WO2009019520A2 - Catalytic pyrolysis device and procedure for the production of the structure of the housing body of the catalytic pyrolysis device - Google Patents

Catalytic pyrolysis device and procedure for the production of the structure of the housing body of the catalytic pyrolysis device Download PDF

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Publication number
WO2009019520A2
WO2009019520A2 PCT/HU2008/000092 HU2008000092W WO2009019520A2 WO 2009019520 A2 WO2009019520 A2 WO 2009019520A2 HU 2008000092 W HU2008000092 W HU 2008000092W WO 2009019520 A2 WO2009019520 A2 WO 2009019520A2
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Prior art keywords
mass
housing body
active material
shell
core
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Application number
PCT/HU2008/000092
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French (fr)
Other versions
WO2009019520A3 (en
Inventor
Árpád HARANGI
Edit SIKLÓSI
Erzsébet Stregova
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3R Carbon Capture And Storage Pty Ltd.
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Priority to AU2008285305A priority Critical patent/AU2008285305B2/en
Publication of WO2009019520A2 publication Critical patent/WO2009019520A2/en
Publication of WO2009019520A3 publication Critical patent/WO2009019520A3/en

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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
    • F23G7/00—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals
    • F23G7/06—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases
    • F23G7/07—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases in which combustion takes place in the presence of catalytic material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86—Catalytic processes
    • B01D53/864—Removing carbon monoxide or hydrocarbons
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/16—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on silicates other than clay
    • C04B35/18—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on silicates other than clay rich in aluminium oxide
    • C04B35/195—Alkaline earth aluminosilicates, e.g. cordierite or anorthite
    • C—CHEMISTRY; METALLURGY
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    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
    • C04B35/16—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on silicates other than clay
    • C04B35/20—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on silicates other than clay rich in magnesium oxide, e.g. forsterite
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/622—Forming processes; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
    • C04B35/626—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B
    • C04B35/63—Preparing or treating the powders individually or as batches ; preparing or treating macroscopic reinforcing agents for ceramic products, e.g. fibres; mechanical aspects section B using additives specially adapted for forming the products, e.g.. binder binders
    • C04B35/632—Organic additives
    • C04B35/636—Polysaccharides or derivatives thereof
    • C04B35/6365—Cellulose or derivatives thereof
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN  A CARRIER GAS OR AIR 
    • F23C13/00—Apparatus in which combustion takes place in the presence of catalytic material
    • F23C13/08—Apparatus in which combustion takes place in the presence of catalytic material characterised by the catalytic material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/204—Alkaline earth metals
    • B01D2255/2047—Magnesium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/207—Transition metals
    • B01D2255/20753—Nickel
    • 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
    • B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/78—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with alkali- or alkaline earth 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/0215—Coating
    • B01J37/023—Coating using molten compounds
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/024—Multiple impregnation or coating
    • B01J37/0242—Coating followed by impregnation
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/024—Multiple impregnation or coating
    • B01J37/0244—Coatings comprising several layers
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3205—Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
    • C04B2235/3215—Barium oxides or oxide-forming salts thereof
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3217—Aluminum oxide or oxide forming salts thereof, e.g. bauxite, alpha-alumina
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
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    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/3231—Refractory metal oxides, their mixed metal oxides, or oxide-forming salts thereof
    • C04B2235/3232—Titanium oxides or titanates, e.g. rutile or anatase
    • C—CHEMISTRY; METALLURGY
    • C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
    • C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
    • C04B2235/30—Constituents and secondary phases not being of a fibrous nature
    • C04B2235/34—Non-metal oxides, non-metal mixed oxides, or salts thereof that form the non-metal oxides upon heating, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
    • C04B2235/349—Clays, e.g. bentonites, smectites such as montmorillonite, vermiculites or kaolines, e.g. illite, talc or sepiolite
    • C—CHEMISTRY; METALLURGY
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    • C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
    • C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
    • C04B2235/94—Products characterised by their shape

Definitions

  • the subject of the invention relates to a catalytic pyrolysis device primarily for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, which contains a housing body enclosing a reaction space and an active material coating covering at least part of the inner side of the housing body, where the housing body is a ceramic material with a solid core and a porous shell that has depressions suitable to receive the particles of the active material coating at least on the boundary surface of the core facing the reaction space, the active material coating has a nickel base containing magnesium.
  • the subject of the invention also relates, furthermore, to the production of the housing body structure of a catalytic pyrolysis device primarily suitable for to the neutralisation of dangerous combustion products and waste materials, the destruction of flue gases and the utilisation of complex carbon chains, during which we form a core material, the formed core material is subject to heat treatment, following this it is coated with a shell former, then is again subjected to heat treatment, following this the shell is given an active material coating, and finally is subjected to a further heat treatment.
