Abstract
Substitution of transition metals for either aluminum and/or phosphorus in the AlPO{sub 4}-11 framework is found to afford novel heterogeneous catalysts for liquid phase hydroxylation of phenol with hydrogen peroxide. AlPO{sub 4}-11 is more active than SAPO-11 and MgAPO-11 for phenol conversion to hydroquinone. The Bronsted acid sites of SAPO-11 and MgAPO-11 may promote the decomposition of hydrogen peroxide to water and oxygen, thus leading to lower phenol conversions. Substitution of divalent and trivalent metal cations, such as Fe, Co and Mn appears to significantly improve the conversion of phenol. The activity follows the order of FeAPO-11>FeMnAPO-11>CoAPO-11>MnAPO-11{much_gt}ALPO{sub 4}-11. FeAPO-11, FeMnAPO-11 and AlPO{sub 4}-11 give similar product selectivities of about 1:1 hydroquitione (HQ) to catechol (CT). MnAPO-11 and CoAPO-11 favor the production of catechol, particularly at low conversions. FeAPO-11 and TS-1 (titanium silicate with MFI topology) are comparable for the phenol conversions with TS-1 giving higher selectivities toward hydroquinone. The external surfaces of the catalysts plays a significant role in these oxidation reactions. MeAPO molecular sieves may be complementary to the metal silicalite catalysts for the catalytic oxidations in the manufacture of fine chemicals.
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