Ordered CoPt oxygen reduction catalyst with high performance and durability

Yung Tin Pan; Dongguo Li; Shubham Sharma; Chenyu Wang; Michael J. Zachman; Evan C. Wegener; A. Jeremy Kropf; Yu Seung Kim; Deborah J. Myers; Andrew A. Peterson; David A. Cullen; Jacob S. Spendelow

doi:10.1016/j.checat.2022.10.030

Ordered CoPt oxygen reduction catalyst with high performance and durability

Yung Tin Pan, Dongguo Li, Shubham Sharma, Chenyu Wang, Michael J. Zachman, Evan C. Wegener, A. Jeremy Kropf, Yu Seung Kim, Deborah J. Myers, Andrew A. Peterson, David A. Cullen, Jacob S. Spendelow

Materials MicroAnalysis

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

21 Scopus citations

Abstract

A high-performance and durable polymer electrolyte membrane fuel cell cathode catalyst composed of an ordered L1₀–CoPt core and a thin Pt shell was designed and prepared. Under practical fuel cell membrane electrode assembly testing conditions, the cathode catalyst showed an outstanding initial mass activity of 0.6 A/mg_Pt, which satisfies the U.S. Department of Energy performance target while also meeting the durability target of less than 40% loss in mass activity after 30,000 accelerated stress test voltage cycles. The high structural stability of the L1₀–CoPt@Pt-shell catalyst was confirmed by postmortem materials characterization, and the origin of this robustness was revealed by density functional theory calculations, where the barriers for diffusion of Co atoms were observed to be significantly increased in the ordered intermetallic core.

Original language	English
Pages (from-to)	3559-3572
Number of pages	14
Journal	Chem Catalysis
Volume	2
Issue number	12
DOIs	https://doi.org/10.1016/j.checat.2022.10.030
State	Published - Dec 15 2022

Funding

The authors thank the U.S. Department of Energy’s Hydrogen and Fuel Cell Technologies Office (DOE-HFTO) for funding support through the project “Advanced Electrocatalysts through Crystallographic Enhancement.” Financial support for this work was also provided by the Laboratory Directed Research and Development (LDRD) program at Los Alamos National Laboratory (LANL) under projects 20190640PRD3 and 20200200DR . Electron microscopy was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility, through user proposal CNMS2018-102. This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357 . MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The perspectives expressed in the article do not represent the views of LANL, the DOE, or the U.S. government. The authors thank the U.S. Department of Energy's Hydrogen and Fuel Cell Technologies Office (DOE-HFTO) for funding support through the project “Advanced Electrocatalysts through Crystallographic Enhancement.” Financial support for this work was also provided by the Laboratory Directed Research and Development (LDRD) program at Los Alamos National Laboratory (LANL) under projects 20190640PRD3 and 20200200DR. Electron microscopy was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility, through user proposal CNMS2018-102. This research used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. MRCAT operations are supported by the Department of Energy and the MRCAT member institutions. The perspectives expressed in the article do not represent the views of LANL, the DOE, or the U.S. government. The work was conceived by Y.-T.P. Y.S.K. and J.S.S. Y.T.P. wrote the experimental portion of the manuscript and carried out most of the experimental work including catalyst preparation, MEA fabrication, testing, and in-house characterization by PXRD and X-ray fluorescence spectroscopy. D.L. performed low magnification TEM for particle size analysis. C.W. assisted with the PXRD analysis. D.A.C. D.L. and J.S.S. carried out high-resolution STEM, EDS elemental mapping, and related analyses. M.J.Z. performed analysis on EDS maps and generated radial distribution plots. E.C.W. A.J.K. and D.J.M. performed the EXAFS experiments and data analysis. S.S. performed the DFT calculation and wrote the DFT portion of the manuscript under the supervision of A.A.P. J.S.S. supervised the research project. There are no conflicts to declare. Yung-Tin Pan is currently affiliated with the Department of Chemical Engineering at National Tsing-Hua University as an assistant professor. However, his participation in the experimental and original manuscript writing was completed during his stay at Los Alamos National Laboratory.

Funders	Funder number
DOE-HFTO
Department of Chemical Engineering at National Tsing-Hua University
U.S. Government
U.S. Department of Energy
Office of Science	CNMS2018-102
Argonne National Laboratory	DE-AC02-06CH11357
Laboratory Directed Research and Development
Los Alamos National Laboratory	20190640PRD3, 20200200DR
Hydrogen and Fuel Cell Technologies Office

Keywords

L1–CoPt
SDG7: Affordable and clean energy
fuel cell
intermetallic
oxygen reduction reaction

UN SDGs

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

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10.1016/j.checat.2022.10.030

Cite this

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title = "Ordered CoPt oxygen reduction catalyst with high performance and durability",

abstract = "A high-performance and durable polymer electrolyte membrane fuel cell cathode catalyst composed of an ordered L10–CoPt core and a thin Pt shell was designed and prepared. Under practical fuel cell membrane electrode assembly testing conditions, the cathode catalyst showed an outstanding initial mass activity of 0.6 A/mgPt, which satisfies the U.S. Department of Energy performance target while also meeting the durability target of less than 40% loss in mass activity after 30,000 accelerated stress test voltage cycles. The high structural stability of the L10–CoPt@Pt-shell catalyst was confirmed by postmortem materials characterization, and the origin of this robustness was revealed by density functional theory calculations, where the barriers for diffusion of Co atoms were observed to be significantly increased in the ordered intermetallic core.",

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AU - Sharma, Shubham

AU - Wang, Chenyu

AU - Zachman, Michael J.

AU - Wegener, Evan C.

AU - Kropf, A. Jeremy

AU - Kim, Yu Seung

AU - Myers, Deborah J.

AU - Peterson, Andrew A.

AU - Cullen, David A.

AU - Spendelow, Jacob S.

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N2 - A high-performance and durable polymer electrolyte membrane fuel cell cathode catalyst composed of an ordered L10–CoPt core and a thin Pt shell was designed and prepared. Under practical fuel cell membrane electrode assembly testing conditions, the cathode catalyst showed an outstanding initial mass activity of 0.6 A/mgPt, which satisfies the U.S. Department of Energy performance target while also meeting the durability target of less than 40% loss in mass activity after 30,000 accelerated stress test voltage cycles. The high structural stability of the L10–CoPt@Pt-shell catalyst was confirmed by postmortem materials characterization, and the origin of this robustness was revealed by density functional theory calculations, where the barriers for diffusion of Co atoms were observed to be significantly increased in the ordered intermetallic core.

AB - A high-performance and durable polymer electrolyte membrane fuel cell cathode catalyst composed of an ordered L10–CoPt core and a thin Pt shell was designed and prepared. Under practical fuel cell membrane electrode assembly testing conditions, the cathode catalyst showed an outstanding initial mass activity of 0.6 A/mgPt, which satisfies the U.S. Department of Energy performance target while also meeting the durability target of less than 40% loss in mass activity after 30,000 accelerated stress test voltage cycles. The high structural stability of the L10–CoPt@Pt-shell catalyst was confirmed by postmortem materials characterization, and the origin of this robustness was revealed by density functional theory calculations, where the barriers for diffusion of Co atoms were observed to be significantly increased in the ordered intermetallic core.

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Ordered CoPt oxygen reduction catalyst with high performance and durability

Abstract

Funding

Keywords

UN SDGs

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