Synthesis of heterogeneous metathesis catalysts for the development of sustainable processes

Selena Gutiérrez-Flores, L. García-Barrera, Daniel Zárate-Saldaña, Jorge A. Cruz-Morales
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Abstract

In recent decades, it has been tried to develop processes that involve the use of catalysts that can be recovered from the reaction medium, to make them green and sustainable. Approximately, 90 % of all processes in chemistry and petrochemicals use heterogeneous catalysts. In this sense, the supported heterogeneous catalysts present advantages in the purification of the products and the reduction of costs. In the present work, the synthesis of a new heterogeneous supported catalyst, highly active in the metathesis reaction, based on a ruthenium-alkylidene complex, was carried out. The new catalyst was obtained by anchoring of dichloro[1,3-bis(2,4,6-trimethylphenyl)-2-imidazolidinylidene](benzylidene)(tricyclohexylphosphine)ruthenium (II) (second generation Grubbs) in various silylated polymeric gels, based on 2-norbornene-5,6-dicarboxylic anhydride (NDA) and cis-cyclooctene (CO) cross-linked with various percentages of 3-aminopropyltriethoxysilane (APTES) (5%, 15%, 100%). The new heterogeneous catalyst was successfully used in the depolymerization reaction via metathesis of natural rubber from Oaxaca (HNO), using 1-octene as CTA; observing the formation of liquid oligomers, achieving a decrease in molecular weight from 137.941 g/mol to 297 g/mol; proving, in this way, its high effectiveness.
多相复分解催化剂的合成及其可持续工艺的发展
近几十年来,人们一直在尝试开发涉及使用可从反应介质中回收的催化剂的工艺,以使其绿色和可持续。大约90%的化学和石油化工过程使用多相催化剂。从这个意义上说,负载型多相催化剂在纯化产物和降低成本方面具有优势。本文以钌-烷基烯配合物为原料,合成了一种在复分解反应中具有高活性的新型多相负载催化剂。以2-降冰片烯-5,6-二羧基酸酐(NDA)和顺式环烯(CO)为原料,与不同比例的3-氨基丙基三乙基氧基硅烷(APTES)(5%、15%、100%)交联,将二氯[1,3-二(2,4,6-三甲基苯基)-2-咪唑烷](苄基)(三环己基膦)钌(II)(第二代Grubbs)锚定在不同的硅基化聚合物凝胶中,得到了新的催化剂。以1-辛烯为CTA,成功地将新型多相催化剂用于瓦哈卡天然橡胶(HNO)的复分解解聚反应;观察液体低聚物的形成,分子量从137.941 g/mol降低到297 g/mol;通过这种方式证明了它的高效性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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