Computers and Chemical Engineering 28 (2004) 24212431

Dynamic modelling of an adsorption storage tank using a hybrid approach combining computational uid dynamics and process simulation
J. P. B. Mota a, , I. A. A. C. Esteves a , M. Rostam-Abadi b,c
a

Departamento de Qumica, Centro de Qumica Fina e Biotecnologia, Faculdade de Ci ncias e Tecnologia, e Universidade Nova de Lisboa, 2829-516 Caparica, Portugal b Department of Civil and Environmental Engineering, University of Illinois, Urbana, IL 61801, USA c Illinois State Geological Survey, Champaign, IL 61820, USA Received 6 October 2003; received in revised form 3 June 2004; accepted 10 June 2004 Available online 20 July 2004

Abstract A computational uid dynamics (CFD) software package has been coupled with the dynamic process simulator of an adsorption storage tank for methane fuelled vehicles. The two solvers run as independent processes and handle non-overlapping portions of the computational domain. The codes exchange data on the boundary interface of the two domains to ensure continuity of the solution and of its gradient. A software interface was developed to dynamically suspend and activate each process as necessary, and be responsible for data exchange and process synchronization. This hybrid computational tool has been successfully employed to accurately simulate the discharge of a new tank design and evaluate its performance. The case study presented here shows that CFD and process simulation are highly complementary computational tools, and that there are clear benets to be gained from a close integration of the two. 2004 Elsevier Ltd. All rights reserved.
Keywords: Process simulation; Computational uid dynamics; Hybrid modelling; Adsorption storage

1. Introduction Industry is increasingly expanding use of simulation as software improvements and increased computing power allow the tools to address commercially relevant problems. It is now apparent that simulation is proving an attractive alternative to costly and time-consuming experimentation. In many cases simulation tools enable scale up from laboratory scale to commercial scale skipping traditional pilot plants and reducing the required life span of R&D projects. Recently, there has been intense interest in linking engineering models with more rigorous simulation tools built from rst principles. Computational uid dynamics (CFD) is widely used when such detailed modelling is required and the equipment performance is dictated by the uid dynamics. Traditionally, CFD and process simulation tools have
Corresponding author. Tel.: +351 212 948300; fax: +351 212 948385. E-mail address: pmota@dq.fct.unl.pt (J.P.B. Mota). 0098-1354/$ see front matter 2004 Elsevier Ltd. All rights reserved. doi:10.1016/j.compchemeng.2004.06.004

addressed different domains in the analysis of chemical processes and equipment. Process simulation is primarily employed to perform material and energy balances, whereas CFD models are used primarily in the detailed engineering phase to model the uid ow and transport phenomena. However, integrating CFD and process simulation is of much interest because it improves workow between process engineering and the more fundamental analysis provided by CFD and facilitates the reuse of CFD knowledge in process design. Recent research on various types of chemical processes and equipment has demonstrated the benets of the combined application of CFD and process simulation. The application areas include, among others, crystallization (Urban & Liberis, 1999), gasliquid bubble columns (Bauer & Eigenberger, 1999, 2001), and column internals for reactive separations (Klker, Kenig, & Grak, 2002, 2003). Most of the models employed in these references can be classied as hybrid multizonal models. From a process simulation point of view, this class of models employs a multizonal repre-

