Skip to main content

Combined Experimental and Theoretical Investigations of Nanoscale Structure-Activity Relationships for Fuel Cell Applications

EMSL Project ID


The proposed work will advance the understanding of metallic nanoparticle catalysts through direct comparison of experimental data and the results of quantum chemistry calculations. This will be accomplished by validating the experimental and theoretical results through rigorous comparison of carefully chosen systems where direct comparison in possible. The work will focus on a family of pure platinum and metallic core-platinum shell nanoparticles that will be synthesized with tightly-controlled size, shape and composition. Though these results are of considerable interest in their own right as catalytic materials, we will use these results to validate the use of the condensed Fukui function as a predictor of localized chemical reactivity in metallic nanoparticle systems. Additionally, we will functionalize the nanoparticles and study their properties using the same combined experimental and theoretical approach. Observables such as vibrational frequencies and chemical/Knight shifts are amenable to computation and will be studied experimentally. The proposed work will establish the condensed Fukui function as a powerful tool aiding in the rational design of new metallic nanoparticle catalysts.

Project Details

Project type
Large-Scale EMSL Research
Start Date
End Date


Principal Investigator

Thomas Allison
National Institute of Standards and Technology

Team Members

Eric Willis
Georgetown University

YuYe Tong
Georgetown University

Related Publications

Allison TC, and YJ Tong. 2011. "Evaluation of Methods to Predict Reactivity of Gold Nanoparticles." Physical Chemistry Chemical Physics. PCCP 13:12858–12864. doi:10.1039/c1cp20376b
Allison TC, and YJ Tong. 2012. "Application of the Condensed Fukui Function to Predict Reactivity in Core–Shell Transition Metal Nanoparticles." Electrochimica Acta 101:334-340. doi:10.1016/j.electacta.2012.12.072
Atienza DO, TC Allison, and YJ Tong. 2012. "Spatially Resolved Electronic Alterations As Seen by in Situ 195Pt and 13CO NMR in Ru@Pt and Au@Pt Core?Shell Nanoparticles." Journal of Physical Chemistry C 116(50):26480-26486. doi:10.1021/jp310313k
Chen DJ, TC Allison, S Sun, and YJ Tong. "Unraveling the Oxygen-Reduction-Reaction Mechanism on Au in Acidic Electrolytes." , Pacific Northwest National Laboratory, Richland, WA. [Unpublished]
Li Y, O Zaluzhna, CD Zangmeister, TC Allison, and YJ Tong. 2012. "Different Mechanisms Govern the Two-Phase Brust?Schiffrin Dialkylditelluride Syntheses of Ag and Au Nanoparticles." Journal of the American Chemical Society 134:1990-1992. doi:10.1021/ja210359r
Y. Li, B. S. Zelakiewicz, T. C. Allison, and Y. J. Tong, Measuring Level Alignment at the Metal-Molecule Interface by In Situ Electrochemical 13C NMR, ChemPhysChem 2015, 16, 747 - 751 (DOI: 10.1002/cphc.201402889)
Zaluzhna O, Y Li, CD Zangmeister, TC Allison, and YJ Tong. 2011. "Mechanistic Insights on One-phase vs.Ttwo-phase Brust–Schi?rin Method Synthesis of Au Nanoparticles with Dioctyl-diselenides." Chemical Communications 48(3):362-364. doi:10.1039/C1CC15955K
Zaluzhna O, Y Li, TC Allison, and YJ Tong. 2012. "Inverse-Micelle-Encapsulated Water-Enabled Bond Breaking of Dialkyl Diselenide/Disulfide: A Critical Step for Synthesizing High- Quality Gold Nanoparticles." Journal of the American Chemical Society 134(43):17991-17996. doi:10.1021/ja3068758