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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.
    2. Xinyan Liu & Jianping Xiao & Hongjie Peng & Xin Hong & Karen Chan & Jens K. Nørskov, 2017. "Understanding trends in electrochemical carbon dioxide reduction rates," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
    3. Sheng-Chih Lin & Chun-Chih Chang & Shih-Yun Chiu & Hsiao-Tien Pai & Tzu-Yu Liao & Chia-Shuo Hsu & Wei-Hung Chiang & Ming-Kang Tsai & Hao Ming Chen, 2020. "Operando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
    4. Jianfeng Huang & Nicolas Hörmann & Emad Oveisi & Anna Loiudice & Gian Luca De Gregorio & Oliviero Andreussi & Nicola Marzari & Raffaella Buonsanti, 2018. "Potential-induced nanoclustering of metallic catalysts during electrochemical CO2 reduction," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    5. Yuvraj Y. Birdja & Elena Pérez-Gallent & Marta C. Figueiredo & Adrien J. Göttle & Federico Calle-Vallejo & Marc T. M. Koper, 2019. "Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels," Nature Energy, Nature, vol. 4(9), pages 732-745, September.
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    3. Jian Zhang & Thomas Quast & Bashir Eid & Yen-Ting Chen & Ridha Zerdoumi & Stefan Dieckhöfer & João R. C. Junqueira & Sabine Seisel & Wolfgang Schuhmann, 2024. "In-situ electrochemical reconstruction and modulation of adsorbed hydrogen coverage in cobalt/ruthenium-based catalyst boost electroreduction of nitrate to ammonia," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    4. 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.
    5. 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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