Russian Chemical Bulletin p. 1071 - 1083 (1998)
Update date:2022-08-11
Topics:
Bruk
Oshanina
Kozlova
Temkin
Odintsov
The mechanism of synthesis of maleic and succinic anhydrides from acetylene and CO in the PdBr2 - LiBr - organic solvent catalytic system was studied using the procedure of advancement and discrimination of hypotheses. The hypotheses were obtained using the data bank on elementary steps and the Comb1 combinatorial program. The discrimination of the hypotheses was based on the data of NMR and IR spectroscopy, studies of isotope exchange, the role of potential organic intermediates, the kinetic isotope effect, and one-factor kinetic experiments. The most probable mechanism of synthesis of maleic anhydride includes insertion of acetylene and CO into the Pd - Pd bond of the Pd1 complex, which is formed from Pd11 at the initial step of the process. Succinic anhydride results from the intramolecular transformation of the hydride complex of palladium and maleic anhydride. The palladium hydride complexes detected in the contact solution apparently play the crucial role in the conjugation of oxidation, reduction, and addition type reactions.
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