Modulating Local CO2 Concentration as a General Strategy for Enhancing C−C Coupling in CO2 Electroreduction

Tan, Ying Chuan; Lee, Kelvin Berm; Song, Hakhyeon; Oh, Jihun

doi:10.1016/j.joule.2020.03.013

Cited by 289 publications

(287 citation statements)

References 46 publications

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“…A comparison of their CO 2 RR performance was shown in Supplementary Fig. 15d : the partial current density and total Faradaic efficiency for CO 2 RR on the Cu/C-extra electrode was similar to that of the Cu/C electrode, but the Faradaic efficiency for C 2+ products was lower on the Cu/C-extra electrode, which was attributed to the relatively lower concentration of CO 2 inside the catalyst layer 16 . This is reasonable as CO 2 needs to diffuse over a longer distance on average to reach the catalyst particles in a thicker catalyst layer.…”

Section: Resultsmentioning

confidence: 97%

“…In particular, the electrochemical reduction of CO 2 over Cu-based catalysts has received considerable interest, because Cu exhibits appreciable activity for C–C coupling to form multicarbon products, including ethylene, ethanol, and propanol 13 , 14 . While efforts are focused on developing catalytic materials, it is also critical to understand other factors beyond catalytic materials, such as the local environment of the catalysts 15 , which can mediate the transport and local concentration of reaction species and influence reaction pathways 16 .…”

Section: Introductionmentioning

confidence: 99%

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Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

et al. 2021

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Electroreduction of carbon dioxide (CO2) over copper-based catalysts provides an attractive approach for sustainable fuel production. While efforts are focused on developing catalytic materials, it is also critical to understand and control the microenvironment around catalytic sites, which can mediate the transport of reaction species and influence reaction pathways. Here, we show that a hydrophobic microenvironment can significantly enhance CO2 gas-diffusion electrolysis. For proof-of-concept, we use commercial copper nanoparticles and disperse hydrophobic polytetrafluoroethylene (PTFE) nanoparticles inside the catalyst layer. Consequently, the PTFE-added electrode achieves a greatly improved activity and Faradaic efficiency for CO2 reduction, with a partial current density >250 mA cm−2 and a single-pass conversion of 14% at moderate potentials, which are around twice that of a regular electrode without added PTFE. The improvement is attributed to a balanced gas/liquid microenvironment that reduces the diffusion layer thickness, accelerates CO2 mass transport, and increases CO2 local concentration for the electrolysis.

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Section: Resultsmentioning

confidence: 97%

Section: Introductionmentioning

confidence: 99%

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

et al. 2021

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“…It indicates there is still an ample space to explore in the aspect of the reaction device and system, such as electrolyte, membrane engineering, and counterreactions. [140] For example, the recent development of solid electrolyte membrane, such as solid alkaline polymer electrolytes, has benefited the anion exchange membrane (AEM) fuel cells with high peak power and good stability, which can be the reference for ECO 2 RR. [141] The mechanic strength, ionic conductivity, and the alkaline stability still need further improvement for better performance of AEM devices.…”

