Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 237, Issue -, Pages 68-73Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2018.05.066
Keywords
Photocatalysis; CO2 reduction; ZnS; Room-temperature synthesis; DFT calculations
Funding
- National Natural Science Foundation of China [21703065, 21633004, 51502075]
- Natural Science Foundation of Hebei Province [B2018209267]
- World Premier International Research Center Initiative (WPI Initiative) on Materials Nanoarchitectonics (MANA), MEXT, Japan
- National Basic Research Program of China (973 Program) [2014CB239301]
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An ideal photocatalyst that can promisingly convert CO2 should have suitable band gap and fully consider the activation of reaction. However, well-designed photocatalytic materials with these aspects are very limited. This study reports a highly efficient CO2 reduction photocatalyst based on ZnS nanocrystals which can be rapidly synthesized at room temperature and operated under solar light irradiation at all-inorganic reaction system. Two functional elements, Cu and Cd, are respectively used as dopant and cocatalyst of ZnS nanocrystal for selective CO2 reduction. Cu+ doping expands the photoabsorption of ZnS into visible light region and the simultaneous Cd2+ surface modification significantly improves the activity of CO2 reduction with 99% formic acid selectivity. A combination of charge density distribution and electronic state studies reveal that the Cd s orbital displays obviously higher density of states near band-edge with a relatively lower lying band center than that of Zn s orbital. This will greatly favor the charge transfer from conduction band of ZnS to the surface state created by Cd2+ for catalyzing CO2 reduction.
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