EP1289650A2 - Dispositif et procede permettant de mettre en oeuvre des reactions en phase gazeuse, a catalyse heterogene, avec chaleur de reaction - Google Patents

Dispositif et procede permettant de mettre en oeuvre des reactions en phase gazeuse, a catalyse heterogene, avec chaleur de reaction

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Publication number
EP1289650A2
EP1289650A2 EP01957805A EP01957805A EP1289650A2 EP 1289650 A2 EP1289650 A2 EP 1289650A2 EP 01957805 A EP01957805 A EP 01957805A EP 01957805 A EP01957805 A EP 01957805A EP 1289650 A2 EP1289650 A2 EP 1289650A2
Authority
EP
European Patent Office
Prior art keywords
catalyst
reactor
reactor space
heat
reaction gas
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP01957805A
Other languages
German (de)
English (en)
Inventor
Franz Josef BRÖCKER
Mathias Haake
Manfred Stroezel
Otto Wörz
Ekkehard Schwab
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
BASF SE
Original Assignee
BASF SE
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by BASF SE filed Critical BASF SE
Publication of EP1289650A2 publication Critical patent/EP1289650A2/fr
Withdrawn legal-status Critical Current

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F28—HEAT EXCHANGE IN GENERAL
    • F28D—HEAT-EXCHANGE APPARATUS, NOT PROVIDED FOR IN ANOTHER SUBCLASS, IN WHICH THE HEAT-EXCHANGE MEDIA DO NOT COME INTO DIRECT CONTACT
    • F28D9/00—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall
    • F28D9/04—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits being formed by spirally-wound plates or laminae
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J12/00—Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor
    • B01J12/007—Chemical processes in general for reacting gaseous media with gaseous media; Apparatus specially adapted therefor in the presence of catalytically active bodies, e.g. porous plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/0006—Controlling or regulating processes
    • B01J19/0013—Controlling the temperature of the process
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/248—Reactors comprising multiple separated flow channels
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C45/00—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds
    • C07C45/27—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by oxidation
    • C07C45/32—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by oxidation with molecular oxygen
    • C07C45/37—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by oxidation with molecular oxygen of >C—O—functional groups to >C=O groups
    • C07C45/38—Preparation of compounds having >C = O groups bound only to carbon or hydrogen atoms; Preparation of chelates of such compounds by oxidation with molecular oxygen of >C—O—functional groups to >C=O groups being a primary hydroxyl group
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00074—Controlling the temperature by indirect heating or cooling employing heat exchange fluids
    • B01J2219/00076—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements inside the reactor
    • B01J2219/00085—Plates; Jackets; Cylinders
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/00074—Controlling the temperature by indirect heating or cooling employing heat exchange fluids
    • B01J2219/00087—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements outside the reactor
    • B01J2219/00096—Plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/19—Details relating to the geometry of the reactor
    • B01J2219/194—Details relating to the geometry of the reactor round
    • B01J2219/1941—Details relating to the geometry of the reactor round circular or disk-shaped
    • B01J2219/1944—Details relating to the geometry of the reactor round circular or disk-shaped spiral
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/324—Composition or microstructure of the elements
    • B01J2219/32466—Composition or microstructure of the elements comprising catalytically active material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/324—Composition or microstructure of the elements
    • B01J2219/32466—Composition or microstructure of the elements comprising catalytically active material
    • B01J2219/32475—Composition or microstructure of the elements comprising catalytically active material involving heat exchange

