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Chinese Academy of Sciences Institutional Repositories Grid
Highly Selective Two-Electron Electrocatalytic CO2 Reduction on Single-Atom Cu Catalysts

文献类型:期刊论文

作者Xu, Chaochen1; Zhi, Xing1; Vasileff, Anthony1; Wang, Dan2; Jin, Bo1; Jiao, Yan1; Zheng, Yao1; Qiao, Shi-Zhang1
刊名SMALL STRUCTURES
出版日期2021
卷号2期号:1页码:7
关键词Cu single-atom catalysts density functional theory electrocatalytic CO2 reduction Faradaic efficiency limiting potential
DOI10.1002/sstr.202000058
英文摘要Cu-based electrocatalysts with high catalytic selectivity for the CO2 reduction reaction present a significant technological challenge. Herein, a catalyst comprised of Cu single atoms in a nitrogen-doped graphene matrix (Cu-N-4-NG) is developed for highly selective electrocatalytic reduction of CO2 to CO. The singleatom structure and coordination environment of Cu-N-4-NG are identified by synchrotron-based characterization. Compared to a conventional bulk Cu catalyst, Cu-N-4-NG achieves a Faradaic efficiency of 80.6% toward CO under a moderate applied potential of -1.0 V versus reversible hydrogen electrode (RHE). Kinetic experiments show that 1) the Cu-N-4 moiety favors the CO2 activation step and 2) the moiety-anchoring graphene facilitates water dissociation, which supplies protons for CO2 reduction. Moreover, density functional theory (DFT) calculations reveal that CO2 reduction is less hindered thermodynamically on Cu-N-4-NG compared to the competing hydrogen evolution reaction (HER) due to their limiting potential differences. Therefore, the highest CO selectivity is observed on Cu-N-4-NG over the bulk Cu catalyst due to more favorable kinetics and thermodynamics.
WOS关键词CARBON-DIOXIDE ; ELECTROCHEMICAL REDUCTION ; COPPER ; ELECTROREDUCTION ; SURFACE
资助项目Australian Research Council[DP160104866] ; Australian Research Council[DP170104464] ; Australian Research Council[FL170100154] ; Beacon of Enlightenment PhD Scholarship
WOS研究方向Chemistry ; Science & Technology - Other Topics ; Materials Science
语种英语
WOS记录号WOS:000736588600008
出版者WILEY
资助机构Australian Research Council ; Beacon of Enlightenment PhD Scholarship
源URL[http://ir.ipe.ac.cn/handle/122111/51590]  
专题中国科学院过程工程研究所
通讯作者Zheng, Yao; Qiao, Shi-Zhang
作者单位1.Univ Adelaide, Ctr Mat Energy & Catalysis, Sch Chem Engn & Adv Mat, Adelaide, SA 5005, Australia
2.Chinese Acad Sci, Inst Proc Engn, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714
Xu, Chaochen,Zhi, Xing,Vasileff, Anthony,et al. Highly Selective Two-Electron Electrocatalytic CO2 Reduction on Single-Atom Cu Catalysts[J]. SMALL STRUCTURES,2021,2(1):7.
APA Xu, Chaochen.,Zhi, Xing.,Vasileff, Anthony.,Wang, Dan.,Jin, Bo.,...&Qiao, Shi-Zhang.(2021).Highly Selective Two-Electron Electrocatalytic CO2 Reduction on Single-Atom Cu Catalysts.SMALL STRUCTURES,2(1),7.
MLA Xu, Chaochen,et al."Highly Selective Two-Electron Electrocatalytic CO2 Reduction on Single-Atom Cu Catalysts".SMALL STRUCTURES 2.1(2021):7.

入库方式: OAI收割

来源:过程工程研究所

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