Abstract: Quantum Chem. Symp. 29 (1995) 221-234

C. Pisani and U. Birkenheuer
Embedded-Cluster Approach to the Study of Catalytic Reactions in Zeolite Cavities
Int. J. Quantum Chem., Quantum Chem. Symp. 29 (1995) 221-234.


This communication compares three different approaches to the study of ammonia protonation in acidic chabazite: the cluster model, the supercell model, and the embedded cluster model. In all cases, the Hartree-Fock approximation has been adopted, and a minimal Slater-type orbital basis set has been used. To calculate the interaction energies of ammonia by means of the periodic model, the CRYSTAL92 program has been used. The same program has been employed to generate the Madelung field in which a molecular cluster may be embedded. It also provides the reference solution necessary for the embedded cluster model calculations, which in turn have been performed with the EMBED93 program. All three techniques lead to similar interaction energies; however, the embedded cluster approach allows for the most natural way of performing the present adsorption study. Only those atoms which are chemically involved in the interaction have to be treated explicitly, while the rest of the system, though chemically inert, is treated as a consistently described background acting on the adsorption complex. The present investigation suggests that cooperative interaction between molecules trapped in the cavities of zeolites is of crucial importance for the protonation of ammonia to occur.