skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Engineered Catalyst Support with Improved Durability at Higher Weight Percentage of Platinum
Proton Exchange Membrane (PEM) fuel cells are a suitable electrochemical power source for heavy duty vehicle (HDV) applications due to their high efficiency and durability. The cathode of the fuel cell uses a higher geometric loading of platinum (∼0.2 to 0.4 mgPt/cm2) for the electrocatalysis of the kinetically sluggish Oxygen Reduction Reaction (ORR) which requires higher weight percent loading of the metal (∼50%) on the carbon support to decrease the catalyst layer thickness and hence, the reactant transport losses. The conventionally used supports for platinum catalyst, such as the KetjenBlackTMtype high surface area carbon (HSC) features limited mesopore area for the dispersion of Pt nanoparticles leading to increased aggregation and poor durability. Here, we show a new class of carbon materials known as the Engineered Catalyst Support (ECS) developed by Pajarito Powder with higher mesopore fraction for the dispersion of higher weight percentage of Pt nanoparticles. ECS materials can disperse up to 50% Pt by weight of the catalyst thereby enabling lower catalyst layer thickness with higher performance retained after durability test. A comprehensive set of physico-chemical and electrochemical studies in membrane electrode assembly (MEA) are reported to understand the performance and durability of Pt/ECS catalysts.  more » « less
Award ID(s):
1719875
PAR ID:
10549354
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Publisher / Repository:
IOP Publishing
Date Published:
Journal Name:
Journal of The Electrochemical Society
Volume:
170
Issue:
11
ISSN:
0013-4651
Page Range / eLocation ID:
114503
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; ; ; ; (, Journal of The Electrochemical Society)
    In this work we investigate the effect of platinum loading and layer thickness on cathode catalyst degradation by a comprehensive in situ and STEM-EDS characterization. To decouple the effect of the platinum loading and layer thickness from each other, the experiments were categorized in two sets, each with cathode loadings varying between 0.1 and 0.4 mgPtcm−2: (i) Samples with a constant Pt/C ratio and thus varying layer thickness, and (ii) samples with varying Pt/C ratios, achieved by dilution with bare carbon, to maintain a constant layer thickness at different platinum loadings. Every MEA was subjected to an accelerated stress test, where the cell was operated for 45,000 cycles between 0.6 and 0.95 V. Regardless of the Pt/C ratio, a higher relative loss in electrochemically active surface area was measured for lower Pt loadings. STEM-EDS measurements showed that Pt was mainly lost close to the cathode—membrane interface by the concentration driven Pt2+ion flux into the membrane. The size of this Pt-depletion zone has shown to be independent on the overall Pt loading and layer thickness, hence causing higher relative Pt loss in low thickness electrodes, as the depletion zone accounts for a larger fraction of the catalyst layer. 
    more » « less
  2. ; ; ; ; ; ; ; ; (, Advanced Energy Materials)
    Abstract For global deployment of proton exchange membrane fuel cells, achieving optimal interaction between the components of the cathode active layer remains challenging. Studies addressing the effect of nanoparticle location (inside vs outside of pores) on performance and durability mostly compare porous and nonporous carbon supports, thus coming short of decoupling nanoparticle locality from carbon support effects. To address the influence of nanoparticle locality on performance and durability, new carbon‐supported electrocatalysts with designed and distinct nanoparticle localities are presented. The developed methodology allows to place Pt nanoparticles preferentially inside or outside of the mesopores of conductive carbon supports from materials under development at Cabot Corporation. Synthesis protocols are tuned to control nanoparticle size, crystallinity, and loading; this way the effect of Pt locality can be studied for two experimental carbon supports in isolation from all other parameters. For one carbon support, Pt active surface area and activity are significantly lower when nanoparticles are placed inside the pores. In contrast, for another, more graphitic carbon support, placing nanoparticles inside or outside of the carbon pores produces no appreciable difference in active surface area and performance rotating disk electrode measurements. Given their carefully tailored structure, these catalysts provide a framework for evaluating locality‐performance‐durability relationships. 
    more » « less
  3. ; ; ; ; ; (, Nature Communications)
    Abstract Ionic liquids (ILs) have shown to be promising additives to the catalyst layer to enhance oxygen reduction reaction in polymer electrolyte fuel cells. However, fundamental understanding of their role in complex catalyst layers in practically relevant membrane electrode assembly environment is needed for rational design of highly durable and active platinum-based catalysts. Here we explore three imidazolium-derived ionic liquids, selected for their high proton conductivity and oxygen solubility, and incorporate them into high surface area carbon black support. Further, we establish a correlation between the physical properties and electrochemical performance of the ionic liquid-modified catalysts by providing direct evidence of ionic liquids role in altering hydrophilic/hydrophobic interactions within the catalyst layer interface. The resulting catalyst with optimized interface design achieved a high mass activity of 347 A g−1Ptat 0.9 V under H2/O2, power density of 0.909 W cm−2under H2/air and 1.5 bar, and had only 0.11 V potential decrease at 0.8 A cm−2after 30 k accelerated stress test cycles. This performance stems from substantial enhancement in Pt utilization, which is buried inside the mesopores and is now accessible due to ILs addition. 
    more » « less
  4. ; ; ; ; ; ; ; ; ; ; et al (, Journal of the American Chemical Society)
    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. 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. 
    more » « less
  5. ; ; ; ; ; ; (, ChemCatChem)
    Abstract We report a new catalytic system by partially covering the uniform Pt nanocrystals on a carbon support with an ultrathin film derived from polyacrylonitrile (PAN). The use of Pt nanocrystals uniform in both size and shape effectively suppresses Ostwald repining, while partially covering them with a PAN‐derived film prevents migration, aggregation, and detachment from the support. In addition, the pyridinic N atoms on the edges of the thermally‐treated PAN film can also weaken the O=O bond, accelerating the reduction of oxygen. Upon optimization, the new catalyst exhibits a mass activity of 0.51 mA ⋅ μg−1Pttoward oxygen reduction, substantially enhanced relative to the same catalyst without PAN (0.22 mA ⋅ μg−1Pt) and a commercial Pt/C (0.41 mA ⋅ μg−1Pt). The mass activity is essentially retained after 10,000 cycles of accelerated durability test between 0.6 V and 1.1 V in oxygen‐saturated HClO4. Even after aging in H3PO4at 220 °C for one week, the electrochemical surface area of the catalyst is still maintained. This catalytic system holds great promise for use in various types of fuel cells with a long lifetime. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email