C-O bond activation and splitting behaviours of CO2 on a 4H-SiC surface a DFT study

doi:10.1039/c8cp04438d

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	C-O bond activation and splitting behaviours of CO2 on a 4H-SiC surface a DFT study
	Wang, D. D.; Zhang, L. L.; Han, D. X.; Niu, L.; Zhong, X.; Qu, X.; Yang, L. H.; Zhao, J. L.; Li, H. B.
	2018
发表期刊	Physical Chemistry Chemical Physics
ISSN	1463-9076
卷号	20 期号:42 页码:26846-26852
摘要	Conversion of CO2 into valuable chemicals can not only reduce the amount of CO2 in the atmosphere, but also realize the reuse of resources. It's well known that C-O bond activation and splitting are critical steps in the CO2 conversion process and it's crucial to employ an appropriate catalyst. Here, the adsorption and activation behaviors of a CO2 molecule on 4H-SiC surfaces were systematically investigated based on DFT calculations. Calculation results show that the CO2 molecule can anchor on 4H-SiC(0001) and (000 (1) over bar) surfaces. On the 4H-SiC(0001) surface, the adsorbed CO2 molecule prefers to dissociate with an energy barrier of 0.52-0.70 eV, producing an O adatom and a CO molecule on the surface. Further dissociation of the CO is hindered due to a large energy barrier of 2.12 eV. However, if a H atom is introduced, the CO molecule may combine with H into a CHO group and the reaction energy barrier is 1.69 eV. Moreover, the CHO group tends to transform into a CH group and an O adatom, a reaction in which a relatively low energy barrier of 0.09 eV needs to be surmounted. For the 4H-SiC(000 (1) over bar) case, the direct C-O bond dissociation energy barrier for CO2 is only 0.37 eV while further breaking of the C-O bond in CO is energetically unfavorable even with the help of a H atom. So the final products are an O adatom and CO chemisorbed on the 4H-SiC(000 (1) over bar) surface. All the calculation results demonstrate that the inert CO2 molecule can be effectively activated on both the 4H-SiC(0001) and (000 (1) over bar) surfaces and different splitting products could be obtained on the two different surfaces, implying that SiC is an applicable catalyst material for CO2 conversion with high efficiency and product selectivity.
关键词	electrocatalytic reduction carbon-dioxide adsorption conversion energy Chemistry Physics
DOI	10.1039/c8cp04438d
收录类别	SCI
引用统计
文献类型	期刊论文
条目标识符	http://ir.ciomp.ac.cn/handle/181722/60591
专题	中国科学院长春光学精密机械与物理研究所
推荐引用方式 GB/T 7714	Wang, D. D.,Zhang, L. L.,Han, D. X.,et al. C-O bond activation and splitting behaviours of CO2 on a 4H-SiC surface a DFT study[J]. Physical Chemistry Chemical Physics,2018,20(42):26846-26852.
APA	Wang, D. D..,Zhang, L. L..,Han, D. X..,Niu, L..,Zhong, X..,...&Li, H. B..(2018).C-O bond activation and splitting behaviours of CO2 on a 4H-SiC surface a DFT study.Physical Chemistry Chemical Physics,20(42),26846-26852.
MLA	Wang, D. D.,et al."C-O bond activation and splitting behaviours of CO2 on a 4H-SiC surface a DFT study".Physical Chemistry Chemical Physics 20.42(2018):26846-26852.

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