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Photocatalyst for High‐Performance H<sub>2</sub> Production: Ga‐Doped Polymeric Carbon Nitride

Wenshuai Jiang, Yu Zhao, Xupeng Zong, Haodong Nie, Lijuan Niu, Li An, Dan Qu, Xiayan Wang, Zhenhui Kang, Zaicheng Sun

2021Angewandte Chemie International Edition186 citationsDOI

Abstract

Abstract 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 4 site is integrated into a polymeric carbon nitride (CN) photocatalyst (GCN), which displays an excellent H 2 production rate of 9904 μmol h −1 g −1 . It is 162 and 3.3 times higher than that of CN with the absence (61 μmol h −1 g −1 ) and presence (2981 μmol h −1 g −1 ), respectively, of 1.0 wt % Pt. Under light irradiation the electron is injected and stored at the GaN 4 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 4 promotes proton adsorption in the excited state. The positive adsorption energy drives H 2 desorption from GaN 4 after passing the electron to the proton. This work opens up opportunities for exploring a novel catalyst for H 2 production.

Topics & Concepts

PhotocatalysisMaterials scienceCatalysisGraphitic carbon nitrideDesorptionAdsorptionHOMO/LUMOPhotochemistryDopingSurface photovoltageAbsorption (acoustics)Carbon fibersOptoelectronicsChemistryPhysical chemistryOrganic chemistrySpectroscopyMoleculeComposite materialPhysicsQuantum mechanicsComposite numberAdvanced Photocatalysis TechniquesZnO doping and propertiesPerovskite Materials and Applications