  • the invention is a uniquely formed hydrogenating, pyrolytic, reductive catalytic pyrolysis device with extended primary and secondary combustion and post-combustion processes that has a small active material content, but in spite of this small active material content has a great reactive ability and operates efficiently, and the procedure for its realisation, the foundation of which became known under the name of "NoCo", but is essentially formed by the combustion equipment that can be known from the patent specifications registration numbers HU 206.148 and HU 225.373, and with publication number WO 99/54660.
  • the device suitable for the combustion of the materials and waste that is to be neutralised has a housing body that encloses a reaction space made up of determined geometrically shaped e.g. suitably cylindrical, sheath parts or ring shaped elements, which are made from a porous, usually ceramic material and which are saturated with the required active material.
  • the selectivity of the catalytic pyrolysis device made in this way and its desired activity may be influenced with the correct selection of the material composition of the housing body, and, furthermore, with the varying of the accelerator(s) and promoter(s) added to the components of the active material coating it, so setting the appropriate optimum effect.
  • the activity of a catalytic pyrolysis device may be increased in a heterogeneous process with the application of active material of the appropriate quality applied to a carrier also of the appropriate quality, with the establishing of a large surface of the carrier, with the increasing of the surface concentration of the active material, with the appropriate selection of the amounts of the active materials, with the use of promoters and accelerators, furthermore, with the application of highly and greatly heat resistant metal oxides, characteristically titanium alloy materials in a layered, sandwich or single layer coating.
  • one of the conditions is available for the production of catalytic pyrolysis devices representing a high specific value and large intellectual work ratio, but the other condition - the availability of the active material is a suitable quantity and at a favourable price - is missing in order to be able to manufacture such devices at an acceptable price.
  • the most suitable core for the aforementioned surface layer is a protoenstatite ceramic stabilised with a sintered glassy phase, where even the material quality of the glassy phase is important because on coming into contact with the surface porous layer, it has an effect on the coating layer through the transitional layer, and so has an effect on the resulting changes to the electron structure.
  • a coating layer containing metal salt silicates with added alpha-corundum with the new internal and external carrier material that is complex unity of the housing body structure and its material, the active material and the modification components added to it set up the final parameters of the device.
  • the housing body encompassing the reaction space of the device is made with a body shape different to the usual, from a ceramic made up of a special material composition, and if the ceramic housing body is encompassed with a highly heat-resistant metal material ceramic alloy with monolithic or metal characteristics and so a novel sandwich layer structure is created, then the chemical stability of the internal operation of the reactor space and the stability of the external infra-effect can both be realised.
  • the active material coating the surface layer of the housing body is coupled with suitably selected additives that have efficiency-increasing and accelerating effects, then we can push the speed and selectivity of the expected reactions into the desired direction even if we use a small amount of active material coating, and so the task may be solved.
  • the catalytic pyrolysis device primarily for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, - which contains a housing body enclosing a reaction space and an active material coating covering at least part of the inner side of the housing body, where the housing body is a ceramic material with a solid core and a porous shell that has depressions suitable to receive the particles of the active material coating at least on the boundary surface of the core facing the reaction space, the active material coating has a nickel base containing magnesium, - is set up in such a way that the core of the housing body is from a protoenstatite ceramic stabilised with a sintered glassy phase, and the porous shell at least partially covering the core is from 0.6-1.1 mm thick magnesium silicate with added alpha-corundum, and the active material coating located on the porous external surface of the shell is Ni-Mg oxide produced using heat treatment from a Ni-Mg double salt and, in a given
  • a further feature of the device according to the invention may be that the housing body has a cylindrical sheath section and dome section, as well as inlet and outlet opening, and is also supplemented with a barrier element.
  • the longitudinal cross-sectional shape of the boundary surface between the solid core and the porous shell is a sine curve wave, where the ratio between the middle diameter of the individual waves and their height falls between 0.3-1.
  • the external middle diameter of the boundary surface between the solid core and the porous shell is between 10-1000 mm.
  • the active material amount of the active material coating established from a Ni-Mg double salt contains 0.64-0.76 mol% nickel, 0.23-0.28 mol% magnesium and, in a given case, Ni-Si, and, in a given case the active material coating contains, as an efficiency-increasing and accelerating component, 0.48-0.65 mass% titanium dioxide, 0.16-0.38 mass% gallium dioxide, and 0.05-0.25 mass% zinc dioxide, related to the mass of the active material calculated in the form of nitrate hexahydrate salt.
  • the procedure according to the invention for the production of the housing body structure of a catalytic pyrolysis device primarily suitable for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains - during which core material is formed, the formed core is subjected to heat treatment, following this it is coated with a shell former, then is subjected to heat treatment again, following this the shell receives an active material coating, and finally receives further heat treatment — which is based on the principle that for the raw material for the production of the solid core we use 50-65 mass% finely ground talcum powder, 15-35 mass% talcum powder fired at 120O +50 0 C and/or talcum powder, 4-7 mass% magnesium carbonate and 5-9 mass% barium carbonate, and, in a given case, 0.1-0.2 mass% rutile titanium dioxide, then the raw material is shaped by pressing and is fired at 750 ⁇ 10 0 C, then as a porous shell by immersion and/or spray
  • a further feature of the procedure according to the invention may be that a 96-°C melt of nitrate-hexahydrate is used as the Ni-Mg double salt.
