Oxidation of Phenol with Nitrous Oxide. Role of Acidity of Zeolite Catalysts

The gas-phase oxidation of phenol with nitrous oxide on zeolite catalysts may be of interest as an alternative method of obtaining dihydroxybenzenes (DHB). Previously, there were found catalysts that provide high selectivity of the reaction toward the sum of all three isomers of DHB (85–90 %). The present work is aimed at the optimization of the catalyst in terms of regulation of the regioselectivity of the reaction. The effectof thermal-steam treatment (TST) of zeolites on their catalytic properties was studied. NMR and IR data showed that the increase in temperature of TST in the range 550–750 °C leads to a 5-fold decrease in the concentration of Bronsted acid sites of the zeolite and to a 2–3-fold increase in the number of α-sites that are responsible for the activity in the oxidation with nitrous oxide. It was found that the variation in the temperature of TST is a powerful instrument to influence the selectivity of the reaction toward individual isomers of DHB. The decrease in the acidity of a zeolite leads to a change in the ratio of isomers in favor of pyrocatechol. The paper discusses the causes of this phenomenon and its relation to the deactivation of the catalyst.

dihydroxybenzenes, oxidation of phenol, nitrous oxide, zeolites, acidity of zeolites, hydroquinone, pyrocatechol, resorcinol

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