Center for Optical Materials Science and Engineering Technologies, Department of Materials Science and Engineering, Clemson University, Clemson, SC 29634-0971, USA.
Center for Optical Materials Science and Engineering Technologies, Department of Chemistry, Clemson University, Clemson, SC 29634-0971, USA.
J Colloid Interface Sci. 2021 Jan 15;582(Pt B):1128-1135. doi: 10.1016/j.jcis.2020.07.125. Epub 2020 Aug 10.
X-rays offer low tissue attenuation with high penetration depth when used in medical applications and when coupled with radioluminescent nanoparticles, offer novel theranostic opportunities. In this role, the ideal scintillator requires a high degree of crystallinity for an application relevant radioluminescence, yet a key challenge is the irreversible aggregation of the particles at most crystallization temperatures. In this communication, a high temperature multi-composite reactor (HTMcR) process was successfully developed to recrystallize monodisperse scintillating particulates by employing a core-multishell architecture. The core-shell morphology of the particles consisted of a silica core over-coated with a rare earth (Re = Y, Lu, Ce) oxide shell. This core-shell assembly was then encapsulated within a poly(divinylbenzene) shell which was converted to glassy carbon during the annealing & crystallization of the silica/rare earth oxide core-shell particle. This glassy carbon acted as a delamination layer and prevented the irreversible aggregation of the particles during the high temperature crystallization step. A subsequent low temperature annealing step in an air environment removed the glassy carbon and resulted in radioluminescent nanoparticles. Two monodisperse nanoparticle systems were synthesized using the HTMcR process including cerium doped YSiO and LuSiO with radioluminescence peaks at 427 and 399 nm, respectively. These particles may be employed as an in vivo light source for a noninvasive X-ray excited optogenetics.
X 射线在医学应用中具有低组织衰减和高穿透深度,如果与放射发光纳米粒子结合使用,则提供了新的治疗诊断机会。在这种情况下,理想的闪烁体需要高度的结晶度才能产生与应用相关的放射发光,但一个关键的挑战是大多数结晶温度下粒子的不可逆聚集。在本通讯中,成功开发了一种高温多复合反应器(HTMcR)工艺,通过采用核壳多壳结构来重结晶单分散闪烁颗粒。颗粒的核壳形态由二氧化硅核上覆盖的稀土(Re = Y、Lu、Ce)氧化物壳组成。然后将这种核壳组装体封装在聚(二乙烯基苯)壳内,在二氧化硅/稀土氧化物核壳颗粒的退火和结晶过程中,该壳转化为玻璃碳。这种玻璃碳充当分层层,防止颗粒在高温结晶过程中发生不可逆聚集。随后在空气环境中进行低温退火步骤,去除玻璃碳并得到放射发光纳米颗粒。使用 HTMcR 工艺合成了两种单分散纳米颗粒系统,包括掺杂铈的 YSiO 和 LuSiO,其放射发光峰分别为 427nm 和 399nm。这些颗粒可作为体内非侵入性 X 射线激发光遗传学的光源。