The Conventional Gas Diffusion Electrode May Not Be Resistant to Flooding during CO2/CO Reduction

Zhang, Tianyu; Li, Zhengyuan; Lyu, Xiang; Raj, Jithu; Zhang, Guangqi; Kim, Hyunsik; Wang, Xiangning; Chae, Soryong; Lemen, Lisa; Shanov, Vesselin N.; Wu, Jingjie

doi:10.1149/1945-7111/ac9b96

The Conventional Gas Diffusion Electrode May Not Be Resistant to Flooding during CO₂/CO Reduction

Journal Article · Mon Oct 31 00:00:00 EDT 2022 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/ac9b96· OSTI ID:1994617

^[1]; ^[1]; ^[2]; Raj, Jithu ^[1]; Zhang, Guangqi ^[1]; Kim, Hyunsik ^[1]; Wang, Xiangning ^[1]; Chae, Soryong ^[1]; Lemen, Lisa ^[1]; Shanov, Vesselin N. ^[1]; ^[1]

Univ. of Cincinnati, OH (United States)
Univ. of Cincinnati, OH (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

The electrochemical CO₂ or CO reduction to chemicals and fuels using renewable energy is a promising way to reduce anthropogenic carbon emissions. The gas diffusion electrode (GDE) design enables low-carbon manufacturing of target products at a current density (e.g., 500 mA cm^–2) relevant to industrial requirements. However, the long-term stability of the GDE is restricted by poor water management and flooding, resulting in a significant hydrogen evolution reaction (HER) within almost an hour. The optimization of water management in the GDE demands a thorough understanding of the role of the gas diffusion layer (GDL) and the catalyst layer (CL) distinctively. In this work, the hydrophobicity of the GDL and CL is independently adjusted to investigate their influence on gas transport efficiency and water management. The gas transport efficiency is more enhanced with the increase in hydrophobicity of the GDL than the CL. Direct visualization of water distribution by optical microscope and micro-computed tomography demonstrates that the water flow pattern transfers from the stable displacement to capillary fingering as GDL hydrophobicity increases. Unfortunately, only increasing the hydrophobicity is not sufficient to prevent flooding. A revolutionary change in the design of the GDE structure is essential to maintain the long-term stability of CO₂/CO reduction.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Fossil Energy and Carbon Management (FECM); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; FE0031919

OSTI ID:: 1994617

Alternate ID(s):: OSTI ID: 2478520

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 10 Vol. 169; ISSN 0013-4651

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

References (32)

