Hollingsworth Javoris V, Bhupathiraju N V S Dinesh K, Sun Jirun, Lochner Eric, Vicente M Graça H, Russo Paul S
Department of Chemistry and Macromolecular Studies Group, Louisiana State University , Baton Rouge, Louisiana 70803, United States.
Department of Chemistry & Physics, University of St. Thomas , Houston, Texas 77006, United States.
ACS Appl Mater Interfaces. 2016 Jan 13;8(1):792-801. doi: 10.1021/acsami.5b10034. Epub 2016 Jan 4.
A facile approach using click chemistry is demonstrated for immobilization of metalloporphyrins onto the surface of silica-coated iron oxide particles. Oleic-acid stabilized iron oxide nanocrystals were prepared by thermal decomposition of iron(III) acetylacetonate. Their crystallinity, morphology, and superparamagnetism were determined using X-ray diffraction, transmission electron microscopy, and a superconducting quantum interference device. Monodisperse core-shell particles were produced in the silica-coating of iron oxide via microemulsion synthesis. Surface modification of these particles was performed in two steps, which included the reaction of silica-coated iron oxide particles with 3-bromopropyltrichlorosilane, followed by azido-functionalization with sodium azide. Monoalkylated porphyrins were prepared using the Williamson ether synthesis of commercially available tetra(4-hydroxyphenyl) porphyrin with propargyl bromide in the presence of a base. (1)H NMR and matrix-assisted laser desorption ionization confirmed the identity of the compounds. The prepared monoalkyne porphyrins were zinc-metalated prior to their introduction to azide-functionalized, silica-coated iron oxide particles in the click reaction. X-ray photoelectron spectroscopy, thermogravimetric analysis, and Fourier transform infrared spectroscopy were used to characterize the surface chemistry after each step in the reaction. In addition, particle size was determined using dynamic light scattering and microscopy. The presented methodology is versatile and can be extended to other photoreactive systems, such as phthalocyanines and boron-dipyrromethane, which may lead to new materials for optical, photonic, and biological applications.
展示了一种使用点击化学将金属卟啉固定在二氧化硅包覆的氧化铁颗粒表面的简便方法。通过乙酰丙酮铁(III)的热分解制备了油酸稳定的氧化铁纳米晶体。使用X射线衍射、透射电子显微镜和超导量子干涉装置确定了它们的结晶度、形态和超顺磁性。通过微乳液合成在氧化铁的二氧化硅包覆过程中制备了单分散的核壳颗粒。这些颗粒的表面改性分两步进行,包括二氧化硅包覆的氧化铁颗粒与3-溴丙基三氯硅烷反应,然后用叠氮化钠进行叠氮基官能化。使用市售的四(4-羟基苯基)卟啉与炔丙基溴在碱存在下通过威廉姆森醚合成制备单烷基化卟啉。1H NMR和基质辅助激光解吸电离证实了化合物的身份。在点击反应中将制备的单炔基卟啉引入叠氮基官能化的二氧化硅包覆的氧化铁颗粒之前,先将其锌金属化。使用X射线光电子能谱、热重分析和傅里叶变换红外光谱对反应各步骤后的表面化学进行表征。此外,使用动态光散射和显微镜测定颗粒尺寸。所提出的方法具有通用性,可扩展到其他光反应体系,如酞菁和硼二吡咯甲烷,这可能会产生用于光学、光子学和生物应用的新材料。