Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO2
Abstract
Realization of heterogeneous electrochemical CO2-to-fuel conversion via molecular catalysis under high-flux conditions requires the assembly of large quantities of reactant-accessible catalysts on conductive surfaces. As a proof of principle, we demonstrate that electrophoretic deposition of thin films of an appropriately chosen metal–organic framework (MOF) material is an effective method for immobilizing the needed quantity of catalyst. For electrocatalytic CO2 reduction, we used a material that contains functionalized Fe-porphyrins as catalytically competent, redox-conductive linkers. The approach yields a high effective surface coverage of electrochemically addressable catalytic sites (~1015 sites/cm2). The chemical products of the reduction, obtained with ~100% Faradaic efficiency, are mixtures of CO and H2. The results validate the strategy of using MOF chemistry to obtain porous, electrode-immobilized, networks of molecular catalysts having competency for energy-relevant electrochemical reactions.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Univ. of California at San Diego, La Jolla, CA (United States)
- Northwestern Univ., Evanston, IL (United States); King Abdulaziz Univ., Jeddah (Saudi Arabia)
- Northwestern Univ., Evanston, IL (United States); Argonne National Lab., Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER); Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1224208
- Alternate Identifier(s):
- OSTI ID: 1224209
- Grant/Contract Number:
- AC02-06CH11357; SC0001059; FA9550-10-1-0572
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Name: ACS Catalysis; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; CO2 reduction; electrocatalysis; metal organic frameworks; Fe-porphyrin; solar fuel; redox conductivity
Citation Formats
Hod, Idan, Sampson, Matthew D., Deria, Pravas, Kubiak, Clifford P., Farha, Omar K., and Hupp, Joseph T. Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO2. United States: N. p., 2015.
Web. doi:10.1021/acscatal.5b01767.
Hod, Idan, Sampson, Matthew D., Deria, Pravas, Kubiak, Clifford P., Farha, Omar K., & Hupp, Joseph T. Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO2. United States. https://doi.org/10.1021/acscatal.5b01767
Hod, Idan, Sampson, Matthew D., Deria, Pravas, Kubiak, Clifford P., Farha, Omar K., and Hupp, Joseph T. Fri .
"Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO2". United States. https://doi.org/10.1021/acscatal.5b01767. https://www.osti.gov/servlets/purl/1224208.
@article{osti_1224208,
title = {Fe-porphyrin-based metal–organic framework films as high-surface concentration, heterogeneous catalysts for electrochemical reduction of CO2},
author = {Hod, Idan and Sampson, Matthew D. and Deria, Pravas and Kubiak, Clifford P. and Farha, Omar K. and Hupp, Joseph T.},
abstractNote = {Realization of heterogeneous electrochemical CO2-to-fuel conversion via molecular catalysis under high-flux conditions requires the assembly of large quantities of reactant-accessible catalysts on conductive surfaces. As a proof of principle, we demonstrate that electrophoretic deposition of thin films of an appropriately chosen metal–organic framework (MOF) material is an effective method for immobilizing the needed quantity of catalyst. For electrocatalytic CO2 reduction, we used a material that contains functionalized Fe-porphyrins as catalytically competent, redox-conductive linkers. The approach yields a high effective surface coverage of electrochemically addressable catalytic sites (~1015 sites/cm2). The chemical products of the reduction, obtained with ~100% Faradaic efficiency, are mixtures of CO and H2. The results validate the strategy of using MOF chemistry to obtain porous, electrode-immobilized, networks of molecular catalysts having competency for energy-relevant electrochemical reactions.},
doi = {10.1021/acscatal.5b01767},
journal = {ACS Catalysis},
number = ,
volume = ,
place = {United States},
year = {Fri Sep 18 00:00:00 EDT 2015},
month = {Fri Sep 18 00:00:00 EDT 2015}
}
Web of Science
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