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
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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 |
DOI | 10.1002/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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