Preface to the First Edition

The RSC Catalysis Book Series has been publishing books focused on many aspects of catalysis since the 1970’s, but to date there has not been a book in the series that has solely focused on computational modeling of heterogeneous catalysis. The importance of computational catalysis has grown over the past two decades and there are an increasing number of young researchers entering this area. The aim of this book is to provide a pedantic presentation of select methods in computational catalysis. Our hope is that this book will prove useful to the graduate student or other researchers already familiar with computer simulations, but interested in applying specific methods to their catalysis research.

In the first chapter, Lars Grabow (University of Houston) discusses the screening of catalysts through the use of first-principles methods. Using density functional theory (DFT), key descriptors and scaling relationships can be identified and incorporated with an appropriate microkinetic model. Such an approach allows for the rapid screening of materials based on DFT calculations.

One of the key challenges in modeling catalysts is the need to predict the appropriate surface structure at reaction conditions. Jason Bray and Bill Schneider (Notre Dame) present a detailed example of a first-principles based thermodynamic model for oxygen adsorption on Pt surfaces. They derive a cluster expansion model, fit to DFT data, which allows for exploring the complex heterogeneous oxygen phase as a function of temperature and oxygen partial pressure using Monte Carlo simulations. These types of simulations also allow for exploring surface reaction behavior under reaction conditions.

In the third chapter, Kuan-Yu Yeh and Mike Janik (Penn State University) present a detailed review of DFT-based modeling of electrocatalysts. The electrochemical interface is one of the more challenging environments to model, and several different models that vary in accuracy and computational expense are presented. With these methods potential dependent reaction energies and barriers can be calculated for elementary steps. Specific examples are presented to illustrate how to apply these various models.

Another important area of computational catalysis is modeling the metal/oxide interface, which is discussed by Tom Senftle, Adri van Duin, and Mike Janik (Penn State). They review several applications, such as the water–gas shift reaction and hydrocarbon activation, and the stability of oxide phases, that applies both DFT-based calculations and charge transfer potentials.

Thomas Manz (New Mexico State University) and David Sholl (Georgia Tech) present the details and application of their charge partitioning method called the density derived electrostatic and chemical (DDEC) method. This method can be used to obtain chemically relevant atomic charges and spin moments for both periodic and non-periodic systems. Such output can assist in understanding the relationship between electronic structure and material properties, and can also be used as input into the fitting of classical potentials.

The last two chapters present details of two classical potentials that incorporate charge transfer. Adri van Duin and co-workers present the details of the ReaxFF potential and discuss several applications. Susan Sinnott and coworkers from the University of Florida present the charge optimized many body (COMB) potentials and its application to molecules and metals on oxide surfaces.

We appreciate the efforts made by the authors to present a wide range of important methods in computational catalysis at a level that can benefit a researcher learning these methods for their research.

Aravind Asthagiri

Michael J. Janik