Boosting hydrogen evolution via work-function-accelerated electronic reconfiguration of Mo-based heterojunction  

功函促进钼基异质结电催化剂的电子结构重整提升其析氢反应活性

作　　者：Xiang Chen Shuai Feng Song Xie Yaping Miao Biao Gao Xuming Zhang Li Huang Yun Li Paul K.Chu Xiang Peng 陈想;冯帅;谢松;苗亚萍;高标;张旭明;黄莉;李筠;Paul KChu;彭祥(Hubei Key Laboratory of Plasma Chemistry and Advanced Materials,Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education,School of Materials Science and Engineering,Wuhan Institute of Technology,Wuhan 430205,China;Department of Physics,Department of Materials Science and Engineering,and Department of Biomedical Engineering,City University of Hong Kong,Hong Kong 999077,China;School of Textile Science and Engineering,Xi’an Polytechnic University,Xi’an 710048,China;The State Key Laboratory of Refractories and Metallurgy,Institute of Advanced Materials and Nanotechnology,Wuhan University of Science and Technology,Wuhan 430081,China;Guizhou Wujiang Hydropower Development Co.,Ltd.,Guiyang 550002,China)

机构地区：[1]Hubei Key Laboratory of Plasma Chemistry and Advanced Materials,Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education,School of Materials Science and Engineering,Wuhan Institute of Technology,Wuhan 430205,China [2]Department of Physics,Department of Materials Science and Engineering,and Department of Biomedical Engineering,City University of Hong Kong,Hong Kong 999077,China [3]School of Textile Science and Engineering,Xi’an Polytechnic University,Xi’an 710048,China [4]The State Key Laboratory of Refractories and Metallurgy,Institute of Advanced Materials and Nanotechnology,Wuhan University of Science and Technology,Wuhan 430081,China [5]Guizhou Wujiang Hydropower Development Co.,Ltd.,Guiyang 550002,China

出　　处：《Science China Materials》2025年第1期189-198,共10页中国科学(材料科学)(英文版)

基　　金：financially supported by the National Natural Science Foundation of China (52002294 and 22379116);Key Scientific Research Program of Department of Education of Hubei Province(D20231501);Graduate Innovative Fund of Wuhan Institute of Technology(CX2023082);City University of Hong Kong Donation Research Grants(DON-RMG 9229021 and 9220061);City University of Hong Kong Strategic Research Grant (SRG)(7005505)。

摘　　要：Molybdenum-based catalysts have demonstrated significant potential in the electrocatalytic hydrogen evolution reaction(HER).However,the limited exposure of active sites and strong hydrogen adsorption result in suboptimal performance.Herein,a Mo_(2)N±MoSe_(2) heterojunction is prepared on carbon cloth(MNS/CC)to enhance the HER.The strong electronic interaction between Mo_(2)N and MoSe_(2),combined with the lower work function of Mo_(2)N,creates an intrinsic electric field at the heterojunction interface,which markedly improves charge transfer efficiency.Additionally,the optimized electronic structure of Mo sites further enhances charge transfer and intrinsically catalytic activity in HER.As a result,MNS/CC requires overpotentials of mere 65 and 210 mV to achieve current densities of 20 mA cm^(−2) and 1 A cm^(−2),respectively,with a Tafel slope of only 96 mV dec−1.Moreover,MNS/CC maintains stable operation at 1 A cm^(−2) for 240 h without significant degradation.The results offer insights into the design of non-precious metal-based electrocatalysts for industrial hydrogen production.Mo基催化剂在电催化析氢反应(HER)中具有巨大应用潜力.然而,其活性位点的暴露不足、极强的氢吸附能力导致其催化性能未能充分体现.本文在碳布上构筑了Mo_(2)N–MoSe_(2)异质结(MNS),以增强Mo基催化剂的HER活性.由于MNS中的Mo_(2)N具有较低的功函数,能够在异质界面产生内建电场,显著提高了其在HER中电荷转移效率.此外,MNS中原子之间的强电子相互作用优化了Mo位点的电子结构,降低了氢吸附能力,进一步增强了其本征催化活性.因此, MNS催化剂产生20 m A cm^(-2)和1 A cm^(-2)的析氢电流密度所需的过电位仅为65和210 mV, Tafel斜率仅为96 mV dec_(-1).此外, MNS在1 A cm^(-2)电流密度下稳定运行240小时后,形貌、结构和性能均无明显变化.以上研究结果为工业大电流制氢所需的非贵金属基电催化剂的设计和合成提供了新思路.

关 键 词：water splitting hydrogen evolution reaction molybdenum-based catalyst HETEROJUNCTION electronic interaction 

分 类 号：TQ116.2[化学工程—无机化工] TQ426