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sentation that divides the equipment volume into a network of perfectly-mixed interconnected zones. The hybrid model is formed by the coupling of the process simulation model with the CFD model, both representing the same spatial domain. The main purpose of the CFD model is to provide an accurate description of the mass and energy uxes between adjacent zones. Bezzo (2002) and Bezzo, Macchietto, and Pantelides (2000, 2003a) proposed a general structure for multizonal/CFD modelling, which applies to both steady-state and dynamic problems. The mapping between the zones and cell descriptions employed by the process simulation and CFD models is achieved by means of appropriate disaggregation and aggregation procedures (Bezzo, 2002). One case study involving a batch reactor was used to illustrate the capabilities of the combined tool (Bezzo et al., 2000). This hybrid methodology has been recently adopted for the modelling and simulation of xanthan gum production in a batch aerobic bioreactor (Bezzo, Macchietto, & Pantelides, 2003b). Fluents CFD software has been recently coupled with Aspen Plus using standard CAPE-OPEN interfaces for unit operations, reactions, and thermo-physical properties. Using this integrated process simulation environment models of a stirred tank reactor (Zitney, & Syamlal, 2001) and fuel cell systems (Syamlal, Madsen, Rogers, & Zitney 2003) have been constructed to demonstrate the feasibility of the approach and its benets. This approach is somewhat different from the hybrid multizonal/CFD modelling discussed above, the two models handle different parts of the equipment or unit operation and communicate with each other through the boundary conditions established for each element in the owsheet. Here, we report the successful integration of a commercial CFD software package and the process simulator of an onboard adsorption storage tank for methane fuelled vehicles. Besides knowledge reuse, our integrated simulation tool combines the robustness of our in-house developed adsorption process modelling system with the detailed ow and heat transfer predictions provided by the CFD software. The two codes act in a cooperative manner, exchanging boundary data during a simulation and continuously updating the dynamic process description. Unlike the multizonal/CFD modelling approach, the process and CFD models of our hybrid simulation tool represent different spatial domains of the storage tank. In this respect our approach is closer to the methodology adopted in the Aspen Plus-Fluent integrated simulation environment. An unusual aspect of our integrated simulation tool is that both the process simulator and the CFD model are inherently dynamic. The combined software tool has been successfully employed to study the discharge dynamics of a new tank design incorporating an external heating jacket. Preliminary results obtained with this hybrid modelling tool on the use of radially-extruded internal ns for enhancing conductive radial heat transfer in the bed are also presented at the end of the paper.

2. Motivation Adsorption storage is the most promising low-pressure alternative for storing natural gas in both automotive and stationary applications (Cook, Komodromos, Quinn, & Ragan, 1999). This storage technology rests on the assumption that the high density of the adsorbed gas conned within the pores of the adsorbent compensates for the volume taken up by the solid and for the lower density of the compressed gas in the interparticle void space. Presently, microporous activated carbons are the most successful adsorbents for adsorbed natural gas (ANG) storage (Lozano-Castell, Alcaiz-Monge, de la Casa-Lillo, Cazorla-Amors, Linares-Solano, 2002). There are, however, some operational difculties that still hinder the extensive use of this technology in commercial markets (Cook et al., 1999; Mota, 1999; Mota et al., 2001). One of the most serious problems, especially in automotive applications, is the negative impact of the heat of desorption on the net deliverable capacity of the storage system. The physical adsorption of a gas is an exothermic phenomenon that decreases with increasing temperature. Conversely, the desorption process is endothermic, the degree of which depends on the afnity of the adsorbent for the gas. Although in vehicular applications the discharge of an onboard ANG storage tank is usually a slow process, under normal driving conditions the consumed heat of desorption is not fully compensated by the wall thermal capacity and by the heat transferred from the surrounding environment (Chang & Talu, 1996; Mota et al., 2001). Furthermore, it is unfeasible to operate the reservoir under sub-atmospheric pressure, since excessive compression hardware would be necessary to extract and boost the gas pressure. Consequently, during discharge the reservoir cools by as much as 40 C and more gas is retained in storage at deletion pressure, thereby reducing the deliverable capacity. To compensate for this capacity loss, the adsorbent must be heated, either directly or indirectly. The approach that we advocate is to indirectly heat the adsorbent bed using the hot exhaust gas. An alternative heat source is the thermouid of the engine cooling system. We prefer the former approach due to the high temperature at which the exhaust gas leaves the combustion chamber (above 500 C; see Shiells, Garcia, Chanchaona, McFeaters, & Raine, 1989), and because it is more economical to adjust the exhaust pipe than to increase the power of the thermouid recirculating pump. Although most of the heat is purposively lost to the environment in the exhaust pipe, in a well-designed system there is sufciently hot exhaust gas readily available to exchange energy with the tank. From the various shell- and tube-heat exchanger designs that are efcient at transferring heat to the adsorbent bed, we selected the simplest conguration that does not require internal modication of a conventional tank. The prototype design is illustrated in Fig. 1, it consists of jacketing the storage tank so that the adsorbent bed is heated by forced con-

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the use of Fluent over its commercial competitors. Note also that good freeware software also exists, such as CFDLIB, the los Alamos library of computer codes for solving CFD problems in 2D and 3D. Apart from minor implementation details, the approach described here can be employed with most CFD packages. By incorporating CFD into our process simulation tool, we can take advantage of its exibility to handle complex geometries in future studies of alternative heat exchanger designs. This point is discussed further at the end of this paper. Besides the inadequacy of the numerical methods employed by most CFD packages to handle the strongly coupled nonlinearities introduced by the presence of the adsorbed phase, each CFD package may have particular constraints that preclude it from being readily applicable to adsorption processes. For example, presently Fluent treats the effective thermal conductivity of the packed bed as an isotropic property of the medium. However, it is well known (Winterberg, Tsotas, Krischke, & Vortmeyer, 2000) that for a cylindrical packed bed, where the gas ows predominantly in the axial direction, is anisotropic and depends on the magnitude of the axial velocity component vz of the uid. The axial (z ) and radial (r ) components of can be written as
Fig. 1. Schematic drawing and main geometrical parameters of an onboard jacketed cylinder for adsorbed methane storage.