  • the most important advantage of the solution according to the invention is that due to the novel formation and composition of the housing body with a relatively small amount, in other words instead of an active material amount that fills the porous volumes of the total mass of the housing body, with just a surface active material amount of a determined thickness, this is with just a fraction of the previous amount of active material a very highly active, very stable reaction can be realise with a good degree of efficiency, while at the same time the housing body has a high degree of heat resistance and heat shock resistance, and so the lifetime of the housing body increased significantly.
  • the active material coating and the given reductive target process characteristically the hydrocarbon middle distillates and the gases input in their environment, that is especially water vapour and carbon dioxide, cyclic disintegration can be performed.
  • the optimal transformation of the CH 4 , H 2 and the CO 2 chain and the re-production of the given elements can be realised, with the help of the optimally environmentally safe extremely effective catalytic and pyrolytic effect.
  • Another advantage that may be listed is that due to the unique production procedure of the housing body the amount of active material coating require to achieve the desired boundary may be less, which also reduces the amount of costly metal alloy components and so the cost price of the device may also be much more favourable.
  • Figure 1 is a sketch drawing of a version of the device with a housing body according to the invention.
  • FIG. 1 contains a sketch drawing of the device 1 according to the invention. It may be observed that the housing body 20 encompasses the reaction space 2 that serves to eliminate the gas-phase combustion products created during combustion.
  • the housing body 20 may be formed from various geometric forms. In this case the housing body 20 is formed by a cylindrical sheath section 24 and a dome section 25, but a longer housing body 20 consisting of several cylindrical sheath sections 24 may also be imagined. A part of the housing body 20 may also be formed by a geometric form different to the cylindrical sheath section 24 and the dome section 25, e.g. conical sheath section.
  • the reaction space 2 also contains the barrier element 3 as well, which has significance from the aspect of pre-combustion and post- combustion.
  • the structure and operation of the device 1 is essentially the same as that described in detail in patent specifications registration numbers HU 206.148 and HU 225.373, therefore we shall not present this separately here as if belongs to the state of the art.
  • the housing body 20 consists of a solid core 21, of a shell 22 covering the boundary surface 21a of the solid core and the active material coating 23 on the external surface 22a of the shell 22.
  • the solid core 21 contains 75-85 mass% finely ground and partially fired at 120O +50 0 C, 6-11 mass% white burning plastic fine clay, and as a melt 4-7 mass% magnesium carbonate and 5-9 mass% barium carbonate, as well as 0.1-2.0 mass% rutile titanium dioxide.
  • the boundary surface 21a of the solid core 21 formed by pressing is formed as a sine wave corrugated pipe piece, and depending on the type of reactor the ratio of the middle diameter and the height of the sine wave is between the values of 0.3 : 1.0 and 1:1.
  • the ration of the external/internal diameters is also between the practical values. These ratios are somewhat amended by the porous surface shell 22, but this change is not significant.
  • the size of the external middle diameter also depending on the type of reactor, may be selected between wide values of 10-1000 mm.
  • the shell 22 located on the boundary surface 21a of the solid core 21 has a porous structure, the practical composition of which shell 22 is 6-14 mass% fine grain calcinated alpha corundum, 4-9 mass% white burning plastic fine clay, 78-89 mass% raw and fired talcum, which contains as a mill additive 3-12 mass% paper industry grade pulped cellulose fibre, 0.1-2.0 mass% ammonium lignosulphate, 0.2-0.8 mass% tri-methylcellulose (molar mass: 1000-5000).
  • the thickness of the shell 22 when the housing body is in a finished condition is 0.5-1.1 mm.
  • the active material coating 23 located on the external surface 22a of the porous shell 22 of the housing body consists of 0.64-0.76 mol% nickel nitrate-hexahydrate and 0.23- 0.28 mol% magnesium nitrate-hexahydrate, which calculated for its- original mass includes an efficiency-increasing and accelerator additive of 0.48-0.65 mass% TiO 2 , 0.16-0.38 mass% GaO 2 and 0.05-0.25 mass% ZnO 2 .
  • the active material coating 23 In the interest of activating the fired housing body 20 in order to achieve the desired surface saturation and peaking we dipped it into a bath once or several times, and in this way we created the active material coating 23.
  • the bath suitable for establishing the active material coating 23 we used 0.64-0.76 mol% nickel nitrate hexahydrate and 0.23- 0.28 mol% magnesium nitrate hexahydrate melted at 96 0 C, in which melt we suspended 0.48-0.65 mass% TiO 2 , 0.16-0.38 mass% GaO 2 and 0.05-0.25 mass% ZnO 2 , calculated according to the original mass of the melt, in the interest of achieving a fine grain structure we precipitated these out of organic compounds together and/or separately in a known way.
