Electrocatalytic reduction of CO<sub>2</sub> and CO to multi-carbon compounds over Cu-based catalysts

Ma, Wenchao; He, Xiaoyang; Wang, Wei; Xie, Shunji; Zhang, Qinghong; Wang, Ye

doi:10.1039/d1cs00535a

Cited by 422 publications

(290 citation statements)

References 49 publications

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“…Then, Cu foam showed the largest current densities at −1.5, −1.6 and −1.7 V compared to Cu 2 O NWs and CuO NWs. However, the current densities of gas-phase CO 2 electroreduction over the catalysts were far less than those of aqueous CO 2 electroreduction [26] due to their high charge transfer resistances (Figure S4). That is the conventional aqueous CO 2 electroreduction showed the excellent ion conductivity, which benefited from the strong electrolyte aqueous solution.…”

Section: Resultsmentioning

confidence: 99%

“…That is the conventional aqueous CO electroreduction showed the excellent ion conductivity, which benefited from the stron electrolyte aqueous solution. While gas-phase CO2 electroreduction highly depended o the conductivity of proton exchange membrane, resulting in the low current densitie [26]. In addition, the total FE of the products over Cu foam and CuO NWs were found t be less than 100% over the entire potential range because of high charge transfe resistance and diffusion resistance in gas-solid interface reaction system [25,27,28 Therefore, Cu2O NWs and Cu foam exhibited the preferable activities of gas-phase CO electroreduction to multicarbon oxygenates compared to CuO NWs.…”

Section: Resultsmentioning

confidence: 99%

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Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Zhao

et al. 2021

Catalysts

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Conversion of CO2 to valuable chemicals driven by renewable electricity via electrocatalytic reduction processes is of great significance for achieving carbon neutrality. Copper-based materials distinguish themselves from other electrocatalysts for their unique capability to produce multicarbon compounds in CO2 electroreduction. However, the intrinsic active composition and C–C coupling mechanism of copper-based catalysts are still ambiguous. This is largely due to the absence of appropriate in situ approaches to monitor the complicated processes of CO2 electroreduction. Here, we adopted operando spectroscopy techniques, including Raman and infrared, to investigate the evolution of compositions and intermediates during gas-phase CO2 electroreduction on Cu foam, Cu2O nanowire and CuO nanowire catalysts. Although all the three copper-based catalysts possessed the activity of electroreducing gas-phase CO2 to multicarbon oxygenates, Cu2O nanowires showed the much superior performance with a 71.9% Faradaic efficiency of acetaldehyde. Operando Raman spectra manifested that the cuprous oxide remained stable during the whole gas-phase CO2 electroreduction, and operando diffuse reflectance infrared Fourier transform spectroscopy (DRFITS) results provide direct evidences of key intermediates and their evolutions for producing multicarbon oxygenates, in consistence with the density functional theory calculations.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Zhao

et al. 2021

Catalysts

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“…Electrode process is a continuous reaction with multiple basic processes, in order: liquid mass transfer, adsorption, electrochemical reaction, desorption, liquid mass transfer, which obeys the kinetic laws of general heterogeneous catalytic reactions 81 . The interface properties and area, mass transfer kinetics, and new phase formation kinetics all affect the reaction rate 82 . In electrochemical CO2RR, the adsorption strength of intermediates and the next reaction path are affected by many factors 83 , including the morphology and size of the catalyst, the composition and pH of electrolyte, etc.…”

