IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v10y2019i1d10.1038_s41467-019-11992-2.html
   My bibliography  Save this article

Highly selective oxygen reduction to hydrogen peroxide on transition metal single atom coordination

Author

Listed:
  • Kun Jiang

    (Harvard University)

  • Seoin Back

    (Stanford University)

  • Austin J. Akey

    (Harvard University)

  • Chuan Xia

    (Harvard University)

  • Yongfeng Hu

    (University of Saskatchewan)

  • Wentao Liang

    (Kostas Research Institute, Northeastern University)

  • Diane Schaak

    (Harvard University)

  • Eli Stavitski

    (Brookhaven National Laboratory)

  • Jens K. Nørskov

    (Stanford University
    SLAC National Accelerator Laboratory)

  • Samira Siahrostami

    (Stanford University
    University of Calgary, 2500 University Drive NW)

  • Haotian Wang

    (Harvard University
    Rice University)

Abstract

Shifting electrochemical oxygen reduction towards 2e– pathway to hydrogen peroxide (H2O2), instead of the traditional 4e– to water, becomes increasingly important as a green method for H2O2 generation. Here, through a flexible control of oxygen reduction pathways on different transition metal single atom coordination in carbon nanotube, we discovered Fe-C-O as an efficient H2O2 catalyst, with an unprecedented onset of 0.822 V versus reversible hydrogen electrode in 0.1 M KOH to deliver 0.1 mA cm−2 H2O2 current, and a high H2O2 selectivity of above 95% in both alkaline and neutral pH. A wide range tuning of 2e–/4e– ORR pathways was achieved via different metal centers or neighboring metalloid coordination. Density functional theory calculations indicate that the Fe-C-O motifs, in a sharp contrast to the well-known Fe-C-N for 4e–, are responsible for the H2O2 pathway. This iron single atom catalyst demonstrated an effective water disinfection as a representative application.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11992-2
    DOI: 10.1038/s41467-019-11992-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-019-11992-2
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-019-11992-2?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
    ---><---

    Citations

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


    Cited by:

    1. 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.
    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. 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.
    4. 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.
    5. 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.
    6. Liangbo Xie & Pengfei Wang & Yi Li & Dongpeng Zhang & Denghui Shang & Wenwen Zheng & Yuguo Xia & Sihui Zhan & Wenping Hu, 2022. "Pauling-type adsorption of O2 induced electrocatalytic singlet oxygen production on N–CuO for organic pollutants degradation," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    7. 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.
    8. Zhiyong Yu & Hao Deng & Qing Yao & Liangqun Zhao & Fei Xue & Tianou He & Zhiwei Hu & Wei-Hsiang Huang & Chih-Wen Pao & Li-Ming Yang & Xiaoqing Huang, 2024. "Selective and durable H2O2 electrosynthesis catalyst in acid by selenization induced straining and phasing," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    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. Huaning Jiang & Weiwei Yang & Mingquan Xu & Erqing Wang & Yi Wei & Wei Liu & Xiaokang Gu & Lixuan Liu & Qian Chen & Pengbo Zhai & Xiaolong Zou & Pulickel M. Ajayan & Wu Zhou & Yongji Gong, 2022. "Single atom catalysts in Van der Waals gaps," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    11. 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.
    12. 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.
    13. 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.
    14. 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.
    15. 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.
    16. Fei He & Seunghyun Weon & Woojung Jeon & Myoung Won Chung & Wonyong Choi, 2021. "Self-wetting triphase photocatalysis for effective and selective removal of hydrophilic volatile organic compounds in air," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    17. Jihyun Baek & Qiu Jin & Nathan Scott Johnson & Yue Jiang & Rui Ning & Apurva Mehta & Samira Siahrostami & Xiaolin Zheng, 2022. "Discovery of LaAlO3 as an efficient catalyst for two-electron water electrolysis towards hydrogen peroxide," Nature Communications, Nature, vol. 13(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:10:y:2019:i:1:d:10.1038_s41467-019-11992-2. 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.

    We have no bibliographic references for this item. You can help adding them by using 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.