Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products

Bao, Haihong; Qiu, Yuan; Peng, Xianyun; Wang, Jia-ao; Mi, Yuying; Zhao, Shunzheng; Liu, Xijun; Liu, Yifan; Cao, Rui; Zhuo, Longchao; Ren, Junqiang; Sun, Jiaqiang; Luo, Jun; Sun, Xuping

doi:10.1038/s41467-020-20336-4

Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products

Journal Article · Mon Jan 11 00:00:00 EST 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-20336-4· OSTI ID:1811911

Bao, Haihong ^[1]; Qiu, Yuan ^[1]; Peng, Xianyun ^[1]; ^[2]; Mi, Yuying ^[1]; Zhao, Shunzheng ^[3]; ^[1]; ^[4]; Cao, Rui ^[5]; ^[6]; Ren, Junqiang ^[7]; Sun, Jiaqiang ^[8]; ^[1]; ^[9]

Tianjin Univ. of Technology, Tianjin (China). Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices
Univ. of Jinan (China). School of Material Science and Engineering,
Univ. of Science and Technology, Beijing (China). Dept. of Environmental Engineering
Tianjin Univ. of Technology, Tianjin (China). Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab of Photoelectric Materials & Devices; Civil Aviation Univ. of China, Tianjin (China). Key Laboratory of Civil Aviation Thermal Hazards Prevention and Emergency Response
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Xi'an Univ. of Technology, Xi'an, Shanxi (China). School of Materials Science and Engineering
Lanzhou Univ. of Science and Technology, Lanzhou, Gansu (China). State Key Lab of Advanced Processing and Recycling of Nonferrous Metals
Chinese Academy of Sciences (CAS), Beijing (China). Institute of Coal Chemistry, State Key Laboratory of Coal Conversion
Univ. of Electronic Science and Technology of China, Chengdu, Sichuan (China). Institute of Fundamental and Frontier Sciences

Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti₃C₂T_x MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at -0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu–O₃sites favor the C–C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Key R&D Program of China; National Natural Science Foundation of China; Tianjin Science Fund; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1811911

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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