制备了不同金属改性的钛硅分子筛样品M-TS-1 (M=V,Cr,Mn,Fe,Co,Ni,Cu,Zn,Cd,La,负载量为1％),并研究了其催化丁二烯环氧化反应的性能.结果表明,V,Cr,Mn的加入导致H2O2无效分解,因而在丁二烯环氧化反应中表现出较高的H2O2转化率和较低有效利用率;Fe,Co,Ni以及稀土金属La均在一定程度上促进了TS-1对H2O2的有效利用;Cu,Zn抑制了H2O2的转化,使得H2O2转化率和有效利用率都较低;Cd有效提高了TS-1的催化活性,H2O2转化率和有效利用率均接近100％.采用X射线衍射、N2吸附-脱附、X射线光电子能谱、傅里叶变换红外光谱等手段表征了上述各金属的改性对TS-1骨架结构以及Ti活性中心周围电子环境的影响.结果表明,各M-TS-1样品的骨架结构都仍保持原有的MFI构型,但是TS-1中Ti活性中心周围的电子环境受到来自各种金属的不同程度影响,关联催化活性时没有特定的规律性.
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