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
  • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
  • B01J8/008—Details of the reactor or of the particulate material; Processes to increase or to retard the rate of reaction
• • 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
  • B01J19/24—Stationary reactors without moving elements inside
  • B01J19/248—Reactors comprising multiple separated flow channels
  • B01J19/2485—Monolithic reactors
• • 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
  • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
  • B01J23/002—Mixed oxides other than spinels, e.g. perovskite
• • 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
  • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
  • B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
  • B01J23/32—Manganese, technetium or rhenium
  • B01J23/36—Rhenium
• • 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
  • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
  • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
  • B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
  • B01J23/56—Platinum group metals
  • B01J23/63—Platinum group metals with rare earths or actinides
• • 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
  • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
  • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
  • B01J23/89—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with noble metals
  • B01J23/892—Nickel and noble metals
• • 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
  • B01J35/00—Catalysts, in general, characterised by their form or physical properties
  • B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
  • B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
• • 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
  • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
  • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
  • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
  • B01J8/0446—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical
  • B01J8/0449—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical beds
  • B01J8/0453—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the flow within the beds being predominantly vertical in two or more cylindrical beds the beds being superimposed one above the other
• • 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
  • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
  • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
  • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
  • B01J8/0496—Heating or cooling the reactor
• • 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
  • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
  • B01J2208/00008—Controlling the process
  • B01J2208/00017—Controlling the temperature
  • B01J2208/00389—Controlling the temperature using electric heating or cooling elements
  • B01J2208/00398—Controlling the temperature using electric heating or cooling elements inside the reactor bed
• • 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
  • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
  • B01J2208/00008—Controlling the process
  • B01J2208/00017—Controlling the temperature
  • B01J2208/00389—Controlling the temperature using electric heating or cooling elements
  • B01J2208/00415—Controlling the temperature using electric heating or cooling elements electric resistance heaters
• • 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
  • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
  • B01J2208/00008—Controlling the process
  • B01J2208/00017—Controlling the temperature
  • B01J2208/00522—Controlling the temperature using inert heat absorbing solids outside the bed
• • 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
  • B01J2219/24—Stationary reactors without moving elements inside
  • B01J2219/2401—Reactors comprising multiple separate flow channels
  • B01J2219/2402—Monolithic-type reactors
  • B01J2219/2409—Heat exchange aspects
  • B01J2219/2416—Additional heat exchange means, e.g. electric resistance heater, coils
• • 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
  • B01J2219/24—Stationary reactors without moving elements inside
  • B01J2219/2401—Reactors comprising multiple separate flow channels
  • B01J2219/2402—Monolithic-type reactors
  • B01J2219/2425—Construction materials
  • B01J2219/2427—Catalysts
  • B01J2219/2428—Catalysts coated on the surface of the monolith channels
• • 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
  • B01J2219/24—Stationary reactors without moving elements inside
  • B01J2219/2401—Reactors comprising multiple separate flow channels
  • B01J2219/2402—Monolithic-type reactors
  • B01J2219/2425—Construction materials
  • B01J2219/2427—Catalysts
  • B01J2219/243—Catalyst in granular form in the channels

Definitions

• the present invention relates to a flow reactor for the reaction of a fluid comprising reactants, comprising a plurality of oil layers as viewed in the flow direction of the fluid. which are electrically heated by means of heating elements and wherein the heating levels can be traversed by the fluid, wherein a catalyst is arranged on at least one heating element and can be heated there. It further relates to a method for operating a flow control element according to the invention.
• synthesis gas is produced by steam reforming of methane. Due to the high heat demand of the reactions involved, they are carried out in externally heated reformer tubes. Characteristic of this method is the limitation by the reaction equilibrium, a heat transport limitation and especially the pressure and temperature! imitation of the reformer tubes used (nickel-based steels). Temperature and pressure side results in a limitation to a maximum of 900 ° C at about 10 to 40 bar.
• An alternative method is autothermal reforming.
• a portion of the fuel is burned by the addition of oxygen within the reformer, so that the reaction gas is heated and the expiring endothermic reactions are supplied with heat.
