IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-52790-9.html
   My bibliography  Save this article

Spontaneous formation of reactive redox radical species at the interface of gas diffusion electrode

Author

Listed:
  • Ruijuan Zhao

    (University of Electronic Science and Technology of China)

  • Lei Li

    (University of Electronic Science and Technology of China)

  • Qianbao Wu

    (University of Electronic Science and Technology of China)

  • Wei Luo

    (University of Electronic Science and Technology of China)

  • Qiu Zhang

    (University of Electronic Science and Technology of China)

  • Chunhua Cui

    (University of Electronic Science and Technology of China)

Abstract

The aqueous interface-rich system has been proposed to act as a trigger and a reservoir for reactive radicals, playing a crucial role in chemical reactions. Although much is known about the redox reactivity of water microdroplets at “droplets-in-gas” interfaces, it remains poorly understood for “bubbles-in-water” interfaces that are created by feeding gas through the porous membrane of the gas diffusion electrode. Here we reveal the spontaneous generation of highly reactive redox radical species detected by using electron paramagnetic resonance under such conditions without applying any bias and loading any catalysts. In combination with ultraviolet-visible spectroscopy, the redox feature has been further verified through several probe molecules. Unexpectedly, introducing crown ether allows to isolate and stabilize both water radical cations and hydrated electrons thus substantially increasing redox reactivity. Our finding suggests a reactive microenvironment at the interface of the gas diffusion electrode owing to the coexistence of oxidative and reductive species.

