IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-42936-6.html
   My bibliography  Save this article

Direct time-resolved observation of surface-bound carbon dioxide radical anions on metallic nanocatalysts

Author

Listed:
  • Zhiwen Jiang

    (University of Science and Technology of China
    CNRS, Institut de Chimie Physique)

  • Carine Clavaguéra

    (CNRS, Institut de Chimie Physique)

  • Changjiang Hu

    (Nanjing University of Aeronautics and Astronautics)

  • Sergey A. Denisov

    (CNRS, Institut de Chimie Physique)

  • Shuning Shen

    (Nanjing University of Aeronautics and Astronautics)

  • Feng Hu

    (Nanjing University of Aeronautics and Astronautics)

  • Jun Ma

    (University of Science and Technology of China)

  • Mehran Mostafavi

    (CNRS, Institut de Chimie Physique)

Abstract

Time-resolved identification of surface-bound intermediates on metallic nanocatalysts is imperative to develop an accurate understanding of the elementary steps of CO2 reduction. Direct observation on initial electron transfer to CO2 to form surface-bound CO2•− radicals is lacking due to the technical challenges. Here, we use picosecond pulse radiolysis to generate CO2•− via aqueous electron attachment and observe the stabilization processes toward well-defined nanoscale metallic sites. The time-resolved method combined with molecular simulations identifies surface-bound intermediates with characteristic transient absorption bands and distinct kinetics from nanosecond to the second timescale for three typical metallic nanocatalysts: Cu, Au, and Ni. The interfacial interactions are further investigated by varying the important factors, such as catalyst size and the presence of cation in the electrolyte. This work highlights fundamental ultrafast spectroscopy to clarify the critical initial step in the CO2 catalytic reduction mechanism.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42936-6
    DOI: 10.1038/s41467-023-42936-6
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-42936-6
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-42936-6?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. 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.
    2. Huihui Zhang & Chang Xu & Xiaowen Zhan & Yu Yu & Kaifu Zhang & Qiquan Luo & Shan Gao & Jinlong Yang & Yi Xie, 2022. "Mechanistic insights into CO2 conversion chemistry of copper bis-(terpyridine) molecular electrocatalyst using accessible operando spectrochemistry," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    3. Yuvraj Y. Birdja & Elena Pérez-Gallent & Marta C. Figueiredo & Adrien J. Göttle & Federico Calle-Vallejo & Marc T. M. Koper, 2019. "Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels," Nature Energy, Nature, vol. 4(9), pages 732-745, September.
    4. Shan Gao & Yue Lin & Xingchen Jiao & Yongfu Sun & Qiquan Luo & Wenhua Zhang & Dianqi Li & Jinlong Yang & Yi Xie, 2016. "Partially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel," Nature, Nature, vol. 529(7584), pages 68-71, January.
    5. 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.
    6. 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.
    Full references (including those not matched with items on IDEAS)

    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. 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.
    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. Qiong Lei & Liang Huang & Jun Yin & Bambar Davaasuren & Youyou Yuan & Xinglong Dong & Zhi-Peng Wu & Xiaoqian Wang & Ke Xin Yao & Xu Lu & Yu Han, 2022. "Structural evolution and strain generation of derived-Cu catalysts during CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    4. 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).
    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. Xin Chen & Junxiang Chen & Huayu Chen & Qiqi Zhang & Jiaxuan Li & Jiwei Cui & Yanhui Sun & Defa Wang & Jinhua Ye & Lequan Liu, 2023. "Promoting water dissociation for efficient solar driven CO2 electroreduction via improving hydroxyl adsorption," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    7. 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.
    8. 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.
    9. Junyuan Duan & Tianyang Liu & Yinghe Zhao & Ruoou Yang & Yang Zhao & Wenbin Wang & Youwen Liu & Huiqiao Li & Yafei Li & Tianyou Zhai, 2022. "Active and conductive layer stacked superlattices for highly selective CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    10. 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.
    11. 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.
    12. 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.
    13. Shijia Mu & Honglei Lu & Qianbao Wu & Lei Li & Ruijuan Zhao & Chang Long & Chunhua Cui, 2022. "Hydroxyl radicals dominate reoxidation of oxide-derived Cu in electrochemical CO2 reduction," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    14. Yong Yin & Bingcheng Luo & Kezhi Li & Benjamin M. Moskowitz & Bar Mosevitzky Lis & Israel E. Wachs & Minghui Zhu & Ye Sun & Tianle Zhu & Xiang Li, 2024. "Plasma-assisted manipulation of vanadia nanoclusters for efficient selective catalytic reduction of NOx," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    15. Chunjun Chen & Xupeng Yan & Yahui Wu & Xiudong Zhang & Shoujie Liu & Fanyu Zhang & Xiaofu Sun & Qinggong Zhu & Lirong Zheng & Jing Zhang & Xueqing Xing & Zhonghua Wu & Buxing Han, 2023. "Oxidation of metallic Cu by supercritical CO2 and control synthesis of amorphous nano-metal catalysts for CO2 electroreduction," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    16. 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.
    17. Guodong Fu & Xiaomin Kang & Yan Zhang & Ying Guo & Zhiwei Li & Jianwen Liu & Lei Wang & Jiujun Zhang & Xian-Zhu Fu & Jing-Li Luo, 2023. "Capturing critical gem-diol intermediates and hydride transfer for anodic hydrogen production from 5-hydroxymethylfurfural," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    18. Seung-Jae Shin & Hansol Choi & Stefan Ringe & Da Hye Won & Hyung-Suk Oh & Dong Hyun Kim & Taemin Lee & Dae-Hyun Nam & Hyungjun Kim & Chang Hyuck Choi, 2022. "A unifying mechanism for cation effect modulating C1 and C2 productions from CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    19. 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.
    20. Subrato Acharjya & Jiacheng Chen & Minghui Zhu & Chong Peng, 2021. "Elucidating the reactivity and nature of active sites for tin phthalocyanine during CO2 reduction," Greenhouse Gases: Science and Technology, Blackwell Publishing, vol. 11(6), pages 1191-1197, 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_s41467-023-42936-6. 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.