cis-Selective Acyclic Diene Metathesis Polymerization of α,ω-Dienes,Journal of the American Chemical Society

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cis-Selective Acyclic Diene Metathesis Polymerization of α,ω-Dienes
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-05-31 , DOI: 10.1021/jacs.3c03978
Samuel J Kempel ₁ , Ting-Wei Hsu ₁ , Jake L Nicholson ₁ , Quentin Michaudel _{1,

2}

Affiliation

The cis/trans stereochemistry of repeating alkenes in polymers provides a powerful handle to modulate the thermal and mechanical properties of these soft materials, but synthetic methods to precisely dictate this parameter remain scarce. We report herein a cis-selective acyclic diene metathesis (ADMET) polymerization of readily available α,ω-diene monomers with high functional group tolerance. Identification of a highly stereoselective cyclometalated Ru catalyst allowed the synthesis of a broad array of polymers with cis contents up to 99%. This platform was leveraged to study the impact of the cis geometry on the thermal and mechanical properties of polyalkenamers, including an ABA triblock copolymer synthesized via extension of a cis-rich telechelic polyoctenamer with d,l-lactide. These results suggest that cis-selective ADMET affords an efficient strategy to tune the properties of a variety of polymers.

中文翻译：

α,ω-二烯的顺式选择性无环二烯复分解聚合

聚合物中重复烯烃的顺式/反式立体化学为调节这些软材料的热性能和机械性能提供了强大的手段，但精确指示该参数的合成方法仍然很少。我们在此报道了具有高官能团耐受性的易于获得的α，ω-二烯单体的顺式选择性无环二烯复分解（ADMET）聚合。高度立体选择性环金属化 Ru 催化剂的鉴定允许合成一系列顺式含量高达 99% 的聚合物。利用该平台研究顺式几何形状对聚烯烃的热性能和机械性能的影响，包括通过用d , L-丙交酯延伸富顺式遥爪聚辛烯异构体合成的 ABA 三嵌段共聚物。这些结果表明顺式选择性 ADMET 提供了调节各种聚合物性能的有效策略。

更新日期：2023-05-31

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