3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media
Abstract
Current platinum group metal (PGM)-free carbon nanocomposite catalysts for the oxygen reduction reaction (ORR) in acidic electrolyte often suffer from rapid degradation associated with carbon corrosion due to the use of large amount of amorphoous carbon black supports. Here, we developed a new concept of using freestanding 3D hydrogel to design support-free Fe-N-C catalysts. A 3D polyaniline (PANI)-based hydrogel was used for preparing a new type of single atomic iron site-rich catalyst, which has exhibited exceptionally enhanced activity and stability compared to conventional Fe-N-C catalysts supported on amorphous carbon blacks. The achieved performance metric on the hydrogel PANI-Fe catalysts is one of the best ever reported PGM-free catalysts, reaching a half-wave potential up to 0.83 V vs. RHE and only leaving 30 mV gap with Pt/C catalysts (60 μgPt/cm2) in challenging acidic media. Remarkable ORR stability was accomplished as well on the same catalyst evidenced by using harsh potential cycling tests. The well dispersion of atomic iron into partially graphitized carbon, featured with dominance of micropores and porous network structures, is capable of accommodating increased number of active sites, strengthening local bonding among iron, nitrogen and carbon, and facilitating mass transfer. The 3D polymer hydrogel approach would be a newmore »
- Authors:
-
- State Univ. of New York (SUNY), Buffalo, NY (United States). Dept. of Chemical and Biological Engineering
- Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemical Engineering
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1377026
- Alternate Identifier(s):
- OSTI ID: 1549696
- Report Number(s):
- BNL-114186-2017-JA
Journal ID: ISSN 0926-3373; R&D Project: 16060; 16060; KC0403020
- Grant/Contract Number:
- SC00112704; SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis B: Environmental
- Additional Journal Information:
- Journal Volume: 219; Journal Issue: C; Journal ID: ISSN 0926-3373
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrocatalysis; polymer hydrogel; single atomic iron sites; oxygen reduction; acidic media; Center for Functional Nanomaterials
Citation Formats
Qiao, Zhi, Zhang, Hanguang, Karakalos, Stavros, Hwang, Sooyeon, Xue, Jing, Chen, Mengjie, Su, Dong, and Wu, Gang. 3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media. United States: N. p., 2017.
Web. doi:10.1016/j.apcatb.2017.08.008.
Qiao, Zhi, Zhang, Hanguang, Karakalos, Stavros, Hwang, Sooyeon, Xue, Jing, Chen, Mengjie, Su, Dong, & Wu, Gang. 3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media. United States. https://doi.org/10.1016/j.apcatb.2017.08.008
Qiao, Zhi, Zhang, Hanguang, Karakalos, Stavros, Hwang, Sooyeon, Xue, Jing, Chen, Mengjie, Su, Dong, and Wu, Gang. Thu .
"3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media". United States. https://doi.org/10.1016/j.apcatb.2017.08.008. https://www.osti.gov/servlets/purl/1377026.
@article{osti_1377026,
title = {3D polymer hydrogel for high-performance atomic iron-rich catalysts for oxygen reduction in acidic media},
author = {Qiao, Zhi and Zhang, Hanguang and Karakalos, Stavros and Hwang, Sooyeon and Xue, Jing and Chen, Mengjie and Su, Dong and Wu, Gang},
abstractNote = {Current platinum group metal (PGM)-free carbon nanocomposite catalysts for the oxygen reduction reaction (ORR) in acidic electrolyte often suffer from rapid degradation associated with carbon corrosion due to the use of large amount of amorphoous carbon black supports. Here, we developed a new concept of using freestanding 3D hydrogel to design support-free Fe-N-C catalysts. A 3D polyaniline (PANI)-based hydrogel was used for preparing a new type of single atomic iron site-rich catalyst, which has exhibited exceptionally enhanced activity and stability compared to conventional Fe-N-C catalysts supported on amorphous carbon blacks. The achieved performance metric on the hydrogel PANI-Fe catalysts is one of the best ever reported PGM-free catalysts, reaching a half-wave potential up to 0.83 V vs. RHE and only leaving 30 mV gap with Pt/C catalysts (60 μgPt/cm2) in challenging acidic media. Remarkable ORR stability was accomplished as well on the same catalyst evidenced by using harsh potential cycling tests. The well dispersion of atomic iron into partially graphitized carbon, featured with dominance of micropores and porous network structures, is capable of accommodating increased number of active sites, strengthening local bonding among iron, nitrogen and carbon, and facilitating mass transfer. The 3D polymer hydrogel approach would be a new pathway to advance PGM-free catalysts.},
doi = {10.1016/j.apcatb.2017.08.008},
journal = {Applied Catalysis B: Environmental},
number = C,
volume = 219,
place = {United States},
year = {Thu Aug 03 00:00:00 EDT 2017},
month = {Thu Aug 03 00:00:00 EDT 2017}
}
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