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用于富勒烯 C60 定量分析的尺寸排他性纳米传感器。

Size-exclusive nanosensor for quantitative analysis of fullerene C60.

机构信息

Center for Advanced Sensors & Environmental System (CASE), Department of Chemistry, State University of New York-Binghamton, Binghamton, New York 13902-6000, USA.

出版信息

Environ Sci Technol. 2011 Jun 15;45(12):5294-300. doi: 10.1021/es1043084. Epub 2011 May 18.

Abstract

This paper presents the first development of a mass-sensitive nanosensor for the isolation and quantitative analyses of engineered fullerene (C₆₀) nanoparticles, while excluding mixtures of structurally similar fullerenes. Amino-modified beta-cyclodextrin (β-CD-NH₂) was synthesized and confirmed by ¹HNMR as the host molecule to isolate the desired fullerene C₆₀. This was subsequently assembled onto the surfaces of gold-coated quartz crystal microbalance (QCM) electrodes using N-dicyclohexylcarbodiimide/N-hydroxysuccinimide (DCC/NHS) surface immobilization chemistry to create a selective molecular configuration described as (Au)-S-(CH₂)²-CONH-beta-CD sensor. The mass change on the sensor configuration on the QCM was monitored for selective quantitative analysis of fullerene C₆₀ from a C₆₀/C₇₀ mixture and soil samples. About ~10¹⁴-10¹⁶ C₆₀ particles/cm² were successfully quantified by QCM measurements. Continuous spike of 200 μL of 0.14 mg C₆₀ /mL produced changes in frequency (-Δf) that varied exponentially with concentration. FESEM and time-of-flight secondary-ion mass spectrometry confirmed the validity of sensor surface chemistry before and after exposure to fullerene C₆₀. The utility of this sensor for spiked real-world soil samples has been demonstrated. Comparable sensitivity was obtained using both the soil and purified toluene samples. This work demonstrates that the sensor has potential application in complex environmental matrices.

摘要

本文首次开发了一种质量敏感的纳米传感器,用于分离和定量分析工程富勒烯(C₆₀)纳米颗粒,同时排除结构相似的富勒烯混合物。合成了氨基修饰的β-环糊精(β-CD-NH₂),并通过 ¹HNMR 确认为分离所需富勒烯 C₆₀ 的主体分子。随后,使用 N-二环己基碳二亚胺/N-羟基琥珀酰亚胺(DCC/NHS)表面固定化化学将其组装到镀金石英晶体微天平(QCM)电极表面,以创建一种选择性的分子构型,描述为(Au)-S-(CH₂)²-CONH-β-CD 传感器。在 QCM 上的传感器构型上的质量变化用于从 C₆₀/C₇₀混合物和土壤样品中选择性定量分析富勒烯 C₆₀。通过 QCM 测量成功定量了约 10¹⁴-10¹⁶ C₆₀ 颗粒/cm²。连续注入 200 μL 0.14 mg C₆₀/mL 的溶液会导致频率(-Δf)发生指数变化,这与浓度有关。FESEM 和飞行时间二次离子质谱证实了传感器表面化学在暴露于富勒烯 C₆₀ 前后的有效性。该传感器在加标实际土壤样品中的实用性已得到证明。从土壤和纯化的甲苯样品中均获得了相当的灵敏度。这项工作表明,该传感器在复杂的环境基质中具有潜在的应用。

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