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Mass production of high-performance single atomic FeNC electrocatalysts via sequenced ultrasonic atomization and pyrolysis process

通过顺序超声雾化和热解法规模化制备高效单原子铁氮碳电催化剂

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Abstract

Mass production of highly efficient, durable, and inexpensive single atomic catalysts is currently the major challenge associated with the oxygen reduction reaction (ORR) for fuel cells. In this study, we develop a general strategy that uses a simple ultrasonic atomization coupling with pyrolysis and calcination process to synthesize single atomic FeNC catalysts (FeNC SACs) at large scale. The microstructure characterizations confirm that the active centers root in the single atomic Fe sites chelating to the four-fold pyridinic N atoms. The identified specific Fe active sites with the variable valence states facilitate the transfer of electrons, endowing the FeNC SACs with excellent electrochemical ORR activity. The FeNC SACs were used as cathode catalysts in a homemade Zn-air battery, giving an open-circuit voltage (OCV) of 1.43 V, which is substantially higher than that of commercial Pt/C catalysts. This study provides a simple approach to the synthesis of single atomic catalysts at large scale.

摘要

燃料电池中氧还原反应(ORR)目前面临的主要挑战是如何 大规模生产高效、耐用、廉价的单原子催化剂. 针对这个问题, 我 们开发了一种通用的策略, 即利用简单的超声雾化耦合热解和煅 烧过程来大规模合成单原子FeNC催化剂(FeNC SACs). 通过微观 结构表征发现, 活性中心位于与四吡啶N原子螯合的单原子Fe位 点. 具有特定可识别的、不同价态的Fe活性位点促进了电子的转 移, 使FeNC SACs具有良好的电化学ORR活性. FeNC SACs被用作 自制的锌空气电池阴极催化剂时, 其开路电压为1.43 V, 远高于商 业Pt/C催化剂. 本研究为大规模合成单原子催化剂提供了一种简单 有效的方法.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (NSFC, 51971029), the NSFC-BRICS STI Framework Program (51861145309), the National S&T Major Project (2018ZX10301201), the Joint Research Project of University of Science and Technology Beijing & Taipei University of Technology (TW2018007), the “1125” Zhihui Zhengzhou Talent Project of Henan Province (39080070), the Fundamental Research Funds for the Central Universities (FRF-BR-15-027A). Yujun Song also appreciates the fund supports from the “100 talent plan” fund of Fujian province (Contract No: 2017-802). This research used 9-BM beamline at the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. Yujun Song appreciates Dr. Zhang from ZKKF (Beijing) Science & Technology Co., Ltd., for the HAADF-STEM characterization.

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Authors and Affiliations

  1. Center for Modern Physics Technology, School of Mathematics and Physics, University of Science and Technology Beijing, Beijing, 100083, China

    Jugang Ma  (马炬刚), Weiwei Zhang  (张伟伟) & Yujun Song  (宋玉军)

  2. X-ray Science Division, Argonne National Laboratory, 9700 S Cass Ave., Lemont, IL, 60439, USA

    Liguang Wang  (王利光) & Tianpin Wu  (吴天品)

  3. Tianjin Key Laboratory of Composite and Functional Materials, Tianjin University, Tianjin, 300072, China

    Yida Deng  (邓意达)

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  1. Jugang Ma  (马炬刚)
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  6. Yujun Song  (宋玉军)
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Contributions

Song Y designed the project, engineered the SAC samples, and discussed with Deng Y. Song Y and Wu T designed the experiment of the XAS characterization of SACs. Ma J performed the catalyst preparation and the characterization of the related microstructure and catalytic performance. Wu T and Wang L conducted the EXAFS and XANES experiments. Ma J and Wang L wrote the paper, revised by Song Y, Deng Y and Zhang W. All authors took part in the data analysis.

Corresponding authors

Correspondence to Tianpin Wu  (吴天品) or Yujun Song  (宋玉军).

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Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary information

Experimental details and supporting data are available in the online version of the paper

Jugang Ma is currently a PhD student at the University of Science and Technology Beijing (USTB) under the direction of Prof. Yujun Song. His main research interests are focused on electrocatalyst synthesis and the related application in fuel cells.

Yujun Song has been a full Professor in physics and applied physics at the USTB, Deputy director of the Center for Modern Physics Research since 2014. His research interests are currently focused on micro/nano-material-mediated integration innovation of modern physics with biomedical engineering, new energy and catalysis, and information science and technology.

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Mass production of high-performance single atomic FeNC electrocatalysts via sequenced ultrasonic atomization and pyrolysis process

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Ma, J., Wang, L., Deng, Y. et al. Mass production of high-performance single atomic FeNC electrocatalysts via sequenced ultrasonic atomization and pyrolysis process. Sci. China Mater. 64, 631–641 (2021). https://doi.org/10.1007/s40843-020-1464-6

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