IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-48209-0.html
   My bibliography  Save this article

Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media

Author

Listed:
  • Longxiang Liu

    (University College London)

  • Liqun Kang

    (Max-Planck-Institute for Chemical Energy Conversion)

  • Jianrui Feng

    (University College London)

  • David G. Hopkinson

    (Harwell Science and Innovation Campus)

  • Christopher S. Allen

    (Harwell Science and Innovation Campus
    University of Oxford)

  • Yeshu Tan

    (University College London)

  • Hao Gu

    (University College London)

  • Iuliia Mikulska

    (Harwell Science and Innovation Campus)

  • Veronica Celorrio

    (Harwell Science and Innovation Campus)

  • Diego Gianolio

    (Harwell Science and Innovation Campus)

  • Tianlei Wang

    (University College London)

  • Liquan Zhang

    (University College London)

  • Kaiqi Li

    (University College London)

  • Jichao Zhang

    (University College London)

  • Jiexin Zhu

    (University College London)

  • Georg Held

    (Harwell Science and Innovation Campus)

  • Pilar Ferrer

    (Harwell Science and Innovation Campus)

  • David Grinter

    (Harwell Science and Innovation Campus)

  • June Callison

    (Rutherford Appleton Laboratory)

  • Martin Wilding

    (Rutherford Appleton Laboratory)

  • Sining Chen

    (University College London)

  • Ivan Parkin

    (University College London)

  • Guanjie He

    (University College London)

Abstract

Electrochemical hydrogen peroxide (H2O2) production (EHPP) via a two-electron oxygen reduction reaction (2e- ORR) provides a promising alternative to replace the energy-intensive anthraquinone process. M-N-C electrocatalysts, which consist of atomically dispersed transition metals and nitrogen-doped carbon, have demonstrated considerable EHPP efficiency. However, their full potential, particularly regarding the correlation between structural configurations and performances in neutral media, remains underexplored. Herein, a series of ultralow metal-loading M-N-C electrocatalysts are synthesized and investigated for the EHPP process in the neutral electrolyte. CoNCB material with the asymmetric Co-C/N/O configuration exhibits the highest EHPP activity and selectivity among various as-prepared M-N-C electrocatalyst, with an outstanding mass activity (6.1 × 105 A gCo−1 at 0.5 V vs. RHE), and a high practical H2O2 production rate (4.72 mol gcatalyst−1 h−1 cm−2). Compared with the popularly recognized square-planar symmetric Co-N4 configuration, the superiority of asymmetric Co-C/N/O configurations is elucidated by X-ray absorption fine structure spectroscopy analysis and computational studies.

