[3] Chongqing Univ, State Key Lab Coal Mine Disaster Dynam & Control, Chongqing 401331, Peoples R China
[4] Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing 100024, Peoples R China
[5] Chongqing Univ, Analyt & Testing Ctr, Chongqing 401331, Peoples R China
基金
中国国家自然科学基金;
关键词
O-1; (2); amorphous carbon nitride (ACN); cyclicity; N3; (C)‐ site vacancies; NO oxidation;
D O I
10.1002/aenm.202004001
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Over the past several decades, much effort has been applied to atmospheric nitrogen oxide (NOx) abatement. The current techniques require high energy consumption and result in secondary pollution. Particularly, the removal of low dose (<200 ppm) of NOx has been very challenging. Though graphitic carbon nitride (g-CN), an eco-friendly and sustainable material was tried as a promising metal-free photocatalyst for NOx abatement. Herein, a one-step, energy efficient calcination approach is developed to prepare amorphous carbon nitride (ACN) with N3(C)-site vacancies. The visible-light responsive range is expanded and the activation barrier of N(sic)O triple bonds is sharply decreased by one order of magnitude; 0.19 eV when compared to the 2.22 eV of g-CN. These modifications allow the NOx removal efficiency of ACN to reach 57.1% which is among the highest in visible light. The unique N3(C)-site vacancies are well maintained after photocatalytic NO oxidation, which shows an exceptional structural stability. This boosts the generation of singlet oxygen (O-1(2)) and superoxide radical (O-center dot(2)-) for complete NO removal. This study sheds light on the active site design and photocatalytic performance enhancement of g-CN based materials by vacancy engineering.
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页数:10
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