Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction
Abstract
Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO2) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here in this paper, we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm2) at a potential of -0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.
- Authors:
-
- Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi 030001, China
- Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi 030001, China, Synfuels China, Beijing, 100195, China
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC); National Science Foundation (NSF)
- OSTI Identifier:
- 1389889
- Alternate Identifier(s):
- OSTI ID: 1416929
- Grant/Contract Number:
- 101528-002; AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- ACS Central Science
- Additional Journal Information:
- Journal Name: ACS Central Science Journal Volume: 3 Journal Issue: 9; Journal ID: ISSN 2374-7943
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Gong, Ming, Cao, Zhi, Liu, Wei, Nichols, Eva M., Smith, Peter T., Derrick, Jeffrey S., Liu, Yi-Sheng, Liu, Jinjia, Wen, Xiaodong, and Chang, Christopher J. Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction. United States: N. p., 2017.
Web. doi:10.1021/acscentsci.7b00316.
Gong, Ming, Cao, Zhi, Liu, Wei, Nichols, Eva M., Smith, Peter T., Derrick, Jeffrey S., Liu, Yi-Sheng, Liu, Jinjia, Wen, Xiaodong, & Chang, Christopher J. Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction. United States. https://doi.org/10.1021/acscentsci.7b00316
Gong, Ming, Cao, Zhi, Liu, Wei, Nichols, Eva M., Smith, Peter T., Derrick, Jeffrey S., Liu, Yi-Sheng, Liu, Jinjia, Wen, Xiaodong, and Chang, Christopher J. Wed .
"Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction". United States. https://doi.org/10.1021/acscentsci.7b00316.
@article{osti_1389889,
title = {Supramolecular Porphyrin Cages Assembled at Molecular–Materials Interfaces for Electrocatalytic CO Reduction},
author = {Gong, Ming and Cao, Zhi and Liu, Wei and Nichols, Eva M. and Smith, Peter T. and Derrick, Jeffrey S. and Liu, Yi-Sheng and Liu, Jinjia and Wen, Xiaodong and Chang, Christopher J.},
abstractNote = {Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO2) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here in this paper, we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm2) at a potential of -0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.},
doi = {10.1021/acscentsci.7b00316},
journal = {ACS Central Science},
number = 9,
volume = 3,
place = {United States},
year = {Wed Sep 13 00:00:00 EDT 2017},
month = {Wed Sep 13 00:00:00 EDT 2017}
}
https://doi.org/10.1021/acscentsci.7b00316
Web of Science
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