Confined Intermediates Boost C2+ Selectivity in CO<sub>2</sub> Electroreduction

Addressing the efficient electrochemical conversion of CO2 (CO2RR) into valuable multicarbon (C2+) products necessitates innovative strategies to boost carbon (C1) intermediate coupling on catalyst surfaces. In this work, we introduce a surface-confinement strategy on Cu2O nanoparticles by long alkyl chain grafting to create a spatially confined environment, impeding C1 intermediate detachment and promoting C–C coupling in the CO2RR. The optimized C12–Cu2O sample exhibits a Faradaic efficiency (FE) over 63.0% for C2H4, more than double the yield of pristine Cu2O (FE = 25.7%). In situ ATR-FTIR spectroscopy provides direct evidence of rapid C1 intermediate enrichment and restricted diffusion within the surface-confined environment. Molecular dynamics simulations further support these findings by identifying a prolonged residency time that is proportionate to the alkyl chain length, thereby maximizing C2+ selectivity. This surface-confinement approach marks a previously overlooked but immensely promising paradigm in the catalyst design for the CO2RR.

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Publication Details

Journal
ACS Catalysis
Published
2024-08-23
DOI
https://doi.org/10.1021/acscatal.4c02823
Citations
38
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
3.89

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article

Confined Intermediates Boost C2+ Selectivity in CO2 Electroreduction

Pengwei Huo, Chengqi Guo, Yiying Zhou, John C. Crittenden et al.
38 citations
ACS Catalysis
CO2 Reduction Techniques and Catalysts
3.89
article

Confined Intermediates Boost C2+ Selectivity in CO2 Electroreduction

Pengwei Huo, Chengqi Guo, Yiying Zhou, John C. Crittenden, Yun Hau Ng, Yahui Chen, Enhui Jiang, Yanjun Gong, Wanhe Li, Xiaoke Chen, Shuhan Jia, Yue Zou, Zhi Zhu, Zhonghuan Liu, Y.F. YAN, Yan Yan
article en
38 citations

Abstract

Addressing the efficient electrochemical conversion of CO2 (CO2RR) into valuable multicarbon (C2+) products necessitates innovative strategies to boost carbon (C1) intermediate coupling on catalyst surfaces. In this work, we introduce a surface-confinement strategy on Cu2O nanoparticles by long alkyl chain grafting to create a spatially confined environment, impeding C1 intermediate detachment and promoting C–C coupling in the CO2RR. The optimized C12–Cu2O sample exhibits a Faradaic efficiency (FE) over 63.0% for C2H4, more than double the yield of pristine Cu2O (FE = 25.7%). In situ ATR-FTIR spectroscopy provides direct evidence of rapid C1 intermediate enrichment and restricted diffusion within the surface-confined environment. Molecular dynamics simulations further support these findings by identifying a prolonged residency time that is proportionate to the alkyl chain length, thereby maximizing C2+ selectivity. This surface-confinement approach marks a previously overlooked but immensely promising paradigm in the catalyst design for the CO2RR.

ACS CatalysisVol. 14(17)
Jiangsu University (CN), Georgia Institute of Technology (US), Shandong University (CN), City University of Hong Kong (HK)
National Natural Science Foundation of China, Science and Technology Planning Social Development Project of Zhenjiang City, Senior Talent Foundation of Jiangsu University, Graduate Research and Innovation Projects of Jiangsu Province
Affordable and clean energy
Openalex Percentile: Top 5%
CO2 Reduction Techniques and Catalysts
3.89
DOISourceOpenAlex
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