DE1767347A1 - Tube reactor for catalytic reactions - Google Patents

Description

R e ctio n g "Tubular reactor for catalytic reactions" The invention relates to a tubular reactor for catalytic reactions as well as chemical ones Procedure. which are carried out with the help of such reactors.

Chemical reactions are often carried out under continuous 1) the reactants in a reactor with solid catalytically active material carried out.

The chemical reaction takes place on the solid catalyst and heat can be developed or absorbed from the berci @ l containing the catalyst be, with appropriate Temperature changes are caused.

For most chemical reactions there are in every reactor area optimal conditions of pressure and temperature for the reactants at which the reaction rate and the concentration of the desired product optimal or are at least justifiable. In the case of a catalytic chemical reaction it is possible to regulate the pressure of the reaction participants reasonably well, however, temperature control is more difficult because heat is the catalytic one Material containing area must be transferred or withdrawn from it a rate that, under optimal conditions, the temperature of each area at the optimal temperature according to the local concentration of the reactants and the products are held.

In known solid particulate catalysts, bases contain reactors temperature control was carried out in various ways. Regarding exothermic Reactions, these temperature control methods can be summarized as follows: 1) The reactor is cooled sufficiently to necessarily keep the reaction temperature to the optimal temperature in Maximum response speed range (the hot spot ") to penetrate, this has the consequence that the temperature in others Areas of the reactor can be below the local optimum and the reactor unnecessary must be big. In addition, such reactors are sensitive to changes of the reactants and small deviations in the conditions of the reactants can cause large changes in local temperatures and concentrations of the Lead products.

E.g. in Journal of the American Institute of Chemical Engineers, Volume 2, 1956, page 117 ff. Stated that an exothermic catalytic reaction first order in a tubular reactor with an inlet temperature of 340 ° K is carried out under the Ee conditions k1 = 3.94 x 1012exp (-11.400 400 and 4h = -0.2 DdB #H 146 (kl = reaction rate constant, h = heat transfer coefficient over the entire reactor wall, D = reactor diameter, d = bulk density of the catalyst in bed, = = heat of reaction per mole and T = temperature, in c.g.s. units) oei a temperature of the reactor wall of 336 ° K the maximum temperature in bed is slightly higher than 3400K, but with a wall temperature that is 3380K is increased, the maximum temperature in the bed rises to about 4200K.

2) The same reactor is built in a number of smaller ones in series switched sub-reactors and each sub-reactor is operated adiabatically. The reaction products in each sub-reactor become indirect through heat exchange or directly with the addition of additional cold starting material (cold-shot) cooled before they are transferred to the next sub-reactor. Because the temperature the reactant in an unregulated manner through each sub-reactor fluctuates, this arrangement was used for reactions in which the temperature sequence is not very important.

5) The reactor is tubular and has a jacket for heat exchange, wherein the catalytic material is arranged in the jacket is. The reactants are introduced into the jacket through the tubes and the products are drawn off from the jacket in countercurrent to the starting materials. This The reactor enables an increasing temperature difference between the starting materials in the tubes and the products in the jacket while the products approach the exit whereby reversible exothermic reactions are carried out somewhat more favorably However, the temperature control of the products can be quite critical of the flow rate through the reactor depends. This arrangement is therefore relative Not very adaptable if changes in throughput are sought.

4) The catalytic material is created by the raw materials and products kept in a fluidized bed. The overall temperature in the reactor can then be quite be uniform, but the residence time in the reactor can be very broadly distributed, which results in poor selectivity; when competitive reactions take place. Also, an abrasion resistant catalytic material must be used and it will some catalyst is lost during the execution of the process.

According to the invention, the desired temperature distribution is in a Tubular reactor for catalytic conversions achieved in that the catalytic Material is distributed in the flow direction of the reactants, aaL in the amount of catalyst present in each reactor section is sufficient to Temperature in the steady state, resulting from time-changing velocities the Heat generation (or heat absorption) and heat transfer in the respective reactor section results is achieved. Accordingly, the amount of solid catalyst per Unit volume of the reactor z. B. by mixing the catalyst with catalytic inert particulate solid material adjusted by, for example, catalyst pellets mixed with similar pellets of the inert material according to the predetermined distribution so that the desired temperature profile is achieved in the reactor.

