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Ionic ammonium and anilinium based polymolybdate hybrid catalysts for olefin epoxidation
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-07-09 , DOI: 10.1016/j.apcata.2018.07.001
Barbara Bożek , Patrícia Neves , Wiesław Łasocha , Anabela A. Valente

Ionic polymolybdate hybrids (IPH) are interesting catalysts for liquid phase olefin epoxidation with tert-butylhydroperoxide; (tbhp), e.g. conversion of terpenic and fatty acid methyl ester (FAME) components of biomass to useful bio-products. IPHs may be easily prepared, under clean, mild, aqueous phase conditions. The type of organic precursor and the synthesis conditions influence the structural features of the IPHs. In this work, IPH epoxidation catalysts possessing one- (1-D) or two-dimensional (2-D) structures were investigated, which included the new materials 1-D methylammonium ammonium trimolybdate [Mo3O10⋅CH3NH3·NH4] (1) and 2-D bis(2,5-dimethylanilinium) pentamolybdate [Mo5O16·2(NH3C6H3(CH3)2)] (4) with solved structures, and 1-D bis(3,5-dimethylanilinium) trimolybdate [Mo3O10·2(NH3C6H3(CH3)2)] (2), bis(4-methylanilinium) trimolybdate [Mo3O10·2(NH3C6H4CH3)] (3), 2-D bis(anilinium) pentamolybdate [Mo5O16·2(NH3C6H5)] (5), bis(4-methylanilinium) pentamolybdate [Mo5O16·2(NH3C6H4CH3)] (6) and bis(4-ethylanilinium) pentamolybdate [Mo5O16·2(NH3C6H4C2H5)] (7). Systematic characterisation and catalytic studies helped gain insights into structure-activity relationships. The best-performing catalyst (2) was effective for the epoxidation of the FAMEs such as, methyl oleate which gave 92% methyl 9,10-epoxyoctadecanoate yield, at 99% conversion, at 70 °C. The reaction conditions (temperature, type of cosolvent and oxidant) influenced the catalytic reaction. Catalytic performance in consecutive batch runs was steady, and the structural features were essentially preserved.



中文翻译:

离子铵和苯胺基聚钼酸酯杂化催化剂用于烯烃环氧化

离子型多钼酸盐杂化物(IPH)是用叔丁基氢过氧化物液相烯烃环氧化的有趣催化剂。(t bhp),例如将生物质中的萜烯和脂肪酸甲酯(FAME)组分转化为有用的生物产品。在干净,温和的水相条件下,可以轻松制备IPH。有机前体的类型和合成条件会影响IPH的结构特征。在这项工作中,IPH环氧化催化剂具有单(1- d)或二维(2-d)的结构进行了研究,其中包括新材料1-d甲基铵铵trimolybdate [沫3 ö 10 ⋅CH 3 NH 3 · NH 4 ](1)和2-D双(2,5-二甲基苯铵)五钼酸盐[Mo 5 O 16 ·2(NH 3 C 6 H 3(CH 32)](4)和具有溶解结构的1-D bis(3, 5-二甲基苯铵)三钼酸盐[Mo 3 O 10 ·2(NH 3 C 6 H 3(CH 32)](2),双(4-甲基苯铵)三钼酸盐[Mo 3 O 10 ·2(NH 3 C 6 H 4 CH 3)](3),2-D双钼酸双(苯胺)[Mo 5 O 16 ·2(NH 3 C 6 H 5)](5),双钼酸双(4-甲基苯胺)[Mo 5 O 16 ·2(NH 3 C 6 H 4) CH 3)](6)和钼酸双(4-乙基苯铵)[Mo 5 O 16 ·2(NH 3 C 6 H 4 C 2 H 5)](7)。系统的表征和催化研究有助于深入了解结构-活性关系。表现最佳的催化剂(2)对于FAMEs(例如油酸甲酯)的环氧化有效,在70°C时,转化率99%时,可得到92%的9,10-环氧十八烷酸甲酯。反应条件(温度,助溶剂和氧化剂的类型)影响了催化反应。连续分批运行中的催化性能稳定,并且基本上保留了结构特征。

更新日期:2018-07-09
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