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Issue 17, 2020
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Testing the predictive power of theory for PdxIr(100−x) alloy nanoparticles for the oxygen reduction reaction

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Abstract

In this report, density functional theory (DFT) calculations of O and OH binding energies on triatomic surface ensembles of PdxIr(100−x) nanoalloys successfully predicted the overall trend in experimental oxygen reduction reaction (ORR) activity as a function of nanoparticle (NP) composition. Specifically, triatomic Pd3 ensembles were found to possess optimal O and OH binding energies and were predicted to be highly active sites for the ORR, rivaling that of Pt(111). However, DFT calculations suggest that the O binding energy increases at active sites containing Ir, thereby decreasing ORR activity. PdxIr(100−x) nanoalloys were synthesized using a microwave-assisted method and their activity towards the ORR was tested using rotating disk voltammetry (RDV). As predicted, the bimetallic electrocatalysts exhibited worse catalytic activity than the Pd-only NPs. The strong qualitative correlation between the theoretical and experimental results demonstrates that the activity of individual active sites on the surface of NPs can serve as a proxy for overall activity. This is a particularly useful strategy for applying DFT calculations to electrocatalysts that are too large for true first-principle analysis.

Graphical abstract: Testing the predictive power of theory for PdxIr(100−x) alloy nanoparticles for the oxygen reduction reaction

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Supplementary files

Article information


Submitted
15 Dec 2019
Accepted
05 Apr 2020
First published
17 Apr 2020

J. Mater. Chem. A, 2020,8, 8421-8429
Article type
Paper
Author version available

Testing the predictive power of theory for PdxIr(100−x) alloy nanoparticles for the oxygen reduction reaction

H. Guo, J. A. Trindell, H. Li, D. Fernandez, S. M. Humphrey, G. Henkelman and R. M. Crooks, J. Mater. Chem. A, 2020, 8, 8421
DOI: 10.1039/C9TA13711D

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