(z , r ) = 0 + (z , r )dp Cg c|vz |,

(1)

vection heat transfer from the exhaust gas as it ows along the annular channel of the jacket. The jacket eliminates the need for internal coils, yet gives a better overall heat-transfer coefcient than external coils. Furthermore, since the jacket is not pressurized, its wall thickness can be minimized by installing reinforcement rings. This work originated from the need to develop a dynamic simulation model of our prototype storage tank, which can safely replace most of the costly and time-consuming experimentation, for performance assessment, scale up, and optimization. For this to be achievable in practice, the heat transfer process must be accurately predicted, both in the adsorbent bed and in the annular channel of the jacket. The starting basis for developing the new simulation tool was our process simulator AngTank (Mota, Saatdjian, Tondeur, & Rodrigues, 1995, 1997b, 1997a; Mota, Rodrigues, Saatdjian, & Tondeur, 2001), which is a 2D code for simulating the dynamics of nonisothermal, multicomponent cylindrical adsorbent beds. This code is described in detail in the next section. In order to accurately simulate the uid ow and heat transfer in the annular channel of the jacket, a commercial CFD software was coupled with AngTank. The CFD package chosen is uent 5.0 from Fluent Inc., a general-purpose CFD software that we have employed previously in other research areas (Lefevre, Mota, Rodrigo, & Saatdjian, 2003a; Lefevre, Leprevost, Mota, Rodrigo, & Saatdjian, 2003; Rodrigo, Mota, Saatdjian, & Levefre, 2003). Note that due to our lack of prociency in using other commercial CFD packages we do not advocate

where 0 is the isotropic stagnant component of , dp is the particle diameter, Cg c is the volumetric heat capacity of the gas, z 0.70.8 and r 0.10.3 (Yagi et al., 1960) (Yagi, Kunii, & Wakao, 1960). Since z > r , the extent of the increase of z with the increase of the ow rate is larger than that of r . The effective conduction heat ux in the packed bed under anisotropic conditions, which we denote by T , is expressed as T = (z ez T) ez (r er T)er , (2) where ez and er are the axial and radial unit vectors, respectively. Although Eq. (2) can in principle be coded in a user-dened subroutine (a standard feature available in most CFD packages) that is added as an extra term to the energy ux, its actual implementation in Fluent is not trivial. It is apparent that the hybrid solution procedure is computationally more demanding than one that does not rely on the CFD package to predict the heat transfer from the exhaust gas. In fact, this simpler approach was adopted in the early stages of the project where the heat transfer process was modelled using a mean heat transfer coefcient estimated from correlations for convective heat transfer in annuli. However, it was soon realized that this method has a high degree of uncertainty for unsteady-state heat transfer where the thermal entry length spreads over an appreciable extent of the domain, a condition which is always met in the problem under study. For the purposes of this work natural gas can be modelled as pure methane. Under this assumption, the thermophysical properties and ow rate of the exhaust gas can be related to the fuel discharge ow rate by a simple combustion model.

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Fuel (methane) and oxidant (air) are presumed to combine in a single step to form a product: CH4 + (2O2 + 7.52N2 ) = CO2 + 2H2 O + 2( 1)O2 + 7.52N2 , (3) where = 1.2 is the air-fuel ratio. Assuming that this model is a good approximation to the real combustion process, the Reynolds number for gas ow in the annular channel of the jacket is given by Rec = e ve ec e MCO2 + 2MH2 O + 2( 1)MO2 + 7.52MN2 = F, (R + ew )e (4) where F is the methane molar discharge ow rate, e , e and ve are the density, viscosity and average axial velocity of the exhaust gas, respectively, R is the internal cylinder radius, ew is the wall thickness, ec is the gap spacing of the annular channel, and MCO2 , . . . , MN2 are the molecular weights. Eq. (4) shows that the nal expression for Rec is independent of ec and further analysis reveals that under normal discharge conditions the ow in the jacket is laminar, i.e. Rec < 103 . The unnecessariness of turbulence modelling reinforces our condence on the accuracy of the heat transfer data obtained using the CFD software.