As the reaction rate of a catalyzed reaction per unit volume of the reactor space depends on the amount of catalyst per unit volume, the desired Temperature in each section of the reactor achieved by the catalytic Material in these areas is introduced in such an amount that the as a result the heat generated or lost in the reaction is substantially offset by the heat that passes into or out of this area at the desired temperature this area is discharged.

While according to previous practice, the temperature at a catalytic Reaction by regulating the rate of heat transfer from each reaction zone has been set, the temperature is according to the invention by a control the The reaction rate of the reactants per unit volume is set by the catalyst is mixed with inert material in particulate form in the necessary amount will.

The dilution material in each reactor area is also used for Heat transfer to the catalytic material or away from it in the relevant Range so that essentially the desired temperature during the process flow is maintained across the cross section of the catalyst bed, perpendicular to the direction of flow of the respondents measured.

The term "bed is used to denote arrangements, where the solid particulate catalyst alone or with diluent material is packed in a zone or for arrangements in which the catalytic Material alone or with thinning material in a row at a distance from each other arranged separate zones, e.g. in a number of one another remote floors in the reactor.

The distribution of the catalytic material in the reactor can be in the general direction of flow of the reactants through the reactor fluctuate, so that essentially the desired temperature profile in the reactor during of working in this direction can be achieved.

In addition, the distribution of the catalytic material can be in the transverse direction to the general direction of flow of the reaction stones fluctuate, so that essentially a desired temperature profile when performing the method in the transverse direction to the direction of flow is achieved.

According to another embodiment of the invention, the bed can be made from consist of a number of floors on which the catalytic material is deposited and is distributed, and the trays can flow in the general direction of flow of the reactants be arranged at a distance from each other.

Preferably, the invention is applied to reactors that have have a cooling on the wall, but in individual cases the reactor can be equipped with a outer annular space must be provided with insulating material, such as a narrow one gas-filled column that separates the reactor wall from a jacket that contains a heat transfer medium contains, e.g. B. a steam jacket, which means that the reactor is at a high temperature that of the steam jacket can be held, the pressure in the reactor however, can be kept appropriately low.

To explain the invention in more detail, an example of the theoretical Calculation of a tube reactor with flow control listed below.

In this example it is assumed that the heat transfer resistance is concentrated on the reactor wall and by an equivalent total heat transfer coefficient can be expressed. In the example it is also assumed that none in the reactor radial temperature gradients exist. This is essentially the case at high Flow rates of the reactants through reactors of small equivalent diameter, because the radial equivalent conductivity within the reactor is proportional to Flow rate is while the heat transfer coefficient between the bed and the reactor wall is proportional to the root of the flow velocity, Ü: er a differential length of the reactor by dividing the flow rate of the starting materials and products for which asa is F, a thermal equilibrium results according to F.Cp .dT = F (- # H) dx + h (Tw - T) dA ........... (1), where dT is the temperature difference caused by the conversion dx, Cp the specific heat at constant pressure of the material, T is the temperature at one represents general location, Tw is the wall temperature of the reactor, h is the heat transfer coefficient on the reactor wall, dA means the area of the differential length of the reactor wall and IH is the heat of reaction.

For a reactant A whose mole fraction is in the feed equals NAO, the corresponding mass equilibrium results in rdw = FNAodXA (2), where w is the mass of catalyst material per unit volume and XA is the fraction of conversion of reactant A is.

If, according to the invention, the mass w of catalyst material is distributed, e.g. by admixing a diluent material, thereby obtaining a total weight W. wlrd, so that the dilution factor Rt of the catalyst material is represented by R '= W, then equation (2) becomes w rdW = FNAO dXA = rdBdV ........... (3), R R 'where dß is the bulk weight of the catalyst material and the Diluent material in a differential length of the reactor and dV is the volume represents the differential reactor length.

For a tube reactor of diameter D, dV = D dA ........... (4).

Substituting equations (3) and (4) into equation (1) gives and from this because of dx = NAo.dXA When working isothermally, dT = O and equation (5) becomes r, = 4h (Tw - T) = constant ............... (6) R #HDdB from which results that the distribution of the catalyst material in the reactor must be such that the reaction rate per unit volume of the reactor space is the same through the length of the reactor.

