Yang Ping, Ye Xingnan, Lau Choiwan, Li Zengxi, Liu Xia, Lu Jianzhong
School of Pharmacy, Fudan University, 138 Yixueyuan Road, Shanghai 200032, China.
Anal Chem. 2007 Feb 15;79(4):1425-32. doi: 10.1021/ac061811+.
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.
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。