Effect of Halide Anions on the Electroreduction of CO2 to C2H4: A Density Functional Theory Study
文献类型：期刊论文
| 作者 | Ma, Xifei2,3; Xing, Lu2,3; Yao, Xiaoqian2; Zhang, Xiangping2; Liu, Lei1,2,4 |
| 刊名 | CHEMPHYSCHEM
 |
| 出版日期 | 2022-11-03 |
| 页码 | 9 |
| ISSN号 | 1439-4235 |
| 关键词 | CO2 reduction electrochemical catalysis C-C coupling density functional theory halide anions |
| DOI | 10.1002/cphc.202200502 |
| 英文摘要 | The halide anions present in the electrolyte improve the Faradaic efficiencies (FEs) of the multi-hydrocarbon (C2+) products for the electrochemical reduction of CO2 over copper (Cu) catalysts. However, the mechanism behind the increased yield of C2+ products with the addition of halide anions remains indistinct. In this study, we analysed the mechanism by investigating the electronic structures and computing the relative free energies of intermediates formed from CO2 to C2H4 on the Cu (100) facet based on density functional theory (DFT) calculations. The results show that formyl *CHO from the hydrogenation reaction of the adsorbed *CO acts as the key intermediate, and the C-C coupling reaction occurs preferentially between *CHO and *CO with the formation of a *CHO-CO intermediate. We then propose a free-energy pathway of C2H4 formation. We find that the presence of halide anions significantly decreases the free energy of the *CHOCH intermediate, and enhances desorption of C2H4 in the order of I->Cl->Br->F-. Lastly, the obtained results are rationalized through Bader charge analysis. |
| WOS关键词 | ELECTROCHEMICAL REDUCTION ; CARBON-DIOXIDE ; COPPER ELECTRODE ; CU ; SELECTIVITY ; ADSORPTION ; ETHYLENE ; CATALYSTS ; MULTICARBON ; INTERFACE |
| 资助项目 | DNL Cooperation Fund, CAS[DNL202007] ; National Natural Science Foundation of China[21978294] ; National Natural Science Foundation of China[21776281] |
| WOS研究方向 | Chemistry ; Physics |
| 语种 | 英语 |
| 出版者 | WILEY-V C H VERLAG GMBH |
| WOS记录号 | WOS:000878330000001 |
| 资助机构 | DNL Cooperation Fund, CAS ; National Natural Science Foundation of China |
| 源URL | [http://ir.ipe.ac.cn/handle/122111/55498]  |
| 专题 | 中国科学院过程工程研究所 |
| 通讯作者 | Yao, Xiaoqian; Liu, Lei |
| 作者单位 | 1.Wuhan Text Univ, Coll Chem & Chem Engn, Ctr Computat Chem, Wuhan 430200, Peoples R China 2.Chinese Acad Sci, Beijing Key Lab Ion Liquids Clean Proc, State Key Lab Multiphase Complex Syst, CAS Key Lab Green Proc & Engn,Inst Proc Engn, Beijing 100190, Peoples R China 3.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China 4.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China |
| 推荐引用方式 GB/T 7714 | Ma, Xifei,Xing, Lu,Yao, Xiaoqian,et al. Effect of Halide Anions on the Electroreduction of CO2 to C2H4: A Density Functional Theory Study[J]. CHEMPHYSCHEM,2022:9. |
| APA | Ma, Xifei,Xing, Lu,Yao, Xiaoqian,Zhang, Xiangping,&Liu, Lei.(2022).Effect of Halide Anions on the Electroreduction of CO2 to C2H4: A Density Functional Theory Study.CHEMPHYSCHEM,9. |
| MLA | Ma, Xifei,et al."Effect of Halide Anions on the Electroreduction of CO2 to C2H4: A Density Functional Theory Study".CHEMPHYSCHEM (2022):9. |
入库方式： OAI收割
来源：过程工程研究所
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