Natural gas sweetening using low temperature distillation: simulation and configuration

ABSTRACT

Hypothesis: Separation of CO₂ from a stream of natural gas using low-temperature distillation process is complicated not only because of the existence of ethane (C₂) and CO₂ azeotrope but owing to the freezing of CO₂. A modified process based on an existing Ryan–Holmes process in the form of a low-temperature distillation is presented here for the separation of sour gases. In addition, solvents were employed to prevent CO₂ freezing and to avoid formation of the C₂-CO₂ azeotrope.

Simulation: Simulation calculations were carried out using a natural gas stream containing CO₂ and H₂S. The process was designed and simulated using Aspen HYSYS 9.

Findings: A low-temperature process for the separation of a feed stream containing up to 30 mole% CO₂ and 2.5 mole% H₂S was achieved, which lowered the levels of these gases to within 50 and 4 ppm, respectively. These values conform to liquefied natural gas specifications. The compositions of the product streams, the required solvent circulation flow rates, and the total energy requirements were estimated. The reported process successfully separated H₂S and produced CO₂ at a pressure of 25.0 bar and a temperature of ?13°C, thereby ensuring its suitability for application in enhanced oil recovery. This described process also delivered the desired natural gas product at 35 bar and ?90°C ready for liquefaction and further cooling.     

“背包式”反应精馏水解乙酸甲酯的工艺

采用“背包式”反应精馏深度水解乙酸甲酯,考察了工艺条件对水解率和酸水比的影响,并与传统的单塔催化精馏工艺进行了对比。结果表明：提高水酯比可以显著提高乙酸甲酯的水解率;回流进料比的增加有利于提高水解率但会增加能耗,较佳回流比为3.0左右;乙酸甲酯水解率随空速的增加而降低的速度较慢,可以适当提高空速以增加处理能力;增加固定床体积有利于酯的预水解,但是不一定有利于酯的总转化率。采用“背包式”催化精馏工艺可以实现乙酸甲酯的深度水解,且优于传统的单塔催化精馏工艺。     

Investigation of a rotating disc reactor for acetone stripping and asymmetric transfer hydrogenation: Modelling and experiments

Asymmetric transfer hydrogenation of acetophenone with isopropanol as hydrogen donor in the presence of a homogeneous catalyst was investigated in a rotating disc reactor. Initially, acetone stripping from binary mixtures acetone-isopropanol with nitrogen as inert gas was studied, since its removal is a key issue in improving reaction performance. The reactor consisted of a stainless steel disc mounted on a horizontal shaft, accommodated in a cylindrical shell. The disc was partially immersed in the liquid phase. Its rotation generated a thin liquid film on its upper part, which could be brought in contact with a gas phase used for stripping. A mathematical model was formulated to simulate the reactor and showed good agreement with experimental data for acetone stripping. It was observed that the efficiency of acetone removal from the liquid phase increased with the gas flowrate per initial liquid volume ratio. The effect of disk rotation was found to be small when the stripping gas was introduced in the liquid bulk. The reactor model agreed well with experimental data of the asymmetric transfer hydrogenation. An advantage of the rotating disk reactor is that the hydrodynamics of the phases can be decoupled and the gas flowrate can be increased without constraints in the liquid phase, unlike conventional agitated reactors that are limited by flooding. Simulations using high stripping gas flowrate per initial liquid volume, unachievable in stirred reactors, showed significant reduction of the residence time required to achieve >99% conversion.     

Modelling and control of a continuous distillation tower through fuzzy techniques

This paper presents a methodology for the design of a fuzzy controller applicable to continuous processes based on local fuzzy models and velocity linearizations. It has been applied to the implementation of a fuzzy controller for a continuous distillation tower. Continuous distillation towers can be subjected to variations in feed characteristics that cause loss of product quality or excessive energy consumption. Therefore, the use of a fuzzy controller is interesting to control process performance.A dynamic model for continuous distillation was implemented and used to obtain data to develop the fuzzy controller at different operating points. The fuzzy controller was built by integration of linear controllers obtained for each linearization of the system. Simulation of the model with controller was used to validate the controller effectiveness under different scenarios, including a study of the sensibility of some parameters to the control.The results showed that the fuzzy controller was able to keep the target output in the desired range for different inputs disturbances, changing smoothly from a predefined target output to another. The developed techniques are applicable to more complex distillation systems including more operating variables.     

Modelling a catalytic membrane reactor with plug flow pattern and a hypothetical equilibrium gas-phase reaction with Δn ≠ 0

The scope of this paper is to present a theoretical study of a catalytic polymeric dense membrane reactor (CPDMR) assuming isothermal conditions, plug flow pattern without pressure drop in both retentate and permeate sides, shell side feed and cocurrent operation. The conversion enhancement over the thermodynamic equilibrium value is studied for a gas-phase reaction of the type aAbB, considering two different stoichiometric ratios: Δn > 0 and Δn < 0, where Δn = b − a. For each of these cases, the influence of the relative sorption and diffusivity of the reaction species is studied. It is concluded that the conversion of a reversible reaction can be significantly enhanced when the diffusivity of the reaction products is higher than that of the reactants and/or the sorption is lower. It is also concluded that, even for equal sorption and diffusion coefficients, the conversion could also be improved for reactions with Δn ≠ 0. The extension of this enhancement depends on the reaction stoichiometry, the overall concentration inside the membrane, the Thiele modulus, and the contact time.     

