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Dynamic transformation of cubic copper catalysts during CO2 electroreduction and its impact on catalytic selectivity

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  • Philipp Grosse

    (Fritz-Haber Institute of the Max Planck Society)

  • Aram Yoon

    (Fritz-Haber Institute of the Max Planck Society)

  • Clara Rettenmaier

    (Fritz-Haber Institute of the Max Planck Society)

  • Antonia Herzog

    (Fritz-Haber Institute of the Max Planck Society)

  • See Wee Chee

    (Fritz-Haber Institute of the Max Planck Society)

  • Beatriz Roldan Cuenya

    (Fritz-Haber Institute of the Max Planck Society)

Abstract

To rationally design effective and stable catalysts for energy conversion applications, we need to understand how they transform under reaction conditions and reveal their underlying structure-property relationships. This is especially important for catalysts used in the electroreduction of carbon dioxide where product selectivity is sensitive to catalyst structure. Here, we present real-time electrochemical liquid cell transmission electron microscopy studies showing the restructuring of copper(I) oxide cubes during reaction. Fragmentation of the solid cubes, re-deposition of new nanoparticles, catalyst detachment and catalyst aggregation are observed as a function of the applied potential and time. Using cubes with different initial sizes and loading, we further correlate this dynamic morphology with the catalytic selectivity through time-resolved scanning electron microscopy measurements and product analysis. These comparative studies reveal the impact of nanoparticle re-deposition and detachment on the catalyst reactivity, and how the increased surface metal loading created by re-deposited nanoparticles can lead to enhanced C2+ selectivity and stability.

Suggested Citation

  • Philipp Grosse & Aram Yoon & Clara Rettenmaier & Antonia Herzog & See Wee Chee & Beatriz Roldan Cuenya, 2021. "Dynamic transformation of cubic copper catalysts during CO2 electroreduction and its impact on catalytic selectivity," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26743-5
    DOI: 10.1038/s41467-021-26743-5
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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.
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    1. Hugo-Pieter Iglesias van Montfort & Mengran Li & Erdem Irtem & Maryam Abdinejad & Yuming Wu & Santosh K. Pal & Mark Sassenburg & Davide Ripepi & Siddhartha Subramanian & Jasper Biemolt & Thomas E. Ruf, 2023. "Non-invasive current collectors for improved current-density distribution during CO2 electrolysis on super-hydrophobic electrodes," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Shikai Liu & Yuheng Li & Di Wang & Shibo Xi & Haoming Xu & Yulin Wang & Xinzhe Li & Wenjie Zang & Weidong Liu & Mengyao Su & Katherine Yan & Adam C. Nielander & Andrew B. Wong & Jiong Lu & Thomas F. J, 2024. "Alkali cation-induced cathodic corrosion in Cu electrocatalysts," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    3. Kaili Yao & Jun Li & Adnan Ozden & Haibin Wang & Ning Sun & Pengyu Liu & Wen Zhong & Wei Zhou & Jieshu Zhou & Xi Wang & Hanqi Liu & Yongchang Liu & Songhua Chen & Yongfeng Hu & Ziyun Wang & David Sint, 2024. "In situ copper faceting enables efficient CO2/CO electrolysis," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Ahmed M. Abdellah & Fatma Ismail & Oliver W. Siig & Jie Yang & Carmen M. Andrei & Liza-Anastasia DiCecco & Amirhossein Rakhsha & Kholoud E. Salem & Kathryn Grandfield & Nabil Bassim & Robert Black & G, 2024. "Impact of palladium/palladium hydride conversion on electrochemical CO2 reduction via in-situ transmission electron microscopy and diffraction," Nature Communications, Nature, vol. 15(1), pages 1-15, December.

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