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Title: 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:
 [1];  [2];  [3];  [1];  [2];  [1];  [4];  [5]; ORCiD logo [6]; ORCiD logo [7]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Univ. of California, Berkeley, CA (United States). Howard Hughes Medical Inst.
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  5. Chinese Academy of Sciences (CAS), Shanxi (China). Inst. of Coal Chemistry
  6. Chinese Academy of Sciences (CAS), Shanxi (China). Inst. of Coal Chemistry; Synfuels China, Beijing (China)
  7. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division; Univ. of California, Berkeley, CA (United States). Howard Hughes Medical Inst.; Univ. of California, Berkeley, CA (United States). Dept. of Molecular and Cell Biology
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:  
AC02-05CH11231; 101528-002
Resource Type:
Published Article
Journal Name:
ACS Central Science
Additional Journal Information:
Journal Volume: 3; Journal Issue: 9; Journal ID: ISSN 2374-7943
Publisher:
American Chemical Society (ACS)
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 = {2017},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acscentsci.7b00316

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Structure-Sensitive CO 2 Electroreduction to Hydrocarbons on Ultrathin 5-fold Twinned Copper Nanowires
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Colloidal Covalent Organic Frameworks
journal, January 2017


Porous Molecular Solids and Liquids
journal, May 2017


Selectivity on Etching: Creation of High-Energy Facets on Copper Nanocrystals for CO 2 Electrochemical Reduction
journal, March 2016


Covalent Organic Frameworks with High Charge Carrier Mobility
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Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO 2 Fixation
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Underpotential Deposition at Single Crystal Surfaces of Au, Pt, Ag and Other Materials
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Cobalt(I) porphyrin catalysts of hydrogen production from water
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Manganese as a Substitute for Rhenium in CO 2 Reduction Catalysts: The Importance of Acids
journal, February 2013

  • Smieja, Jonathan M.; Sampson, Matthew D.; Grice, Kyle A.
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