An active site model and the catalytic activity mechanism of the new fullerene-based catalyst-(eta(2)-C-60)Pd(PPh3)(2)

A theoretical description of the adsorption of acetylene molecules on palla dium-phosphine fullerene complexes has been developed based on the results of ab initio quantum chemical calculations. This process can be considered as a model of the preliminary stage of C=C triple bond scission in acetylen e compounds. The HF, LSDA, BPW91, B3LYP, and MP2 levels of theory with diff erent basis sets were employed in the theoretical predictions. The calculat ions were performed for the cluster model of the active site. Based on the performed calculations and experimental data one can conclude that the prel iminary interactions of the catalyst with the substrate facilitates the int eraction of the complex substrate-catalyst with H-2 by decreasing the energ y barrier. The theoretical results indicate that it is possible to explain this effect without including solvent interactions into the model system.