assumptions, which are assumed to hold based on the discharge slowness during normal vehicle operation (Mota et al., 2001): The momentum equation is governed by steady-state Darcys law. There is instantaneous equilibrium between gas and adsorbed phase. Intraparticle gradients are negligible. The temperature of the adsorbent particle and that of the surrounding gas are identical at every point in the bed. The assumption of fast kinetics relative to the overall discharge dynamics justies the adoption of an adsorption equilibrium model at the particle level. In this study we have selected a typical granular activated carbon employed for ANG storage (Chang & Talu, 1996). The methane adsorption equilibrium on the carbon adsorbent is well correlated by a truncated Virial isotherm equation: ln P q = k1 + k2 T + k3 + k4 T q, (5)

where q is the equilibrium adsorbed concentration at pressure P and temperature T . Eq. (5) gives a linear variation of the isosteric heat of adsorption, Qst , with loading: Qst = Rg (k2 + k4 q) (6)

3. Problem formulation The model of the jacketed reservoir is an extension of our previous numerical work (Mota et al., 1995, 1997a,b, 2001) on the dynamic behavior of ANG storage cylinders under realistic operating conditions. The model has been shown (Mota, 1999) to accurately reproduce the experimental pressure history and temperature proles in an adsorbed methane storage cylinder during discharge. The governing equations for the adsorbent bed are based on the following

A realistically model of the storage cylinder is formulated in axisymmetric cylindrical coordinates (z, r), where z is the axial coordinate and r is the radial coordinate. Using this coordinate system one can take into account the temperature gradients induced by the lateral, front, and rear faces of the cylinder. The continuity and energy equations in the carbon bed (domain D1 in Fig. 2) are, respectively, c q + b = (cv), t t P K c= , v= P; (Rg T)

(7)

Fig. 2. Partition of the computational domain between the two solvers. (a) Physical domain in two-dimensional axially-symmetric cylindrical coordinates; (b) computational domain handled by AngTank; (c) computational domain handled by Fluent.

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[b Cs + Cg (c + b q)]

P T q b Qst t t t = ( T) Cg cv T

ver = 0, (8)

vez (r) = 2vin 1 e Te z

r Rc

, on B6, (18) (19)

These equations are subjected to the following boundary conditions: T vr = 0, = 0 on B1; (9) r n v = 0, cvz = F , (R2 ) i n T = hw (Tw T) on B2 T = 0 on B3 z (10) (11)

e Ce vez (Te Tein ) = e Pe = 1 atm, Te = 0 on B7, z

Symbol n denotes the outwards unit vector normal to the boundary B2, Ri is the radius of the discharge tube (see Fig. 1), and hw = h0 + w Cg c|vz | is the wall heat-transfer w coefcient, where w = 0.054 (Yagi et al., 1960) and the stagnant contribution h0 can be estimated by the equations w given in Ofuchi and Kunni (1965). An energy balance on the steel cylinder wall (D2) is required, since it cannot be neglected due to the large thermal capacity of the material. The equation in vector form can be written as Cw Tw w (n Tw )n|| t hw (T Tw )B2 + n (e Te )B4 = , ew

where vin is the average velocity at the entrance of exhaust e inlet tube and is obtained from Eq. (4). It is assumed that the ow across the boundary B7 is already fully-developed so that Eq. (19) is complemented with the condition of zero diffusion ux of all ow variables in the exit direction (in practice, this means that the conditions of the outow plane can be extrapolated from within the domain and have no impact on the upstream ow).