Definitions

  • the invention relates to a method and a device for the approximately isothermal implementation of gas phase reactions with high heat emission, especially of oxidative dehydrogenations, on a solid catalyst.
  • DE-A 42 43 500 discloses the use of special wire mesh catalyst inserts coated with catalyst for exhaust gas purification.
  • the wire mesh or wire mesh layers are thermally and / or mechanically fixed in the wound state.
  • the complicated construction of the catalyst insert and the poor heat transfer within it are problematic.
  • Materials of the filter or catalyst body one of compression-molded wires or fibers as a tangle, braid, knitted fabric or in or
  • the filter or catalyst body can be traversed by heat exchanger tubes or channels transversely or counter to the exhaust gas flow direction directed through the filter or catalyst body.
  • EP-B 201 614 describes a reactor for carrying out heterogeneous, catalyzed chemical reactions which contains ribbon-shaped, at least partially corrugated catalyst bodies, the corrugation of which is inclined at an angle to the main flow axis and directed in the opposite direction in the case of adjacent plates, the wavelength of the corrugation of the catalyst body being smaller than the wavelength of the adjacent corrugated plate and the surface of the catalyst is larger than the surface of an adjacent corrugated plate.
  • the catalyst can be a body coated with a catalytically active material, which can optionally be designed as a wire mesh or wire mesh.
  • the complicated corrugation of the plates favors bypass formation, makes vortex formation difficult and thus impairs the mass transfer.
  • the compact packing element provided does not allow effective removal of the heat of reaction.
  • EP-B 0 305 203 describes the implementation of heterogeneously catalyzed reactions under non-adiabatic conditions.
  • monolithic catalysts in the form of catalyst plates are placed in an annular reactor chamber which has heat-dissipating walls.
  • the monolithic catalysts have channels which are at an angle to the main flow axis, so that the reaction fluid is conducted at an acute angle from one reactor wall to the other.
  • the shear stress that is exerted on the reaction fluid is extremely high near the reactor wall (high pressure loss) and otherwise rather low (poor material transport).
  • the manufacturing method of the reactor is complex since the pressure loss depends crucially on the geometry between the reactor wall and the monolithic catalyst.
  • EP-B 0 149 456 relates to a process for the preparation of a glyoxylic acid ester by oxydehydrogenation of the corresponding glycolic acid ester in the gas phase.
  • a tubular reactor is used which has a catalyst support made of at least one cylindrical monolith, the monolith having essentially the same diameter as the reactor tube and containing channels with a diameter of 1 to 10 mm which lead from the inlet to the outlet of the reaction tube , and wherein 60 to 90% of the monolith volume of Cavities is formed.
  • the channels can form an angle of 20 to 70 ° with the reactor axis. This measure directs the reaction fluid to the reactor walls and thus promotes the removal of the heat of reaction.
  • This method has the same disadvantages as the method known from EP-B 0 305 203.
  • DE-A 197 25 378 describes a compact fixed bed reactor for catalytic reactions in the gaseous and / or liquid phase through which two streams of material flow in cocurrent or countercurrent.
  • the flow channels for the two material flows are formed here by an accordion-like folding of a partition.
  • Corrugated structures are installed in the folds of the partition thus formed in such a way that continuous flow channels for the fluid flows are created.
  • the corrugated structures serve both as a spacer between the opposite folds of the partition and as a catalyst carrier and ensure improved heat transfer to / from the partition.
  • the corrugated structures are rigid structures, the dimensions of which limit the minimum distance between the folds of the partition walls and the amount of catalyst that can be applied to these corrugated structures.
  • the ratio of the surface of the corrugated structures (ie the catalyst) to the heat exchanger volume is a maximum of 800 m 2 / m 3 if one assumes a maximum technically feasible bend width of 5 mm and a corner angle of 90 °.
  • the manufacturing method of the reactor is relatively complex.
  • a device for largely isothermally carrying out a heterogeneously catalyzed reaction in the gas phase with high heat emission having at least one reactor space with inlet and outlet, wherein the reactor space is delimited by heat-dissipating walls which have a substantially constant distance along the main flow axis of a reaction gas of 30 30 mm,
  • the reactor room is equipped with strips coated with catalyst
  • the strips are flexible in all spatial directions and permeable to the reaction gas, have a surface-to-volume ratio of 50 to 5000 m 2 / m 3 and good thermal conductivity,
  • reaction gas flows through the reactor space at a speed of ⁇ 200 m 3 per m 2 of flow area and per hour, and