• DE 10 2008 027 882 A1 relates to a process for the production of a carbon monoxide-rich, low-methane gas (synthesis gas), wherein an insert containing hydrocarbons
• an apparatus for producing a low carbon, low methane gas comprising a refractory lined, pressure resistant reactor (ATR reactor) in which a hydrocarbon containing feed (fuel) is co-charged with carbon dioxide (CO2) and / or Steam and Oxidationsmittei by catalytically assisted partial oxidation (autothermal reforming or ATR) can be implemented and a reactor burner through which the starting materials in the reaction chamber of the ATR reactor can be introduced, the synthesis gas as product gas from the ATR reactor at a temperature of more than 1100 ° C is deductible.
• ATR reactor refractory lined, pressure resistant reactor
• ATR reactor in which a hydrocarbon containing feed (fuel) is co-charged with carbon dioxide (CO2) and / or Steam and Oxidationsmittei by catalytically assisted partial oxidation (autothermal reforming or ATR) can be implemented and a reactor burner through which the starting materials in the reaction chamber of the ATR reactor can be introduced, the synthesis gas as product gas from the
• a device for removing oil mist and / or odors by oxidation to a solid catalyst which is characterized in that the solid noble metal catalyst on a metallic conductive wire, belt mesh or tubular support in adhering thinly or firmly bonding by burn-in with the metallic carrier, or by first coating the metallic carrier with a substantially porous mass, anchoring it to the metallic carrier by baking and loading the porous mass by impregnation with noble metal catalysts and the metallic carrier to heat by DC or AC current to the required oxidation temperature, wherein the change of the electrical resistance is used for temperature control and the effluent gas from the converter is used to preheat the incoming gas.
• DE 10 2010 033316 A1 describes an exhaust gas treatment system comprising: M electrically heated substrates coated with a catalyst material and arranged in series to receive exhaust gas from a machine, M being an integer greater than one; and a heater control module that applies power to N of the M substrates to heat the N substrates for a predetermined period, where N is an integer less than M, wherein during the predetermined period the engine is off and the M electrically heated substrates are not Absorb exhaust.
• DE 103 171 7 relates to an electrically heated reactor for carrying out gas reactions at high temperature, comprising a reactor block surrounded by an enclosure of one or more monolithic modules of a material suitable for resistance heating or inductive heating, designed as a reaction space channels one on the opposite side of the reactor block, each one device for supplying and discharging a gaseous medium to / from the channels and at least two connected to a power source and the reactor block electrodes (8, 8 ') / to pass a current through the reactor block or a device / to induce a flow in the reactor block, wherein the enclosure of the reactor block comprises a gas-tight sealing double jacket and at least one device for supplying an inert gas in the double jacket.
• the object of the present invention is therefore to provide a reactor suitable for this purpose.
• a flow reactor for the reaction of a fluid comprising reactants comprising in the flow direction of the fluid a plurality of heating levels, which are electrically heated by heating elements and wherein the heating levels are flowed through by the fluid, wherein disposed on at least one heating element, a catalyst is and is heated there.
• the flow reactor is characterized in that at least once an intermediate level between two heating levels is arranged, wherein the intermediate level is also traversed by the fluid.
• the intermediate level or its contents can also be catalytically coated. This not only serves as a bearing surface for the metallic conductor, but also generates a pressure loss depending on the porosity and thickness, which results in better flow distribution, especially in the reactor inlet.
• the combination of heat conductor and intermediate level (or support surface) can then be on a metallic support structure, which ensures the mechanical stability. It is preferred that the intermediate plane is an electrical insulation, in particular in the presence of a metallic support structure.
• a dwell of a reacting fluid can continue to be achieved, within which there is a more favorable heat distribution.
• the reaction can be influenced in a comparatively simple manner. Furthermore, it is possible to influence the reaction by catalytic coatings in different type or amount in the intermediate level or their content.
• Another object of the present invention is a method for operating a flow reactor, comprising the steps: a) providing the above-mentioned flow reactor according to the invention; b) electrically heating at least one of the heating elements of the above-mentioned flow reactor according to the invention; and c) passing a reactant-comprising fluid through the flow reactor with at least partial reaction of the reactants of the fluid.