Combining equations (3) and (6) gives and it where e denotes the distance from the reactor inlet of the reactor section concerned and L denotes the reactor outlet.

For a first order catalytic reaction with a reaction rate constant kl, r = k1 NAO (1-XA) (9) Substituting equation (9) into equation (8), one obtains If klWL = NR (number of reactor units) and R '= 1 F fort = L results which is the same result as obtained by the kinetics of a first order reaction in a continuously stirred tank reactor. If equation (11) is introduced into equation (10), one obtains which specifies the manner in which the catalyst material must be distributed as a function of the reactor length, if undiluted catalyst material is provided at the reactor outlet, t / L = 0 at the reactor inlet.

From equation (12) it follows that when XAL = 0.5, R 'is 2 and when XAL = 0.9, R '= 10.

The total weight of diluent in the reactor can be determined as follows: From the definition of R 'and equation (10) results and from this WL = -F In (1 - XAL) ................ (13) by comparison with the equation (11), the mean dilution factor 7 for the catalyst material is given by the equation for example if XAL = 0.9, Rl = 4.

For catalytic reactions of the second order, which are carried out isothermally, it can be shown that the equations analogous to equations (12) and (14) result in the following approach: and R = 1 ............. (14a).

1 - XAL has If e.g. XAL = 0.9, / R 'at the inlet of the reactor has the Value 100 and R 'the value 10.

In the following it is shown that a reactor according to the invention essentially is stable with regard to fluctuations in the maximum bed temperature, which result from Changes in reactor wall temperatures result.

Using the values given for the known reactor (1) according to equation (11), the following results: @o da @ if XAL = 0.75, WL = 276.

F results from equations (6) and (8) Since T = 3400K, Tw = 3380K and from equation (14) - - 3 = 2.2, 71n1 / 4 shows that with an average dilution of the catalyst material of 2.2 the reaction isothermal at 340 ° K goes when the reactor wall temperature is 5580K. If it is desired to operate according to a non-isothermal optimal temperature sequence, the optimal relationship for dT must be derived and inserted into equation (5), which is then solved using the appropriate kinetic thermodynamic data. For a reversible exothermic reaction it has been shown that the optimal temperature sequence through where To is the optimal reaction temperature, Te is the equilibrium temperature, E1 is the activation energy of the reaction and E2 is the activation energy of the retrograde reaction, where using the Vantt Hoff isochore the equilibrium temperature is Te = #H ..... .......... (15a), where R is the gas constant, C is a constant and K div is the equilibrium constant of the reaction.

A number of examples are given below to illustrate the practice of the invention explain in the case of special applications.

1) Methanol synthesis, The chemical equation for methanol synthesis is usually given by and the rate of reaction per unit catalyst in a generalized reactor zone is given by the rate equation given in the book "Catalysis", published by PH Emmet, Verlag Reinhold, New York, 19559, page 549 where a represents the activity of each component and an effect factor for the catalyst.

For a feed of 12% CO, 80% H2 and 8% inert substances at 5950C and 280 atm, A '= 125, B' = 1.0, C '= 0.125 and D' = 4.63. Further values are: # = 0.67, # (volatility) CO, H2 = 1, # CH3OH = 0.52, Kp = 2.67 x 10-5 atm-2, #H = -24.450 g.mol, Cp = 7.6 cal / g.mol0C, ATAd (the adiabatic temperature rise for complete conversion = = 386 ° C.

From equations (6) and (8) results It is taken into account here that when the synthesis is carried out on a ZnO / Cr2O3 catalyst, the optimum reaction temperature should be 395 ° C. and the maximum permissible conversion of CO 30 ffi, so that substantial methane formation is avoided.

Using the rate equation for r according to equation (17) and with R '= 1> 0 when XAL = 0.3 results in rb = 6.7 x 10-2 g mol / g catalyst . Hour and WL = 0.556 g hour

F g Mcl.

