4.8 Article

Inducing Covalent Atomic Interaction in Intermetallic Pt Alloy Nanocatalysts for High-Performance Fuel Cells

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 62, Issue 23, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202302134

Keywords

Covalent Interaction; Electrocatalysis; Fuel Cells; Intermetallics; Oxygen Reduction Reaction

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In this study, L1(0)-Pt2CuGa intermetallic nanoparticles with a unique covalent atomic interaction between Pt-Ga were reported as high-performance cathode catalysts in proton exchange membrane fuel cells (PEMFCs). The L1(0)-Pt2CuGa/C catalyst showed superb oxygen reduction reaction (ORR) activity and stability. The theoretical calculations revealed that the optimized adsorption of oxygen intermediates on the L1(0)-Pt2CuGa surface resulted from the formed biaxial strain, and the durability enhancement was attributed to the stronger Pt-M bonds compared to L1(1)-PtCu due to the Pt-Ga covalent interactions.
The harsh working environments of proton exchange membrane fuel cells (PEMFCs) pose huge challenges to the stability of Pt-based alloy catalysts. The widespread presence of metallic bonds with significantly delocalized electron distribution often lead to component segregation and rapid performance decay. Here we report L1(0)-Pt2CuGa intermetallic nanoparticles with a unique covalent atomic interaction between Pt-Ga as high-performance PEMFC cathode catalysts. The L1(0)-Pt2CuGa/C catalyst shows superb oxygen reduction reaction (ORR) activity and stability in fuel cell cathode (mass activity=0.57 A mg(Pt)(-1) at 0.9 V, peak power density=2.60/1.24 W cm(-2) in H-2-O-2/air, 28 mV voltage loss at 0.8 A cm(-2) after 30 000 cycles). Theoretical calculations reveal the optimized adsorption of oxygen intermediates via the formed biaxial strain on L1(0)-Pt2CuGa surface, and the durability enhancement stems from the stronger Pt-M bonds than those in L1(1)-PtCu resulted from Pt-Ga covalent interactions.

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