• Reactions that can be carried out in the flow reactor according to the invention for example, the dry reforming of methane (DR, C 1 h + CO2 ⁇ - '* 2 CO + 2 H2), the reverse water gas shift reaction (RWGS, C0 2 + 1!: ⁇ ⁇ CO + H 2 0), the partial oxidation of methane
• FIG. I -4 schematically flow reactors according to the invention in an expanded representation
• FIG. 5-10 results of simulation calculations
• FIG. 1 schematically shown flow reactor is flowed through by a reactant fluid from top to bottom, as shown by the arrows in the drawing.
• the fluid may be liquid or gaseous and may be single-phase or multi-phase.
• the fluid is gaseous. It is conceivable that the fluid contains only reactants and reaction products, but also that additionally inert components such as inert gases are present in the fluid.
• the reactor has a plurality of (four in the present case) heating levels 100, 101, 102, 103, which by means of corresponding heating elements 1 10, 1 1 1. 1 12. 1 1 electrically heated.
• the heating levels 100, 101, 102, 103 are flowed through during operation of the reactor of the fluid and the heating elements 1 10, 1 1 1, 1 12, 1 13 are contacted by the fluid.
• At least one heating element 1 10, 1 1 1, 1 12, 1 1 3, a catalyst is arranged and is heated there.
• the catalyst can directly or indirectly with the heating elements 1 10, 1 1 1, 1 12, 1 13 be connected, so that these heating elements represent the catalyst support or a support for the catalyst support.
• the heat supply of the reaction takes place electrically and is not introduced from the outside by means of radiation through the walls of the reactor, but directly into the interior of the reaction space. It is realized a direct electrical heating of the catalyst.
• the heating elements 110, 111, 112, 113 are preferably Bankleiterlegtechniken such as FeCrAl alloys used.
• electrically conductive Si-based materials particularly preferably SiC, and / or carbon-based materials.
• a ceramic intermediate level 200, 201, 202 (which is preferably supported by a ceramic or metallic support frame plane) between two heating levels 100, 101, 102, 103, wherein the intermediate level (s) 200, 201, 202 or the contents 210, 21 1, 212 of an intermediate level 200, 201, 202 are likewise flowed through by the fluid during operation of the reactor. This has the effect of homogenizing the fluid flow.
• additional catalyst is present in one or more intermediate levels 200, 201, 202 or other isolation elements in the reactor. Then an adiabatic reaction can take place.
• the electrical connections are shown in FIG. 1 only shown very schematically. They can be performed in the cold area of the reactor within an insulation to the ends of the reactor or laterally from the heating elements 1 10, III, 1 12, 1 I 3 performed so that the actual electrical connections can be provided in the cold region of the reactor.
• the electrical heating is done with direct current or alternating current.
• inlet temperatures are often reached by 600 ° C, which are often below the desired inlet temperatures that reduce the formation of soot / carbon in reforming reactions.
• the connection of one or more of the described electrically heated elements as a gas heater allows a rapid heating of the educt gases to temperatures higher than usual in the prior art, without an oxygen-containing atmosphere is required.
• the use of the electrically heated elements in the inlet region of the reactor also has a positive effect with regard to the cold start and starting behavior, in particular with regard to rapid heating to the reaction temperature and better controllability.
• heating elements 110, 1 1 1. 112, 113 are arranged, which spiral, meandering. gitt erförmig and / or net-shaped are constructed.
• At least one heating element 110, 111, 112, 113 one of the remaining heating elements 110, I I I. 112, 1 13 different amount and / or to the catalyst is present.
• the heating elements 110, 11, 112, 113 are arranged so that they can each be electrically heated independently of each other.
• the individual heating levels can be individually controlled and regulated.
• a catalyst in the heating levels can also be dispensed with in the reactor inlet area, so that only the heating and no reactivation takes place in the inlet area. This is particularly advantageous in view of starting the reactor.
• a temperature profile adapted to the respective reaction can be achieved.
