廉价ts-1中不同钛物种在丙烯环氧化反应中的作用研究-study on the role of different titanium species in the epoxidation of propylene in cheap ts - 1.docxVIP

廉价Ts．1中不同钛物种在丙烯环氧化反应中的作用研究Study on the Effect of Different Titanium Species in Low-·cost TS--1 Zeolite for Propylene EpoxidationAbstractTitanium silicalite(TS—l、possess unique catalytic properties in oxidation reactions under mild conditions，especially with the use of hydrogen peroxide(H202)as the oxidant．It is commonly believed that the isolated titanium species in the framework of the TS-1 zeolite is the active center for the selective oxidation。However，the role of the nonframework Tispecies，especially that of amorphous Ti species in the epoxidation reactions is still debated． Different synthetic methods may result in the formation of different titanium species．which increases the complexity of the research．Therefore，a systematic study on the function of thedifferent titanium species in titanium silicalite(TS-1、is highly required．The low-cost TS—l zeolites with different titanium species were synthesized andcharacterized by ultraviolet visible(uv．Vis)diffuse reflectance spectroscopies，ultraviolet (UV)一Raman，pyridine adsorption Fourier-transform infrared(Py—IR)and NH3一TPD method． The roles of different Ti species in TS一1 samples have been investigated by gaschromatography-Raman spectrometry(GC—Raman)during the propylene epoxidation process． By building the correlation among the concentration of framework Ti species，the amount ofactive intermediate Ti-OOH(02)，the conversion of propylene and the yield of PO，the influence of the different titanium species to the Ti-OOH(rj上)and the PO was investigated．The results give evidence that the framework titanium species iS the active center，andthe concentration of framework Ti species iS positively realted to the amount of activeintermediate Ti-OOH(oz、．The presence of extraframework anatase Ti02 species iS harmful topropylene epoxidation reaction because of its ability of decomposing H202 solution． Furthermore，the Py-lR and NH3一TPD results reveal that the extraframework Ti species are more acidic and should be mainly