Bifunctional Porphyrin Aluminum Catalyzed Copolymerization of Carbon Dioxide and Long Chain Terminal Epoxide

Ke-gong Liu; Shun-jie Liu; Pei-xin Fan; Ruo-yu Zhang; Xue-si Chen; Xian-hong Wang

doi:10.11777/j.issn1000-3304.2024.24185

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Bifunctional Porphyrin Aluminum Catalyzed Copolymerization of Carbon Dioxide and Long Chain Terminal Epoxide

Research Article | 更新时间：2026-05-12

- Bifunctional Porphyrin Aluminum Catalyzed Copolymerization of Carbon Dioxide and Long Chain Terminal Epoxide
- Acta Polymerica Sinica Vol. 56, Issue 2, Pages: 242-252(2025)
- 作者机构：
  
  1.中国科学院长春应用化学研究所生态环境高分子材料重点实验室长春 130022
  2.中国科学技术大学应用化学与工程学院合肥 230026
- 作者简介：
  
  Shun-jie Liu, E-mail: sjliu@ciac.ac.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2024.24185
  CLC：
- CSTR：32057.14.GFZXB.2024.7289
- Received：26 June 2024，
  
  Accepted：25 July 2024，
  
  Online First：14 November 2024，
  
  Published：20 February 2025
- 稿件说明：
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刘克共, 刘顺杰, 范培鑫, 张若禹, 陈学思, 王献红. 双功能卟啉铝催化二氧化碳与长链末端环氧化物共聚. 高分子学报, 2025, 56(2), 242-252

Liu, K. G.; Liu, S. J.; Fan, P. X.; Zhang, R. Y.; Chen, X. S.; Wang, X. H. Bifunctional porphyrin aluminum catalyzed copolymerization of carbon dioxide and long chain terminal epoxide. Acta Polymerica Sinica, 2025, 56(2), 242-252
刘克共, 刘顺杰, 范培鑫, 张若禹, 陈学思, 王献红. 双功能卟啉铝催化二氧化碳与长链末端环氧化物共聚. 高分子学报, 2025, 56(2), 242-252 DOI： 10.11777/j.issn1000-3304.2024.24185. CSTR： 32057.14.GFZXB.2024.7289.

Liu, K. G.; Liu, S. J.; Fan, P. X.; Zhang, R. Y.; Chen, X. S.; Wang, X. H. Bifunctional porphyrin aluminum catalyzed copolymerization of carbon dioxide and long chain terminal epoxide. Acta Polymerica Sinica, 2025, 56(2), 242-252 DOI： 10.11777/j.issn1000-3304.2024.24185. CSTR： 32057.14.GFZXB.2024.7289.

摘要

长链末端环氧化物(LCTE)由于大位阻侧基的存在，难以高选择性地与二氧化碳(CO

)共聚并得到高碳酸酯单元含量的聚合物. 本研究通过在卟啉meso苯环不同位置引入大位阻有机碱1

7-三叠氮双环[4.4.0

]

癸-5-烯(TBD)，设计了一系列双功能卟啉铝催化剂，旨在调控TBD

基团与铝中心的空间协同作用. 其中TBD连接在meso苯环间位上的催化剂

-4展现出最佳的催化效果，可高选择性(99%)催化1

2-环氧丁烷或1

2-环氧己烷与CO

完全交替共聚，制备得到分子量大于32 kg/mol的聚碳酸酯. 通过原位红外光谱对反应进行动力学研究证明该催化剂分子内协同的催化特征. 本文工作探究了双功能催化剂分子内催化位点的空间分布与所产生协同作用的关系，为LCTE/CO

高效交替共聚合成聚碳酸酯提供了一种新思路.

Abstract

Long chain terminal epoxide (LCTE)

due to the existence of large steric hindrance side groups

is more difficult to achieve high selectivity in obtaining polymers with high carbonate unit content through copolymerization with carbon dioxide (CO

). This work reported bifunctional catalysts with large steric hindrance organic base 1

‍5

‍7-triazo bicyclic [4.4.0

]

decane-5-ene (TBD) introduced into the meso-benzene ring of porphyrin

aiming to regulate the spatial synergistic effect between the anchored TBD and aluminum centers. Among them

the catalyst

-4 with TBD anchored at the meso-benzene ring's

meso

-position exhibited the best catalytic activity

which could selectively (99%) catalyze the alternating copolymerization of 1

2-epoxybutane or 1

2-epoxyhexane with CO

. Catalyst

-4 could prepare polymers with molecular we

ight higher than 32 kg/mol. The obtained polymer's glass transition temperature was lower than room temperature.

In situ

FTIR kinetic studies demonstrated the intramolecular synergistic effect in the designed catalysts. In summary

this work probed differences in the spatial distribution of intramolecular catalytic sites in bifunctional catalysts and the resulting synergistic effect

providing a way of efficiently synthesizing polycarbonate for LCTE/CO

copolymerization.

关键词

Keywords

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