Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States.
J Org Chem. 2012 Jan 6;77(1):143-59. doi: 10.1021/jo201490y. Epub 2011 Dec 5.
A systematic study of the preparation of porphyrins with extended conjugation by meso,β-fusion with polycyclic aromatic hydrocarbons (PAHs) is reported. The meso-positions of 5,15-unsubstituted porphyrins were readily functionalized with PAHs. Ring fusion using standard Scholl reaction conditions (FeCl(3), dichloromethane) occurs for perylene-substituted porphyrins to give a porphyrin β,meso annulated with perylene rings (0.7:1 ratio of syn and anti isomers). The naphthalene, pyrene, and coronene derivatives do not react under Scholl conditions but are fused using thermal cyclodehydrogenation at high temperatures, giving mixtures of syn and anti isomers of the meso,β-fused porphyrins. For pyrenyl-substituted porphyrins, a thermal method gives synthetically acceptable yields (>30%). Absorption spectra of the fused porphyrins undergo a progressive bathochromic shift in a series of naphthyl (λ(max) = 730 nm), coronenyl (λ(max) = 780 nm), pyrenyl (λ(max) = 815 nm), and perylenyl (λ(max) = 900 nm) annulated porphyrins. Despite being conjugated with unsubstituted fused PAHs, the β,meso-fused porphyrins are more soluble and processable than the parent nonfused precursors. Pyrenyl-fused porphyrins exhibit strong fluorescence in the near-infrared (NIR) spectral region, with a progressive improvement in luminescent efficiency (up to 13% with λ(max) = 829 nm) with increasing degree of fusion. Fused pyrenyl-porphyrins have been used as broadband absorption donor materials in photovoltaic cells, leading to devices that show comparatively high photovoltaic efficiencies.
本文报道了通过与多环芳烃(PAHs)的中-β融合来扩展卟啉共轭的方法。5,15-未取代卟啉的中位置可通过 PAHs 进行易功能化。使用标准的 Scholl 反应条件(FeCl3,二氯甲烷)进行环融合,可得到带有苝环的卟啉β,中稠合环(顺式和反式异构体的比例为 0.7:1)。萘、并五苯和蔻的衍生物在 Scholl 条件下不反应,但在高温下通过热环脱氢反应进行融合,得到中-β稠合卟啉的顺式和反式异构体混合物。对于芘基取代卟啉,热法可获得可接受的合成产率(>30%)。融合卟啉的吸收光谱在一系列萘基(λmax=730nm)、蔻基(λmax=780nm)、芘基(λmax=815nm)和苝基(λmax=900nm)稠合卟啉中发生逐渐红移。尽管与未取代的稠合 PAHs 共轭,但β,中稠合卟啉比母体非稠合前体更具可溶性和可加工性。芘基稠合卟啉在近红外(NIR)光谱区域显示出强荧光,随着融合程度的增加,荧光效率逐渐提高(最大λ=829nm 时高达 13%)。稠合芘基-卟啉已被用作光伏电池中的宽带吸收供体材料,导致器件具有相对较高的光伏效率。