Journal
SMALL
Volume 18, Issue 22, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202201391
Keywords
CO; (2) reduction; dual-metal sites; electrocatalysis; electronic effect; single-atom catalysts
Categories
Funding
- National Natural Science Foundation of China [21825802, 22138003, 22108083]
- Foundation of Advanced Catalytic Engineering Research Center of the Ministry of Education [2020AC006]
- Introduced Innovative R&D Team Leadership of Dongguan City [2020607263005]
- Natural Science Foundation of Guangdong Province [2017A030312005, 2018B030306050]
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In this study, the authors demonstrate that introducing HER-inert main-group metal single atoms adjacent to transition-metal single atoms can enhance the CO2RR to CO without inducing the HER side reaction. The dual-metal Cu and In single-site atoms prepared by pyrolysis show superior catalytic performance compared to their monometallic counterparts.
Single-atom sites can not only act as active centers, but also serve as promising catalyst regulators and/or promoters. However, in many complex reaction systems such as electrochemical CO2 reduction reaction (CO2RR), the introduction of single-atom regulators may inevitably induce the competitive hydrogen evolution reaction (HER) and thus reduce the selectivity. Here, the authors demonstrate that introducing HER-inert main-group metal single atoms adjacent to transition-metal single atoms can modify their electronic structure to enhance the CO2RR to CO without inducing the HER side reaction. Dual-metal Cu and In single-site atoms anchored on mesoporous nitrogen-doped carbon (denoted as Cu-In-NC) are prepared by the pyrolysis of a multimetallic metal-organic framework. Cu-In-NC shows a high faradic efficiency of 96% toward CO formation at -0.7 V versus reversible hydrogen electrode, superior to that of its monometallic single-atom counterparts. Density functional theory studies reveal that the HER-inert In sites can activate the adjacent Cu sites through electronic modifications, strengthening the binding of *COOH intermediate and thus boosting the electrochemical reduction of CO2 to CO.
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