@ARTICLE{Xiao20182824,
author={Xiao, M. and Zhu, J. and Ma, L. and Jin, Z. and Ge, J. and Deng, X. and Hou, Y. and He, Q. and Li, J. and Jia, Q. and Mukerjee, S. and Yang, R. and Jiang, Z. and Su, D. and Liu, C. and Xing, W.},
title={Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N4 Active Site Identification Revealed by X-ray Absorption Spectroscopy},
journal={ACS Catalysis},
year={2018},
volume={8},
number={4},
pages={2824-2832},
doi={10.1021/acscatal.8b00138},
note={cited By 130},
url={https://www.scopus.com/inward/record.uri?eid=2-s2.0-85045109552&doi=10.1021%2facscatal.8b00138&partnerID=40&md5=e34d94f78ed7b428d6de9a53701c1538},
abstract={Developing highly efficient, low-cost oxygen reduction catalysts, especially in acidic medium, is of significance toward fuel cell commercialization. Although pyrolyzed Fe-N-C catalysts have been regarded as alternatives to platinum-based catalytic materials, further improvement requires precise control of the Fe-Nx structure at the molecular level and a comprehensive understanding of catalytic site structure and the ORR mechanism on these materials. In this report, we present a microporous metal-organic-framework-confined strategy toward the preferable formation of single-atom dispersed catalysts. The onset potential for Fe-N-C is 0.92 V, comparable to that of Pt/C and outperforming most noble-metal-free catalysts ever reported. A high-spin Fe3+-N4 configuration is revealed by the 57Fe Mössbauer spectrum and X-ray absorption spectroscopy for Fe L-edge, which will convert to Fe2+-N4 at low potential. The in situ reduced Fe2+-N4 moiety from high-spin Ox-Fe3+-N4 contributes to most of the ORR activity due to its high turnover frequency (TOF) of ca. 1.71 e s-1 sites-1. © 2018 American Chemical Society.},
keywords={Atoms;  Catalyst activity;  Crystalline materials;  Electrocatalysts;  Electrolytic reduction;  Fuel cells;  Microporosity;  Organometallics;  Precious metals;  X ray absorption spectroscopy, Active site;  Catalytic materials;  Fuel cell commercialization;  Metal-free catalysts;  Microporous metal organic frameworks;  Oxygen reduction catalysts;  Oxygen reduction reaction;  Single atoms, Iron compounds},
document_type={Business Article},
source={Scopus},
}

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Although pyrolyzed Fe-N-C catalysts have been regarded as alternatives to platinum-based catalytic materials, further improvement requires precise control of the Fe-Nx structure at the molecular level and a comprehensive understanding of catalytic site structure and the ORR mechanism on these materials. In this report, we present a microporous metal-organic-framework-confined strategy toward the preferable formation of single-atom dispersed catalysts. The onset potential for Fe-N-C is 0.92 V, comparable to that of Pt/C and outperforming most noble-metal-free catalysts ever reported. A high-spin Fe3+-N4 configuration is revealed by the 57Fe Mössbauer spectrum and X-ray absorption spectroscopy for Fe L-edge, which will convert to Fe2+-N4 at low potential. The in situ reduced Fe2+-N4 moiety from high-spin Ox-Fe3+-N4 contributes to most of the ORR activity due to its high turnover frequency (TOF) of ca. 1.71 e s-1 sites-1. © 2018 American Chemical Society.","keywords":"Atoms; Catalyst activity; Crystalline materials; Electrocatalysts; Electrolytic reduction; Fuel cells; Microporosity; Organometallics; Precious metals; X ray absorption spectroscopy, Active site; Catalytic materials; Fuel cell commercialization; Metal-free catalysts; Microporous metal organic frameworks; Oxygen reduction catalysts; Oxygen reduction reaction; Single atoms, Iron compounds","document_type":"Business Article","source":"Scopus","bibtex":"@ARTICLE{Xiao20182824,\nauthor={Xiao, M. and Zhu, J. and Ma, L. and Jin, Z. and Ge, J. and Deng, X. and Hou, Y. and He, Q. and Li, J. and Jia, Q. and Mukerjee, S. and Yang, R. and Jiang, Z. and Su, D. and Liu, C. and Xing, W.},\ntitle={Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N4 Active Site Identification Revealed by X-ray Absorption Spectroscopy},\njournal={ACS Catalysis},\nyear={2018},\nvolume={8},\nnumber={4},\npages={2824-2832},\ndoi={10.1021/acscatal.8b00138},\nnote={cited By 130},\nurl={https://www.scopus.com/inward/record.uri?eid=2-s2.0-85045109552&doi=10.1021%2facscatal.8b00138&partnerID=40&md5=e34d94f78ed7b428d6de9a53701c1538},\nabstract={Developing highly efficient, low-cost oxygen reduction catalysts, especially in acidic medium, is of significance toward fuel cell commercialization. Although pyrolyzed Fe-N-C catalysts have been regarded as alternatives to platinum-based catalytic materials, further improvement requires precise control of the Fe-Nx structure at the molecular level and a comprehensive understanding of catalytic site structure and the ORR mechanism on these materials. In this report, we present a microporous metal-organic-framework-confined strategy toward the preferable formation of single-atom dispersed catalysts. The onset potential for Fe-N-C is 0.92 V, comparable to that of Pt/C and outperforming most noble-metal-free catalysts ever reported. A high-spin Fe3+-N4 configuration is revealed by the 57Fe Mössbauer spectrum and X-ray absorption spectroscopy for Fe L-edge, which will convert to Fe2+-N4 at low potential. 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