Abstract
A series of Brønsted-Lewis acidic catalysts, denoted RE-TPA (MyH3‒3yPW12O40; M=La, Ce, Pr, Nd, Sm; y = 1/3, 2/3, 1), prepared by incorporating rare earth (RE) metal cations as Lewis centers onto the superacidic tungstophosphoric acid (TPA), were characterized by XRD, FT-IR, TGA-DTA and NMR. In particular, their acidic properties were studied by Pyridine-IR and solid-state 31P NMR of adsorbed phosphorous probe molecule. The high catalytic activity for the RE-TPAs was found to invoke Brønsted-Lewis acid synergy. Among various catalysts examined for oxidation of benzyl alcohol (BzOH) with hydrogen peroxide, the Ce1/3H2PW12O40 was utilized to optimize the reaction conditions while nearly full BzOH conversion, and excellent bezaldehyde yield (98.2%) and selectivity (98.4%) could reach by response surface methodology (RSM). Additional recyclability and kinetic studies revealed that the RE-TPA catalysts are robust, reusable, and highly efficient for alcohols oxidation reaction with an apparent order of 2.5 and an active energy of 37.3kJ/mol.
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