Single Atomic Iron Site Catalysts via Benign Aqueous Synthesis for Durability Improvement in Proton Exchange Membrane Fuel Cells

Chen, Mengjie; Cullen, David A.; Karakalos, Stavros; Lu, Xiner; Cui, Jiang; Kropf, A. Jeremy; Mistry, Hemma; He, Kai; Myers, Deborah J.; Wu, Gang

doi:10.1149/1945-7111/abf014

Title: Single Atomic Iron Site Catalysts via Benign Aqueous Synthesis for Durability Improvement in Proton Exchange Membrane Fuel Cells

Journal Article · Thu Apr 01 00:00:00 EDT 2021 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/abf014· OSTI ID:1797652

Chen, Mengjie ^[1]; Cullen, David A. ^[2];

^[3]; Lu, Xiner ^[4]; Cui, Jiang ^[4]; Kropf, A. Jeremy ^[5]; Mistry, Hemma ^[5];

^[4];

^[5];

^[1]

State Univ. of New York (SUNY), Buffalo, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of South Carolina, Columbia, SC (United States)
Clemson Univ., SC (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

Atomically-dispersed iron-nitrogen-carbon (Fe-N-C) catalysts have arisen as promising candidates for replacing the costly precious metal catalysts in fuel cells but still face some grand challenges, such as insufficient site density and durability. Herein, we report a self-assembly method in an aqueous solution to develop an atomically-dispersed iron catalyst with high oxygen reduction reaction (ORR) activity and stability in acidic electrolytes. As determined by high-resolution transmission electron microscopy (HR-TEM), X-ray absorption spectroscopy (XAS), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), this benign aqueous synthesis strategy facilitates the formation of homogeneous atomic nitrogen-coordinated iron sites embedded in a popcorn-like porous graphitic carbon matrix. These catalyst properties contribute to the improved ORR kinetic current density and mass transport. By controlling synthesis chemistry, the correlation between structure and property is systematically investigated. The iron content is the most critical material property and can regulate site density and graphitic carbon structures in the catalyst, impacting catalytic activity and stability. The enhanced performance and durability were examined in both acidic aqueous electrolytes and membrane electrode assemblies.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Science (SC)

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

OSTI ID:: 1797652

Alternate ID(s):: OSTI ID: 1828902

Journal Information:: Journal of the Electrochemical Society, Vol. 168, Issue 4; ISSN 0013-4651

Publisher:: IOP Publishing - The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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