Enhanced CO<sub>2</sub> reduction with hydrophobic cationic-ionomer layer-modified zero-gap MEA in acidic electrolyte

Zhao, Xueyang; Xie, Hongtao; Deng, Bangwei; Wang, Lili; Li, Yizhao; Dong, Fan

doi:10.1039/d3cc05277j

Cited by 3 publications

(1 citation statement)

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“…Various catalyst design strategies have been reported to effectively regulate the selectivity of the CO 2 RR. 15–17 Notably, by altering the electronic structure of Cu-based catalysts by the addition of a second metal 18–20 or metal oxide promoter 21 phase provides a significant improvement for C 2 H 4 production. Ceria (CeO 2 ) is widely used as a catalyst, support and promoter for a variety of heterogeneous catalytic reactions involving the hydrogenation of CO 2 22 due to its acid–base and unique redox properties of oxygen storage and release.…”

Section: Introductionmentioning

confidence: 99%

CeO₂-promoted Cu₂O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

Alarcón,

Andreu,

Ponce de León

2024

Mater. Adv.

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Section: Introductionmentioning

confidence: 99%

CeO₂-promoted Cu₂O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

Alarcón,

Andreu,

Ponce de León

2024

Mater. Adv.

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Anionic Ionomer: Released Surface-Immobilized Cations and an Established Hydrophobic Microenvironment for Efficient and Durable CO₂-to-Ethylene Electrosynthesis at High Current over One Month

Fang,

Miao,

Huang

et al. 2024

J. Am. Chem. Soc.

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Electrosynthesis of multicarbon products, such as C 2 H 4 , from CO 2 reduction on copper (Cu) catalysts holds promise for achieving carbon neutrality. However, maintaining a steady high current-level C 2 H 4 electrosynthesis still encounters challenges, arising from unstable alkalinity and carbonate precipitation caused by undesired ion migration at the cathode under a repulsive electric field. To address these issues, we propose a universal "charge release" concept by incorporating tiny amounts of an oppositely charged anionic ionomer (e.g., perfluorinated sulfonic acid, PFSA) into a cationic covalent organic framework on the Cu surface (cCOF/PFSA). This strategy effectively releases the hidden positive charge within the cCOF, enhancing surface immobilization of cations to impede both outward migration of generated OH − and inward migration of cations, inhibiting carbonate precipitation and creating a strong alkaline microenvironment. Meanwhile, the ionomer's hydrophobic chains create a hydrophobic environment within the cCOF, facilitating efficient gas transport. In situ characterizations and theoretical calculations demonstrate that the cCOF/PFSA catalyst establishes a hydrophobic strong alkaline microenvironment, optimizing the adsorption strength and configuration of *CO intermediates to promote the C 2 H 4 formation. The optimized catalyst achieves a 70.5% Faradaic efficiency for C 2 H 4 with a partial current density over 470 mA cm −2 . Notably, it delivers a high single-pass carbon efficiency of 96.5% for CO 2 RR and sustains an exceptional stability over 760 h. When implemented in a large-area MEA electrolyzer and a 5-cell MEA stack, the system achieves an industrial current of 15 A and continuous C 2 H 4 production exceeding 19 mL min −1 , marking a significant step toward industrial feasibility in CO 2 RR-to-C 2 H 4 conversion.

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Accelerating acidic CO₂ electroreduction: strategies beyond catalysts

Deng,

Sun,

Zhao

et al. 2024

Chem. Sci.

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Enhanced CO₂ reduction with hydrophobic cationic-ionomer layer-modified zero-gap MEA in acidic electrolyte

Abstract: A hydrophobic cationic-ionomer adlayer is constructed to enhance CO2 electroreduction with 95.6% Faradaic efficiency for MEA under acidic conditions.

Cited by 3 publications

References 29 publications

CeO₂-promoted Cu₂O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

CeO₂-promoted Cu₂O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

Anionic Ionomer: Released Surface-Immobilized Cations and an Established Hydrophobic Microenvironment for Efficient and Durable CO₂-to-Ethylene Electrosynthesis at High Current over One Month

Accelerating acidic CO₂ electroreduction: strategies beyond catalysts

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Enhanced CO2 reduction with hydrophobic cationic-ionomer layer-modified zero-gap MEA in acidic electrolyte

Abstract: A hydrophobic cationic-ionomer adlayer is constructed to enhance CO2 electroreduction with 95.6% Faradaic efficiency for MEA under acidic conditions.

Cited by 3 publications

References 29 publications

CeO2-promoted Cu2O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

CeO2-promoted Cu2O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

Anionic Ionomer: Released Surface-Immobilized Cations and an Established Hydrophobic Microenvironment for Efficient and Durable CO2-to-Ethylene Electrosynthesis at High Current over One Month

Accelerating acidic CO2 electroreduction: strategies beyond catalysts

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Enhanced CO₂ reduction with hydrophobic cationic-ionomer layer-modified zero-gap MEA in acidic electrolyte

CeO₂-promoted Cu₂O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

CeO₂-promoted Cu₂O-based catalyst sprayed on the gas diffusion layer for the electroreduction of carbon dioxide to ethylene

Anionic Ionomer: Released Surface-Immobilized Cations and an Established Hydrophobic Microenvironment for Efficient and Durable CO₂-to-Ethylene Electrosynthesis at High Current over One Month

Accelerating acidic CO₂ electroreduction: strategies beyond catalysts