Abstract: | Macroscopically homogeneous and visually transparent fullerene-containing glasses are fabricated from sol-gel mixtures of aminated C60 derivatives and tetraethyl orthosilicate (TEOS) through physical blending and chemical reaction. The aminated fullerenes are synthesized by the amination reactions of C60 with 6-amino-1-hexanol, cyclohexylamine, 2-(2-aminoethoxy)ethanol, and 3-aminopropyltriethoxysilane at 100°C under nitrogen. The amination products are purified by filtration, precipitation, and column chromatography and are isolated in good to excellent yields (32–82%). Characterization by NMR, MS, and TGA analyses reveals that the aminated fullerenes possess molecular structures H
x
C60NH(CH2)6OH]
x
, H
x
C60(NH-cyclo-C6H11)
x
, H
x
C60NH(CH2CH2O)2H]
x
, and H
x
C60NH(CH2)3Si(OCH2CH3)3]
x
. All the aminated fullerenes except 2 are completely soluble in aqueous alcoholic solutions of TEOS and can be incorporated into silica gel networks by sol-gel process in the absence or presence of drying-control chemical additives, giving crack-free monoliths of large sizes (up to 60 mm). Electronic absorption spectrum of the fullerene glass continuously red shifts with an increase in the C60 content, suggesting the formation of fullerene nanoclusters in the sol-gel process. The fullerene glasses are thermally and optically stable, resisting continuous attack of strong laser pulses of 532 nm for a prolonged period of time without losing their optical limiting power. |