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Deducing Subnanometer Cluster Size and Shape Distributions of Heterogeneous Supported Catalysts by Vinson Liao; Maximilian Cohen; Yifan Wang; Dionisios G. Vlachos is a Biochemistry, Genetics and Molecular Biology article available to read on EtoBox.

What is Deducing Subnanometer Cluster Size and Shape Distributions of Heterogeneous Supported Catalysts about?

Infrared (IR) spectra of adsorbate vibrational modes are sensitive to adsorbate/metal interactions, accurate, and easily obtainable in-situ or operando. While they are the gold standards for characterizing single-crystals and large nanoparticles, analogous spectra for highly dispersed heterogeneous catalysts consisting of single-atoms and ultra-small clusters are lacking. Here, we combine data-based approaches with physics-driven surrogate models to generate synthetic IR spectra from first-principles. We bypass the vast combinatorial space of clusters by determining viable, low-energy structures using machine-learned Hamiltonians, genetic algorithm optimization, and grand canonical Monte Carlo calculations. We obtain first-principles vibrations on this tractable ensemble and generate single-cluster primary spectra analogous to pure component gas-phase IR spectra. With such spectra as standards, we predict cluster size distributions from computational and experimental data, demonstrated in the case of CO adsorption on Pd/CeO~2~(111) catalysts, and quantify uncertainty using Bayesian Inference. We discuss extensions for characterizing complex materials towards closing the materials g

Who reads Deducing Subnanometer Cluster Size and Shape Distributions of Heterogeneous Supported Catalysts?

Author

Vinson Liao; Maximilian Cohen; Yifan Wang; Dionisios G. Vlachos

Publisher

Springer Science and Business Media LLC

Published

2023

Language

EN

Field

Biochemistry, Genetics and Molecular Biology (Life Sciences)