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Potential-induced nanoclustering of metallic catalysts during electrochemical CO2 reduction

Author

Listed:
  • Jianfeng Huang

    (École Polytechnique Fédérale de Lausanne)

  • Nicolas Hörmann

    (École Polytechnique Fédérale de Lausanne)

  • Emad Oveisi

    (École Polytechnique Fédérale de Lausanne)

  • Anna Loiudice

    (École Polytechnique Fédérale de Lausanne)

  • Gian Luca De Gregorio

    (École Polytechnique Fédérale de Lausanne)

  • Oliviero Andreussi

    (École Polytechnique Fédérale de Lausanne
    University of North Texas)

  • Nicola Marzari

    (École Polytechnique Fédérale de Lausanne)

  • Raffaella Buonsanti

    (École Polytechnique Fédérale de Lausanne)

Abstract

In catalysis science stability is as crucial as activity and selectivity. Understanding the degradation pathways occurring during operation and developing mitigation strategies will eventually improve catalyst design, thus facilitating the translation of basic science to technological applications. Herein, we reveal the unique and general degradation mechanism of metallic nanocatalysts during electrochemical CO2 reduction, exemplified by different sized copper nanocubes. We follow their morphological evolution during operation and correlate it with the electrocatalytic performance. In contrast with the most common coalescence and dissolution/precipitation mechanisms, we find a potential-driven nanoclustering to be the predominant degradation pathway. Grand-potential density functional theory calculations confirm the role of the negative potential applied to reduce CO2 as the main driving force for the clustering. This study offers a novel outlook on future investigations of stability and degradation reaction mechanisms of nanocatalysts in electrochemical CO2 reduction and, more generally, in electroreduction reactions.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-05544-3
    DOI: 10.1038/s41467-018-05544-3
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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. Chen, Jiateng & Xu, Le & Shen, Boxiong, 2024. "Recent advances in tandem electrocatalysis of carbon dioxide: A review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 199(C).
    4. Xin, Liyong & Yu, Wei & Liu, Chao & Liu, Lang & Wang, Shukun & Li, Xiaoxiao & Liu, Yu, 2023. "Thermal stability of a mixed working fluid (R513A) for organic Rankine cycle," Energy, Elsevier, vol. 263(PF).
    5. 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.
    6. Woong Choi & Younghyun Chae & Ershuai Liu & Dongjin Kim & Walter S. Drisdell & Hyung-suk Oh & Jai Hyun Koh & Dong Ki Lee & Ung Lee & Da Hye Won, 2024. "Exploring the influence of cell configurations on Cu catalyst reconstruction during CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    7. Li Zhang & Xiaoju Yang & Qing Yuan & Zhiming Wei & Jie Ding & Tianshu Chu & Chao Rong & Qiao Zhang & Zhenkun Ye & Fu-Zhen Xuan & Yueming Zhai & Bowei Zhang & Xuan Yang, 2023. "Elucidating the structure-stability relationship of Cu single-atom catalysts using operando surface-enhanced infrared absorption spectroscopy," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    8. Cornelius A. Obasanjo & Guorui Gao & Jackson Crane & Viktoria Golovanova & F. Pelayo García de Arquer & Cao-Thang Dinh, 2023. "High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    9. Wei Liu & Xiting Wang & Fan Wang & Kaifa Du & Zhaofu Zhang & Yuzheng Guo & Huayi Yin & Dihua Wang, 2021. "A durable and pH-universal self-standing MoC–Mo2C heterojunction electrode for efficient hydrogen evolution reaction," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    10. 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.
    11. Jing Xue & Xue Dong & Chunxiao Liu & Jiawei Li & Yizhou Dai & Weiqing Xue & Laihao Luo & Yuan Ji & Xiao Zhang & Xu Li & Qiu Jiang & Tingting Zheng & Jianping Xiao & Chuan Xia, 2024. "Turning copper into an efficient and stable CO evolution catalyst beyond noble metals," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    12. 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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