CAS Key Laboratory of Design and Assembly of Functional Nanostructures, and Fujian Key Laboratory of Nanomaterials, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
Nanoscale. 2018 Jun 21;10(24):11477-11484. doi: 10.1039/c8nr03252a.
Lanthanide (Ln3+)-doped NaREF4 (RE = rare earth) nanocrystals (NCs) are one of the most widely studied upconversion and downshifting luminescent nanoprobes. However, the size and optical performance of the Ln3+-doped NaREF4 NCs produced by the available lab-scale synthesis may vary from batch to batch, which inevitably limits their practical bioapplications. Herein, we report the synthesis of uniform Ln3+-doped NaREF4 NCs via a facile solid-liquid-thermal-decomposition (SLTD) method by directly employing NaHF2 powder as a fluoride and sodium precursor. The proposed SLTD strategy is easy to perform, time-saving and cost-effective, making it ideal for scale-up syntheses. Particularly, over 63 g of β-NaGdF4:Yb,Er@NaYF4 core/shell NCs with narrow size variation (<7%) were synthesized via a one-pot reaction. By virtue of their superior upconversion and downshifting luminescence, we employed the synthesized core/shell nanoprobes for the in vitro detection of prostate-specific antigen with a limit of detection down to 1.8 ng mL-1, and for in vivo near-infrared imaging with a high signal-to-noise ratio of 12. These findings may pave the way for the commercialization of Ln3+-doped nanoprobes in bioassay kits for versatile clinical applications.
镧系元素(Ln3+)掺杂的 NaREF4(RE = 稀土)纳米晶体(NCs)是研究最广泛的上转换和下转换发光纳米探针之一。然而,通过现有实验室规模的合成方法制备的 Ln3+掺杂的 NaREF4 NCs 的尺寸和光学性能可能会在批次之间有所不同,这不可避免地限制了它们在实际生物应用中的应用。在此,我们通过直接使用 NaHF2 粉末作为氟化物和钠前体,通过简便的固-液-热分解(SLTD)方法报告了均匀的 Ln3+掺杂的 NaREF4 NCs 的合成。所提出的 SLTD 策略易于实施、节省时间且具有成本效益,非常适合扩大规模合成。特别是,通过一锅反应合成了超过 63 g 的具有窄尺寸变化(<7%)的β-NaGdF4:Yb,Er@NaYF4 核/壳 NCs。由于其优异的上转换和下转换发光性能,我们使用合成的核/壳纳米探针用于体外检测前列腺特异性抗原,检测限低至 1.8 ng mL-1,并用于体内近红外成像,信噪比高达 12。这些发现可能为商业应用于生物分析试剂盒中的 Ln3+掺杂纳米探针铺平道路。