globalchange  > 气候变化与战略
DOI: 10.1016/j.scib.2020.06.023
论文题名:
Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction
作者: Bai H.; Cheng T.; Li S.; Zhou Z.; Yang H.; Li J.; Xie M.; Ye J.; Ji Y.; Li Y.; Zhou Z.; Sun S.; Zhang B.; Peng H.
刊名: Science Bulletin
ISSN: 20959273
出版年: 2021
卷: 66, 期:1
起始页码: 62
结束页码: 68
语种: 英语
中文关键词: CO adsorption ; CO2 electroreduction ; Dimerization ; Hydrogenation
英文关键词: Adsorption ; Carbon dioxide ; Catalyst selectivity ; Copper metallography ; Density functional theory ; Electrolytic reduction ; Ethylene ; Fourier transform infrared spectroscopy ; High resolution transmission electron microscopy ; Hydrogenation ; Mathematical transformations ; Methane ; Nanocatalysts ; Product design ; Reaction intermediates ; Scanning electron microscopy ; X ray absorption spectroscopy ; Density functional theory studies ; Dimerization reactions ; Hydrocarbon product ; Methane production ; Reaction pathways ; Reduction conditions ; Scanning transmission electron microscopy ; Situ attenuated total reflection-Fourier transform infrared spectroscopy ; Copper compounds
英文摘要: Among all CO2 electroreduction products, methane (CH4) and ethylene (C2H4) are two typical and valuable hydrocarbon products which are formed in two different pathways: hydrogenation and dimerization reactions of the same CO intermediate. Theoretical studies show that the adsorption configurations of CO intermediate determine the reaction pathways towards CH4/C2H4. However, it is challenging to experimentally control the CO adsorption configurations at the catalyst surface, and thus the hydrocarbon selectivity is still limited. Herein, we seek to synthesize two well-defined copper nanocatalysts with controllable surface structures. The two model catalysts exhibit a high hydrocarbon selectivity toward either CH4 (83%) or C2H4 (93%) under identical reduction conditions. Scanning transmission electron microscopy and X-ray absorption spectroscopy characterizations reveal the low-coordination Cu0 sites and local Cu0/Cu+ sites of the two catalysts, respectively. CO-temperature programed desorption, in-situ attenuated total reflection Fourier transform infrared spectroscopy and density functional theory studies unveil that the bridge-adsorbed CO (COB) on the low-coordination Cu0 sites is apt to be hydrogenated to CH4, whereas the bridge-adsorbed CO plus linear-adsorbed CO (COB + COL) on the local Cu0/Cu+ sites are apt to be coupled to C2H4. Our findings pave a new way to design catalysts with controllable CO adsorption configurations for high hydrocarbon product selectivity. © 2020 Science China Press
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资源类型: 期刊论文
标识符: http://119.78.100.158/handle/2HF3EXSE/170190
Appears in Collections:气候变化与战略

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作者单位: State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science and Laboratory of Advanced Materials, Fudan University, Shanghai, 200438, China; Institute of Functional Nano & Soft Materials (FUNSOM) and Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China; Institute of Chemical Sciences and Engineering, École polytechnique fédérale de Lausanne, Lausanne, 1015, Switzerland; State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

Recommended Citation:
Bai H.,Cheng T.,Li S.,et al. Controllable CO adsorption determines ethylene and methane productions from CO2 electroreduction[J]. Science Bulletin,2021-01-01,66(1)
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