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Metal single-site catalyst design for electrocatalytic production of hydrogen peroxide at industrial-relevant currents

Author

Listed:
  • Peike Cao

    (Dalian University of Technology)

  • Xie Quan

    (Dalian University of Technology)

  • Xiaowa Nie

    (Dalian University of Technology)

  • Kun Zhao

    (North China Electric Power University)

  • Yanming Liu

    (Dalian University of Technology)

  • Shuo Chen

    (Dalian University of Technology)

  • Hongtao Yu

    (Dalian University of Technology)

  • Jingguang G. Chen

    (Columbia University)

Abstract

Direct hydrogen peroxide (H2O2) electrosynthesis via the two-electron oxygen reduction reaction is a sustainable alternative to the traditional energy-intensive anthraquinone technology. However, high-performance and scalable electrocatalysts with industrial-relevant production rates remain to be challenging, partially due to insufficient atomic level understanding in catalyst design. Here we utilize theoretical approaches to identify transition-metal single-site catalysts for two-electron oxygen reduction using the *OOH binding energy as a descriptor. The theoretical predictions are then used as guidance to synthesize the desired cobalt single-site catalyst with a O-modified Co-(pyrrolic N)4 configuration that can achieve industrial-relevant current densities up to 300 mA cm−2 with 96–100% Faradaic efficiencies for H2O2 production at a record rate of 11,527 mmol h−1 gcat−1. Here, we show the feasibility and versatility of metal single-site catalyst design using various commercial carbon and cobalt phthalocyanine as starting materials and the high applicability for H2O2 electrosynthesis in acidic, neutral and alkaline electrolytes.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-35839-z
    DOI: 10.1038/s41467-023-35839-z
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    References listed on IDEAS

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    1. Qiaowan Chang & Pu Zhang & Amir Hassan Bagherzadeh Mostaghimi & Xueru Zhao & Steven R. Denny & Ji Hoon Lee & Hongpeng Gao & Ying Zhang & Huolin L. Xin & Samira Siahrostami & Jingguang G. Chen & Zheng , 2020. "Promoting H2O2 production via 2-electron oxygen reduction by coordinating partially oxidized Pd with defect carbon," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Qingran Zhang & Xin Tan & Nicholas M. Bedford & Zhaojun Han & Lars Thomsen & Sean Smith & Rose Amal & Xunyu Lu, 2020. "Direct insights into the role of epoxy groups on cobalt sites for acidic H2O2 production," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    3. 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.
    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. Lei Fan & Xiaowan Bai & Chuan Xia & Xiao Zhang & Xunhua Zhao & Yang Xia & Zhen-Yu Wu & Yingying Lu & Yuanyue Liu & Haotian Wang, 2022. "CO2/carbonate-mediated electrochemical water oxidation to hydrogen peroxide," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    6. Yang Xia & Xunhua Zhao & Chuan Xia & Zhen-Yu Wu & Peng Zhu & Jung Yoon (Timothy) Kim & Xiaowan Bai & Guanhui Gao & Yongfeng Hu & Jun Zhong & Yuanyue Liu & Haotian Wang, 2021. "Highly active and selective oxygen reduction to H2O2 on boron-doped carbon for high production rates," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
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    Cited by:

    1. 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.
    2. Xiao Zhou & Yuan Min & Changming Zhao & Cai Chen & Ming-Kun Ke & Shi-Lin Xu & Jie-Jie Chen & Yuen Wu & Han-Qing Yu, 2024. "Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    3. 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.

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