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Trends in oxygenate/hydrocarbon selectivity for electrochemical CO(2) reduction to C2 products

Author

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  • Hong-Jie Peng

    (SLAC National Accelerator Laboratory
    Stanford University)

  • Michael T. Tang

    (SLAC National Accelerator Laboratory
    Stanford University)

  • Joakim Halldin Stenlid

    (SLAC National Accelerator Laboratory
    Stanford University)

  • Xinyan Liu

    (Stanford University)

  • Frank Abild-Pedersen

    (SLAC National Accelerator Laboratory)

Abstract

The electrochemical conversion of carbon di-/monoxide into commodity chemicals paves a way towards a sustainable society but it also presents one of the great challenges in catalysis. Herein, we present the trends in selectivity towards specific dicarbon oxygenate/hydrocarbon products from carbon monoxide reduction on transition metal catalysts, with special focus on copper. We unveil the distinctive role of electrolyte pH in tuning the dicarbon oxygenate/hydrocarbon selectivity. The understanding is based on density functional theory calculated energetics and microkinetic modeling. We identify the critical reaction steps determining selectivity and relate their transition state energies to two simple descriptors, the carbon and hydroxide binding strengths. The atomistic insight gained enables us to rationalize a number of experimental observations and provides avenues towards the design of selective electrocatalysts for liquid fuel production from carbon di-/monoxide.

Suggested Citation

  • Hong-Jie Peng & Michael T. Tang & Joakim Halldin Stenlid & Xinyan Liu & Frank Abild-Pedersen, 2022. "Trends in oxygenate/hydrocarbon selectivity for electrochemical CO(2) reduction to C2 products," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-29140-8
    DOI: 10.1038/s41467-022-29140-8
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    References listed on IDEAS

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    1. Xinyue Wang & Yuanjun Chen & Feng Li & Rui Kai Miao & Jianan Erick Huang & Zilin Zhao & Xiao-Yan Li & Roham Dorakhan & Senlin Chu & Jinhong Wu & Sixing Zheng & Weiyan Ni & Dongha Kim & Sungjin Park & , 2024. "Site-selective protonation enables efficient carbon monoxide electroreduction to acetate," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Jing Li & Haocheng Xiong & Xiaozhi Liu & Donghuan Wu & Dong Su & Bingjun Xu & Qi Lu, 2023. "Weak CO binding sites induced by Cu–Ag interfaces promote CO electroreduction to multi-carbon liquid products," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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