Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells

He, Yanghua; Guo, Hui; Hwang, Sooyeon; Yang, Xiaoxuan; He, Zizhou; Braaten, Jonathan; Karakalos, Stavros; Shan, Weitao; Wang, Maoyu; Zhou, Hua; Feng, Zhenxing; More, Karren L.; Wang, Guofeng; Su, Dong; Cullen, David A.; Fei, Ling; Litster, Shawn; Wu, Gang

doi:10.1002/adma.202003577

Title: Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells

Journal Article · Thu Oct 15 00:00:00 EDT 2020 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202003577· OSTI ID:1706606

He, Yanghua ^[1]; Guo, Hui ^[2];

^[3]; Yang, Xiaoxuan ^[1]; He, Zizhou ^[2]; Braaten, Jonathan ^[4]; Karakalos, Stavros ^[5]; Shan, Weitao ^[6]; Wang, Maoyu ^[7]; Zhou, Hua ^[8]; Feng, Zhenxing ^[7]; More, Karren L. ^[9]; Wang, Guofeng ^[6]; Su, Dong ^[3]; Cullen, David A. ^[9]; Fei, Ling ^[2]; Litster, Shawn ^[4];

^[1]

Univ. at Buffalo, NY (United States)
Univ. of Louisiana, Lafayette, LA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Carnegie Mellon Univ., Pittsburgh, PA (United States)
Univ. of South Carolina, Columbia, SC (United States)
Univ. of Pittsburgh, PA (United States)
Oregon State Univ., Corvallis, OR (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Increasing catalytic activity and durability of atomically dispersed metal–nitrogen–carbon (M–N–C) catalysts for the oxygen reduction reaction (ORR) cathode in proton-exchange-membrane fuel cells remains a grand challenge. Here, a high-power and durable Co–N–C nanofiber catalyst synthesized through electrospinning cobalt-doped zeolitic imidazolate frameworks into selected polyacrylonitrile and poly(vinylpyrrolidone) polymers is reported. The distinct porous fibrous morphology and hierarchical structures play a vital role in boosting electrode performance by exposing more accessible active sites, providing facile electron conductivity, and facilitating the mass transport of reactant. The enhanced intrinsic activity is attributed to the extra graphitic N dopants surrounding the CoN4 moieties. The highly graphitized carbon matrix in the catalyst is beneficial for enhancing the carbon corrosion resistance, thereby promoting catalyst stability. The unique nanoscale X-ray computed tomography verifies the well-distributed ionomer coverage throughout the fibrous carbon network in the catalyst. The membrane electrode assembly achieves a power density of 0.40 W cm-2 in a practical H2/air cell (1.0 bar) and demonstrates significantly enhanced durability under accelerated stability tests. The combination of the intrinsic activity and stability of single Co sites, along with unique catalyst architecture, provide new insight into designing efficient PGM-free electrodes with improved performance and durability.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. at Buffalo, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; EE0008076; AC02-06CH11357; CBET-1604392; CBET-1804326; 1832963; ACI-1053575; AC05-00OR22725

OSTI ID:: 1706606

Alternate ID(s):: OSTI ID: 1772633; OSTI ID: 1788373; OSTI ID: 1804193; OSTI ID: 1897113

Report Number(s):: BNL-220579-2020-JAAM

Journal Information:: Advanced Materials, Vol. 32, Issue 46; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells

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