Oxidation-induced water-solubilization and chemical functionalization of fullerenes C-60, Gd@C-60 and Gd@C-82: atomistic insights into the formation mechanisms and structures of fullerenols synthesized by different methods

	Oxidation-induced water-solubilization and chemical functionalization of fullerenes C-60, Gd@C-60 and Gd@C-82: atomistic insights into the formation mechanisms and structures of fullerenols synthesized by different methods
	Wang ZZ(王真真); Wang, ZZ; Zhao YL(赵宇亮); Gao XF(高兴发); Lu, ZH; Zhao, YL; Gao, XF
刊名	NANOSCALE
	2015
卷号	7 期号:7 页码:2914-2925
通讯作者	高兴发
英文摘要	Water-solubilization is the prerequisite to endow the pristinely hydrophobic fullerenes with biocompatibility and biofunctionality, which has been widely applied to derive fullerene-based nanomaterials for biomedical applications. Oxidation reactions using O-2 and H2O2 are the most commonly used approaches to this end, through which fullerenols with different structural features can be obtained. Despite the progress in the syntheses and bioapplications of fullerenols, their formation mechanisms and structures at the atomic level, which substantialize their physical properties and biofunctions, have been little understood. Using density functional theory calculations, we comparatively study the mechanisms and product structures for the oxidations of C-60, Gd@C-60 and Gd@C-82 using both O-2 and H2O2 as oxidizing agents under both neutral and alkaline aqueous conditions. We predict the formation mechanisms and product structures corresponding to the different synthetic conditions. Briefly, the H2O2 oxidations of C-60, Gd@C-60 and Gd@C-82 under neutral conditions do not occur readily at room temperature because of the high energy barriers, whereas the H2O2 oxidations can readily proceed under alkaline conditions. The oxygen-containing groups of the fullerenols obtained under these conditions include hydroxyl, carbonyl, hemiacetal and deprotonated vic-diol. In contrast, through O-2 oxidation under alkaline conditions, the most probable oxygen-containing groups for C-60 fullerenols are epoxide and deprotonated vic-diol, and those for Gd@C-60 and Gd@C-82 fullerenols are hydroxyls and carbonyls. The results explain a wide range of experimental findings reported before. More importantly, they provide atomistic-level insights into the formation mechanisms and structures for various fullerenols, which are of fundamental interest for understanding their biomedical applications in the future.
学科主题	Chemistry; Science & Technology - Other Topics; Materials Science; Physics
类目[WOS]	Chemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied
收录类别	SCI ; EI
WOS记录号	WOS:000349473200013
公开日期	2016-05-03
内容类型	期刊论文
源URL	[http://ir.ihep.ac.cn/handle/311005/228173]
专题	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Wang ZZ,Wang, ZZ,Zhao YL,et al. Oxidation-induced water-solubilization and chemical functionalization of fullerenes C-60, Gd@C-60 and Gd@C-82: atomistic insights into the formation mechanisms and structures of fullerenols synthesized by different methods[J]. NANOSCALE,2015,7(7):2914-2925.
APA	王真真.,Wang, ZZ.,赵宇亮.,高兴发.,Lu, ZH.,...&Gao, XF.(2015).Oxidation-induced water-solubilization and chemical functionalization of fullerenes C-60, Gd@C-60 and Gd@C-82: atomistic insights into the formation mechanisms and structures of fullerenols synthesized by different methods.NANOSCALE,7(7),2914-2925.
MLA	王真真,et al."Oxidation-induced water-solubilization and chemical functionalization of fullerenes C-60, Gd@C-60 and Gd@C-82: atomistic insights into the formation mechanisms and structures of fullerenols synthesized by different methods".NANOSCALE 7.7(2015):2914-2925.