Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells

Tatyana Reshetenko; Madeleine Odgaard; Günter Randolf; Kenta K. Ohtaki; John P. Bradley; Barr Zulevi; Xiang Lyu; David A. Cullen; Charl J. Jafta; Alexey Serov; Andrei Kulikovsky

doi:10.1016/j.apcatb.2022.121424

Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells

Tatyana Reshetenko, Madeleine Odgaard, Günter Randolf, Kenta K. Ohtaki, John P. Bradley, Barr Zulevi, Xiang Lyu, David A. Cullen, Charl J. Jafta, Alexey Serov, Andrei Kulikovsky

Research output: Contribution to journal › Article › peer-review

27 Scopus citations

Abstract

The design of cathodic catalysts layer (CCL) consisted of Platinum Group Metal-free (PGM-free) electrocatalysts was done by catalyst coated membrane approach. Three different Fe-Mn-N-C compounds were synthesized with Fe:Mn ratio of 1:1, 2:1 and 2:1 with modified heat treatment profile. The catalysts were characterized by X-ray photoelectron spectroscopy, X-ray powder diffraction, pore and particle size distribution, zeta potential and transmission electron microscopy. Electrocatalysts were integrated into membrane electrode assembly and evaluated by electrochemical methods. Electrochemical impedance spectroscopy in combination with modeling were used for estimation of proton conductivity of CCL and its oxygen diffusivity. It was found that all CCLs possess extremely high proton conductivity, which was demonstrated for the first time for these types of PGM-free catalysts. The observed ORR mechanism was predominantly 4e^- due to peroxide/radicals scavenging effect of Mn.

Original language	English
Article number	121424
Journal	Applied Catalysis B: Environmental
Volume	312
DOIs	https://doi.org/10.1016/j.apcatb.2022.121424
State	Published - Sep 5 2022

Funding

TR gratefully acknowledges funding from US Office of Naval Research (N00014-18-1-2127, N00014-19-1-2159). MO, BZ, AS and TR gratefully acknowledge financial support from U.S. Department of Energy's Office of Energy Efficiency and Renewable Energy (EERE) under the Hydrogen and Fuel Cells Technologies Office (HFTO), FY2018 Hydrogen and Fuel Cell R&D FOA, Award no. DE-EE0008419. AS gratefully acknowledge financial support from the Oak Ridge National Laboratory SEED 10609 project ?Single-Atom Catalysts for CO2 Conversion?. Aberration-corrected STEM was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. TR gratefully acknowledges funding from US Office of Naval Research ( N00014-18-1-2127, N00014-19-1-2159 ). MO, BZ, AS and TR gratefully acknowledge financial support from U.S. Department of Energy’s Office of Energy Efficiency and Renewable Energy (EERE) under the Hydrogen and Fuel Cells Technologies Office (HFTO), FY2018 Hydrogen and Fuel Cell R&D FOA , Award no. DE-EE0008419 . AS gratefully acknowledge financial support from the Oak Ridge National Laboratory SEED 10609 project “Single-Atom Catalysts for CO 2 Conversion”. Aberration-corrected STEM was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility.

Keywords

Electron conductivity
Impedance
Modeling
PEM fuel cell
PGM-free electrode
Proton conductivity

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.apcatb.2022.121424

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title = "Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells",

abstract = "The design of cathodic catalysts layer (CCL) consisted of Platinum Group Metal-free (PGM-free) electrocatalysts was done by catalyst coated membrane approach. Three different Fe-Mn-N-C compounds were synthesized with Fe:Mn ratio of 1:1, 2:1 and 2:1 with modified heat treatment profile. The catalysts were characterized by X-ray photoelectron spectroscopy, X-ray powder diffraction, pore and particle size distribution, zeta potential and transmission electron microscopy. Electrocatalysts were integrated into membrane electrode assembly and evaluated by electrochemical methods. Electrochemical impedance spectroscopy in combination with modeling were used for estimation of proton conductivity of CCL and its oxygen diffusivity. It was found that all CCLs possess extremely high proton conductivity, which was demonstrated for the first time for these types of PGM-free catalysts. The observed ORR mechanism was predominantly 4e- due to peroxide/radicals scavenging effect of Mn.",

keywords = "Electron conductivity, Impedance, Modeling, PEM fuel cell, PGM-free electrode, Proton conductivity",

author = "Tatyana Reshetenko and Madeleine Odgaard and G{\"u}nter Randolf and Ohtaki, {Kenta K.} and Bradley, {John P.} and Barr Zulevi and Xiang Lyu and Cullen, {David A.} and Jafta, {Charl J.} and Alexey Serov and Andrei Kulikovsky",

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doi = "10.1016/j.apcatb.2022.121424",

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AU - Reshetenko, Tatyana

AU - Odgaard, Madeleine

AU - Randolf, Günter

AU - Ohtaki, Kenta K.

AU - Bradley, John P.

AU - Zulevi, Barr

AU - Lyu, Xiang

AU - Cullen, David A.

AU - Jafta, Charl J.

AU - Serov, Alexey

AU - Kulikovsky, Andrei

PY - 2022/9/5

Y1 - 2022/9/5

N2 - The design of cathodic catalysts layer (CCL) consisted of Platinum Group Metal-free (PGM-free) electrocatalysts was done by catalyst coated membrane approach. Three different Fe-Mn-N-C compounds were synthesized with Fe:Mn ratio of 1:1, 2:1 and 2:1 with modified heat treatment profile. The catalysts were characterized by X-ray photoelectron spectroscopy, X-ray powder diffraction, pore and particle size distribution, zeta potential and transmission electron microscopy. Electrocatalysts were integrated into membrane electrode assembly and evaluated by electrochemical methods. Electrochemical impedance spectroscopy in combination with modeling were used for estimation of proton conductivity of CCL and its oxygen diffusivity. It was found that all CCLs possess extremely high proton conductivity, which was demonstrated for the first time for these types of PGM-free catalysts. The observed ORR mechanism was predominantly 4e- due to peroxide/radicals scavenging effect of Mn.

AB - The design of cathodic catalysts layer (CCL) consisted of Platinum Group Metal-free (PGM-free) electrocatalysts was done by catalyst coated membrane approach. Three different Fe-Mn-N-C compounds were synthesized with Fe:Mn ratio of 1:1, 2:1 and 2:1 with modified heat treatment profile. The catalysts were characterized by X-ray photoelectron spectroscopy, X-ray powder diffraction, pore and particle size distribution, zeta potential and transmission electron microscopy. Electrocatalysts were integrated into membrane electrode assembly and evaluated by electrochemical methods. Electrochemical impedance spectroscopy in combination with modeling were used for estimation of proton conductivity of CCL and its oxygen diffusivity. It was found that all CCLs possess extremely high proton conductivity, which was demonstrated for the first time for these types of PGM-free catalysts. The observed ORR mechanism was predominantly 4e- due to peroxide/radicals scavenging effect of Mn.

KW - Electron conductivity

KW - Impedance

KW - Modeling

KW - PEM fuel cell

KW - PGM-free electrode

KW - Proton conductivity

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DO - 10.1016/j.apcatb.2022.121424

M3 - Article

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VL - 312

JO - Applied Catalysis B: Environmental

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M1 - 121424

ER -

Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells

Abstract

Funding

Keywords

UN SDGs

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