Section: Reaction Routes Of Electrochemical Co2rrmentioning

confidence: 99%

Cu-Based Tandem Catalysts for Electrochemical CO<sub>2</sub> Reduction

Shi¹,

Hou²,

Li³

et al. 2022

Acta Physico Chimica Sinica

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Through the combustion of fossil fuels and other human activities, large amounts of CO2 gas have been emitted into the atmosphere, causing many environmental problems, such as the greenhouse effect and global warming. Thus, developing and utilizing renewable clean energy is crucial to reduce CO2 emission and achieve carbon neutrality. The electrochemical CO2 reduction reaction (CO2RR) has been considered as an effective approach to obtain high value-added chemicals and fuels, which can store intermittent renewable energy and achieve the artificial carbon cycle. In addition, due to its multiple advantages, such as mild reaction conditions, tunable products, and simple implementation, electrochemical CO2RR has attracted extensive attention. Electrochemical CO2RR involves multiple electron-proton transfer steps to obtain multitudinous products, such as C1 products (CO, HCOOH, CH4, etc.) and C2 products (C2H4, C2H5OH, etc.). The intermediates, among which * CO is usually identified as the key intermediate, and reaction pathways of different products intersect, resulting in an extremely complex reaction mechanism. Currently, copper has been widely proven to be the only metal catalyst that can efficiently reduce CO2 to hydrocarbons and oxygenates due to its suitable adsorption energy for * CO. However, the low product selectivity, poor stability, and high overpotential of pure Cu hinder its use for the production of industrial-grade multi-carbon products. Tandem catalysts with multiple types of active sites can sequentially reduce CO2 molecules into desired products. When loaded onto a co-catalyst that can efficiently convert CO2 to * CO (such as Au and Ag), Cu acts as an electron donor owing to its high electrochemical potential. * CO species generated from the substrate can spillover onto the surface of electron-poor Cu due to the stronger adsorption and be further reduced to C2+ products. The use of Cu-based tandem catalysts for electrochemical CO2RR is a promising strategy for improving the performance of CO2RR and thus, has become a research hotspot in recent years. In this review, we first introduce the reaction routes and tandem mechanisms of electrochemical CO2RR. Then, we systematically summarize the recent research progress of Cu-based tandem catalysts for electrochemical CO2RR, including Cu-based metallic materials (alloys, heterojunction, and core-shell structures) as well as Cu-based framework materials, carbon materials, and polymer-modified materials. Importantly, the preparation methods of various Cu-based tandem catalysts and their structure-activity relationship in CO2RR are discussed and analyzed in detail. Finally, the challenges and opportunities of the rational design and controllable synthesis of advanced tandem catalysts for electrochemical CO2RR are proposed.

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“…Since the electrochemical conversion of CO 2 into various carbon products usually requires multiple proton-coupled electron transfer steps through different pathways depending on the kinetics of the electron transfer process, the dissociated protons and key intermediates are essential to determine the final products. 17,18 As one of the highly reduced carbon products, CH 4 is the main component of conventional fuels with the cleanest burning emission in modern energetics. 19,20 Nevertheless, the production of CH 4 involves an eight-electron reduction process together with proton transfers.…”

Section: Introductionmentioning

confidence: 99%

Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO₂ reduction to methane

Zhao

Wang

et al. 2022

SmartMat

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The electrochemical reduction reaction of carbon dioxide (CO2RR) is considered to be an effective way to realize carbon neutrality. As a type of intensively studied materials, covalent organic frameworks (COFs) with a tunable pore structure and various functional groups are promising catalysts for CO2RR. Herein, COF synthesized by 2,6‐diaminoanthraquinone and 2,4,6‐triformylphloroglucinol is employed to assist the synthesis of electrocatalysts from Cu single atoms (SAs) to nanoclusters by controlling the electrodeposition. A tandem catalyst for CO2‐to‐CH4 conversion is thus achieved by the Cu nanoclusters dispersed among the isolated Cu SAs in the COF network. It is proposed that CO2 is first reduced to CO over the atomically isolated Cu SAs, followed by diffusion onto the neighboring Cu nanoclusters for further reduction into CH4. In addition, mechanistic analysis suggests that the coordinated K+ ions on the COF network promote the activation of CO2 and the adsorption of reaction intermediates, thus realizing the suppressed hydrogen evolution reaction and selective production of CH4. This study presents a new insight of COFs for the confined synthesis of a tunable SA to nanocluster electrocatalysts, disclosing the great potential of COFs in electrocatalysis.

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Electrocatalytic reduction of CO₂ and CO to multi-carbon compounds over Cu-based catalysts

Abstract: This tutorial review discusses the similarities and differences between the electrocatalytic reduction of CO2 and CO to C2+ olefins and oxygenates over Cu-based catalysts.

Cited by 422 publications

References 49 publications

Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Cu-Based Tandem Catalysts for Electrochemical CO<sub>2</sub> Reduction

Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO₂ reduction to methane

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Electrocatalytic reduction of CO2 and CO to multi-carbon compounds over Cu-based catalysts

Abstract: This tutorial review discusses the similarities and differences between the electrocatalytic reduction of CO2 and CO to C2+ olefins and oxygenates over Cu-based catalysts.

Cited by 422 publications

References 49 publications

Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Insight into Composition and Intermediate Evolutions of Copper-Based Catalysts during Gas-Phase CO2 Electroreduction to Multicarbon Oxygenates

Cu-Based Tandem Catalysts for Electrochemical CO<sub>2</sub> Reduction

Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO2 reduction to methane

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Product

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Electrocatalytic reduction of CO₂ and CO to multi-carbon compounds over Cu-based catalysts

Organic frameworks confined Cu single atoms and nanoclusters for tandem electrocatalytic CO₂ reduction to methane