Hasegawa Hiroko, Hirakawa Kazutaka
Department of Optoelectronics and Nanostructure Science, Graduate School of Science and Technology, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561, Japan.
Department of Optoelectronics and Nanostructure Science, Graduate School of Science and Technology, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561, Japan; Applied Chemistry and Biochemical Engineering Course, Department of Engineering, Graduate School of Integrated Science and Technology, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561, Japan; Cooperative Major in Medical Photonics, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561, Japan.
Spectrochim Acta A Mol Biomol Spectrosc. 2024 Mar 5;308:123765. doi: 10.1016/j.saa.2023.123765. Epub 2023 Dec 12.
Under visible light irradiation, water-insoluble P(V)porphyrins oxidized 1-benzyl-1,4-dihydronicotinamide (BNADH), a model compound for nicotinamide adenine dinucleotide, and diminished the typical absorption of BNADH at around 340 nm. A singlet oxygen quencher, sodium azide, partially inhibited photosensitized BNADH oxidation. This BNADH oxidation photosensitized by P(V)porphyrins in the presence of sodium azide can be explained by electron transfer oxidation from BNADH to the photoexcited P(V)porphyrins. The quantum yields of BNADH oxidation via electron transfer by these P(V)porphyrins were larger than those of a singlet oxygen mechanism. Redox potential measurements supported the electron transfer mechanism from a thermodynamic point of view, and fluorescence lifetime measurement also suggests this mechanism. The process of this electron transfer oxidation involves the radical formation of BNADH and the further reaction of this radical to the oxidized form (cationic form of BNADH). Analysis of the quantum yields of BNADH photooxidation by P(V)porphyrins suggests that the photoinduced electron transfer from BNADH to photoexcited P(V)porphyrins triggers the radical chain reaction of BNADH oxidation. The electron transfer rate coefficient and this efficiency were increased with an increase in the Gibbs energy of electron transfer from tryptophan to photoexcited P(V)porphyrins (-ΔG). However, the BNADH oxidation quantum yield via electron transfer decreased with an increase in the -ΔG of electron transfer. These results suggest that reverse electron transfer inhibits the decomposition of BNAD radicals. This assay using BNADH can be used to evaluate the photosensitizer activity of water-insoluble compounds. These P(V)porphyrins may be used as photosensitizers for photodynamic therapy in a relatively hydrophobic environment in cancer tissues.
在可见光照射下,水不溶性的聚(V)卟啉氧化了烟酰胺腺嘌呤二核苷酸的模型化合物1 - 苄基 - 1,4 - 二氢烟酰胺(BNADH),并使BNADH在340nm左右的典型吸收减弱。单线态氧猝灭剂叠氮化钠部分抑制了光敏性BNADH氧化。在叠氮化钠存在下,聚(V)卟啉光敏的这种BNADH氧化可以通过从BNADH到光激发的聚(V)卟啉的电子转移氧化来解释。这些聚(V)卟啉通过电子转移进行BNADH氧化的量子产率大于单线态氧机制的量子产率。氧化还原电位测量从热力学角度支持了电子转移机制,荧光寿命测量也表明了这一机制。这种电子转移氧化过程涉及BNADH的自由基形成以及该自由基与氧化形式(BNADH的阳离子形式)的进一步反应。对聚(V)卟啉光氧化BNADH的量子产率分析表明,从BNADH到光激发的聚(V)卟啉的光诱导电子转移引发了BNADH氧化的自由基链反应。电子转移速率系数和该效率随着从色氨酸到光激发的聚(V)卟啉的电子转移吉布斯自由能(-ΔG)的增加而增加。然而,通过电子转移的BNADH氧化量子产率随着电子转移的-ΔG增加而降低。这些结果表明反向电子转移抑制了BNAD自由基的分解。这种使用BNADH的测定方法可用于评估水不溶性化合物的光敏剂活性。这些聚(V)卟啉可在癌症组织相对疏水的环境中用作光动力疗法的光敏剂。