Accelerating H^(*)desorption of hollow Mo_(2)C nanoreactor via in-situ grown carbon dots for electrocatalytic hydrogen evolution  

作　　者：Mengmeng Liu Yuanyuan Jiang Zhuwei Cao Lulu Liu Hong Chen Sheng Ye 

机构地区：[1]School of Materials and Chemistry,Anhui Agricultural University,Hefei 230036,Anhui,China

出　　处：《Journal of Energy Chemistry》2024年第9期464-471,共8页能源化学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (22372001);Starting Fund for Scientific Research of High-Level Talents, Anhui Agricultural University (rc382108);Anhui Provincial Key Research and Development Plan (2022e07020037);Innovation and Entrepreneurship Training Program for College Students (X202310364204, S202210364046, X202310364209)

摘　　要：Molybdenum carbide(Mo_(2)C)is a promising non-noble metal electrocatalyst with electronic structures similar to Pt for hydrogen evolution reaction(HER).However,strong H^(*)adsorption at the Mo sites hinders the improvement of HER performance.Here,we synthesized monodisperse hollow Mo_(2)C nanoreactors,in which the carbon dots(CD)were in situ formed onto the surface of Mo_(2)C through carburization reactions.According to finite element simulation and analysis,the CD@Mo_(2)C possesses better mesoscale diffusion properties than Mo_(2)C alone.The optimized CD@Mo_(2)C nanoreactor demonstrates superior HER performance in alkaline electrolyte with a low overpotential of 57 mV at 10 mA cm^(−2),which is better than most Mo_(2)C-based electrocatalysts.Moreover,CD@Mo_(2)C exhibits excellent electrochemical stability during 240 h,confirmed by operando Raman and X-ray diffraction(XRD).Density functional theory(DFT)calculations show that carbon dots cause the d-band center of CD@Mo_(2)C to shift away from Fermi level,promoting water dissociation and the desorption of H^(*).This study provides a reasonable strategy towards high-activity Mo-based HER eletrocatalysts by modulating the strength of Mo–H bonds.

关 键 词：Mo_(2)C nanoreactor Carbon dots H^(*)desorption Electrocatalytic hydrogen evolution 

分 类 号：TQ426[化学工程] TQ116.2