Electrochemical carbon dioxide reduction on copper–zinc alloys: ethanol and ethylene selectivity analysis

Baek, Yeji; Song, Hakhyeon; Hong, Deokgi; Wang, Suneon; Lee, Sungwoo; Joo, Young‐Chang; Lee, Gun-Do; Oh, Jihun

doi:10.1039/d1ta10345h

Cited by 27 publications

(23 citation statements)

References 51 publications

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“…The electrochemical recycling of CO 2 has emerged as an attractive strategy for addressing energy and environmental solutions in the future. − To enhance catalytic efficiency and achieve desired product outcomes, alloy metals are increasingly being used in these applications. − Cu-based bimetals, including CuNi − and CuZn, − have received significant attention due to their unique ability to produce high yields of CH 4 and C 2+ (oxy)hydrocarbons. Yan et al reported a high Faradaic efficiency (FE) of 80.5% for C ≥2 products (C 2 H 4 and ethanol) at −1.5 V (vs RHE) with ∼250 mA/cm 2 in 0.5 M KHCO 3 using ultrathin hexagonal CuNi nanosheets .…”

Section: Introductionmentioning

confidence: 99%

Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO₂/CO Reduction for Ternary CuNiZn Alloys

Park

Jang

Maeng

et al. 2023

ACS Appl. Energy Mater.

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Metal alloy electrocatalysts are commonly used in electrochemical (EC) CO 2 reduction. In this study, we demonstrate the application of a ternary CuNiZn alloy as an electrocatalyst for both CO 2 and CO reductions. Our results show that formate, CO, CH 4 , and C 2−7 hydrocarbons were produced through the process of initial CO 2 adsorption followed by subsequent stepwise reactions. Interestingly, we also observed the production of CH 4 and C 2−7 hydrocarbons (C n H 2n+2 and C n H 2n ) through EC CO reduction, which occurred via direct CO adsorption, followed by hydrogenation reactions. Furthermore, we discovered an electrochemically-induced surface reaction that mimics the Fischer−Tropsch (F−T) synthesis, resulting in the formation of long-chain hydrocarbons through C−C coupling/polymerization. We utilized X-ray photoelectron spectroscopy with Ar + ion sputtering depth to investigate the interfacial electronic structures and surface elemental composition distributions of Cu, Ni, and Zn. Our results indicate that these properties are highly dependent on both the applied potential and the depth at which they are measured. These unique observation provides significant insights into the EC F−T synthesis process, C−C coupling mechanism, the design of efficient metal alloy electrodes, and the theoretical modeling of alloys in both electrochemical CO 2 reduction and CO reduction.

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Section: Introductionmentioning

confidence: 99%

Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO₂/CO Reduction for Ternary CuNiZn Alloys

Park

Jang

Maeng

et al. 2023

ACS Appl. Energy Mater.

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“…33,34 Baek et al demonstrated that a Cu–Zn electrocatalyst produces C 2 H 5 OH with 25% faradaic efficiency. 35 Because metal-bound CO is a key intermediate in producing multicarbon products, Ag is an excellent catalyst for CO formation, and Cu facilitates CO–CO coupling, Ag–Cu catalysts are widely employed to generate C2+ products. Among the possible C2+ products, most Ag–Cu catalysts produce C 2 H 4 in high yields.…”

Section: Introductionmentioning

confidence: 99%

Membrane-controlled CO₂ electrocatalysts with switchable C2 product selectivity and high faradaic efficiency for ethanol

Akter

Barile

2023

J. Mater. Chem. A

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“…Chen et al demonstrated that a hollow-fiber Cu–Sn catalyst is capable of selectively producing HCOOH with 90.9% Faradaic efficiency at −0.75 V vs RHE . Baek et al fabricated a Cu–Zn electrocatalyst that preferentially produces ethanol over C 2 H 4 with 25% Faradaic efficiency . The selectivity toward ethanol was attributed to the local atomic arrangement.…”

