Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells
Abstract
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.
- Authors:
-
[3];
[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)
- Publication Date:
- Research Org.:
- 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 Org.:
- 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)
- OSTI Identifier:
- 1706606
- Alternate Identifier(s):
- OSTI ID: 1772633; OSTI ID: 1788373; OSTI ID: 1804193; OSTI ID: 1897113
- Report Number(s):
- BNL-220579-2020-JAAM
Journal ID: ISSN 0935-9648
- Grant/Contract Number:
- SC0012704; EE0008076; AC02-06CH11357; CBET-1604392; CBET-1804326; 1832963; ACI-1053575; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Materials
- Additional Journal Information:
- Journal Volume: 32; Journal Issue: 46; Journal ID: ISSN 0935-9648
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; electrocatalysis; electrospinning; fuel cells; oxygen reduction; single Co sites
Citation Formats
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, and Wu, Gang. Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells. United States: N. p., 2020.
Web. doi:10.1002/adma.202003577.
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. Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells. United States. https://doi.org/10.1002/adma.202003577
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, and Wu, Gang. Thu .
"Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells". United States. https://doi.org/10.1002/adma.202003577. https://www.osti.gov/servlets/purl/1706606.
@article{osti_1706606,
title = {Single Cobalt Sites Dispersed in Hierarchically Porous Nanofiber Networks for Durable and High-Power PGM-Free Cathodes in Fuel Cells},
author = {He, Yanghua and Guo, Hui and Hwang, Sooyeon and Yang, Xiaoxuan and He, Zizhou and Braaten, Jonathan and Karakalos, Stavros and Shan, Weitao and Wang, Maoyu and Zhou, Hua and Feng, Zhenxing and More, Karren L. and Wang, Guofeng and Su, Dong and Cullen, David A. and Fei, Ling and Litster, Shawn and Wu, Gang},
abstractNote = {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.},
doi = {10.1002/adma.202003577},
journal = {Advanced Materials},
number = 46,
volume = 32,
place = {United States},
year = {Thu Oct 15 00:00:00 EDT 2020},
month = {Thu Oct 15 00:00:00 EDT 2020}
}
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