Investigation of catalytic activities of new heterogeneous molybdenum catalysts in epoxidation of olefins

Investigation of catalytic activities of new heterogeneous molybdenum catalysts in epoxidation of olefins
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新型多相钼催化剂在烯烃环氧化中的催化活性研究

DOI:
10.1016/j.molcata.2009.09.020
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发表时间:
2010
影响因子:
--
通讯作者:
M. Masteri‐Farahani
M. Masteri‐Farahani
中科院分区:
化学2区
文献类型:
--
作者:
M. Masteri‐Farahani

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将介孔分子筛MCM-41依次与3-氨基丙基三甲氧基硅烷和乙酰丙酮(acac)共价接枝,得到改性MCM-41(acacAmpMCM-41)。该材料与氨基酸的反应,例如丙氨酸、苯丙氨酸、亮氨酸、异亮氨酸、组氨酸和缬氨酸提供相应的支撑氨基酸席夫碱配体。随后与双(乙酰丙酮)二氧代钼(VI)反应生成通过丙基链间隔基负载在 MCM-41 上的各种钼络合物。采用 FT-IR、原子吸收光谱、粉末 X 射线衍射 (XRD) 和 BET 氮气吸附-解吸方法对这些材料进行了表征。 XRD 和 BET 分析表明,在接枝实验过程中,载体的结构特性得到了保留。所得材料成功催化环辛烯、环己烯、1-己烯和1-辛烯与叔丁基过氧化氢(TBHP)环氧化成相应的环氧化物。
The mesoporous molecular sieve MCM-41 was covalently grafted with 3-aminopropyl trimethoxysilane and acetyl acetone (acac) successively to give modified MCM-41 (acacAmpMCM-41). Reaction of this material with amino acids, e.g. alanine, phenyl alanine, leucine, isoleucine, histidine and valine afforded the corresponding supported amino acid Schiff base ligands. Subsequent reaction with bis (acetylacetonato)dioxomolybdenum(VI) lead to various molybdenum complexes supported on MCM-41 through propyl chain spacer. Characterization of these materials was carried out with FT-IR, atomic absorption spectroscopy, powder X-ray diffraction (XRD) and BET nitrogen adsorption–desorption methods. The XRD and BET analyses revealed that textural properties of support were preserved during the grafting experiments. The resultant materials successfully catalyzed the epoxidation of cyclooctene, cyclohexene, 1-hexene and 1-octene with tert-butyl hydroperoxide (TBHP) to the corresponding epoxides.