• this is, for example, a temperature profile which achieves the highest temperatures and thus the highest conversion at the reactor outlet.
• the (for example ceramic) intermediate levels 200, 201, 202 or their contents 210, 211, 212 comprise a material resistant to the reaction conditions, for example a ceramic foam. They serve for mechanical support of the heating levels 100, 101, 102, 103 and for mixing and distribution of the gas stream. At the same time is such an electrical
• the material of the content 210, 211, 212 of an intermediate level 200, 201, 202 comprises oxides, carbides, nitrides, phosphides and / or borides of aluminum, silicon and / or zirconium.
• An example of this is SiC, Further preferred is cordierite.
• the intermediate level 200, 201, 202 may include, for example, a loose bed of solids. These solids themselves may be porous or solid, so that the fluid flows through gaps between the solids. It is preferred that the material of the solid bodies comprises oxides, carbides, nitrides, phosphides and / or borides of aluminum, silicon and / or zirconium. An example of this is SiC. Further preferred is cordierite.
• the intermediate level 200, 201, 202 comprises a one-piece porous solid.
• the fluid flows through the intermediate plane via the pores of the solid. This is shown in FIG. 1 shown.
• Preference is given to honeycomb monoliths, as used for example in the exhaust gas purification of internal combustion engines.
• the average length of a heating level 100, 101, 102, 103 is viewed in the direction of flow of the fluid and the average length of an intermediate level 200, 201, 202 in the direction of flow of the fluid is in a ratio of> 0.01: 1 to ⁇ 100: 1 to each other. Even more advantageous are ratios of> 0.1: 1 to ⁇ 10: 1 or 0.5: 1 to ⁇ 5: 1.
• Suitable catalysts may for example be selected from the group consisting of:
• A, A 'and A are independently selected from the group: Mg, Ca, Sr, Ba, Li, Na, K,
• B, B 'and B are independently selected from the group: Cr, Mn, Fe, Bi, Cd, Co, Cu, Ni, Sn, Al, Ga, Sc, Ti, V, Nb, Ta, Mo, Pb H, Zr, Tb, W. (id.Yb, Mg, Li, Na, K. Ce, and / or Zu, and
• B is selected from the group: Cr, Mn, Fe, Bi, Cd, Co, Cu, Ni, Sn, Al, Ga, Sc, Ti, V, Nb, Ta, Mo, Pb. ⁇ ⁇ . Zr, Tb. W. Gd. Yb, Mg, Cd. To. Re. Ru. Rh. Pd. Os, Ir and / or Pt;
• B ' is selected from the group: Re, Ru, Rh, Pd, Os, Ir and / or Pt;
• Ml and M2 are independently selected from the group: Re, Ru, Rh, Ir, Os, Pd and / or Pt;
• M3 is selected from the group: Sc, Y, La, Ce, Pr. Nd, Sm, Eu. Gd. Tb, Dy. Ho, he. Tin. Yb and / or Lu;
• M is selected from the group: Ti, Zr. Hf, V, Nb. Ta, Cr, Mo, W. Mn. Re. Fe, Ru. Os, Co, Rh. Ir, Ni, Pd. Pt. Zn. Cu, Ag and / or Au;
• L is selected from the group: Na, K, Rh. Cs, Mg, Ca, Sr, Ba, Sc, Y, Sn, Pb, Mn, In. Tl, La, Ce, Pr, Nd, Sm, Eu, (id Tb, Dy Ho, Er, Tm Yb, and / or Lu;
• (Vi) oxide catalyst comprising Ni and Ru.
• Ml and M2 are independently selected from the group: Cr, Mn, Fe, Co, Ni, Re, Ru, Rh. Ir. Os, Pd, Pt, Zn, Cu, La. Ce, Pr. Nd. Sm, Eu, Gd, Tb. Dy. 1 lo. He. Tm, Yb. and / or Lu;
• a and B are independently selected from the group: Be. Mg, Ca, Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Y. Zr, Nb, Mo, I I f. Ta, W. La. Ce, Pr. Nd, Sm, Eu. Gd. Tb, Dy. Ho, he. Tm. Yb. and / or Lu; and / or reaction products of (I), (II), (III), (IV), (V), (VI) and / or (VII) in the presence of carbon dioxide, hydrogen, carbon monoxide and / or water at a temperature of > 700 ° C.
