During the past decades, reactive distillation has received intensive attention due to the well known benefits of integrating distillation with reaction in a single unit. Significant capital savings, improved conversion and selectivity, avoidance of azeotropes, together with heat integration are some of the main advantages of using reactive distillation. Many applications have proven to be economically advantageous by using reactive distillation (e.g. MTBE and TAME synthesis, production of methyl-acetate, manufacture of di-isopropyl-ether, oligomerisation of linear butenes and others). Whereas there are many procedures available for the synthesis of non-reactive columns or reactive-separation systems, the synthesis of reactive distillation columns is still a challenge, due to the complexity and the high number of design parameters involved. Available conceptual design methods generally address three (or four) components and fully reactive columns, but there is still a lack of systematic conceptual design methods for more general column configurations and for multi-component systems. The aim of this work is to develop a methodology to identify promising column configurations and to obtain column design parameters (number of reactive and non-reactive stages, reflux and reboil ratios, feed condition) for a given feed mixture and a set of desired products. A new systematic design method for reactive systems reaching equilibrium allows the analysis of the impact of different configurations (fully reactive or hybrid columns) and feed policies (single- or double-feed columns) on column performance. The methodology is extended to account for kinetically-controlled reactions in synthesis and design of reactive distillation columns. Systems with two degrees of freedom (according to the Gibbs phase rule) were considered for equilibrium reactions, and ternary and quaternary systems for kinetically-controlled reactions. Reactive distillation column designs generated by the methodology are presented as illustrative examples. Their predicted performances are shown to be in good agreement with those predicted by rigorous simulation using HYSYS. The approach can easily be automated and typically generates multiple designs, allowing a design engineer to efficiently compare various design options including hybrid and fully reactive columns, single- and double-feed configurations, and different sets of operating parameters for a given column configuration. The new methodology developed in this work facilitates a stepchange in conceptual design practice, offering a systematic and easy to use tool for the synthesis and design of reactive distillation columns.

Yes / In this work, for the first time, the synthesis of benzyl acetate via the esterification of acetic acid and benzyl alcohol is investigated in the reactive distillation system using a middle vessel (MVD), inverted (IBD), and conventional batch reactive distillation columns. The measurement of the performance of these column schemes is determined in terms of profitability through minimization of the batch time for a defined separation task. The control variables (reboil ratio for MVD, IBD columns) and (reflux ratio in case of CBD column) are considered as piecewise constants over batch time. The optimization results obviously indicate that the CBD system is a more attractive process in terms of batch time reduction, and maximum achievable yearly profit as compared to the MVD, and IBD operations.

This thesis presents advancements in the development of hybrid and data-driven models of distillation columns. First, it introduces a hybrid model structure that incorporates a novel multiplicative correction term for inferential monitoring. This model architecture outperforms previous hybrid structures, especially in extrapolation conditions, and can be adapted for different conditions. Second, it presents a methodology for selecting temperature measurement for inferential models. This methodology demonstrates that nonlinear columns can be effectively modeled with linear models requiring two temperature measurements per section (previous works state requiring more) when the measurements are selected systematically. Finally, an iterative Real-Time Optimization (RTO) based on an augmented inferential data-driven model is demonstrated. The accuracy of the model enables estimation of the sensitivity matrix of the plant from the model without the need for additional plant measurements. The proposed RTO framework produces results similar to those achieved by optimizing rigorous tray to tray distillation models. / Thesis / Candidate in Philosophy / This thesis presents advancements in the development of hybrid and data-driven models of distillation columns. First, it introduces a hybrid model structure that incorporates a novel multiplicative correction term for inferential monitoring. This model architecture outperforms previous hybrid structures, especially in extrapolation conditions, and can be adapted for different conditions. Second, it presents a methodology for selecting temperature measurement for inferential models. This methodology demonstrates that nonlinear columns can be effectively modeled with linear models requiring two temperature measurements per section (previous works state requiring more) when the measurements are selected systematically. Finally, an iterative Real-Time Optimization (RTO) based on an augmented inferential data-driven model is demonstrated. The accuracy of the model enables estimation of the sensitivity matrix of the plant from the model without the need for additional plant measurements. The proposed RTO framework produces results similar to those achieved by optimizing rigorous tray to tray distillation models.

