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Title: Tailoring FeN 4 Sites with Edge Enrichment for Boosted Oxygen Reduction Performance in Proton Exchange Membrane Fuel Cell

Abstract

Transition metal atoms with corresponding nitrogen-coordination (MNx moieties) are widely proposed as catalytic centers for the oxygen reduction reaction (ORR) in metal-nitrogen-carbon (M-N-C) catalysts. Here, an effective strategy that can tailor Fe-N-C catalysts to simultaneously enrich the number of active sites while boost their intrinsic activity and utilization is reported. This is achieved by edge engineering of FeN4 sites via a simple ammonium chloride salt-assisted approach, where a high fraction of FeN4 sites are preferentially generated and hosted in a graphene-like porous scaffold. Theoretical calculations demonstrate that the FeN4 moieties with adjacent pore defects are likely to be more active than the non-defective configuration. Coupled with the facilitated accessibility of active sites, this prepared catalyst when applied in a practical H2-air proton exchange membrane fuel cell delivers a remarkable peak power density of 0.43 W cm-2, ranking it as one of the most active M-N-C catalysts reported to date. This work presents a new avenue for boosting ORR activity by edge manipulation of FeN4 sites.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [3];  [3];  [3]; ORCiD logo [2];  [3];  [4];  [4];  [3];  [3]; ORCiD logo [3]
  1. Henan Normal Univ., Xinxiang (China). Key Lab. of Green Chemical Media and Reaction; Univ. of Waterloo, ON (Canada)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  3. Univ. of Waterloo, ON (Canada)
  4. Henan Normal Univ., Xinxiang (China). Key Lab. of Green Chemical Media and Reaction
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1507104
Alternate Identifier(s):
OSTI ID: 1492460
Report Number(s):
BNL-211552-2019-JAAM
Journal ID: ISSN 1614-6832
Grant/Contract Number:  
SC0012704; DE‐SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 11; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY AND ECONOMY; M-N-C catalysts; FeN4 sites; oxygen reduction reaction; edge engineering; fuel cells

Citation Formats

Fu, Xiaogang, Li, Na, Ren, Bohua, Jiang, Gaopeng, Liu, Yanru, Hassan, Fathy M., Su, Dong, Zhu, Jianbing, Yang, Lin, Bai, Zhengyu, Cano, Zachary P., Yu, Aiping, and Chen, Zhongwei. Tailoring FeN 4 Sites with Edge Enrichment for Boosted Oxygen Reduction Performance in Proton Exchange Membrane Fuel Cell. United States: N. p., 2019. Web. doi:10.1002/aenm.201803737.
Fu, Xiaogang, Li, Na, Ren, Bohua, Jiang, Gaopeng, Liu, Yanru, Hassan, Fathy M., Su, Dong, Zhu, Jianbing, Yang, Lin, Bai, Zhengyu, Cano, Zachary P., Yu, Aiping, & Chen, Zhongwei. Tailoring FeN 4 Sites with Edge Enrichment for Boosted Oxygen Reduction Performance in Proton Exchange Membrane Fuel Cell. United States. doi:10.1002/aenm.201803737.
Fu, Xiaogang, Li, Na, Ren, Bohua, Jiang, Gaopeng, Liu, Yanru, Hassan, Fathy M., Su, Dong, Zhu, Jianbing, Yang, Lin, Bai, Zhengyu, Cano, Zachary P., Yu, Aiping, and Chen, Zhongwei. Mon . "Tailoring FeN 4 Sites with Edge Enrichment for Boosted Oxygen Reduction Performance in Proton Exchange Membrane Fuel Cell". United States. doi:10.1002/aenm.201803737. https://www.osti.gov/servlets/purl/1507104.
@article{osti_1507104,
title = {Tailoring FeN 4 Sites with Edge Enrichment for Boosted Oxygen Reduction Performance in Proton Exchange Membrane Fuel Cell},
author = {Fu, Xiaogang and Li, Na and Ren, Bohua and Jiang, Gaopeng and Liu, Yanru and Hassan, Fathy M. and Su, Dong and Zhu, Jianbing and Yang, Lin and Bai, Zhengyu and Cano, Zachary P. and Yu, Aiping and Chen, Zhongwei},
abstractNote = {Transition metal atoms with corresponding nitrogen-coordination (MNx moieties) are widely proposed as catalytic centers for the oxygen reduction reaction (ORR) in metal-nitrogen-carbon (M-N-C) catalysts. Here, an effective strategy that can tailor Fe-N-C catalysts to simultaneously enrich the number of active sites while boost their intrinsic activity and utilization is reported. This is achieved by edge engineering of FeN4 sites via a simple ammonium chloride salt-assisted approach, where a high fraction of FeN4 sites are preferentially generated and hosted in a graphene-like porous scaffold. Theoretical calculations demonstrate that the FeN4 moieties with adjacent pore defects are likely to be more active than the non-defective configuration. Coupled with the facilitated accessibility of active sites, this prepared catalyst when applied in a practical H2-air proton exchange membrane fuel cell delivers a remarkable peak power density of 0.43 W cm-2, ranking it as one of the most active M-N-C catalysts reported to date. This work presents a new avenue for boosting ORR activity by edge manipulation of FeN4 sites.},
doi = {10.1002/aenm.201803737},
journal = {Advanced Energy Materials},
number = 11,
volume = 9,
place = {United States},
year = {2019},
month = {1}
}

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