Experimental and theoretical investigation of sulfur-doped g-C_(3)N_(4)nanosheets/FeCo_(2)O_(4)nanorods S-scheme heterojunction for photocatalytic H_(2)evolution  

作　　者：Haitao Wang Lianglang Yu Jiahe Peng Jing Zou Weiping Gong Jizhou Jiang 

机构地区：[1]School of Chemistry and Environmental Engineering,School of Environmental Ecology and Biological Engineering,Key Laboratory of Green Chemical Engineering Process of Ministry of Education,Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education,Novel Catalytic Materials of Hubei Engineering Research Center,Wuhan Institute of Technology,Wuhan 430205,China [2]Guangdong Provincial Key Laboratory for Electronic Functional Materials and Devices,Huizhou University,Huizhou 516007,China

出　　处：《Nano Research》2024年第9期8007-8016,共10页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(No.62004143);the Key R&D Program of Hubei Province(No.2022BAA084);the Natural Science Foundation of Hubei Province(Nos.2021CFB133 and 2024AFB890).

摘　　要：g-C_(3)N_(4)emerges as a promising metal-free semiconductor photocatalyst due to its cost-effectiveness,facile synthesis,suitable visible light response,and robust thermal stability.However,its practical application in photocatalytic hydrogen evolution reaction(HER)is impeded by rapid carrier recombination and limited light absorption capacity.In this study,we successfully develop a novel g-C_(3)N_(4)-based step-scheme(S-scheme)heterojunction comprising two-dimensional(2D)sulfur-doped g-C_(3)N_(4)nanosheets(SCN)and one-dimensional(1D)FeCo_(2)O_(4)nanorods(FeCo_(2)O_(4)),demonstrating enhanced photocatalytic HER activity.The engineered SCN/FeCo_(2)O_(4)S-scheme heterojunction features a well-defined 2D/1D heterogeneous interface facilitating directed interfacial electron transfer from FeCo_(2)O_(4)to SCN,driven by the lower Fermi level of SCN compared to FeCo_(2)O_(4).This establishment of electron-interacting 2D/1D S-scheme heterojunction not only facilitates the separation and migration of photogenerated carriers,but also enhances visible-light absorption and mitigates electron-hole pair recombination.Band structure analysis and density functional theory calculations corroborate that the carrier migration in the SCN/FeCo_(2)O_(4)photocatalyst adheres to a typical S-scheme heterojunction mechanism,effectively retaining highly reactive photogenerated electrons.Consequently,the optimized SCN/FeCo_(2)O_(4)heterojunction exhibits a substantially high hydrogen production rate of 6303.5μmol·g^(-1)·h^(-1)under visible light excitation,which is 2.4 times higher than that of the SCN.Furthermore,the conjecture of the S-scheme mechanism is confirmed by in situ XPS measurement.The 2D/1D S-scheme heterojunction established in this study provides valuable insights into the development of high-efficiency carbon-based catalysts for diverse energy conversion and storage applications.

关 键 词：g-C_(3)N_(4) FeCo_(2)O_(4) S-scheme heterojunction photocatalytic hydrogen evolution reaction(HER) 

分 类 号：O64[理学—物理化学]