  • a heat exchange medium flows on the side of the reactor wall facing away from the reactor space.
  • the device according to the invention is suitable for carrying out strongly exothermic as well as strongly endothermic reactions since it enables rapid heat dissipation or heat supply.
  • strongly endothermic reactions are oxidative dehydrogenations such as that of 3-methyl-3-buten-l-ol, hydrogenation of double or triple bonds and aromatics such as the hydrogenation of benzene to cyclohexane are examples of strongly exothermic reactions.
  • the enthalpies of these reactions are, for example, in the range from 30 to 75 kcal / mol.
  • the device according to the invention also makes it possible to work under negative or positive pressure, that is to say at pressures from 1-10 -3 to 100 bar, in particular from 0.5 to 40 bar.
  • the device according to the invention can therefore be used in a wide pressure range.
  • Reaction gas is understood to mean the mixture of gaseous reactants and any further gaseous substances added, which do not react with the reactants under the reaction conditions.
  • the heat exchange medium can be a liquid, a gas or a molten salt bath, depending on the desired temperature. Does the warmth Exchange medium for the absorption and removal of heat, this is also called a cooling fluid. Temperatures from -20 ° C to 400 ° C can be easily achieved. The rapid heat dissipation or heat supply that is made possible by the device according to the invention enables very precise heat control. For example, temperatures of 370 ° C ⁇ 10 ° C, in particular ⁇ 5 ° C, can be set. In contrast to conventional fixed bed reactors, no temperature peaks occur when using the device according to the invention.
  • the reactor space can be annular, cylindrical, rectangular or square.
  • the device according to the invention can be easily realized by introducing the catalyst-coated strips (catalyst strips) into the gap of a commercially available heat exchanger. So there is no adaptation of the reactor tube to the catalyst, but an adaptation of the catalyst bands to the reaction space. Any heat exchanger can be used. Annular gap heat exchangers as well as plate heat exchangers or spiral heat exchangers are suitable. Examples of heat exchangers are constructions such as those in ISO 15547 or in WRA Vauck, HA Müller, basic operations of chemical process engineering, Verlag Theodor Steinkopff Dresden 1974, 4th edition, pp.
  • the distance from the wall and thus the gap width or the gap diameter of the heat exchangers used is preferably 0.5 to 30 mm, especially 1 to 20 mm, in particular 1.5 to 10 mm or 1.8 to 5 mm.
  • the catalyst belts are introduced into the reactor space formed by two coaxial tubes and cooled (or heated) through the wall of the inner tube and or of the outer tube.
  • This device according to the invention is also referred to as an "annular gap heat exchanger reactor".
  • Plate heat exchangers have a square or rectangular reactor space which is optionally subdivided by additional heat-dissipating walls which force the reaction gas through the reactor space in a zigzag course.
  • the catalyst strips are introduced into the reactor space, catalyst strips possibly being omitted at the points where the greatest change in direction occurs * in order to avoid an excessive pressure drop.
  • a device according to the invention which uses a spiral heat exchanger (“spiral heat exchanger reactor”), has an in particular cylindrical reactor space which is equipped with catalyst belts as evenly as possible.
  • the catalyst belts are flat, smooth structures which can be formed as woven, knitted and knitted fabrics, perforated sheets or - in the case of metal as a material - as expanded metal.
  • felts or foils can also be used, however, these have to be combined with fabrics, knitted fabrics, knitted fabrics, perforated sheets or expanded metals, whereby the felts or foils must be aligned parallel to the main flow direction and the fabrics, knitted fabrics, knitted fabrics, perforated sheets or expanded metals as spacers for the felts or foils are used.
  • felts or foils which are oriented parallel to the main flow direction, can be introduced into the reactor space with woven fabrics, knitted fabrics, knitted fabrics, perforated sheets or expanded metals. Woven fabrics, knitted fabrics or knitted fabrics are preferably used.
  • the catalyst belts are characterized by the fact that they are flexible in all spatial directions, that is to say bendable and stretchable. These are unstructured shaped catalyst bodies which can easily be adapted to the dimensions of the reactor space, in particular the columns of commercial heat exchangers. When using them, fixation and alignment on the main flow axis are not required. Since the catalyst belts are flexible in all spatial directions, they fix themselves. In general, the catalyst belts are introduced individually, rolled or layered into the reactor space without prior deformation (eg by stamping a surface layer such as waves with the aid of a gear roller). This enables a higher one Packing density of the catalyst belts with uniform filling of the reactor space and maximum suppression of undesired bypass formation, which is reflected in an increase in the mass exchange.
