IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-40970-y.html
   My bibliography  Save this article

Activating dynamic atomic-configuration for single-site electrocatalyst in electrochemical CO2 reduction

Author

Listed:
  • Chia-Shuo Hsu

    (National Taiwan University)

  • Jiali Wang

    (National Taiwan University)

  • You-Chiuan Chu

    (National Taiwan University)

  • Jui-Hsien Chen

    (National Taiwan University)

  • Chia-Ying Chien

    (National Taiwan University)

  • Kuo-Hsin Lin

    (Industrial Technology Research Institute)

  • Li Duan Tsai

    (Industrial Technology Research Institute)

  • Hsiao-Chien Chen

    (Chang Gung University)

  • Yen-Fa Liao

    (National Synchrotron Radiation Research Center)

  • Nozomu Hiraoka

    (Japan Synchrotron Radiation Research Institute)

  • Yuan-Chung Cheng

    (National Taiwan University)

  • Hao Ming Chen

    (National Taiwan University
    National Synchrotron Radiation Research Center
    Taipei Medical University)

Abstract

One challenge for realizing high-efficiency electrocatalysts for CO2 electroreduction is lacking in comprehensive understanding of potential-driven chemical state and dynamic atomic-configuration evolutions. Herein, by using a complementary combination of in situ/operando methods and employing copper single-atom electrocatalyst as a model system, we provide evidence on how the complex interplay among dynamic atomic-configuration, chemical state change and surface coulombic charging determines the resulting product profiles. We further demonstrate an informative indicator of atomic surface charge (φe) for evaluating the CO2RR performance, and validate potential-driven dynamic low-coordinated Cu centers for performing significantly high selectivity and activity toward CO product over the well-known four N-coordinated counterparts. It indicates that the structural reconstruction only involved the dynamic breaking of Cu–N bond is partially reversible, whereas Cu–Cu bond formation is clearly irreversible. For all single-atom electrocatalysts (Cu, Fe and Co), the φe value for efficient CO production has been revealed closely correlated with the configuration transformation to generate dynamic low-coordinated configuration. A universal explication can be concluded that the dynamic low-coordinated configuration is the active form to efficiently catalyze CO2-to-CO conversion.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40970-y
    DOI: 10.1038/s41467-023-40970-y
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-40970-y
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-40970-y?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. 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.
    2. 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.
    3. 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. "Author Correction: Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu," Nature Communications, Nature, vol. 14(1), pages 1-1, December.
    4. Hemma Mistry & Ana Sofia Varela & Cecile S. Bonifacio & Ioannis Zegkinoglou & Ilya Sinev & Yong-Wook Choi & Kim Kisslinger & Eric A. Stach & Judith C. Yang & Peter Strasser & Beatriz Roldan Cuenya, 2016. "Correction: Corrigendum: Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene," Nature Communications, Nature, vol. 7(1), pages 1-1, December.
    5. Hong Nhan Nong & Lorenz J. Falling & Arno Bergmann & Malte Klingenhof & Hoang Phi Tran & Camillo Spöri & Rik Mom & Janis Timoshenko & Guido Zichittella & Axel Knop-Gericke & Simone Piccinin & Javier P, 2020. "Key role of chemistry versus bias in electrocatalytic oxygen evolution," Nature, Nature, vol. 587(7834), pages 408-413, November.
    6. Wen Ju & Alexander Bagger & Guang-Ping Hao & Ana Sofia Varela & Ilya Sinev & Volodymyr Bon & Beatriz Roldan Cuenya & Stefan Kaskel & Jan Rossmeisl & Peter Strasser, 2017. "Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO2," Nature Communications, Nature, vol. 8(1), pages 1-9, December.
    7. Kun Zhao & Xiaowa Nie & Haozhi Wang & Shuo Chen & Xie Quan & Hongtao Yu & Wonyong Choi & Guanghui Zhang & Bupmo Kim & Jingguang G. Chen, 2020. "Selective electroreduction of CO2 to acetone by single copper atoms anchored on N-doped porous carbon," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    8. Zhe Weng & Yueshen Wu & Maoyu Wang & Jianbing Jiang & Ke Yang & Shengjuan Huo & Xiao-Feng Wang & Qing Ma & Gary W. Brudvig & Victor S. Batista & Yongye Liang & Zhenxing Feng & Hailiang Wang, 2018. "Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    9. 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.
    10. Hong Bin Yang & Sung-Fu Hung & Song Liu & Kaidi Yuan & Shu Miao & Liping Zhang & Xiang Huang & Hsin-Yi Wang & Weizheng Cai & Rong Chen & Jiajian Gao & Xiaofeng Yang & Wei Chen & Yanqiang Huang & Hao M, 2018. "Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction," Nature Energy, Nature, vol. 3(2), pages 140-147, February.
    11. Min Liu & Yuanjie Pang & Bo Zhang & Phil De Luna & Oleksandr Voznyy & Jixian Xu & Xueli Zheng & Cao Thang Dinh & Fengjia Fan & Changhong Cao & F. Pelayo García de Arquer & Tina Saberi Safaei & Adam Me, 2016. "Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration," Nature, Nature, vol. 537(7620), pages 382-386, September.
    12. Hemma Mistry & Ana Sofia Varela & Cecile S. Bonifacio & Ioannis Zegkinoglou & Ilya Sinev & Yong-Wook Choi & Kim Kisslinger & Eric A. Stach & Judith C. Yang & Peter Strasser & Beatriz Roldan Cuenya, 2016. "Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene," Nature Communications, Nature, vol. 7(1), pages 1-9, November.
    13. Kristjan Kunnus & Morgane Vacher & Tobias C. B. Harlang & Kasper S. Kjær & Kristoffer Haldrup & Elisa Biasin & Tim B. Driel & Mátyás Pápai & Pavel Chabera & Yizhu Liu & Hideyuki Tatsuno & Cornelia Tim, 2020. "Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. 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.
    2. 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.

