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Highly selective electrocatalytic CO2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper

Author

Listed:
  • Haiping Xu

    (Argonne National Laboratory
    Department of Chemistry and Biochemistry Northern Illinois University)

  • Dominic Rebollar

    (Argonne National Laboratory
    Department of Chemistry and Biochemistry Northern Illinois University)

  • Haiying He

    (Valparaiso University)

  • Lina Chong

    (Argonne National Laboratory)

  • Yuzi Liu

    (Argonne National Laboratory)

  • Cong Liu

    (Argonne National Laboratory)

  • Cheng-Jun Sun

    (Argonne National Laboratory Argonne)

  • Tao Li

    (Department of Chemistry and Biochemistry Northern Illinois University
    Argonne National Laboratory Argonne)

  • John V. Muntean

    (Argonne National Laboratory)

  • Randall E. Winans

    (Argonne National Laboratory Argonne)

  • Di-Jia Liu

    (Argonne National Laboratory
    The University of Chicago)

  • Tao Xu

    (Department of Chemistry and Biochemistry Northern Illinois University)

Abstract

Direct electrochemical conversion of CO2 to ethanol offers a promising strategy to lower CO2 emissions while storing energy from renewable electricity. However, current electrocatalysts offer only limited selectivity toward ethanol. Here we report a carbon-supported copper (Cu) catalyst, synthesized by an amalgamated Cu–Li method, that achieves a single-product Faradaic efficiency (FE) of 91% at −0.7 V (versus the reversible hydrogen electrode) and onset potential as low as −0.4 V (reversible hydrogen electrode) for electrocatalytic CO2-to-ethanol conversion. The catalyst operated stably over 16 h. The FE of ethanol was highly sensitive to the initial dispersion of Cu atoms and decreased significantly when CuO and large Cu clusters become predominant species. Operando X-ray absorption spectroscopy identified a reversible transformation from atomically dispersed Cu atoms to Cun clusters (n = 3 and 4) on application of electrochemical conditions. First-principles calculations further elucidate the possible catalytic mechanism of CO2 reduction over Cun.

Suggested Citation

  • Haiping Xu & Dominic Rebollar & Haiying He & Lina Chong & Yuzi Liu & Cong Liu & Cheng-Jun Sun & Tao Li & John V. Muntean & Randall E. Winans & Di-Jia Liu & Tao Xu, 2020. "Highly selective electrocatalytic CO2 reduction to ethanol by metallic clusters dynamically formed from atomically dispersed copper," Nature Energy, Nature, vol. 5(8), pages 623-632, August.
  • Handle: RePEc:nat:natene:v:5:y:2020:i:8:d:10.1038_s41560-020-0666-x
    DOI: 10.1038/s41560-020-0666-x
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    Citations

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    Cited by:

    1. Charles E. Creissen & Marc Fontecave, 2022. "Keeping sight of copper in single-atom catalysts for electrochemical carbon dioxide reduction," Nature Communications, Nature, vol. 13(1), pages 1-4, December.
    2. Xiaozhi Su & Zhuoli Jiang & Jing Zhou & Hengjie Liu & Danni Zhou & Huishan Shang & Xingming Ni & Zheng Peng & Fan Yang & Wenxing Chen & Zeming Qi & Dingsheng Wang & Yu Wang, 2022. "Complementary Operando Spectroscopy identification of in-situ generated metastable charge-asymmetry Cu2-CuN3 clusters for CO2 reduction to ethanol," Nature Communications, Nature, vol. 13(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. Yongxiang Liang & Jiankang Zhao & Yu Yang & Sung-Fu Hung & Jun Li & Shuzhen Zhang & Yong Zhao & An Zhang & Cheng Wang & Dominique Appadoo & Lei Zhang & Zhigang Geng & Fengwang Li & Jie Zeng, 2023. "Stabilizing copper sites in coordination polymers toward efficient electrochemical C-C coupling," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Chia-Shuo Hsu & Jiali Wang & You-Chiuan Chu & Jui-Hsien Chen & Chia-Ying Chien & Kuo-Hsin Lin & Li Duan Tsai & Hsiao-Chien Chen & Yen-Fa Liao & Nozomu Hiraoka & Yuan-Chung Cheng & Hao Ming Chen, 2023. "Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    6. Hao Sun & Ling Chen & Likun Xiong & Kun Feng & Yufeng Chen & Xiang Zhang & Xuzhou Yuan & Baiyu Yang & Zhao Deng & Yu Liu & Mark H. Rümmeli & Jun Zhong & Yan Jiao & Yang Peng, 2021. "Promoting ethylene production over a wide potential window on Cu crystallites induced and stabilized via current shock and charge delocalization," Nature Communications, Nature, vol. 12(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. Janis Timoshenko & Clara Rettenmaier & Dorottya Hursán & Martina Rüscher & Eduardo Ortega & Antonia Herzog & Timon Wagner & Arno Bergmann & Uta Hejral & Aram Yoon & Andrea Martini & Eric Liberra & Mar, 2024. "Reversible metal cluster formation on Nitrogen-doped carbon controlling electrocatalyst particle size with subnanometer accuracy," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    9. Baiyu Yang & Ling Chen & Songlin Xue & Hao Sun & Kun Feng & Yufeng Chen & Xiang Zhang & Long Xiao & Yongze Qin & Jun Zhong & Zhao Deng & Yan Jiao & Yang Peng, 2022. "Electrocatalytic CO2 reduction to alcohols by modulating the molecular geometry and Cu coordination in bicentric copper complexes," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    10. Kaihang Yue & Yanyang Qin & Honghao Huang & Zhuoran Lv & Mingzhi Cai & Yaqiong Su & Fuqiang Huang & Ya Yan, 2024. "Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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