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Title: Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy

Abstract

Development of platinum group metal (PGM)-free catalysts for oxygen reduction reaction (ORR) is essential for affordable proton exchange membrane fuel cells. Herein, a new type of atomically dispersed Co doped carbon catalyst with a core–shell structure has been developed via a surfactant-assisted metal–organic framework approach. The cohesive interactions between the selected surfactant and the Co-doped zeolitic imidazolate framework (ZIF-8) nanocrystals lead to a unique confinement effect. During the thermal activation, this confinement effect suppressed the agglomeration of Co atomic sites and mitigated the collapse of internal microporous structures of ZIF-8. Among the studied surfactants, Pluronic F127 block copolymer led to the greatest performance gains with a doubling of the active site density relative to that of the surfactant-free catalyst. According to density functional theory calculations, unlike other Co catalysts, this new atomically dispersed Co–N–C@F127 catalyst is believed to contain substantial CoN2+2 sites, which are active and thermodynamically favorable for the four-electron ORR pathway. The Co–N–C@F127 catalyst exhibits an unprecedented ORR activity with a half-wave potential (E1/2) of 0.84 V (vs. RHE) as well as enhanced stability in the corrosive acidic media. It also demonstrated high initial performance with a power density of 0.87 W cm–2 along with encouraging durability inmore » H2–O2 fuel cells. The atomically dispersed Co site catalyst approaches that of the Fe–N–C catalyst and represents the highest reported PGM-free and Fe-free catalyst performance.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [4];  [5]; ORCiD logo [6];  [7];  [7];  [1];  [1];  [7];  [3];  [3];  [5];  [4]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. at Buffalo, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  5. Univ. of Pittsburgh, PA (United States)
  6. Univ. of South Carolina, Columbia, SC (United States)
  7. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Univ. at Buffalo, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Carnegie Mellon Univ., Pittsburgh, PA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1897112
Alternate Identifier(s):
OSTI ID: 1480361; OSTI ID: 1480958; OSTI ID: 1502561
Report Number(s):
BNL-209357-2018-JAAM
Journal ID: ISSN 1754-5692
Grant/Contract Number:  
EE0008076; AC05-00OR22725; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE

Citation Formats

He, Yanghua, Hwang, Sooyeon, Cullen, David A., Uddin, M. Aman, Langhorst, Lisa, Li, Boyang, Karakalos, Stavros, Kropf, A. Jeremy, Wegener, Evan C., Sokolowski, Joshua, Chen, Mengjie, Myers, Debbie, Su, Dong, More, Karren L., Wang, Guofeng, Litster, Shawn, and Wu, Gang. Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy. United States: N. p., 2018. Web. doi:10.1039/c8ee02694g.
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He, Yanghua, Hwang, Sooyeon, Cullen, David A., Uddin, M. Aman, Langhorst, Lisa, Li, Boyang, Karakalos, Stavros, Kropf, A. Jeremy, Wegener, Evan C., Sokolowski, Joshua, Chen, Mengjie, Myers, Debbie, Su, Dong, More, Karren L., Wang, Guofeng, Litster, Shawn, & Wu, Gang. Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy. United States. https://doi.org/10.1039/c8ee02694g
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He, Yanghua, Hwang, Sooyeon, Cullen, David A., Uddin, M. Aman, Langhorst, Lisa, Li, Boyang, Karakalos, Stavros, Kropf, A. Jeremy, Wegener, Evan C., Sokolowski, Joshua, Chen, Mengjie, Myers, Debbie, Su, Dong, More, Karren L., Wang, Guofeng, Litster, Shawn, and Wu, Gang. Tue . "Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy". United States. https://doi.org/10.1039/c8ee02694g. https://www.osti.gov/servlets/purl/1897112.
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@article{osti_1897112,
title = {Highly active atomically dispersed CoN4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy},
author = {He, Yanghua and Hwang, Sooyeon and Cullen, David A. and Uddin, M. Aman and Langhorst, Lisa and Li, Boyang and Karakalos, Stavros and Kropf, A. Jeremy and Wegener, Evan C. and Sokolowski, Joshua and Chen, Mengjie and Myers, Debbie and Su, Dong and More, Karren L. and Wang, Guofeng and Litster, Shawn and Wu, Gang},
abstractNote = {Development of platinum group metal (PGM)-free catalysts for oxygen reduction reaction (ORR) is essential for affordable proton exchange membrane fuel cells. Herein, a new type of atomically dispersed Co doped carbon catalyst with a core–shell structure has been developed via a surfactant-assisted metal–organic framework approach. The cohesive interactions between the selected surfactant and the Co-doped zeolitic imidazolate framework (ZIF-8) nanocrystals lead to a unique confinement effect. During the thermal activation, this confinement effect suppressed the agglomeration of Co atomic sites and mitigated the collapse of internal microporous structures of ZIF-8. Among the studied surfactants, Pluronic F127 block copolymer led to the greatest performance gains with a doubling of the active site density relative to that of the surfactant-free catalyst. According to density functional theory calculations, unlike other Co catalysts, this new atomically dispersed Co–N–C@F127 catalyst is believed to contain substantial CoN2+2 sites, which are active and thermodynamically favorable for the four-electron ORR pathway. The Co–N–C@F127 catalyst exhibits an unprecedented ORR activity with a half-wave potential (E1/2) of 0.84 V (vs. RHE) as well as enhanced stability in the corrosive acidic media. It also demonstrated high initial performance with a power density of 0.87 W cm–2 along with encouraging durability in H2–O2 fuel cells. The atomically dispersed Co site catalyst approaches that of the Fe–N–C catalyst and represents the highest reported PGM-free and Fe-free catalyst performance.},
doi = {10.1039/c8ee02694g},
journal = {Energy & Environmental Science},
number = 1,
volume = 12,
place = {United States},
year = {Tue Oct 23 00:00:00 EDT 2018},
month = {Tue Oct 23 00:00:00 EDT 2018}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/c8ee02694g
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Figures / Tables:

Figure 1 Figure 1: (a) Proposed in-situ confinement pyrolysis strategy to synthesize core-shell-structured Co-N-C@surfactants catalysts with increased active site density (The yellow, grey and blue balls represent Co, Zn and N atoms, respectively). (b) SEM images to show the changes in the size and morphology of the catalysts with varying surfactants includingmore » SDS, CTAB, F127 and PVP.« less
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