Multiscale confinement nitridation in molybdenum carbide for efficient hydrogen production  

作　　者：Liming Dai Chenchen Fang Xiaoyuan Zhang Xuefeng Xu Xuanxuan Chen Xinyue Zong Xueming Hu Wenyao Zhang Liang Xue Pan Xiong Yongsheng Fu Jingwen Sun Junwu Zhu 

机构地区：[1]Key Laboratory for Soft Chemistry and Functional Materials,Ministry of Education,Nanjing University of Science and Technology,Nanjing 210094,Jiangsu,China

出　　处：《Journal of Energy Chemistry》2024年第7期61-69,共9页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(52372201,52125202,52202247);the Natural Science Foundation of Jiangsu Province(1192261031693);the Fundamental Research Funds for the Central Universities(30919011110,1191030558)。

摘　　要：The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inherent limitation of high density of empty valence band significantly reduces its catalytic reactivity by reason of strong hydrogen desorption resistance.Herein,we propose a multiscale confinement synthesis method to design the nitrogen-rich Mo_(2)C for modulating the band structure via decomposing the pre-coordination bonded polymer in a pressure-tight tube sealing system.Pre-bonded c/N-Mo in the coordination precursor constructs a micro-confinement space,enabling the homogeneous nitrogenization in-situ happened during the formation of Mo_(2)C.Simultaneously,the evolved gases from the precursor decomposition in tube sealing system establish a macro-confinement environment,preventing the lattice N escape and further endowing a continuous nitridation.Combining the multiscale confinement effects,the nitrogen-rich Mo2C displays as high as 25%N-Mo concentration in carbide lattice,leading to a satisfactory band structure.Accordingly,the constructed nitrogen-rich Mo_(2)C reveals an adorable catalytic activity for HER in both alkaline and acid solution.It is anticipated that the multiscale confinement synthesis strategy presents guideline for the rational design of electrocatalysts and beyond.

关 键 词：Molybdenum carbide Hydrogen evolution reaction Multiscale confinement synthesis Valence band modulation Nitrogen doping 

分 类 号：TQ116.2[化学工程—无机化工] TQ426