Suggested Citation

  • Longxiang Liu & Liqun Kang & Jianrui Feng & David G. Hopkinson & Christopher S. Allen & Yeshu Tan & Hao Gu & Iuliia Mikulska & Veronica Celorrio & Diego Gianolio & Tianlei Wang & Liquan Zhang & Kaiqi , 2024. "Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-48209-0
    DOI: 10.1038/s41467-024-48209-0
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-48209-0
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-48209-0?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. Gao-Feng Han & Feng Li & Wei Zou & Mohammadreza Karamad & Jong-Pil Jeon & Seong-Wook Kim & Seok-Jin Kim & Yunfei Bu & Zhengping Fu & Yalin Lu & Samira Siahrostami & Jong-Beom Baek, 2020. "Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Jiajun Zhao & Cehuang Fu & Ke Ye & Zheng Liang & Fangling Jiang & Shuiyun Shen & Xiaoran Zhao & Lu Ma & Zulipiya Shadike & Xiaoming Wang & Junliang Zhang & Kun Jiang, 2022. "Manipulating the oxygen reduction reaction pathway on Pt-coordinated motifs," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Anqi Zeng & Wu Chen & Kasper Dalgas Rasmussen & Xuehong Zhu & Maren Lundhaug & Daniel B. Müller & Juan Tan & Jakob K. Keiding & Litao Liu & Tao Dai & Anjian Wang & Gang Liu, 2022. "Battery technology and recycling alone will not save the electric mobility transition from future cobalt shortages," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    4. Qingran Zhang & Xin Tan & Nicholas M. Bedford & Zhaojun Han & Lars Thomsen & Sean Smith & Rose Amal & Xunyu Lu, 2020. "Direct insights into the role of epoxy groups on cobalt sites for acidic H2O2 production," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    5. Kun Jiang & Seoin Back & Austin J. Akey & Chuan Xia & Yongfeng Hu & Wentao Liang & Diane Schaak & Eli Stavitski & Jens K. Nørskov & Samira Siahrostami & Haotian Wang, 2019. "Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination," Nature Communications, Nature, vol. 10(1), pages 1-11, 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. Xiao Zhang & Xunhua Zhao & Peng Zhu & Zachary Adler & Zhen-Yu Wu & Yuanyue Liu & Haotian Wang, 2022. "Electrochemical oxygen reduction to hydrogen peroxide at practical rates in strong acidic media," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    2. Jiannan Du & Guokang Han & Wei Zhang & Lingfeng Li & Yuqi Yan & Yaoxuan Shi & Xue Zhang & Lin Geng & Zhijiang Wang & Yueping Xiong & Geping Yin & Chunyu Du, 2023. "CoIn dual-atom catalyst for hydrogen peroxide production via oxygen reduction reaction in acid," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Qilong Wu & Haiyuan Zou & Xin Mao & Jinghan He & Yanmei Shi & Shuangming Chen & Xuecheng Yan & Liyun Wu & Chengguang Lang & Bin Zhang & Li Song & Xin Wang & Aijun Du & Qin Li & Yi Jia & Jun Chen & Xia, 2023. "Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    4. Jinxing Chen & Qian Ma & Xiliang Zheng & Youxing Fang & Jin Wang & Shaojun Dong, 2022. "Kinetically restrained oxygen reduction to hydrogen peroxide with nearly 100% selectivity," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    5. Qiang Tian & Lingyan Jing & Hongnan Du & Yunchao Yin & Xiaolei Cheng & Jiaxin Xu & Junyu Chen & Zhuoxin Liu & Jiayu Wan & Jian Liu & Jinlong Yang, 2024. "Mesoporous carbon spheres with programmable interiors as efficient nanoreactors for H2O2 electrosynthesis," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    6. Peike Cao & Xie Quan & Xiaowa Nie & Kun Zhao & Yanming Liu & Shuo Chen & Hongtao Yu & Jingguang G. Chen, 2023. "Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    7. Ping Liu & Teng Liang & Yutong Li & Ziqing Zhang & Zhuo Li & Ji Bian & Liqiang Jing, 2024. "Photocatalytic H2O2 production over boron-doped g-C3N4 containing coordinatively unsaturated FeOOH sites and CoOx clusters," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    8. Hu, Xueyue & Wang, Chunying & Elshkaki, Ayman, 2024. "Material-energy Nexus: A systematic literature review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 192(C).
    9. Che Lah, Nurul Akmal, 2021. "Late transition metal nanocomplexes: Applications for renewable energy conversion and storage," Renewable and Sustainable Energy Reviews, Elsevier, vol. 145(C).
    10. Yang, Jingluan & Chen, Wei, 2023. "Unravelling the landscape of global cobalt trade: Patterns, robustness, and supply chain security," Resources Policy, Elsevier, vol. 86(PB).
    11. Adeline Gu'eret & Wolf-Peter Schill & Carlos Gaete-Morales, 2024. "Impacts of electric carsharing on a power sector with variable renewables," Papers 2402.19380, arXiv.org, revised Oct 2024.
    12. Zhou, Na & Su, Hui & Wu, Qiaosheng & Hu, Shougeng & Xu, Deyi & Yang, Danhui & Cheng, Jinhua, 2022. "China's lithium supply chain: Security dynamics and policy countermeasures," Resources Policy, Elsevier, vol. 78(C).
    13. Kaiyuan Wang & Qing Hong & Caixia Zhu & Yuan Xu & Wang Li & Ying Wang & Wenhao Chen & Xiang Gu & Xinghua Chen & Yanfeng Fang & Yanfei Shen & Songqin Liu & Yuanjian Zhang, 2024. "Metal-ligand dual-site single-atom nanozyme mimicking urate oxidase with high substrates specificity," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    14. Huang, Jianbai & Dong, Xuesong & Chen, Jinyu & Zeng, Anqi, 2023. "The slow-release effect of recycling on rapid demand growth of critical metals from EV batteries up to 2050: Evidence from China," Resources Policy, Elsevier, vol. 82(C).
    15. Song, Huiling & Wang, Chang & Sun, Kun & Geng, Hongjun & Zuo, Lyushui, 2023. "Material efficiency strategies across the industrial chain to secure indium availability for global carbon neutrality," Resources Policy, Elsevier, vol. 85(PB).
    16. Wei Peng & Jiaxin Liu & Xiaoqing Liu & Liqun Wang & Lichang Yin & Haotian Tan & Feng Hou & Ji Liang, 2023. "Facilitating two-electron oxygen reduction with pyrrolic nitrogen sites for electrochemical hydrogen peroxide production," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    17. Mao, Ning & Gadkari, Siddharth & Wang, Zhirong & Zhang, Teng & Bai, Jinglong & Cai, Qiong, 2023. "A comparative analysis of lithium-ion batteries with different cathodes under overheating and nail penetration conditions," Energy, Elsevier, vol. 278(PB).
    18. Zhirong Zhang & Chen Feng & Dongdi Wang & Shiming Zhou & Ruyang Wang & Sunpei Hu & Hongliang Li & Ming Zuo & Yuan Kong & Jun Bao & Jie Zeng, 2022. "Selectively anchoring single atoms on specific sites of supports for improved oxygen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    19. Jun Qi & Yadong Du & Qi Yang & Na Jiang & Jiachun Li & Yi Ma & Yangjun Ma & Xin Zhao & Jieshan Qiu, 2023. "Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    20. Rashmi Mehrotra & Dongrak Oh & Ji-Wook Jang, 2021. "Unassisted selective solar hydrogen peroxide production by an oxidised buckypaper-integrated perovskite photocathode," Nature Communications, Nature, vol. 12(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_s41467-024-48209-0. 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.