物理化学学报2025，Vol.41Issue(8)：115-125,11.DOI:10.1016/j.actphy.2025.100083
Co/Mn/Mo掺杂加速NiSe2重构以提高其电催化尿素氧化性能
Accelerating the reconstruction of NiSe2 by Co/Mn/Mo doping for enhanced urea electrolysis
摘要
Abstract
As a highly promising renewable energy technology,the urea oxidation reaction(UOR)not only enables efficient utilization of urea wastewater but also provides an effective alternative for hydrogen production via water electrolysis,thereby reducing the energy consumption of conventional electrolysis.Therefore,the development of UOR catalysts with high catalytic activity and long-term stability is of great significance for advancing clean energy technologies.In this study,a nickel-based selenide catalyst(NiCoMnMo-Se)with coexisting nanoparticles and nanosheets was synthesized using a NaBH4 reduction and selenization strategy.X-ray photoelectron spectroscopy(XPS),ultraviolet-visible(UV-vis)and in situ bode phase plots,revealed that the synergistic effect of Mn and Mo regulated the electronic structure of Ni/Co,enhancing the conductivity of selenide and accelerating charge transfer kinetics,which facilitates the rapid transformation of Ni2+/Co2+into active Ni3+/Co3+and significantly reduces the onset potential of NiCoMnMo-Se.During the UOR process,Mo and Se are oxidized to form molybdate and selenate,which subsequently dissolve into the electrolyte.This transformation results in the partial conversion of the original spherical nanoparticle surfaces into nanosheets,thereby exposing more Ni(Co)OOH active sites and significantly enhancing the UOR reaction.Additionally,the introduction of Mn stabilizes the active sites,thereby improving the overall stability of the catalyst.As anticipated,the synthesized NiCoMnMo-Se catalyst demonstrates outstanding electrocatalytic performance and stability in the UOR process,achieving a current density of 50 mA·cm-2 at a potential of only 1.38 V vs.RHE(reversible hydrogen electrode),with a voltage increase of only 3.0%after 50 h of operation at a 50 mA·cm-2.When NiCoMnMo-Se and commercial Pt/C were assembled into a dual-electrode system for alkaline urea electrolysis,it only requires 1.59 V vs.RHE to achieve a current density of 50 mA·cm-2.This paper designs an efficient and stable Ni-based selenide catalyst,which is expected to promote the further development of selenides in relevant energy technologies.关键词
尿素氧化反应/制氢/NiCoMnMo-Se/协同效应/尿素电解/镍基硒化物Key words
Urea oxidation reaction/Hydrogen production/NiCoMnMo-Se/Synergetic effect/Urea electrolysis/Ni-based selenide分类
化学化工引用本文复制引用
雷明杰,潘园,张玉微,魏笛野,高平,胡文婷,林可心,孙秀娟,张澔珅,钱烨,康彤玥,吴秀琳,廖海龙..Co/Mn/Mo掺杂加速NiSe2重构以提高其电催化尿素氧化性能[J].物理化学学报,2025,41(8):115-125,11.基金项目
The project was supported by the Scientific Research Fund of Hunan Provincial Education Department(23B0114),the Natural Science Foundation of Hunan Province(2024JJ5368),the National Natural Science Foundation of China(22122402),and the Natural Science Foundation of Guangdong Province(2021B1515020048).湖南省教育厅科研基金(23B0114),湖南省自然科学基金(2024JJ5368),国家自然科学基金(22122402)和广东省自然科学基金(2021B1515020048)资助项目 （23B0114）
