4.8 Article

Biaxial Strains Mediated Oxygen Reduction Electrocatalysis on Fenton Reaction Resistant L10-PtZn Fuel Cell Cathode

Journal

ADVANCED ENERGY MATERIALS
Volume 10, Issue 29, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202000179

Keywords

electrocatalysis; Fenton reaction; fuel cells; intermetallics; oxygen reduction

Funding

  1. National Nature Science Foundation of China [21972051]
  2. NSF-PREM program [DMR-1828019]
  3. U.S. Department of Energy (DOE), Office of Basic Energy Science [DE-SC0012704]

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PtM alloy catalysts (e.g., PtFe, PtCo), especially in an intermetallic L1(0) structure, have attracted considerable interest due to their respectable activity and stability for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). However, metal-catalyzed formation of center dot OH from H2O2 (i.e., Fenton reaction) by Fe- or Co-containing catalysts causes severe degradation of PEM/catalyst layers, hindering the prospects of commercial applications. Zinc is known as an antioxidant in Fenton reaction, but is rarely alloyed with Pt owing to its relatively negative redox potential. Here, sub-4 nm intermetallic L1(0)-PtZn nanoparticles (NPs) are synthesized as high-performance PEMFC cathode catalysts. In PEMFC tests, the L1(0)-PtZn cathode achieves outstanding activity (0.52 A mg(Pt)(-1) at 0.9 V-iR(-free), and peak power density of 2.00 W cm(-2)) and stability (only 16.6% loss in mass activity after 30 000 voltage cycles), exceeding the U.S. DOE 2020 targets and most of the reported ORR catalysts. Density function theory calculations reveal that biaxial strains developed upon the disorder-order (A1-L1(0)) transition of PtZn NPs would modulate the surface Pt-Pt distances and optimize Pt-O binding for ORR activity enhancement, while the increased vacancy formation energy of Zn atoms in an ordered structure accounts for the improved stability.

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