Hollow fiber gas-diffusion electrodes with tailored crystal facets for tuning syngas production in electrochemical CO2 reduction

Chen, Guoliang; Ge, Lei; Kuang, Yizhu; Rabiee, Hesamoddin; Ma, Beibei; Dorosti, Fatereh; Kumar Nanjundan, Ashok; Zhu, Zhonghua; Wang, Hao

doi:10.1016/j.cej.2024.151651

Cited by 9 publications

(3 citation statements)

References 49 publications

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“…The unique tubular shape of HFGDEs provides abundant catalytically active sites for triple-phase interface reactions during the CO 2 RR process. The gas delivery configuration of HFGDEs facilitates a flow-through mechanism owing to its special hierarchical porous structure. , Furthermore, the pressure difference between the inside and outside of the hollow fiber wall could force CO 2 to diffuse toward the active sites, enhancing the local concentration of CO 2 . , These effectively improve the activity and selectivity of CO 2 conversion . For example, Rabiee et.al.…”

Section: Introductionmentioning

confidence: 99%

“…42,45 Furthermore, the pressure difference between the inside and outside of the hollow fiber wall could force CO 2 to diffuse toward the active sites, enhancing the local concentration of CO 2 . 47,48 These effectively improve the activity and selectivity of CO 2 conversion. 49 For example, Rabiee et.al.…”

Section: Introductionmentioning

confidence: 99%

“…In addition to the enhancement of electrocatalyst efficiency, the structure of electrodes plays a critical role in CO 2 RR. − One approach to enhance the conversion efficiency and selectivity in CO 2 RR is employing gas-diffusion electrodes (GDEs). ,, GDEs can provide sufficient CO 2 directly to electrocatalyst active sites, improving CO 2 concentration near the electrode and enhancing the formation of a triple-phase boundary (CO 2 electrocatalyst–electrolyte). , Therefore, high current densities using GDEs for CO 2 RR have been achieved. , Recently, hollow fiber gas-diffusion electrodes (HFGDEs) fabricated with metals (Cu, Ag, Bi, etc.) have captured significant interest in CO 2 RR owing to their distinctive tubular shape, porous structured walls, and high catalytic active area. − HFGDEs represent a novel electrode structure via industrially feasible phase-inversion and sintering techniques using a metal powder and a polymer binder solution. , The three-dimensional structure of HFGDEs allows for direct utilization of CO 2 when they are used as the working electrode. The unique tubular shape of HFGDEs provides abundant catalytically active sites for triple-phase interface reactions during the CO 2 RR process.…”

Section: Introductionmentioning

confidence: 99%

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Steering CO Selectivity in CO₂ Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

Kuang,

Chen,

Rabiee

et al. 2024

Energy Fuels

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An efficient gas diffusion electrode (GDE) is crucial for enhancing mass transport involving gas-phase CO2 conversion in the electrochemical CO2 reduction reaction (CO2RR). Microtubular hollow fiber GDE (HFGDE) with a porous hierarchical wall has garnered significant attention, which can modulate the triple-phase reaction zone and improve the performance of CO2RR. Simultaneously, engineering nano/microstructure surfaces of electrocatalysts have been demonstrated to effectively enhance the selectivity and activity in CO2RR. Here, we developed a porous microparticle Ag-based HFGDE via an in situ electrochemical oxidation–reduction method. Both the activity and selectivity of CO2 to CO conversion in the porous microparticle Ag-based HFGDE showed significant enhancement over the pristine and thermal reduced Ag HFGDE without surface reconstruction. At −1.2 V vs RHE, the faradaic efficiency for CO is 94%, with a partial current density of 83.4 mA cm–2, surpassing that of thermal treatment electrodes, which is only 26% with a partial current density of 12.3 mA cm–2. The distinctive reconstruction nano/microstructure on the electrocatalyst surface could be attributed to decreasing the activation energy barrier in the rate-limiting step of initial electron/proton transfer. This work represents a facile strategy for surface reconstruction of electrocatalysts in HFGDE as advanced electrode materials to enhance the efficiency of the CO2 conversion.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Steering CO Selectivity in CO₂ Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

Kuang,

Chen,

Rabiee

et al. 2024

Energy Fuels

Self Cite

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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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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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Hollow fiber gas-diffusion electrodes with tailored crystal facets for tuning syngas production in electrochemical CO2 reduction

Cited by 9 publications

References 49 publications

Steering CO Selectivity in CO₂ Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

Steering CO Selectivity in CO₂ Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

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

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Hollow fiber gas-diffusion electrodes with tailored crystal facets for tuning syngas production in electrochemical CO2 reduction

Cited by 9 publications

References 49 publications

Steering CO Selectivity in CO2 Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

Steering CO Selectivity in CO2 Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

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

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Product

Resources

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Steering CO Selectivity in CO₂ Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

Steering CO Selectivity in CO₂ Electroreduction over Silver Microtubular Gas-Diffusion Electrodes via Surface Reconstruction

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