Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products

Gao, Dunfeng; Arán‐Ais, Rosa M.; Jeon, Hyo Sang; Cuenya, Beatriz Roldán

doi:10.1038/s41929-019-0235-5

Cited by 1,152 publications

(959 citation statements)

References 136 publications

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“…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. These surface sites might be more favorable for C−C coupling during CO 2 RR, 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 + ) via an electrolyte‐driven nanostructuring pre‐treatment strategy, which was found to lead to enhanced C 2+ selectivity.…”

Section: Resultsmentioning

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 (C 2+ )from CO 2 electroreduction reaction (CO 2 RR) is highly desirable for storing renewable energy and reducing carbon emission. The electrochemical synthesis of CO 2 RR catalysts that are highly selective for C 2+ products via electrolyte-driven nanostructuring is presented. Nanostructured Cu catalysts synthesized in the presence of specific anions selectively convert CO 2 into ethylene and multicarbon alcohols in aqueous 0.1m KHCO 3 solution, with the iodine-modified catalyst displaying the highest Faradaic efficiency of 80 %a nd ap artial geometric current density of ca. 31.2 mA cm À2 for C 2+ products at À0.9 V vs.RHE. Operando X-rayabsorption spectroscopyand quasi in situ X-rayp hotoelectron spectroscopym easurements revealed that the high C 2+ selectivity of these nanostructured Cu catalysts can be attributed to the highly roughened surface morphology induced by the synthesis,p resence of subsurface oxygen and Cu + species,and the adsorbed halides.

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Section: Resultsmentioning

confidence: 99%

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

et al. 2019

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“…As a result, we are in urgent need to develop proper electrocatalysts so as to significantly expedite the reaction rate and steer the reaction selectivity toward the target product. Since the pioneering works by Hori et al in 1980s and 1990s, great efforts have been devoted to the design and engineering of CO 2 RR electrocatalysts especially within the past decade . There have been many encouraging experimental progresses as well as increasing mechanistic understanding of this complex reaction.…”

Section: Introductionmentioning

confidence: 99%

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO₂ Reduction to Formate

Han

Pan

et al. 2019

Advanced Energy Materials

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Selective CO2 reduction to formic acid or formate is the most technologically and economically viable approach to realize electrochemical CO2 valorization. Main group metal–based (Sn, Bi, In, Pb, and Sb) nanostructured materials hold great promise, but are still confronted with several challenges. Here, the current status, challenges, and future opportunities of main group metal–based nanostructured materials for electrochemical CO2 reduction to formate are reviewed. Firstly, the fundamentals of electrochemical CO2 reduction are presented, including the technoeconomic viability of different products, possible reaction pathways, standard experimental procedure, and performance figures of merit. This is then followed by detailed discussions about different types of main group metal–based electrocatalyst materials, with an emphasis on underlying material design principles for promoting the reaction activity, selectivity, and stability. Subsequently, recent efforts on flow cells and membrane electrode assembly cells are reviewed so as to promote the current density as well as mechanistic studies using in situ characterization techniques. To conclude a short perspective is offered about the future opportunities and directions of this exciting field.

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“…Among other strategies to reduce CO 2 emissions, the use of renewable electricity to convert CO 2 into clean fuels and chemicals, coupled to heterogeneous catalysis, is a promising and environmentally friendly approach that also contributes to reduce the consumption of fossil fuel resources . Electrochemical CO 2 reduction at room temperature and in aqueous electrolyte produces formic acid, syngas (CO+H 2 ), alcohols and hydrocarbons, among other interesting products . Thus, CO 2 can be seen as an abundant and cheap source of carbon to generate valuable compounds and not only as an environmental issue.…”

Section: Introductionmentioning

confidence: 99%

“…(4) Stability of the catalyst and cell components, which is probably the least studied aspect among the above figures of merit. Details about these challenges can be found in several reviews on the topic …”

Section: Introductionmentioning

confidence: 99%

Structure‐Sensitivity and Electrolyte Effects in CO₂ Electroreduction: From Model Studies to Applications

et al. 2019

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Aiming to reduce anthropogenic CO2 emissions, there is an urgent demand to develop more efficient and affordable technologies which convert CO2 into valuable feedstock molecules. The use of renewable electricity is a promising and sustainable approach to overcome this environmental issue, while producing valuable chemicals and clean fuels. However, the CO2 electroreduction reaction (CO2RR) still shows two main gaps: poor selectivity and required large overpotentials make the process not profitable enough. To overcome these challenges, model studies on single‐crystalline surfaces aiming to find the relations between surface structure/electrolyte interactions and activity/selectivity are necessary. In these model studies, tuning the electrolyte composition is also key for the fundamental understanding of the CO2RR. In this review, we first discuss the structure‐activity‐selectivity relations from studies on well‐ordered surfaces, i. e., single crystalline electrodes, for the CO2RR. We then summarise the role of the electrolyte, presenting work on classical aqueous solvents as well as non‐aqueous electrolytes such as ionic liquids. We illustrate the importance of carrying out studies on well‐defined electrified interfaces in order to get deep fundamental insights on the mechanism of the CO2RR, as well as scaling the process for real applications. Ultimately, this knowledge will be essential to rationally design the catalyst with tailored activity and selectivity for CO2 reduction.

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Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products

Cited by 1,152 publications

References 136 publications

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

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

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO₂ Reduction to Formate

Structure‐Sensitivity and Electrolyte Effects in CO₂ Electroreduction: From Model Studies to Applications

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Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products

Cited by 1,152 publications

References 136 publications

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

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

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO2 Reduction to Formate

Structure‐Sensitivity and Electrolyte Effects in CO2 Electroreduction: From Model Studies to Applications

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Product

Resources

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

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

Promises of Main Group Metal–Based Nanostructured Materials for Electrochemical CO₂ Reduction to Formate

Structure‐Sensitivity and Electrolyte Effects in CO₂ Electroreduction: From Model Studies to Applications