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Direct hydroxylation of aromatics with a mixture of H2 and O2 gases over Fe- and Pd-incorporated zeolites

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The hydroxylation of benzene and phenol with in-situ-generated oxidant was performed under mild reaction conditions over the bicatalytic system which has dual abilities of direct H2O2 generation and the hydroxylation activity by combining Pd-zeolite with redox zeolites such as TS-1, Ti-MCM-41, V-MCM-41 and Fe-zeolite. The amount of H2O2 formed directly from H2 and O2 increases with increasing Pd loading over zeolite up to 0.6% and subsequently decreases slightly as the Pd loading increases. The optimum amount of H2O2 produced is 6.4 mmol. Over Pd/HBEA + Fe/Y, when H2 : O2 = 40 : 40 ml/min is supplied, phenol conversion increases from 4.6% at 2 h to 13.6% at 8 h with high catechol selectivity in the range of 65–79%. The hydroxylation activities over redox catalyst with H2O2 are compared. Hydroxylation activity is improved by encapsulating FePc onto Y zeolite. In terms of TON, FePc/Y exhibits 3.5 times higher capacity than Fe/Y.


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