Assuming cylinders of 9.5 mm in a catalyst bed packing according to Industrial and Engineering Chemistry, Volume 23, 1931 (page 910), which are considered equivalent compared to the reactor bed material, h = 2 x 10-3 if the The flow rate per unit cross-sectional area of the bed is G = 0.225 Has. Assuming that D = 5 cm and d3 = 0.8 (c.g.s. units), then gives Substituting these values in equation (17) for Tw = 167 ° C, which is the temperature of the steam is 7.7 ata and WL = 1370 g, which is 87 cm of a tube of 5 cm diameter is equivalent to.

At other positions along the reactor, the corresponding values of r can be included in the equation. (17) can be used. Since XA = @ from equation (8), one finds - LXL at (/ L = O, R '= 2.6. When @ / L = 0.5, R' = 1.8 and when @ / L = 1 , 0 is, R '= 10, R' = 2.6-1.6 f '/ L, which is the equation for optimum distribution of catalyst material along the reactor and WL = .536 = 0.3 g hrs.

F is 1.8 g moles which indicates the length of the catalyst bed of the reactor is 80% higher than the fixed bed of known reactors. However, since the reactor bed is only 87 cm long, this is Ar. rose insignificantly.

For a reactor of 5 cm in diameter, the production speed becomes of methanol NAOFXAL # 3 kg per hour. So around a ton per hour To produce methanol would require 553 such reactors and that Total weight of their beds would be about 1/2 ton, About what consists of about 1/4 ton of catalyst.

The available heat would be about 1 1/2 tons of steam at about 7.7 ata require.

Instead of introducing starting materials and products from the reactor removes while maintaining a temperature of 5950C, the products could be preheated of the starting materials to about 565 0C and a short adiabatic Bed containing neat catalyst material could be applied to raise the temperature to 395 ° C. The conversion of CO would be around 8%, so that the reactors according to the invention to 30-8 times the calculated 30 Length could be reduced. The optimal dilution would then be given by Rt = 2, - 1.6 ß and the mean L catalyst dilution given by ~ = 1.4.

R 'The diameter of the reactor and the flow rate of the Starting materials can of course be selected so that the results of those differ from this example. For example, it could be the production speed of the reactor according to the example can be doubled by both the reactor length and the flow rate is doubled by the reactor. The temperature on the reactor wall would be poor 260 ° C, corresponding to a water dam of 46 ata. The latter change arises from daii the relationship between the heat transfer coefficient h and the flow rate G is given by hOC G0.75. When the diameter of the reactor is reduced, the heat transfer area per unit volume increases of the reactor and a higher temperature of the reactor wall must be maintained, so that the desired reaction temperatures can be maintained.

2) ammonia synthesis. Ammonia becomes catalytic from the components according to the equation manufactured. The reaction is exothermic and reversible and therefore has a falling optimal temperature sequence. The synthesis is usually carried out at pressures of about 300 atm and the iron / promoter catalyst requires an upper temperature limit of about 560 ° C. The degree of conversion usually achieved per pass is somewhat less than 0.1 mole of N2 per mole of gas feed. The optimum starting temperature of the product is sufficiently high to be able to preheat the feed and an adiabatic reactor can be used to raise the temperature of the preheated feed to 560 ° C. above the reactor feed according to the invention. An optimally decreasing temperature sequence is maintained in such a reactor.

For a molar bond of hydrogen in the feed and a consumption of x moles of nitrogen per lWol of feed, it is shown according to feta Physiocochim, Volume 12, (1940), page 32 (that per cm3 of catalyst are consumed per second, where P indicates the pressure in atmospheres and kl and k2 indicate the reaction rates for the back and forth reactions.

Using the following values taken from the Journal of the American Chemical Society, Volume 45 (1923), page 2918 and "Chemical Engineering Science", Volume 1 (1952), page 145, @ = 0.686, P = 245 atm, #H = = - 2.66 x 104 cal / g mol, Cp = 7.0 cal / g mol ° C, Kp = exp 26.600 - 27.911 # (empty part of the reactor bed) = RTo and M (according to # equation (15) = 6.1939 x C (according to # equation (16)) = -2 '(, 911.

For the optimum temperature range, the general equilibrium temperature Te using equation (15a) is: where from equation (18) The dilution factor R 'for the catalyst becomes off calculated. For the reactor according to the invention and operating isothermally, this results in To = Te = 560 ° C = 8550K at 560 ° C.