4. Coupled solution procedure AngTank and Fluent handle different regions of the adsorption tank, i.e., the computational domains employed by the two codes do not overlap. Our process simulation tool solves the nonisothermal adsorption dynamics in the cylindrical packed bed of adsorbent [Eqs. (7) and (8)], whereas the CFD software describes the uid ow and heat transfer [Eqs. (14) and (15)] in the annular channel of the jacket including the heat transfer [Eq. (12)] across the wall of the tank. Both codes employ two-dimensional axisymmetric cylindrical coordinates. The different regions of the computational domain are depicted in Fig. 2. AngTank employs the method-of-lines approach (Schiesser, 1991) to solve the conservation equations in the adsorbent bed taking into account the adsorption dynamics. The spatial derivatives are discretized using the control-volume method (Patankar, 1980) and converted into a large system of differential-algebraic equations (DAEs) to which an efcient stiff-DAE solver is applied. In order to prevent non-physical oscillations of the solution, the convective terms are spatially discretized using the van Leer harmonic ux-limited scheme implemented in the form advocated by Waterson and Deconinck (1995). In the early stages of the project the DAE system was solved using the numerical library DASSL (Brenan et al., 1989), but it was later replaced by the more advanced DAEPACK numeric component DSL48S (Tolsma & Barton, 2000). DSL48S contains a number of extensions to DASSL including exploitation of sparsity using the Harwell library MA48 routines and an efcient staggered-corrector sensitivity algorithm. Furthermore, the additional information required by DSL48S (notably sparse Jacobian matrix, analytical partial derivatives with respect to model parameters, and sparsity information) are generated automatically with other DAEPACK components. To render the hybrid solution procedure computationally more efcient, the grid nodes employed by Fluent and

(12)

where n is the positive unit vector parallel to the wall and ew is the thickness of the cylinder wall. Eq. (12) is subjected to the following boundary conditions: n|| Tw = 0 on B8. (13)

The ow of exhaust gas in the annular channel of the jacket (domain D3) is governed by the continuity and momentum equations for an incompressible, Newtonian uid: ve = 0, e ve + ve ve t = e 2 ve Pe , (14) subjected to the usual no-slip wall boundary condition (ve = 0 on B4 and B5). The energy equation equation for the exhaust gas in domain D3 is Te e 2 Te ve Te , (15) = t e Ce with boundary conditions Te = Tw on B4, n Te = 0 on B5 (16) (17)

Fully developed ow is assumed at the entrance to the inlet tube of the jacket, and constant pressure at the exit of the outlet tube. The inlet and outlet boundary conditions for the exhaust gas can be written as

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AngTank do not need to be identical at the boundary where the two computational domains meet. To allow for this exibility, data is exchanged between the two grids using an interpolation procedure that is consistent with the control-volume formulation employed by both solvers. This procedure is described in the appendix. The two codes run as independent processes and communicate through shared memory. The software interface, which has been implemented as a user-dened function in uent, dynamically suspends or activates each process as necessary, and is responsible for data exchange and process synchronization. This strategy leads to an optimum allocation of CPU usage. The two codes interact with each other as follows. Suppose that we wish to advance the solution from current time tn to time tn+1 . At the start of the integration step Fluent is active whereas AngTank is on hold in a suspended state. Before computing the new solution, Fluent rst updates its inlet and boundary conditions. In order to do this, it transfers (n) the wall-temperature prole data, Tw , to AngTank. These data are dened on the boundary interface between the two computational domains, which is identied as B2 in Fig. 2. Once this has been accomplished, Fluent is suspended by the software interface and AngTank is reactivated. The process (n) simulation software interpolates Tw from uents grid to its local grid, and then advances the solution in the adsorbent bed (domain D1) from tn to tn+1 using the newly received (n) Tw data. Prior to being suspended again, AngTank computes the heat ux data on the boundary B2, and interpolates them from its grid to uents grid. AngTank also updates the value of the exhaust gas molar ow rate, which is one of uents input conditions [cf. Eq. (4)], and then transfers the boundary data to the CFD solver. Finally, Fluent computes the solution at tn+1 . The data exchange between the two codes ensures continuity of temperature and heat ux along the outer surface of the cylinder wall, and is the mechanism by which the two solutions are synchronized. An algorithm describing the

software interface is provided in Fig. 3. The function calls given there are specic to the WindowsTM operating system and handle the notication of events across process boundaries. These functions are fairly standard and equivalent functions also exist in other operating systems. Since the two packages do not employ the same DAE solver, there is a slight decrease in the overall order of the time integration because the heat ux data on boundary B2 is (n) computed as hw [Tw T (n+1) ], whereas the correct expression that is consistent with the implicit methods employed (n+1) by both DAE solvers should be hw [Tw T (n+1) ]. However, for the small time steps employed in Fluent no signicant loss in accuracy of the computed solution was observed when our simplied procedure was employed.

