CATIVIC: Parametric quantum chemistry package for catalytic reactions: I

Abstract

A quantum chemistry package for catalytic reactions, referred to as CATIVIC and based on simulation techniques of parametric Hamiltonians, is presented. We describe in detail the computational procedures for modeling adsorption on a catalytic substrate, especially the parameterization scheme using examples of atomic Al and AlOX bonds (X ϭ H, N, O, Si, Fe) for atomic and molecular parameters. The code features are illustrated with the adsorption of NO on models of ZSM-5 zeolite doped with Fe.

Application of computational methods to catalytic systems

“…It means that Al atoms, in spite of having long separation distances, maintain important interactions, and their presence influences the electronic charge concentration at other adsorption sites. Similar results were reported in previous work [79] with different clusters and smaller charged systems. In addition, long-range interactions in the computation of adsorbate-substrate interactions have been proposed to be relevant in molecular dynamics simulations [87].…”

“…Some of the ideas presented above have been implemented in our program CATIVIC [17,[79][80][81]. This is the first version of a code specially tailored for catalytic reactions that offers several tools to facilitate their modeling.…”

“…The methodology for optimization of atomic and molecular parameters using standard parametric functionals are described elsewhere [79,85]. We are working on more sophisticated functionals that depend on functional expansions [78] and lead to a more involved reparameterization.…”

Modeling formation of molecules in the interstellar medium by radical reactions with polycyclic aromatic hydrocarbons

“…All calculations were performed with the parametric CATIVIC code [16], a modified version of MINDO/SR [22] employed to model catalytic and molecular systems. This method is based on simulation techniques to mimic the total energy functional using basic parametric functionals [23].…”

“…Recently, calculations with DFT [15] and CAT-IVIC [16] ) radicals with coronene was studied [19,20], with the adsorption of radicals or the formation of neutral molecules. Calculations of chemisorption and recombination of organic fragments on the coronene surface leading to the formation of glycine and aniline were also reported [21].…”