• reaction products includes the catalyst phases present under reaction conditions.
• the reactor according to the invention may be modular.
• a module may include, for example, a heating level, an intermediate level, the electrical contact and the corresponding further insulation materials and thermal insulation materials.
• electrical heating of at least one of the heating elements 110, 111, 112, 113 takes place in the reactor provided. This can, but does not have to, take place before flow of a reactant comprising fluid through the flow reactor with at least partial reaction of the reactants of the fluid ,
• the individual heating elements 110, 111, 112, 113 are operated with a respective different heating power.
• the reaction temperature in the reactor is at least in places> 700 ° C to ⁇ 1300 ° C. More preferred ranges are> 800 ° C to ⁇ 1200
• the average (average) contact time of the fluid to a heating element 110, 11, 112, 13 can be, for example,> 0.01 seconds to ⁇ 1 second and / or the average contact time of the fluid to an intermediate level 110, 111, 112, 113 may be, for example,> 0.001 seconds to ⁇ 5 seconds.
• Preferred contact times are> 0.005 to ⁇ 1 second, more preferably> 0.01 to ⁇ 0.9 seconds.
• the Reakti n can be carried out at a pressure of> 1 bar to ⁇ 200 bar.
• the pressure is> 2 bar to ⁇ 50 bar, more preferably> 6 bar to ⁇ 30 bar.
• the reactants in the fluid are selected from the group comprising alkanes, alkenes, alkynes, alkanols, alkenols, alkynols, carbon monoxide, carbon dioxide, water, ammonia, hydrogen and / or oxygen.
• the alkanes methane is particularly suitable, among the alkanols methanol and / or ethanol are preferred.
• FIG. FIG. 2 shows another reactor according to the invention, which can preferably be used for the RWGS reaction.
• the first heating level 100 with heating element 110 is not yet provided with a catalyst and serves as a gas heater.
• the subsequent intermediate level 200 contains a monolithic shaped catalyst body 210 which is coated catalytically table. Alternatively, it may also be a catalyst bed. This is followed by a heating level 101 with heating element 1 1 1, an intermediate level 201 with a porous support layer 211 (optionally catalytically coated) and a further heating level 102 with heating element 1 12 at.
• this heating level 102 Downstream of this heating level 102 is again an intermediate level 202 with a monolithic shaped catalyst body or catalyst bed 212, a heating level 103 with a heating element 13, and in the form of a catalyst body or catalyst bed 213. At least one of the heating elements 1 1 1, 1 12 and 1 13 also includes a catalyst. Again, the individual catalyst-carrying elements of the reactor can differ in the type and amount of the catalyst and the heating elements can be controlled and regulated individually or in groups.
• the characteristics of the RWGS reaction lie in a comparatively moderate heat requirement and in the fact that it is an equilibrium reaction.
• methanation may occur especially at elevated pressure and at temperatures below 800 ° C. Therefore, a high gas inlet temperature is preferably selected in order to thermodynamically suppress the side reactions and in particular the methanation.
• a high outlet tem- perature ensures high sales.
• the catalytic reaction takes place here for the most part adiabatically to the monolithic Katalysatorformkörp ern and to a lesser extent provided with the catalyst
• FIG. 3 shows a further reactor according to the invention, which can preferably be used for dry reforming.
• the first heating level 100 with heating element 110 can not yet be provided with a catalyst and then serves as a pure gas heater. In order to avoid unwanted side reactions, however, a (weakly) catalytically active layer may already be applied to the heating element 110.
• the subsequent intermediate level 200 contains a porous support layer 210, which may optionally be catalytically coated. This is followed by a heating level 101 with catalytically coated 1 lei / element 11 1, an intermediate level 201 with a porous support layer 21 1 (optionally catalytically coated) and a further heating level 102 with catalytically coated heating element 1 12 at.