Engineered Water Highways in Fuel Cells: Radiation Grafting of Gas Diffusion Layers Forner-Cuenca, Antoni; Biesdorf, Johannes; Gubler, Lorenz Advanced Materials, Vol. 27, Issue 41 https://doi.org/10.1002/adma.201503557	journal	September 2015
Emerging Carbon‐Based Heterogeneous Catalysts for Electrochemical Reduction of Carbon Dioxide into Value‐Added Chemicals Wu, Jingjie; Sharifi, Tiva; Gao, Ying Advanced Materials, Vol. 31, Issue 13 https://doi.org/10.1002/adma.201804257	journal	December 2018
A Gross-Margin Model for Defining Technoeconomic Benchmarks in the Electroreduction of CO ₂ Verma, Sumit; Kim, Byoungsu; Jhong, Huei-Ru “Molly” ChemSusChem, Vol. 9, Issue 15 https://doi.org/10.1002/cssc.201600394	journal	June 2016
Durable Cathodes and Electrolyzers for the Efficient Aqueous Electrochemical Reduction of CO ₂ Nwabara, Uzoma O.; Cofell, Emiliana R.; Verma, Sumit ChemSusChem, Vol. 13, Issue 5 https://doi.org/10.1002/cssc.201902933	journal	February 2020
Effective diffusivity and water-saturation distribution in single- and two-layer PEMFC diffusion medium Nam, Jin Hyun; Kaviany, Massoud International Journal of Heat and Mass Transfer, Vol. 46, Issue 24, p. 4595-4611 https://doi.org/10.1016/S0017-9310(03)00305-3	journal	November 2003
Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells Reshetenko, Tatyana; Odgaard, Madeleine; Randolf, Günter Applied Catalysis B: Environmental, Vol. 312 https://doi.org/10.1016/j.apcatb.2022.121424	journal	September 2022
Oxygen transport resistance correlated to liquid water saturation in the gas diffusion layer of PEM fuel cells Owejan, Jon P.; Trabold, Thomas A.; Mench, Matthew M. International Journal of Heat and Mass Transfer, Vol. 71 https://doi.org/10.1016/j.ijheatmasstransfer.2013.12.059	journal	April 2014
Effects of flow field and diffusion layer properties on water accumulation in a PEM fuel cell Owejan, J.; Trabold, T.; Jacobson, D. International Journal of Hydrogen Energy, Vol. 32, Issue 17 https://doi.org/10.1016/j.ijhydene.2007.05.044	journal	December 2007
Enhance CO2-to-C2+ products yield through spatial management of CO transport in Cu/ZnO tandem electrodes Zhang, Tianyu; Li, Zhengyuan; Zhang, Jianfang Journal of Catalysis, Vol. 387 https://doi.org/10.1016/j.jcat.2020.05.002	journal	July 2020
Ex situ visualization of liquid water transport in PEM fuel cell gas diffusion layers Litster, S.; Sinton, D.; Djilali, N. Journal of Power Sources, Vol. 154, Issue 1 https://doi.org/10.1016/j.jpowsour.2005.03.199	journal	March 2006
Two-phase flow dynamics in a gas diffusion layer - gas channel - microporous layer system Niblett, Daniel; Mularczyk, Adrian; Niasar, Vahid Journal of Power Sources, Vol. 471 https://doi.org/10.1016/j.jpowsour.2020.228427	journal	September 2020
Materials, technological status, and fundamentals of PEM fuel cells – A review Wang, Yun; Ruiz Diaz, Daniela Fernanda; Chen, Ken S. Materials Today, Vol. 32 https://doi.org/10.1016/j.mattod.2019.06.005	journal	January 2020
Hydrogen production by PEM water electrolysis – A review Shiva Kumar, S.; Himabindu, V. Materials Science for Energy Technologies, Vol. 2, Issue 3 https://doi.org/10.1016/j.mset.2019.03.002	journal	December 2019
CO-CO coupling on Cu facets: Coverage, strain and field effects Sandberg, Robert B.; Montoya, Joseph H.; Chan, Karen Surface Science, Vol. 654 https://doi.org/10.1016/j.susc.2016.08.006	journal	December 2016
Tandem Electrodes for Carbon Dioxide Reduction into C2+ Products at Simultaneously High Production Efficiency and Rate She, Xiaojie; Zhang, Tianyu; Li, Zhengyuan Cell Reports Physical Science, Vol. 1, Issue 4 https://doi.org/10.1016/j.xcrp.2020.100051	journal	April 2020
Numerical models and experiments on immiscible displacements in porous media Lenormand, Roland; Touboul, Eric; Zarcone, Cesar Journal of Fluid Mechanics, Vol. 189 https://doi.org/10.1017/S0022112088000953	journal	April 1988
General Techno-Economic Analysis of CO ₂ Electrolysis Systems Jouny, Matthew; Luc, Wesley; Jiao, Feng Industrial & Engineering Chemistry Research, Vol. 57, Issue 6 https://doi.org/10.1021/acs.iecr.7b03514	journal	February 2018