  • the device 1 with the unique housing body 20 according to the invention may be used to good effect in all applications where dangerous materials and/or waste needs to be eliminated in an environmentally friendly way.

Abstract

The subject of the invention relates to a catalytic pyrolysis device primarily for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, which contains a housing body enclosing a reaction space and an active material coating covering at least part of the inner side of the housing body, where the housing body is a ceramic material with a solid core and a porous shell that has depressions suitable to receive the particles of the active material coating at least on the boundary surface of the core facing the reaction space, the active material coating has a nickel base containing magnesium. The characteristic feature of the device is that the core (21) of the housing body (20) is from a protoenstatite ceramic stabilised with a sintered glassy phase, and the porous shell (22) at least partially covering the core (21) is from 0.6-1.1 mm thick magnesium silicate with added alpha-corundum, and the active material coating (23) located on the porous external surface (22a) of the shell (22) is Ni-Mg oxide produced using heat treatment from a Ni-Mg double salt and, in a given case, contains Ni-Si components. The subject of the invention also relates to the production of the housing body structure of a catalytic pyrolysis device primarily suitable for to the neutralisation of dangerous combustion products and waste materials, the destruction of flue gases and the utilisation of complex carbon chains, during which we form a core material, the formed core material is subject to heat treatment, following this it is coated with a shell former, then is again subjected to heat treatment, following this the shell is given an active material coating, and finally is subjected to a further heat treatment. The characteristic feature of the invention is that for the raw material for the production of the solid core (21) we use 50-65 mass% finely ground talcum powder, 15- 35 mass% talcum powder fired at 1200+50 °C and/or talcum powder, 4-7 mass% magnesium carbonate and 5-9 mass% barium carbonate, and, in a given case, 0.1-0.2 mass% rutile titanium dioxide, then the raw material is shaped by pressing and is fired at 750±10 °C, then as a porous shell (22) by immersion and/or spraying we apply a fine ground material slurry to the boundary surface (21a) of the solid core (21) produced in this way consisting of 6-14 mass% fine grain calcinated alpha corundum, 4-9 mass% white burning plastic fine clay, 55-68 mass% raw talcum and 22-28 mass% talcum powder fired at 1200+50 and 3-12 mass% paper industry grade pulped cellulose fibre, 0.1-0.2 mass% ammonium lignosulphate and 0.2-0.8 mass% tri-methylcellulose with a molar mass of between 1000-5000, we apply a material mixture with a density of 1250-1300 g/l and we continue thickening the porous shell (22) until the theoretical post-firing thickness of the porous shell (22) reaches 0.6-1.1 mm, following creating the porous shell (22) the housing body (20) is dried and fired at 1200±10 °C, then the housing body (20) with its solid core (21) and porous shell (22) is dipped once or several times in a Ni-Mg double salt melt and then any surplus is removed from the housing body (20) an in this way an active material coating is applied to the housing body (20), then finally the housing body (20) with the applied active material coating (23) is heat- treated at 600±10 °C.

Description

Catalytic pyrolysis device and procedure for the production of the structure of the housing body of the catalytic pyrolysis device
The subject of the invention relates to a catalytic pyrolysis device primarily for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, which contains a housing body enclosing a reaction space and an active material coating covering at least part of the inner side of the housing body, where the housing body is a ceramic material with a solid core and a porous shell that has depressions suitable to receive the particles of the active material coating at least on the boundary surface of the core facing the reaction space, the active material coating has a nickel base containing magnesium.
The subject of the invention also relates, furthermore, to the production of the housing body structure of a catalytic pyrolysis device primarily suitable for to the neutralisation of dangerous combustion products and waste materials, the destruction of flue gases and the utilisation of complex carbon chains, during which we form a core material, the formed core material is subject to heat treatment, following this it is coated with a shell former, then is again subjected to heat treatment, following this the shell is given an active material coating, and finally is subjected to a further heat treatment.
From closer up, the invention is a uniquely formed hydrogenating, pyrolytic, reductive catalytic pyrolysis device with extended primary and secondary combustion and post-combustion processes that has a small active material content, but in spite of this small active material content has a great reactive ability and operates efficiently, and the procedure for its realisation, the foundation of which became known under the name of "NoCo", but is essentially formed by the combustion equipment that can be known from the patent specifications registration numbers HU 206.148 and HU 225.373, and with publication number WO 99/54660.
The essence of the known equipment is that the device suitable for the combustion of the materials and waste that is to be neutralised has a housing body that encloses a reaction space made up of determined geometrically shaped e.g. suitably cylindrical, sheath parts or ring shaped elements, which are made from a porous, usually ceramic material and which are saturated with the required active material. The selectivity of the catalytic pyrolysis device made in this way and its desired activity may be influenced with the correct selection of the material composition of the housing body, and, furthermore, with the varying of the accelerator(s) and promoter(s) added to the components of the active material coating it, so setting the appropriate optimum effect.
