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Regulating local charges of atomically dispersed Moδ+ sites by nitrogen coordination on cobalt nanosheets to trigger water dissociation for boosted hydrogen evolution in alkaline media

引用

Journal of Energy Chemistry 2022年第9期31卷 125-132,I0004页

作者： Maoqi Cao Kang Liu Yao Song Chao Ma Yiyang Lin Huangjingwei Li Kejun Chen Junwei Fu Hongmei Li Jun Luo Yida Zhang Xusheng Zheng Junhua Hu Min Liu School of Chemistry and Chemical Engineering Qiannan Normal University for NationalitiesDuyun 558000GuizhouChina State Key Laboratory of Powder Metallurgy School of Physics and ElectronicsShenzhen Research InstituteSchool of Physical and ElectronicsCentral South UniversityChangsha 410083HunanChina School of Materials Science and Engineering Central South University of Forestry and TechnologyChangsha 410004HunanChina School of Materials Science and Engineering Hunan UniversityChangsha 410082HunanChina National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina

Now,Pt-based materials are still the best catalysts for hydrogen evolution reaction(HER).Nevertheless,the scarcity of Pt makes it impossible for the large-scale applications in *** cobalt is taken as an excellent HER catalyst due to its suitable H*binding,its alkali HER catalytic property need to be improved because of the sluggish water dissociation *** this work,nitrogen with small atomic radius and metallophilicity is employed to adjust local charges of atomically dispersed Mo^(δ+)sites on Co nanosheets to trigger water *** calculations suggest that the energy barrier of water dissociation can be effectively reduced by introducing nitrogen coordinated Mo^(δ+)*** realize this speculation,atomically dispersed Mo^(δ+)sites with nitrogen coordination of Mo(N)/Co were prepared via reconstruction of CoMoO_(4).High angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)and X-ray absorption spectroscopy(XAS)demonstrate the coordination of N atoms with atomically dispersed Mo atoms,leading to the local charges of atomically dispersed Mo^(δ+)sites in Mo(N)/*** measurement from ambient pressure X-ray photoelectron spectroscopy(AP-XPS)reveals that the Mo^(δ+)sites promote the adsorption and activation of water ***,the Mo(N)/Co exhibits an excellent activity,which need only an overpotential of 39 mV to reach the current density of 10 mA cm^(-2).The proposed strategy provides an advance pathway to design and boost alkaline HER activity at the atomic-level.

关键词： Charge localized Mo nitrogen coordination Co nanosheet Water dissociation Alkaline HER

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