We have studied the oxidative addition of chlorobenzene on gold, gold/palladium and palladium zeolites using DFT calculations. The 34T quantum cluster of Au4-, Au2Pd2- and Pd4-ZSM-5 zeolites were optimized with M06L/6-31G(d,p)+LanL2DZ calculations. The charge transfer occurs from the zeolite framework to Au4, Au2Pd2 and Pd4 clusters, which enhance the reactivity of the clusters. The Au/Pd alloy cluster has asymmetric charge distribution leading to its high reactivity. Thus, the reactivity is in the order of Au2Pd2- ZSM-5 > Pd4-ZSM-5 > Au4-ZSM-5. The Au2Pd2- ZSM-5 zeolite provides the highly active site with the activation energy barrier of only 8.2 kcal/mol. The bimetallic Au/Pd zeolite is preferable for stabilizingnot only the adsorption complexes, but also the transition state. Thus, bimetallic Au/Pd zeolite has been predicted to be effective for the C-Cl activation.

Oxidation of chlorobenzene using Au-, Au/Pd- and Pd-ZSM-5 zeolite catalysts: A DFT study

248th National Meeting (2014)

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