Enhanced electrochemical CO<sub>2</sub>-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst

Shen, Yi; Pan, Yongliang; Xiao, Huanyong; Zhang, Haizhong; Zhu, Chao; Fang, Qile; Li, Yungui; Lu, Lun; Ye, Liqun; Song, Shuang

doi:10.1039/d3ta08073k

J. Mater. Chem. A

2024

DOI: 10.1039/d3ta08073k

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Enhanced electrochemical CO₂-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst

Yi Shen,

Yongliang Pan,

Huanyong Xiao

et al.

Abstract: Electrocatalytic reduction of carbon dioxide (CO2RR) to C2+ products presents an ideal approach to mitigate the continuous accumulation of CO2 for achieving carbon neutrality. However, the selectivity for C2+ products...

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Synergistic Coordination in Cu Single‐Atom Catalysts Enhances High‐Valent Copper‐Oxo Species for Efficient PMS Activation

Shen,

Pan,

Zhu

et al. 2024

Small

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In the domain of heterogeneous catalytic activation of peroxymonosulfate (PMS), high‐valent metal‐oxo (HVMO) species are widely recognized as potent oxidants for the abatement of organic pollutants. However, the generation selectivity and efficiency of HVMO are often constrained by stringent requirements for catalyst adsorption sites and electron transfer efficiency. In this study, a single‐atom catalyst, CuSA/CNP&S, is synthesized featuring multiple types (planar/axial) of heteroatom coordination via an H‐bond‐assisted self‐assembly strategy. It is confirmed that CuN3 active centers with axial S coordination are uniformly distributed in a carbon matrix modified by planar P atoms. CuSA/CNP&S activated PMS to selectively generate Cu(III)═OH species as the primary reactive oxygen species (ROS). The pseudo‐first‐order kinetic rate for bisphenol A degradation reached 1.51 min−1, a 17.57‐fold increase compared to the unmodified CuSA/CN catalyst. Additionally, the CuSA/CNP&S catalyst demonstrates high efficiency and durability in removing contaminants from various aqueous matrices. Theoretical calculations and experimental results indicate that the intrinsic electric field generated by distal planar P atoms enhances electron transfer efficiency within the carbon matrix. Meanwhile, axial S coordination elevates the d‐band center and tunes the eg* band broadening of Cu, thereby enhancing the adsorption selectivity for the terminal oxygen of PMS. This multitype coordination synergistically mitigates the issues of low selectivity and yield of HVMO species.

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Synergistic Coordination in Cu Single‐Atom Catalysts Enhances High‐Valent Copper‐Oxo Species for Efficient PMS Activation

Shen,

Pan,

Zhu

et al. 2024

Small

View full text Add to dashboard Cite

show abstract

Recent advances in electrocatalytic conversion of CO2-to-ethylene: From reaction mechanisms to tuning strategies

Zhang,

Zhang

2025

Applied Catalysis B: Environment and Energy

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Masked second-shell sulfur coordinating atomically dispersed Pd on tin oxide boosts the direct synthesis of hydrogen peroxide

Li,

Zheng,

et al. 2024

Chemical Engineering Journal

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Enhanced electrochemical CO₂-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst

Abstract: Electrocatalytic reduction of carbon dioxide (CO2RR) to C2+ products presents an ideal approach to mitigate the continuous accumulation of CO2 for achieving carbon neutrality. However, the selectivity for C2+ products...

Cited by 3 publications

References 83 publications

Synergistic Coordination in Cu Single‐Atom Catalysts Enhances High‐Valent Copper‐Oxo Species for Efficient PMS Activation

Synergistic Coordination in Cu Single‐Atom Catalysts Enhances High‐Valent Copper‐Oxo Species for Efficient PMS Activation

Recent advances in electrocatalytic conversion of CO2-to-ethylene: From reaction mechanisms to tuning strategies

Masked second-shell sulfur coordinating atomically dispersed Pd on tin oxide boosts the direct synthesis of hydrogen peroxide

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Enhanced electrochemical CO2-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst

Abstract: Electrocatalytic reduction of carbon dioxide (CO2RR) to C2+ products presents an ideal approach to mitigate the continuous accumulation of CO2 for achieving carbon neutrality. However, the selectivity for C2+ products...

Cited by 3 publications

References 83 publications

Synergistic Coordination in Cu Single‐Atom Catalysts Enhances High‐Valent Copper‐Oxo Species for Efficient PMS Activation

Synergistic Coordination in Cu Single‐Atom Catalysts Enhances High‐Valent Copper‐Oxo Species for Efficient PMS Activation

Recent advances in electrocatalytic conversion of CO2-to-ethylene: From reaction mechanisms to tuning strategies

Masked second-shell sulfur coordinating atomically dispersed Pd on tin oxide boosts the direct synthesis of hydrogen peroxide

Contact Info

Product

Resources

About

Enhanced electrochemical CO₂-to-ethylene conversion through second-shell coordination on a Cu single-atom catalyst