Insights into electrolyte flooding in flexible gas diffusion electrodes for CO<sub>2</sub> electrolysis: from mechanisms to effective mitigation strategies

Wu, Yuming; Rabiee, Hesamoddin; Zhao, Xiu Song; Wang, Geoff; Jiang, Yijiao

doi:10.1039/d4ta01994f

J. Mater. Chem. A

2024

DOI: 10.1039/d4ta01994f

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Insights into electrolyte flooding in flexible gas diffusion electrodes for CO₂ electrolysis: from mechanisms to effective mitigation strategies

Yuming Wu,

Hesamoddin Rabiee,

Xiu Song Zhao

et al.

Abstract: The advancement of CO2 electrolysis has reached a stage where practical CO2 electrolysers show promise for high conversion rate, low manufacture cost, and extended system durability. While gas diffusion electrodes...

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Cited by 4 publications

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Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO₂ Reduction

Rabiee,

Ma,

Yang

et al. 2024

Adv Funct Materials

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Electrochemical CO2 reduction reaction (CO2RR) coupled with renewable electricity holds promises for efficient mitigation of carbon emission impacts on the environment and turning CO2 into valuable chemicals. One important task in CO2RR development is the design and fabrication of efficient electrodes for stable operation in the long term. Gas‐diffusion electrodes (GDEs) have been employed to continuously feed CO2 to the electrolyzers. Despite significant advances in GDE design and tailoring GDE properties, the present GDEs often suffer from the critical issue of flooding due to the electrowetting of carbon‐based substrates, which hinders the transition to industrial application. To address flooding, GDEs with intrinsically hydrophobic polymeric substrates have been recently fabricated and have shown promising performances. Herein, the advances and challenges associated with carbon‐free GDEs are reviewed for CO2RR. This review first briefly outlines GDE and electrolyzers basics. Through critical discussion around the shortcomings of conventional carbon‐based GDEs, the most recent efforts to resolve flooding are summarized. Subsequently, the advances, advantages, and challenges of carbon‐free GDEs are elaborated. Finally, priorities for future studies are suggested, with the aim to support the advancement and scale‐up of carbon‐free GDEs and extend them to other electrochemical systems where gas and the electrolyte are in contact.

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Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO₂ Reduction

Rabiee,

Ma,

Yang

et al. 2024

Adv Funct Materials

View full text Add to dashboard Cite

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Rational Designing Microenvironment of Gas‐Diffusion Electrodes via Microgel‐Augmented CO₂ Availability for High‐Rate and Selective CO₂ Electroreduction to Ethylene

Rabiee,

Li,

Yan

et al. 2024

Advanced Science

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Efficient electrochemical CO2 reduction reaction (CO2RR) requires advanced gas‐diffusion electrodes (GDEs) with tunned microenvironment to overcome low CO2 availability in the vicinity of catalyst layer. Herein, for the first time, pyridine‐containing microgels‐augmented CO2 availability is presented in Cu2O‐based GDE for high‐rate CO2 reduction to ethylene, owing to the presence of CO2‐phil microgels with amine moieties. Microgels as three‐dimensional polymer networks act as CO2 micro‐reservoirs to engineer the GDE microenvironment and boost local CO2 availability. The superior ethylene production performance of the GDE modified by 4‐vinyl pyridine microgels, as compared with the GDE with diethylaminoethyl methacrylate microgels, indicates the bifunctional effect of pyridine‐based microgels to enhance CO2 availability, and electrocatalytic CO2 reduction. While the Faradaic efficiency (FE) of ethylene without microgels was capped at 43% at 300 mA cm−2, GDE with the pyridine microgels showed 56% FE of ethylene at 700 mA cm−2. A similar trend was observed in zero‐gap design, and GDEs showed 58% FE of ethylene at −4.0 cell voltage (>350 mA cm−2 current density), resulting in over 2‐fold improvement in ethylene production. This study showcases the use of CO2‐phil microgels for a higher rate of CO2RR‐to‐C2+, opening an avenue for several other microgels for more selective and efficient CO2 electrolysis.

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Machine Learning Exploration of Experimental Conditions for Optimized Electrochemical CO₂ Reduction

Ayu Setyowati,

Mukaida,

Nagita

et al. 2024

ChemElectroChem

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Electrochemical CO2 reduction has attracted significant attention as a potential method to close the carbon cycle. In this study, we investigated the impact of the electrode fabrication and electrolysis conditions on the product selectivity of Ag electrocatalysts using a machine learning (ML) approach. Specifically, we explored the experimental conditions for obtaining the desired H2/CO mixture ratio with high CO efficiency. Notably, unlike previous ML‐based studies, we used experimental results as training data. This ML‐based approach allowed us to quantitatively assess the effect of experimental parameters on these targets with a reduced number of experimental trials (only 56 experiments). An inverse analysis based on the ML model suggested the optimal experimental conditions for achieving the desired characteristics of the electrolysis system, with the proposed conditions experimentally validated. This study constitutes the first demonstration of optimal experimental conditions for electrochemical CO2 reduction with desired characteristics using the experimental results as training data.

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Insights into electrolyte flooding in flexible gas diffusion electrodes for CO₂ electrolysis: from mechanisms to effective mitigation strategies

Abstract: The advancement of CO2 electrolysis has reached a stage where practical CO2 electrolysers show promise for high conversion rate, low manufacture cost, and extended system durability. While gas diffusion electrodes...

Cited by 4 publications

References 155 publications

Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO₂ Reduction

Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO₂ Reduction

Rational Designing Microenvironment of Gas‐Diffusion Electrodes via Microgel‐Augmented CO₂ Availability for High‐Rate and Selective CO₂ Electroreduction to Ethylene

Machine Learning Exploration of Experimental Conditions for Optimized Electrochemical CO₂ Reduction

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Insights into electrolyte flooding in flexible gas diffusion electrodes for CO2 electrolysis: from mechanisms to effective mitigation strategies

Abstract: The advancement of CO2 electrolysis has reached a stage where practical CO2 electrolysers show promise for high conversion rate, low manufacture cost, and extended system durability. While gas diffusion electrodes...

Cited by 4 publications

References 155 publications

Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO2 Reduction

Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO2 Reduction

Rational Designing Microenvironment of Gas‐Diffusion Electrodes via Microgel‐Augmented CO2 Availability for High‐Rate and Selective CO2 Electroreduction to Ethylene

Machine Learning Exploration of Experimental Conditions for Optimized Electrochemical CO2 Reduction

Contact Info

Product

Resources

About

Insights into electrolyte flooding in flexible gas diffusion electrodes for CO₂ electrolysis: from mechanisms to effective mitigation strategies

Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO₂ Reduction

Advances and Challenges of Carbon‐Free Gas‐Diffusion Electrodes (GDEs) for Electrochemical CO₂ Reduction

Rational Designing Microenvironment of Gas‐Diffusion Electrodes via Microgel‐Augmented CO₂ Availability for High‐Rate and Selective CO₂ Electroreduction to Ethylene

Machine Learning Exploration of Experimental Conditions for Optimized Electrochemical CO₂ Reduction