Modeling, Analysis and Control of Nonlinear Switching Systems

The first part of this two-part thesis examines the reverse-flow operation of auto-thermal methane reforming in a microreactor. A theoretical study is undertaken to explain the physical origins of the experimentally observed improvements in the performance of the reverse-flow operation compared to the unidirectional operation. First, a scaling analysis is presented to understand the effect of various time scales existing within the microreactor, and to obtain guidelines for the optimal reverse-flow operation. Then, the effect of kinetic parameters, transport properties, reactor design and operating conditions on the reactor operation is parametrically studied through numerical simulations. The reverse-flow operation is shown to be more robust than the unidirectional operation with respect to both optimal operating conditions as well as variations in hydrogen throughput requirements. A rational scheme for improved catalyst placement in the microreactor, which exploits the spatial temperature profiles in the reactor, is also presented. Finally, a design modification of the microreactor called "opposed-flow" reactor, which retains the performance benefits of the reverse-flow operation without requiring the input / output port switching, is suggested. In the second part of this thesis, a novel simulation-based Approximate Dynamic Programming (ADP) framework is presented for optimal control of switching between multiple metabolic states in a microbial bioreactor. The cybernetic modeling framework is used to capture these cellular metabolic switches. Model Predictive Control, one of the most popular advanced control methods, is able to drive the reactor to the desired steady state. However, the nonlinearity and switching nature of the system cause computational and performance problems with MPC. The proposed ADP has an advantage over MPC, as the closed-loop optimal policy is computed offline in the form of so-called value or cost-to-go function. Through the use of an approximation of the value function, the infinite horizon problem is converted into an equivalent single-stage problem, which can be solved online. Various issues in implementation of ADP are also addressed.Ph.D.Committee Chair: Jay H. Lee; Committee Member: Andrei G. Fedorov; Committee Member: Athanasios Nenes; Committee Member: Martha Gallivan; Committee Member: Matthew Realf

The Effect of Catalyst Placement on the Stability of a U-Bend Catalytic Heat-Recirculating Micro-Combustor: A Numerical Investigation

This study investigates the combined effect of catalyst placement and solid thermal conductivity on the stability of a U-bend catalytic heat-recirculating micro-combustor. The CFD code ANSYS Fluent 2020 R1 was used for two-dimensional simulations of lean premixed propane/air combustion by varying the inlet gas velocity, i.e., the input power. Three configurations were compared at low (3 W/(m K)) and high (30 W/(m K)) wall thermal conductivity: (A) the configuration in which both inner and outer walls are catalyst coated; (B) only the inner wall is catalyst coated; and (C) only the outer wall is catalyst coated. Numerical results show that, at low thermal conductivity, configuration (B) exhibits the same resistance to extinction as configuration (A), whereas at high thermal conductivity, configurations (B) and (C) exhibit much lower resistance to blowout than configuration (A). Accordingly, for low-power systems, which typically lose stability via extinction and thus require low-conductive materials, an optimal catalyst placement can be the partial coating of configuration (B). Conversely, for high-power systems, which are prone to blowout and thus require high-conductivity materials, a full coating of both the inner and outer walls is needed to guarantee higher stability. To elucidate these findings, a detailed analysis of the combustion behavior of the three configurations is presented

Millisecond Production of Hydrogen from Alternative, High Hydrogen Density Fuels in a Cocurrent Multifunctional Microreactor

A pseudo-2-dimensional model is used for modeling a multifunctional microreactor for hydrogen generation by coupling catalytic ammonia decomposition on ruthenium with catalytic propane combustion on platinum. The two reactions are carried out in adjacent parallel plate channels in a cocurrent flow mode. Operating lines defining the attainable region are computed. The high temperatures and fast heat transfer ensure that both reactions go to completion in as low as submillisecond contact times and enable compact hydrogen production for portable and distributed power generation. The ammonia decomposition reaction tends to be limited by the intrinsic rate of reaction, whereas catalytic combustion is also affected by mass and heat diffusion. We have found that moderate and high conductivity materials are preferable because they support a rather wide attainable region. We show that one such device could enable variable hydrogen supply for variable power needs. A simple operating strategy to dial in the desirable power is proposed, which ensures high thermal efficiency (∼75% once-through efficiency of the integrated device and ∼85% reformer efficiency, both without any heat recuperation), wall isothermicity, and high conversions. © 2009 American Chemical Society.status: publishe

Hierarchical multiscale model-based design of experiments, catalysts, and reactors for fuel processing

Abstract In this paper a hierarchical multiscale simulation framework is outlined and experimental data injection into this framework is discussed. Specifically, we discuss multiscale model-based design of experiments to optimize the chemical information content of a detailed reaction mechanism in order to improve the fidelity and accuracy of reaction models. Extension of this framework to product (catalyst) design is briefly touched upon. Furthermore, we illustrate the use of such detailed and reduced kinetic models in reactor optimization as an example toward more conventional process design. It is proposed that hierarchical multiscale modeling offers a systematic framework for identification of the important scale(s) and model(s) where one should focus research efforts on. The ammonia decomposition on ruthenium to produce hydrogen and the water-gas shift reactions on platinum for converting syngas to hydrogen serve as illustrative fuel processing examples of various topics. The former is used to illustrate hierarchical multiscale model development and model-based parameter estimation as well as product engineering. The latter is employed to demonstrate model reduction and process optimization. Finally, opportunities for process design and control in portable microchemical devices (lab-on-a chip) for power generation are discussed

Methane Steam Reforming at Microscales: Operation Strategies for Variable Power Output at Millisecond Contact Times

The potential of methane steam, reforming at microscale is theoretically explored. To this end, a multifunctional catalytic plate microreactor, comprising of a propane combustion channel and a methane steam reforming channel, separated by a solid wall, is simulated with a pseudo 2-D (two-dimensional) reactor model. Newly developed lumped kinetic rate expressions for both processes, obtained front a posteriori reduction of detailed microkinetic models, are used. It is shown that the steam, reforming at millisecond contact times is feasible at microscale, and in agreement with a recent experimental report. Furthermore, the attainable operating regions delimited from the materials stability limit, the breakthrough limit, and the maximum, power output limit are mapped out. A simple operation strategy is presented for obtaining variable power output along the breakthrough line (a nearly iso-flow rate ratio linej, while ensuring good overlap of reaction zones, and provide guidelines for reactor sizing. Finally, it is shown that the choice of the wall material depeneis on the targeted operating regime. Low-conductivity materials increase the methane conversion and power output at the expense of higher wall temperatures and steeper temperature gradients along the wall. For operation close to the breakthrough limit, intermediate conductivity materials, such as stainless steel, offer a good compromise between methane conversion and wall temperature. Even without recuperative heat exchange, the thermal efficiency of the multifunctional device and the reformer approaches -65% and -85%, respectively. © 2008 American Institute of Chemical Engineers.status: publishe