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Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction

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Abstract

Recently, nitrogen-doped porous carbon supported single atom catalysts (SACs) have become one of the most promising alternatives to precious metal catalysts in oxygen reduction reaction (ORR) due to their outstanding performance, especially those derived from porphyrin-based materials. However, most of them involve other metal residuals, which would cause the tedious pre- and/or post-treatment, even mislead the mechanistic investigations and active-site identification. Herein, we report a precursor-dilution strategy to synthesize Fe SACs through the Schiff-based reaction via co-polycondensation of amino-metalloporphyrin, followed by pyrolysis at high temperature. Systematic characterization results provide the compelling evidence of the dominant presence of atomically dispersed Fe-Nx species. Our catalyst shows superior ORR performance with positive half-wave potential (E1/2=0.85 V vs. RHE) in alkaline condition and moderate activity (E1/2=0.68 V vs. RHE) under the acidic condition, excellent methanol tolerance and good long-term stability. All the results indicate Fe SACs would be a promising candidate for replacing the precious Pt in metal-air batteries and fuel cells.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (21938001, 21606260, 21576302, 21376278, 21425627, 21701199), the National Natural Science Foundation of China-SINOPEC Joint Fund (U1663220), the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01C102), the Natural Science Foundation of Guangdong Province (2015A030313104), the Fundamental Research Funds for the Central Universities of Sun Yatsen University (15lgjc33, 19lgpy129).

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Fine Chemical Industry Research Institute, School of Chemistry, Sun Yat-sen University, Guangzhou, 510275, China

    Qian He, Qingdi Sun, Tao Gan, Xiaohui He & Hongbing Ji

  2. Institute of Advanced Wear & Corrosion Resistant and Functional Materials, Jinan University, Guangzhou, 510632, China

    Yuying Meng

  3. Fine Chemical Industry Research Institute, School of Chemical Engineering and Technology, Sun Yat-sen University, Zhuhai, 519082, China

    Hao Zhang, Ying Zhang & Huajian Xiao

  4. School of Chemical Engineering, Guangdong University of Petrochemical Technology, Maoming, 525000, China

    Hongbing Ji

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  1. Qian He
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Correspondence to Xiaohui He or Hongbing Ji.

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The supporting information is available online at http://chem.scichina.com and http://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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He, Q., Meng, Y., Zhang, H. et al. Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction. Sci. China Chem. 63, 810–817 (2020). https://doi.org/10.1007/s11426-019-9703-7

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