Modelling hydrate formation kinetics of a hydrate promoter-water-natural gas system in a semi-batch spray reactor

Hydrate formation kinetic modelling studies reported so far mainly concentrates on pure water-gas systems in stirred-tank batch environments. This work proposes a model for gas hydrate formation kinetics of a hydrate promoter-water-natural gas system in a semi-batch reactor assuming steady-state, isothermal and isobaric conditions. The hydrate formation kinetics was modelled after extending the recent method proposed by Kashchiev and Firoozabadi (J. Crystral Growth 241 (2002a) 220; J. Crystal Growth 243 (2002b) 476; J. Crystal Growth 250 (2003) 499) for a single component gas-water system to a multi-component gas-water-additive system. The extended Kashchiev and Firoozabadi model was applied for a semi-batch spray reactor here for the first time. The hydrate formation experiments were carried out in a pilot plant spray reactor at three different pressure-temperature regimes to determine the actual hydrate formation kinetics in the spray reactor. The experiment results were then used to finetune the adjustable parameters to facilitate accurate model predictions.     

Global modelling of a gas-liquid-solid airlift reactor

This paper presents a global model of three phase flow (gas-liquid-solid) in an internal airlift reactor. The airlift is composed of four zones: a riser (on the aerated side on the internal wall), a downcomer (on the opposite side) and two turning zones above and below the internal wall. Tap water is the liquid continuous phase and the dispersed phases are air bubbles and polyethylene particles. The global modelling of the airlift involves mass and momentum equations for the three phases. The model enables phase velocities and phase volume fractions to be estimated, which can be compared to experimental data. Closure relations for the gas and solid drift velocities are based on the model proposed by Zuber and Findlay. The drift flux coefficients are derived from CFD numerical simulations of the airlift. Gas bubble and solid particle averaged slip velocities are deduced from momentum balances, including drag coefficient correlations. The link between Zuber and Findlay model and the two-fluid model is established. In the experiment as well as in the model, the gas flow rate is fixed. However, the liquid and solid flow rates are unknown. Two closure relations are needed to predict these flow rates: the first closure relation expresses that the volume of solid injected into the airlift remains constant; the second closure relation expresses a global balance between the difference of column height in the riser and the downcomer and the total pressure drop in the airlift. The main parameters of a three phase airlift reactor, like gas and solid volume fractions, are well predicted by the global model. With increasing solid filling rate (40%), the model starts to depart from the experimental values as soon as coalescence of bubbles appears.     

Analysis of packed distillation columns with a rate-based model

Multicomponent packed column distillation is simulated using a rate-based model and the simulation results are compared with the experimental results obtained from a 0.2 m diameter pilot-scale packed column. The simulation algorithm used is previously proposed by the authors, which based on an equation-tearing method for (6c+7) equations of one packing segment and the whole column is solved by an iterative segmentwise calculation with the overall normalized θ method for acceleration. The performance of two packings is examined by simulating the pilot-scale column experiments using the published correlations for estimating liquid and vapor phase mass transfer coefficients and an effective interfacial area.     

Modelling and Analysis of Electro‐chemical,Thermal, and Reactant Flow Dynamics for a PEM Fuel Cell System

In this paper an approach for the dynamic modelling of polymer electrolyte membrane fuel cells is presented. A mathematical formulation based on empirical equations is discussed and several features, exhibiting dynamic phenomena, are investigated. A generalized steady state fuel cell model is extended for the development of a method for dynamic electrochemical analysis. Energy balance and reactant flow dynamics are also explained through physical and empirical relationships. A well‐researched system (Ballard MK5‐E stack based PGS‐105B system) is considered in order to understand the operation of a practical fuel cell unit. Matlab‐SIMULINK^TM has been used in simulating the models. The proposed method appears to be relatively simple and consequently requires less computation time. Simulation results are compared with available experimental findings and a good match has been observed.     

乙烯淤浆聚合反应器的模型与模拟

建立了乙烯淤浆聚合反应器的多相全混流模型,描述了包括乙烯共聚合反应动力学、气液和液固传质、反应器传热在内的物理化学过程。通过模拟计算分析了聚合过程的控制步骤,得到了反应器生产能力与有关操作变量之间的关系,对某工业反应器的模拟结果表明计算值与生产数据具有很好的一致性。     

Design of a fully thermally coupled distillation column based on dynamic simulations

A dynamic simulation of a fully thermally coupled distillation column is conducted for the design of a possible operation scheme, and its performance is examined with an example process of butanol isomer ternary system. The outcome of the dynamic simulation indicates that the column can be operated by using a 3 × 3 control structure. The structure consists of three controlled variables of the compositions of overhead, bottom and side products and three manipulated variables of the flow rates of reflux and steam and liquid split ratio between a main column and a prefractionator. This paper was presented at The 5th International Symposium on Separation Technology-Korea and Japan held at Seoul between August 19 and 21, 1999.     

