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通过原子转移自由基聚合(ATRP)对共聚物进行后修饰以应用于非均相不对称席夫碱催化。

Post-Modification of Copolymers Obtained by ATRP for an Application in Heterogeneous Asymmetric Salen Catalysis.

机构信息

Centre National de la Recherche Scientifique (CNRS), Institut de Chimie Moléculaire et des Matériaux d'Orsay, UMR 8182, Université Paris-Saclay, 420 Bâtiment, 91405 Orsay, France.

Laboratoire de Physique de la Matière Condensée, Centre National de la Recherche Scientifique (CNRS), Ecole Polytechnique, Institut Polytechnique de Paris, 91120 Palaiseau, France.

出版信息

Molecules. 2022 Jul 21;27(14):4654. doi: 10.3390/molecules27144654.

DOI:10.3390/molecules27144654
PMID:35889526
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9319095/
Abstract

Copolymers are valuable supports for obtaining heterogeneous catalysts that allow their recycling and therefore substantial savings, particularly in the field of asymmetric catalysis. This contribution reports the use of two comonomers: Azido-3-propylmethacrylate (AZMA) bearing a reactive azide function was associated with 2-methoxyethyl methacrylate (MEMA), used as a spacer, for the ATRP synthesis of copolymers, and then post-functionalized with a propargyl chromium salen complex. The controlled homopolymerization of MEMA by ATRP was firstly described and proved to be more controlled in molar mass than that of AZMA for conversions up to 63%. The ATRP copolymerization of both monomers made it possible to control the molar masses and the composition, with nevertheless a slight increase in the dispersity (from 1.05 to 1.3) when the incorporation ratio of AZMA increased from 10 to 50 mol%. These copolymers were post-functionalized with chromium salen units by click chemistry and their activity was evaluated in the asymmetric ring opening of cyclohexene oxide with trimethylsilyl azide. At an equal catalytic ratio, a significant increase in enantioselectivity was obtained by using the copolymer containing the largest part of salen units, probably allowing, in this case, the more favorable bimetallic activation of both the engaged nucleophile and electrophile. Moreover, the catalytic polymer was recovered by simple filtration and re-engaged in subsequent catalytic runs, up to seven times, without loss of activity or selectivity.

摘要

共聚物是获得异相催化剂的有价值的载体,允许它们回收利用,从而实现实质性的节约,特别是在不对称催化领域。本贡献报告了两种共聚单体的使用:带有反应性叠氮基官能团的叠氮基-3-丙基甲基丙烯酸酯(AZMA)与 2-甲氧基乙基甲基丙烯酸酯(MEMA)结合使用,用作间隔基,用于 ATRP 合成共聚物,然后用炔丙基铬席夫碱络合物进行后功能化。首先描述了 MEMA 的 ATRP 均聚,并且证明其在摩尔质量上比 AZMA 更可控,转化率高达 63%。两种单体的 ATRP 共聚使得可以控制摩尔质量和组成,但是当 AZMA 的掺入比从 10 增加到 50mol%时,分散度略有增加(从 1.05 增加到 1.3)。这些共聚物通过点击化学进行铬席夫碱单元的后功能化,并在环己烯氧化物与三甲基硅基叠氮化物的不对称开环反应中评估了它们的活性。在相等的催化比下,使用含有最大部分席夫碱单元的共聚物可以获得显著提高的对映选择性,这可能允许在这种情况下,参与的亲核试剂和亲电试剂的双金属活化更为有利。此外,通过简单过滤回收催化聚合物,并在随后的七个催化循环中重新使用,而没有活性或选择性的损失。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/53ecd487b5d7/molecules-27-04654-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/988d8c298782/molecules-27-04654-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/7f24e8dd7131/molecules-27-04654-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/70f4dbc02dd5/molecules-27-04654-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/dafc68a99bdb/molecules-27-04654-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/6987d17f77a6/molecules-27-04654-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/59254cb2b448/molecules-27-04654-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/50376f10fef4/molecules-27-04654-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/b75c9b3eb778/molecules-27-04654-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/236ff96b6515/molecules-27-04654-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/53ecd487b5d7/molecules-27-04654-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/988d8c298782/molecules-27-04654-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/7f24e8dd7131/molecules-27-04654-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/70f4dbc02dd5/molecules-27-04654-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/dafc68a99bdb/molecules-27-04654-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/6987d17f77a6/molecules-27-04654-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/59254cb2b448/molecules-27-04654-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/50376f10fef4/molecules-27-04654-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/b75c9b3eb778/molecules-27-04654-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/236ff96b6515/molecules-27-04654-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/274e/9319095/53ecd487b5d7/molecules-27-04654-sch003.jpg

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