5. Results and discussion The hybrid computational tool described in the previous section has been successfully employed to size, simulate and evaluate the performance of the new tank design. The grid employed by the CFD package is shown in Fig. 4; the packed bed was discretized using a uniform grid with 40 nodes in the axial direction and 15 nodes in the radial direction. These values are the result of several tests to determine the optimum grid size. The time step employed by the CFD solver is 30 s. The values of the main parameters employed in the numerical simulations are listed in Table 1. The depletion pressure is P1 = 1.4 atm, while the charge pressure is P2 = 35 atm. Upper pressure limits in the range 3540 atm are the more commonly accepted charge pressure values. The simulations were performed on a Pentium IV 1.7 GHz processor with 512 MB RAM, running the Windows 2000 Operating system. Each run was completed in less than 10 min. Since the jacket takes up extra space that in a conventional unjacketed storage tank would be lled with adsorbent, the performance of the proposed prototype is compared with

Fig. 3. Algorithm of software interface to manage process synchronization and exchange data between AngTank and Fluent.

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Fig. 4. Computational grid employed by the CFD solver. The grid is symmetrical with regards to the cross-sectional plane located at z = L/2. The number of grid nodes employed by the process simulation code is 40 15 (z r).

Fig. 5. Exhaust gas temperature required for attaining the equivalent to isothermal performance ( = 1) as a function of discharge duration ( = 0.2 W m1 K1 ).

those of two conventional tanks: one having the same volume as the prototype (i.e., tank and jacket) and the other having the same weight. This leads to two different values of the dynamic efciency, respectively v and w , for the same exhaust gas temperature. The dynamic efciency, which is dened as CH4 delivered under dynamic conditions = , (20) CH4 delivered isothermally provides a direct measure of the capacity loss due to nonisothermal operation. These two types of comparison are suitable benchmarks for mobile applications in which the limiting constraint is, respectively, volume (v ) or weight of storage (w ). It is easy to see that the following relations hold: w w > 1 and lim =1 (21) ec 0 v v The second relation is strictly true only if the thickness of the outer wall of the jacket can be neglected, which is usually the case.

Table 1 Data employed in numerical simulations Cg = 36.0 J mol1 K1 Cs = 1.05 J g1 K1 Cw = 3.92 J cm3 K1 ew = 5.0 mm L = 74.0 cm P1 = 1.4 atm P2 = 35.0 atm R = 10.0 cm Ri = 5.0 mm T0 = 20.0 C = 0.45 w = 42.0 W m1 K1 b = 0.48 g cm3

Adsorption isotherm parameters (P in atm, T in K, q in mol/kg) k1 = 6.132 k3 = 0.221 k2 = 2019 k4 = 29.73

An effective means to assess the feasibility of the proposed approach for heat management is determining the exhaust gas temperature that increases the net deliverable capacity to that of an hypothetical isothermal discharge ( = 1). The results of this study are plotted in Fig. 5 as a function of discharge duration. The two benchmark cases are compared for two values of the annular gap spacing of the jacket, ec = 2 mm and ec = 5 mm. As expected, a higher Te value is required to obtain the equivalent of isothermal performance when the comparison is made on volume basis than on weight basis. If the discharge duration is increased, which is equivalent to decreasing the fuel discharge ow rate, then isothermal performance can be attained with a lower Te value. Decreasing ec improves the performance of the storage cylinder because heat transfer to the carbon bed is enhanced. This increase in performance is more pronounced when the comparison between prototype and regular cylinder is made on a volume basis because less effective storage space is lost due to the jacket. The energy demand of a city vehicle, equipped with three cylinders like the one considered in this work (Table 1) and travelling at cruising speed, gives a discharge duration of about 3 h. Fig. 5 shows that, under these conditions, the Te value that increases the discharge performance to that of isothermal operation is in a perfectly feasible range (80100 C). This conclusion applies to a regular carbon bed with a typical value of effective bed thermal conductivity ( = 0.2 W m1 K1 ). Fig. 6 compares the temperature eld during a three-hour discharge for a conventional storage cylinder (left) with that for the prototype (right). The plots were obtained for an exhaust gas temperature Te = 80 C and the same value as in Fig. 5. The clear difference in gray shading between the two temperature plots demonstrates the effectiveness of the jacket at transferring heat from the exhaust gas to the adsorbent bed. At the end of discharge the average bed tem-

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Fig. 6. Comparison of the temperature eld during a three-hour discharge for a conventional storage cylinder (left) and that for a jacketed cylinder (right); ec = 5 mm, = 0.2 W m1 K1 , Te = 80 C.

