Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area

Wang, Lei; Nitopi, Stephanie A.; Wong, Andrew Barnabas; Snider, Jonathan L.; Nielander, Adam C.; Morales‐Guio, Carlos G.; Orazov, Marat; Higgins, Drew; Hahn, Christopher; Jaramillo, Thomas F.

doi:10.1038/s41929-019-0301-z

Cited by 210 publications

(238 citation statements)

References 47 publications

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“…With the above knowledge in hand, we then aimed to explore the impacts of the electrode surface area on COR selectivity. It has been previously demonstrated that the electrode roughness factor can steer COR selectivity toward multicarbon oxygenates on pure Cu catalysts by suppressing the competing HER (63). To test whether this surface area effect can further enhance the selectivity to acetaldehyde for the CuAg system, a porous CuAg nanoflower electrode (CuAg-NF) was prepared and evaluated for COR similarly.…”

Section: Resultsmentioning

confidence: 99%

Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Wang

Higgins

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

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102

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Electrochemical CO reduction can serve as a sequential step in the transformation of CO2into multicarbon fuels and chemicals. In this study, we provide insights on how to steer selectivity for CO reduction almost exclusively toward a single multicarbon oxygenate by carefully controlling the catalyst composition and its surrounding reaction conditions. Under alkaline reaction conditions, we demonstrate that planar CuAg electrodes can reduce CO to acetaldehyde with over 50% Faradaic efficiency and over 90% selectivity on a carbon basis at a modest electrode potential of −0.536 V vs. the reversible hydrogen electrode. The Faradaic efficiency to acetaldehyde was further enhanced to 70% by increasing the roughness factor of the CuAg electrode. Density functional theory calculations indicate that Ag ad-atoms on Cu weaken the binding energy of the reduced acetaldehyde intermediate and inhibit its further reduction to ethanol, demonstrating that the improved selectivity to acetaldehyde is due to the electronic effect from Ag incorporation. These findings will aid in the design of catalysts that are able to guide complex reaction networks and achieve high selectivity for the desired product.

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Section: Resultsmentioning

confidence: 99%

Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Wang

Higgins

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

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102

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“…The latter is probably attributed to its nanoporous structure . At the end, we should also highlight the role of the high ECSA of the present nanostructured Cu catalysts . Apart from having a higher surface area, a drastic increase in the ECSA during nanostructuring a flat Cu surface is usually coupled with the creation of highly reactive surface sites such as defects and low‐coordinated sites.…”

Section: Resultsmentioning

confidence: 80%

“…[43] At the end, we should also highlight the role of the high ECSA of the present nanostructured Cu catalysts. [44] Apart from having ahigher surface area, adrastic increase in the ECSA during nanostructuring aflat Cu surface is usually coupled with the creation of highly reactive surface sites such as defects and low-coordinated sites.T hese surface sites might be more favorable for CÀCc oupling during CO 2 RR, [1,45] not only improving the apparent activity but also helping to tune the selectivity towards multicarbon products. In this work we were able to modify the surface morphology and its composition and chemical state (Cu + )v ia an electrolyte-driven nanostructuring pre-treatment strategy,which was found to lead to enhanced C 2+ selectivity.…”

Section: Angewandte Chemiementioning

confidence: 99%

Selective CO₂ Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte‐Driven Nanostructuring

et al. 2019

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Production of multicarbon products (C2+) from CO2 electroreduction reaction (CO2RR) is highly desirable for storing renewable energy and reducing carbon emission. The electrochemical synthesis of CO2RR catalysts that are highly selective for C2+ products via electrolyte‐driven nanostructuring is presented. Nanostructured Cu catalysts synthesized in the presence of specific anions selectively convert CO2 into ethylene and multicarbon alcohols in aqueous 0.1 m KHCO3 solution, with the iodine‐modified catalyst displaying the highest Faradaic efficiency of 80 % and a partial geometric current density of ca. 31.2 mA cm−2 for C2+ products at −0.9 V vs. RHE. Operando X‐ray absorption spectroscopy and quasi in situ X‐ray photoelectron spectroscopy measurements revealed that the high C2+ selectivity of these nanostructured Cu catalysts can be attributed to the highly roughened surface morphology induced by the synthesis, presence of subsurface oxygen and Cu+ species, and the adsorbed halides.

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“…In order to develop efficient and highly selective catalysts, a large number of self‐supporting metal dendritic nanoarrays have been developed, including transition metals (such as Au, Ag, Cu, Bi, and Zn) and their composites. The electrodeposited Cu dendrites mainly brought forth multielectron products, including C 2 H 4 67,68,72,77 and CH 3 CHO 76. Especially, this kind of CO 2 RR electrocatalysts could even generate a remarkable ≈170 mA cm −2 current density, which might meet the commercial standard.…”

Section: Metal Nanoarrays On Conductive Substratementioning

confidence: 99%

“…Moreover, the electric field can drive almost all chemical reactions, which could be utilized as an effective method to produce the desired compounds in a controlled manner. Table 3 displays the summary of the electrodeposited metal nanodendrites as efficient CO 2 RR electrocatalysts,66–77 including, electrolyte, main product, cathode potential, current density, and Faradaic efficiency. Up till now, electrochemical deposition has been frequently adopted to prepare all kinds of self‐supported metal nanodendrite arrays as CO 2 RR electrocatalysts.…”

Section: Metal Nanoarrays On Conductive Substratementioning

confidence: 99%

Recent Progress in Self‐Supported Catalysts for CO₂ Electrochemical Reduction

Yang

Wang

et al. 2020

Small Methods

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Electrochemical reduction of CO2 may provide a promising method to mitigate the concentration of CO2 in the atmosphere, and simultaneously convert this greenhouse gas into value‐added fuels or chemicals. However, electrocatalysts for CO2 reduction are mostly powder based; therefore, polymer binders are always employed to make these catalysts useful as working electrodes. As a consequence, plenty of active sites are embedded inside without catalytic performance, causing a relatively low efficiency. On the contrary, self‐supported electrocatalysts do not involve the typical powdering and drop‐coating procedure with the aid of polymer binders or additives, avoiding the weak contact between active materials and current collector. Moreover, the superior self‐supported structure can also provide an accelerated electron transfer, guarantee ample electrolyte access to the active sites, offer large electrochemical surface areas, and increase CO2 adsorption capacity around the active sites, finally leading to the excellent efficiency and long‐term stability in CO2 reduction. In this manuscript, recent advances regarding CO2 reduction by self‐supported electrocatalysts are comprehensively reviewed, including the synthesis methods, chemical compositions, nanostructures, and catalytic efficiencies. Furthermore, the existing challenges and perspectives on the research and development of self‐supported electrocatalysts for CO2 reduction are discussed.

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Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area

Cited by 210 publications

References 47 publications

Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Selective CO₂ Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte‐Driven Nanostructuring

Recent Progress in Self‐Supported Catalysts for CO₂ Electrochemical Reduction

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Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area

Cited by 210 publications

References 47 publications

Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Selective reduction of CO to acetaldehyde with CuAg electrocatalysts

Selective CO2 Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte‐Driven Nanostructuring

Recent Progress in Self‐Supported Catalysts for CO2 Electrochemical Reduction

Contact Info

Product

Resources

About

Selective CO₂ Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte‐Driven Nanostructuring

Recent Progress in Self‐Supported Catalysts for CO₂ Electrochemical Reduction