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Title: Porous Carbon-Hosted Atomically Dispersed Iron-Nitrogen Moiety as Enhanced Electrocatalysts for Oxygen Reduction Reaction in a Wide Range of pH

Abstract

As one of the alternatives to replace precious metal catalysts, transition metal-nitrogen-carbon (M-N-C) electrocatalysts have attracted great research interest due to their low cost and good catalytic activities. Despite nanostructured M-N-C catalysts can achieve good electrochemical performances, they are vulnerable to aggregation and insufficient catalytic sites upon continuous catalytic reaction. Thus, M-N-C’s stability and selectivity have not been comparable to their noble metal counterparts. In this work, metal-organic frameworks (MOFs)-derived porous single-atom electrocatalysts (SAEs) were successfully prepared by simple pyrolysis procedure without any further post-treatment. Combining the X-ray absorption near-edge spectroscopy (XANES) and electrochemical measurements, the SAEs have been identified with superior ORR activity and stability compared with Pt/C catalysts in alkaline condition. More impressively, the SAEs also show excellent ORR electrocatalytic performance in both acid and neutral media. Furthermore, this study of nonprecious catalysts provides new insights on nano-engineering catalytically active sites and porous structures for nonprecious metal ORR catalysis in a wide range of pH.

Authors:
 [1];  [2]; ORCiD logo [3];  [1];  [3];  [1];  [4];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Washington State Univ., Pullman, WA (United States)
  2. Washington State Univ., Pullman, WA (United States); College of Chemistry Central China Normal Univ., Wuhan (People's Republic of China)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1438319
Alternate Identifier(s):
OSTI ID: 1420179
Report Number(s):
BNL-205679-2018-JAAM
Journal ID: ISSN 1613-6810
Grant/Contract Number:  
SC0012704; DE‐AC05‐76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Volume: 14; Journal Issue: 12; Journal ID: ISSN 1613-6810
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY AND ECONOMY; Metal organic frameworks; nonprecious metal nanocatalysts; single-atom catalysts; Fe-N-C electrocatalysts; oxygen reduction reaction

Citation Formats

Fu, Shaofang, Zhu, Chengzhou, Su, Dong, Song, Junhua, Yao, Siyu, Feng, Shuo, Engelhard, Mark H., Du, Dan, and Lin, Yuehe. Porous Carbon-Hosted Atomically Dispersed Iron-Nitrogen Moiety as Enhanced Electrocatalysts for Oxygen Reduction Reaction in a Wide Range of pH. United States: N. p., 2018. Web. doi:10.1002/smll.201703118.
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Fu, Shaofang, Zhu, Chengzhou, Su, Dong, Song, Junhua, Yao, Siyu, Feng, Shuo, Engelhard, Mark H., Du, Dan, & Lin, Yuehe. Porous Carbon-Hosted Atomically Dispersed Iron-Nitrogen Moiety as Enhanced Electrocatalysts for Oxygen Reduction Reaction in a Wide Range of pH. United States. https://doi.org/10.1002/smll.201703118
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Fu, Shaofang, Zhu, Chengzhou, Su, Dong, Song, Junhua, Yao, Siyu, Feng, Shuo, Engelhard, Mark H., Du, Dan, and Lin, Yuehe. Mon . "Porous Carbon-Hosted Atomically Dispersed Iron-Nitrogen Moiety as Enhanced Electrocatalysts for Oxygen Reduction Reaction in a Wide Range of pH". United States. https://doi.org/10.1002/smll.201703118. https://www.osti.gov/servlets/purl/1438319.
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@article{osti_1438319,
title = {Porous Carbon-Hosted Atomically Dispersed Iron-Nitrogen Moiety as Enhanced Electrocatalysts for Oxygen Reduction Reaction in a Wide Range of pH},
author = {Fu, Shaofang and Zhu, Chengzhou and Su, Dong and Song, Junhua and Yao, Siyu and Feng, Shuo and Engelhard, Mark H. and Du, Dan and Lin, Yuehe},
abstractNote = {As one of the alternatives to replace precious metal catalysts, transition metal-nitrogen-carbon (M-N-C) electrocatalysts have attracted great research interest due to their low cost and good catalytic activities. Despite nanostructured M-N-C catalysts can achieve good electrochemical performances, they are vulnerable to aggregation and insufficient catalytic sites upon continuous catalytic reaction. Thus, M-N-C’s stability and selectivity have not been comparable to their noble metal counterparts. In this work, metal-organic frameworks (MOFs)-derived porous single-atom electrocatalysts (SAEs) were successfully prepared by simple pyrolysis procedure without any further post-treatment. Combining the X-ray absorption near-edge spectroscopy (XANES) and electrochemical measurements, the SAEs have been identified with superior ORR activity and stability compared with Pt/C catalysts in alkaline condition. More impressively, the SAEs also show excellent ORR electrocatalytic performance in both acid and neutral media. Furthermore, this study of nonprecious catalysts provides new insights on nano-engineering catalytically active sites and porous structures for nonprecious metal ORR catalysis in a wide range of pH.},
doi = {10.1002/smll.201703118},
journal = {Small},
number = 12,
volume = 14,
place = {United States},
year = {Mon Feb 12 00:00:00 EST 2018},
month = {Mon Feb 12 00:00:00 EST 2018}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1002/smll.201703118
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Citation Metrics:
Cited by: 109 works
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Figures / Tables:

Figure 1 Figure 1: (A) Schematic synthesis of MOF-derived Fe-N-C SAEs. TEM (B), HAADF-STEM (C, F) images of Fe50-N-C-900 SAEs. (D) EELS spectrum of Fe50-N-C-900 SAEs. (E) Elemental distribution of C, N, O, and Zn in Fe50-N-C-900 SAEs.
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    Carbon-Supported Single Atom Catalysts for Electrochemical Energy Conversion and Storage
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    Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application
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    Densely Populated Single Atom Catalysts
    journal, November 2019

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