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Operando studies reveal active Cu nanograins for CO2 electroreduction

Author

Listed:
  • Yao Yang

    (University of California
    University of California
    Lawrence Berkeley National Laboratory)

  • Sheena Louisia

    (University of California
    Lawrence Berkeley National Laboratory)

  • Sunmoon Yu

    (Lawrence Berkeley National Laboratory
    University of California)

  • Jianbo Jin

    (University of California)

  • Inwhan Roh

    (University of California
    Lawrence Berkeley National Laboratory)

  • Chubai Chen

    (University of California
    Lawrence Berkeley National Laboratory)

  • Maria V. Fonseca Guzman

    (University of California
    Lawrence Berkeley National Laboratory)

  • Julian Feijóo

    (University of California
    Lawrence Berkeley National Laboratory)

  • Peng-Cheng Chen

    (University of California
    Kavli Energy NanoScience Institute)

  • Hongsen Wang

    (Cornell University)

  • Christopher J. Pollock

    (Cornell University)

  • Xin Huang

    (Cornell University)

  • Yu-Tsun Shao

    (Cornell University)

  • Cheng Wang

    (Lawrence Berkeley National Laboratory)

  • David A. Muller

    (Cornell University
    Cornell University)

  • Héctor D. Abruña

    (Cornell University
    Cornell University)

  • Peidong Yang

    (University of California
    Lawrence Berkeley National Laboratory
    University of California
    Kavli Energy NanoScience Institute)

Abstract

Carbon dioxide electroreduction facilitates the sustainable synthesis of fuels and chemicals1. Although Cu enables CO2-to-multicarbon product (C2+) conversion, the nature of the active sites under operating conditions remains elusive2. Importantly, identifying active sites of high-performance Cu nanocatalysts necessitates nanoscale, time-resolved operando techniques3–5. Here, we present a comprehensive investigation of the structural dynamics during the life cycle of Cu nanocatalysts. A 7 nm Cu nanoparticle ensemble evolves into metallic Cu nanograins during electrolysis before complete oxidation to single-crystal Cu2O nanocubes following post-electrolysis air exposure. Operando analytical and four-dimensional electrochemical liquid-cell scanning transmission electron microscopy shows the presence of metallic Cu nanograins under CO2 reduction conditions. Correlated high-energy-resolution time-resolved X-ray spectroscopy suggests that metallic Cu, rich in nanograin boundaries, supports undercoordinated active sites for C–C coupling. Quantitative structure–activity correlation shows that a higher fraction of metallic Cu nanograins leads to higher C2+ selectivity. A 7 nm Cu nanoparticle ensemble, with a unity fraction of active Cu nanograins, exhibits sixfold higher C2+ selectivity than the 18 nm counterpart with one-third of active Cu nanograins. The correlation of multimodal operando techniques serves as a powerful platform to advance our fundamental understanding of the complex structural evolution of nanocatalysts under electrochemical conditions.

Suggested Citation

  • Yao Yang & Sheena Louisia & Sunmoon Yu & Jianbo Jin & Inwhan Roh & Chubai Chen & Maria V. Fonseca Guzman & Julian Feijóo & Peng-Cheng Chen & Hongsen Wang & Christopher J. Pollock & Xin Huang & Yu-Tsun, 2023. "Operando studies reveal active Cu nanograins for CO2 electroreduction," Nature, Nature, vol. 614(7947), pages 262-269, February.
  • Handle: RePEc:nat:nature:v:614:y:2023:i:7947:d:10.1038_s41586-022-05540-0
    DOI: 10.1038/s41586-022-05540-0
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    Cited by:

    1. Hefei Li & Pengfei Wei & Tianfu Liu & Mingrun Li & Chao Wang & Rongtan Li & Jinyu Ye & Zhi-You Zhou & Shi-Gang Sun & Qiang Fu & Dunfeng Gao & Guoxiong Wang & Xinhe Bao, 2024. "CO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Ruixin Yang & Yanming Cai & Yongbing Qi & Zhuodong Tang & Jun-Jie Zhu & Jinxiang Li & Wenlei Zhu & Zixuan Chen, 2024. "How local electric field regulates C–C coupling at a single nanocavity in electrocatalytic CO2 reduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Yamei Fan & Rongtan Li & Beibei Wang & Xiaohui Feng & Xiangze Du & Chengxiang Liu & Fei Wang & Conghui Liu & Cui Dong & Yanxiao Ning & Rentao Mu & Qiang Fu, 2024. "Water-assisted oxidative redispersion of Cu particles through formation of Cu hydroxide at room temperature," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Jiawei Zhu & Yu Zhang & Zitao Chen & Zhenbao Zhang & Xuezeng Tian & Minghua Huang & Xuedong Bai & Xue Wang & Yongfa Zhu & Heqing Jiang, 2024. "Superexchange-stabilized long-distance Cu sites in rock-salt-ordered double perovskite oxides for CO2 electromethanation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    5. Lin Li & Ying Lv & Hongting Sheng & Yonglei Du & Haifeng Li & Yapei Yun & Ziyi Zhang & Haizhu Yu & Manzhou Zhu, 2023. "A low-nuclear Ag4 nanocluster as a customized catalyst for the cyclization of propargylamine with CO2," Nature Communications, Nature, vol. 14(1), pages 1-7, December.
    6. 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.
    7. 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.
    8. 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).
    9. Kang Yang & Ming Li & Tianqi Gao & Guoliang Xu & Di Li & Yao Zheng & Qiang Li & Jingjing Duan, 2024. "An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    10. Lei Wang & Zhiwen Chen & Yi Xiao & Linke Huang & Xiyang Wang & Holly Fruehwald & Dmitry Akhmetzyanov & Mathew Hanson & Zuolong Chen & Ning Chen & Brant Billinghurst & Rodney D. L. Smith & Chandra Veer, 2024. "Stabilized Cuδ+-OH species on in situ reconstructed Cu nanoparticles for CO2-to-C2H4 conversion in neutral media," Nature Communications, Nature, vol. 15(1), pages 1-11, 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.

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