Section: Discussionmentioning

confidence: 99%

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives

Chen

Zhang

et al. 2020

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million (ppm), which is ≈50% higher than that of the pre-industrial level (280 ppm). [1] The consequent climate change (the average temperature increase of 0.8 °C above the pre-industrial level) causes global warming, one of the top environmental concerns. [2] To maintain the sustainable development of the society, the Intergovernmental Panel on Climate Change (IPCC) recently recommended the warming limit to 1.5 °C rather than 2.0 °C to reduce catastrophic climate change issues, requiring the commitment to take action to control global carbon emission. [3] Under the Paris Agreement, many countries endeavor to reduce greenhouse gas emissions gradually by 2030. [4] The carbon capture and storage (CCS) is a feasible strategy to lower the CO 2 emissions substantially. Long-term storage issues related to the leakage of CO 2 and the lack of economic incentives limited its development. [5] The CO 2 reduction reactions (CO 2 RR) that convert CO 2 into other value-added carbon products could provide a well alternative to the utilization of the captured CO 2 , which not only contributes to the mitigation of CO 2 emission but also offers useful products that can serve as fuels such as CO, HCOOH, CH 3 OH, and CH 4. [6] Moreover, the drive power of CO 2 RR could come from renewable energy resources, such as solar, wind, and hydraulic resources, which indicates that in a green concept, CO 2 RR could complete the carbon loop and potentially solve the issues of global warming and energy crisis simultaneously. [7] 1.1. Fundamental Reaction Pathways of CO 2 RR CO 2 RR is not thermodynamically and kinetically favorable. Every reduction pathway demands a certain amount of energy input. Equations (1-13) shows the reaction steps involved in CO 2 RR (in pH = 7 aqueous solution, vs Normal Hydrogen Electrode (NHE)). [8] As illustrated, it requires a significant amount of reorganizational energy between the linear molecule CO 2 and the bent radical anion − CO 2 • (Equation (1)). When coupling with proton in the reaction, the required reaction energy decreases (Equations (2-12)). Aqueous media with H 2 O molecules become ideal for providing proton into the CO 2 RR system. The reduction potential of hydrogen evolution reaction (HER) (Equation (13)) is close to that of CO 2 RR. It makes HER a competitive reaction against CO 2 RR during the reduction CO 2 reduction reaction (CO 2 RR) provides a promising strategy for sustainable carbon fixation by converting CO 2 into value-added fuels and chemicals. In recent years, considerable efforts are focused on the development of transition-metal (TM)-based catalysts for the selectively electrochemical CO 2 reduction reaction (ECO 2 RR). Co-based catalysts emerge as one of the most promising electrocatalysts with high Faradaic efficiency, current density, and low overpotential, exhibiting excellent catalytic performance toward ECO 2 RR for CO and HCOOH productions that are economically viable. The intrinsic contribution of Co and the synergistic effects in Co-hybrid catalysts play essential roles for ...

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“…Most recently, it has been demonstrated that C 2+ selectivity could be enhanced by tuning CO 2 mass transport via the catalyst layer structure, feed concentration, and flow rate of CO 2 in gas-diffusion electrode electrolyzers. Modulation of local CO 2 concentration enabled an optimized faradaic efficiency toward C 2+ products of up to 75.5% at 300 mA cm −2 in 1.0 M KHCO 3 [86].…”

Section: Introductionmentioning

confidence: 99%

Three-Dimensional Cathodes for Electrochemical Reduction of CO2: From Macro- to Nano-Engineering

et al. 2020

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Rising anthropogenic CO2 emissions and their climate warming effects have triggered a global response in research and development to reduce the emissions of this harmful greenhouse gas. The use of CO2 as a feedstock for the production of value-added fuels and chemicals is a promising pathway for development of renewable energy storage and reduction of carbon emissions. Electrochemical CO2 conversion offers a promising route for value-added products. Considerable challenges still remain, limiting this technology for industrial deployment. This work reviews the latest developments in experimental and modeling studies of three-dimensional cathodes towards high-performance electrochemical reduction of CO2. The fabrication–microstructure–performance relationships of electrodes are examined from the macro- to nanoscale. Furthermore, future challenges, perspectives and recommendations for high-performance cathodes are also presented.

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Modulating Local CO2 Concentration as a General Strategy for Enhancing C−C Coupling in CO2 Electroreduction

Cited by 289 publications

References 46 publications

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives

Three-Dimensional Cathodes for Electrochemical Reduction of CO2: From Macro- to Nano-Engineering

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Modulating Local CO2 Concentration as a General Strategy for Enhancing C−C Coupling in CO2 Electroreduction

Cited by 289 publications

References 46 publications

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

Enhancing carbon dioxide gas-diffusion electrolysis by creating a hydrophobic catalyst microenvironment

Nanostructured Cobalt‐Based Electrocatalysts for CO2Reduction: Recent Progress, Challenges, and Perspectives

Three-Dimensional Cathodes for Electrochemical Reduction of CO2: From Macro- to Nano-Engineering

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Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives