Morel Anne-Laure, Nikitenko Sergei I, Gionnet Karine, Wattiaux Alain, Lai-Kee-Him Josephine, Labrugere Christine, Chevalier Bernard, Deleris Gerard, Petibois Cyril, Brisson Alain, Simonoff Monique
CNAB, UMR 5084, Universite Bordeaux I, II, CNRS, Le Haut Vigneau, 33170 Gradignan, France.
ACS Nano. 2008 May;2(5):847-56. doi: 10.1021/nn800091q.
In this study, we report a rapid sonochemical synthesis of monodisperse nonaggregated Fe(3)O(4)@SiO(2) magnetic nanoparticles (NPs). We found that coprecipitation of Fe(II) and Fe(III) in aqueous solutions under the effect of power ultrasound yields smaller Fe(3)O(4) NPs with a narrow size distribution (4-8 nm) compared to the silent reaction. Moreover, the coating of Fe(3)O(4) NPs with silica using an alkaline hydrolysis of tetraethyl orthosilicate in ethanol-water mixture is accelerated many-fold in the presence of a 20 kHz ultrasonic field. The thickness of the silica shell can be easily controlled in the range of several nanometers during sonication. Mossbauer spectra revealed that nonsuperparamagnetic behavior of obtained core-shell NPs is mostly related to the dipole-dipole interactions of magnetic cores and not to the particle size effect. Core-shell Fe(3)O(4)@SiO(2) NPs prepared with sonochemistry exhibit a higher magnetization value than that for NPs obtained under silent conditions owing to better control of the deposited silica quantities as well as to the high speed of sonochemical coating, which prevents the magnetite from oxidizing.
在本研究中,我们报道了一种快速的声化学合成法来制备单分散、无团聚的Fe(3)O(4)@SiO(2)磁性纳米颗粒(NPs)。我们发现,与无声反应相比,在功率超声作用下,水溶液中Fe(II)和Fe(III)的共沉淀会产生尺寸分布较窄(4 - 8纳米)的更小的Fe(3)O(4) NPs。此外,在乙醇 - 水混合物中使用原硅酸四乙酯的碱性水解对Fe(3)O(4) NPs进行二氧化硅包覆时,在20 kHz超声场存在的情况下,包覆速度会加快许多倍。在超声处理过程中,二氧化硅壳层的厚度可以很容易地控制在几纳米范围内。穆斯堡尔谱表明,所获得的核壳NPs的非超顺磁行为主要与磁芯的偶极 - 偶极相互作用有关,而不是与粒径效应有关。通过声化学制备的核壳Fe(3)O(4)@SiO(2) NPs表现出比在无声条件下获得的NPs更高的磁化值,这归因于对沉积二氧化硅量的更好控制以及声化学包覆的高速性,从而防止了磁铁矿氧化。