Electrocatalytic Carbon Dioxide Reduction to Ethylene over Copper‐based Catalytic Systems

Yang, Yisen; Tan, Zhonghao; Zhang, Jianling

doi:10.1002/asia.202200893

Cited by 11 publications

(9 citation statements)

References 113 publications

(214 reference statements)

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“…Different from H-cell, CO 2 flows continuously from the back to the catalyst surface through the gas diffusion layer (GDL). Within the flow cell, the rich three-phase boundary composed of CO 2 , catalyst and electrolyte significantly improve the reaction efficiency [ 50 , 59 , 135 ]. The advantages of a short CO 2 diffusion path and no solubility limitation strengthen the mass transfer of CO 2 , thereby improving the current density and selectivity [ 59 ].…”

Section: Discussionmentioning

confidence: 99%

“…The *CO species can be directly desorbed from the catalysts (e.g., Ag and Au) when *CO adsorption energy is low, forming CO gas (the mechanism of electrochemical CO 2 RR to form CO) (Fig. 2 c) [ 49 , 50 ]. Alternatively, moderate *CO adsorption energy (e.g., Cu) can lead to further coupling and formation of C–C bonds for promoting the following C 2+ production, based on the Sabatier principle [ 40 ].…”

Section: Fundamental and Mechanism Of Co 2 Rr To E...mentioning

confidence: 99%

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Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Cao

et al. 2023

Nano-Micro Lett.

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Electrochemical carbon dioxide reduction reaction (CO2RR) provides a promising way to convert CO2 to chemicals. The multicarbon (C2+) products, especially ethylene, are of great interest due to their versatile industrial applications. However, selectively reducing CO2 to ethylene is still challenging as the additional energy required for the C–C coupling step results in large overpotential and many competing products. Nonetheless, mechanistic understanding of the key steps and preferred reaction pathways/conditions, as well as rational design of novel catalysts for ethylene production have been regarded as promising approaches to achieving the highly efficient and selective CO2RR. In this review, we first illustrate the key steps for CO2RR to ethylene (e.g., CO2 adsorption/activation, formation of *CO intermediate, C–C coupling step), offering mechanistic understanding of CO2RR conversion to ethylene. Then the alternative reaction pathways and conditions for the formation of ethylene and competitive products (C1 and other C2+ products) are investigated, guiding the further design and development of preferred conditions for ethylene generation. Engineering strategies of Cu-based catalysts for CO2RR-ethylene are further summarized, and the correlations of reaction mechanism/pathways, engineering strategies and selectivity are elaborated. Finally, major challenges and perspectives in the research area of CO2RR are proposed for future development and practical applications.

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Section: Discussionmentioning

confidence: 99%

Section: Fundamental and Mechanism Of Co 2 Rr To E...mentioning

confidence: 99%

Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Cao

et al. 2023

Nano-Micro Lett.

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“…Copper-based nanoscale electrocatalysts have shown great potential in the electroreduction of carbon dioxide to multicarbon products; however, their catalytic efficiency is still low. − The results show that at least two neighboring copper sites are required to achieve C–C coupling on copper-based electrocatalysts, ,− while C 1 products are formed on dispersed copper sites. Based on this result, it is expected to improve the selectivity of multicarbon products by precisely controlling the arrangement of copper atoms in copper-based electrocatalysts. − For example, Zheng et al effectively shortened the distance between two single copper atoms by increasing the distribution concentration of copper single atoms on the carrier.…”

Section: Introductionmentioning

confidence: 99%

“…It is especially true that specific C 2+ products, such as ethylene (C 2 H 4 ) and ethane (C 2 H 6 ), are important in chemical feedstocks due to their high energy density. , Copper (Cu) is widely regarded as the only metal capable of electrocatalytic catalyzing the conversion of carbon dioxide into multicarbon molecules due to its unique d-band center. , However, enhancing the design of copper-based catalysts to achieve high production rates and selectivity to C 2+ products requires a series of measures, including tuning the surface morphology to expose preferred crystalline surfaces or grain boundaries, , performing interfacial engineering, introducing surface dopants, , forming alloys, , and other methods. However, challenges arise in achieving large-scale synthesis of multicarbon products through CO 2 electrocatalysis due to the sluggish kinetics of the C–C coupling reaction occurring on copper surfaces, coupled with the comparatively low production rates of C 2+ compounds.…”

Section: Introductionmentioning

confidence: 99%

Copper/Cobalt-Loaded Carbon Nanostructures as Catalysts for Electrochemical CO₂ Reduction

Wu,

Zhao

et al. 2024

ACS Appl. Nano Mater.

