Selective epoxidation of propylene to propylene oxide with H2 and O2 over Au/Ti-MWW catalysts

被引:12
作者
Ren, Yingjie [1 ]
Xu, Le [1 ]
Zhang, Liyan [1 ]
Wang, Jianggan [1 ]
Liu, Yueming [1 ]
He, Mingyuan [1 ]
Wu, Peng [1 ]
机构
[1] E China Normal Univ, Dept Chem, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
关键词
catalysis; epoxidation; gold nanoparticles; oxidation; propylene; propylene oxide; Ti-MWW; titanosilicate; zeolites; VAPOR-PHASE EPOXIDATION; PROPENE EPOXIDATION; HIGHLY EFFICIENT; MOLECULAR-SIEVE; TI-MWW; GOLD; TITANOSILICATE; OXIDATION; HYDROGEN; REARRANGEMENT;
D O I
10.1351/PAC-CON-11-07-10
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Direct epoxidation of propylene to propylene oxide (PO) with H-2 and O-2 has been performed on bifunctional catalysts, Au nanoparticles supported on novel Ti-MWW titanosilicate (Au/Ti-MWW). In comparison to conventional Au/TS-1 catalysts, Au/Ti-MWW exhibited a similar phenomenon with respect to PO formation, that is, the PO selectivity increased with increasing Si/Ti ratio of titanosilicate. However, at optimized Ti contents corresponding to Si/Ti ratio > 140, the PO selectivity of Au/Ti-MWW catalysts was lower than 60 % in comparison to ca. 90 % achieved on Au/TS-1. A large number of boron species and defect-site-related hydroxyl groups contained in Ti-MWW were assumed to retard the desorption of PO from the channels or crystallite surface of zeolite, which favors side reactions such as over-oxidation and decomposition of PO. Poststructural rearrangement was then carried out on Ti-MWW with piperidine (PI) solution to improve effectively its hydrophobicity, leading to defect-less Re-Ti-MWW. This enhanced significantly the PO selectivity of Au/Re-Ti-MWW thus prepared, which reached as high as 92 % at Si/Ti ratio of 135. Au/Re-Ti-MWW(135) then gave the highest PO formation rate of 22.0 gPO kg(-1) h(-1).
引用
收藏
页码:561 / 578
页数:18
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