Journal
ACS MATERIALS LETTERS
Volume 3, Issue 12, Pages 1729-1737Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsmaterialslett.1c00543
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Funding
- National Key Research and Development Program of China [2018YFA0209401, 2017YFA0206901]
- National Science Foundation of China [22025502, 21975051, 21773036]
- Science and Technology Commission of Shanghai Municipality [21DZ1206800, 19XD1420400]
- Shanghai Municipal Education Commission [2019-01-0700-07-E00045]
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The study introduces a dual metal atomic catalyst with Cu-Cu atoms demonstrating high efficiency and selectivity in CO electroreduction to C2+ products, while the Cu-Ni atoms mainly convert CO to CH4.
Monodispersed single metal atoms have been demonstrated with unique potentials for electroreduction of CO2 or CO, while the capability of producing multicarbon (C2+) products is still limited. In this work, we developed a dual metal atomic catalyst with uniform distributions of two adjacent Cu-Cu or Cu-Ni atoms anchored on nitrogen-doped carbon frameworks, featuring distinctive catalytic sites for CO electroreduction. Due to the synergistic effect between adjacent metal sites, the dual Cu-Cu atomic catalyst enables efficient CO electroreduction to C2+ products with an outstanding Faradaic efficiency of similar to 91% and a high partial current density over 90 mA.cm(-2). In contrast, the dual Cu-Ni atomic catalyst exhibits a remarkably different CO electroreduction selectivity mainly toward CH4. Theoretical calculations suggest that the dual Cu atomic sites facilitate the electroreduction of two CO molecules and subsequent carbon-carbon coupling toward ethylene and acetate, while the replacement of one of the dual Cu atoms with Ni results in too strong CO adsorption, and thus only the single Cu atom functions as the catalytic site for the C-1 reduction pathway.
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