Nowadays, industrial processes are having to be rapidly developed to meet high standards regarding increases in the production rate and/or improving product quality. Fulfilling these requirements is having to work in tandem with the pressure to reduce energy consumption due to global environmental regulations. Consequently, most industrial processes critically rely on automatic control, which can provide efficient solutions to meet such challenges and prerequisites. For this thesis, an intelligent system design has been investigated for controlling the distillation process, which is characterised by highly nonlinear and dynamic behaviour. These features raise very challenging tasks for control systems designers. Fuzzy logic and artificial neural networks (ANNs) are the main methods used in this study to design different controllers, namely: PI- PD- and PID-like fuzzy controllers, ANN-based NARMAL2 in addition to a conventional PID controller for comparison purposes. Genetic algorithm (GA) and particle swarm optimisation (PSO) have also been utilised to tune fuzzy controllers by finding the best set of scaling factors. Finally, an intelligent controller is proposed, called ANFIS-based NARMA-L2, which uses ANFIS as an approximation approach for identifying the underlying systems in a NARMA-L2 configuration. The controllers are applied to control two compositions of a binary distillation column, which has been modelled and simulated in MATLAB® and on the Simulink® platform. Comparative analysis has been undertaken to investigate the controllers' performance, which shows that PID-like FLC outperforms the other tested fuzzy control configurations, i.e. PI- and PD-like. Moreover, PSO has been found to outperform GA in finding the best set of scaling factors and over a shorter time period. Subsequently, the performance of PID-like FLC has been compared with ANN-based NARMA-L2 and the proposed ANFIS-based NARMA-L2, by subjecting the controlled column to different test scenarios. Furthermore, the stability and robustness of the controllers have been assessed by subjecting the controlled column to inputs variance and disturbances situations. The proposed ANFIS-based NARMAL2 controller outperforms and demonstrates more tolerance of disturbances than the other controllers. Finally, the study has involved investigating the control of a multicomponent distillation column due to its significant enhancement in operational efficiency regarding energy saving and recent widespread implementation. That is, Kaibel's distillation column with 4×4 configuration has been simulated also in MATLAB® and on the Simulink® platform with the proposed controller being implemented to control the temperatures of the column and the outcomes subsequently compared with conventional PID controllers. Again, the novel controller has proven its superiority regarding the disturbances tolerance as well as dealing with the high dynamics and nonlinear behaviour.

A reactive distillation column for the alkylation of benzene with long chain linear olefin was studied. The study involved design, construction, experimentation, and simulation of the column. Establishing the design required study of reaction rates, thermodynamic relationships, and packing structures. A heuristic was developed for the design of such columns. This heuristic involved estimating an amount of catalyst loading and subsequently determining the operating parameters for a column. This method is particularly applicable to systems with high concentrations of inert feeds. A column was constructed following the design. Data was collected from the column and compared to simulations. The simulations were performed with Aspen Plus RADFRAC. In this manner, the data was used to validate the commercial steady state models for reactive distillation. In addition, dynamic simulations of the system were performed. These dynamic simulations provided insight into more design considerations. For example, steady state simulations indicated an optimal feed stage based on steady state conversion of the olefin. However, the dynamic simulations showed a potential disadvantage to the utilization of the optimal feed stage. With some disturbances, a column configured with the feed stage with the highest steady state conversion also deviated from the steady state faster and with greater amplitude than other configurations. These considerations were further explored in developing a control scheme for reactive distillation columns. Control of reactive distillation differs from traditional distillation in that one control variable is conversion. Traditional distillation generally focuses on production rates and product purity. To this end, control schemes were analyzed and dynamic simulations were performed. These simulations showed an advantage to a variable pairing in which duty is paired with conversion. The conversion was inferred from a stage temperature in the reactive zone. In addition, distillate rate may be paired with product composition. In conclusion, the reactive distillation column design for long chain olefin alkylation of benzene requires careful estimation of catalyst requirements and valid simulation tools. In addition, dynamic response should be considered in the design. Finally, a simple inferential control scheme may be adequate. / text

