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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. Rosa M. Arán-Ais & Fabian Scholten & Sebastian Kunze & Rubén Rizo & Beatriz Roldan Cuenya, 2020. "The role of in situ generated morphological motifs and Cu(i) species in C2+ product selectivity during CO2 pulsed electroreduction," Nature Energy, Nature, vol. 5(4), pages 317-325, April.
    2. Miao Zhong & Kevin Tran & Yimeng Min & Chuanhao Wang & Ziyun Wang & Cao-Thang Dinh & Phil De Luna & Zongqian Yu & Armin Sedighian Rasouli & Peter Brodersen & Song Sun & Oleksandr Voznyy & Chih-Shan Ta, 2020. "Accelerated discovery of CO2 electrocatalysts using active machine learning," Nature, Nature, vol. 581(7807), pages 178-183, May.
    3. Stefan Ringe & Carlos G. Morales-Guio & Leanne D. Chen & Meredith Fields & Thomas F. Jaramillo & Christopher Hahn & Karen Chan, 2020. "Double layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    4. Dan Ren & Jinhuan Fong & Boon Siang Yeo, 2018. "The effects of currents and potentials on the selectivities of copper toward carbon dioxide electroreduction," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    5. Christina W. Li & Jim Ciston & Matthew W. Kanan, 2014. "Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper," Nature, Nature, vol. 508(7497), pages 504-507, April.
    6. Xinyan Liu & Philomena Schlexer & Jianping Xiao & Yongfei Ji & Lei Wang & Robert B. Sandberg & Michael Tang & Kristopher S. Brown & Hongjie Peng & Stefan Ringe & Christopher Hahn & Thomas F. Jaramillo, 2019. "pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
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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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