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水基分散绿色发光氧化钇:铽微球,具有纳米二氧化硅壳层涂层。

Aqueous dispersible green luminescent yttrium oxide:terbium microspheres with nanosilica shell coating.

机构信息

King Abdullah Institute for Nanotechnology, King Saud University, Riyadh 11451, Saudi Arabia.

Department of Chemistry, College of Sciences, King Saud University, Riyadh 11451, Saudi Arabia.

出版信息

Spectrochim Acta A Mol Biomol Spectrosc. 2019 Mar 15;211:348-355. doi: 10.1016/j.saa.2018.12.015. Epub 2018 Dec 11.

Abstract

Tb-doped YO microspheres (MSs) were prepared via a homogeneous thermal degradation process at a low temperature and then coated with a nanosilica shell (YO:Tb@SiO) using a sol-gel process. The core MSs were highly crystalline and spherical with a porous surface, single cubic phase, and particle size of 100-250 nm. Transmission electron microscopy (TEM) images clearly showed the spherical shape of the as-prepared core MSs, which were fully covered with a thick and mesoporous nanosilica shell. Fourier transform infrared (FTIR) spectra displayed the well-resolved infrared absorption peaks of silica (SiO, SiOSi, etc.), confirming the presence of the silica surface coating. The core MSs retained their spherical shape even after heat treatment and subsequent silica surface coating. It was observed that the core/shell MSs are easily dispersible in aqueous media and form a semi-transparent colloidal solution. Ultraviolet/visible and zeta potential studies were tested to prove the changes in the surface chemistry of the as-designed core/shell MSs and compare with their core counterpart. The growth of the amorphous silica shell not only increased the particle size but also enhanced remarkably the solubility and colloidal stability of the MSs in aqueous media. The strongest emission lines originating from the characteristic intra-shell 4f-4f electronic transitions of Tb ions were quenched after silica layer deposition, but the MSs still showed strong green (D → F at 530-560 nm as most dominant) emission efficiency, which indicates great potential in fluorescent bio-probes. The emission intensity is discussed in relation to the quenching mechanism induced by surface silanol (Si-OH) groups, particle size, and surface charge.

摘要

Tb 掺杂的 YO 微球(MSs)通过低温下的均相热降解过程制备,然后使用溶胶-凝胶法用纳米二氧化硅壳(YO:Tb@SiO)涂覆。核 MSs 具有高度结晶性和球形多孔表面、单相和粒径为 100-250nm。透射电子显微镜(TEM)图像清楚地显示了所制备的核 MSs 的球形形状,它们完全被厚的介孔纳米二氧化硅壳覆盖。傅里叶变换红外(FTIR)光谱显示了二氧化硅(SiO、SiOSi 等)的良好分辨红外吸收峰,证实了二氧化硅表面涂层的存在。即使在热处理和随后的二氧化硅表面涂层后,核 MSs 仍保持其球形形状。观察到核/壳 MSs 很容易在水介质中分散,并形成半透明胶体溶液。紫外/可见和 zeta 电位研究用于证明所设计的核/壳 MSs 的表面化学变化,并与它们的核对应物进行比较。非晶态二氧化硅壳的生长不仅增加了颗粒尺寸,而且显著提高了 MSs 在水介质中的溶解度和胶体稳定性。源自 Tb 离子特征内壳 4f-4f 电子跃迁的最强发射线在沉积二氧化硅层后被猝灭,但 MSs 仍显示出强绿色(D→F 在 530-560nm 处作为最主要的发射效率),这表明在荧光生物探针中具有很大的潜力。发射强度与由表面硅醇(Si-OH)基团、颗粒尺寸和表面电荷引起的猝灭机制有关。

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