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Title: Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts

Abstract

Single-atom catalysts (SACs) have sparked broad interest recently while the low metal loading poses a big challenge for further applications. Herein, a dual protection strategy has been developed to give high-content SACs by nanocasting SiO2 into porphyrinic metal–organic frameworks (MOFs). The pyrolysis of SiO2@MOF composite affords singleatom Fe implanted N-doped porous carbon (FeSA–N–C) with high Fe loading (3.46 wt%). The spatial isolation of Fe atoms centered in porphyrin linkers of MOF sets the first protective barrier to inhibit the Fe agglomeration during pyrolysis. The SiO2 in MOF provides additional protection by creating thermally stable FeN4/SiO2 interfaces. Thanks to the high-density FeSA sites, FeSA–N–C demonstrates excellent oxygen reduction performance in both alkaline and acidic medias. Meanwhile, FeSA–N–C also exhibits encouraging performance in proton exchange membrane fuel cell, demonstrating great potential for practical application. More far-reaching, this work grants a general synthetic methodology toward high-content SACs (such as FeSA, CoSA, NiSA). https://doi.org/10.1038/s41467-020-16715-6 OPEN 1

Authors:
 [1];  [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Science and Technology of China, Hefei (China)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. North China Electric Power Univ., Baoding(China)
  4. Beihang Univ. (China)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1632832
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Jiao, Long, Zhang, Rui, Wan, Gang, Yang, Weijie, Wan, Xin, Zhou, Hua, Shui, Jianglan, Yu, Shu-Hong, and Jiang, Hai-Long. Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts. United States: N. p., 2020. Web. https://doi.org/10.1038/s41467-020-16715-6.
Jiao, Long, Zhang, Rui, Wan, Gang, Yang, Weijie, Wan, Xin, Zhou, Hua, Shui, Jianglan, Yu, Shu-Hong, & Jiang, Hai-Long. Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts. United States. https://doi.org/10.1038/s41467-020-16715-6
Jiao, Long, Zhang, Rui, Wan, Gang, Yang, Weijie, Wan, Xin, Zhou, Hua, Shui, Jianglan, Yu, Shu-Hong, and Jiang, Hai-Long. Fri . "Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts". United States. https://doi.org/10.1038/s41467-020-16715-6. https://www.osti.gov/servlets/purl/1632832.
@article{osti_1632832,
title = {Nanocasting SiO2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts},
author = {Jiao, Long and Zhang, Rui and Wan, Gang and Yang, Weijie and Wan, Xin and Zhou, Hua and Shui, Jianglan and Yu, Shu-Hong and Jiang, Hai-Long},
abstractNote = {Single-atom catalysts (SACs) have sparked broad interest recently while the low metal loading poses a big challenge for further applications. Herein, a dual protection strategy has been developed to give high-content SACs by nanocasting SiO2 into porphyrinic metal–organic frameworks (MOFs). The pyrolysis of SiO2@MOF composite affords singleatom Fe implanted N-doped porous carbon (FeSA–N–C) with high Fe loading (3.46 wt%). The spatial isolation of Fe atoms centered in porphyrin linkers of MOF sets the first protective barrier to inhibit the Fe agglomeration during pyrolysis. The SiO2 in MOF provides additional protection by creating thermally stable FeN4/SiO2 interfaces. Thanks to the high-density FeSA sites, FeSA–N–C demonstrates excellent oxygen reduction performance in both alkaline and acidic medias. Meanwhile, FeSA–N–C also exhibits encouraging performance in proton exchange membrane fuel cell, demonstrating great potential for practical application. More far-reaching, this work grants a general synthetic methodology toward high-content SACs (such as FeSA, CoSA, NiSA). https://doi.org/10.1038/s41467-020-16715-6 OPEN 1},
doi = {10.1038/s41467-020-16715-6},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {2020},
month = {6}
}

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