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Selective and Rapid Light-Induced RAFT Single Unit Monomer Insertion in Aqueous Solution.
Macromolecular Rapid Communications ( IF 4.6 ) Pub Date : 2019-11-10 , DOI: 10.1002/marc.201900478
Yanyan Zhou 1 , Zhengbiao Zhang 1 , Cassandra M Reese 2 , Derek L Patton 2 , Jiangtao Xu 3 , Cyrille Boyer 3 , Almar Postma 4 , Graeme Moad 4
Affiliation  

The photocatalyst Zn(II) meso-tetra(4-sulfonatophenyl)porphyrin (ZnTPPS) is found to substantially accelerate visible-light-initiated (red, yellow, green light) single unit monomer insertion (SUMI) of N,N-dimethylacrylamide into the reversible addition-fragmentation chain transfer (RAFT) agent, 4-((((2-carboxyethyl)thio)carbonothioyl)thio)-4-cyanopentanoic acid (RAFT1 ), in aqueous solution. Thus, under irradiation with red (633 nm) or yellow (593 nm) light with 50 mpm (moles per million mole of monomer) ZnTPPS at 30 °C, the rate enhancement provided by photoinduced energy or electron transfer (PET) is ≈sevenfold over the rate of direct photoRAFT-SUMI (without catalyst), which corresponds to achieving full and selective reaction in hours versus days. Importantly, the selectivity, as judged by the absence of oligomers, is retained. Under green light at similar power, higher rates of SUMI are also observed. However, the degree of enhancement provided by PET-RAFT-SUMI over direct photoRAFT-SUMI as a function of catalyst concentration is less and some oligomers are formed.

中文翻译:

选择性和快速光诱导的RAFT单体在水溶液中的插入。

发现光催化剂Zn(II)内四(4-磺酰基苯基)卟啉(ZnTPPS)大大促进了N,N-二甲基丙烯酰胺的可见光引发的(红色,黄色,绿色)单单元单体插入(SUMI)水溶液中的可逆加成-断裂链转移(RAFT)剂4-(((((2-羧乙基)硫代)羰基硫酰)硫基)-4-氰基戊酸(RAFT1)。因此,在30°C下以50 mpm(摩尔/百万摩尔单体的摩尔数)ZnTPPS照射红色(633 nm)或黄色(593 nm)的光时,由光致能量或电子转移(PET)提供的速率增强约为七倍超过直接photoRAFT-SUMI(不含催化剂)的速率,相当于在数小时内相对于数天即可实现完全和选择性反应。重要的是,保留了通过不存在低聚物来判断的选择性。在类似功率的绿灯下,还可以观察到较高的SUMI率。但是,PET-RAFT-SUMI相对于直接photoRAFT-SUMI所提供的增强程度随催化剂浓度而变小,并且形成了一些低聚物。
更新日期:2019-11-11
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