Heterogeneous amino acid-based tungstophosphoric acids as efficient and recyclable catalysts for selective oxidation of benzyl alcohol

被引:5
|
作者
Han, Xiaoxiang [1 ]
Kuang, Yingying [1 ]
Xiong, Chunhua [1 ]
Tang, Xiujuan [2 ]
Chen, Qing [1 ]
Hung, Chin-Te [3 ]
Liu, Li-Li [3 ]
Liu, Shang-Bin [3 ]
机构
[1] Zhejiang Gongshang Univ, Dept Appl Chem, Hangzhou 310018, Peoples R China
[2] Zhejiang Gongshang Univ, Coll Environm Sci & Engn, Hangzhou 310018, Peoples R China
[3] Acad Sinica, Inst Atom & Mol Sci, Taipei 10617, Taiwan
关键词
Amino Acid; Heteropolyacid; Benzaldehyde; Oxidation of Alcohol; Process Optimization; Kinetic Model; SOLVENT-FREE OXIDATION; PHOSPHOTUNGSTIC ACID; AEROBIC OXIDATION; PALMITIC ACID; IONIC LIQUIDS; SILICA; KEGGIN; MCM-41; NMR; HETEROPOLYACIDS;
D O I
10.1007/s11814-017-0097-y
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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) (x) H3-x PW12O40 (M=Phe, Ala, and Gly; x=1-3) composite materials were characterized by a variety of different analytical and spectroscopic techniques, namely TGA, XRD, FT-IR, 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 center dot mol(-1) under optimized experimental variables: BzOH/H2O2 molar ratio=1 : 1.5 mol/mol, amount of catalyst=6.1 wt%, reaction time (x(3))=3.8 h, and amount of water (x(4))=30.2 mL.
引用
收藏
页码:1914 / 1923
页数:10
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