Amino-tethering synthesis strategy toward highly accessible sub-3-nm L10-PtM catalysts for high-power fuel cells

Qing Gong; Hong Zhang; Haoran Yu; Sungho Jeon; Yang Ren; Zhenzhen Yang; Cheng Jun Sun; Eric A. Stach; Alexandre C. Foucher; Yikang Yu; Matthew Smart; Gabriel M. Filippelli; David A. Cullen; Ping Liu; Jian Xie

doi:10.1016/j.matt.2022.12.011

Amino-tethering synthesis strategy toward highly accessible sub-3-nm L1₀-PtM catalysts for high-power fuel cells

Qing Gong, Hong Zhang, Haoran Yu, Sungho Jeon, Yang Ren, Zhenzhen Yang, Cheng Jun Sun, Eric A. Stach, Alexandre C. Foucher, Yikang Yu, Matthew Smart, Gabriel M. Filippelli, David A. Cullen, Ping Liu, Jian Xie

Materials MicroAnalysis

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

22 Scopus citations

Abstract

Because of the poor accessibility of embedded active sites, platinum (Pt)-based electrocatalysts suffer from insufficient Pt utilization and mass transport in membrane electrode assemblies (MEAs), limiting their performance in polymer electrolyte membrane fuel cells. Here, we report a simple and universal approach to depositing sub-3-nm L1₀-PtM nanoparticles over external surfaces of carbon supports through pore-tailored amino (NH₂)-modification, which enables not only excellent activity for the oxygen reduction reaction, but also enhanced Pt utilization and mass transport in MEAs. Using a low loading of 0.10 mg_Pt·cm⁻², the MEA of PtCo/KB-NH₂ delivered an excellent mass activity of 0.691 A·mg_Pt⁻¹, a record-high power density of 0.96 W·cm⁻² at 0.67 V, and only a 30-mV drop at 0.80 A·cm⁻² after 30,000 voltage cycles, which meets nearly all targets set by the Department of Energy. This work provides an efficient strategy for designing advanced Pt-based electrocatalysts and realizing high-power fuel cells.

Original language	English
Pages (from-to)	963-982
Number of pages	20
Journal	Matter
Volume	6
Issue number	3
DOIs	https://doi.org/10.1016/j.matt.2022.12.011
State	Published - Mar 1 2023

Funding

This work was partially supported by the Hydrogen and Fuel Cell Technologies Office, Office of Energy Efficiency and Renewable Energy, U.S. Department of Energy (DOE). This research utilized resources of the Advanced Photon Source, an Office of Science User Facility operated by Argonne National Laboratory for the U.S. DOE Office of Science under contract DE- AC02-06CH11357 . The Center for Nanophase Materials Sciences (CNMS), which is a U.S. DOE Office of Science User Facility at Oak Ridge National Laboratory , and the Singh Center for Nanotechnology at the University of Pennsylvania , which is supported by the NSF National Nanotechnology Coordinated Infrastructure Program under grant NNCI-1542153 and by the NSF through the University of Pennsylvania Materials Research Science and Engineering Center (MRSEC) ( DMR-1720530 ), carried out the electron microscopy work. A.C.F. acknowledges support from IMASC, an Energy Frontier Research Center funded by the U.S. DOE Office of Science. S.J. and E.A.S. acknowledge support from the Center for Hybrid Approaches in Solar Energy to Liquid Fuels (CHASE), an Energy Innovation Hub funded by the U.S. DOE Office of Science, Office of Basic Energy Sciences under award DE-SC0021173 . Theoretical studies were performed at Brookhaven National Laboratory and supported by the Chemical Sciences, Geosciences, and Biosciences Division , U.S. DOE Office of Basic Energy Science, under contract DE-SC0012704 . The calculations performed in this work used computational resources at the Center for Functional Nanomaterials (CFN) and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory , under contract DE-SC0012704 and at Stony Brook University , which was funded by a National Science Foundation grant ( 1531492 ). The authors gratefully acknowledge help from the Post Test Facility at Argonne National Laboratory, supported by the U.S. DOE Vehicle Technologies Office under contract DE-AC02-06CH11357 .

Funders	Funder number
Center for Nanophase Materials Sciences
IMASC
University of Pennsylvania Materials Research Science and Engineering Center
National Science Foundation	NNCI-1542153, DE-AC02-06CH11357, 1531492
U.S. Department of Energy
Office of Science	DE- AC02-06CH11357
Office of Energy Efficiency and Renewable Energy
Basic Energy Sciences	DE-SC0021173, DE-SC0012704
Argonne National Laboratory
Oak Ridge National Laboratory
Brookhaven National Laboratory
Hydrogen and Fuel Cell Technologies Office
Materials Research Science and Engineering Center, Harvard University	DMR-1720530
Chemical Sciences, Geosciences, and Biosciences Division

Keywords

L1-PtCo nanoparticle
MAP5: Improvement
amino modification
membrane electrode assembly
oxygen reduction reaction
platinum-based intermetallic
proton exchange membrane fuel cell

UN SDGs

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

Access to Document

10.1016/j.matt.2022.12.011

Cite this

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title = "Amino-tethering synthesis strategy toward highly accessible sub-3-nm L10-PtM catalysts for high-power fuel cells",

abstract = "Because of the poor accessibility of embedded active sites, platinum (Pt)-based electrocatalysts suffer from insufficient Pt utilization and mass transport in membrane electrode assemblies (MEAs), limiting their performance in polymer electrolyte membrane fuel cells. Here, we report a simple and universal approach to depositing sub-3-nm L10-PtM nanoparticles over external surfaces of carbon supports through pore-tailored amino (NH2)-modification, which enables not only excellent activity for the oxygen reduction reaction, but also enhanced Pt utilization and mass transport in MEAs. Using a low loading of 0.10 mgPt·cm−2, the MEA of PtCo/KB-NH2 delivered an excellent mass activity of 0.691 A·mgPt−1, a record-high power density of 0.96 W·cm−2 at 0.67 V, and only a 30-mV drop at 0.80 A·cm−2 after 30,000 voltage cycles, which meets nearly all targets set by the Department of Energy. This work provides an efficient strategy for designing advanced Pt-based electrocatalysts and realizing high-power fuel cells.",

keywords = "L1-PtCo nanoparticle, MAP5: Improvement, amino modification, membrane electrode assembly, oxygen reduction reaction, platinum-based intermetallic, proton exchange membrane fuel cell",

author = "Qing Gong and Hong Zhang and Haoran Yu and Sungho Jeon and Yang Ren and Zhenzhen Yang and Sun, {Cheng Jun} and Stach, {Eric A.} and Foucher, {Alexandre C.} and Yikang Yu and Matthew Smart and Filippelli, {Gabriel M.} and Cullen, {David A.} and Ping Liu and Jian Xie",

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AU - Gong, Qing

AU - Zhang, Hong

AU - Yu, Haoran

AU - Jeon, Sungho

AU - Ren, Yang

AU - Yang, Zhenzhen

AU - Sun, Cheng Jun

AU - Stach, Eric A.

AU - Foucher, Alexandre C.

AU - Yu, Yikang

AU - Smart, Matthew

AU - Filippelli, Gabriel M.

AU - Cullen, David A.

AU - Liu, Ping

AU - Xie, Jian

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