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Cu/Mo2C synthesized through Anderson-type polyoxometalates modulate interfacial water structure to achieve hydrogen evolution at high current density

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Nano Research 2024年第4期17卷 2546-2554页

作者： dunyuan Jin Fen Qiao Yan Zhou Junfeng Wang Kecheng Cao Jing Yang Jikang Zhao Lei Zhou Haitao Li School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013China School of Physical Science and Technology and Shanghai Key Laboratory of High-resolution Electron Microscopy ShanghaiTech UniversityShanghai 201210China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China

The development of efficient non-precious metal catalysts is important for the large-scale application of alkaline hydrogen evolution reaction(HER).Here,we synthesized a composite catalyst of Cu and Mo_(2)C(Cu/Mo_(2)C)using Anderson-type polyoxometalates(POMs)synthesized by the facile soaking method as *** electronic interaction between Cu and Mo_(2)C drives the positive charge of Cu,alleviating the strong adsorption of hydrogen at the Mo site by modulating the d-band center of Mo_(2)*** studying the interfacial water structure using in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),we determined that the positively charged Cu crystals have the function of activating water molecules and optimizing the interfacial water *** interfacial water of Cu/Mo_(2)C contains a large amount of free water,which could facilitate the transport of reaction *** to activated water molecules and optimized interfacial water structure and hydrogen adsorption energy,the overpotential of Cu/Mo_(2)C is 24 mV at a current density of 10 mA·cm^(-2) and 178 mV at a current density of 1000 mA·cm^(-2).This work improves catalyst performance in terms of interfacial water structure optimization and deepens the understanding of water-mediated catalysis.

关键词： electrocatalytic hydrogen production interfacial water charge transport d band center in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)

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Selective photocatalytic CO2 reduction over Zn-based layered double hydroxides containing tri or tetravalent metals

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Science Bulletin 2020年第12期65卷 987-994,M0003页

作者： Xuyang Xiong Yufei Zhao Run Shi Wenjin Yin Yunxuan Zhao Geoffrey I.N.Waterhouse Tierui Zhang Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academmy of SciencesBeijing WO 190China center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China School of Physics and Electronic Science Hunan University of Science and TechnologyXiangtan 411201China School of Chemical Sciences The University of AucklandAuckland 1142New Zealand

Photocatalytic CO2 reduction holds promise as a future technology for the manufacture of fuels and commodity ***,factors controlling product selectivity remain poorly ***,we compared the performance of a homologous series of Zn-based layered double hydroxide(ZnM-LdH)photocatalysts for CO2 *** varying the trivalent or tetravalent metal cations in the ZnM-LdH photocatalysts(M=Ti4+,Fe3+,Co3+,Ga3+,Al3+),the product selectivity of the reaction could be precisely ***-LdH afforded CH4 as the main reduction product;ZnFe-LdH and ZnCo-LdH yielded H2 exclusively from water splitting;whilst ZnGa-LdH and ZnAl-LdH generated ***-situ diffuse reflectance infrared measurements,valence band XPS and density function theory calculations were applied to rationalize the CO2 reduction selectivities of the different ZnM-LdH *** analyses revealed that the d-band center(ed)position of the M3+or M4+cations controlled the adsorption strength of CO2 and thus the selectivity to carbon-containing products or *** with d-band centers relatively close to the Fermi level(Ti4+,Ga3+and Al3+)adsorbed CO2 strongly yielding CH4 or CO,whereas metal cations with d-band centers further from the Fermi level(Fe3+and Co3+)adsorbed CO2 poorly,thereby yielding H2 only(from water splitting).Our findings clarify the role of trivalent and tetravalent metal cations in LdH photocatalysts for the selective CO2 reduction,paving new ways for the development of improved LdH photocatalyst with high selectivities to specific products.

关键词： Photocatalytic CO2 reduction Layered double hydroxide Selectivity Tri/tetravalent metal cations d band center

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