Xu Chao, Bakker Eric
Department of Chemistry, Purdue University, 560 Oval Drive, West Lafayette, Indiana 47907, USA.
Anal Chem. 2007 May 15;79(10):3716-23. doi: 10.1021/ac0701233. Epub 2007 Apr 17.
Multicolor quantum dot-encoded polymeric microspheres are prepared with controllable and uniform doping levels that function as chemical sensors on the basis of bulk optode theory. TOP/TOPO-capped CdSe quantum dots and CdTe quantum dots capped with CdS (lambdaem = 610 and 700 nm, lambdaex = 510 nm) are blended with a THF solution of poly(methyl methacrylate-co-decyl methacrylate), poly(n-butylacrylate), or poly(vinyl chloride) plasticized with bis(2-ethylhexyl) sebacate without a need for ligand exchange. Polymeric microspheres are generated under mild, nonreactive conditions with a particle caster that breaks down a polymer stream containing the quantum dots into fine droplets by the vibration of a piezocrystal. The resulting microspheres exhibit uniform size and fluorescence emission intensities. Fluorescent bar codes are obtained by subsequent doping of two quantum dots with different colors and mass ratios into the microspheres. A linear relationship is found between the readout fluorescence ratio of the two types of nanocrystals and the mixing ratio. Quantum dot-encoded ion sensing optode microspheres are prepared by simultaneous doping of sodium ionophore X, chromoionophore II, a lipophilic tetraphenylborate cation exchanger, and TOPO-capped CdSe/CdS quantum dot as the fluorescent label. A net positive charge of the quantum dots is found to induce an anion-exchange effect on the sensor function, and therefore, an increased concentration of the lipophilic cation exchanger is required to achieve proper ion sensing properties. The modified quantum dot-labeled sodium sensing microspheres show satisfactory sodium response between 10(-4) and 0.1 M at pH 4.8, with excellent selectivity toward common interferences. The amount of the carried positive charges of the CdSe quantum dots is estimated as 2.8 mumol/g of quantum dots used in this study.
制备了具有可控且均匀掺杂水平的多色量子点编码聚合物微球,其基于体光学传感器理论用作化学传感器。用TOP/TOPO包覆的CdSe量子点和用CdS包覆的CdTe量子点(发射波长λem = 610和700 nm,激发波长λex = 510 nm)与聚(甲基丙烯酸甲酯 - 共 - 甲基丙烯酸癸酯)、聚(丙烯酸正丁酯)或用双(2 - 乙基己基)癸二酸酯增塑的聚氯乙烯的四氢呋喃溶液混合,无需进行配体交换。在温和的非反应条件下,使用颗粒铸造机通过压电晶体的振动将包含量子点的聚合物流分解成细液滴,从而生成聚合物微球。所得微球呈现出均匀的尺寸和荧光发射强度。通过随后将两种不同颜色和质量比的量子点掺杂到微球中获得荧光条形码。发现两种类型纳米晶体的读出荧光比与混合比之间存在线性关系。通过同时掺杂钠离子载体X、发色离子载体II、亲脂性四苯基硼酸盐阳离子交换剂和作为荧光标记的TOPO包覆的CdSe/CdS量子点,制备了量子点编码的离子传感光学传感器微球。发现量子点的净正电荷对传感器功能产生阴离子交换效应,因此,需要增加亲脂性阳离子交换剂的浓度以实现适当的离子传感性能。修饰后的量子点标记的钠传感微球在pH 4.8时,在10^(-4)至0.1 M之间显示出令人满意的钠响应,对常见干扰具有优异的选择性。本研究中使用的CdSe量子点所携带的正电荷量估计为2.8 μmol/g量子点。