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用于正己烷的高效沸石传感材料的设计

Design of efficient zeolite sensor materials for n-hexane.

作者信息

Yang Ping, Ye Xingnan, Lau Choiwan, Li Zengxi, Liu Xia, Lu Jianzhong

机构信息

School of Pharmacy, Fudan University, 138 Yixueyuan Road, Shanghai 200032, China.

出版信息

Anal Chem. 2007 Feb 15;79(4):1425-32. doi: 10.1021/ac061811+.

DOI:10.1021/ac061811+
PMID:17297941
Abstract

The effectiveness of several zeolite catalysts was investigated using the cataluminescence (CTL) gas sensor system. Trace amounts of n-hexane in air samples were detected by this method. This research establishes that the specific pore size of the zeolite offers designable environment for selective CTL reaction, and "Lewis-type" basic sites appear to contribute to the catalytic nature of the zeolite surface. By incorporating either Cs+ or K+, the velocity and luminescence intensity of these catalytic reactions increase while going from Na to Cs, according to the basic nature of this group of cations in the following order: Cs > K > Na. The proposed sensor shows high sensitivity and selectivity to n-hexane at a mild reaction temperature of 225 degrees C. Quantitative analysis was performed at a selected wavelength of 460 nm. The linear range of CTL intensity versus concentration of n-hexane was 0.776-23.28 microg/mL (R = 0.997, n = 7) on CsNaY, and 0.776-23.28 microg/mL (R = 0.998, n = 7) on CsNaX, with a detection limit of 0.155 microg/mL (signal-to-noise ratio 3). Interferences from foreign substances such as methanol, ethanol, 2-propanol, acetone, acetonitrile, chloroform, or dichlormethane and other alkanes, aromatics, and alkyl aromatics such as methane, n-pentane, 3-methylpentane, 3,3-dimethylpentane, methylbenzene, ethylbenzene, and sec-butylbenzene were very low or not detectable. Results of a series of GC and GC/MS experiments suggest that the possible mechanism of the reaction is the formation of an unstable transition structure with a four-member ring, and this ring most probably consists of an oxygen atom and a carbonium ion localized on the zeolite suface.

摘要

使用催化发光(CTL)气体传感器系统研究了几种沸石催化剂的有效性。通过该方法检测空气样品中的痕量正己烷。本研究表明,沸石的特定孔径为选择性CTL反应提供了可设计的环境,并且“Lewis型”碱性位点似乎有助于沸石表面的催化性质。通过掺入Cs+或K+,这些催化反应的速度和发光强度从Na到Cs逐渐增加,这是根据该组阳离子的碱性按以下顺序排列的:Cs > K > Na。所提出的传感器在225℃的温和反应温度下对正己烷表现出高灵敏度和选择性。在选定的460nm波长下进行定量分析。在CsNaY上,CTL强度与正己烷浓度的线性范围为0.776 - 23.28μg/mL(R = 0.997,n = 7),在CsNaX上为0.776 - 23.28μg/mL(R = 0.998,n = 7),检测限为0.155μg/mL(信噪比3)。来自甲醇、乙醇、2-丙醇、丙酮、乙腈、氯仿或二氯甲烷等外来物质以及其他烷烃、芳烃和烷基芳烃(如甲烷、正戊烷(n-pentane)、3-甲基戊烷、3,3-二甲基戊烷、甲苯、乙苯和仲丁基苯)的干扰非常低或不可检测。一系列气相色谱(GC)和气相色谱/质谱(GC/MS)实验的结果表明,该反应的可能机制是形成具有四元环的不稳定过渡结构,并且该环很可能由位于沸石表面的一个氧原子和一个碳正离子组成。

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