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A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction

Author

Listed:
  • Jiaqi Feng

    (Chinese Academy of Sciences
    University of Chinese Academy of Science)

  • Hongshuai Gao

    (Chinese Academy of Sciences)

  • Lirong Zheng

    (Chinese Academy of Sciences)

  • Zhipeng Chen

    (Dalian National Laboratory for Clean Energy
    Chinese Academy of Sciences)

  • Shaojuan Zeng

    (Chinese Academy of Sciences)

  • Chongyang Jiang

    (Chinese Academy of Sciences
    University of Chinese Academy of Science)

  • Haifeng Dong

    (Chinese Academy of Sciences)

  • Licheng Liu

    (Dalian National Laboratory for Clean Energy
    Chinese Academy of Sciences)

  • Suojiang Zhang

    (Chinese Academy of Sciences
    University of Chinese Academy of Science)

  • Xiangping Zhang

    (Chinese Academy of Sciences
    University of Chinese Academy of Science
    Dalian National Laboratory for Clean Energy)

Abstract

Developing effective catalysts based on earth abundant elements is critical for CO2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (jCO) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a jCO of 14.0 mA cm−2 at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher jCO of 29.7 mA cm−2 is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N3 site, which facilitates the formation of the key intermediate COOH* through a lowered free energy barrier.

Suggested Citation

  • Jiaqi Feng & Hongshuai Gao & Lirong Zheng & Zhipeng Chen & Shaojuan Zeng & Chongyang Jiang & Haifeng Dong & Licheng Liu & Suojiang Zhang & Xiangping Zhang, 2020. "A Mn-N3 single-atom catalyst embedded in graphitic carbon nitride for efficient CO2 electroreduction," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-18143-y
    DOI: 10.1038/s41467-020-18143-y
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    Cited by:

    1. Jiaqi Feng & Limin Wu & Xinning Song & Libing Zhang & Shunhan Jia & Xiaodong Ma & Xingxing Tan & Xinchen Kang & Qinggong Zhu & Xiaofu Sun & Buxing Han, 2024. "CO2 electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Jiqing Jiao & Qing Yuan & Meijie Tan & Xiaoqian Han & Mingbin Gao & Chao Zhang & Xuan Yang & Zhaolin Shi & Yanbin Ma & Hai Xiao & Jiangwei Zhang & Tongbu Lu, 2023. "Constructing asymmetric double-atomic sites for synergistic catalysis of electrochemical CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Yiyan Yin & Xiyang Ge & Jin Ouyang & Na Na, 2024. "Tumor-activated in situ synthesis of single-atom catalysts for O2-independent photodynamic therapy based on water-splitting," Nature Communications, Nature, vol. 15(1), pages 1-16, December.
    4. Ruiz-López, Estela & Gandara-Loe, Jesús & Baena-Moreno, Francisco & Reina, Tomas Ramirez & Odriozola, José Antonio, 2022. "Electrocatalytic CO2 conversion to C2 products: Catalysts design, market perspectives and techno-economic aspects," Renewable and Sustainable Energy Reviews, Elsevier, vol. 161(C).

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