An Efficient and Recyclable Sn-Based Phosphotungstic Acid with Tunable Brønsted/Lewis Acidity for Selective Oxidation of Benzyl Alcohol
AUTOR(ES)
Zhou, Yousheng; Mei, Xingyu; Cai, Zhe; Wang, Qing; Duanmu, Jiahui; Kai, Ouyang; Zhang, Haijiang; Tang, Xiujuan; Han, Xiaoxiang
FONTE
J. Braz. Chem. Soc.
DATA DE PUBLICAÇÃO
2021-01
RESUMO
A series of metal ion (M = Sn2+, Fe3+, Ni2+, Co2+, Ag+, Cu2+) exchanged tungstophosphoric acid (H3PW12O40; TPA) catalysts with tunable Brønsted/Lewis acidity were synthesized and exploited for the oxidation of benzyl alcohol (BzOH) to benzaldehyde (BzH) using hydrogen peroxide (H2O2) as oxidant. The structure of these M-TPA composite salts was also characterized by Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), thermogravimetric analyses (TGA) and solid-state 31P nuclear magnetic resonance (NMR) probe molecule method. Among these M-TPAs, the Sn1/2H2PW12O40 catalyst, which presented strong Brønsted acidity, the synergistic effect of Brønsted/Lewis and pseudo-liquid characteristic property, exhibited excellent catalytic activity and durability with 98.2% of BzH selectivity and 95.1% of BzH yield. The optimal conditions for the oxidation of BzOH optimized by response surface methodology (RSM) were as follows: n(BzOH)/n(H2O2) = 1:1.25, catalyst amount of 5.5 wt.% to BzOH, water amount of 17 mL, 3.3 h of reaction time, and temperature 393 K. Moreover, further kinetic study confirmed that the reaction order was 2.64 and the activation energy was 21.75 kJ mol-1.
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