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

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

doi:10.1021/jacs.3c03345

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

Journal Article · Fri Aug 04 00:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c03345· OSTI ID:1995471

Zeng, Yachao ^[1]; Liang, Jiashun ^[1];

^[2]; Qiao, Zhi ^[1]; Li, Boyang ^[3];

^[4]; Kariuki, Nancy N. ^[5]; Chang, Chun-Wai ^[6]; Wang, Maoyu ^[7]; Lyons, Mason ^[6];

^[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)

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 (Mn_SA-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 Mn_SA-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@Mn_SA-NC catalyst achieved a mass activity (MA) of 0.63 A mg_Pt^–1 at 0.9 V_iR-free and maintained 78% of its initial performance after a 30,000-cycle accelerated stress test (AST). The L1₂-Pt₃Co@Mn_SA-NC catalyst accomplished a much higher MA of 0.91 A mg_Pt^–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 kPa_abs and 0.10 mg_Pt cm^–2). Furthermore, the same catalyst in an HDV MEA (250 kPa_abs and 0.20 mg_Pt 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.

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Research Organization:: 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 Organization:: 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)

Grant/Contract Number:: SC0012704; AC02-06CH11357; CBET-2016192; CBET-1949870; DMR-1905572; AC05-00OR22725

OSTI ID:: 1995471

Alternate ID(s):: OSTI ID: 2224167

Report Number(s):: BNL-224659-2023-JAAM

Journal Information:: Journal of the American Chemical Society, Vol. 145, Issue 32; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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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

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