中孔洞氧化石墨烯奈米粒子表面吸附大氣中之氧氣及水氣在光譜上的影響及應用

Abstract

本研究利用中孔洞氧化石墨烯奈米粒子 (Mesoporous graphene oxide nanoparticles, MGNs) 表面吸附氧氣與水氣，探討在光照下與表面吸附氣體之相互作用。MGNs表面存在碳自由基，並在照光後透過單線氧捕捉劑 (1,3-Diphenylisobenzofuran, DPBF) 證實其可以作為一個光敏劑，在照光後具有與氧氣能量交換的能力，並產生單線態氧 (Singlet state oxygen, 1O2)。此外，利用MGNs的中孔洞特性吸附水氣，結合表面類似於氧化石墨烯具有光熱轉換的能力，進行水吸附與脫附的循環。我們採用化學氣相沉積法，於高溫 (825 °С) 下裂解乙烯，成功在中孔洞沸石奈米粒子 (Mesoporous zeolite nanoparticles, MZNs) 表面形成了類似氧化石墨烯的碳層，並具有碳自由基及親水性官能基。經過高溫處理後，孔洞材料仍保持中孔 (3–8 nm) 及微孔 (<1.5 nm) 的特性，以及具有高比表面積 (800–900 m2/g)。MGNs展現出強大的光吸收能力以及在近紅外光 (1000–2500 nm) 範圍內的發光特性。基於這些特點，MGNs可以作為光動力療法 (Photodynamic therapy, PDT) 中的光敏劑，提供新穎且有吸引力的治療方法，同時還可作為光熱材料，解決水資源短缺危機。為了解決MGNs團聚的問題，我們在MZNs表面修飾上聚乙二醇，利用空間斥力讓材料能夠均勻分散。而後，選擇MZNs複合銀奈米粒子，因為銀奈米粒子本身也具有特殊的光化學特性。我們加入銀前驅物並且利用大氣壓微電漿法，有效促進了銀的還原，使分散性之孔洞材料同時具有產生活性氧物質的能力。最終，得到了複合材料Ag@s-PEG-MZNs，為生物醫學領域發展出新的可能性。This study uses mesoporous graphene oxide nanoparticles (MGNs) to adsorb oxygen and water on the surface to explore the interaction with surface-adsorbed gases under irradiation. The surface of MGNs have carbon radicals, and after irradiation passes through singlet oxygen probe (1,3-diphenylisobenzofuran, DPBF), which confirms that it can be used as a photosensitizer, with the ability to exchange energy with oxygen after irradiation and generate singlet states oxygen (1O2). Furthermore, the mesoporosity of MGNs is used to absorb water, and the surface is similar to graphene oxides, with photothermal conversion capabilities to perform water adsorption and desorption cycles. We used chemical vapor deposition to cleavage ethylene at high temperatures, and successfully formed a thin carbon layer similar to graphene oxide on the surface of mesoporous zeolite nanoparticles (MZNs). The thin carbon layer has carbon radicals and hydrophilic functional groups. The porous materials still maintain mesoporous (3–8 nm) and microporous (<1.5 nm), as well as a high surface area (800–900 m2/g). MGNs exhibit strong optical absorption capabilities and the properties of photoluminescence in near-infrared. On the basis of these properties, MGNs can used as a photosensitizer in photodynamic therapy (PDT) to provide novel and attractive treatments. In addition, MGNs can also be used as photothermal materials to solve water shortages crisis. To solve the problem of MGNs aggregation, we modified the surface of MZNs with polyethylene glycol that through spatial repulsion to allow the material to be distributed uniformly. Then, MZNs composite silver nanoparticles were selected because the silver nanoparticles themselves also have special photochemical properties. We add silver precursor and use atmospheric pressure microplasma method to effectively promote silver reduction, so that the dispersed porous materials have the ability to generate reactive oxygen species. Finally, the composite material Ag@s-PEG-MZN has been obtained, opening up new possibilities in the biomedical field.