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1. INTRODUCTION There is a long and fairly rich literature that discusses the design and control issues involved in systems with high-temperature exothermic adiabatic tubular reactors. The design of the reactor in isolation is fairly straightforward. If the reaction is irreversible, there is usually a maximum temperature limitation due to catalyst degradation, undesirable side reactions, or materials-of-construction limitations. In this case, there is an optimum design in terms of reactor size, reactor inlet temperature, and per-pass conversion. The last of these design optimization variables impacts recycle ow rates and separation costs. The colder the reactor inlet temperature, the higher the conversion can be without exceeding the maximum temperature limitation. This reduces the required amount of recycle of unconverted reactants, which lowers separation costs. However, the size of the reactor increases as reactor inlet temperature is decreased, which increases capital investment in the reactor vessel and catalyst. If the reaction is reversible and exothermic, there is also an optimum design in terms of reactor size and reactor inlet temperature. But now the eect of temperature on the chemical equilibrium constant establishes the reactor inlet temperature that maximizes conversion. The reactor must be large enough to approach this limiting conversion. The maximum temperature limitation is usually not an issue. A number of alternative owsheets have been studied for this type of system, which is sometimes referred to as an autothermal reactor. Some of these congurations are illustrated in Figure 1. Heat-exchanger bypassing with no furnace is shown in owsheet A in Figure 1. This conguration has only one manipulated variable and can prevent a temperature runaway but cannot prevent a quench. Note that dual split-ranged valves are used to regulate the ows through and around the heat
2012 American Chemical Society
exchanger. A gas-phase system is assumed with a valve on the gas stream leaving the unit, which holds pressure in the gas system. The dual-valve setup is permitted in a gas system where pressures vary from location to location. This setup would not work in a liquid system since there would be two valves in series in a single liquid line. Heat-exchanger bypassing with a furnace before the reactor is shown in owsheet B in Figure 1. Now there are two control degrees of freedom (bypassing and furnace heat input). This conguration has the potential of being able to prevent both a quench (using furnace heat input to maintain reactor inlet temperature) and a temperature runaway (using bypassing) Flowsheet C in Figure 1 shows a process in which a cooler (steam generator) is used on the hot reactor euent before it enters the heat exchanger. The system also has two control degrees of freedom. Flowsheet D in Figure 1 illustrates the use of multiple FEHEs with multiple coolers, which increases the number of manipulative variables available for control. Five decades ago, Douglas et al.1 presented one of the earliest papers that studied the control of FEHE/reactor systems. Analog simulation was the high-tech tool used in this pioneering work. The investigation showed the tendency of these systems to either quench (blowout or extinguish to a low-temperature steady state) or runaway (blowup to a high-temperature steady state) because of the inherent positive feedback of energy from the adiabatic reactor back to the heat exchanger. A higher reactor inlet temperature produces a higher reactor exit temperature that then raises the reactor inlet temperature coming from the heat
Received: Revised: Accepted: Published:
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exchanger. These authors studied two systems. In the rst, which is similar to the reactor in the ammonia process, there was both heat transfer and reaction in a heat exchanger/reactor in which cold feed owed in one direction in the tubes and returned in the other direction in the shell. There was no adiabatic reactor section. The second system had both a heat exchanger and an adiabatic reactor. Silverstein and Shinnar2 studied the eects of design parameters on dynamic stability of systems with a FEHE followed by a furnace before the adiabatic reactor. They recommended controlling reactor inlet temperature with the furnace duty. Bypassing of cold material around the FEHE to provide an additional manipulated variable was explored. Terrill and Douglas3 examined the use of multiple feedeuent heat exchangers in the complex HDA process, which had a furnace before the reactor and used the hot reactor euent (after quenching to prevent coking) to preheat the reactor feed in several FEHEs in series. Coolers (reboilers of distillation columns) were installed between these multiple FEHEs. The dynamics of these FEHE/reactor systems can be quite complex as another early paper4 demonstrated and can lead to unconventional controller tuning. The system studied used FEHE bypassing to control reactor inlet temperature. No furnace or cooler was used. Unlike most processes, using integral action in the feedback controller improved dynamics. The reactor can exhibit inverse response to changes in inlet temperature because of the slower heat transfer to the solid catalyst. Bildea and Dimian5 explored the stability and multiplicity of systems with a FEHE, a furnace, a reactor, and a cooler on the reactor euent before it recycled back to the FEHE. The cooler generated high-pressure steam. Bypassing around the FEHE was
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not considered. They presented a design procedure to produce a design with large enough FEHE, furnace, and cooler to yield an openloop stable process. The resulting conservative design may be expensive in terms of capital investment and energy consumption (furnace duty). Morud and Skogestad6 studied instability in an industrial ammonia reactor with an FEHE. An extensive discussion7 of reactor/FEHE systems covered the eects of bypassing and adding a furnace. The HDA process was used as an example in which a reactor exit quench stream provided an additional manipulated variable. Chen and Yu8 extended the work of Terrill and Douglas, demonstrating that the use of multiple FEHEs improved disturbance rejection capability. Reactor/FEHE systems were explored9 using both linear analysis and nonlinear simulations to develop control structures. The recommended control structure had the following loops: (1) The temperature of the mixed stream (hot heat-exchanger exit plus cold bypass) is controlled by manipulating the bypass ow rate. (2) Temperature of the reactor inlet is controlled by manipulating fuel to the preheat furnace. A recent study by Jogwar et al.10 explored process networks with large energy recycles. All these studies demonstrated that the primary control issue is to maintain the reactor inlet temperature. If it drops too much, reaction rates slow up and the reactor exit temperature drops. Since this ows back to the heat exchanger as its hot inlet stream, the temperature of the stream leaving the heat exchanger (and entering the reactor) drops. A quench can easily occur. Mathematically this is equivalent to the system going to a stable low-temperature steady state. In this condition, nothing is reacting in the reactor (zero conversion). These studies demonstrated quantitatively that control is improved when a larger fraction of the total feed ow rate is bypassed around the heat exchanger. However, this requires a larger heat exchanger, which means higher capital investment. Bypassing can prevent reactor temperature runaways. However, it cannot prevent quenching. Using a cooler on the reactor euent is similar to FEHE bypassing in that it changes the temperature of the stream leaving the heat exchanger and entering the reactor (or furnace). However, bypassing and mixing hot and cold streams gives much faster dynamics than manipulating heat removal in a cooler because the dynamics of the cooler are involved. These studies also demonstrated that using a furnace improves dynamic control. In particular, a furnace can prevent quenching. However, use of a furnace increases energy costs. It is therefore desirable to use as little furnace energy input as possible. In this paper we present an alternative process and control structure that has the advantage of reducing furnace energy consumption while still providing e ective dynamic control for very large disturbances.
2. PROCESS STUDIED The chemical system used in this study is the production of dimethyl ether (DME) from methanol. The vapor-phase reaction is exothermic and reversible.
2MeOH DME + H 2O
dx.doi.org/10.1021/ie3004896 | Ind. Eng. Chem. Res. 2012, 51, 85668574
Industrial & Engineering Chemistry Research The kinetics equations for the forward and reverse reactions are