Advances in the direct electro-conversion of captured CO<sub>2</sub> into valuable products

Langie, Kezia; Bak, Gwangsu; Lee, Ung; Lee, Dong Ki; Lee, Chan Woo; Hwang, Yun Jeong; Won, Da Hye

doi:10.1039/d4ta01178c

J. Mater. Chem. A

2024

DOI: 10.1039/d4ta01178c

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Advances in the direct electro-conversion of captured CO₂ into valuable products

Kezia Langie,

Gwangsu Bak,

Ung Lee

et al.

Abstract: The direct electrochemical conversion of captured CO2 (c-eCO2R) into valuable chemicals has recently emerged as a promising carbon capture and utilisation technology that will contribute to achieving net-zero carbon emissions....

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Cited by 3 publications

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Exploring the critical role of binders in electrochemical CO2 reduction reactions

Chae,

Kim,

Lee

et al. 2024

Nano Energy

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Exploring the critical role of binders in electrochemical CO2 reduction reactions

Chae,

Kim,

Lee

et al. 2024

Nano Energy

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Microwave-Assisted Synthesis of a Defect-Rich CuO Electrode for Selective Electrochemical CO₂ Reduction to C₂₊ Products

Chen,

Luo,

et al. 2024

ACS Sustainable Chem. Eng.

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Electrochemical reduction of CO2 to valuable C2+ chemicals using renewable energy is a crucial pathway for sustainable development, replacing traditional nonrenewable feedstocks. In this study, CuO-based materials were synthesized with and without microwave heating as electrocatalysts for CO2 reduction. The CuO synthesized under microwave irradiation (MW-CuO) showed a similar morphology to the conventionally heated samples but exhibited a higher density of defect sites with increased grain boundaries (GBs). MW-CuO electrodes with a Cu2+ and CO3 2– reactant ratio of 1.1 showed superior catalytic performance under identical reaction conditions. In particular, the catalytic activity of the MW-CuO electrode at −1.04 V vs RHE for the C2+ products is 49.3% higher than that of the CuO electrode. A faradaic efficiency (FE) of 71.9% is achieved for C2+ products, which is among the highest yields reported for OD-Cu catalysts. The spent MW-CuO electrode exhibited a significantly higher Cu+ to Cu0 ratio compared to the CuO electrode. The synergy of Cu(I) species and defective surface features is speculated to be responsible for the improved CO2ER selectivity toward multicarbon products. However, the activity decreased for longer reactions, which was attributed to the loss of defect sites and Cu agglomerations. This study highlights the effectiveness of a simple synthesis approach for the production of defect-rich electrocatalysts that improve the efficiency and selectivity of CO2 reduction.

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Integrated Carbon Dioxide Capture by Amines and Conversion to Methane on Single-Atom Nickel Catalysts

Neves-Garcia,

Hasan,

Zhu

et al. 2024

J. Am. Chem. Soc.

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Direct electrochemical reduction of carbon dioxide (CO 2 ) capture species, i.e., carbamate and (bi)carbonate, can be promising for CO 2 capture and conversion from point-source, where the energetically demanding stripping step is bypassed. Here, we describe a class of atomically dispersed nickel (Ni) catalysts electrodeposited on various electrode surfaces that are shown to directly convert captured CO 2 to methane (CH 4 ). A detailed study employing X-ray photoelectron spectroscopy (XPS) and electron microscopy (EM) indicate that highly dispersed Ni atoms are uniquely active for converting capture species to CH 4 , and the activity of single-atom Ni is confirmed using control experiments with a molecularly defined Ni phthalocyanine catalyst supported on carbon nanotubes. Comparing the kinetics of various capture solutions obtained from hydroxide, ammonia, primary, secondary, and tertiary amines provide evidence that carbamate, rather than (bi)carbonate and/or dissolved CO 2 , is primarily responsible for CH 4 production. This conclusion is supported by 13 C nuclear magnetic resonance (NMR) spectroscopy of capture solutions as well as control experiments comparing reaction selectivity with and without CO 2 purging. These findings are understood with the help of density functional theory (DFT) calculations showing that single-atom nickel (Ni) dispersed on gold (Au) is active for the direct reduction of carbamate, producing CH 4 as the primary product. This is the first example of direct electrochemical conversion of carbamate to CH 4 , and the mechanism of this process provides new insight on the potential for integrated capture and conversion of CO 2 directly to hydrocarbons.

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Advances in the direct electro-conversion of captured CO₂ into valuable products

Abstract: The direct electrochemical conversion of captured CO2 (c-eCO2R) into valuable chemicals has recently emerged as a promising carbon capture and utilisation technology that will contribute to achieving net-zero carbon emissions....

Cited by 3 publications

References 66 publications

Exploring the critical role of binders in electrochemical CO2 reduction reactions

Exploring the critical role of binders in electrochemical CO2 reduction reactions

Microwave-Assisted Synthesis of a Defect-Rich CuO Electrode for Selective Electrochemical CO₂ Reduction to C₂₊ Products

Integrated Carbon Dioxide Capture by Amines and Conversion to Methane on Single-Atom Nickel Catalysts

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Advances in the direct electro-conversion of captured CO2 into valuable products

Abstract: The direct electrochemical conversion of captured CO2 (c-eCO2R) into valuable chemicals has recently emerged as a promising carbon capture and utilisation technology that will contribute to achieving net-zero carbon emissions....

Cited by 3 publications

References 66 publications

Exploring the critical role of binders in electrochemical CO2 reduction reactions

Exploring the critical role of binders in electrochemical CO2 reduction reactions

Microwave-Assisted Synthesis of a Defect-Rich CuO Electrode for Selective Electrochemical CO2 Reduction to C2+ Products

Integrated Carbon Dioxide Capture by Amines and Conversion to Methane on Single-Atom Nickel Catalysts

Contact Info

Product

Resources

About

Advances in the direct electro-conversion of captured CO₂ into valuable products

Microwave-Assisted Synthesis of a Defect-Rich CuO Electrode for Selective Electrochemical CO₂ Reduction to C₂₊ Products