Defect-modulated and heteroatom-functionalized Ti_(3−x)C_(2)T_(y)MXene 3D nanocavities induce growth of MoSe_(2)nanoflakes toward electrocatalytic hydrogen evolution in all pH electrolytes  

作　　者：Ming Du Xianzhi Yang Jian Zhang Wei Chen Huajie Huang Xinbao Zhu Xing’ao Li 

机构地区：[1]State Key Laboratory for Organic Electronics and Information Displays and Institute of Advanced Materials(IAM),Jiangsu National Synergetic Innovation Centre for Advanced Materials(SICAM),Nanjing University of Posts and Telecommunications(NJUPT),Nanjing 210023,China [2]College of Electronic and Optical Engineering and College of Flexible Electronics Nanjing University of Posts and Telecommunications(NJUPT),Nanjing 210023,China [3]New Energy Technology Engineering Lab of Jiangsu Province,College of Science,Nanjing University of Posts and Telecommunications(NJUPT),Nanjing 210023,China [4]College of Pharmaceutical and Chemical Engineering,Taizhou University,Jiaojiang 318000,China [5]College of Mechanics and Materials,Hohai University,Nanjing 210098,China [6]College of Chemical Engineering,Nanjing Forestry University,Nanjing 210037,China

出　　处：《Nano Research》2024年第7期6294-6304,共11页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.52072182 and 51872145);Natural Science Foundation of Jiangsu Province(No.BK20211278);the China Postdoctoral Science Foundation(Nos.2019M650120 and 2020M671554);the National Synergetic Innovation Center for Advanced Materials(SICAM);Postgraduate Research Practice Innovation Program of Jiangsu Province(No.KYCX22_0977).

摘　　要：Reducing kinetic energy barriers and developing accessible active sites are critical to deliver high hydrogen evolution reaction(HER)efficiency.In this paper,we synthesized defect-modulated and heteroatom(boron)-functionalized three-dimensional(3D)bowl-shaped Ti_(3−x)C_(2)T_(y)MXene(B-TCT)nanocavities coupled with the vertical growth of MoSe_(2)nanoflakes.The B-TCT@MoSe_(2)nanohybrids catalyst delivers the overpotentials of 49.9,52.7,and 67.8 mV to reach a HER current density of 10 mA·cm^(−2)under acidic,alkaline,and neutral conditions,respectively.Such outstanding HER activity is predominantly attributed to the heteroatom functionalization,self-adapting Ti vacancy(VTi)defect modulation,and spatial configuration design in the 3D B-TCT nanocavity,which synergistically regulate the electronic structure,activate the basal plane/edge unsaturated sites,and reduce the reaction energy barrier.Experimental and theoretical calculations demonstrate that strong heterogeneous interfacial bonding interactions between B-TCT and MoSe_(2)can dramatically reduce the free energy of hydrogen adsorption and facilitate efficient interfacial charge migration,thus essentially improving the HER kinetics.We used this 3D porous nanohybrid system assembled by defectrich lamellar structures to elucidate the advantageous synergistic effects of multiple mechanisms among defect structure,heteroatom functionalization,and interfacial coupling,which provided important insights for the development of efficient hybridtype catalysts.

关 键 词：electrocatalytic H_(2)evolution three-dimensional(3D)MXene nanocavity MoSe_(2)nanoflake self-adapting Ti vacancy defect heteroatom-functionalized interfacial interaction 

分 类 号：O64[理学—物理化学]