Single-Iron Site Catalysts with Self-Assembled Dual-size Architecture and Hierarchical Porosity for Proton-Exchange Membrane Fuel Cells

Zhao, Xiaolin; Yang, Xiaoxuan; Wang, Maoyu; Hwang, Sooyeon; Karakalos, Stavros; Chen, Mengjie; Qiao, Zhi; Wang, Lei; Liu, Bin; Ma, Qing; Cullen, David A.; Su, Dong; Yang, Haipeng; Zang, Hong-Ying; Feng, Zhenxing; Wu, Gang

doi:10.1016/j.apcatb.2020.119400

Title: Single-Iron Site Catalysts with Self-Assembled Dual-size Architecture and Hierarchical Porosity for Proton-Exchange Membrane Fuel Cells

Journal Article · 05 August 2020 · Applied Catalysis B: Environmental

DOI: https://doi.org/10.1016/j.apcatb.2020.119400 · OSTI ID:1649998

Zhao, Xiaolin ^[1]; Yang, Xiaoxuan ^[2]; Wang, Maoyu ^[3];

^[4]; Karakalos, Stavros ^[5]; Chen, Mengjie ^[2]; Qiao, Zhi ^[2]; Wang, Lei ^[6]; Liu, Bin ^[6]; Ma, Qing ^[7]; Cullen, David A. ^[8]; Su, Dong ^[4]; Yang, Haipeng ^[6]; Zang, Hong-Ying ^[9]; Feng, Zhenxing ^[3]; Wu, Gang ^[2]

Shenzhen Univ. (China); Univ. at Buffalo, NY (United States); State Univ. of New York (SUNY), Buffalo, NY (United States)
Univ. at Buffalo, NY (United States); State Univ. of New York (SUNY), Buffalo, NY (United States)
Oregon State Univ., Corvallis, OR (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. of South Carolina, Columbia, SC (United States)
Shenzhen Univ. (China)
Northwestern Univ., Evanston, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Northeast Normal Univ., Changchun (China)

Atomically dispersed and nitrogen coordinated single iron site (i.e., FeN₄) catalysts (Fe-N-C) are the most promising platinum group metal (PGM)-free cathode for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells (PEMFCs). However, current Fe-N-C catalysts are limited by the inferior exposure of active FeN4 sites due to the inevitable agglomeration of particles in cathodes. In this paper, we report a self-assembled strategy to synthesize the atomically dispersed FeN₄ site catalysts with a hierarchically porous matrix derived from dual-size Fe-doped ZIF-8 crystal precursors. The tailored structure is effective in mitigating the particle migration, agglomeration, and spatial overlap, thereby exposing increased accessible active sites and facilitating mass transport. The best performing catalyst composed of 100 nm "nucleated seed" assembled by 30 nm "satellite" demonstrates exceptional ORR activity in acidic electrolyte and membrane electrode assembly. This work provides new concepts for designing hierarchically porous catalysts with single metal atom dispersion via self-assembly of ZIF-8 crystal precursors with tunable particle size and nanostructures.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); State Univ. of New York (SUNY); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Univ. at Buffalo

Grant/Contract Number:: AC02-06CH11357; AC05-00OR22725; EE0008076; SC0012704

OSTI ID:: 1649998

Report Number(s):: BNL-216285-2020-JAAM

Journal Information:: Applied Catalysis B: Environmental, Journal Name: Applied Catalysis B: Environmental Vol. 279; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Single-Iron Site Catalysts with Self-Assembled Dual-size Architecture and Hierarchical Porosity for Proton-Exchange Membrane Fuel Cells

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