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Promoting ethylene production over a wide potential window on Cu crystallites induced and stabilized via current shock and charge delocalization

Author

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  • Hao Sun

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Ling Chen

    (The University of Adelaide)

  • Likun Xiong

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Kun Feng

    (Soochow University)

  • Yufeng Chen

    (Soochow University)

  • Xiang Zhang

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Xuzhou Yuan

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Baiyu Yang

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Zhao Deng

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Yu Liu

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Mark H. Rümmeli

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

  • Jun Zhong

    (Soochow University)

  • Yan Jiao

    (The University of Adelaide)

  • Yang Peng

    (Soochow University
    Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province)

Abstract

Electrochemical CO2 reduction (CO2RR) in a product-orientated and energy-efficient manner relies on rational catalyst design guided by mechanistic understandings. In this study, the effect of conducting support on the CO2RR behaviors of semi-conductive metal-organic framework (MOF) — Cu3(HITP)2 are carefully investigated. Compared to the stand-alone MOF, adding Ketjen Black greatly promotes C2H4 production with a stabilized Faradaic efficiency between 60-70% in a wide potential range and prolonged period. Multicrystalline Cu nano-crystallites in the reconstructed MOF are induced and stabilized by the conducting support via current shock and charge delocalization, which is analogous to the mechanism of dendrite prevention through conductive scaffolds in metal ion batteries. Density functional theory calculations elucidate that the contained multi-facets and rich grain boundaries promote C–C coupling while suppressing HER. This study underlines the key role of substrate-catalyst interaction, and the regulation of Cu crystalline states via conditioning the charge transport, in steering the CO2RR pathway.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27169-9
    DOI: 10.1038/s41467-021-27169-9
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    Cited by:

    1. Shifu Wang & Fuhua Li & Jian Zhao & Yaqiong Zeng & Yifan Li & Zih-Yi Lin & Tsung-Ju Lee & Shuhui Liu & Xinyi Ren & Weijue Wang & Yusen Chen & Sung-Fu Hung & Ying-Rui Lu & Yi Cui & Xiaofeng Yang & Xuni, 2024. "Manipulating C-C coupling pathway in electrochemical CO2 reduction for selective ethylene and ethanol production over single-atom alloy catalyst," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. 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.
    3. 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.
    4. Weihua Guo & Siwei Zhang & Junjie Zhang & Haoran Wu & Yangbo Ma & Yun Song & Le Cheng & Liang Chang & Geng Li & Yong Liu & Guodan Wei & Lin Gan & Minghui Zhu & Shibo Xi & Xue Wang & Boris I. Yakobson , 2023. "Accelerating multielectron reduction at CuxO nanograins interfaces with controlled local electric field," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    5. 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.
    6. Wenpeng Ni & Houjun Chen & Naizhuo Tang & Ting Hu & Wei Zhang & Yan Zhang & Shiguo Zhang, 2024. "High-purity ethylene production via indirect carbon dioxide electrochemical reduction," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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