Center for Electrochemistry, Chemistry and Biochemistry Department, The University of Texas at Austin, Austin, Texas 78712, USA.
J Am Chem Soc. 2011 Jun 8;133(22):8633-45. doi: 10.1021/ja2010219. Epub 2011 May 12.
Synthesis of the C(8) BODIPY monomers, dimers, and trimers, a C(8) polymer, and N(8) aza-BODIPY monomer and dimer was carried out. Methyl and mesityl C(8)-substituted monomers, dimers, and trimers were used. Dimers, trimers, and polymer were formed chemically through the β-β (2/6) positions by oxidative coupling using FeCl(3). A red shift of the absorbance and fluorescence is observed with addition of monomer units from monomer to polymer for C(8) dyes. The aza-BODIPY dye shows red-shifted absorbance and fluorescence compared with the C(8) analogue. Cyclic voltammetry shows one, two, and three one-electron waves on both reduction and oxidation for the monomer, dimer, and trimer, respectively, for the C(8) BODIPYs. The separation for the reduction peaks for the C(8) dimers is 0.12 V compared with 0.22 V for the oxidation, while the trimers show separations of 0.09 V between reduction peaks and 0.13 V for oxidation peaks. The larger separations between the second and third peaks, 0.25 V for the oxidation and 0.2 V for the reduction, are consistent with a larger energy to remove or add a third electron compared with the second one. The BODIPY polymer shows the presence of many sequential one-electron waves with a small separation. These results provide evidence for significant electronic interactions between different monomer units. The aza-BODIPY dye shows a reduction peak 0.8 V more positive compared to the C(8) compound. Aza-BODIPY dimer shows the appearance of four waves in dichloromethane. The separation between two consecutive waves is around 0.12 V for reduction compared with 0.2 V for oxidation, which is comparable with the results for the C(8) dyes. Electrogenerated chemiluminescence (ECL) of the different species was obtained, including weak ECL of the polymer.
合成了 C(8) BODIPY 单体、二聚体和三聚体、C(8) 聚合物以及 N(8) 氮杂-BODIPY 单体和二聚体。使用了甲基和均三甲基取代的 C(8) 单体、二聚体和三聚体。通过使用 FeCl(3)进行氧化偶联,二聚体、三聚体和聚合物通过β-β(2/6)位置化学形成。对于 C(8)染料,随着单体单元从单体到聚合物的添加,观察到吸光度和荧光的红移。与 C(8)类似物相比,氮杂-BODIPY 染料显示出吸光度和荧光的红移。循环伏安法显示单体、二聚体和三聚体在还原和氧化时分别有一个、两个和三个单电子波。对于 C(8) BODIPYs,C(8) 二聚体的还原峰分离为 0.12 V,而氧化峰为 0.22 V,而三聚体的还原峰之间的分离为 0.09 V,氧化峰为 0.13 V。氧化峰和还原峰之间的第二和第三峰之间较大的分离,氧化峰为 0.25 V,还原峰为 0.2 V,这与与第二个相比,去除或添加第三个电子的能量更大一致。BODIPY 聚合物显示出许多具有小分离的连续单电子波的存在。这些结果为不同单体单元之间存在显著的电子相互作用提供了证据。氮杂-BODIPY 染料的还原峰比 C(8) 化合物正 0.8 V。氮杂-BODIPY 二聚体在二氯甲烷中显示出四个波的出现。与氧化相比,还原时两个连续波之间的分离约为 0.12 V,与 C(8) 染料的结果相当。获得了不同物种的电致化学发光(ECL),包括聚合物的弱 ECL。