Wavelength-sensitive photocatalytic H2 evolution from H2S splitting over g-C3N4 with S,N-codoped carbon dots as the photosensitizer  

作　　者：Zhanghui Xie Shan Yu Xiang-Bing Fan Shiqian Wei Limei Yu Yunqian Zhong Xue-Wang Gao Fan Wu Ying Zhou 

机构地区：[1]State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation,Southwest Petroleum University,Chengdu 610500,Sichuan,China [2]The Center of New Energy Materials and Technology,School of New Energy and Materials,Southwest Petroleum University,Chengdu 610500,Sichuan,China [3]Department of Engineering,University of Cambridge,Cambridge CB30FA,United Kingdom [4]College of Chemistry,Leshan Normal University,Leshan 614000,Sichuan,China [5]Technical Institute of Physics and Chemistry,Chinese Academy of Sciences,Beijing 100190,China

出　　处：《Journal of Energy Chemistry》2021年第1期234-242,I0008,共10页能源化学（英文版）

基　　金：financial support from the National Natural Science Foundation of China (U1862111 and 21702213);Cheung Kong Scholars Programme of China;Chinese Academic of Science “light of west China” Program;Provincial International Cooperation Project 2020YFH0118, Sichuan, China;Open Fund (PLN201802 and 201928) of State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation (Southwest Petroleum University);Open Fund of State Key Laboratory of Industrial Vent Gas Reuse (SKLIVGR-SWPU-2020-05)。

摘　　要：Photocatalytic splitting of hydrogen sulfide(H2S) for hydrogen evolution is a promising method to solve the energy and environmental issues.In this work,S,N-codoped carbon dots(S,N-CDs)/graphitic carbon nitride(g-C3N4) nanosheet is synthesized by hydrothermal method as an efficient photocatalyst for the decomposition of H2S.In addition to the characterization of the morphology and structure,chemical state,optical and electrochemical performances of S,N-CDs/g-C3N4,hydrogen evolution tests show that the activity of g-C3N4 is improved by introducing S,N-CDs,and the enhancement depends strongly on the wavelength of incident light.The photocatalytic hydrogen production rate of S,N-CDs/g-C3N4 composite reaches 832 μmol g-1h-1, which is 38 times to that of g-C3N4 under irradiation at 460 nm.Density functional theory calculations and electron paramagnetic resonance as well as photoluminescence technologies have altogether authenticated that the unique wavelength-dependent photosensitization of S,N-CDs on g-C3N4;meanwhile,a good match between the energy level of S,N-CDs and g-C3N4 is pivotal for the effective photocatalytic activity.Our work has unveiled the detailed mechanism of the photocatalytic activity enhancement in S,N-CDs/g-C3N4 composite and showed its potential in photocatalytic splitting of H2S for hydrogen evolution.

关 键 词：PHOTOSENSITIZATION S N-codoped carbon dots Hydrogen sulfide splitting Photocatalytic hydrogen evolution 

分 类 号：TQ116.2[化学工程—无机化工] O643.36[理学—物理化学] O644.1[理学—化学]