Evaluation of Rate Parameters during Heterogeneous Catalysisin Supercritical Fluids

流体在其临界点附近的独特性质可以 可用于改变反应器内的主要反应途径， 反应体系 一种不寻常的溶剂性质 超临界流体（SCF）可以促进反应， 在传统溶剂中无法实现。 发生这种情况 因为超临界溶剂提供了一种环境 在此，由于 溶剂的物理性质介于 气体和液体。 因此，高溶剂密度相对 与相对于气体的高溶质扩散率相结合， 在液体中的扩散性，创造一个环境， 浓度的溶质可以溶解在溶液中， 不存在严重的传质限制。 这个目标 研究项目是调查超临界流体溶剂的影响 在控制总体速率的速率过程上， 催化反应 具体而言，PI将尝试测量 吸附，速率内扩散，和 超临界条件下催化剂的吸附能力 条件 他将使用色谱技术来测量 在各种实验条件下， 条件，并考虑SCF对 通过测量转化率和产物的反应途径 选择性 这项技术的一个应用是在该地区 通过联合超临界流体萃取进行危险废物修复 从多孔土壤和溶剂再生的有机物， 氧化 代替这种系统的这种潜在用途， 这项工作将涉及五氧化二钒（V2 O 5）催化 氧化1，4-二氯苯（许多研究的模型化合物 危险物质）在超临界水和 超临界一氧化二氮（N2 O）。

The unique properties of a fluid near its critical point can be utilized to alter principle reaction pathways within a reacting system. The unusual solvent properties of a supercritical fluid (SCF) can facilitate reactions which cannot be achieved in traditional solvents. This happens because the supercritical solvent provides an environment where mass transfer limitations are eliminated due to the solvent's physical properties, which lie intermediate between a gas and a liquid. Thus, the high solvent density relative to a gas combined with high solute diffusivity relative to diffusivity in a liquid, create an environment where high concentrations of solute can dissolve in the solution and yet severe mass transfer limitations are absent. The goal of this research project are to investigate the effect of SCF solvents on the rate processes which control the overall rate of a catalytic reaction. Specifically, the PI will attempt to measure the rate of adsorption, the rate intraparticle diffusion, and the adsorptive capacity of the catalyst under supercritical conditions. He will use chromatographic techniques to measure the desired rate parameters under a variety of experimental conditions and consider the overall effect of the SCF on the reaction pathways by measuring conversion and product selectivity. An application of this technology is in the area of hazardous waste remediation through combined SCF extraction of organics from the porous soil and solvent regeneration by oxidation. In lieu of this potential use of such systems, this work will involve the vanadium pentoxide (V2O5) catalyzed oxidation of 1,4-dichlorobenzene (a model compound for many hazardous materials) in both supercritical water and supercritical nitrous oxide (N2O).