Lewis-Basic EDTA as a Highly Active Molecular Electrocatalyst for CO2 Reduction to CH4

doi:10.1002/anie.202110594

	Lewis-Basic EDTA as a Highly Active Molecular Electrocatalyst for CO2 Reduction to CH4
	Huang, Minxue 2,3; Gong, Shipeng 2,3; Wang, Changlai 1,2,3; Yang, Yang 2,3; Jiang, Peng 5; Wang, Pengcheng 2,3; Hu, Lin 4; Chen, Qianwang 2,3,4
刊名	ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
	2021-09-12
关键词	carbon dioxide carbon nanotubes electrocatalysis EDTA molecular catalysts
ISSN号	1433-7851
DOI	10.1002/anie.202110594
通讯作者	Chen, Qianwang(cqw@ustc.edu.cn)
英文摘要	The most active catalysts so far successful in hydrogenation reduction of CO2 are mainly heterogeneous Cu-based catalysts. The complex coordination environments and multiple active sites in heterogeneous catalysts result in low selectivity of target product, while molecular catalysts with well-defined active sites and tailorable structures allow mechanism-based performance optimization. Herein, we firstly report a single ethylenediaminetetraacetic acid (EDTA) molecular-level immobilized on the surface of carbon nanotube as a catalyst for transferring CO2 to CH4 with an excellent performance. This catalyst exhibits a high Faradaic efficiency of 61.6 % toward CH4, a partial current density of -16.5 mA cm(-2) at a potential of -1.3 V versus reversible hydrogen electrode. Density functional theory calculations reveal that the Lewis basic COO- groups in EDTA molecule are the active sites for CO2 reduction reaction (CO2RR). The energy barrier for the generation of CO from CO intermediate is as high as 0.52 eV, while the further protonation of CO to CHO follows an energetic downhill path (-1.57 eV), resulting in the high selectivity of CH4. This work makes it possible to control the product selectivity for CO2RR according to the relationship between the energy barrier of CO intermediate and molecular structures in the future.
资助项目	National Natural Science Foundation[51772283] ; National Natural Science Foundation[22072140] ; National Natural Science Foundation[21972145] ; Fundamental Research Funds for the Central Universities[WK2060000032] ; Hong Kong Scholars Program[XJ2019022]
WOS关键词	ETHYLENEDIAMINETETRAACETIC ACID COMPLEXES ; CARBON-DIOXIDE ; INFRARED-SPECTRA ; ELECTROREDUCTION ; EFFICIENT ; CATALYST ; CONVERSION
WOS研究方向	Chemistry
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000695014100001
资助机构	National Natural Science Foundation ; Fundamental Research Funds for the Central Universities ; Hong Kong Scholars Program
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/125271]
专题	中国科学院合肥物质科学研究院
通讯作者	Chen, Qianwang
作者单位	1.City Univ Hong Kong, Dept Mat Sci & Engn, Ctr Super Diamond & Adv Films, Kowloon, Hong Kong, Peoples R China 2.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Peoples R China 3.Univ Sci & Technol China, Dept Mat Sci & Engn, Hefei 230026, Peoples R China 4.Chinese Acad Sci, Anhui Prov Key Lab Condensed Matter Phys Extreme, High Magnet Field Lab, Hefei 230031, Peoples R China 5.Tsinghua Univ, Dept Chem, Beijing, Peoples R China
推荐引用方式 GB/T 7714	Huang, Minxue,Gong, Shipeng,Wang, Changlai,et al. Lewis-Basic EDTA as a Highly Active Molecular Electrocatalyst for CO2 Reduction to CH4[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2021.
APA	Huang, Minxue.,Gong, Shipeng.,Wang, Changlai.,Yang, Yang.,Jiang, Peng.,...&Chen, Qianwang.(2021).Lewis-Basic EDTA as a Highly Active Molecular Electrocatalyst for CO2 Reduction to CH4.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION.
MLA	Huang, Minxue,et al."Lewis-Basic EDTA as a Highly Active Molecular Electrocatalyst for CO2 Reduction to CH4".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021).