1 + MTe The temperature of the reactor wall Tw is selected so that a temperature of 195 ° C is obtained in a jacket around the reactor, the is designed for rising water vapor # from a pressure of about 14 ata.

It can be calculated that with D = 10 cm and G = 0.04 g / cm2. Sec. the total length of the reactor bed including an adlabatic section, with the reactants being heated to 8220K, and one subsequent isothermal section of 833 ° K and finally a section of an optimal temperature sequence up to an output of 738 ° K would be 2.15 In. The optimal temperature sequence lies as follows: T ° K 825 799 776 756 738 1 (cm) 52.8 92.6 133.2 174.8 214.0 Rt 10.8 5.5 2.99 1.7 1.0 X 0.05 0.06 0.07 0.08 0.09 For production of 20 tons of ammonia per T @ g can be derived from these calculations, since # 210 Reactors are needed, each reactor having an adiabatic, an isotherm and have a portion of the optimal temperature sequence.

So that the jacket can be kept at 195 ° C, the total heat transfer coefficient must be h @ the value 0.0004 haberi instead of the taken value of 0.002 in e.g.s.-units.

This is achieved by providing an annular space mL.t of insulating material, such as a gas, between the reactor wall and the surrounding jacket. I) the width of this space is calculated from where D is the diameter of the reactor bed, Do is the diameter of the jacket at the outer boundary of the annular space and A is the thermal conductivity of the material in the annular space. In this example it is found that h + = 0.0004 when the annulus is 2 mm wide and contains synthesis gas.

When the reactants to the maximum allowable temperature in the adiabatic reactor part are fed and then the optimal temperature sequence is adhered to in the reactor according to the invention, needs only a minimal amount Catalyst to be used.

In certain circumstances it may be preferred to have an isolation room around the reactor as a means of lowering the temperature in a space surrounding this Sheath rather than the diameter of the reactor to achieve the same Effect is increased. In the latter I "all there is a probability that radial temperature gradients are promoted, leading to poor performance of the process could lead if the optimal reaction temperature is critical, e.g. at Reactions for the catalytic oxidation of hydrocarbons.

The isolation room is also cheaper than using, for example, boiling mercury or Baths made of eutectic salt mixture, which were previously used in reactors with a fixed catalyst bed for phthalic anhydride synthesis, so that the necessary high reactor wall temperature can be maintained.

The calculations given can apply to other catalytic chemical Reactions are used, e.g. for the production of sulfur dioxide, Phthalic anhydride and oxidation reactions of hydrocarbons.

The imaginary calculations do not take into account the effect of radial temperature gradients. For reactors with small diameters, this is Effect generally does not matter. The radial heat transfer rate is relatively large in reactors according to the invention compared to the speed the heat generated by the reaction and this can lead to reactors using unusually large diameter can be used. To explain this advantage, a self-optimizing (hill-climbing) computer program can be worked out.

In principle it is a triangular matrix that is a single tightly packed Representing layer of particles, worked out. Hexagonal connections are on the matrix is set which define a reactor diameter and it becomes a pseudo-random number generator used to identify a specific part of the particles in the reactor bed, which is to be accepted as catalytically active. Heat and mass equilibria are then made over each particle in the matrix, causing a reaction to go through the active particles and a lateral mixing of all adjacent streams between the particles is simulated. At the connecting lines of the matrix (the reactor wall) material is reflected and the temperature can be determined from the specific jacket temperature and the heat transfer coefficient on the wall according to "Advances in Chemical Engineering, Volume 3 (1962), page 204. The mean turnover about one a small number of finishes is then calculated.

The procedure is active for an increased number of randomly distributed Particles repeated and the mean conversion compared with the previous value. The program iterates with increasing amounts of active catalyst material up to the mean conversion or temperature reaches a desired value when the optimal Dilution of the catalyst material is printed out and the calculation goes to the next Group of layers of particles superimposed on it, causing you to move through from the inside out the reactor progresses. The program can be general, in the kinetic one and thermodynamic data can be fed in for each catalytic reaction. For complex reaction schemes, methods of variation can be used and es the selectivity instead of the implementation can be optimized while the effects a change in the reactor diameter and the temperatures of the jacket and the Reactor interior can be checked.

