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作为降解光氧催化剂的氧定制的结构-属性关系

Blaine G McCarthy¹, Ryan M Pearson¹, Chern-Hooi Lim¹

¹Department of Chemistry , Colorado State University , Fort Collins , Colorado 80523-1872 , United States.

Journal of the American Chemical Society

|March 8, 2018

概括

研究人员开发了可见光吸收的有机光反氧化催化剂 (PCs),具有可调节的聚合特性. 这些氧衍生物显示出各种有机合成的潜力,包括聚合物生产.

科学领域:

有机化学
摄影化学
聚合物化学

背景情况:

可见的吸光有机光电还原催化剂 (PC) 对于可持续的合成至关重要.
氧衍生物已被证明是有机PCs,但它们的结构-性质关系需要进一步阐明.

研究的目的:

设计和合成可见光吸收有机光反氧催化剂的新型素衍生物.
调查这些衍生物的结构-属性关系,重点关注激发状态属性和催化活性.
在有机催化转移基聚合 (O-ATRP) 中评估它们的性能.

主要方法:

使用了实验和计算分析的组合,包括时间依赖密度函数理论 (TD-DFT) 建模.
合成和表征N-aryl和核心修饰的素衍生物.
在白光照射下对聚甲酸 (PMMA) 合成的O-ATRP进行了评估.

主要成果:

开发出具有与过渡金属PC可比的激发状态降解潜力的素衍生物.
证明N-aryl替代剂影响电荷转移激发状态,而核心修改使不同的CT激发状态.
所有衍生品都适合O-ATRP,产生具有受控分子量和低分散性的PMMA.
确定强烈的可见光吸收和三重激发状态的减少潜力是持续聚合控制的关键.

结论:

基于素的有机PC的已确定的结构性质关系.
这些发现使得用于O-ATRP和其他光催化反应的有机PC能够合理设计.
氧衍生物为光氧化催化剂提供了可行的替代品.

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