期刊
NANO ENERGY
卷 60, 期 -, 页码 43-51出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.nanoen.2019.03.024
关键词
CO2 electroreduction; Energy conversion; Carbon monoxide; Catalytic mechanism; Sulfur vacancy
类别
资金
- National Natural Science Foundation of China [21373091]
- Provincial Science and Technology Project of Guangdong [2014A030312007]
- Information and Network Engineering and Research Center, SCUT
Electrochemical conversion of carbon dioxide (CO2) into useful chemicals has attracted a lot of attention to store energy and reduce the greenhouse effect. Herein, a new electrocatalyst of carbon nanotubes coated with cadmium sulfide is reported, the faradaic efficiency (FE) of CO2 reduction reaction (CO2RR) to carbon monoxide (CO) is as high as 95%. We clearly demonstrate that sulfur vacancies (S-vacancies) are in-situ generated on the catalyst surface in CO2RR, which is evidenced by electron paramagnetic resonance spectra (EPR), in-situ differential electrochemical mass spectrometry (DEMS) and inductively-coupled plasma spectrometer (ICP). With the increase of S-vacancies, the catalytic activity of CO2RR to CO improve significantly and the charge-transfer resistance decrease. Combined with in-situ infrared absorption spectroscopy and density functional theory calculations, it can be concluded that the formation of S-vacancies changes the electron density of the catalyst surface and decreases the energy barrier for the conversion of COOH* to CO*. Finally, we tried to power electrochemical reduction of CO2 with solar panel under natural light conditions, the energy conversion efficiency on CdS-CNT catalyst from solar energy to CO has been calculated, predicting a hopeful application prospect in the future.
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