锌卟啉共价有机框架和共轭微孔聚合物的光催化可逆加成-断裂链转移聚合

莫依天; 刘衣铭; 王晓鸽; 童瑜洁; 魏瑶; 马玉国

doi:10.11777/j.issn1000-3304.2023.23134

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锌卟啉共价有机框架和共轭微孔聚合物的光催化可逆加成-断裂链转移聚合

研究论文 | 更新时间：2023-09-25

- 锌卟啉共价有机框架和共轭微孔聚合物的光催化可逆加成-断裂链转移聚合
  增强出版
- Zinc Porphyrin-based Covalent Organic Framework and Conjugated Microporous Polymer as Heterogeneous Photocatalysts for Reversible Addition-fragmentation Chain Transfer Polymerization
- 高分子学报 2023年54卷第10期页码：1521-1532
- 作者机构：
  
  北京分子科学国家实验室北京大学高分子化学与物理教育部重点实验室软物质科学与工程中心化学与分子工程学院北京 100871
- 作者简介：
  
  E-mail: ygma@pku.edu.cn
- 基金信息：
  
  国家自然科学基金(基金号 52273001)
- DOI：10.11777/j.issn1000-3304.2023.23134
  中图分类号：
- 纸质出版日期：2023-10-20，
  
  网络出版日期：2023-09-01，
  
  收稿日期：2023-05-16，
  
  录用日期：2023-06-30
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莫依天,刘衣铭,王晓鸽等.锌卟啉共价有机框架和共轭微孔聚合物的光催化可逆加成-断裂链转移聚合[J].高分子学报,2023,54(10):1521-1532.

Mo Yi-tian,Liu Yi-ming,Wang Xiao-ge,et al.Zinc Porphyrin-based Covalent Organic Framework and Conjugated Microporous Polymer as Heterogeneous Photocatalysts for Reversible Addition-fragmentation Chain Transfer Polymerization[J].ACTA POLYMERICA SINICA,2023,54(10):1521-1532.
莫依天,刘衣铭,王晓鸽等.锌卟啉共价有机框架和共轭微孔聚合物的光催化可逆加成-断裂链转移聚合[J].高分子学报,2023,54(10):1521-1532. DOI： 10.11777/j.issn1000-3304.2023.23134.

Mo Yi-tian,Liu Yi-ming,Wang Xiao-ge,et al.Zinc Porphyrin-based Covalent Organic Framework and Conjugated Microporous Polymer as Heterogeneous Photocatalysts for Reversible Addition-fragmentation Chain Transfer Polymerization[J].ACTA POLYMERICA SINICA,2023,54(10):1521-1532. DOI： 10.11777/j.issn1000-3304.2023.23134.

摘要

制备基于锌卟啉共价有机框架(COFs)和共轭微孔聚合物(CMPs)的异相光催化剂用于催化光诱导电子转移可逆加成-断裂链转移(PET-RAFT)聚合. 这些光催化剂可以高效地将电子转移到链转移剂制备得到具有窄分子量分布(<1.20)和高链端保真度的聚丙烯酰胺和聚丙烯酸酯，聚合速率高于具有相似构建单元的卟啉或镍卟啉光催化体系. 同时，对于锌卟啉COF和CMP材料，不同堆积模式和共轭程度影响了光催化剂的结构和光物理性质. 比较两者的结构性质和催化性能，说明了在光控聚合中选择高效催化性质的构建单元是催化剂设计的关键要素. 此外，相比于COF，CMP光催化剂具有更高的化学稳定性，可以被有效分离并循环使用. 这项工作阐明了多孔有机聚合物在光控聚合中的设计要素，为实现异相的光聚合提供重要借鉴.

Abstract

Zinc porphyrin-based covalent organic framework (COF) DhaTph-Zn-COF and conjugated microporous polymer (CMP) DhaTph-Zn-CMP as heterogeneous photocatalysts were prepared to activate photoinduced electron transfer-reversible addition-fragmentation chain transfer (PET-RAFT) polymerization under broad-range wavelengths. They could efficiently transfer electrons to chain transfer agents to synthesize polyacrylamides and polyacrylates with controllable molecular weight

narrow molecular weight distribution (

1.20)

and high chain-end fidelity. The apparent polymerization rate constants were 0.0522 h

-1

and 0.0621 h

-1

for polymerization of

-dimethacrylamide with 2.5 mg/mL DhaTph-Zn-COF or DhaTph-Zn-CMP

respectively

under yellow light irradiation. The different stacking patterns and the degree of conjugation for the freshly prepared COF and CMP materials affected structure and photophysical properties

such as crystallinity

specific surface area

band gap

fluorescence lifetime

charge transfer resistance

etc

. Although DhaTph-Zn-COF had an ordered stacking with better electron transfer properties

their similar catalytic properties indicated that the stacking patterns were not the primary factor to enhance the performance of photocatalysts. Meanwhile

the difference in photocatalytic polymerization of metalloporphyrin-based COFs displayed that a building block (zinc porphyrin) with high photocatalytic efficiency in a homogenous system is vital to the design of the heterogeneous photocatalysts for polymerization. Besides

the stability of photocatalysts directly affected the efficiency of catalytic cycles. Compared with DhaTph-Zn-COF

the amorphous DhaTph-Zn-CMP showed more robust chemical stability after several rounds of polymerization and could be used at least five times. The reduced efficiency of DhaTph-Zn-COF after recycling resulted from the loss of active components. The scanning electron microscopy (SEM) revealed the morphological difference between the COF and CMP photocatalysts. Better stability could be credited to the tight-packed particles formed by the disorderly stacked structure

which avoided the destruction by external factors such as monomers

solvents

and stir. This work provides insights into the design factors of heterogeneous POP photocatalysts for photopolymerization and promotes the development of efficient semiconductors and heterogeneous photocatalysts.

关键词

共价有机框架共轭微孔聚合物异相光催化剂光诱导电子转移可逆加成-断裂链转移聚合

Keywords

Covalent organic frameworksConjugated microporous polymersHeterogeneous photocatalystsPhotoinduced electron transfer reversible addition-fragmentation chain transfer polymerization

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