Polymer Institute, Center of excellence GLYCOMED, Slovak Academy of Sciences, Dubravska cesta 9, 845 41 Bratislava 45, Slovakia.
J Fluoresc. 2012 Sep;22(5):1371-81. doi: 10.1007/s10895-012-1076-7. Epub 2012 Jun 24.
The adducts of simple chromophore 4-N,N-dimethylamino benzoic acid with 2,2,6,6-tetrametyl-4-hydroxy- or 4-amino-piperidine were examined as fluorescence probes (spin double sensors) to monitor radical processes. The links in the adducts were either an ester or amide group, and the sterically hindered amines were in the form of -NH, -NO• and -NOR. The spectral properties of the three related derivatives (esters or amides) were quite similar. The maxima of the absorption spectra were in the range of 295-315 nm, and the maximum of fluorescence was located in the range of 330-360 nm, depending on the polarity of the solvent. In polar solvents, a red-shifted fluorescence band at 460-475 nm was observed. The fluorescence of these derivatives was rather weak as compared to anthracene under the same conditions. The Stokes shift was large, as high as 6,000 cm(-1), indicating the formation of a twisted intra-molecular charge transfer (TICT) state. No large differences in Stokes shifts were observed in polymer matrices of poly(methyl methacrylate), polystyrene and poly(vinyl chloride). The extent of intramolecular quenching was expressed as Φ(NX)/Φ(NO) (X = H, NOR) and was in the range of 1-3 in solution and as high as 8 in polymer matrices. The low efficiency of intramolecular quenching limits the application of these new adducts as fluorescence probes for the monitoring of radical processes in solution but favors their application in polymer matrices.
将简单生色团 4-N,N-二甲基氨基苯甲酸与 2,2,6,6-四甲基-4-羟基-或 4-氨基-哌啶的加合物作为荧光探针(自旋双传感器)用于监测自由基过程。加合物的键合基团为酯基或酰胺基,位阻胺以-NH、-NO•和-NOR 的形式存在。三种相关衍生物(酯或酰胺)的光谱性质非常相似。吸收光谱的最大值在 295-315nm 范围内,荧光的最大值位于 330-360nm 范围内,这取决于溶剂的极性。在极性溶剂中,观察到在 460-475nm 处有红移的荧光带。与相同条件下的蒽相比,这些衍生物的荧光相当弱。Stokes 位移很大,高达 6000cm-1,表明形成了扭曲的分子内电荷转移(TICT)态。在聚甲基丙烯酸甲酯、聚苯乙烯和聚氯乙烯的聚合物基质中,Stokes 位移没有明显差异。分子内猝灭的程度表示为 Φ(NX)/Φ(NO)(X = H,NOR),在溶液中范围为 1-3,在聚合物基质中高达 8。分子内猝灭效率低限制了这些新加合物作为荧光探针在溶液中监测自由基过程的应用,但有利于它们在聚合物基质中的应用。