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. 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.
    2. 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.
    3. 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.
    4. 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.
    5. Eamonn Murphy & Yuanchao Liu & Ivana Matanovic & Martina Rüscher & Ying Huang & Alvin Ly & Shengyuan Guo & Wenjie Zang & Xingxu Yan & Andrea Martini & Janis Timoshenko & Beatriz Roldán Cuenya & Iryna , 2023. "Elucidating electrochemical nitrate and nitrite reduction over atomically-dispersed transition metal sites," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    6. Wei Liu & Pengbo Zhai & Aowen Li & Bo Wei & Kunpeng Si & Yi Wei & Xingguo Wang & Guangda Zhu & Qian Chen & Xiaokang Gu & Ruifeng Zhang & Wu Zhou & Yongji Gong, 2022. "Electrochemical CO2 reduction to ethylene by ultrathin CuO nanoplate arrays," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    7. Ji Wei Sun & Xuefeng Wu & Peng Fei Liu & Jiacheng Chen & Yuanwei Liu & Zhen Xin Lou & Jia Yue Zhao & Hai Yang Yuan & Aiping Chen & Xue Lu Wang & Minghui Zhu & Sheng Dai & Hua Gui Yang, 2023. "Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    8. 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.
    9. 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.
    10. 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.
    11. Sung-Fu Hung & Aoni Xu & Xue Wang & Fengwang Li & Shao-Hui Hsu & Yuhang Li & Joshua Wicks & Eduardo González Cervantes & Armin Sedighian Rasouli & Yuguang C. Li & Mingchuan Luo & Dae-Hyun Nam & Ning W, 2022. "A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    12. Ahmad, Naveed & Chen, Ying & Wang, Xiaoxiao & Sun, Peixu & Bao, Yuting & Xu, Xia, 2022. "Highly efficient electrochemical upgrade of CO2 to CO using AMP capture solution as electrolyte," Renewable Energy, Elsevier, vol. 189(C), pages 444-453.
    13. Jie Yin & Jing Jin & Zhouyang Yin & Liu Zhu & Xin Du & Yong Peng & Pinxian Xi & Chun-Hua Yan & Shouheng Sun, 2023. "The built-in electric field across FeN/Fe3N interface for efficient electrochemical reduction of CO2 to CO," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    14. Yinchao Yao & Tong Shi & Wenxing Chen & Jiehua Wu & Yunying Fan & Yichun Liu & Liang Cao & Zhuo Chen, 2024. "A surface strategy boosting the ethylene selectivity for CO2 reduction and in situ mechanistic insights," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    15. Cai Wang & Xiaoyu Wang & Houan Ren & Yilin Zhang & Xiaomei Zhou & Jing Wang & Qingxin Guan & Yuping Liu & Wei Li, 2023. "Combining Fe nanoparticles and pyrrole-type Fe-N4 sites on less-oxygenated carbon supports for electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    16. 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.
    17. Yizhou Dai & Huan Li & Chuanhao Wang & Weiqing Xue & Menglu Zhang & Donghao Zhao & Jing Xue & Jiawei Li & Laihao Luo & Chunxiao Liu & Xu Li & Peixin Cui & Qiu Jiang & Tingting Zheng & Songqi Gu & Yao , 2023. "Manipulating local coordination of copper single atom catalyst enables efficient CO2-to-CH4 conversion," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    18. 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.
    19. Ruiz-López, Estela & Gandara-Loe, Jesús & Baena-Moreno, Francisco & Reina, Tomas Ramirez & Odriozola, José Antonio, 2022. "Electrocatalytic CO2 conversion to C2 products: Catalysts design, market perspectives and techno-economic aspects," Renewable and Sustainable Energy Reviews, Elsevier, vol. 161(C).
    20. Antonia Herzog & Mauricio Lopez Luna & Hyo Sang Jeon & Clara Rettenmaier & Philipp Grosse & Arno Bergmann & Beatriz Roldan Cuenya, 2024. "Operando Raman spectroscopy uncovers hydroxide and CO species enhance ethanol selectivity during pulsed CO2 electroreduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40970-y. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.