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A Hybrid Catalyst-Bonded Membrane Device for Electrochemical Carbon Monoxide Reduction at Different Relative Humidities

Sullivan, Ian and Han, Lihao and Lee, Soo Hong and Lin, Meng and Larson, David M. and Drisdell, Walter S. and Xiang, Chengxiang (2019) A Hybrid Catalyst-Bonded Membrane Device for Electrochemical Carbon Monoxide Reduction at Different Relative Humidities. ACS Sustainable Chemistry & Engineering, 7 (20). pp. 16964-16970. ISSN 2168-0485. https://resolver.caltech.edu/CaltechAUTHORS:20190920-113304665

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Abstract

A hybrid catalyst-bonded membrane device using gaseous reactants for a carbon monoxide reduction (COR) reaction in the cathode chamber, an aqueous electrolyte for an oxygen evolution reaction (OER) in the anode chamber, and an anion exchange membrane (AEM) for product separation was modeled, constructed, and tested. The Cu electrocatalyst was electrodeposited onto gas diffusion layers (GDLs) and was directly bonded to AEM by mechanical pressing in the hybrid device. The impacts of relative humidity at the cathode inlet on the selectivity and activity of COR were investigated by computational modeling and experimental methods. At a relative humidity of 30%, the Cu-based catalyst in the hybrid device exhibited a total operating current density of 87 mA cm⁻² with a −2.0 V vs Ag/AgCl reference electrode, a Faradaic efficiency (FE) for C₂H₄ generation of 32.6%, and an FE for a liquid-based carbon product of 42.6%. Significant improvements in the partial current densities for COR were observed in relation to planar electrodes or flooded gas diffusion electrodes (GDEs). In addition, a custom test bed was constructed to characterize the oxidation states of the Cu catalysts in real time along with product analysis though the backside of the GDLs via operando X-ray absorption (XAS) measurements.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acssuschemeng.9b04959DOIArticle
ORCID:
AuthorORCID
Sullivan, Ian0000-0003-0632-4607
Han, Lihao0000-0002-0452-3381
Lee, Soo Hong0000-0002-2734-9654
Lin, Meng0000-0001-7785-749X
Drisdell, Walter S.0000-0002-8693-4562
Xiang, Chengxiang0000-0002-1698-6754
Additional Information:© 2019 American Chemical Society. Received: August 22, 2019; Revised: September 19, 2019; Published: September 20, 2019. This material is based on work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The authors declare no competing financial interest.
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-76SF00515
Subject Keywords:Gas Diffusion Electrode, Carbon Monoxide Reduction, Relative Humidity, Multiphysics modeling, Vapor-fed, operando X-ray Absorption Spectroscopy
Issue or Number:20
Record Number:CaltechAUTHORS:20190920-113304665
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20190920-113304665
Official Citation:A Hybrid Catalyst-Bonded Membrane Device for Electrochemical Carbon Monoxide Reduction at Different Relative Humidities. Ian Sullivan, Lihao Han, Soo Hong Lee, Meng Lin, David M. Larson, Walter S. Drisdell, and Chengxiang Xiang. ACS Sustainable Chemistry & Engineering 2019 7 (20), 16964-16970. DOI: 10.1021/acssuschemeng.9b04959
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:98777
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:20 Sep 2019 18:39
Last Modified:24 Oct 2019 16:33

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