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Title: Highly active atomically dispersed CoN 4 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 CoN 2+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 (E 1/2) 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 withmore » encouraging durability in H 2–O 2 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];  [8];  [5];  [4]; ORCiD logo [1]
  1. Department of Chemical and Biological Engineering; University at Buffalo; The State University of New York; Buffalo; USA
  2. Center for Functional Nanomaterials; Brookhaven National Laboratory; Upton; USA
  3. Materials Science and Technology Division; Oak Ridge National Laboratory; Oak Ridge; USA
  4. Department of Mechanical Engineering; Carnegie Mellon University; Pittsburgh; USA
  5. Department of Mechanical Engineering and Materials Science; University of Pittsburgh; Pittsburgh; USA
  6. Department of Chemical Engineering; University of South Carolina; Columbia; USA
  7. Chemical Sciences and Engineering Division; Argonne National Laboratory; Lemont; USA
  8. Center for Nanophase Materials Sciences; Oak Ridge National Laboratory; Oak Ridge; USA
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Brookhaven National Lab. (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:
1480958
Alternate Identifier(s):
OSTI ID: 1480361; OSTI ID: 1502561
Report Number(s):
BNL-209357-2018-JAAM
Journal ID: ISSN 1754-5692
Grant/Contract Number:  
AC05-00OR22725; SC0012704; EE0008076
Resource Type:
Journal Article: 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 CoN 4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy. United States: N. p., 2018. Web. doi:10.1039/C8EE02694G.
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 CoN 4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy. United States. doi:10.1039/C8EE02694G.
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 CoN 4 fuel cell cathode catalysts derived from surfactant-assisted MOFs: carbon-shell confinement strategy". United States. doi:10.1039/C8EE02694G. https://www.osti.gov/servlets/purl/1480958.
@article{osti_1480958,
title = {Highly active atomically dispersed CoN 4 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},
issn = {1754-5692},
number = 1,
volume = 12,
place = {United States},
year = {2018},
month = {10}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 82 works
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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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    journal, January 2019

    • Zhang, Ming; Luo, Rui; Wang, Chaohai
    • Journal of Materials Chemistry A, Vol. 7, Issue 20
    • DOI: 10.1039/c9ta02931a

    Metal organic framework-derived hollow cactus-like carbon sheets for oxygen reduction
    journal, January 2019

    • Zhang, Ming; Wang, Chaohai; Yan, Xin
    • Journal of Materials Chemistry A, Vol. 7, Issue 35
    • DOI: 10.1039/c9ta06609h

    Atomic-level active sites of efficient imidazolate framework-derived nickel catalysts for CO 2 reduction
    journal, January 2019

    • Pan, Fuping; Zhang, Hanguang; Liu, Zhenyu
    • Journal of Materials Chemistry A, Vol. 7, Issue 46
    • DOI: 10.1039/c9ta08862h

    Cobalt/zinc dual-sites coordinated with nitrogen in nanofibers enabling efficient and durable oxygen reduction reaction in acidic fuel cells
    journal, January 2020

    • Zang, Jian; Wang, Feiteng; Cheng, Qingqing
    • Journal of Materials Chemistry A, Vol. 8, Issue 7
    • DOI: 10.1039/c9ta12207a

    Atomically Dispersed Iron Cathode Catalysts Derived from Binary Ligand-Based Zeolitic Imidazolate Frameworks with Enhanced Stability for PEM Fuel Cells
    journal, January 2019

    • Zhang, Hanguang; Ding, Shuo; Hwang, Sooyeon
    • Journal of The Electrochemical Society, Vol. 166, Issue 7
    • DOI: 10.1149/2.0141907jes

    Experimental and Theoretical Trends of PGM-Free Electrocatalysts for the Oxygen Reduction Reaction with Different Transition Metals
    journal, January 2019

    • Martinez, Ulises; Holby, Edward F.; Babu, Siddharth Komini
    • Journal of The Electrochemical Society, Vol. 166, Issue 7
    • DOI: 10.1149/2.0201907jes

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.