Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis

Electrochemical CO2 reduction has emerged as a promising CO2 utilization technology, with Gas Diffusion Electrodes becoming the predominant architecture to maximize performance. Such electrodes must maintain robust hydrophobicity to prevent flooding, while also ensuring high conductivity to minimize...

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Main Authors: Rufer, Simon, Nitzsche, Michael P, Garimella, Sanjay, Lake, Jack R, Varanasi, Kripa K
Other Authors: Massachusetts Institute of Technology. Department of Mechanical Engineering
Format: Article
Language:English
Published: Springer Science and Business Media LLC 2025
Online Access:https://hdl.handle.net/1721.1/158170
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author Rufer, Simon
Nitzsche, Michael P
Garimella, Sanjay
Lake, Jack R
Varanasi, Kripa K
author2 Massachusetts Institute of Technology. Department of Mechanical Engineering
author_facet Massachusetts Institute of Technology. Department of Mechanical Engineering
Rufer, Simon
Nitzsche, Michael P
Garimella, Sanjay
Lake, Jack R
Varanasi, Kripa K
author_sort Rufer, Simon
collection MIT
description Electrochemical CO2 reduction has emerged as a promising CO2 utilization technology, with Gas Diffusion Electrodes becoming the predominant architecture to maximize performance. Such electrodes must maintain robust hydrophobicity to prevent flooding, while also ensuring high conductivity to minimize ohmic losses. Intrinsic material tradeoffs have led to two main architectures: carbon paper is highly conductive but floods easily; while expanded Polytetrafluoroethylene is flooding resistant but non-conductive, limiting electrode sizes to just 5 cm2. Here we demonstrate a hierarchically conductive electrode architecture which overcomes these scaling limitations by employing inter-woven microscale conductors within a hydrophobic expanded Polytetrafluoroethylene membrane. We develop a model which captures the spatial variability in voltage and product distribution on electrodes due to ohmic losses and use it to rationally design the hierarchical architecture which can be applied independent of catalyst chemistry or morphology. We demonstrate C2+ Faradaic efficiencies of ~75% and reduce cell voltage by as much as 0.9 V for electrodes as large as 50 cm2 by employing our hierarchically conductive electrode architecture.
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spelling mit-1721.1/1581702025-02-05T15:43:02Z Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis Rufer, Simon Nitzsche, Michael P Garimella, Sanjay Lake, Jack R Varanasi, Kripa K Massachusetts Institute of Technology. Department of Mechanical Engineering Electrochemical CO2 reduction has emerged as a promising CO2 utilization technology, with Gas Diffusion Electrodes becoming the predominant architecture to maximize performance. Such electrodes must maintain robust hydrophobicity to prevent flooding, while also ensuring high conductivity to minimize ohmic losses. Intrinsic material tradeoffs have led to two main architectures: carbon paper is highly conductive but floods easily; while expanded Polytetrafluoroethylene is flooding resistant but non-conductive, limiting electrode sizes to just 5 cm2. Here we demonstrate a hierarchically conductive electrode architecture which overcomes these scaling limitations by employing inter-woven microscale conductors within a hydrophobic expanded Polytetrafluoroethylene membrane. We develop a model which captures the spatial variability in voltage and product distribution on electrodes due to ohmic losses and use it to rationally design the hierarchical architecture which can be applied independent of catalyst chemistry or morphology. We demonstrate C2+ Faradaic efficiencies of ~75% and reduce cell voltage by as much as 0.9 V for electrodes as large as 50 cm2 by employing our hierarchically conductive electrode architecture. 2025-02-05T15:43:01Z 2025-02-05T15:43:01Z 2024-11-13 2025-02-05T15:37:35Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/158170 Rufer, S., Nitzsche, M.P., Garimella, S. et al. Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis. Nat Commun 15, 9429 (2024). en 10.1038/s41467-024-53523-8 Nature Communications Creative Commons Attribution-NonCommercial-NoDerivatives https://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf Springer Science and Business Media LLC Springer Science and Business Media LLC
spellingShingle Rufer, Simon
Nitzsche, Michael P
Garimella, Sanjay
Lake, Jack R
Varanasi, Kripa K
Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis
title Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis
title_full Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis
title_fullStr Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis
title_full_unstemmed Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis
title_short Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis
title_sort hierarchically conductive electrodes unlock stable and scalable co2 electrolysis
url https://hdl.handle.net/1721.1/158170
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AT garimellasanjay hierarchicallyconductiveelectrodesunlockstableandscalableco2electrolysis
AT lakejackr hierarchicallyconductiveelectrodesunlockstableandscalableco2electrolysis
AT varanasikripak hierarchicallyconductiveelectrodesunlockstableandscalableco2electrolysis