Este trabalho apresenta todos os passos para a implementação de técnicas de controle preditivo em uma coluna de destilação. Inicialmente a tese introduz basicamente o funcionamento e a meta do processo de destilação. Modelos linearizados em tempo contínuo da coluna de destilação são obtidos a partir de ensaios experimentais da coluna em diferentes pontos de operação. Com base nestes modelos, várias topologias de controladores preditivos baseados em modelo são implementadas. Um otimizador em tempo real é integrado aos controladores preditivos para a redução do custo operacional da planta. Resultados simulados e resultados experimentais de todas as topologias de controladores preditivos estudados são apresentados. / This work presents all the steps to the implementation of predictive control techniques in a distillation column. First the thesis basically introduces the working and the goal of the distillation process. Linearized models in continuous time of the distillation column are obtained from experimental tests of the column in different operating points. Based on this models, several model based predictive controllers topologies are implemented. A real time optimizer is integrated with the predictive controllers to the reduction of the plant operational cost. Simulated results and experimental results of all studied predictive controllers topologies are presented.

Este trabalho aborda a predição da eficiência de pratos valvulados de dois passes, de escoamento cruzado com downcomers de uma coluna de destilação industrial, através do uso de diferentes modelos com e sem o uso do método Stagnant Regions Model proposto por Lockett em 1986. Contrariando o esperado, poucos artigos foram publicados sobre as principais características de pratos valvulados e bem menos sobre eficiência de pratos valvulados de dois passes. Os resultados encontrados sugerem que a correlação de O'Connell, o modelo de Chan e Fair aplicado aos pratos valvulados de dois passes convertidos para um passe e o modelo de Chan e Fair com uso do método SRM são os que melhor predizem a eficiência de pratos valvulados de dois passes, de escoamento cruzado com downcomers, no caso estudado.Em consonância com os estudos prévios, a correlação de O'Connell subestima o valor da eficiência, mostrando-se levemente conservativa, enquanto as predições pelo uso do modelo de Chan e Fair e do modelo modificado de Chan e Fair com uso do comprimento equivalente proposto por Klemola e Ilme superestimam o valor da eficiência, mostrando-se levemente não-conservativas. / This work approaches the prediction of the efficiency of two passes, crossflow valve trays with downcomers of an industrial distillation column, through the use of different models with and without the use the Stagnant Regions Model, method proposed by Lockett in 1986.Contradicting what it could be expected, few papers were published about the main characteristics of valve trays and fewer about efficiency of two passes valve trays. The results suggest that the O'Connell's correlation, the model of Chan and Fair applied to the two passes valve trays converted for one pass valve tray and the model of Chan and Fair with SRM method are those that best predict the efficiency of two passes, crossflow valve trays with downcomers. In consonance with the previous published studies, the O'Connell'correlation underestimates the value of the efficiency, showing a slightly conservative value, while the predictions using Chan and Fair model and the modified Chan and Fair model with equivalent length proposed by Klemola and Ilme overestimates the value of the efficiency, showing a slightly non-conservative results.

