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
  • 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
  • B01J35/58—Fabrics or filaments
• • 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
  • B01J19/32—Packing elements in the form of grids or built-up elements for forming a unit or module inside the apparatus for mass or heat transfer
• • 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
  • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
  • B01J23/42—Platinum
• • 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
  • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
  • B01J23/46—Ruthenium, rhodium, osmium or iridium
  • B01J23/464—Rhodium
• • C—CHEMISTRY; METALLURGY
  • C01—INORGANIC CHEMISTRY
  • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
  • C01B21/00—Nitrogen; Compounds thereof
  • C01B21/20—Nitrogen oxides; Oxyacids of nitrogen; Salts thereof
  • C01B21/24—Nitric oxide (NO)
  • C01B21/26—Preparation by catalytic or non-catalytic oxidation of ammonia
  • C01B21/265—Preparation by catalytic or non-catalytic oxidation of ammonia characterised by the catalyst
• • C—CHEMISTRY; METALLURGY
  • C01—INORGANIC CHEMISTRY
  • C01C—AMMONIA; CYANOGEN; COMPOUNDS THEREOF
  • C01C3/00—Cyanogen; Compounds thereof
  • C01C3/02—Preparation, separation or purification of hydrogen cyanide
  • C01C3/0208—Preparation in gaseous phase
  • C01C3/0212—Preparation in gaseous phase from hydrocarbons and ammonia in the presence of oxygen, e.g. the Andrussow-process
  • C01C3/0216—Preparation in gaseous phase from hydrocarbons and ammonia in the presence of oxygen, e.g. the Andrussow-process characterised by the catalyst used
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
  • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
  • B01J2219/322—Basic shape of the elements
  • B01J2219/32203—Sheets
  • B01J2219/32213—Plurality of essentially parallel sheets
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
  • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
  • B01J2219/322—Basic shape of the elements
  • B01J2219/32203—Sheets
  • B01J2219/32248—Sheets comprising areas that are raised or sunken from the plane of the sheet
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
  • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
  • B01J2219/322—Basic shape of the elements
  • B01J2219/32203—Sheets
  • B01J2219/32248—Sheets comprising areas that are raised or sunken from the plane of the sheet
  • B01J2219/32251—Dimples, bossages, protrusions
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
  • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
  • B01J2219/324—Composition or microstructure of the elements
  • B01J2219/32408—Metal
  • B01J2219/32416—Metal fibrous
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
  • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
  • B01J2219/324—Composition or microstructure of the elements
  • B01J2219/32466—Composition or microstructure of the elements comprising catalytically active material
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
  • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
  • B01J2219/324—Composition or microstructure of the elements
  • B01J2219/32491—Woven or knitted materials

Definitions

• the present invention relates to a catalyst comprising a gas-permeable textile fabric made of noble metal-containing wire with a three-dimensional secondary structure produced thereon.
• Catalysts according to the invention are used in particular for heterogeneous catalysis, for example in the production of hydrocyanic acid by the Andrussow process or in the production of nitric acid by the Ostwald process.
• the reactants and the catalyst are present in different phases; the reactions take place on the surface of the catalyst.
• the catalyst-shaped body has one or more catalyst networks arranged one behind the other, which are arranged transversely to the flow direction of the fluid containing the reactants to be reacted.
• An important parameter of such catalyst networks is their catalytic effectiveness. Permanently high conversions of the educts and good yields are achieved if the catalyst network has a large catalytically active surface area, low flow resistance and at the same time high strength. Catalyst networks having a good catalytically active surface are often made by using textile processing techniques of precious metal wire, such as by machine weaving, knitting or knitting.
• the bending and tensile strengths and the ductility of the precious metal wires play a limiting role.
• the bending and tensile strengths and the ductility of the precious metal wires play a limiting role.
• the bending and tensile strengths and the ductility of the precious metal wires play a limiting role.
• only noble metal wires with specific wire diameters and tensile strengths are suitable.
• the catalytically active surface is determined within a certain range.
• the catalyst nets produced by textile processing techniques have high flexibility and low rigidity.
• the catalyst network is usually flowed through by an ammonia-oxygen mixture at high speed.
• the reaction temperature is usually about 800 ° C to 1 .100 ° C and the pressure 1 to 12 bar.
• Catalyst networks with high dimensional stability can withstand high pressures better and contribute to a uniform flow through the catalyst; a high rigidity and dimensional stability of the catalyst networks are therefore basically desirable for reasons of reproducibility. It is known that a higher strength of catalyst networks can be achieved if they have a secondary structure.
• US Pat. Nos. 5,401,483 and 6,030,594 A describe a secondary structure in the form of a fold.
• a catalyst support with a plurality of successively arranged knitted wire nets of folded metal is known from DE 23 53 640 A1. Also in this catalyst carrier, the individual networks are folded to their mechanical stabilization.
• Catalyst networks secondary structure of three-dimensional embossing patterns as known for example from US 2,045,632 A and in particular from WO 93/24229 A1 avoid this disadvantage.
• the catalyst network of the last-mentioned document is used for the catalytic conversion of ammonia into nitrogen oxide.
• the three-dimensional embossing pattern includes elevations and depressions and is referred to, for example, as "embossed, contoured or pitted.
• the secondary structure imprinted on the network serves to prevent a deformation observed in the use of planar nets into a turtle-chip-like structure, which reduces the flexibility of the netting. It is either produced directly during mesh production or subsequently by pressing.
• the invention is therefore based on the object to provide an easy-to-produce catalyst, on the one hand has a high mechanical stability and on the other hand is optimized in terms of its flow behavior and concomitantly with respect to catalytic efficiency and yield.
