College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637000, PR China.
Anal Chem. 2012 Feb 7;84(3):1765-71. doi: 10.1021/ac2029908. Epub 2012 Jan 26.
This paper presents a simple and convenient methodology to separate and characterize water-soluble gold nanocluster stabilized with penicillamine ligands (AuNC-SR) in aqueous medium by sequential size-selective precipitation (SSSP) and mass spectrometry (MS). The highly polydisperse crude AuNC-SR product with an average core diameter of 2.1 nm was initially synthesized by a one-phase solution method. AuNCs were then precipitated and separated successively from larger to smaller ones by progressively increasing the concentration of acetone in the aqueous AuNCs solution. The SSSP fractions were analyzed by UV-vis spectroscopy, matrix-assisted laser desorption/ionization time-of-flight-MS, and thermogravimetric analysis (TGA). The MS and TGA data confirmed that the fractions precipitated from 36, 54, 72, and 90% v/v acetone (F(36%), F(54%), F(72%), and F(90%)) comprised families of close core size AuNCs with average molecular formulas of Au(38)(SR)(18), Au(28)(SR)(15), Au(18)(SR)(12), and Au(11)(SR)(8), respectively. In addition, F(36%), F(54%), F(72%), and F(90%) contained also the typical magic-sized gold nanoparticles of Au(38), Au(25), Au(18), and Au(11), respectively, together with some other AuNCs. This study shed light on the potential use of SSSP for simple and large-scale preliminary separation of polydisperse water-soluble AuNCs into different fractions with a relatively narrower size distribution.
本文提出了一种简单便捷的方法,通过顺序尺寸选择性沉淀(SSSP)和质谱(MS),在水介质中分离和表征与半胱氨酸配体稳定的水溶性金纳米簇(AuNC-SR)。最初通过单相溶液法合成高度多分散的粗 AuNC-SR 产物,其平均核心直径为 2.1nm。然后,通过逐渐增加水相 AuNC 溶液中丙酮的浓度,将 AuNC 依次从较大尺寸沉淀并分离成较小尺寸。通过紫外可见光谱、基质辅助激光解吸/电离飞行时间质谱和热重分析(TGA)对 SSSP 级分进行分析。MS 和 TGA 数据证实,从 36、54、72 和 90%v/v 丙酮(F(36%)、F(54%)、F(72%)和 F(90%))沉淀的级分包含具有平均分子式 Au(38)(SR)(18)、Au(28)(SR)(15)、Au(18)(SR)(12)和 Au(11)(SR)(8)的紧密核心尺寸 AuNC 家族。此外,F(36%)、F(54%)、F(72%)和 F(90%)还分别包含典型的 magic-sized 金纳米粒子 Au(38)、Au(25)、Au(18)和 Au(11),以及一些其他的 AuNC。本研究揭示了 SSSP 在简单、大规模初步分离多分散水溶性 AuNC 成具有相对较窄尺寸分布的不同级分方面的潜力。