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The electrochemical reduction of CO 2 to produce high-value multicarbon products represents a challenging yet highly desirable process, particularly due to the inefficient C−C coupling observed in current electrocatalysts. In this study, Cu 2+ and Co 2+ were introduced into ZIF-8 as precursors to synthesize a series of Co-and CuCo-doped carbon nanostructure materials with varying Co-to-Cu ratios. X-ray diffraction and X-ray photoelectron spectroscopy (XPS) analyses confirmed the successful doping of metal Co in the form of Co−N x , while Cu was partly doped as nanoparticles attached to the carbon substrate surface and partly as single atoms forming Cu−N x . Transmission electron microscopy and energy-dispersive X-ray spectroscopy analyses revealed uniform distribution of elemental Co and Cu on the carbon substrate, with Cu loaded as nanocluster on the surface. Linear sweep voltammetry tests indicated that Cu/CoCu-N x -C composites exhibited enhanced reactivity toward CO 2 reduction compared to other samples. At −0.19 V (vs RHE), the Faradaic efficiencies (FEs %) of C 2 H 4 , C 2 H 6 , CH 4 , CO, and H 2 over Cu/CoCu-N x -C were 29.7, 8.6, 20.2, 9.8, and 31.5%, respectively. The influence of Co and Cu doping modes on the selectivity of electrocatalytic reduction products was investigated. Results showed that Cu/CoCu-N x -C exhibited a higher FE of C 2 compared to Cu/Cu−N x -C, with nearly 10 times higher C 2 current density. Mechanistic insights from acid-etching experiments and XPS revealed a synergistic interaction between metallic Co and Cu, promoting the generation of multicarbon products. Co−N x improved *CO coverage, facilitating subsequent C−C coupling on neighboring Cu−N x . Additionally, CH 4 production was attributed to the (111) crystalline facets in the Cu nanocluster and isolated Cu−N x . Overall, this research provides an important understanding of the creation of straightforward and effective catalysts for the reduction of CO 2 . It holds considerable potential for the production of hydrocarbons using carbon dioxide.

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“…As an alternative, CO 2 capture and utilization have received much attention, as CO 2 can be used to produce high-value chemicals via chemical transformation or electrocatalytic, , photocatalytic, , and photothermocatalytic processes. In this regard, CO 2 has been used as a C 1 building block to produce value-added chemicals (carbon monoxide, methanol, formic acid, formaldehyde, acetic acid, and acetaldehyde), high-energy-density fuels (methane, propane, and ethanol), and precursors for polymers such as ethylene and carbonate . Production of liquid electro-fuels (e-fuels) derived from CO 2 , to substitute fossil fuel is vital to reaching a net-zero carbon footprint.…”

Section: Introductionmentioning

confidence: 99%

Rational Design of Heterogeneous Dual-Atom Catalysts for CO₂ Electroreduction Reactions

Jafarzadeh

Daasbjerg

2023

ACS Appl. Energy Mater.

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One of the strategies to mitigate the concentration of CO 2 in the atmosphere and reduce the global warming effect is to capture CO 2 and convert it to synthetic fuels and fine chemicals. Although CO 2 is structurally and chemically stable, the electrochemical transformation has attracted much attention because it offers mild reaction conditions regarding temperature, pressure, and process controllability. Among various electrocatalysts, dualatom catalysts (DACs) have been extensively developed in the past few years due to their unique features for the electrochemical reactions of small molecules. The catalytic activity of DACs in the electrochemical CO 2 reduction reaction (eCO 2 RR) has surpassed single-atom catalysts (SACs) by providing a higher metal loading, two active sites (cf. one active site for SACs), a synergistic effect of adjacent metal atoms, the possibility of tuning the electronic state (adjusting the d-band center), and more possible configuration modes (side-on and side-bridge) for adsorption of CO 2 (cf. only end-on and end-bridge modes for SACs). As a result, both higher reactivity and selectivity in eCO 2 RR can be achieved by breaking scaling relationships with more possible interactions between intermediates and active sites. This review highlights and discusses the recent progress in applying homo-and heteronuclear DACs for eCO 2 RR focusing on the synthesis, characterization, and electrochemical catalytic performance.

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Electrocatalytic Carbon Dioxide Reduction to Ethylene over Copper‐based Catalytic Systems

Cited by 11 publications

References 113 publications

Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Copper/Cobalt-Loaded Carbon Nanostructures as Catalysts for Electrochemical CO₂ Reduction

Rational Design of Heterogeneous Dual-Atom Catalysts for CO₂ Electroreduction Reactions

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Electrocatalytic Carbon Dioxide Reduction to Ethylene over Copper‐based Catalytic Systems

Cited by 11 publications

References 113 publications

Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Electrochemical Carbon Dioxide Reduction to Ethylene: From Mechanistic Understanding to Catalyst Surface Engineering

Copper/Cobalt-Loaded Carbon Nanostructures as Catalysts for Electrochemical CO2 Reduction

Rational Design of Heterogeneous Dual-Atom Catalysts for CO2 Electroreduction Reactions

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Product

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Copper/Cobalt-Loaded Carbon Nanostructures as Catalysts for Electrochemical CO₂ Reduction

Rational Design of Heterogeneous Dual-Atom Catalysts for CO₂ Electroreduction Reactions