用无金属催化剂通过非共价相互作用绿色合成聚ε-己内酯

IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Green Chemistry Pub Date : 2024-11-19 DOI:10.1039/D4GC04411H
Shweta Sagar, Priyanku Nath, Shiva Lall Sunar, Aranya Ray, Mridula Choudhary, Alok Sarkar, Saurabh K. Singh and Tarun K. Panda
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引用次数: 0

摘要

研究了无金属引发剂N,N′-二丁基-N,N,N′,N′-四甲基乙烷1,2-溴化二铵[nBuMe2NCH2CH2NnBuMe2]Br2 (DBTMEDA)Br2催化ε-己内酯(CL)的开环聚合(ROP)。催化剂(DBTMEDA)Br2在温和的条件下促进聚合,没有任何外部引发剂。聚合被证明是在一个可控的和生活的方式,生产pcl精确控制分子量高达50 kDa与窄的多分散性。密度泛函理论(DFT)计算表明,DBTMEDA阳离子与ε-CL羰基之间的C-H⋯O型非共价相互作用参与了单体活化步骤。值得注意的是,DBTMEDA也可以很容易地回收和重复使用长达六个连续循环,而催化活性没有明显下降。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Green synthesis of poly ε-caprolactone using a metal-free catalyst via non-covalent interactions†

Green synthesis of poly ε-caprolactone using a metal-free catalyst via non-covalent interactions†

The ring-opening polymerization (ROP) of ε-caprolactone (CL) catalyzed by a metal-free initiator N,N′-dibutyl-N,N,N′,N′-tetramethylethane1,2-diammonium bromide [nBuMe2NCH2CH2NnBuMe2]Br2 (DBTMEDA)Br2 has been investigated. The catalyst (DBTMEDA)Br2 promotes polymerization under mild conditions without any external initiator. Polymerization was demonstrated in a controlled and living manner, producing PCLs with a precisely controlled molecular weight of up to 50 kDa with narrow polydispersity. Density Functional Theory (DFT) calculations indicated the involvement of a C–H⋯O type non-covalent interaction between DBTMEDA cations and the carbonyl group of ε-CL in the monomer activation step. Remarkably, DBTMEDA can also be easily recovered and reused for up to six consecutive cycles without an appreciable decrease in catalytic activity.

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来源期刊
Green Chemistry
Green Chemistry 化学-化学综合
CiteScore
16.10
自引率
7.10%
发文量
677
审稿时长
1.4 months
期刊介绍: Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.
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