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Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2

Author

Listed:
  • Gao-Feng Han

    (Ulsan National Institute of Science and Technology (UNIST))

  • Feng Li

    (Ulsan National Institute of Science and Technology (UNIST))

  • Wei Zou

    (University of Science and Technology of China (USTC))

  • Mohammadreza Karamad

    (University of Calgary, 2500 University Drive NW)

  • Jong-Pil Jeon

    (Ulsan National Institute of Science and Technology (UNIST))

  • Seong-Wook Kim

    (Ulsan National Institute of Science and Technology (UNIST))

  • Seok-Jin Kim

    (Ulsan National Institute of Science and Technology (UNIST))

  • Yunfei Bu

    (School of Environmental Science and Engineering, Nanjing University of Information Science and Technology (NUIST), 219 Ningliu)

  • Zhengping Fu

    (University of Science and Technology of China (USTC)
    University of Science and Technology of China (USTC))

  • Yalin Lu

    (University of Science and Technology of China (USTC)
    University of Science and Technology of China (USTC))

  • Samira Siahrostami

    (University of Calgary, 2500 University Drive NW)

  • Jong-Beom Baek

    (Ulsan National Institute of Science and Technology (UNIST))

Abstract

The one-step electrochemical synthesis of H2O2 is an on-site method that reduces dependence on the energy-intensive anthraquinone process. Oxidized carbon materials have proven to be promising catalysts due to their low cost and facile synthetic procedures. However, the nature of the active sites is still controversial, and direct experimental evidence is presently lacking. Here, we activate a carbon material with dangling edge sites and then decorate them with targeted functional groups. We show that quinone-enriched samples exhibit high selectivity and activity with a H2O2 yield ratio of up to 97.8 % at 0.75 V vs. RHE. Using density functional theory calculations, we identify the activity trends of different possible quinone functional groups in the edge and basal plane of the carbon nanostructure and determine the most active motif. Our findings provide guidelines for designing carbon-based catalysts, which have simultaneous high selectivity and activity for H2O2 synthesis.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-15782-z
    DOI: 10.1038/s41467-020-15782-z
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    Cited by:

    1. 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.
    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. 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.
    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. 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.
    6. 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.
    7. 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.
    8. 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.
    9. 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.

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