Bridging Trans-Scale Electrode Engineering for Mass CO<sub>2</sub> Electrolysis

Wen, Guobin; Ren, Bohua; Liu, Y.; Dong, Shaojun; Luo, Dan; Jin, Mingliang; Wang, Xin; Yu, Aiping; Chen, Zhongwei

doi:10.1021/jacsau.3c00174

Cited by 3 publications

(1 citation statement)

References 118 publications

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“…The electrochemical carbon dioxide reduction reaction (CO 2 RR), driven by renewable electricity to produce high-value chemicals, is a promising approach for the efficient utilization of carbon dioxide and the development of a carbon-neutral society. − However, the use of alkaline or neutral electrolytes inevitably causes the reaction between CO 2 and OH – species, leading to a significant drop in carbon utilization efficiency. − Moreover, the migration of carbonate (CO 3 2– )/bicarbonate (HCO 3 – ) ions through the anion exchange membrane (AEM) to the anolyte side further decreases the carbon efficiency. − Additionally, the formation of carbonate deposits near the cathode electrode can clog the porous channels of the gas diffusion electrode, ,, resulting in reduced stability (Figure a). These issues pose limitations to the practical long-term operation of alkaline or neutral CO 2 RR.…”

Section: Introductionmentioning

confidence: 99%

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

Ge,

Dong,

Wang

et al. 2024

ACS Catal.

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Acidic CO2 electroreduction offers a promising strategy for achieving a high CO2 utilization efficiency. However, it is highly challenging to inhibit the competing hydrogen evolution reactions (HER) due to the high concentration of protons at the electrode–electrolyte interface. The interfacial hydrogen-bond environment greatly affects proton transfer and the kinetics of hydrogen-related reactions, e.g., HER and CO2 reduction. In this work, we demonstrate that sulfonate-based electrolyte additives, including sodium p-styrenesulfonate (SPS), sodium p-toluene sulfonate (STS), and sodium benzenesulfonate (SBS), enable reconstruction of the interfacial hydrogen-bond environment and enhance the CO2 electrolysis performance. Mechanistic studies uncover that the strong hydrogen-bond interactions of these sulfonate-based additives with H2O achieve the construction of a low proton-flux interface. This leads to the suppression of proton concentration-dependent HER. The SPS-assisted acidic CO2 electrolysis yields CO with a high selectivity of 97.8% and a high single-pass carbon efficiency of 66.3% at 250 mA cm–2 on commercial Ag catalysts in acid. This work provides a facile strategy to promote acidic CO2 electrolysis by modulating the interfacial hydrogen-bond environment through electrolyte design.

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Section: Introductionmentioning

confidence: 99%

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

Ge,

Dong,

Wang

et al. 2024

ACS Catal.

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Cu‐In Dual Sites with Sulfur Defects toward Superior Ethanol Electrosynthesis from CO₂ Electrolysis

Wen,

Ren,

Zhang

et al. 2024

Advanced Materials

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The electrosynthesis of multi‐carbon chemicals from excess CO2 is an area of great interest for research and commercial applications. However, improving both the yield of CO2‐to‐ethanol conversion and the stability of the catalyst at the same time is proving to be a challenging issue. Here we propose to stabilize active Cu(I) and In dual sites with sulfur defects through an electro‐driven intercalation strategy, which leads to the delocalization of electron density that enhances orbital hybridizations between the Cu‐C and In‐H bonds. Hence, the energy barrier for the rate‐limiting *CHO formation step is reduced toward the key *OCHCHO* formation during ethanol production, which is also facilitated by the combined Cu site enabling C‐C coupling and In site with a higher oxygen affinity based on both thermodynamic and kinetic calculations. Accordingly, such dual‐site catalyst achieves a high partial current density toward ethanol of 409 ± 15 mA/cm2 for over 120 hours. Furthermore, a scaled‐up flow cell is assembled with an industrial‐relevant current of 5.7 A for over 36 hours, in which the carbon loss is less than 2.5% and single‐pass carbon efficiency is around 19%.This article is protected by copyright. All rights reserved

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Lewis-base ligand-reshaped interfacial hydrogen-bond network boosts CO2 electrolysis

Ge,

Tao,

Dong

et al. 2024

National Science Review

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Both the catalyst and electrolyte strongly impact the performance of CO2 electrolysis. Despite substantial progress in catalysts, it remains highly challenging to tailor electrolyte compositions and understand their functions at the catalyst interface. Here, we report that the ethylenediaminetetraacetic acid (EDTA) and its analogs, featuring strong Lewis acid-base interaction with metal cations, are selected as electrolyte additives to reshape the catalyst-electrolyte interface for promoting CO2 electrolysis. Mechanistic studies reveal that EDTA molecules are dynamically assembled toward interface region in response to bias potential due to strong Lewis acid-base interaction of EDTA4–-K+. As a result, the original hydrogen-bond network among interfacial H2O is disrupted, and a hydrogen-bond gap layer at the electrified interface is established. The EDTA-reshaped K+ solvation structure promotes the protonation of *CO2 to *COOH and suppressing *H2O dissociation to *H, thereby boosting the co-electrolysis of CO2 and H2O toward carbon-based products. In particular, when 5 mM of EDTA is added into the electrolytes, the faradaic efficiency of CO on the commercial Ag nanoparticle catalyst is increased from 57.0% to 90.0% at an industry-relevant current density of 500 mA cm−2. More importantly, the Lewis-base ligand-reshaped interface allows a range of catalysts (Ag, Zn, Pd, Bi, Sn, and Cu) to deliver substantially increased selectivity of carbon-based products in both H-type and flow-type electrolysis cells.

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Bridging Trans-Scale Electrode Engineering for Mass CO₂ Electrolysis

Cited by 3 publications

References 118 publications

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

Cu‐In Dual Sites with Sulfur Defects toward Superior Ethanol Electrosynthesis from CO₂ Electrolysis

Lewis-base ligand-reshaped interfacial hydrogen-bond network boosts CO2 electrolysis

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Bridging Trans-Scale Electrode Engineering for Mass CO2 Electrolysis

Cited by 3 publications

References 118 publications

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO2 Electrolysis

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO2 Electrolysis

Cu‐In Dual Sites with Sulfur Defects toward Superior Ethanol Electrosynthesis from CO2 Electrolysis

Lewis-base ligand-reshaped interfacial hydrogen-bond network boosts CO2 electrolysis

Contact Info

Product

Resources

About

Bridging Trans-Scale Electrode Engineering for Mass CO₂ Electrolysis

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

Modulating Interfacial Hydrogen-Bond Environment by Electrolyte Engineering Promotes Acidic CO₂ Electrolysis

Cu‐In Dual Sites with Sulfur Defects toward Superior Ethanol Electrosynthesis from CO₂ Electrolysis