|About this Abstract
||2018 TMS Annual Meeting & Exhibition
||Computational Thermodynamics and Kinetics
||Computationally Tractable Methods for Studying the Roles of Water Molecules on Aqueous Phase Heterogeneous Catalysis
||Tianjun Xie, Rachel B. Getman
|On-Site Speaker (Planned)
Understanding reaction mechanisms is crucial to catalyst design; however, this understanding is limited for reactions in the aqueous phase due to uncertainties in how fluctuations in the structure of liquid water influence catalytic thermodynamics and kinetics. We use a combination of density functional theory (DFT) and classical molecular dynamics (cMD) to simulate the structure of liquid water and investigate its influence on the catalytic thermodynamics and kinetics of Pt-catalyzed aqueous phase reforming (APR) of glycerol (C3H8O3). Exploring the comprehensive reaction network, including various reaction branches of glycerol APR requires a significant number of calculations. We present strategies for calculating catalytic thermodynamics and kinetics using accurate yet computationally tractable methods, which take advantage of linear scaling relationships (LSRs) for estimating binding energies and Brønsted–Evans–Polanyi (BEP) relations for estimating reaction barriers, coupled with methods developed by our group for inexpensively interrogating the structure of liquid water at the water-catalyst interface.
||Planned: Supplemental Proceedings volume