Citation: NING Hui, WANG Wenhang, MAO Qinhu, ZHENG Shirui, YANG Zhongxue, ZHAO Qingshan, WU Mingbo. Catalytic Electroreduction of CO₂ to C₂H₄ Using Cu₂O Supported on 1-Octyl-3-methylimidazole Functionalized Graphite Sheets[J]. Acta Physico-Chimica Sinica, ;2018, 34(8): 938-944. doi: 10.3866/PKU.WHXB201801263 shu

Catalytic Electroreduction of CO₂ to C₂H₄ Using Cu₂O Supported on 1-Octyl-3-methylimidazole Functionalized Graphite Sheets

1.
State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum, Qingdao 266580, Shandong Province, P. R. China
2.
CAS Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China

Corresponding author: WU Mingbo, wumb@upc.edu.cn
Received Date: 3 January 2018
Revised Date: 23 January 2018
Accepted Date: 23 January 2018
Available Online: 26 August 2018
Fund Project: the National Natural Science Foundation of China U1662113The project was supported by the CAS Key Laboratory of Carbon Materials, China (KLCMKFJJ1706) and the National Natural Science Foundation of China (51372277, 51572296, U1662113)the National Natural Science Foundation of China 51572296the National Natural Science Foundation of China 51372277The project was supported by the CAS Key Laboratory of Carbon Materials, China KLCMKFJJ1706

The electrocatalytic reduction of CO₂ to C₂H₄ is a topic of great interest. It is known that the preparation of efficient catalysts for this transformation is the key factor that determines the yield of C₂H₄. In this study, we prepared 1-octyl-3-methylimidazole functionalized graphite sheets (ILGS) in a facile manner by the electro-exfoliation of pure graphite rod in an aqueous solution of 1-octyl-3-methylimidazolium chloride (OmimCl : H₂O = 1 : 5, V/V) at 10 V. They were then dispersed in an aqueous solution of copper chloride and sodium citrate. Subsequent reduction with sodium borohydride led to the formation of a composite comprised of cuprous oxide supported on Omim-functionalized graphite sheets (Cu₂O/ILGS). This composite was found to be an efficient catalyst for the electroreduction of carbon dioxide to ethylene. The as-made materials were characterized by transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and X-ray diffraction (XRD). The TEM images showed that the ILGS were composed of multiple layers of graphene. The XRD pattern and Raman spectrum indicated that the surface of the ILGS possessed several defects. In the electro-exfoliation process, the defects in the ILGS were modified in situ by covalent bonding with Omim groups, which was also confirmed by XPS. The Cu₂O nanoparticles with an average diameter of 5 nm were uniformly distributed on the surface of the ILGS because the Omim groups grafted to the graphite sheets acted as anchors and prevented their aggregation by the steric effect. The electrocatalytic activities of Cu₂O/ILGS for CO₂ reduction were measured at different voltages in 0.1 mol L^–1 KHCO₃ aqueous solution under ambient temperature and pressure. These experiments showed that the catalytic performance of the Cu₂O/ILGS composite was determined by cuprous oxide, while the ILGS displayed nearly no catalytic activity in the electroreduction of carbon dioxide. The faradaic efficiency of hydrogen and carbon dioxide reduction products changed with the reaction time because of the reduction of Cu₂O to Cu under the electroreduction conditions. The faradaic efficiency of ethylene was ~14.8% at –1.3 V (versus reversible hydrogen electrode). The performance of Cu₂O/ILGS in the catalytic electroreduction of carbon dioxide was attributed to the stabilization of the Cu₂O nanoparticles by the nest-like microstructures in the Cu₂O/ILGS composite.
- Cu₂O,
- Graphite sheets,
- CO₂ reduction,
- Ethylene,
- Ionic liquids
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Catalytic Electroreduction of CO2 to C2H4 Using Cu2O Supported on 1-Octyl-3-methylimidazole Functionalized Graphite Sheets

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通讯作者: 陈斌, bchen63@163.com

Catalytic Electroreduction of CO₂ to C₂H₄ Using Cu₂O Supported on 1-Octyl-3-methylimidazole Functionalized Graphite Sheets