  • the catalyst belts are inserted by manual insertion, positioning or pushing into the gap of the heat exchanger.
  • the limiting factors are the dimensions of the reactor space and the thickness of the catalyst strips. Both one and several catalyst belts can be introduced.
  • the catalyst belts can be distributed over the entire reactor space of the heat exchangers, or can only be positioned on sections selected by the person skilled in the art. Since the catalyst belts are flexible in all spatial directions, they can be stretched as well as layered, folded or rolled.
  • Stretching is understood to mean pulling a catalyst belt into length or width.
  • the catalyst strips can be stretched by up to 60%, depending on the material of the strip.
  • Layers are understood to mean the laying on of at least two catalyst bands, folding means the laying of one and the same catalyst band, the direction of the band being changed by 180 ° in certain or arbitrarily selected sections.
  • the catalyst strips stacked one on top of the other can optionally also be folded or rolled.
  • the surface of the catalyst belts can be increased by folding or rolling the catalyst belts more strongly, without the space requirement (the volume) of these more folded or rolled catalyst belts being significantly increased.
  • the catalyst belts have a high surface-to-volume ratio of 50 to 5000 m / m. Such a high surface-to-volume
  • the small wall clearances of the reactor space which are generally 30 30 mm, preferably ⁇ 20 mm, particularly preferably 10 10 mm, are also advantageous for rapid heat transport.
  • the volume of the reactor space is determined by the volume of the column of commercial heat exchangers.
  • the catalyst belts are also mechanically very stable, so that the heterogeneously catalyzed reactions in the gas phase can also be carried out at high flow rates of the reaction gas without the catalyst being subject to any significant abrasion.
  • the device according to the invention can also be used at low flow velocities, but it is precisely at flow velocities ⁇ 200
  • the flow rate is selected depending on the process (working at negative, normal or positive pressure) and depending on the ratio of the volume of the catalyst belts to the volume of the reactor space.
  • Gas flow rates of up to 70 m / s can be achieved in the apparatus according to the invention not equipped with catalyst belts. Typical values for gas flow velocities in heat exchangers are 40 m / s.
  • the catalyst-bands equipped apparatus according to the invention can be combined with m flow rates from 200 to 15,000 5 - at zero incidence area [m] h, in particular at flow rates from 300 to 15,000 m and especially at flow rates of at zero incidence area [m] hm
  • the specified flow area mh Speeds are empty tube speeds that were determined with a gas meter.
  • the device according to the invention is also designed to maintain a high but uniform shear stress on the reaction gas. On the one hand, as already mentioned above, it withstands a high cross-sectional load without the catalyst being ground. On the other hand, the reaction gas is exposed to a uniformly high shear stress in the reactor space provided with catalyst belts. This leads to a uniform swirling of the reaction gas and thus to a constant level of mixing of the reaction gas as it passes through the reactor space. Due to the high flow velocities and the thorough mixing of the reaction gas, the devices according to the invention can achieve sales as high as with conventional reactors, the catalyst requirement being lower when the reactions are carried out in conventional reactors when the reactions are carried out in the devices according to the invention. Another advantage of the device according to the invention is that no complex structuring of the Catalyst or catalyst support is required, so that costs can be saved.
  • the catalyst belts usually have a fine structure.
  • the fine structure consists of the rectangles formed by the wire or thread, which each share the sides with one another.
  • the setting angle which one side of the two sides forming a rectangle form with the main flow axis of the reaction gas is even preferably randomly distributed.
  • the term of the randomly distributed setting angle means that the catalyst belts are brought into the reactor space in such a way that ideally all possible setting angles are realized and that consequently a chaotic meshwork is created. With such a chaotic meshwork, the sequence of cavities, wires or threads in the reactor space is random due to the random orientation of the catalyst strips. This minimizes the bypass formation within the reactor and maximizes the heat and mass transfer due to a turbulent flow.
  • the materials used for the band are selected from the metallic and ceramic materials and plastics in accordance with the deformations that occur during manufacture, reworking and use.
  • those metallic and ceramic materials and plastics are suitable that form fibrous structures.
  • metallic materials are pure metals such as iron, copper, nickel, silver, aluminum and titanium or alloys such as steels such as nickel, chromium and / or molybdenum steel, brass, phosphor bronze, monel and / or nickel silver.
