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作 者:周放[1] 朱玉超[1] 周永华[1] 叶红齐[1] 金一粟[1]
出 处:《石油学报(石油加工)》2014年第1期24-31,共8页Acta Petrolei Sinica(Petroleum Processing Section)
基 金:国家自然科学基金项目(21006129);中央高校基本科研业务费(721500170)资助
摘 要:提出了一种无需涂层就可获得较高Pd负载量,且分散性好的Pd/堇青石催化剂的制备方法。对堇青石载体及孔道表面进行氨基官能团化,然后负载金属Pd。利用傅里叶红外光谱(FT-IR)、X射线衍射(XRD)、透射电镜(TEM)、电感耦合等离子体发射光谱(ICP-AES)以及滴定方法表征载体表面及负载的Pd粒子。结果表明,在3-氨丙基三乙氧基硅烷(APTS)与载体质量比0.015、80℃条件下对堇青石改性12h,所得载体负载金属Pd,可得到最高的Pd粒子分散度,制备的Pd/堇青石催化剂表现出对苯乙烯加氢反应最高的活性。采用N-氨乙基-γ-氨丙基三甲氧基硅烷(TPED)改性堇青石载体,Pd粒子负载量能提高1倍以上,但Pd粒子的分散度降低。此外堇青石的酸预处理不利于其氨基官能团化和Pd粒子在其上的分散。A simple method to achieve high Pd dispersion as well as improved Pd loading on cordierite monolith without washcoat layer was reported.The cordierite monolith was functionalized with aminesilanes,and then Pd was loaded.Fourier transform infrared spectroscopy (FT-IR),X-ray diffraction (XRD),transmission electron microscopy (TEM),inductively coupled plasma atomic emission spectroscopy (ICP-AES) and titration were used to characterize the functionalized monolith and the loaded Pd particles.Results showed that the highest dispersion of Pd particles could be obtained by functionalizing monolith by 3-aminopropyltrimethoxysilane (APTS) with the mass ratio of APTS to support of 0.015 at 80℃ for 12 h.The obtained Pd/cordierite catalyst exhibited the highest activity for styrene hydrogenation reaction.The utilization of N-[3-(trimethoxysilyl)-propylethylene] diamine (TPED) in functionalizing cordierite monolith could improve the Pd loading amount more than one fold,while the dispersion of Pd particles decreased.In addition,the acid pretreatment of monolith was not beneficial to aminesilane functionalizing of monolith and the dispersion of Pd particles on it.
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