Abstract
Structurally ordered PtCo intermetallics are one of the most promising oxygen-reduction catalysts in proton exchange membrane fuel cells (PEMFCs) due to their intrinsically improved catalytic activity and stability relative to PtCo solid-solution alloys. However, increasing the heating temperature to achieve a desirable high degree of ordering results in severe particle agglomeration and low mass activity and stability. Herein, a two-step synthesis approach is developed to create an L12-Pt3Co intermetallic structure with an increased ordering degree and well-dispersed ultrafine particles. The first step of the synthesis yields ultrafine Pt nanoparticles that are well-dispersed on the ZIF-8-derived carbon support. The second adsorption step enables us to fine-tune the Pt and Co interfaces, assisted by optimal amino acids, to establish a favorable Co-rich environment around fine Pt nanoparticles, facilitating Co diffusion into the Pt crystalline under mild thermal conditions (<800 °C). This two-step ordered L12-Pt3Co catalyst is systematically evaluated using membrane electrode assemblies under heavy-duty vehicle (HDV) conditions and demonstrated exceptional performance and durability, retaining 1.35 A cm-2 only a 7% loss in current density at 0.7 V after an extensive accelerated stress test of 150,000 voltage cycles.
| Original language | English |
|---|---|
| Journal | Advanced Materials |
| DOIs | |
| State | Accepted/In press - 2025 |
Funding
J.L. and H.Y. contributed equally to this work. This work was financially supported by the start‐up fund at Washington University in St. Louis and the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office, and the Million Mile Fuel Cell Truck (MFCT) Consortium ( https://millionmilefuelcelltruck.org ). This work was also partially supported by the U.S. Department of Energy, SBIR project (DE‐SC0021671) led by Giner Inc. This research used the Electron Microscopy facility of the Center for Functional Nanomaterials (CFN), for catalyst characterizations and in situ experiments, a U.S. Department of Energy Office of Science User Facility, at Brookhaven National Laboratory under Contract No. DE‐SC0012704 (Figures 1b–d,2 ; Figures S6–S8 and S13–S14 , Supporting Information). WAXS experiments were supported at the Molecular Foundry, and the Advanced Light Source was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE‐AC02‐ 05CH11231. Post‐mortem MEA electron microscopy research was supported by the Center for Nanophase Materials Sciences (CNMS), which is the U.S. Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory (Figures 1e , 5 ; and Figures S26–S30 , Supporting Information). 2
Keywords
- ORR
- PEMFC
- PtCo catalyst
- electrocatalysis
- heavy-duty vehicle