  • ceramic materials are aluminum oxide, silicon dioxide (glass fibers), zirconium dioxide and / or carbon.
  • plastic fibers are those made from polyamides, polyethers, polyvinyl, polyethylene, polypropylene, polytetrafluoroethylene, polyketones, polyether sulfones, epoxy resins, alkyd resins, urea and / or melamine resins.
  • Metals, asbestos substitutes, glass fibers, carbon fibers and / or plastics, in particular metals, that is to say pure metals and alloys, are preferred since these have a very good heat transfer coefficient.
  • Inexpensive stainless steels are particularly preferred, which are catalytically coated accordingly.
  • the tapes coated with catalyst according to the invention are in particular metal mesh or knitted metal.
  • metal mesh is understood to mean a wickerwork made of metal, which is formed by a circumferential metal thread.
  • Metal mesh is understood to be a wickerwork made from at least two metal threads.
  • the wire diameter is generally 0.01 to 5.0 mm, preferably 0.04 to 1.0 mm in the case of metal mesh or knitted metal.
  • the mesh size can be varied over a wide range.
  • the catalyst belts can be produced by the process described in US Pat. No. 4,686,202 and EP-B 0 965 384.
  • Catalyst belts in the form of metal mesh can also be coated using the method described in EP-B 0 564 830.
  • the coating of metal knitted fabrics with a catalyst is not explicitly described in EP-B 0 564 830, but the procedure is the same as for metal fabrics.
  • the coating of metal fabrics or knitted fabrics with catalysts can also be carried out by conventional immersion processes, e.g. by the process described in EP-A 0 056 435. Reference is made in full to US-A 4 686 202, EP-B 0 965 384, EP-B 0 564 830 and EP-A 0 056 435.
  • metal from which the metal fabric or knitted fabric is made (possibly after treatment) is itself catalytically active, then a coating can be dispensed with entirely.
  • FIG. 1 is a schematic drawing of a plate heat exchanger reactor according to the invention
  • FIG. 2 shows a side view of the inside of a spiral heat exchanger reactor
  • FIG. 3 shows a further side view of a spiral heat exchanger reactor.
  • Fig. 1 an inventive plate heat exchanger reactor (101) is shown.
  • the strips coated with catalyst have the reference symbol 120.
  • 131 denotes the inlet of the reaction gas into the reactor space, 143 the outlet.
  • Inlet and outlet of the heat exchange by means of cooling fluids are provided with the reference numbers 144 and 142, respectively.
  • Fig. 2 shows a side view of a spiral heat exchanger reactor according to the invention.
  • 131 denotes the feed of the reaction gas into the reactor space (reactor inlet).
  • 132 denotes the reactor space (gap), which receives the catalyst-coated tapes, which fill the entire space in more or less dense packing.
  • 133 denotes the (cooling) gap that is to receive the heat exchange medium / cooling fluid.
  • FIG. 3 shows a side view of a spiral heat exchanger reactor and denotes the arrangement of the inlet and outlet connections.
  • 141 Reaction gas inlet (reactor inlet)
  • 142 Heat exchange medium / cooling fluid outlet
  • 143 Reaction gas outlet (reactor outlet)
  • 144 Inlet
  • Heat exchange medium / cooling fluid Reaction gas and heat exchange medium / cooling fluid are arranged here in counterflow in order to exchange maximum amounts of heat. Is just the amount of heat released at the reactor inlet with regard to z. B. selectivity and catalyst stability critical, an arrangement in the direct current principle is recommended.
  • the reaction is carried out on a silver catalyst.
  • the catalyst according to the invention is coated by coating a metal fabric strip made of heat-resistant stainless steel, material no. 1.4764 (according to the Stahl-Eisenliste, 8th edition, publisher: disclose Deutscher Ironworkers), made with silver in an electron beam deposition system. With this coating technique, the metal fabric tape was coated on both sides with 300 ⁇ m Ag. 50 cm 2 of this catalyst fabric tape were introduced undeformed in the form of a double layer into a 2 mm wide annular gap heat exchanger reactor. The amount of active component was 34 mg silver.
  • MBE 3-methyl-3-buten-l-ol
  • the gaseous reaction product was cooled with cooling brine at a temperature of 0 ° C. and the condensate was collected in a cooled separator.
  • the gaseous fraction of the reaction product was passed through dry ice cooling, with which the low boiler fractions were condensed, for gas chromatographic analysis and then via a gas meter into the exhaust gas.
  • the combined amounts of condensate were separated into an organic and an aqueous phase. Both phases were analyzed. The result was a selectivity of 83% with a turnover of 54%.
  • the selectivity of the comparative example is 10% worse than that of the example according to the invention.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Thermal Sciences (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Catalysts (AREA)
  • Devices And Processes Conducted In The Presence Of Fluids And Solid Particles (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)