• this heating level 102 Downstream of this heating level 102 is again an intermediate level 202 with a porous support layer 212 (optionally catalytically coated), a heating level 103 with catalytically coated heating element 1 13 and an intermediate level 203 with a porous support layer 213 (optionally catalytically coated).
• the catalyst supporting elements of the reactor may differ in the type and amount of catalyst and the heating elements may be controlled and controlled individually or in groups.
• the main feature of the (O-reforming is a high heat requirement, which is locally limited, especially in the first third of the reactor.) It is an equilibrium reaction with a soot formation as side reaction, therefore it is preferable to use high gas inlet temperatures
• the reaction takes place essentially on the catalytically coated heating elements, and FIG. 4 shows a further reactor according to the invention which can preferably be used for methane steam reforming With heating element 110, this can not yet be provided with a catalyst and then serves as a pure gas heater However, a (weakly) catalytically active layer can already be applied to heating element 110.
• the subsequent intermediate plane 200 contains a porous supporting layer 210, which may optionally be catalytically coated.
• a heating level 101 with a catalytically coated heating element 11 1 is followed by a heating level 101 with a catalytically coated heating element 11 1, an intermediate level 201 with a porous support layer 211 (optionally catalytically coated) and a further heating level 102 with a catalytically coated heating element 112. Downstream of this heating level 102 is again an intermediate level 202 with a porous support layer 212 (optionally catalytically coated), a heating level 103 with a catalytically coated heating element 13 and an intermediate level 203 with a monolithic shaped catalyst body or catalyst 213.
• the individual catalyst-carrying elements of the reactor can differ in the type and amount of the catalyst and the heating elements can be controlled and regulated individually or in groups.
• the main feature of methane steam reforming is a high heat requirement. It is an equilibrium reaction with a soot formation as a side reaction. Therefore, it is preferable to select high gas inlet temperatures to thermodynamically suppress the side reaction. 1 l he exit temperatures ensure a high turnover.
• the reaction is carried out essentially in the first reactor segment on the catalytically coated heating elements.
• the first segment is characterized by the fact that the reactant concentration and the heat requirement of the reaction are very high.
• the further reaction of the starting material e can take place on catalytically coated moldings.
• the heating elements then act as an intermediate heating according to Bedar.
• the model includes a solid phase and a gas phase
• FIG. Figure 5 shows the conversion (XCH 4 , XCCM) over the normalized reactor length.
• the "peaks" in the sales profile result from the consideration of a bypass flow, which is mixed in behind each lei / element.
• the turnover rises steadily and reaches 90% after the first half of the reactor, then the turnover flattens off and approaches on Output to the corresponding equilibrium value.
• FIG. 6 shows the temperature profile of the gas and solid phase.
• the maximum power of the heating elements is given up in the inlet area (corresponds to 1 00% in the power profile). Much of the electrical energy is consumed by the heat of reaction.
• the power input is selected such that the solid-state temperature (including the catalysis) is in the range around 1 100 ° C.
• the reaction gas enters the reactor at 800 ° C, through heat exchange with the solid, the temperature of the gas phase increases the reactor length. The reaction takes place on the solid, reactions in the gas phase are not taken into account.
• FIG. 7 shows the relative heating power per heating element.
• the profile of heat input per element (in percent based on the maximum power of a single element) shows that the highest power is introduced in the first third of the reactor. At the rear of the reactor, sales level off and only a small input of power is required. This is where the concepts derive. which provide monolithic shaped bodies or catalyst charge in the area.
• Mode II In contrast to the mode of operation I, the advantage of the reactor concept is illustrated here, in order to be able to impose a desired temperature profile on the reaction.
• the gas temperature in the inlet is 800 ° C and the power input per heating element is chosen so that a continuous
• FIG. 8 shows the conversion (XCH4, Xcce) over the normalized reactor length
• FIG. 9 shows the temperature profile of the gas and solid phase
• FIG. 1 0 shows the relative heating power per heating element.

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Citations (8)

• 2013
  • 2013-03-12 WO PCT/EP2013/054947 patent/WO2013135660A1/fr not_active Ceased

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