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Fully Conjugated Two‐Dimensional sp2‐Carbon Covalent Organic Frameworks as Artificial Photosystem I with High Efficiency
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2019-03-13 , DOI: 10.1002/anie.201901194
Yingjie Zhao 1 , Hui Liu 1 , Chenyu Wu 1 , Zhaohui Zhang 1 , Qingyan Pan 1 , Fan Hu 1 , Ruiming Wang 2 , Piwu Li 2 , Xiaowen Huang 2 , Zhibo Li 1
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2019-03-13 , DOI: 10.1002/anie.201901194
Yingjie Zhao 1 , Hui Liu 1 , Chenyu Wu 1 , Zhaohui Zhang 1 , Qingyan Pan 1 , Fan Hu 1 , Ruiming Wang 2 , Piwu Li 2 , Xiaowen Huang 2 , Zhibo Li 1
Affiliation
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The synthesis of fully conjugated sp2‐carbon covalent organic frameworks (COF) is extremely challenging given the difficulty of the formation of very stable carbon‐carbon double bonds (‐C=C‐). Here, we report the successful preparation of a 2D COF (TP‐COF) based on triazine as central planar units bridged by sp2‐carbon linkers through the ‐C=C‐ condensation reaction. High‐resolution‐transmission electron microscopy (HRTEM) clearly confirmed the tessellated hexagonal pore structure with a pore center‐to‐center distance of 2 nm. Powder X‐ray diffraction (PXRD) together with structural simulations revealed an AA stacking mode of the obtained layered structure. TP‐COF turned out to be an excellent semiconductor material with a LUMO energy of −3.23 eV and a band gap of 2.36 eV. Excitingly, this novel sp2‐carbon conjugated TP‐COF exhibited unprecedented coenzyme regeneration efficiency and can significantly boost the coenzyme‐assisted synthesis of l‐glutamate to a record‐breaking 97 % yield within 12 minutes.
中文翻译：
全共轭二维sp2-碳共价有机骨架作为高效的人工光系统I
鉴于很难形成非常稳定的碳-碳双键（-C = C-），完全共轭的sp 2-碳共价有机骨架（COF）的合成极具挑战性。在这里，我们报告了成功制备基于三嗪作为由sp 2桥接的中央平面单元的2D COF（TP-COF）通过-C = C-缩合反应的碳连接基。高分辨率透射电子显微镜（HRTEM）清楚地确认了棋盘格结构的六边形孔结构，孔中心距为2 nm。粉末X射线衍射（PXRD）与结构模拟一起显示了所获得的层状结构的AA堆积模式。TP-COF被证明是一种出色的半导体材料，其LUMO能量为-3.23 eV，带隙为2.36 eV。令人兴奋的是，这种新颖的sp 2-碳共轭TP-COF展现了前所未有的辅酶再生效率，可以在12分钟内显着提高辅酶辅助的l-谷氨酸的合成，达到创纪录的97％的收率。
更新日期：2019-03-13
中文翻译：
全共轭二维sp2-碳共价有机骨架作为高效的人工光系统I
鉴于很难形成非常稳定的碳-碳双键（-C = C-），完全共轭的sp 2-碳共价有机骨架（COF）的合成极具挑战性。在这里，我们报告了成功制备基于三嗪作为由sp 2桥接的中央平面单元的2D COF（TP-COF）通过-C = C-缩合反应的碳连接基。高分辨率透射电子显微镜（HRTEM）清楚地确认了棋盘格结构的六边形孔结构，孔中心距为2 nm。粉末X射线衍射（PXRD）与结构模拟一起显示了所获得的层状结构的AA堆积模式。TP-COF被证明是一种出色的半导体材料，其LUMO能量为-3.23 eV，带隙为2.36 eV。令人兴奋的是，这种新颖的sp 2-碳共轭TP-COF展现了前所未有的辅酶再生效率，可以在12分钟内显着提高辅酶辅助的l-谷氨酸的合成，达到创纪录的97％的收率。
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