【作者】 胡永有；

【导师】 褚健； 苏宏业；

【作者基本信息】 浙江大学 ， 控制科学与工程， 2004， 博士

【摘要】 流程模拟优化技术在流程工业得到了广泛应用，带来了显著的经济效益，特别是用于复杂催化反应过程的专用模拟优化软件日益受到了石油化工和炼油企业的重视和青睐。本论文围绕催化重整过程，对重整反应机理、过程模型建立、模型参数估计、过程优化等问题进行了研究。论文面向工业应用，其目标是开发出自主的、应用方便的、功能齐全的专用催化重整流程模拟优化软件。本论文的主要研究工作包括以下几个方面内容。 1．研究了催化重整反应机理，针对国内工业重整装置的特点和应用条件，提出了只包含17个重整反应的17集总反应动力学模型，保证模型较高精度，并降低机理模型复杂度和化验室分析要求，方便了模型工业应用。深入探讨了重整催化剂的结焦失活机理，首次提出了连续重整装置催化剂失活的平均活性函数概念，给出了催化剂结焦失活模型。讨论了加热炉的传热机理，给出了一个简化的加热炉模型。针对含氢混合物的特殊性，提出了采用不含氢汽液分离系统替代含氢汽液分离系统的汽液平衡计算模型。 2．讨论了过程模拟中集总组分6种重要物性计算方法和机理模型参数估计方法。针对反应模型待估参数过多的特点，把模型参数进行分类和归并，使待估参数从68个减少为17个，降低了参数估计的难度。提出了采用动态结焦模型以及新鲜催化剂结焦速率的线性回归模型来估计结焦模型参数的方法。研究了机理模型参数估计算法，提出了基于BFGS变尺度和微分精确线性搜索的优化算法求解参数估计优化问题，取得了理想的收敛效果。 3．针对重整反应模型方程的特殊结构和刚性问题，提出了一种形式更简单方便的近似解析数值算法和吉尔法相结合的混合数值算法，并引入了最优步长方法。 4．对重整过程优化问题进行了分析描述，采用有效的SQP算法对该非线性规划问题进行了求解。讨论了机理模型参数误差对优化结果的影响，说明了基于该静态模型的离线优化结果是可靠的。 5．研究了重整过程动态特性。在静态模型基础上建立了全流程主要装置(重整反应器、加热炉、分离罐)的动态模型，采用分段线性化方法对重整反应分布参数模型离散化成一组常微分线性方程组进行了求解。最后利用该动态模型分析了主要操作变量的闭环动态响应曲线。浙江大学博士学位论文6.在MATLAB平台上开发了基于图形用户界面的专用重整模拟优化软件，利用 一套半再生重整工业装置和两套连续重整工业装置数据对建立的过程模型 进行了验证，表明了模型的有效性和应用方便性。利用模型对重整过程主要 操作变量进行了分析，说明了模型在过程分析和操作指导上的重要意义。 最后，在总结全文研究工作的基础上，指出了重整流程模拟优化技术在开发和应用中需要进一步解决的问题。更多还原

【Abstract】 The process simulation and optimization technology is widely applied to the process industry and brings large profits for related plants and companies. Especially the special simulation and optimization software on complex catalytic reaction process is more important and pursued by the corporations and institutes involved.In this dissertation, the reaction kinetics, modeling and optimization of naphtha catalytic reforming process, which is a very important process in hydrocarbon processing industry for octane improvement or as sources of aromatics and hydrogen, is studied. The objective of this dissertation is to develop the simulation and optimization software with good features of easy using and complete functions and to apply to commercial naphtha catalytic reforming processes. In this dissertation, the main contributions are as follows.1. The kinetics of naphtha catalytic reforming reactions are studied and a kinetics-based reaction model with only 17 lumps consisting of PNA (Paraffins, Naphthenes and Aromatics) and 17 reactions is developed according to the character and applying conditions of domestic industrial reformers. The lumping scheme and reaction network of this model largely decrease the complexity of model and demand for detailed component analysis, so it is easy to apply this model to the commercial units. The catalyst coking model with average activation function of catalyst is presented. The heat transferring model of furnace and gas-liquid balancing separation model are also described here.2. The calculation methods of physical and chemical properties of lumps are presented and the model kinetic parameters are benchmarked with plant data. The procedure of parameter estimation is done by minimization of the sum of the squares of the deviations between plant and predicted values of key variables. In order to decrease the difficulty of parameters estimation, a new parameter estimation method is proposed and the estimated parameters are drastically decreased from 68 to 17. A dynamic catalyst coking model and multi-variant linear regression model are used to estimate the parameters of catalyst coking model. Especially parameter estimation algorithms are discussed and a new method based on BFGS and differential precise linear searching is proposed tosolve the unconstrained optimization problem successfully deriving from parameter estimation. This new algorithm looses the strict demand for the initial point and also avoids the inverse operation of Jacobin matrix.3. A new numerical algorithm integrating a quasi-analytic numerical algorithm with the Gear numerical algorithm is used to solve the ordinary differential equations with stiff problem. To accelerate the solving of ODE, the optimum step method is introduced into the composite numerical algorithm.4. Process optimization based on kinetic model is studied. The solving of process optimization problem with process constraints is performed by SQP. And the sensitiveness analysis of optimization results to the kinetic parameter errors is also given.5. A dynamic model of catalytic reforming process is described and the dynamics of this process are studied. The dynamic model is a typical nonlinear distributed-parameter system with high dimension about19XN X4, where N is the section number in one reformer. Method of lines is adopted to reduce these partial differetial equations (PDEs) into N lumped-parameter ordinary differetial equations (ODEs) solved by numerical algorithm. The responses with the step or impulse disturbances of key process variables such as reaction temperature, pressure and feed charge are given and the agreements between dynamic model calculation and static model calculation are satisfactory.6. The process simulation and optimization software with Graphic User Interface (GUI) is developed with MATLAB language based on MATLAB platform. With this software, the model parameters are benchmarked with plant data and the simulation results of the model validated for更多还原