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Unveiling the dynamic active site of defective carbon-based electrocatalysts for hydrogen peroxide production

Author

Listed:
  • Qilong Wu

    (Jilin University
    University of Wollongong, Squires Way
    Griffith University, Nathan Campus)

  • Haiyuan Zou

    (Southern University of Science and Technology)

  • Xin Mao

    (Queensland University of Technology, Gardens Point Campus)

  • Jinghan He

    (Jilin University)

  • Yanmei Shi

    (Tianjin University)

  • Shuangming Chen

    (University of Science and Technology of China)

  • Xuecheng Yan

    (Griffith University, Nathan Campus)

  • Liyun Wu

    (Jilin University)

  • Chengguang Lang

    (Griffith University, Nathan Campus
    Sun Yat-Sen University (Shenzhen))

  • Bin Zhang

    (Tianjin University)

  • Li Song

    (University of Science and Technology of China)

  • Xin Wang

    (Zhejiang University of Technology
    Moganshan Institute ZJUT, Kangqian District)

  • Aijun Du

    (Queensland University of Technology, Gardens Point Campus)

  • Qin Li

    (Griffith University, Nathan Campus)

  • Yi Jia

    (Zhejiang University of Technology
    Moganshan Institute ZJUT, Kangqian District)

  • Jun Chen

    (University of Wollongong, Squires Way)

  • Xiangdong Yao

    (Jilin University
    Sun Yat-Sen University (Shenzhen))

Abstract

Active sites identification in metal-free carbon materials is crucial for developing practical electrocatalysts, but resolving precise configuration of active site remains a challenge because of the elusive dynamic structural evolution process during reactions. Here, we reveal the dynamic active site identification process of oxygen modified defective graphene. First, the defect density and types of oxygen groups were precisely manipulated on graphene, combined with electrocatalytic performance evaluation, revealing a previously overlooked positive correlation relationship between the defect density and the 2 e- oxygen reduction performance. An electrocatalytic-driven oxygen groups redistribution phenomenon was observed, which narrows the scope of potential configurations of the active site. The dynamic evolution processes are monitored via multiple in-situ technologies and theoretical spectra simulations, resolving the configuration of major active sites (carbonyl on pentagon defect) and key intermediates (*OOH), in-depth understanding the catalytic mechanism and providing a research paradigm for metal-free carbon materials.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41947-7
    DOI: 10.1038/s41467-023-41947-7
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    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. Hui Li & Peng Wen & Dominique S. Itanze & Zachary D. Hood & Shiba Adhikari & Chang Lu & Xiao Ma & Chaochao Dun & Lin Jiang & David L. Carroll & Yejun Qiu & Scott M. Geyer, 2020. "Scalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
    4. Qihao Yang & Wenwen Xu & Shun Gong & Guokui Zheng & Ziqi Tian & Yujie Wen & Luming Peng & Linjuan Zhang & Zhiyi Lu & Liang Chen, 2020. "Atomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
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    Cited by:

    1. Yingzhang Shi & Peng Li & Huiling Chen & Zhiwen Wang & Yujie Song & Yu Tang & Sen Lin & Zhiyang Yu & Ling Wu & Jimmy C. Yu & Xianzhi Fu, 2024. "Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Zhiqiang Zheng & Lu Qi & Xiaoyu Luan & Shuya Zhao & Yurui Xue & Yuliang Li, 2024. "Growing highly ordered Pt and Mn bimetallic single atomic layers over graphdiyne," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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