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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(5):1279-1283
We report a new family of multifunctional liquid‐crystalline porphyrin‐core dendrimers that have coumarin functional groups around the porphyrin core. Porphyrin metalation strongly affects the photophysical properties, and therefore ZnII and CuII derivatives have also been prepared. All the synthesized dendrimers form a nematic discotic mesophase. Their high tendency for homeotropic alignment makes these dendrimers excellent candidates for device applications, owing to their easy processability, spontaneous alignment between electrodes, and self‐healing of defects because of their dynamic nature. The charge mobility values of these materials are the highest ever reported for a nematic discotic phase. Moreover, these values are similar to the highest values reported for ordered columnar mesophases, and this shows that a supramolecular organization in columns is not necessary to achieve high charge mobility. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(12):3377-3381
A ruthenium complex, porphyrin sensitizer, fullerene acceptor molecular pentad has been synthesized and a long‐lived hole–electron pair was achieved in aqueous solution by photoinduced multistep electron transfer: Upon irradiation by visible light, the excited‐state of a zinc porphyrin (1ZnP*) was quenched by fullerene (C60) to afford a radical ion pair, 1,3(ZnP.+‐C60.−). This was followed by the subsequent electron transfer from a water oxidation catalyst unit (RuII) to ZnP.+ to give the long‐lived charge‐separated state, RuIII‐ZnP‐C60.−, with a lifetime of 14 μs. The ZnP worked as a visible‐light‐harvesting antenna, while the C60 acted as an excellent electron acceptor. As a consequence, visible‐light‐driven water oxidation by this integrated photosynthetic model compound was achieved in the presence of sacrificial oxidant and redox mediator. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(31):9239-9243
Main‐group complexes are shown to be viable electrocatalysts for the H2‐evolution reaction (HER) from acid. A series of antimony porphyrins with varying axial ligands were synthesized for electrocatalysis applications. The proton‐reduction catalytic properties of TPSb(OH)2 (TP=5,10,15,20‐tetra(p ‐tolyl)porphyrin) with two axial hydroxy ligands were studied in detail, demonstrating catalytic H2 production. Experiments, in conjunction with quantum chemistry calculations, show that the catalytic cycle is driven via the redox activity of both the porphyrin ligand and the Sb center. This study brings insight into main group catalysis and the role of redox‐active ligands during catalysis. 相似文献