Journal
ACS CATALYSIS
Volume 11, Issue 18, Pages 11786-11792Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c02980
Keywords
metal-organic framework; copper; carbon dioxide; methane; electrocatalysis
Categories
Funding
- NSFC [21890380, 21821003]
- Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program [2017BT01C161]
- Science and Technology Key Project of Guangdong Province, China [2020B010188002]
- Guangzhou Science and Technology Project [202002030291]
- Guangdong Natural Science Funds for Distinguished Young Scholar [2018B030306009]
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In this study, a Cu-based metal-organic framework was introduced as a catalyst for the efficient and selective reduction of CO2 to CH4. The in situ-generated trigonal pyramidal Cu(I)N-3 was identified as the electrochemical active site, while the hydrogen-bonding interactions of adjacent aromatic hydrogen atoms played a key role in stabilizing key intermediates of carbon dioxide reduction and inhibiting the hydrogen evolution reaction, demonstrating a high performance in electroreduction of CO2 to CH4.
High-efficiency electrocatalysts for CO2 reduction reaction are extremely desirable to produce valuable hydrocarbon productions, as well as addressing the current environmental challenges. In this work, we introduce a Cu-based metal-organic framework as a catalyst for the efficient and selective reduction of CO2 to CH4 in neutral aqueous electrolytes. Detailed examination of [Cu4ZnCl4(btdd)(3)] (Cu-4-MFU-4l, H(2)btdd = bis(1H-1,2,3-triazolo-[4,5-b],[4',5'-i])dibenzo-[1,4]-dioxin) revealed the highest activity for yielding methane with a Faradaic efficiency of 92%/88% and a partial current density of 9.8/18.3 mA cm(-2) at a potential of -1.2/1.3 V (vs RHE). In situ X-ray absorption and infrared spectroscopy spectra, as well as density functional theory calculations, revealed that the in situ generated trigonal pyramidal Cu(I)N-3 acts as the electrochemical active site and that the strong coordination ability of the Cu(I)N-3 site and the synergistic effect of adjacent aromatic hydrogen atoms, via hydrogen-bonding interactions, play an important role in stabilizing the key intermediates of carbon dioxide reduction and inhibiting the hydrogen evolution reaction, thus showing a high performance of electroreduction of CO2 to CH4.
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