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Anomalous Structural Disorder in Supported Pt Nanoparticles.

Fernando D Vila¹, John J Rehr¹, Ralph G Nuzzo²

¹Department of Physics, University of Washington , Seattle, Washington 98195, United States.

The Journal of Physical Chemistry Letters

|July 4, 2017

Summary

This summary is machine-generated.

Supported platinum (Pt) nanocatalysts show unusual behavior due to thermal effects. New analysis reveals "anomalous structural disorder" (ASD) decreases with temperature, challenging traditional models.

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Area of Science:

Materials Science
Nanotechnology
Computational Chemistry

Background:

Supported platinum (Pt) nanocatalysts often display anomalous properties like negative thermal expansion and significant structural disorder.
Existing simulations using Density Functional Theory (DFT) and Molecular Dynamics (MD) attribute these behaviors to thermal vibrations and low-frequency disorder.

Purpose of the Study:

To provide a more comprehensive interpretation of the anomalous behavior observed in supported Pt nanocatalysts.
To dissect the contributions to mean-square relative displacements (MSRD) beyond simple vibrational and static disorder models.

Main Methods:

Utilized finite temperature DFT/MD simulations to model supported Pt nanocatalysts.
Developed a refined analysis to separate MSRD into vibrational disorder, dynamic structural disorder (DSD), and anomalous structural disorder (ASD).

Main Results:

Identified that vibrational and DSD components increase linearly with temperature, behaving as expected.
Demonstrated that ASD decreases with increasing temperature, reflecting changes in the mean nanoparticle geometry.
Showed that traditional methods of fitting MSRD lead to unphysical results for bond strengths and Grüneisen parameters.

Conclusions:

The anomalous behavior of supported Pt nanocatalysts is more complex than previously understood, involving a distinct 'anomalous structural disorder' (ASD) component.
Accurate interpretation requires distinguishing ASD from vibrational and dynamic disorder.
Current fitting procedures for MSRD in these systems require revision to account for ASD, preventing unphysical parameter estimations.