On the basis of the specialist literature and our practical experience, the activity of a catalytic pyrolysis device may be increased in a heterogeneous process with the application of active material of the appropriate quality applied to a carrier also of the appropriate quality, with the establishing of a large surface of the carrier, with the increasing of the surface concentration of the active material, with the appropriate selection of the amounts of the active materials, with the use of promoters and accelerators, furthermore, with the application of highly and greatly heat resistant metal oxides, characteristically titanium alloy materials in a layered, sandwich or single layer coating.
With respect to Hungary in the past a procedure was used containing Ni and an Ni- Mg double salt applied by immersion to a mullite-based - aluminium-silicate, 3 Al2O3.2 SiO2 ~ 2 Al2O3-SiO2 mixed crystal series -, heavily porous carrier activated with heat treatment for the air-cyclic breaking up of mixed hydrocarbons with a maximum of 6 carbon atoms. The basic principle did not change as time progressed, but was refined, the range of hydrocarbons that could be processed was increased to higher homologues. In general similar catalytic pyrolysis devices currently known contain 12-14% by mass of Ni-based active material.
The disadvantage of the known solutions, however, is that active material coating to suitable material quality requires a very porous carrier in order to achieve high surface active material concentration. A carrier with a high degree of porosity though means that a great deal of active material is used. Due to the high price of active materials, however, the price of complete catalytic pyrolysis devices also increases significantly. Hungary, however, is a country poor in noble metals or semi-noble active material metals that may be used in catalysers, but it does have very favourable features for the production of certain ceramic material types, primarily corundum-based ceramic material types or those containing corundum. Therefore, one of the conditions is available for the production of catalytic pyrolysis devices representing a high specific value and large intellectual work ratio, but the other condition - the availability of the active material is a suitable quantity and at a favourable price - is missing in order to be able to manufacture such devices at an acceptable price.
With the solution and procedure according to the invention our objective was to overcome the deficiencies of catalytic pyrolysis devices primarily suitable for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, and the creation of a high- activity version in which increased reaction activity and so the total elimination or neutralisation of flue gasses containing undesirable components can be realised with minimal active material content.
The basis of the idea behind the invention was formed by that on the basis of our investigations we came to the conclusion that the most suitable core for the aforementioned surface layer is a protoenstatite ceramic stabilised with a sintered glassy phase, where even the material quality of the glassy phase is important because on coming into contact with the surface porous layer, it has an effect on the coating layer through the transitional layer, and so has an effect on the resulting changes to the electron structure. While the most favourable interaction is exerted by a coating layer containing metal salt silicates with added alpha-corundum with the new internal and external carrier material. That is complex unity of the housing body structure and its material, the active material and the modification components added to it set up the final parameters of the device.
Starting from this point the recognition that led to the solution according to the invention was that if the housing body encompassing the reaction space of the device is made with a body shape different to the usual, from a ceramic made up of a special material composition, and if the ceramic housing body is encompassed with a highly heat-resistant metal material ceramic alloy with monolithic or metal characteristics and so a novel sandwich layer structure is created, then the chemical stability of the internal operation of the reactor space and the stability of the external infra-effect can both be realised. Furthermore, if the active material coating the surface layer of the housing body is coupled with suitably selected additives that have efficiency-increasing and accelerating effects, then we can push the speed and selectivity of the expected reactions into the desired direction even if we use a small amount of active material coating, and so the task may be solved.
In accordance with the set objective the catalytic pyrolysis device according to the invention primarily for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, - which contains a housing body enclosing a reaction space and an active material coating covering at least part of the inner side of the housing body, where the housing body is a ceramic material with a solid core and a porous shell that has depressions suitable to receive the particles of the active material coating at least on the boundary surface of the core facing the reaction space, the active material coating has a nickel base containing magnesium, - is set up in such a way that the core of the housing body is from a protoenstatite ceramic stabilised with a sintered glassy phase, and the porous shell at least partially covering the core is from 0.6-1.1 mm thick magnesium silicate with added alpha-corundum, and the active material coating located on the porous external surface of the shell is Ni-Mg oxide produced using heat treatment from a Ni-Mg double salt and, in a given case, contains Ni-Si components.
A further feature of the device according to the invention may be that the housing body has a cylindrical sheath section and dome section, as well as inlet and outlet opening, and is also supplemented with a barrier element.
In the case of a possible embodiment of the device the longitudinal cross-sectional shape of the boundary surface between the solid core and the porous shell is a sine curve wave, where the ratio between the middle diameter of the individual waves and their height falls between 0.3-1. The external middle diameter of the boundary surface between the solid core and the porous shell is between 10-1000 mm.
In the case of a further different embodiment of the invention the active material amount of the active material coating established from a Ni-Mg double salt contains 0.64-0.76 mol% nickel, 0.23-0.28 mol% magnesium and, in a given case, Ni-Si, and, in a given case the active material coating contains, as an efficiency-increasing and accelerating component, 0.48-0.65 mass% titanium dioxide, 0.16-0.38 mass% gallium dioxide, and 0.05-0.25 mass% zinc dioxide, related to the mass of the active material calculated in the form of nitrate hexahydrate salt.
