Theoretical & Computational Tools for Modeling of Energy Relevant Catalysis on Multiple Scales

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Multi-scale modeling of catalytic reaction-diffusion processes in nanoporous materials, particularly
in functionalized mesoporous silicananoparticles (MSN). This includes detailed quantum chemical analysis of reaction mechanisms, Langevin simulation of key diffusive dynamics, coarse-grained modeling of the overall reaction process and kinetics.

This project supports efforts in electronic structure theory and non-equilibrium statistical mechanical & multiscale modeling of complex catalytic chemical systems. The primary focus is on the development and application of methods that enable the study of condensed-phase chemistry and surface reaction phenomena, especially heterogeneous catalysis. Also of interest are solvent effects and homogeneous organometallic catalysis. Electronic structure theory efforts integrate development of fundamental theory, expanding the capability for accurate treatment of large systems of interest to USDOE BES, with optimal strategies for computational implementation within GAMESS. Theory development includes fragment molecular orbital, effective fragment molecular orbital and effective fragment potential approaches with applications to liquid-solid interfaces, and embedding methods for solid surfaces. Statistical mechanical and multiscale modeling studies also focus on catalytic reaction-diffusion phenomena and catalytic nanomaterials. This modeling often incorporates input from relevant electronic structure analyses. A core focus in this effort is on molecular-level and coarse-grained modeling the interplay between restricted transport and catalytic reaction in functionalized nanoporous materials. Another major effort is on the predictive molecular-level modeling of chemisorption and heterogeneous catalysis on metal surfaces and nanoclusters. In addition, our modeling explores the synthesis and stability of catalytic nanomaterials, currently focusing on metallic nanocrystals formed in the solution-phase or by deposition.

Au nanoclusters
Accelerated decay of 2D Au nanoclusters (NCs) on Au(111) due to mass transport via Au-S complex formation. Top: STM images. Lower left: NC area decay vs S coverage. Lower right: Au-S complexes enhancing decay. ChemPhysChem 2021, 22, 349.

 

PD Nanocubes
Surface-diffusion-mediated reshaping of Pd nanocubes. Top: Evolution tracked by TEM. Lower left: Theoretical energy variation vs extent of reshaping yielding an effective barrier. Lower right: KMC simulation. ACS Nano 2020, 14, 8551.

Principal Investigator: James Evans

Co-PIs: Mark Gordon, Klaus Ruedenberg, Theresa Windus

Staff Scientists: Da-Jiang Liu, Georg Schoendorff, Yong Han, Federico Zahariev

Post Doctoral Researcher: Andres Garcia 

Publications
Giuseppe M. J. Barca Colleen Bertoni Laura Carrington Dipayan Datta Nuwan DeSilva J. Emiliano Deustua Dmitri G. Fedorov Jeffrey R. Gour Anastasia O. Gunina Emilie Guidez Taylor Harville Stephan Irle Joe Ivanic Karol Kowalski Sarom S. Leang Hui Li Wei Li Jesse J. Lutz Ilias Magoulas Joani Mato Vladimir Mironov Hiroya Nakata Buu Q. Pham Piotr Piecuch David Poole Spencer R. Pruitt Alistair P. Rendell Luke B. Roskop Klaus Ruedenberg Tosaporn Sattasathuchana Michael W. Schmidt Jun Shen Lyudmila Slipchenko Masha Sosonkina Vaibhav Sundriyal Ananta Tiwari Jorge L. Galvez Vallejo Bryce Westheimer Marta Włoch Peng Xu Federico Zahariev Mark S. Gordon

Recent Developments in the General Atomic and Molecular Electronic Structure System

Journal of Chemical Physics, 2020