IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v13y2022i1d10.1038_s41467-022-30411-7.html
   My bibliography  Save this article

Kinetically restrained oxygen reduction to hydrogen peroxide with nearly 100% selectivity

Author

Listed:
  • Jinxing Chen

    (State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences
    University of Science and Technology of China)

  • Qian Ma

    (State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences
    University of Science and Technology of China)

  • Xiliang Zheng

    (State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences)

  • Youxing Fang

    (State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences)

  • Jin Wang

    (Stony Brook University)

  • Shaojun Dong

    (State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences
    University of Science and Technology of China)

Abstract

Hydrogen peroxide has been synthesized mainly through the electrocatalytic and photocatalytic oxygen reduction reaction in recent years. Herein, we synthesize a single-atom rhodium catalyst (Rh1/NC) to mimic the properties of flavoenzymes for the synthesis of hydrogen peroxide under mild conditions. Rh1/NC dehydrogenates various substrates and catalyzes the reduction of oxygen to hydrogen peroxide. The maximum hydrogen peroxide production rate is 0.48 mol gcatalyst−1 h−1 in the phosphorous acid aerobic oxidation reaction. We find that the selectivity of oxygen reduction to hydrogen peroxide can reach 100%. This is because a single catalytic site of Rh1/NC can only catalyze the removal of two electrons per substrate molecule; thus, the subsequent oxygen can only obtain two electrons to reduce to hydrogen peroxide through the typical two-electron pathway. Similarly, due to the restriction of substrate dehydrogenation, the hydrogen peroxide selectivity in commercial Pt/C-catalyzed enzymatic reactions can be found to reach 75%, which is 30 times higher than that in electrocatalytic oxygen reduction reactions.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30411-7
    DOI: 10.1038/s41467-022-30411-7
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-022-30411-7
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-022-30411-7?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. 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.
    3. Yoann Roux & Rémy Ricoux & Frédéric Avenier & Jean-Pierre Mahy, 2015. "Bio-inspired electron-delivering system for reductive activation of dioxygen at metal centres towards artificial flavoenzymes," Nature Communications, Nature, vol. 6(1), pages 1-8, 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. 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.
    2. Qianjun Zhi & Rong Jiang & Xiya Yang & Yucheng Jin & Dongdong Qi & Kang Wang & Yunpeng Liu & Jianzhuang Jiang, 2024. "Dithiine-linked metalphthalocyanine framework with undulated layers for highly efficient and stable H2O2 electroproduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    3. 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.
    4. Hongni Chen & Chao Wang & Han Wu & Lili Li & Yali Xing & Chuanhui Zhang & Xiaojing Long, 2024. "Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-14, 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. 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.
    2. 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.
    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. 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.
    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. 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.
    7. 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).
    8. 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.
    9. 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.
    10. 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.
    11. 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.
    12. 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.
    13. 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.
    14. 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.
    15. Yangyang Liu & Can Li & Chunhui Tan & Zengxia Pei & Tao Yang & Shuzhen Zhang & Qianwei Huang & Yihan Wang & Zheng Zhou & Xiaozhou Liao & Juncai Dong & Hao Tan & Wensheng Yan & Huajie Yin & Zhao-Qing L, 2023. "Electrosynthesis of chlorine from seawater-like solution through single-atom catalysts," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    16. 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.
    17. 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.
    18. 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.
    19. 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.
    20. 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.

    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:13:y:2022:i:1:d:10.1038_s41467-022-30411-7. 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.