In accordance with the set objective the procedure according to the invention for the production of the housing body structure of a catalytic pyrolysis device primarily suitable for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, - during which core material is formed, the formed core is subjected to heat treatment, following this it is coated with a shell former, then is subjected to heat treatment again, following this the shell receives an active material coating, and finally receives further heat treatment — which is based on the principle that for the raw material for the production of the solid core we use 50-65 mass% finely ground talcum powder, 15-35 mass% talcum powder fired at 120O+50 0C and/or talcum powder, 4-7 mass% magnesium carbonate and 5-9 mass% barium carbonate, and, in a given case, 0.1-0.2 mass% rutile titanium dioxide, then the raw material is shaped by pressing and is fired at 750±10 0C, then as a porous shell by immersion and/or spraying we apply a fine ground material slurry to the boundary surface of the solid core produced in this way consisting of 6-14 mass% fine grain calcinated alpha corundum, 4-9 mass% white burning plastic fine clay, 55-68 mass% raw talcum and 22-28 mass% talcum powder fired at 120O+50 and 3- 12 mass% paper industry grade pulped cellulose fibre, 0.1-0.2 mass% ammonium lignosulphate and 0.2-0.8 mass% tri-methylcellulose with a molar mass of between 1000-5000, we apply a material mixture with a density of 1250-1300 g/1 and we continue thickening the porous shell until the theoretical post-firing thickness of the porous shell reaches 0.6-1.1 mm, following creating the porous shell the housing body is dried and fired at 1200±10 0C, then the housing body with its solid core and porous shell is dipped once or several times in a Ni-Mg double salt melt and then any surplus is removed from the housing body an in this way an active material coating is applied to the housing body, then finally the housing body with the applied active material coating is heat-treated at 600±10 oC.
A further feature of the procedure according to the invention may be that a 96-°C melt of nitrate-hexahydrate is used as the Ni-Mg double salt.
In a favourable realisation of the procedure before the housing body with its solid core and porous shell is dipped a finely distributed efficiency-increasing and acceleration additive is mixed into the Ni-Mg double salt.
The most important advantage of the solution according to the invention is that due to the novel formation and composition of the housing body with a relatively small amount, in other words instead of an active material amount that fills the porous volumes of the total mass of the housing body, with just a surface active material amount of a determined thickness, this is with just a fraction of the previous amount of active material a very highly active, very stable reaction can be realise with a good degree of efficiency, while at the same time the housing body has a high degree of heat resistance and heat shock resistance, and so the lifetime of the housing body increased significantly.
It is an advantage that with the device according to the invention due to the unique surface porous layer, the active material coating and the given reductive target process characteristically the hydrocarbon middle distillates and the gases input in their environment, that is especially water vapour and carbon dioxide, cyclic disintegration can be performed. Especially the optimal transformation of the CH4, H2 and the CO2 chain and the re-production of the given elements can be realised, with the help of the optimally environmentally safe extremely effective catalytic and pyrolytic effect.
Another advantage that may be listed is that due to the unique production procedure of the housing body the amount of active material coating require to achieve the desired boundary may be less, which also reduces the amount of costly metal alloy components and so the cost price of the device may also be much more favourable.
A further favourable effect deriving from this is that such devices may be used in greater numbers for the elimination of dangerous materials and waste - because of the favourable pricing - as a consequence of which the emission of environmentally damaging combustion production can be essentially completely terminated.
In the following we present the device according to the invention in more detail in connection with a construction example on the basis of a drawing. In the drawing
Figure 1 is a sketch drawing of a version of the device with a housing body according to the invention.
Figure 1 contains a sketch drawing of the device 1 according to the invention. It may be observed that the housing body 20 encompasses the reaction space 2 that serves to eliminate the gas-phase combustion products created during combustion. The housing body 20 may be formed from various geometric forms. In this case the housing body 20 is formed by a cylindrical sheath section 24 and a dome section 25, but a longer housing body 20 consisting of several cylindrical sheath sections 24 may also be imagined. A part of the housing body 20 may also be formed by a geometric form different to the cylindrical sheath section 24 and the dome section 25, e.g. conical sheath section.
The reaction space 2 also contains the barrier element 3 as well, which has significance from the aspect of pre-combustion and post- combustion. Here it must be remarked that the structure and operation of the device 1 is essentially the same as that described in detail in patent specifications registration numbers HU 206.148 and HU 225.373, therefore we shall not present this separately here as if belongs to the state of the art.
