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Operando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction

Author

Listed:
  • Sheng-Chih Lin

    (National Taiwan University)

  • Chun-Chih Chang

    (Department of Chemical and Material Engineering, Chinese Culture University)

  • Shih-Yun Chiu

    (National Taiwan University)

  • Hsiao-Tien Pai

    (National Taiwan Normal University)

  • Tzu-Yu Liao

    (National Taiwan University)

  • Chia-Shuo Hsu

    (National Taiwan University)

  • Wei-Hung Chiang

    (National Taiwan University of Science and Technology)

  • Ming-Kang Tsai

    (National Taiwan Normal University)

  • Hao Ming Chen

    (National Taiwan University
    National Synchrotron Radiation Research Center)

Abstract

Copper electrocatalysts have been shown to selectively reduce carbon dioxide to hydrocarbons. Nevertheless, the absence of a systematic study based on time-resolved spectroscopy renders the functional agent—either metallic or oxidative Copper—for the selectivity still undecidable. Herein, we develop an operando seconds-resolved X-ray absorption spectroscopy to uncover the chemical state evolution of working catalysts. An oxide-derived Copper electrocatalyst is employed as a model catalyst to offer scientific insights into the roles metal states serve in carbon dioxide reduction reaction (CO2RR). Using a potential switching approach, the model catalyst can achieve a steady chemical state of half-Cu(0)-and-half-Cu(I) and selectively produce asymmetric C2 products - C2H5OH. Furthermore, a theoretical analysis reveals that a surface composed of Cu-Cu(I) ensembles can have dual carbon monoxide molecules coupled asymmetrically, which potentially enhances the catalyst’s CO2RR product selectivity toward C2 products. Our results offer understandings of the fundamental chemical states and insights to the establishment of selective CO2RR.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17231-3
    DOI: 10.1038/s41467-020-17231-3
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    References listed on IDEAS

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    1. Christina W. Li & Jim Ciston & Matthew W. Kanan, 2014. "Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper," Nature, Nature, vol. 508(7497), pages 504-507, April.
    2. Dohyung Kim & Joaquin Resasco & Yi Yu & Abdullah Mohamed Asiri & Peidong Yang, 2014. "Synergistic geometric and electronic effects for electrochemical reduction of carbon dioxide using gold–copper bimetallic nanoparticles," Nature Communications, Nature, vol. 5(1), pages 1-8, December.
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    2. Zhiwen Jiang & Carine Clavaguéra & Changjiang Hu & Sergey A. Denisov & Shuning Shen & Feng Hu & Jun Ma & Mehran Mostafavi, 2023. "Direct time-resolved observation of surface-bound carbon dioxide radical anions on metallic nanocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    3. 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.
    4. 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.
    5. Carina Yi Jing Lim & Meltem Yilmaz & Juan Manuel Arce-Ramos & Albertus D. Handoko & Wei Jie Teh & Yuangang Zheng & Zi Hui Jonathan Khoo & Ming Lin & Mark Isaacs & Teck Lip Dexter Tam & Yang Bai & Chee, 2023. "Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    6. 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.
    7. 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.
    8. Erfan Shirzadi & Qiu Jin & Ali Shayesteh Zeraati & Roham Dorakhan & Tiago J. Goncalves & Jehad Abed & Byoung-Hoon Lee & Armin Sedighian Rasouli & Joshua Wicks & Jinqiang Zhang & Pengfei Ou & Victor Bo, 2024. "Ligand-modified nanoparticle surfaces influence CO electroreduction selectivity," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    9. Jiali Wang & Chia-Shuo Hsu & Tai-Sing Wu & Ting-Shan Chan & Nian-Tzu Suen & Jyh-Fu Lee & Hao Ming Chen, 2023. "In situ X-ray spectroscopies beyond conventional X-ray absorption spectroscopy on deciphering dynamic configuration of electrocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-23, December.
    10. Khandelwal, Akshat & Maarisetty, Dileep & Baral, Saroj Sundar, 2022. "Fundamentals and application of single-atom photocatalyst in sustainable energy and environmental applications," Renewable and Sustainable Energy Reviews, Elsevier, vol. 167(C).
    11. 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.
    12. Yajun Zheng & Hedan Yao & Ruinan Di & Zhicheng Xiang & Qiang Wang & Fangfang Lu & Yu Li & Guangxing Yang & Qiang Ma & Zhiping Zhang, 2022. "Water coordinated on Cu(I)-based catalysts is the oxygen source in CO2 reduction to CO," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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