期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 285, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119800
关键词
Heterostructured electrocatalyst; Metal selenides; Methanol oxidation; Hydrogen evolution reaction; Synergistic active centers
资金
- National Natural Science Foundation of China [21805187, 21975163]
- Shenzhen Science and Technology Program [KQTD20190929173914967]
By constructing Cu2Se/Co3Se4 multivalent hetero-nanocrystals, it is possible to convert methanol upgrading into high-value formate, reducing energy consumption and eliminating CO2 emissions.
Integrating organic upgrading and hydrogen electrolysis is recently regarded as a win-win strategy. However, it is still challenging to construct efficient robust electrocatalysts to considerably minimize their energy demand for such coupled reaction and simultaneously avoid the emission of environment-unfriendly CO2. Herein, the Cu2Se/ Co3Se4 multivalent hetero-nanocrystals (CuCoSe-HNCs) are fabricated as efficient electrocatalysts through interfacial engineering, thus constructing abundant hetero-junctions on monodispersed CuCoSe-HNCs and facilitating the charge transfer at Cu-Se-Co hetero-interfaces. DFT studies reveal the multivalent CuCoSe-HNCs with hydroxylated surfaces, which possess complex species (Cu*-OOH, Co*-OOH, and SeOx) as synergistic active centers, thus effectively optimizing the surface adsorption/dissociation performance and suppress excessive oxidation to CO2. Hence, the methanol upgrading conversion to value-added formate is achieved at much low working potential (1.11V) with high faradaic efficiency (>98 %) and without CO2 emission, thus considerably decreasing the energy consumption for generating the only gas product of pure hydrogen.
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