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

Guo, Hongyu; Trindell, Jamie A.; Li, Hao; Fernandez, Desiree; Humphrey, Simon M.; Henkelman, Graeme; Crooks, Richard M.

doi:10.1039/C9TA13711D

Title: Testing the predictive power of theory for Pd_xIr_(100-x) alloy nanoparticles for the oxygen reduction reaction

Journal Article · Fri Apr 17 00:00:00 EDT 2020 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/C9TA13711D· OSTI ID:1617193

Guo, Hongyu ^[1];

^[1]; Li, Hao ^[1]; Fernandez, Desiree ^[1];

^[1];

^[1]

Univ. of Texas, Austin, TX (United States)

Here, density functional theory (DFT) calculations of O and OH binding energies on triatomic surface ensembles of Pd_xIr_(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. Pd_xIr_(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.

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Research Organization:: Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); Robert A; Welch Foundation

Grant/Contract Number:: SC0010576; CHE-1807847; F-0032; F-1841; F-1738

OSTI ID:: 1617193

Alternate ID(s):: OSTI ID: 1615133

Journal Information:: Journal of Materials Chemistry. A, Vol. 8, Issue 17; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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