perature in the conventional cylinder has dropped 27 C, whereas that in the jacketed cylinder has been increased by 8 C above its initial value. We have employed the hybrid simulation tool to carry out a parametric study of the inuence of Te , discharge duration (Td ), and , on the values of v and w . The results are

shown as contour plots in Fig. 7. The top-left region of each contour plot shows that our prototype can even surpass the isothermal performance level by up to 20% depending on the values of the Te , Td , and . In order to be conservative about the results presented, the data plotted in Fig. 7 were obtained for the largest annular gap spacing considered in

Fig. 7. Dynamics efciencies, v and w , for a jacketed storage cylinder as a function of exhaust gas temperature temperature Te ( C), discharge duration td (hr), and effective thermal conductivity of adsorbent bed (W m1 K1 ), for ec = 5 mm. The values of v are given in the left-hand-side plots, those of w are plotted on the right-hand-side.

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this work (ec = 5 mm). As is shown in Fig. 5, reducing the annular gap spacing would lead to even better results. Note that the contour plots obtained for = 1 W m1 K1 and = are not unrealistic, since good adsorptive and thermal properties can be combined in densied or immobilized adsorbents, provided the incorporation of the binder is not deleterious to adsorptive capacity (Cook et al., 1999). Two examples of such types of beds are dual-size particle packing and carbon monoliths. Their good thermal conductivities make them particularly attractive candidates for adsorptive storage applications with enhanced thermal management such as the one proposed here. In an ordinary adsorptive storage cylinder the gas ows axially through the carbon bed, which means that radial heat transfer takes place mainly by conduction. This is not particularly effective because granular beds are known to exhibit poor heat transfer characteristics. Chang and Talu (1996) proposed changing the ow direction during discharge from axial to radial by a perforated tube inserted at the center of the cylinder. An alternative approach considered here is using radiallyextruded internal ns to enhance radial heat transfer in the carbon bed. The ns effectively change the ow direction from axial to radial, which promotes energy transfer by convection from the hot wall to the central region. Furthermore, the high conductivity of the ns increases the overall conductive radial heat transfer. To handle this new conguration, the ns were made part of the computational domain handled by the CFD code and were treated by the process simulation tool as extensions of the internal wall of the storage tank. Obviously, the ns take up some space that otherwise

would be lled with carbon; hence, the thickness, number, and location of the ns must be optimized. This is a complex problem that is currently under study. Nevertheless, the preliminary results already obtained suggest that net deliverable capacity can be increased with n insertion. For example, the conguration shown in Fig. 8, which has has not been optimized with respect to individual n location nor thickness, increases the net deliverable capacity by an extra 5%.

6. Conclusions By exploiting the ability of CFD to provide a detailed analysis of uid dynamics and heat transfer in complex geometries, our integrated simulation model is a powerful tool for the analysis of heat-transfer enhancement alternatives that can be applied to our prototype storage tank. Fin insertion in the packed bed has been briey discussed above, but other options exist. For example, on the jacket side the heat transfer rate can be increased by a suitable heat-transfer enhancement mechanism, such as rough walls or the insertion of turbulence inducing elements in the annular channel (Vilemas, Simonis, & Adomaitis, 1994). Such changes to the internal conguration of the jacket can be easily studied using our hybrid simulation tool. In accordance with some recently reported work, the case study presented here shows that CFD and process simulation technologies are highly complementary, and that there are clear benets to be gained from a close integration of the two. The combined application of CFD and process simulation opens the possibility for process modelling with an increased degree of detail and predictive accuracy and can gradually circumvent some of the limitations of traditional process simulation models.

Acknowledgements Financial support provided by Fundao para a Ci ncia e e Tecnologia, under project grant POCTI/EQU/45102/02 and PhD grant PRAXIS XXI/BD/19832/99, is gratefully acknowledged.

Appendix A In this appendix we briey describe the interpolation procedure for exchanging boundary data at the interface between the two computational grids. The procedure adopted in this work is consistent with the control-volume formulation employed by both solvers. For simplicity, let us suppose that we wish to interpolate the axial bed temperature prole near the wall, i.e. T(z) at r = R, from grid 1 to grid 2, as illustrated in Fig. 9. Note, however, that the procedure described next is not restricted to a one-dimensional boundary and can be easily extended to a two-dimensional boundary.

Fig. 8. Predicted temperature eld at the end of a three-hour discharge for various n congurations ( = 0.2 W m1 K1 , ec = 5 mm, Te = 80 C).