Theoretical Insights into a CO Dimerization Mechanism in CO ₂ Electroreduction Montoya, Joseph H.; Shi, Chuan; Chan, Karen The Journal of Physical Chemistry Letters, Vol. 6, Issue 11 https://doi.org/10.1021/acs.jpclett.5b00722	journal	May 2015
Investigation of Electrolyte-Dependent Carbonate Formation on Gas Diffusion Electrodes for CO₂ Electrolysis Cofell, Emiliana R.; Nwabara, Uzoma O.; Bhargava, Saket S. ACS Applied Materials & Interfaces, Vol. 13, Issue 13 https://doi.org/10.1021/acsami.0c21997	journal	March 2021
Liquid–Solid Boundaries Dominate Activity of CO ₂ Reduction on Gas-Diffusion Electrodes Nesbitt, Nathan T.; Burdyny, Thomas; Simonson, Hunter ACS Catalysis, Vol. 10, Issue 23 https://doi.org/10.1021/acscatal.0c03319	journal	November 2020
Mechanism of CO ₂ Reduction at Copper Surfaces: Pathways to C ₂ Products Garza, Alejandro J.; Bell, Alexis T.; Head-Gordon, Martin ACS Catalysis, Vol. 8, Issue 2 https://doi.org/10.1021/acscatal.7b03477	journal	January 2018
Role of the Carbon-Based Gas Diffusion Layer on Flooding in a Gas Diffusion Electrode Cell for Electrochemical CO ₂ Reduction Yang, Kailun; Kas, Recep; Smith, Wilson A. ACS Energy Letters, Vol. 6, Issue 1 https://doi.org/10.1021/acsenergylett.0c02184	journal	November 2020
The future of low-temperature carbon dioxide electrolysis depends on solving one basic problem Rabinowitz, Joshua A.; Kanan, Matthew W. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-19135-8	journal	October 2020
Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment Xing, Zhuo; Hu, Lin; Ripatti, Donald S. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-020-20397-5	journal	January 2021
Gas diffusion electrodes, reactor designs and key metrics of low-temperature CO2 electrolysers Wakerley, David; Lamaison, Sarah; Wicks, Joshua Nature Energy, Vol. 7, Issue 2 https://doi.org/10.1038/s41560-021-00973-9	journal	February 2022
High-rate electroreduction of carbon monoxide to multi-carbon products Jouny, Matthew; Luc, Wesley; Jiao, Feng Nature Catalysis, Vol. 1, Issue 10 https://doi.org/10.1038/s41929-018-0133-2	journal	August 2018
Carbon monoxide electroreduction as an emerging platform for carbon utilization Jouny, Matthew; Hutchings, Gregory S.; Jiao, Feng Nature Catalysis, Vol. 2, Issue 12 https://doi.org/10.1038/s41929-019-0388-2	journal	December 2019
Absence of CO2 electroreduction on copper, gold and silver electrodes without metal cations in solution Monteiro, Mariana C. O.; Dattila, Federico; Hagedoorn, Bellenod Nature Catalysis, Vol. 4, Issue 8 https://doi.org/10.1038/s41929-021-00655-5	journal	July 2021
CO ₂ electrolysis to multicarbon products at activities greater than 1 A cm ⁻² García de Arquer, F. Pelayo; Dinh, Cao-Thang; Ozden, Adnan Science, Vol. 367, Issue 6478 https://doi.org/10.1126/science.aay4217	journal	February 2020
Liquid Water Transport in Gas Diffusion Layer of Polymer Electrolyte Fuel Cells Pasaogullari, Ugur; Wang, C. Y. Journal of The Electrochemical Society, Vol. 151, Issue 3 https://doi.org/10.1149/1.1646148	journal	January 2004
Estimation of Mass-Transport Overpotentials during Long-Term PEMFC Operation Wood, David L.; Borup, Rodney L. Journal of The Electrochemical Society, Vol. 157, Issue 8 https://doi.org/10.1149/1.3454740	journal	January 2010
Liquid-Water Interactions with Gas-Diffusion-Layer Surfaces Santamaria, Anthony D.; Das, Prodip K.; MacDonald, James C. Journal of The Electrochemical Society, Vol. 161, Issue 12 https://doi.org/10.1149/2.0321412jes	journal	January 2014

Figures / Tables (6)

Similar Records

Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO₂ Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer

Journal Article · Tue Nov 08 23:00:00 EST 2022 · Journal of Physical Chemistry. C · OSTI ID:1902016

Minor Product Polymerization Causes Failure of High-Current CO₂-to-Ethylene Electrolyzers

Journal Article · Sun Jan 09 23:00:00 EST 2022 · ACS Energy Letters · OSTI ID:1894313

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY