2D sp2 Carbon-Conjugated Porphyrin Covalent Organic Framework for Cooperative Photocatalysis with TEMPO.,Angewandte Chemie International Edition

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2D sp2 Carbon-Conjugated Porphyrin Covalent Organic Framework for Cooperative Photocatalysis with TEMPO.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-03-12 , DOI: 10.1002/anie.202000723
Ji-Long Shi ₁ , Rufan Chen ₁ , Huimin Hao ₁ , Cheng Wang ₁ , Xianjun Lang ₁

Affiliation

2D covalent organic frameworks (COFs) are receiving ongoing attention in semiconductor photocatalysis. Herein, we present a photocatalytic selective chemical transformation by combining sp2 carbon-conjugated porphyrin-based covalent organic framework (Por-sp2 c-COF) photocatalysis with TEMPO catalysis illuminated by 623 nm red light-emitting diodes (LEDs). Highly selective conversion of amines into imines was swiftly afforded in minutes. Specifically, the π-conjugation of porphyrin linker leads to extensive absorption of red light; the sp2 -C=C- double bonds linkage ensures the stability of Por-sp2 c-COF under high concentrations of amine. Most importantly, we found that crystalline framework of Por-sp2 c-COF is pivotal for cooperative photocatalysis with (2,2,6,6-tetramethylpiperidin-1-yl)oxyl (TEMPO). This work foreshadows that the outstanding hallmarks of COFs, particularly crystallinity, could be exploited to address energy and environmental challenges by cooperative photocatalysis.

中文翻译：

TEMPO协同光催化的2D sp2碳缀合的卟啉共价有机骨架。

二维共价有机骨架（COF）在半导体光催化领域正受到持续关注。在这里，我们通过结合sp2碳共轭卟啉基共价有机框架（Por-sp2 c-COF）光催化和623 nm红色发光二极管（LED）照明的TEMPO催化，提出光催化选择性化学转化。在几分钟内迅速实现了胺向亚胺的高度选择性转化。具体地说，卟啉接头的π共轭导致红光的大量吸收；sp2-C = C-双键连接确保了在高浓度胺下Por-sp2 c-COF的稳定性。最重要的是，我们发现Por-sp2 c-COF的晶体骨架对于与（2,2,6,6-四甲基哌啶-1-基）氧基（TEMPO）的协同光催化至关重要。

更新日期：2020-03-12

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