期刊
CHEMICAL ENGINEERING JOURNAL
卷 430, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132940
关键词
Photocatalysis; Carbon dioxide reduction; Ethanol; Hot electrons; LSPR effects
资金
- Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China [51888103]
The study presents a novel STO/Cu @ Ni/TiN nanomaterial for efficient photocatalytic conversion of CO2 into ethanol, using non-noble metallic materials to enhance the plasmonic effect. The results demonstrate high ethanol evolution rate and selectivity, with confirmation of the ethanol pathway through DFT calculations and isotope experiments.
Photocatalytic carbon dioxide (CO2) reduction to valuable chemicals (ethanol) is an ideal way to realize artificial photosynthesis. It is still extremely difficult to achieve the challenge for photocatalytic CO2 reduction to multi electronic products (C2H5OH). Here, we design the SrTiO3 (La Cr)/Cu @ Ni/TiN (STO/Cu @ Ni/TiN) to realize the high efficiency of photocatalytic CO2 reduction conversion into ethanol in the absence of sacrificial reagents. Furthermore, we use non-noble metallic materials such as Cu, Ni, and TiN to enhance the plasmonic effect for efficiently capturing solar full-spectrum energy instead of noble metals. Meanwhile, the TPD results show that Cu@Ni nanoparticles can enhance the chemical adsorption of CO2 molecules. STO/Cu @ Ni/TiN exhibit an optimal ethanol evolution rate of 21.3 mu mol/(h.gcat.) and the ethanol selectivity of 79%, which is the highest value for photocatalytic CO2 reduction to ethanol, among the best values of our knowledge. Furthermore, the pathway of ethanol is confirmed by density functional theory (DFT) calculations and the C-13 isotope experiment.
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