CAREER: Investigation of Catalysis at Solid-Liquid Interfaces by Non-Linear Optical Spectroscopy

提出的研究目标是发展和使用非线性光学技术来研究精细化学合成中重要的固-液催化反应。本研究是利用现代原位光谱技术研究非均相精细化学品和药物催化表面化学的核心部分。将使用的两种方法是和频谱（SFS）和二次谐波产生（SHG）。这两种技术都是纯粹的表面选择性，因为只有催化剂表面和吸附在其上的分子被检测到。计划进行两种不同类型的实验。第一部分是利用全内反射（TIR） SFS和SHG研究模型负载型金属催化剂。第二种类型的实验将尝试将SHG（最终是SFS）研究扩展到溶液中的催化剂颗粒。这两种方法都将构成非线性光学技术在固液催化系统中的首次应用。表面增强拉曼和红外光谱测量将提供有关催化剂表面状态的额外信息。平行反应速率测量将进行，以便将界面表面性质与催化速率和选择性联系起来，并提出反应机理。精细化学品和药品是化学工业中迅速发展的一个部门。多相催化显示了促进平稳过渡到更环保的处理的希望。

The goal of the proposed research is to develop and use nonlinear optical techniques to study solid-liquid catalytic reactions important for fine chemical synthesis. The proposed research is a central part of an effort to study surface chemistry of heterogeneous fine chemicals and pharmaceuticals catalysis with modern in-situ spectroscopic techniques. The two approaches that will be used are sum frequency spectroscopy (SFS) and second harmonic generation (SHG). Both techniques are purely surface-selective, in that only the catalyst surface and the molecules adsorbed on it are detected. Two different types of experiments are planned. The first involves the study of model supported metal catalysts by total internal reflection (TIR) SFS and SHG. The second type of experiment will attempt to extend SHG (and eventually SFS) studies to catalyst particles in solution. Both methods will constitute the first application of nonlinear optical techniques to solid-liquid catalytic systems. Surface-enhanced Raman and infrared spectroscopic measurements will provide additional information regarding the state of catalyst surfaces. Parallel reaction rate measurements will be made in order to correlate surface in interface properties with catalytic rates and selectivity, and reaction mechanisms will be proposed. Fine chemicals and pharmaceuticals represent a rapidly expanding sector of the chemical industry. Heterogeneous catalysis shows promise for facilitating a smooth transition to more environmentally benign processing.