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Regulating Catalytic Properties and Thermal Stability of Pt and PtCo Intermetallic Fuel-Cell Catalysts via Strong Coupling Effects between Single-Metal Site-Rich Carbon and Pt
Abstract
Developing low platinum-group-metal (PGM) catalysts for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells (PEMFCs) for heavy-duty vehicles (HDVs) remains a great challenge due to the highly demanded power density and long-term durability. Here, this work explores the possible synergistic effect between single Mn site-rich carbon (MnSA-NC) and Pt nanoparticles, aiming to improve intrinsic activity and stability of PGM catalysts. Density functional theory (DFT) calculations predicted a strong coupling effect between Pt and MnN4 sites in the carbon support, strengthening their interactions to immobilize Pt nanoparticles during the ORR. The adjacent MnN4 sites weaken oxygen adsorption at Pt to enhance intrinsic activity. Well-dispersed Pt (2.1 nm) and ordered L12-Pt3Co nanoparticles (3.3 nm) were retained on the MnSA-NC support after indispensable high-temperature annealing up to 800 °C, suggesting enhanced thermal stability. Both PGM catalysts were thoroughly studied in membrane electrode assemblies (MEAs), showing compelling performance and durability. The Pt@MnSA-NC catalyst achieved a mass activity (MA) of 0.63 A mgPt–1 at 0.9 ViR-free and maintained 78% of its initial performance after a 30,000-cycle accelerated stress test (AST). The L12-Pt3Co@MnSA-NC catalyst accomplished a much higher MA of 0.91 A mgPt–1 and a current density of 1.63 A cm–2 at 0.7 Vmore »
- Authors:
-
[2];
[4];
[5];
[6];
[3];
[8];
[9];
[5];
[1]
- State Univ. of New York (SUNY), Buffalo, NY (United States)
- Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States); Purdue Univ., West Lafayette, IN (United States)
- Univ. of Pittsburgh, PA (United States)
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Oregon State Univ., Corvallis, OR (United States)
- Oregon State Univ., Corvallis, OR (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States)
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); National Science Foundation (NSF)
- OSTI Identifier:
- 1995471
- Alternate Identifier(s):
- OSTI ID: 2224167
- Report Number(s):
- BNL-224659-2023-JAAM
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- SC0012704; AC02-06CH11357; CBET-2016192; CBET-1949870; DMR-1905572; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 145; Journal Issue: 32; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; catalysts; platinum; redox reactions; stability; transition metals
Citation Formats
Zeng, Yachao, Liang, Jiashun, Li, Chenzhao, Qiao, Zhi, Li, Boyang, Hwang, Sooyeon, Kariuki, Nancy N., Chang, Chun-Wai, Wang, Maoyu, Lyons, Mason, Lee, Sungsik, Feng, Zhenxing, Wang, Guofeng, Xie, Jian, Cullen, David A., Myers, Deborah J., and Wu, Gang. Regulating Catalytic Properties and Thermal Stability of Pt and PtCo Intermetallic Fuel-Cell Catalysts via Strong Coupling Effects between Single-Metal Site-Rich Carbon and Pt. United States: N. p., 2023.
Web. doi:10.1021/jacs.3c03345.
Zeng, Yachao, Liang, Jiashun, Li, Chenzhao, Qiao, Zhi, Li, Boyang, Hwang, Sooyeon, Kariuki, Nancy N., Chang, Chun-Wai, Wang, Maoyu, Lyons, Mason, Lee, Sungsik, Feng, Zhenxing, Wang, Guofeng, Xie, Jian, Cullen, David A., Myers, Deborah J., & Wu, Gang. Regulating Catalytic Properties and Thermal Stability of Pt and PtCo Intermetallic Fuel-Cell Catalysts via Strong Coupling Effects between Single-Metal Site-Rich Carbon and Pt. United States. https://doi.org/10.1021/jacs.3c03345
Zeng, Yachao, Liang, Jiashun, Li, Chenzhao, Qiao, Zhi, Li, Boyang, Hwang, Sooyeon, Kariuki, Nancy N., Chang, Chun-Wai, Wang, Maoyu, Lyons, Mason, Lee, Sungsik, Feng, Zhenxing, Wang, Guofeng, Xie, Jian, Cullen, David A., Myers, Deborah J., and Wu, Gang. Fri .
"Regulating Catalytic Properties and Thermal Stability of Pt and PtCo Intermetallic Fuel-Cell Catalysts via Strong Coupling Effects between Single-Metal Site-Rich Carbon and Pt". United States. https://doi.org/10.1021/jacs.3c03345.
@article{osti_1995471,
title = {Regulating Catalytic Properties and Thermal Stability of Pt and PtCo Intermetallic Fuel-Cell Catalysts via Strong Coupling Effects between Single-Metal Site-Rich Carbon and Pt},
author = {Zeng, Yachao and Liang, Jiashun and Li, Chenzhao and Qiao, Zhi and Li, Boyang and Hwang, Sooyeon and Kariuki, Nancy N. and Chang, Chun-Wai and Wang, Maoyu and Lyons, Mason and Lee, Sungsik and Feng, Zhenxing and Wang, Guofeng and Xie, Jian and Cullen, David A. and Myers, Deborah J. and Wu, Gang},
abstractNote = {Developing low platinum-group-metal (PGM) catalysts for the oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells (PEMFCs) for heavy-duty vehicles (HDVs) remains a great challenge due to the highly demanded power density and long-term durability. Here, this work explores the possible synergistic effect between single Mn site-rich carbon (MnSA-NC) and Pt nanoparticles, aiming to improve intrinsic activity and stability of PGM catalysts. Density functional theory (DFT) calculations predicted a strong coupling effect between Pt and MnN4 sites in the carbon support, strengthening their interactions to immobilize Pt nanoparticles during the ORR. The adjacent MnN4 sites weaken oxygen adsorption at Pt to enhance intrinsic activity. Well-dispersed Pt (2.1 nm) and ordered L12-Pt3Co nanoparticles (3.3 nm) were retained on the MnSA-NC support after indispensable high-temperature annealing up to 800 °C, suggesting enhanced thermal stability. Both PGM catalysts were thoroughly studied in membrane electrode assemblies (MEAs), showing compelling performance and durability. The Pt@MnSA-NC catalyst achieved a mass activity (MA) of 0.63 A mgPt–1 at 0.9 ViR-free and maintained 78% of its initial performance after a 30,000-cycle accelerated stress test (AST). The L12-Pt3Co@MnSA-NC catalyst accomplished a much higher MA of 0.91 A mgPt–1 and a current density of 1.63 A cm–2 at 0.7 V under traditional light-duty vehicle (LDV) H2–air conditions (150 kPaabs and 0.10 mgPt cm–2). Furthermore, the same catalyst in an HDV MEA (250 kPaabs and 0.20 mgPt cm–2) delivered 1.75 A cm–2 at 0.7 V, only losing 18% performance after 90,000 cycles of the AST, demonstrating great potential to meet the DOE targets.},
doi = {10.1021/jacs.3c03345},
journal = {Journal of the American Chemical Society},
number = 32,
volume = 145,
place = {United States},
year = {Fri Aug 04 00:00:00 EDT 2023},
month = {Fri Aug 04 00:00:00 EDT 2023}
}
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