Section: Introductionmentioning

confidence: 99%

“…39 Baek et al fabricated a Cu−Zn electrocatalyst that preferentially produces ethanol over C 2 H 4 with 25% Faradaic efficiency. 40 The selectivity toward ethanol was attributed to the local atomic arrangement. He et al demonstrated that ternary alloys of Cu− Zn−Sn can achieve >80% CO and HCOOH Faradaic efficiency at an overpotential of 200 mV.…”

Section: ■ Introductionmentioning

confidence: 99%

Electrochemical CO₂ Reduction on Zinc and Brass with Modulated Proton Transfer Using Membrane-Modified Electrodes

Pan

Akter

Barile

2022

ACS Appl. Energy Mater.

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In this manuscript, we fabricate copolymer blends of polyvinylidene fluoride (PVDF) and Nafion as overlayers on Zn and brass substrates to create electrodes for the CO 2 reduction reaction with enhanced selectivity. By varying the blend composition, the rates of proton transfer and polymer stabilization of reaction intermediates are modulated. C 2 H 4 was obtained with a Faradaic efficiency of 74.1% at −0.89 V vs RHE using 52 wt % PVDF in Nafion on top of a brass electrode. Synergy among Cu, Zn, Nafion, and PVDF allows for this high yield of C 2 H 4 . Additionally, Zn and brass electrodes modified with a Nafion overlayer in a mixed acetonitrile−water electrolyte, which contain a lower proton concentration than aqueous electrolytes, produce 60% CH 3 OH and 65% C 2 H 4 , respectively. These results enable us to develop a mechanistic framework that explains CO 2 reduction catalyst selectivity in terms of proton transfer rates and the stability of reaction intermediates. In particular, we demonstrate that slowing proton transfer to the electrode results in more CO−CO coupling and that brass stabilizes a *C 2 O 2 − intermediate to generate C 2 H 4 . As a whole, these findings will aid the CO 2 reduction community in developing next-generation catalysts with improved selectivity.

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Electrochemical carbon dioxide reduction on copper–zinc alloys: ethanol and ethylene selectivity analysis

Abstract: The effect of local atomic arrangement of CuZn alloys was demonstrated on enhanced ethanol selectivity from CO2RR and supported by density functional theory (DFT) calculations.

Cited by 27 publications

References 51 publications

Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO₂/CO Reduction for Ternary CuNiZn Alloys

Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO₂/CO Reduction for Ternary CuNiZn Alloys

Membrane-controlled CO₂ electrocatalysts with switchable C2 product selectivity and high faradaic efficiency for ethanol

Electrochemical CO₂ Reduction on Zinc and Brass with Modulated Proton Transfer Using Membrane-Modified Electrodes

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Electrochemical carbon dioxide reduction on copper–zinc alloys: ethanol and ethylene selectivity analysis

Abstract: The effect of local atomic arrangement of CuZn alloys was demonstrated on enhanced ethanol selectivity from CO2RR and supported by density functional theory (DFT) calculations.

Cited by 27 publications

References 51 publications

Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO2/CO Reduction for Ternary CuNiZn Alloys

Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO2/CO Reduction for Ternary CuNiZn Alloys

Membrane-controlled CO2 electrocatalysts with switchable C2 product selectivity and high faradaic efficiency for ethanol

Electrochemical CO2 Reduction on Zinc and Brass with Modulated Proton Transfer Using Membrane-Modified Electrodes

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Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO₂/CO Reduction for Ternary CuNiZn Alloys

Interfacial Electronic Structures and the Fischer–Tropsch Synthesis Path by Electrochemical CO₂/CO Reduction for Ternary CuNiZn Alloys

Membrane-controlled CO₂ electrocatalysts with switchable C2 product selectivity and high faradaic efficiency for ethanol

Electrochemical CO₂ Reduction on Zinc and Brass with Modulated Proton Transfer Using Membrane-Modified Electrodes