The use of dilute acetic acid for butyl acetate production in a reactive distillation: Simulation and control studies

The recovery of dilute acetic acid, which is widely found as a by-product in many chemical and petrochemical industries, becomes an important issue due to economic and environmental awareness. In general, separation of acetic acid in aqueous solution by conventional distillation columns is difficult, requiring a column with many stages and high energy consumption. As a result, the primary concern of the present study is the application of reactive distillation as a potential alternative method to recover dilute acetic acid. The direct use of dilute acetic acid as reactant for esterification with butanol to produce butyl acetate in the reactive distillation is investigated. Simulation studies are performed in order to investigate effect of the concentration of dilute acetic acid and key process parameters on the performance of the reactive distillation in terms of acetic acid conversion and butyl acetate production. In addition, three alternative control strategies are studied for the closed loop control of the reactive distillation. The control objective is to maintain the butyl acetate in a bottom product stream at the desired purity of 99.5 wt%.     

A simple,reliable and fast algorithm for the simulation of multicomponent distillation columns

This work has developed a simple, reliable and fast algorithm for the simulation of multicomponent distillation columns, where any equilibrium stage can accept a feed-stream and/or a vapor-side-stream and/or liquid-side-stream. The new scheme considers internal molar overflows and constant relative volatilities to avoid the need of heat balances and vapor–liquid equilibrium calculations. The solution scheme is founded on a Newton-based formulation in block algebra, which relies in a simple, reliable and fast algorithm. Although the proposed calculation scheme can be classified as an approximate method, it is very useful when accurate phase equilibrium and enthalpy data are lacking. Numerical experimentations show good agreement with the results obtained with well-known rigorous simulation approaches.     

Polymerisation of methyl methacrylate in a pilot-scale tubular reactor: modelling and experimental studies

A pilot-scale tubular reactor fitted with in-line static mixers is experimentally and theoretically evaluated for the polymerisation of methyl methacrylate (MMA). A non-isothermal and non-adiabatic axially dispersed plug-flow model is used to describe the flow characteristics of the reactor. The model is applied to the polymerisation of a concentrated MMA solution (up to 72% (v/v)). Key model parameters were attained through independent bench and pilot-scale experiments. Measured monomer conversions and polymer molecular weight were accurately predicted by model simulation. The presence of static mixers is shown to give near-ideal plug-flow operation for the experimental conditions of this study. Furthermore, an approximately four-fold increase in overall heat transfer coefficient is indicated due to the radial mixing incited by the mixers. Studies also demonstrated the importance of inhibitor kinetics on the dynamic and steady-state performance of the reactor.     

Comparison of the performance of a direct-contact bubble reactor and an indirectly heated tubular reactor for solar-aided methane dry reforming employing molten salt

A theoretical approach is presented for the comparison of two different atmospheric pressure reactors—a direct-contact bubble reactor (DCBR) and an indirectly heated tubular reactor (IHTR)—to evaluate the reactor performance in terms of heat transfer and available catalytic active surface area. The model considers the catalytic endothermic reactions of methane dry reforming that proceeds in both reactors by employing molten salts at elevated temperatures (700–900 °C) in the absence of catalyst deactivation effects. The methane conversion process is simulated for a single reactor using both a reaction kinetics model and a heat transfer model. A well-tested reaction kinetics model, which showed an acceptable agreement with the empirical observations, was implemented to describe the methane dry reforming. In DCBR, the heat is internally transferred by direct contact with the three phases of the system: the reactant gas bubbles, the heat carrier molten salts and the solid catalyst (Ni-Al₂O₃). In contrast, the supplied heat in the conventional shell-and-tube heat exchanger of the IHTR is transferred across an intervening wall. The results suggest a combination system of DCBR and IHTR would be a suitable configuration for process intensification associated with higher thermal efficiency and cost reduction.     

The effects of modes of hydrogen input and reactor configuration on reaction rate and H2 efficiency in the catalytic hydrogenation of alkynol to alkenol

Hydrogenation often involves three phases where hydrogen-on-demand is the typical mode of operation in industrial scale reactors. In research labs and publications, however, continuous hydrogen flow has been used. This paper investigates the effect of such modes of operation on reaction rate using a selective hydrogenation of 3-butyn-2-ol over Pd/Al₂O₃ to obtain 3-buten-2-ol as the model reaction. The two modes of operation were first tested in a commercial PARR stirred tank reactor and then repeated in an oscillatory baffled reactor (OBR) in order to validate the experimental results. Our investigation demonstrates that an enhanced reaction performance and 10 times better H₂ efficiency were obtained when the pressure was maintained constant during the reaction by feeding gas as required, ie hydrogen-on-demand mode. The method of a continuous flow of hydrogen in hydrogenation means that excess hydrogen is vented out when operating at ambient pressures or builds up at elevated pressures. Our work also enables a comparison of reactor designs on reactor performance, and three times higher H₂ efficiency and 2.3 times shorter residence time were achieved when using the OBR instead of the PARR due to its enhanced and uniform mixing, regardless of the mode of operation.