MOF encapsulated sub-nm Pd skin/Au nanoparticles as antenna-reactor plasmonic catalyst for light driven CO2 hydrogenation
Nano Energy(2021)
摘要
Activation of CO2 with plasmon induced hot electrons has attracted great attention due to its moderate reaction conditions, but high-efficiency plasmonic catalysts still remains challenging. Herein, we designedly prepared an antenna-reactor plasmonic catalyst with core-shell structure, i.e. sub-nm Pd skin/Au NPs encapsulated within UiO-66-NH2 (Au@Pd@UiO-66-NH2-0.5) for CO2 hydrogenation under light-heat dual activation. Under the photo-thermal synergism, CO2 can be efficiently converted into CO and the optimal production rate reaches 3737 µmol/gmetal/h at 150 °C. Thereinto, ultrafast transient absorption spectroscopy reveals that the sub-nm Pd skin provides a longer time window for hot electron transfer and efficient retardation of energy dissipation. Theoretical calculations further confirm the significant reductions in HOMO-LUMO gap of CO2 and reaction energy barrier from CO2* to COOH* through adsorption of CO2 on sub-nm Pd skin, promoting its efficiency and selectivity. Our findings provide new insights into design of bimetallic plasmonic catalysts for low-temperature catalysis.
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关键词
Heterogeneous catalysis,Plasmonic catalysis,CO2 hydrogenation,Metal-organic frameworks (MOFs),Core shell structure
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