Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis

Wei, Pengfei; Gao, Dunfeng; Liu, Tian‐Fu; Li, Hefei; Sang, Jiaqi; Wang, Chao; Cai, Rui; Wang, Guoxiong; Bao, Xinhe

doi:10.1038/s41565-022-01286-y

Cited by 127 publications

(124 citation statements)

References 76 publications

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Section: Resultsmentioning

confidence: 99%

“…Along with the flow cell, membrane electrode assembly (MEA) electrolyzers are being actively explored for practical applications owing to the simplified reactor design, lower operating cell voltage, and higher energetic efficiency. 29 Thus, we tested the CO 2 RR performance for the Cu CF catalyst in an MEA electrolyzer. The prepared cathode was coupled with an anion-exchange membrane and iridium oxide-based anode for oxygen evolution in the MEA electrolyzer (area: 4 cm 2 , details in the Methods section).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

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Hydrophobic, Ultrastable Cu^δ+ for Robust CO₂ Electroreduction to C₂ Products at Ampere-Current Levels

Fang

Wang

et al. 2023

J. Am. Chem. Soc.

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Copper (Cu) is the only known material that can efficiently electrocatalyze CO 2 to value-added multicarbon products. Owing to the instability of the Cu δ+ state and microscopic structure in reactions, Cu catalysts are still facing big challenges with low selectivity and poor durability, particularly at high current densities. Herein, we report a rational one-step surface coordination approach for the synthesis of Cu dendrites with an ultrastable Cu δ+ state and hydrophobicity (Cu CF), even after exposure to air for over 6 months. As a result, Cu CF exhibited a C 2 FE of 90.6% at a partial current density of 453.3 mA cm −2 in a flow cell. A 400 h stable electrolysis at 800 mA and even a ground-breaking stable operation at a large industrial current of 10 A were achieved in the membrane electrode assembly (MEA) form. We further demonstrated a continuous production of C 2 H 5 OH solution with 90% relative purity at 600 mA over 50 h in a solid-electrolyte reactor. Spectroscopy and computation results suggested that Cu(II) carboxylate coordination species formed on the surface of Cu CF, which ensured the stability of the Cu δ+ state and hydrophobicity. As a result, rich active sites and a stable three-phase interface on the catalyst surface were achieved, along with the optimized *CO adsorption strength and adsorption configuration. The mixed *CO adsorption configurations on Cu CF made the *CO dimerization process easier, which promoted the conversion of CO 2 to C 2 products. This work provides a promising paradigm for the design and development of Cu-based catalysts with ultrahigh stability under industrial current densities.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Results and Discussionmentioning

confidence: 99%

Hydrophobic, Ultrastable Cu^δ+ for Robust CO₂ Electroreduction to C₂ Products at Ampere-Current Levels

Fang

Wang

et al. 2023

J. Am. Chem. Soc.

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“…À and H 2 O. [20][21][22] To date, microenvironment-dependent CO 2 electrolysis under acidic MEA electrolyzer conditions has rarely been reported, especially at industrial current densities. Ni-N-C is an efficient catalyst for CO 2 electrolysis, with a CO FE of over 90% and considerable CO partial current density within a wide potential range in alkaline and neutral electrolytes.…”

mentioning

confidence: 99%

“…The MEA configuration results in high complexity in the microenvironment near the catalyst surface, such as local concentrations of H + , OH − , K + , CO 2 , HCO 3 − and H 2 O. 20–22 To date, microenvironment-dependent CO 2 electrolysis under acidic MEA electrolyzer conditions has rarely been reported, especially at industrial current densities.…”

mentioning

confidence: 99%

Tailoring acidic microenvironments for carbon-efficient CO₂electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer

Wei

et al. 2023

Energy Environ. Sci.

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“…Another application of the GDEM-cell is the ability to tune the composition of inlet gas. Wei et al studied the coelectrolysis reaction of mixed CO/CO 2 feed on CuO nanosheets by using GDEM-cell Figure c,d shows the composition of the electrolytic cell stack used.…”

Section: Engineering Of Electrolyzersmentioning

confidence: 99%

Bridging Trans-Scale Electrode Engineering for Mass CO₂ Electrolysis

Wen

Ren

Liu

et al. 2023

JACS Au

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Electrochemical CO 2 upgrade offers an artificial route for carbon recycling and neutralization, while its widespread implementation relies heavily on the simultaneous enhancement of mass transfer and reaction kinetics to achieve industrial conversion rates. Nevertheless, such a multiscale challenge calls for trans-scale electrode engineering. Herein, three scales are highlighted to disclose the key factors of CO 2 electrolysis, including triple-phase boundaries, reaction microenvironment, and catalytic surface coordination. Furthermore, the advanced types of electrolyzers with various electrode design strategies are surveyed and compared to guide the system architectures for continuous conversion. We further offer an outlook on challenges and opportunities for the grand-scale application of CO 2 electrolysis. Hence, this comprehensive Perspective bridges the gaps between electrode research and CO 2 electrolysis practices. It contributes to facilitating the mixed reaction and mass transfer process, ultimately enabling the on-site recycling of CO 2 emissions from industrial plants and achieving net negative emissions.

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Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis

Cited by 127 publications

References 76 publications

Hydrophobic, Ultrastable Cu^δ+ for Robust CO₂ Electroreduction to C₂ Products at Ampere-Current Levels

Hydrophobic, Ultrastable Cu^δ+ for Robust CO₂ Electroreduction to C₂ Products at Ampere-Current Levels

Tailoring acidic microenvironments for carbon-efficient CO₂electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer

Bridging Trans-Scale Electrode Engineering for Mass CO₂ Electrolysis

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Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis

Cited by 127 publications

References 76 publications

Hydrophobic, Ultrastable Cuδ+ for Robust CO2 Electroreduction to C2 Products at Ampere-Current Levels

Hydrophobic, Ultrastable Cuδ+ for Robust CO2 Electroreduction to C2 Products at Ampere-Current Levels

Tailoring acidic microenvironments for carbon-efficient CO2electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer

Bridging Trans-Scale Electrode Engineering for Mass CO2 Electrolysis

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Hydrophobic, Ultrastable Cu^δ+ for Robust CO₂ Electroreduction to C₂ Products at Ampere-Current Levels

Hydrophobic, Ultrastable Cu^δ+ for Robust CO₂ Electroreduction to C₂ Products at Ampere-Current Levels

Tailoring acidic microenvironments for carbon-efficient CO₂electrolysis over a Ni–N–C catalyst in a membrane electrode assembly electrolyzer

Bridging Trans-Scale Electrode Engineering for Mass CO₂ Electrolysis