Keggin type molybdovanadophosphoric heteropoly acids, H3+nPMo12-nVnO40(n=1-3), were prepared by a novel environmentally benign method, and their catalytic performances were evaluated via hydroxylation of benzene to phenol with hydrogen peroxide as oxidant in a mixed solvent of glacial acetic acid and acetonitrile. Various reaction parameters, such as reaction time, reaction temperature, ratio of benzene to hydrogen peroxide, concentration of aqueous hydrogen peroxide, ratio of glacial acetic acid to acetonitrile in solvent and catalyst con- centration, were changed to obtain an optimal reaction conditions. H3+nPMo12-nVnO40(n=1-3) are revealed to be highly efficient catalyst for hydroxylation of benzene. In case of H5PMo10V2O40, a conversion of benzene of 34.5% with the selectivity of phenol of 100% can be obtained at the optimal reaction conditions.
The bimetal-bearing (CePt or LaPt) 12-tungstophosphoric acid (H3PW12O40 (PW)) catalysts supported on dealuminated USY zeolite (DUSY) were prepared by impregnation and characterized by XRD, BET, IR, and H2-chemisorption. Their catalytic activities were tested in the hydroisomerization of n-heptane with a continuous atmospheric fixed-bed reactor. After the steam treatment combined with the acid leaching, as well as the supporting with PW and the bimetals, the DUSY support retains the Y zeolite porosity and the PW well keeps its Keggin structure in catalysts. The doping of Ce into the catalysts enhances the dispersion of Pt on the catalyst surface. The Pt-bearing PW catalysts doped with Ce or La, especially Ce, exhibit much higher catalytic activity and selectivity than the catalysts without dopants at lowered reaction temperatures. At the optimal reaction conditions, i.e., the reaction temperature of 250℃ and WHSV of 1.4 h1, the catalyst with a Pt loading of 0.4%, PW loading of 10% and a molar ratio of Ce to Pt of 15:1 shows a conversion of n-heptane of 70.3% with a high selectivity for isomerization products of 94.1%.
WEI RuiPing1,2, GU YanBo1 & WANG Jun1 1 State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemistry and Chemical Engineering, Nanjing Uni- versity of Technology, Nanjing 210009, China