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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
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    Cited by:

    1. 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.
    2. 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.
    3. 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.
    4. 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.
    5. 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.
    6. 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.
    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. 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.
    9. 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.
    10. 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.
    11. 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.
    12. 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.
    13. 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.
    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. 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.

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