Equipment Proposal: Multiple Capillary Probe Inlet System for Spatio-Temporal Studies of Catalysis in Multi-Functional Reactors

该奖项是根据2009年《美国复苏和再投资法案》(公法111-5)资助的。多功能和周期性运行的催化反应器正在出现，特别是在与环境和能源相关的应用中。这些催化反应器的一个共同主线是多个化学和运输过程的复杂的非线性相互作用，这些过程产生了浓度和温度的空间和时间梯度。催化剂和反应器的合理设计和操作需要全面了解这些相互作用，希望以通过系统实验和分析开发的预测模型的形式出现。测量一定空间速度范围内出口浓度的经典方法不能提供阐明反应路径和反应器性能特征所需的详细程度，也不能与严格的反应器模型进行比较。为此，PI将采用多毛细管探针质谱计进样系统，对多功能反应器中的催化进行空间分辨研究。该系统将与现有的四极质谱计相结合，并纳入最近建造的先进的实验室规模反应堆系统。质谱仪系统将用于解析催化过程中选定的反应物和产物的浓度，具有空间和/或时间梯度，包括由当前NSF拨款支持的周期性NOx存储和还原，耦合的周期性NOx存储和还原和选择性催化还原，以及催化膜反应器中的自热重整，这是NSF最近授予的主题。智力优点：拟议的工作的智力优点包括催化反应器中流动和反应过程中物种浓度和温度的时空分辨率。这些测量将提供有关反应路径和导致浓度和温度前沿传播的反应-传输相互作用的性质的基本信息。从这些测量中获得的详细见解将被用于开发微动力学和反应器模型，从而改进设计和操作策略。广泛影响：这项研究的更广泛影响是发展了空间分辨质谱学，作为研究多相反应器中催化作用的新工具，并将此类实验与空间/多维催化反应器模型紧密结合。这项研究将促进对环境和替代能源至关重要的新兴催化过程的理解，特别是催化膜反应器中自热重整过程中稀薄NOx的储存和还原、选择性催化还原以及氢气的生成和提纯。

0933271HaroldThis award is funded under the American Recovery and Reinvestment Act of 2009 (Public Law 111-5).Multi-functional and periodically-operated catalytic reactors are emerging, particularly in environmental and energy related applications. A common thread these catalytic reactors is the complex nonlinear interactions of multiple chemical and transport processes that give rise to spatial and temporal gradients of concentration and temperature. The rational design and operation of the catalyst and reactor requires a comprehensive understanding of these interactions, hopefully in the form of a predictive model that developed through systematic experimentation and analysis. The classical approach of measuring outlet concentration for a range of space velocities does not provide the level of detail needed to elucidate reaction pathways and reactor performance features, or to compare with rigorous reactor models. To this end, the PI will employ a multiple capillary probe mass spectrometer inlet system for carrying out spatially-resolved studies of catalysis in multi-functional reactors. The system will be coupled with an existing quadrupole mass spectrometer and incorporated into a recently built advanced bench-scale reactor system. The mass spectrometer system will be used to resolve the concentrations of selected reactants and products in catalytic processes with spatial and/or temporal gradients, including periodic NOx storage and reduction for which the PI is supported by a current NSF grant, coupled periodic NOx storage and reduction and selective catalytic reduction, and autothermal reforming in catalytic membrane reactors, the subject of a recent NSF grant.Intellectual Merit: The intellectual merit of the proposed work comprises the spatial and temporal resolution of species concentrations and temperature during flow and reaction in catalytic reactors. These measurements will provide essential information about reaction pathways and the nature of reaction-transport interactions leading to propagating concentration and temperature fronts. The detailed insight gained from these measurements will be utilized in the development of microkinetic and reactor models leading to improved designs and operating strategies.Broader Impact: The broader impact of this study is the development of spatially-resolved mass spectrometry as a new tool to study catalysis in heterogeneous reactors and to closely couple such experiments with spatial/multi-dimensional catalytic reactor modeling. The study will advance the understanding of emerging catalytic processes critical to the environment and alternative energy; specifically lean NOx storage and reduction, selective catalytic reduction, and hydrogen generation and purification during autothermal reforming in catalytic membrane reactors.