Enhanced electron separation on in-plane benzene-ring doped g-C3N4 nanosheets for visible light photocatalytic hydrogen evolution

• Published in: Applied catalysis. B, Environmental Vol. 244; pp. 459 - 464
• Main Authors: Liu, Jian, Yu, Yu, Qi, Ruilian, Cao, Changyan, Liu, Xiaoyan, Zheng, Yujun, Song, Weiguo
• Format: Journal Article
• Language: English
• Published: Amsterdam Elsevier B.V 05.05.2019; Elsevier BV
• Subjects: Benzene; Benzene-ring doping; Carbon nitride; Catalysis; Catalysts; Chemical energy; Clean energy; Copolymerization; Current carriers; Efficiency; Electromagnetic absorption; Electronic structure; Energy conversion; Energy conversion efficiency; Energy storage; Etching; Evolution; g-C3N4; Heterostructures; Hydrocarbons; Hydrogen; Hydrogen evolution; Hydrogen-based energy; In-plane; Nanosheets; NMR; Nuclear magnetic resonance; Organic chemistry; Photocatalysis; Polymerization; Quantum efficiency; Ring structures; Separation; Solar energy; Urea; g-C3N4; Hydrogen evolution; Photocatalysis; In-plane; Benzene-ring doping
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2018.11.070

Benzene-ring doped g-C3N4 nanosheets (BS-CN) exhibited extended light adsorption and enhanced separation/transfer of photoinduced holes and electrons, which promoted it an excellent visible-light-driven hydrogen evolution catalyst by 12-fold improvement. [Display omitted] •Homogeneous benzene-ring doped g-C3N4 nanosheets for photocatalytic hydrogen evolution.•Enhanced photocatalytic hydrogen evolution rate of 12.3 mmol h−1 g−1.•High quantum efficiency of 17.7% at 420 nm. Solar-to-chemical energy conversion by photocatalytic hydrogen evolution (PHE) is critical for reduction of the pollution and storage of clean energy. To improve the solar conversion efficiency, it is highly imperative to accelerate the photocarrier separation and transportation through materials design. Herein, we describe a highly effective PHE catalyst based on in-plane benzene-ring doped g-C3N4 nanosheets heterostructure through the thermal co-polymerization of urea and 4, 4'-sulfonyldiphenol (BPS) followed by a controlled heat-etching step. The solid-state 13C NMR confirms the existence of benzene-ring structure in g-C3N4 nanosheets. Experimental results and theoretical calculations show that the energy and electronic structure of the catalyst are optimally regulated, inducing increased light absorption and effectively accelerated separation of the photo-driven charge carriers. It exhibits enhanced photocatalytic hydrogen evolution efficiency with a PHE rate of 12.3 mmol h−1 g−1 (almost 12 times higher than that of pure g-C3N4 nanosheets) and the quantum efficiency of 17.7% at 420 nm.