Photocatalyst for High-Performance H2 Production: Ga-Doped Polymeric Carbon Nitride

被引:169
作者
Jiang, Wenshuai [1 ]
Zhao, Yajie [2 ]
Zong, Xupeng [1 ]
Nie, Haodong [2 ]
Niu, Lijuan [1 ]
An, Li [1 ]
Qu, Dan [1 ]
Wang, Xiayan [1 ]
Kang, Zhenhui [2 ,3 ]
Sun, Zaicheng [1 ]
机构
[1] Beijing Univ Technol, Ctr Excellence Environm Safety & Biol Effects, Beijing Key Lab Green Catalysis & Separat, Dept Biol & Chem, 100 Pingleyuan, Beijing 100124, Peoples R China
[2] Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, 199 Renai Rd, Suzhou 215123, Jiangsu, Peoples R China
[3] Macau Univ Sci & Technol, Macao Inst Mat Sci & Engn, Taipa 999078, Macau, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
carbon nitride; hydrogen; gallium; photocatalysis; structure elucidation; X-RAY-ABSORPTION; HYDROGEN EVOLUTION; CATHODE CATALYSTS; OXYGEN REDUCTION; CO2; REDUCTION; SINGLE-ATOM; G-C3N4; ELECTROCATALYSTS; SPECTROSCOPY; COCATALYST;
D O I
10.1002/anie.202015779
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A photocatalyst system is generally comprises a catalyst and cocatalyst to achieve light absorption, electron-hole separation, and surface reaction. It is a challenge to develop a single photocatalyst having all functions so as to lower the efficiency loss. Herein, the active GaN4 site is integrated into a polymeric carbon nitride (CN) photocatalyst (GCN), which displays an excellent H-2 production rate of 9904 mu mol h(-1) g(-1). It is 162 and 3.3 times higher than that of CN with the absence (61 mu mol h(-1) g(-1)) and presence (2981 mu mol h(-1) g(-1)), respectively, of 1.0 wt % Pt. Under light irradiation the electron is injected and stored at the GaN4 site, where the LUMO locates. The HOMO distributes on the aromatic ring resulting in spatial charge separation. Transient photovoltage discloses the electron-storage capability of GCN. The negative GaN4 promotes proton adsorption in the excited state. The positive adsorption energy drives H-2 desorption from GaN4 after passing the electron to the proton. This work opens up opportunities for exploring a novel catalyst for H-2 production.
引用
收藏
页码:6124 / 6129
页数:6
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