Abstract

La présente invention concerne un dispositif permettant de mettre en oeuvre, de manière sensiblement isotherme, une réaction en phase gazeuse, à catalyse hétérogène, avec une grande chaleur de réaction. Ce dispositif comprend au moins une chambre de réacteur (101) présentant une entrée (131, 141) et une sortie (143). Cette chambre de réacteur est définie par des parois dissipant la chaleur, qui se trouvent à une distance sensiblement constante, inférieure ou égale à 30 mm, le long de l'axe d'écoulement principal d'un gaz de réaction. Ladite chambre de réacteur est pourvue de bandes (120, 132) qui sont recouvertes de catalyseur. Ces bandes sont souples dans toutes les directions spatiales, sont perméables au gaz de réaction et présentent un rapport aire/volume qui va de 50 à 5000 m2/m3, ainsi qu'une bonne conductivité thermique. Le gaz de réaction s'écoule à travers la chambre de réacteur à une vitesse supérieure ou égale à 200 m?3 par m2¿ de surface d'écoulement et par heure. Un agent d'échange thermique s'écoule sur la face de la paroi du réacteur qui est opposée à la chambre de réacteur.
EP01957805A 2000-05-24 2001-05-25 Dispositif et procede permettant de mettre en oeuvre des reactions en phase gazeuse, a catalyse heterogene, avec chaleur de reaction Withdrawn EP1289650A2 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE10025382 2000-05-24
DE10025382A DE10025382A1 (de) 2000-05-24 2000-05-24 Vorrichtung und Verfahren zur Durchführung von heterogen katalysierten Gasphasenreaktionen mit Wärmetönung
PCT/EP2001/006034 WO2001089683A2 (fr) 2000-05-24 2001-05-25 Dispositif et procede permettant de mettre en oeuvre des reactions en phase gazeuse, a catalyse heterogene, avec chaleur de reaction

Publications (1)

Publication Number Publication Date
EP1289650A2 true EP1289650A2 (fr) 2003-03-12

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Application Number Title Priority Date Filing Date
EP01957805A Withdrawn EP1289650A2 (fr) 2000-05-24 2001-05-25 Dispositif et procede permettant de mettre en oeuvre des reactions en phase gazeuse, a catalyse heterogene, avec chaleur de reaction

Country Status (7)

Country Link
EP (1) EP1289650A2 (fr)
JP (1) JP2003534299A (fr)
KR (1) KR20030022131A (fr)
CN (1) CN1188212C (fr)
DE (1) DE10025382A1 (fr)
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IT955185B (it) * 1972-04-29 1973-09-29 Saes Getter Spa Cartuccia catalitica
DE3402713A1 (de) * 1984-01-26 1985-08-08 Linde Ag, 6200 Wiesbaden Verfahren und reaktor zur durchfuehrung einer endothermen reaktion
DK169060B1 (da) * 1990-10-29 1994-08-08 Topsoe Haldor As Reaktor til dampreforming af carbonhydrider under varmeveksling
DE4207905A1 (de) * 1992-03-12 1993-09-16 Bayer Ag Festbettreaktoren mit kurzem katalysatorbett in stroemungsrichtung
JP3313766B2 (ja) * 1992-07-15 2002-08-12 財団法人石油産業活性化センター 水蒸気改質用薄膜状触媒
DE19725378A1 (de) * 1997-06-16 1998-12-17 Gerhard Friedrich Kompakter Festbettreaktor für katalytische Reaktionen mit integriertem Wärmeaustausch
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WO2001089683A3 (fr) 2002-05-10
CN1188212C (zh) 2005-02-09
WO2001089683A2 (fr) 2001-11-29
WO2001089683A9 (fr) 2004-11-11
JP2003534299A (ja) 2003-11-18
TW575462B (en) 2004-02-11
KR20030022131A (ko) 2003-03-15
CN1437506A (zh) 2003-08-20
DE10025382A1 (de) 2001-12-06

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