Jiang Wenshuai, Zhao Yajie, Zong Xupeng, Nie Haodong, Niu Lijuan, An Li, Qu Dan, Wang Xiayan, Kang Zhenhui, Sun Zaicheng
Center of Excellence for Environmental Safety and Biological Effects, Beijing Key Laboratory for Green Catalysis and Separation, Department of Chemistry and Biology, Beijing University of Technology, 100 Pingleyuan, Beijing, 100124, P. R. China.
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Department, Soochow University, 199 Ren'ai Road, Suzhou, 215123, Jiangsu, P. R. China.
Angew Chem Int Ed Engl. 2021 Mar 8;60(11):6124-6129. doi: 10.1002/anie.202015779. Epub 2021 Jan 28.
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 GaN site is integrated into a polymeric carbon nitride (CN) photocatalyst (GCN), which displays an excellent H production rate of 9904 μmol h g . It is 162 and 3.3 times higher than that of CN with the absence (61 μmol h g ) and presence (2981 μmol h g ), respectively, of 1.0 wt % Pt. Under light irradiation the electron is injected and stored at the GaN 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 GaN promotes proton adsorption in the excited state. The positive adsorption energy drives H desorption from GaN after passing the electron to the proton. This work opens up opportunities for exploring a novel catalyst for H production.
光催化剂体系通常由催化剂和助催化剂组成，以实现光吸收、电子 - 空穴分离和表面反应。开发一种具有所有功能的单一光催化剂以降低效率损失是一项挑战。在此，将活性氮化镓位点整合到聚合物氮化碳（CN）光催化剂（GCN）中，其显示出9904 μmol h⁻¹ g⁻¹ 的优异产氢速率。分别比不含1.0 wt% Pt（61 μmol h⁻¹ g⁻¹）和含1.0 wt% Pt（2981 μmol h⁻¹ g⁻¹）的CN高出162倍和3.3倍。在光照射下，电子被注入并存储在氮化镓位点（LUMO所在位置）。HOMO分布在芳香环上，导致空间电荷分离。瞬态光电压揭示了GCN的电子存储能力。负的氮化镓促进激发态下的质子吸附。正的吸附能在将电子传递给质子后驱动氢从氮化镓上解吸。这项工作为探索新型产氢催化剂开辟了机会。
