Gao Zhe, Sharma Krishna K, Andres Angelo E, Walls Brandon, Boumelhem Fadel, Woydziak Zachary R, Peterson Blake R
Division of Medicinal Chemistry and Pharmacognosy, The Ohio State University Columbus OH 43210 USA
Department of Physical and Life Sciences, Nevada State College Henderson NV 89002 USA.
RSC Med Chem. 2022 Mar 7;13(4):456-462. doi: 10.1039/d1md00395j. eCollection 2022 Apr 20.
Fluorinated analogues of the fluorophore pyronin B were synthesized as a new class of amine-reactive drug-like small molecules. In water, 2,7-difluoropyronin B was found to reversibly react with primary amines to form covalent adducts. When this fluorinated analogue is added to proteins, these adducts undergo additional oxidation to yield fluorescent 9-aminopyronins. Irradiation with visible blue light enhances this oxidation step, providing a photochemical method to modify the biological properties of reactive amines. In living HeLa cells, 2,7-difluoropyronin B becomes localized in mitochondria, where it is partially transformed into fluorescent aminopyronins, as detected by spectral profiling confocal microscopy. Further excitation of these cells with the blue laser of a confocal microscope can depolarize mitochondria within seconds. This biological activity was only observed with 2,7-difluoropyronin B and was not detected with analogues such as pyronin B or 9-methyl-2,7-difluoropyronin B. This irradiation with blue light enhances the cellular production of reactive oxygen species (ROS), suggesting that increased ROS in mitochondria promotes the formation of aminopyronins that inactivate biomolecules critical for maintenance of mitochondrial membrane potential. The unique reactivity of 2,7-difluoropyronin B offers a novel tool for photochemical control of mitochondrial biology.
荧光团派若宁B的氟化类似物被合成为一类新型的胺反应性类药物小分子。在水中,发现2,7 - 二氟派若宁B与伯胺可逆反应形成共价加合物。当将这种氟化类似物添加到蛋白质中时,这些加合物会进一步氧化生成荧光9 - 氨基派若宁。用可见蓝光照射可增强这一氧化步骤,提供了一种光化学方法来改变反应性胺的生物学性质。在活的HeLa细胞中,2,7 - 二氟派若宁B定位于线粒体中,通过光谱分析共聚焦显微镜检测发现它在那里部分转化为荧光氨基派若宁。用共聚焦显微镜的蓝色激光进一步激发这些细胞可在几秒钟内使线粒体去极化。这种生物学活性仅在2,7 - 二氟派若宁B中观察到,而在派若宁B或9 - 甲基 - 2,7 - 二氟派若宁B等类似物中未检测到。这种蓝光照射增强了细胞内活性氧(ROS)的产生,表明线粒体中ROS的增加促进了氨基派若宁的形成,而氨基派若宁会使维持线粒体膜电位至关重要的生物分子失活。2,7 - 二氟派若宁B的独特反应性为线粒体生物学的光化学控制提供了一种新型工具。