Korean Journal of Chemical Engineering, Vol.34, No.7, 1914-1923, 2017
Heterogeneous amino acid-based tungstophosphoric acids as efficient and recyclable catalysts for selective oxidation of benzyl alcohol
A series of organic-inorganic composite catalysts, prepared by modifying tungstophosphoric acid (TPA; H3PW12O40) with different amino acids such as phenylalanine (Phe), alanine (Ala), and glycine (Gly) were synthesized. The physicochemical and acidic properties of these (MH)xH3-xPW12O40 (M=Phe, Ala, and Gly; x=1-3) composite materials were characterized by a variety of different analytical and spectroscopic techniques, namely TGA, XRD, FTIR, XPS, and NMR, and exploited as heterogeneous catalysts for selective oxidation of benzyl alcohol (BzOH) with hydrogen peroxide (H2O2). Among them, the [PheH]H2PW12O40 catalyst exhibited the best oxidative activity with an excellent BzOH conversion of 99.0% and a desirable benzaldehyde (BzH) selectivity of 99.6%. Further kinetic studies and model analysis by response surface methodology (RSM) revealed that the oxidation of BzOH with H2O2 follows a second-order reaction with an activation energy of 56.7 kJ·mol-1 under optimized experimental variables: BzOH/H2O2 molar ratio=1 : 1.5mol/mol, amount of catalyst=6.1 wt%, reaction time (x3)=3.8 h, and amount of water (x4)=30.2mL.
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