The significant difference to the known solutions lies in the formation of the housing body 20. Here structurally the housing body 20 consists of a solid core 21, of a shell 22 covering the boundary surface 21a of the solid core and the active material coating 23 on the external surface 22a of the shell 22. The solid core 21 contains 75-85 mass% finely ground and partially fired at 120O+50 0C, 6-11 mass% white burning plastic fine clay, and as a melt 4-7 mass% magnesium carbonate and 5-9 mass% barium carbonate, as well as 0.1-2.0 mass% rutile titanium dioxide. The boundary surface 21a of the solid core 21 formed by pressing is formed as a sine wave corrugated pipe piece, and depending on the type of reactor the ratio of the middle diameter and the height of the sine wave is between the values of 0.3 : 1.0 and 1:1.
In the case of the wave form middle diameters the ration of the external/internal diameters is also between the practical values. These ratios are somewhat amended by the porous surface shell 22, but this change is not significant. The size of the external middle diameter, also depending on the type of reactor, may be selected between wide values of 10-1000 mm.
The shell 22 located on the boundary surface 21a of the solid core 21 has a porous structure, the practical composition of which shell 22 is 6-14 mass% fine grain calcinated alpha corundum, 4-9 mass% white burning plastic fine clay, 78-89 mass% raw and fired talcum, which contains as a mill additive 3-12 mass% paper industry grade pulped cellulose fibre, 0.1-2.0 mass% ammonium lignosulphate, 0.2-0.8 mass% tri-methylcellulose (molar mass: 1000-5000). The thickness of the shell 22 when the housing body is in a finished condition is 0.5-1.1 mm.
The active material coating 23 located on the external surface 22a of the porous shell 22 of the housing body consists of 0.64-0.76 mol% nickel nitrate-hexahydrate and 0.23- 0.28 mol% magnesium nitrate-hexahydrate, which calculated for its- original mass includes an efficiency-increasing and accelerator additive of 0.48-0.65 mass% TiO2, 0.16-0.38 mass% GaO2 and 0.05-0.25 mass% ZnO2.
The operation of the device 1 according to figure 1 - as we have already mentioned - is essentially the same as that presented in detail in patent specifications registration numbers HU 206.148 and HU 225.373, we shall not repeat it here. The difference is that as a consequence of the novel ceramic structure forming the housing body 20 and the minimal active material coating 23 located on the shell 22 denitrification and desulfuration reactions can be entirely and quickly executed in a stable manner.
The procedure according to the invention is now presented in connection with an example.
Example 1:
In this procedure version of the structural formation of the housing body 20 for the production of the solid core 21 we mixed together 50-65 mass% finely ground talcum powder, 15-35 mass% talcum powder fired at 120O+50 0C and/or talcum powder, and 4-7 mass% magnesium carbonate and 5-9 mass% barium carbonate, and, in a given case, 0.1-0.2 mass% rutile titanium dioxide, then using a known ceramics industry method the mixture of materials was ground using wet fine grinding, filtered, deironed, and finally dehydrated. Following this from the ground material we formed the shape according to the housing body 20 by extruding and dried it, then it was pre-fϊred at 750±10 0C. During the extruding the pressure tool was formed so that during shaping the boundary surface 21a of the solid core 21 is corrugated in a sine wave, where the middle diameter/height ratio is a value of 0.5.
Independently of the production of the solid core 21, in this case during the firing of the solid core 21 we made the coating mass forming the shell 22 material. During this we produced a fine ground material slurry of 6-14 mass% fine grain calcinated alpha corundum, 4-9 mass% white burning plastic fine clay, 55-68 mass% raw talcum and 22- 28 mass% talcum powder fired at 120O+50, as well as 3-12 mass% paper industry grade pulped cellulose fibre, 0.1-0.2 mass% ammonium lignosulphate and 0.2-0.8 mass% tri- methylcellulose with a molar mass of between 1000-5000, with a density of between 1250-1300 g/1.
Here we must remark that in order to create the thin porous shell 22 to be applied later we had to carry out grinding so that the permitted sieve residue on a DIN 10000 filter is a maximum of 0.2%. After preparing the fine ground material slurry we dipped the pre-fired solid core 21 in the slurry forming the raw material for the shell 22 so that the shell 22 layer thickness formed on the boundary surface 21a of the solid core is in a raw state between 0.65-1.1 mm. After a shell 22 of the desired thickness is formed the housing body 20 was dried and then fired at 1280±100C.
In the interest of activating the fired housing body 20 in order to achieve the desired surface saturation and peaking we dipped it into a bath once or several times, and in this way we created the active material coating 23. For the bath suitable for establishing the active material coating 23 we used 0.64-0.76 mol% nickel nitrate hexahydrate and 0.23- 0.28 mol% magnesium nitrate hexahydrate melted at 96 0C, in which melt we suspended 0.48-0.65 mass% TiO2, 0.16-0.38 mass% GaO2 and 0.05-0.25 mass% ZnO2, calculated according to the original mass of the melt, in the interest of achieving a fine grain structure we precipitated these out of organic compounds together and/or separately in a known way. Finally the dipping was repeated several times in the interest of the total saturation of the external surface 22a of the shell 22, superfluous impregnation material used to form the active material coating 23 was removed from the external surface 22a of the shell 22 of the housing body 20 using a short duration of low amplitude vibration. The housing body 20 activated in this was again fired at 600±10 0C, and so we gain a housing body 20 of the desired shape, composition and structure.
