CAREER: Steering Chemical Reactions Through Spatial Confinement: Catalytic Reaction Engineering in Microchannel Reactors

项目编号：0448147研究项目：该职业项目旨在通过微通道反应器的空间限制来研究、控制并最终引导催化反应。它基于微机械催化反应器系统的开发，用于对多相-均相耦合反应进行详细的实验和数值研究，具体包括以下步骤：通过改变微通道直径来允许或逐渐抑制均相反应，探测和确定均相和非均相反应途径的贡献；通过淬火控制非均相反应，即完全抑制潜在的爆炸性气相反应，从而为这些“禁制区”的化学反应的探索性研究开辟了新的参数范围；通过选择性猝灭反应路径来引导多个反应系统，从而以一种新的、非常规的方式引入工艺选择性；在广泛的实际操作条件下，通过非侵入式原位红外光谱研究反应流（特别是边界层动力学）。该方法将用高温催化进行测试，高温催化是一类具有广泛工业和环境影响以及基础科学意义的反应。然而，所开发的系统将适用于这些条件之外的一系列多相反应系统的研究。教育：研究项目的主要部分紧密结合到教育计划中，该计划基于在整个本科课程中引入过程强化和微反应器工程。它还将以微反应器工程为例，向学生介绍跨越许多长度和时间尺度的“多尺度思维”，这是现代工程问题的特征。该计划将被整合到一个更广泛的教育项目中，在匹兹堡大学及其他地方实施。更广泛的影响：该项目可能对氢燃料电池燃料转化剂的发展产生重大影响，从而通过成功演示CO/ h2混合物中完全选择性CO氧化（计划中的测试反应之一）对“氢经济”的发展产生重大影响。对微通道反应堆中爆炸反应的熄灭进行详细调查，从而证明反应堆的内在安全性，可能对工业过程的安全，特别是对广泛和分散的氢气分配系统的安全产生重大影响。

ABSTRACTPI: Goetz Veser Institution: University of PittsburghProposal Number: 0448147Research: This CAREER project aims to investigate, control and ultimately steer catalytic reactions through spatial confinement in a microchannel reactor. It is based on the development of a micromachined catalytic reactor system for detailed experimental and numerical investigations of coupled heterogeneous-homogeneous reactions, and specifically comprises the following steps:Probe and identify contributions from homogeneous and heterogeneous reaction pathways by varying the microchannel diameter to either allow or gradually suppress homogeneous reactions;Control heterogeneous-homogeneous reactions by quenching, i.e. completely suppressing, potentially explosive gas phase reactions, thus opening up new parameter ranges for exploratory studies of chemical reactions in these 'forbidden regimes';Steer multiple reaction systems by selectively quenching reaction pathways and thus introduce process selectivity in a new, non-conventional way;Investigate the reacting flow (and in particular boundary-layer kinetics) via non-invasive, in-situ IR spectroscopy over a wide range of realistic operating conditions.The approach will be tested with high-temperature catalysis, a class of reactions with broad industrial and environmental impact as well as fundamental scientific significance. However, the developed system will be applicable well beyond these conditions to the study of a range of multiphase reaction systems. Education:Major parts of the research project are closely integrated into the education plan, which is based on the introduction of process intensification and microreactor engineering throughout the undergraduate curriculum. It will furthermore use microreactor engineering as an example to introduce students to 'multi-scale thinking' across the many length and time scales that characterize modern engineering problems. The plan will be integrated within a broader educational program for implementation at the University of Pittsburgh and beyond.Broader Impact: The project could have a major impact on the development of fuel reformers for hydrogen fuel cells and thus on the development of the 'hydrogen economy' through the successful demonstration of perfectly selective CO oxidation in CO/H2-mixtures (one of the planned test reactions). The detailed investigation of the quenching of explosive reactions in microchannel reactors, and hence the demonstration of intrinsic reactor safety, could have significant impact on the safety of industrial processes and, in particular, on a widespread and decentralized hydrogen distribution system.