The distribution of the catalytic material in the reactor according to the invention and the above calculated examples is to be homogeneous or discontinuous Heaktorbett related. The matrix model used in the above computer program a histogram-like display the distribution of the catalytic Material and is therefore more realistic. The step length of the histogram corresponds to exactly the mean diameter of each individual body of the catalyst material.

Ythalic acid pearl synthesis The above processes were used to study the catalytic oxidation of O-xylene to phthalic anhydride using the kinetic schemes and values in "Industrial and Engineering Chemistry" (No. 2), Volume 59, page 18 (1967). The author used a two-dimensional but homogeneous model to show the sensitivity of the parameters of this reaction in a cooled tubular reactor, with the proviso that the length of the reactor should not be more than 7 m.

A = o-xylene B = phthalic anhydride C = combined products.

There is excess air.

(NO) = 0.208; (NO) = 0.00924 = 44 o-xylene dB = 1.3 g / cm3; D - 2.5 cm; d = 0.3 cm; G = 0.13 g / cm2 sec. D = the particle diameter of the catalyst, G = the 1st speed of the mass. From the mentioned activation energies it can be clearly seen that the best yield is from i3 at such a low temperature is obtained as it is more useful with a high conversion of A in a reactor Length is tolerable.

For isothermal conditions of the reaction it can easily be shown that the nlaxi. male yield of phthalic anhydride by the equation is given and the corresponding reactor length for the working conditions mentioned the value Has.

This results in the following scheme, for example: Temp. ° C Ymax Z o (selectivity) 555 0.739 3210 0.785 365 0.721 2340 0.769 575 0.715 1575 0.765 585 0.710 113Q 0.761 395 0.710 811 0.755 showing that yield and selectivity are not very temperature dependent and a temperature of about 3900C a yield of about 70.5% in a 3 m reactor with catalyst particles 0.3 cm in diameter. It appears from these values that the most important factor that determines the functioning of the reactor, an avoidance of Temperature instabilities. The matrix program of the catalyst was therefore designed for various temperatures of the feed jacket are allowed to drain using of catalyst dilutions, which just adjust the reaction temperatures to different previously selected values Tmax forced. To this end and taking into account practical Requirements, the reactor of 3 m length was divided into 10 equal sections, each of which should contain catalyst with a constant dilution factor. The calculator calculated then the maximum uniform catalyst concentration in each section, the temperature inevitably randomly each in the section distributed catalyst particles forced to the preselected maximum. By repetition the calculations were in good agreement with a reasonable random rate of the catalyst pellets shown with the pseudo-random numbering applied became.

A catalyst compound has been shown to reduce the yield of phthalic anhydride increased by about 10% and the fluctuations in jacket temperature doubled that without Runaway of the reactor can be allowed.

The results were also obtained when the reactor diameter was increased checked from 2.4 cm to 7.2 cm.

Large reactor diameters naturally have the disadvantage that if the central core is heated according to the desired temperature sequence, a liquid Current on the reactor wall of a lower and less effective temperature sequence will obey. When increasing the diameter, the radial temperature gradients must be kept to a minimum by increasing the effective thermal conductivity of the bed is made as big as possible.

For working in the steady state, the value of the heat transfer coefficient is i the fluctuation is not critical, as a low value due to a drop in the jacket temperature can be compensated. This situation is however against disturbances less stable than when the heat transfer coefficient of the wall is high and the Temperature drop on the wall is small. To reduce the radial temperature gradients a catalyst dilution can be carried out, but the in a Given the reactor length, the yields obtained are not as high as those obtained with Iicairtoren smaller diameter is the case where little or no dilution is required is.

This is explained by the results for the reactor of 7> 2 cm Diameter and 5 m in length, which contains catalyst particles of 9 mm in diameter. The maximum yield of 57 ß was obtained at a jacket temperature of 510 0C compared to 70% in the reactor with a diameter of 2.4 cm and a jacket temperature of 370 ° C. By increasing the particle diameter to 1.2 cm, the yield increased 62% increased, assuming that the kinetic data on particles of this Size are applicable. (The active surface area was considered proportional to the particle weight accepted). The effect of disturbances in jacket temperature has not been studied, however, it is likely that stability will be poor. It was closed that any increase in tube diameter is negligible if the yield of primary The importance of the catalyst dilution in radial direction is and was coincidental is.