O aumento do custo e da demanda de energia, juntamente com a escassez de recursos não renováveis e o crescente apelo para a sustentabilidade dos processos, incentiva o desenvolvimento de equipamentos e sistemas mais eficientes mediante a otimização e o controle dos recursos energéticos disponíveis. A proposta deste trabalho consiste em estabelecer uma abordagem termodinâmica para o controle e a otimização de processos visando o aumento da eficiência na operação dos mesmos. Para tanto, foi desenvolvido um problema de controle ótimo formulado com base no critério de eficiência termodinâmica de acordo com a 2ª Lei, com o objetivo de otimizar a transição entre estados com respeito a taxa de geração de entropia do sistema, mantendo as variáveis controladas como restrições de desigualdade dependentes do tempo. A estratégia proposta, chamada COBET (controle baseado na eficiência termodinâmica), foi aplicada a uma coluna de destilação binária para controlar a pureza do destilado e do produto de fundo, manipulando a razão de refluxo e a taxa de transferência de calor do refervedor. O COBET apresentou ajuste simples, tempo computacional razoável e desempenho de controle aceitável, quando comparado com controladores convencionais. Foi proposta uma estratégia alternativa, de modo a aprimorar o COBET, chamada R-COBET, que consiste no uso de restrições adicionais que garantem que as variáveis de controle permaneçam entre o estado inicial e final. O R-COBET obteve um desempenho aceitável, menor integral do erro quadrático das variáveis de controle e maior lucro, quando comparado ao COBET. A fim de demonstrar a aplicabilidade da metodologia proposta a outras funções objetivo, uma função empírica de eficiência baseada na 1ª Lei da Termodinâmica foi determinada e utilizada no problema de controle ótimo, sujeito às mesmas restrições consideradas no controlador R-COBET. Também se aplicou a metodologia proposta a um reator CSTR com o intuito de controlar a temperatura e a concentração do produto, considerando-se o controlador na forma R-COBET, e obteve-se um desempenho similar ao do estudo da coluna de destilação. Com estas análises, concluiu-se que a metodologia proposta pode ser aplicada com sucesso a problemas de controle ótimo com estados final e inicial definidos. / The increasing demand of energy and its rising costs, in addition to the non-renewable resources depletion and to the growing interest in the sustainability in industrial processes, stimulate the development of equipment and systems that are more efficient through the control and optimization of available energy resources. The purpose of this work is to establish a thermodynamic approach to process control and optimization, in order to improve operational efficiency. To this end, it is developed in this work an optimal control problem formulated on the basis of a thermodynamic efficiency criterion, as dictated by the 2nd Law. The principle is to optimize the transition between states with respect to thermodynamic efficiency – regarded as the square of entropy generation rate – while maintaining the controlled variables as time dependent inequality constraints. The proposed strategy, called here TEBC (Thermodynamic Efficiency Based Control) was applied to a binary distillation column in order to control distillate and bottom product purities within specifications while manipulating the reflux ratio and reboiler heat transfer rate. When compared to other controllers, TEBC presented practical tuning, reasonable computational time and acceptable control performance. An alternative strategy was also proposed in order to improve TEBC, called R-TEBC, which considers additional constraints to ensure that control variables remain between the initial and final states. The R-TEBC achieved acceptable performance, smaller integral squared error in the control variables and larger profit, when compared to TEBC. In order to demonstrate the applicability of the proposed methodology to other objective functions, an empirical efficiency function was proposed for the distillation column example and used in the optimal control problem, in the form of a R-TEBC controller. Moreover, an exothermic CSTR reactor with product concentration and reactor temperature as controlled variables was also studied, using additional constraints (R-TEBC), and the results was similar to those obtained in the distillation column. With this analysis, it was concluded that the proposed methodology can be applied to optimal control problems of this kind with fixed initial and final states.

Este trabalho aborda a predição da eficiência de pratos valvulados de dois passes, de escoamento cruzado com downcomers de uma coluna de destilação industrial, através do uso de diferentes modelos com e sem o uso do método Stagnant Regions Model proposto por Lockett em 1986. Contrariando o esperado, poucos artigos foram publicados sobre as principais características de pratos valvulados e bem menos sobre eficiência de pratos valvulados de dois passes. Os resultados encontrados sugerem que a correlação de O'Connell, o modelo de Chan e Fair aplicado aos pratos valvulados de dois passes convertidos para um passe e o modelo de Chan e Fair com uso do método SRM são os que melhor predizem a eficiência de pratos valvulados de dois passes, de escoamento cruzado com downcomers, no caso estudado.Em consonância com os estudos prévios, a correlação de O'Connell subestima o valor da eficiência, mostrando-se levemente conservativa, enquanto as predições pelo uso do modelo de Chan e Fair e do modelo modificado de Chan e Fair com uso do comprimento equivalente proposto por Klemola e Ilme superestimam o valor da eficiência, mostrando-se levemente não-conservativas. / This work approaches the prediction of the efficiency of two passes, crossflow valve trays with downcomers of an industrial distillation column, through the use of different models with and without the use the Stagnant Regions Model, method proposed by Lockett in 1986.Contradicting what it could be expected, few papers were published about the main characteristics of valve trays and fewer about efficiency of two passes valve trays. The results suggest that the O'Connell's correlation, the model of Chan and Fair applied to the two passes valve trays converted for one pass valve tray and the model of Chan and Fair with SRM method are those that best predict the efficiency of two passes, crossflow valve trays with downcomers. In consonance with the previous published studies, the O'Connell'correlation underestimates the value of the efficiency, showing a slightly conservative value, while the predictions using Chan and Fair model and the modified Chan and Fair model with equivalent length proposed by Klemola and Ilme overestimates the value of the efficiency, showing a slightly non-conservative results.

