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Study on intra-zeolite diffusional motion by fluorescence correlation spectroscopy

荧光相关光谱研究沸石内扩散运动

基本信息

批准号：
16550024
负责人：
HASHIMOTO Shuichi
金额：
$ 2.56万
依托单位：
The University of Tokushima (2005)Gunma National College of Technology (2004)
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2004
资助国家：
日本
起止时间：
2004 至 2005
项目状态：
已结题

项目摘要

Diffusion in zeolites plays an important role in most of the applications of zeolites as adsorbents and catalysts. The concise picture of the diffusion in a group of these microporous crystals is drawn as in the following : adsorbed species migrate among a few adsorption sites within a cage besides a jump to neighboring cages through interconnecting windows, and occasionally travel from one zeolite crystal to another. Various methods have been developed for the measurement of intracrysalline diffusivity of adsorbed species including the NMR spin-lattice relaxation, pulsed field-gradient (PFG) NMR, quasielastic neutron scattering (QENS) and triplet-triplet energy transfer techniques. The results were also discussed on the theoretical basis utilizing molecular dynamics and Monte Carlo simulation methods. In spite of these efforts, their still remains a difficulty in the precise measurement of diffusivity of molecules larger than benzene. Our idea is to apply a relatively new technique, f … More luorescence correlation spectroscopy which has been very successful in the measurement of diffusion coefficients in solution and biological systems (membranes and cells) but so far not been applied to heterogeneous systems such as zeolites. We have constructed a setup based on microscope with an Ar-ion laser as a excitation light source, a Si-avalanche photodiode as a detector and a correlation board as an analyzing system. We confirmed that our setup works properly for solution systems, however, difficulty arises when we applied to the zeolite systems. Because of too slow diffusion in zeolites we could not measure proper correlation, thus we are forced to modify the detection system. We, therefore, applied a single molecule spectroscopy to the problem of diffusion within a single zeolite crystal. We used epi-illumination technique coupled with the image capture by cooled CCD camera. We followed the time course of the fluorescence image of single molecules on a zeolite crystals and analyzed the trajectories of 20-30 molecules. By doing so, we could obtain the diffusion coefficient of adsorbed species. We could establish the methodology for the measurements of diffusivity within zeolites for various molecules, we could not obtain data for many molecules because of time limitation. As a result, we have no solid view for the outcome and this will be our future works. Less

在沸石作为吸附剂和催化剂的大多数应用中，沸石中的扩散起着重要作用。一组这些微孔晶体中扩散的简明图像如下：被吸附的物质除了通过互连窗口跳到邻近的笼之外，还在笼内的几个吸附位点之间迁移，偶尔从一个沸石晶体移动到另一个沸石晶体。已经开发了各种方法用于测量吸附物种的晶内扩散率，包括NMR自旋-晶格弛豫、脉冲场梯度（PFG）NMR、准弹性中子散射（QENS）和三重态-三重态能量转移技术。利用分子动力学和蒙特卡罗模拟方法对结果进行了理论分析。尽管这些努力，他们仍然是一个困难，在比苯更大的分子的扩散率的精确测量。我们的想法是应用一种相对较新的技术， ...更多信息荧光相关光谱法在测量溶液和生物系统（膜和细胞）中的扩散系数方面非常成功，但迄今为止尚未应用于非均相系统如沸石。以氩离子激光器为激发光源，硅雪崩光电二极管为探测器，相关板为分析系统，建立了一套基于显微镜的实验装置。我们证实，我们的设置工作正常的溶液系统，然而，困难出现时，我们应用到沸石系统。由于分子筛中的扩散太慢，我们不能测量适当的相关性，因此我们被迫修改检测系统。因此，我们将单分子光谱应用于单个沸石晶体内的扩散问题。我们使用落射照明技术，结合冷却CCD相机的图像捕获。我们跟踪了单分子在沸石晶体上的荧光图像的时间过程，并分析了20-30个分子的轨迹。通过这样做，我们可以得到吸附物种的扩散系数。我们可以建立各种分子在沸石中扩散系数的测量方法，但由于时间限制，我们无法获得许多分子的数据。因此，我们对结果没有明确的看法，这将是我们未来的工作。少

项目成果

期刊论文数量（30）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Application of time- and space-resolved fluorescence spectroscopy to the distribution of guest species into micrometer-sized zeolite crystals

应用时间和空间分辨荧光光谱将客体物质分布到微米尺寸的沸石晶体中

DOI：
发表时间：
2006
期刊：
Phys. Chem. Chem. Phys 8・12
影响因子：
0
作者：
K.Yamada;H.Nakamura;S.Matsushima;H.Yamane;T.Haishi;K.Kuamda;Hiroshi Kominami;古南博;Hiroshi Kominami;古南博;Hiroshi Kominami;Hiroshi Kominami;Hiroshi Kominami;S.Hashimoto;橋本修一;S.Hashimoto
通讯作者：
S.Hashimoto

Fluorescence microscopy investigation on the manipulation of guest species in zeolites

沸石中客体物质操控的荧光显微镜研究

DOI：
发表时间：
2004
期刊：
Res. Chem. Intermed. 30.2
影响因子：
0
作者：
S.Hashimoto;M.Saitoh;N.Taira;W.Schmidt;K.Hirai;H.Tomioka;S.Hashimoto;S.Hashimoto
通讯作者：
S.Hashimoto

Emission spectroscopic investigation of triplet diarylcarbene generated in molecular sieve VPI-5.

DOI：
10.1021/jp0548974
发表时间：
2005-10
期刊：
The journal of physical chemistry. B
影响因子：
0
作者：
S. Hashimoto;M. Saitoh;Nobuyuki Taira;W. Schmidt;Katsuyuki Hirai;H. Tomioka
通讯作者：
S. Hashimoto;M. Saitoh;Nobuyuki Taira;W. Schmidt;Katsuyuki Hirai;H. Tomioka

Photochemistry of Charge-Transfer Complexes in a Viologen Periodic Mesoporous Organosilica. From Femtosecond to Minutes Time Evolution

紫罗碱周期性介孔有机二氧化硅中电荷转移复合物的光化学。