Suggested Citation

  • Ruijuan Zhao & Lei Li & Qianbao Wu & Wei Luo & Qiu Zhang & Chunhua Cui, 2024. "Spontaneous formation of reactive redox radical species at the interface of gas diffusion electrode," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52790-9
    DOI: 10.1038/s41467-024-52790-9
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-52790-9
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-52790-9?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. Chanyeon Kim & Justin C. Bui & Xiaoyan Luo & Jason K. Cooper & Ahmet Kusoglu & Adam Z. Weber & Alexis T. Bell, 2021. "Tailored catalyst microenvironments for CO2 electroreduction to multicarbon products on copper using bilayer ionomer coatings," Nature Energy, Nature, vol. 6(11), pages 1026-1034, November.
    2. Hongxia Hao & Itai Leven & Teresa Head-Gordon, 2022. "Can electric fields drive chemistry for an aqueous microdroplet?," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. 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.
    4. David Wakerley & Sarah Lamaison & Joshua Wicks & Auston Clemens & Jeremy Feaster & Daniel Corral & Shaffiq A. Jaffer & Amitava Sarkar & Marc Fontecave & Eric B. Duoss & Sarah Baker & Edward H. Sargent, 2022. "Gas diffusion electrodes, reactor designs and key metrics of low-temperature CO2 electrolysers," Nature Energy, Nature, vol. 7(2), pages 130-143, February.
    5. Yan B. Vogel & Cameron W. Evans & Mattia Belotti & Longkun Xu & Isabella C. Russell & Li-Juan Yu & Alfred K. K. Fung & Nicholas S. Hill & Nadim Darwish & Vinicius R. Gonçales & Michelle L. Coote & K. , 2020. "The corona of a surface bubble promotes electrochemical reactions," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    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. 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.
    2. 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.
    3. Xinyi Sun & Xiaowei Mu & Wei Zheng & Lei Wang & Sixie Yang & Chuanchao Sheng & Hui Pan & Wei Li & Cheng-Hui Li & Ping He & Haoshen Zhou, 2023. "Binuclear Cu complex catalysis enabling Li–CO2 battery with a high discharge voltage above 3.0 V," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    4. Wenzhe Niu & Jie Feng & Junfeng Chen & Lei Deng & Wen Guo & Huajing Li & Liqiang Zhang & Youyong Li & Bo Zhang, 2024. "High-efficiency C3 electrosynthesis on a lattice-strain-stabilized nitrogen-doped Cu surface," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. Ahmad Ijaz & SeyedSepehr Mostafayi & Mohammadreza Esmaeilirad & Mohammad Asadi & Javad Abbasian & Hamid Arastoopour, 2025. "Numerical Modeling of CO 2 Reduction Reactions in a Batch Cell with Different Working Electrodes," Sustainability, MDPI, vol. 17(3), pages 1-25, January.
    6. Mengyang Fan & Rui Kai Miao & Pengfei Ou & Yi Xu & Zih-Yi Lin & Tsung-Ju Lee & Sung-Fu Hung & Ke Xie & Jianan Erick Huang & Weiyan Ni & Jun Li & Yong Zhao & Adnan Ozden & Colin P. O’Brien & Yuanjun Ch, 2023. "Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    7. Xiaojie She & Lingling Zhai & Yifei Wang & Pei Xiong & Molly Meng-Jung Li & Tai-Sing Wu & Man Chung Wong & Xuyun Guo & Zhihang Xu & Huaming Li & Hui Xu & Ye Zhu & Shik Chi Edman Tsang & Shu Ping Lau, 2024. "Pure-water-fed, electrocatalytic CO2 reduction to ethylene beyond 1,000 h stability at 10 A," Nature Energy, Nature, vol. 9(1), pages 81-91, January.
    8. Yan Lin & Tuo Wang & Lili Zhang & Gong Zhang & Lulu Li & Qingfeng Chang & Zifan Pang & Hui Gao & Kai Huang & Peng Zhang & Zhi-Jian Zhao & Chunlei Pei & Jinlong Gong, 2023. "Tunable CO2 electroreduction to ethanol and ethylene with controllable interfacial wettability," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    9. Simon Rufer & Michael P. Nitzsche & Sanjay Garimella & Jack R. Lake & Kripa K. Varanasi, 2024. "Hierarchically conductive electrodes unlock stable and scalable CO2 electrolysis," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    10. Tian, Di & Qu, Zhiguo & Zhang, Jianfei, 2023. "Electrochemical condition optimization and techno-economic analysis on the direct CO2 electroreduction of flue gas," Applied Energy, Elsevier, vol. 351(C).
    11. Jiawei Li & Hongliang Zeng & Xue Dong & Yimin Ding & Sunpei Hu & Runhao Zhang & Yizhou Dai & Peixin Cui & Zhou Xiao & Donghao Zhao & Liujiang Zhou & Tingting Zheng & Jianping Xiao & Jie Zeng & Chuan X, 2023. "Selective CO2 electrolysis to CO using isolated antimony alloyed copper," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    12. Junmei Chen & Haoran Qiu & Yilin Zhao & Haozhou Yang & Lei Fan & Zhihe Liu & ShiBo Xi & Guangtai Zheng & Jiayi Chen & Lei Chen & Ya Liu & Liejin Guo & Lei Wang, 2024. "Selective and stable CO2 electroreduction at high rates via control of local H2O/CO2 ratio," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    13. Lele Cui & Bin Chen & Dongxu Chen & Chen He & Yi Liu & Hongyi Zhang & Jian Qiu & Le Liu & Wenheng Jing & Zhenghua Zhang, 2024. "Species mass transfer governs the selectivity of gas diffusion electrodes toward H2O2 electrosynthesis," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    14. Xiaoyang He & Li Lin & Xiangying Li & Minzhi Zhu & Qinghong Zhang & Shunji Xie & Bingbao Mei & Fanfei Sun & Zheng Jiang & Jun Cheng & Ye Wang, 2024. "Roles of copper(I) in water-promoted CO2 electrolysis to multi-carbon compounds," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    15. Ruijie Xie & Kaiheng Guo & Yong Li & Yingguang Zhang & Huanran Zhong & Dennis Y. C. Leung & Haibao Huang, 2024. "Harnessing air-water interface to generate interfacial ROS for ultrafast environmental remediation," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    16. Hugo-Pieter Iglesias van Montfort & Mengran Li & Erdem Irtem & Maryam Abdinejad & Yuming Wu & Santosh K. Pal & Mark Sassenburg & Davide Ripepi & Siddhartha Subramanian & Jasper Biemolt & Thomas E. Ruf, 2023. "Non-invasive current collectors for improved current-density distribution during CO2 electrolysis on super-hydrophobic electrodes," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    17. Ren, Junjie & Yin, Zhenyuan & Lu, Hongfeng & Xu, Chenlu & Kuang, Zenggui & Deng, Wei & Liu, Yunting & Linga, Praveen, 2024. "Effects of South China Sea clayey-silty sediments on the kinetics and morphology of CH4 hydrate: Implication on energy recovery," Applied Energy, Elsevier, vol. 367(C).
    18. Cornelius A. Obasanjo & Guorui Gao & Jackson Crane & Viktoria Golovanova & F. Pelayo García de Arquer & Cao-Thang Dinh, 2023. "High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    19. Kang Yang & Ming Li & Tianqi Gao & Guoliang Xu & Di Li & Yao Zheng & Qiang Li & Jingjing Duan, 2024. "An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    20. Joey Disch & Luca Bohn & Susanne Koch & Michael Schulz & Yiyong Han & Alessandro Tengattini & Lukas Helfen & Matthias Breitwieser & Severin Vierrath, 2022. "High-resolution neutron imaging of salt precipitation and water transport in zero-gap CO2 electrolysis," Nature Communications, Nature, vol. 13(1), pages 1-9, 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:15:y:2024:i:1:d:10.1038_s41467-024-52790-9. 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.