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Fig. 9. Node location at the boundary interface between the two computational grids. The solution is to be interpolated from grid 1 to grid 2 while preserving integral conservation over the computational boundary.

The faces of the control volumes normal to the interface boundary are located at zi+1/2 = zi +
() () 1 2

the discrete analog of integral conservation over the computational boundary, i.e.
n1 i=1

zi = zi+1

()

()

1 2

zi+1 ,

()

(A.1)

where the superscript () means that the expression is applicable to both grids. Although the number of nodes and their location along the interface boundary may be different for the two grids, they have the same extent, i.e. z11/2 = z11/2 = z0 0
(1) (2) (1) (2)

z i Ti

(1) (1)

n2

=
j=1

zj Tj

(2) (2)

(A.7)

References
Bauer, M., & Eigenberger, G. (1999). A concept for multi-scale modeling of bubble columns and loop reactors. Chem. Eng. Sci., 54, 5109. Bauer, M., & Eigenberger, G. (2001). Multiscale modeling of hydrodynamics, mass transfer and reaction in bubble column reactors. Chem. Eng. Sci., 56, 1067. Bezzo, F. (2002). Design of a General Architecture for the Integration of Process Engineering Simulation and Computational Fluid Dynamics, PhD Thesis, University of London, London. Bezzo, F., Macchietto, S., & Pantelides, C. C. (2000). A general framework for the integration of computational uid dynamics and process simulation. Computers Chem. Eng., 24, 653658. Bezzo F., Macchietto, S., & Pantelides, C. C., 2003a. An object-oriented approach to hybrid multizonal/CFD modelling. PSE2003, International Symposium on Process Systems Engineering. Bezzo, F., Macchietto, S., & Pantelides, C. C. (2003b). General hybrid multizonal/CFD approach for bioreactor modeling. AIChE J., 49, 21332148. Brenan, K.E., Campbell, S.L., Petzold, L.R., 1989. Numerical Solution of Initial-Value Problems in Differential-Algebraic Equations. New York: Elsevier. Chang, K. J., & Talu, O. (1996). App. Thermal Eng., 16, 359. Cook T. L., Komodromos, C., Quinn, D. F., & Ragan, S. (1999). Adsorbent storage for natural gas vehicles. In T. D. Burchell, Carbon Materials for Advanced Technologies. Oxford, UK: Elsevier, pp. 269302. Klker, M., Kenig, E., & Grak, A. (2002). On the Development of New Column Internals for Reactive Separations via Integration of CFD and Process Simulation. Proceedings of International Conference on Catalysis in Multiphase Reactors, Lausanne, Switzerland. Klker M., Kenig, E., Grak, A., Egorov, Y., & Menter F. (2003). Improved Design of Reactive Separation Internals via CFD and Process Simulation. Proceedings of ACHEMA 2003, Frankfurt, Germany. Lefevre, A., Mota, J. P. B., Rodrigo, A. J. S., & Saatdjian, E. (2003a). Chaotic advection and heat transfer enhancement in Stokes ows. Int. J. Heat Fluid Flow, 24, 310321. Lefevre, A., Leprevost, J. C., Mota, J. P. B., Rodrigo, A. J. S., & Saatdjian, E. Chaotic advection in a 3-D Stokes ow. AIChE J., in press.

and (A.2)

zn1 +1/2 = zn2 +1/2 = zL L

For consistency with the control-volume formulation employed by both solvers, it is assumed that the value of T(z) at a given node prevails over the control volume surrounding it, so that the following approximation holds:
zi+1/2
() zi1/2 ()

T(z) =

zi Ti

() ()

(A.3)

The piecewise constant function that interpolates the node (1) values Ti on grid 1 and satises Eq. (A.3) can be written as T (1) (z) = where H(z) = 0, 1, z<0 z0 (A.5)
n1

i=1

Ti [H(z zi1/2 ) H(z zi+1/2 )], (A.4)

(1)

(1)

(1)

denotes the unit step function (also called the Heaviside function). Since Eq. (A.3) also applies to grid 2, the node values (2) of Tj can be computed from those of grid 1 using the following formula: Tj
(2)

1 zj
(2)

zj+1/2 zj1/2
(2)

(2)

T (1) (z)

(A.6)

Eq. (A.6) gives the closest piecewise-constant approximation to T (1) (z) that satises Eq. (A.3) on grid 2. Consequently, this grid-to-grid interpolation procedure preserves

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