O aumento do custo e da demanda de energia, juntamente com a escassez de recursos não renováveis e o crescente apelo para a sustentabilidade dos processos, incentiva o desenvolvimento de equipamentos e sistemas mais eficientes mediante a otimização e o controle dos recursos energéticos disponíveis. A proposta deste trabalho consiste em estabelecer uma abordagem termodinâmica para o controle e a otimização de processos visando o aumento da eficiência na operação dos mesmos. Para tanto, foi desenvolvido um problema de controle ótimo formulado com base no critério de eficiência termodinâmica de acordo com a 2ª Lei, com o objetivo de otimizar a transição entre estados com respeito a taxa de geração de entropia do sistema, mantendo as variáveis controladas como restrições de desigualdade dependentes do tempo. A estratégia proposta, chamada COBET (controle baseado na eficiência termodinâmica), foi aplicada a uma coluna de destilação binária para controlar a pureza do destilado e do produto de fundo, manipulando a razão de refluxo e a taxa de transferência de calor do refervedor. O COBET apresentou ajuste simples, tempo computacional razoável e desempenho de controle aceitável, quando comparado com controladores convencionais. Foi proposta uma estratégia alternativa, de modo a aprimorar o COBET, chamada R-COBET, que consiste no uso de restrições adicionais que garantem que as variáveis de controle permaneçam entre o estado inicial e final. O R-COBET obteve um desempenho aceitável, menor integral do erro quadrático das variáveis de controle e maior lucro, quando comparado ao COBET. A fim de demonstrar a aplicabilidade da metodologia proposta a outras funções objetivo, uma função empírica de eficiência baseada na 1ª Lei da Termodinâmica foi determinada e utilizada no problema de controle ótimo, sujeito às mesmas restrições consideradas no controlador R-COBET. Também se aplicou a metodologia proposta a um reator CSTR com o intuito de controlar a temperatura e a concentração do produto, considerando-se o controlador na forma R-COBET, e obteve-se um desempenho similar ao do estudo da coluna de destilação. Com estas análises, concluiu-se que a metodologia proposta pode ser aplicada com sucesso a problemas de controle ótimo com estados final e inicial definidos. / The increasing demand of energy and its rising costs, in addition to the non-renewable resources depletion and to the growing interest in the sustainability in industrial processes, stimulate the development of equipment and systems that are more efficient through the control and optimization of available energy resources. The purpose of this work is to establish a thermodynamic approach to process control and optimization, in order to improve operational efficiency. To this end, it is developed in this work an optimal control problem formulated on the basis of a thermodynamic efficiency criterion, as dictated by the 2nd Law. The principle is to optimize the transition between states with respect to thermodynamic efficiency – regarded as the square of entropy generation rate – while maintaining the controlled variables as time dependent inequality constraints. The proposed strategy, called here TEBC (Thermodynamic Efficiency Based Control) was applied to a binary distillation column in order to control distillate and bottom product purities within specifications while manipulating the reflux ratio and reboiler heat transfer rate. When compared to other controllers, TEBC presented practical tuning, reasonable computational time and acceptable control performance. An alternative strategy was also proposed in order to improve TEBC, called R-TEBC, which considers additional constraints to ensure that control variables remain between the initial and final states. The R-TEBC achieved acceptable performance, smaller integral squared error in the control variables and larger profit, when compared to TEBC. In order to demonstrate the applicability of the proposed methodology to other objective functions, an empirical efficiency function was proposed for the distillation column example and used in the optimal control problem, in the form of a R-TEBC controller. Moreover, an exothermic CSTR reactor with product concentration and reactor temperature as controlled variables was also studied, using additional constraints (R-TEBC), and the results was similar to those obtained in the distillation column. With this analysis, it was concluded that the proposed methodology can be applied to optimal control problems of this kind with fixed initial and final states.