The device 1 with the unique housing body 20 according to the invention may be used to good effect in all applications where dangerous materials and/or waste needs to be eliminated in an environmentally friendly way.
List of references
Device Reaction space barrier element housing body 21 solid core
21a boundary surface
22 shell
22a external surface
23 active material coating
24 cylindrical sheath section
25 dome section

Claims

1. Catalytic pyrolysis device primarily for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, which contains a housing body enclosing a reaction space and an active material coating covering at least part of the inner side of the housing body, where the housing body is a ceramic material with a solid core and a porous shell that has depressions suitable to receive the particles of the active material coating at least on the boundary surface of the core facing the reaction space, the active material coating has a nickel base containing magnesium, characterised by that the core (21) of the housing body (20) is from a protoenstatite ceramic stabilised with a sintered glassy phase, and the porous shell (22) at least partially covering the core (21) is from 0.6-1.1 mm thick magnesium silicate with added alpha-corundum, and the active material coating (23) located on the porous external surface (22a) of the shell (22) is Ni-Mg oxide produced using heat treatment from a Ni-Mg double salt and, in a given case, contains Ni-Si components.
2. The device according to claim 1, characterised by that the housing body (20) has a cylindrical sheath section (24) and dome section (25), as well as inlet and outlet opening, and is also supplemented with a barrier element (3).
3. The device according to claim 1 or 2, characterised by that the longitudinal cross- sectional shape of the boundary surface (21a) between the solid core (21) and the porous shell (22) is a sine curve wave, where the ratio between the middle diameter of the individual waves and their height falls between 0.3-1.
4. The device according to any of claims 1-3, characterised by that the external middle diameter of the boundary surface (21a) between the solid core (21) and the porous shell (22) is between 10-1000 mm.
5. The device according to any of claims 1-4, characterised by that the active material amount of the active material coating (23) established from a Ni-Mg double salt contains 0.64-0.76 mol% nickel, 0.23-0.28 mol% magnesium and, in a given case, Ni-Si.
6. The device according to any of claims 1-5, characterised by that the active material coating (23) contains, as an efficiency-increasing and accelerating component, 0.48-0.65 mass% titanium dioxide, 0.16-0.38 mass% gallium dioxide, and 0.05-0.25 mass% zinc dioxide.
7. Procedure for the production of the housing body structure of a catalytic pyrolysis device primarily suitable for the neutralisation of dangerous combustion products and waste materials, the elimination of flue gases and the utilisation of complex carbon chains, during which core material is formed, the formed core is subjected to heat treatment, following this it is coated with a shell former, then is subjected to heat treatment again, following this the shell receives an active material coating, and finally receives further heat treatment, characterised by that for the raw material for the production of the solid core (21) we use 50-65 mass% finely ground talcum powder, 15- 35 mass% talcum powder fired at 120O+50 0C and/or talcum powder, 4-7 mass% magnesium carbonate and 5-9 mass% barium carbonate, and, in a given case, 0.1-0.2 mass% rutile titanium dioxide, then the raw material is shaped by pressing and is fired at 750±10 0C, then as a porous shell (22) by immersion and/or spraying we apply a fine ground material slurry to the boundary surface (21a) of the solid core (21) produced in this way consisting of 6-14 mass% fine grain calcinated alpha corundum, 4-9 mass% white burning plastic fine clay, 55-68 mass% raw talcum and 22-28 mass% talcum powder fired at 120O+50 and 3-12 mass% paper industry grade pulped cellulose fibre, 0.1-0.2 mass% ammonium lignosulphate and 0.2-0.8 mass% tri-methylcellulose with a molar mass of between 1000-5000, we apply a material mixture with a density of 1250- 1300 g/1 and we continue thickening the porous shell (22) until the theoretical post- firing thickness of the porous shell (22) reaches 0.6-1.1 mm, following creating the porous shell (22) the housing body (20) is dried and fired at 1200±10 0C, then the housing body (20) with its solid core (21) and porous shell (22) is dipped once or several times in a Ni-Mg double salt melt and then any surplus is removed from the housing body (20) an in this way an active material coating is applied to the housing body (20), then finally the housing body (20) with the applied active material coating (23) is heat- treated at 600±10 0C.
8. The procedure according to claim 7, characterised by that a 96-0C melt of nitrate- hexahydrate is used as the Ni-Mg double salt.
9. The procedure according to claim 7 or 8, characterised by that before the housing body (20) with its solid core (21) and porous shell (22) is dipped a finely distributed efficiency-increasing and acceleration additive is mixed into the Ni-Mg double salt.
PCT/HU2008/000092 2007-08-03 2008-07-31 Catalytic pyrolysis device and procedure for the production of the structure of the housing body of the catalytic pyrolysis device WO2009019520A2 (en)

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