Improvements in the effectiveness of the reactor; are of course because of this possible, that mali provides a radial distribution of the catalyst, so that a larger one Amount of active catalyst to lie closer to the wall comes to de temperature to support in this area and to flatten the radial temperature profile. In in practice this can easily be done by using a coaxial cylinder introduced into the empty reactor by wire mesh or rolled-out metal and the outer space is filled with pure 1 catalyst, the much larger one inner space is filled with dilute catalyst as before.

For the production of a reactor bed for use in an invention Reactor can be used a process wherein the bed of a diluent material consists in which pellets of catalyst material are distributed and where the bed is divided into layers in the direction of flow, which are equal to the mean diameter j each individual particle of the catalyst material siiid. Then for each shift an approach with the calculated amount of catalyst material and diluent thoroughly mixed and arranged in the assumed) layer of the catalyst bed. This Wouldn't be so difficult in the case. of ammonia synthesis at 210 Reactors in converter 210 batches of essentially identical preparations for each there is a partially limed converter layer and each batch contains about 12,600 pellets, when the catalytic material is in the form of pellets with a mean diameter 1 cm is present. III in this case it is assumed that the ammonine converter with Catalyst could be filled in about 2 days per worker.

Sollerl reactors according to the invention with beds of relatively large size Diameter are used to carry out chemical catalytic reactions, so the given calculations can be adapted or modified to accommodate arrangements calculate where the distribution of the catalyst material is transverse to the direction of flow the respondent fluctuates.

The bed in the reactor would then have to be physically divided into zones, which extend parallel to the transverse periphery of the bed, so that a gradation can be effected in the transverse direction in the distribution of the catalyst material.

PATENT CLAIMS:

Claims (1)

PATENT CLAIMS: 1) Tubular reactor for catalytic reaction with solid Catalyst material, characterized in that aas catalyst material in alternating Amount in the direction of flow of the reactants is arranged so that in each Reactor section, the amount of catalyst present is sufficient that the desired temperature in the steady state, resulting from the competing speeds of heat generation (or heat absorption) and the heat transfer in the respective reactor section results is achieved. 2) tubular reactor according to claim 1, characterized in that the Amount of catalyst material per unit volume by mixing the catalyst material is adjusted with catalytically inert particulate material. )) Tubular reactor according to claim 1 or 2, characterized in that the distribution of the catalyst material also in the transverse direction to the direction of flow the respondent is changed. 4) tubular reactor according to claim 1 to 3, characterized in that Means are provided for circulating a coolant around the reactor wall. 5) Method of Performing Catalytic I-Reactions Using a tubular reactor at a preselected temperature, characterized in that the preselected temperature distribution in the tubular reactor by introducing such a The amount of catalyst material is adjusted in the direction of flow of the reactants, that the amount of catalyst present in each reactor section is sufficient that the Desired steady-state temperature resulting from the competing speeds heat generation (or heat absorption) and heat transfer in the respective Reactor section results is achieved. 6) Method according to claim 5, characterized in that the amount of catalyst per unit volume of the reactor by mixing the catalyst material with catalytic inert Particulate matter is adjusted. 7) to method llach claim 5 or G, characterized in that the distribution of the catalyst material also in the transverse direction to the direction of flow is varied so that in the reactor a temperature profile in the transverse direction to the direction of flow is set. 8) Method according to claim 5 to 7, characterized in that a Coolant is circulated around the reactor wall. 9) Method according to claim 5 to 8, characterized in that as catalytic reaction the production of methanol from carbon dioxide and hydrogen is carried out. io) Method according to claim 1 to 8, characterized in that because the catalytic reaction is the production of ammonia from nitrogen and hydrogen is carried out. 11) Method according to claim 5 to 8, characterized in that as catalytic reaction the production of phthalic anhydride by oxidation of o-xylene is carried out.