• the secondary structure is a buckling structure, which has juxtaposed, adjacent dentures in two spatial directions, which have the shape of a hexagon, wherein the buckling structure in a buckling process by self-organization is trained.
• Catalysts with a textile fabric made of noble metal-containing wire regularly have a low dimensional stability; they are flexible and easily mechanically deformable.
• a secondary structure in the form of a buckling structure hereinafter also referred to as a "buckle structure").
• the buckling structure of the textile fabric comprises a plurality of three-dimensional indentations generated on the fabric, which contribute to the mechanical stabilization thereof. Because the buckling structure extends in two spatial directions and has indentations that are lined up in two spatial directions, a planar increase in strength and dimensional stability is achieved.
• a textile fabric having such a buckling structure is initially distinguished in comparison to a textile fabric having a secondary structure in the form of a fold by a good dimensional stability in three spatial directions.
• the textile fabric is produced by self-organizing buckling structuring and as a result less mechanically stressed, in particular by tensile forces.
• buckling structuring in contrast to folding and Imprinting hardly any flow processes; It is therefore also associated with no significant increase in surface area. This is explained in more detail below:
• the buckling structure is formed as part of the buckling process, at least partially by self-organization.
• self-organization means a process in which the surface of the workpiece to be reshaped, without being completely predetermined by a negative mold, at least partially form independently during the forming process.
• Secondary structures generated by self-assembly have an energetically particularly favorable shape and a lower plastic deformation and, consequently, a lower local weakening. As a result, a textile fabric having particularly good mechanical dimensional stability and rigidity is obtained.
• the buckling structure is produced with a pressure medium using a structured support element, for example with a liquid pressure medium (hydraulically), with a gaseous pressure medium (pneumatically) and / or by means of a solid, elastic pressure medium.
• the buckling pressure used to produce the buckling structure can consist of both an overpressure and a negative pressure.
• the support element defines the buckling structure in contact with the textile fabric moving thereover.
• the support element is serpentine or zigzag-shaped; but it may also be formed, for example, spiral, annular or disc-shaped.
• the indentations have a circumference, for example in a projection onto a base surface of the textile fabric.
• the basic form of the denting is determined by the extent of the denting.
• the self-governing The generated dentures according to the invention have the shape of a Hexagons. Indentations with a hexagonal basic shape contain a low internal energy and they contribute to a high mechanical stability and dimensional stability of the textile fabric.
• the hexagonal basic shape may be rounded in the area of the junction of the hexagon sides.
• a beulDeutschABLEs textile fabric contributes to an optimized flow behavior of both a single sheet and the entire catalyst.
• the textile fabric is arranged regularly transversely to the direction of flow through the catalyst; it has openings, for example in the form of meshes or loops, which ensure a flow through the catalyst in the direction of flow.
• the smaller the opening width of these openings the more likely they are to impact the catalyst surface so that reaction catalysis occurs and the speed and direction of the chemical processes can be affected. In terms of good contact catalysis, the openings are therefore as small as possible. However, a small opening width is associated with a high flow resistance and thus high pressure differences.
• Each buckling of the buckling structure includes a plurality of such openings.
• the opening planes in the region of the indentations extend partially obliquely to a base surface of the textile fabric, so that in principle an oblique arrangement of the openings with respect to the flow direction results. This results in a reduction in the effective opening width of the fabric despite the same opening width and also causes the probability of contact of a reactant with the catalyst surface is increased and therefore also contributes to a more effective catalysis.
• the sheet defines a base in which the Beulpatented extends in two spatial directions, wherein the indentations are perpendicular to the base.
• a sheet-like extending catalyst net with indentations arranged perpendicular thereto has a high mechanical stability due to the indentations; It is also easy and inexpensive to manufacture.
• the catalyst is designed to flow through with a fluid in the flow direction, and that the base surface is perpendicular to the flow direction.
• the arrangement of the base perpendicular to the flow direction contributes to the most uniform flow through the catalyst.
• the individual indentations have in this arrangement, a central region in which the openings of the textile fabric are arranged parallel and offset from the base surface, and an edge region.
• the openings in the edge region are arranged transversely to the direction of flow; they have a smaller opening width in a projection onto the base area, and thus facilitate the impact of an educt on the catalyst surface and thus the catalysis.
• adjacent dentures are separated by a peripheral zone.
• the border zone defines a base of the textile fabric and the hexagonal basic structure of the denting. Based on the base area defined by the edge zone, the indentations have a region of maximum denting (deflection). Adjacent dentures are separated by the peripheral zone.
• the edge zone avoids sharp transitions between adjacent dentures and thus contributes to the mechanical strength of the catalyst network. It can be formed areally or approximately linear. In the case of a planar edge zone, it has proven useful if it has a width in the range of 0.1 mm to 10 mm, preferably in the range of 1 mm to 5 mm.
• the textile fabric comprises several dentures with edge zones.
• An edge zone with a width of at least 0.1 mm contributes to a good stabilization of the sheet and a good dimensional stability.
• An edge zone with a width of more than 10 mm is associated with a large proportion of edge zone area on the entire surface of the textile fabric.
• the area of one of the hexagonal indentations in a projection on a flat base has a size in the range of 0.25 cm 2 to 15 cm 2 , preferably in the range of 0.5 cm 2 to 3 cm 2 , Buckling whose area is less than 0.25 cm 2 , consequently lead to a large proportion of the surface associated with the surface area of the total surface of the textile fabric, whereby the effect of the obliquely arranged in the region of the denting openings loses the flow behavior of the catalyst. Bumps with a size of more than 15 cm 2 contribute only slightly to a mechanical stabilization and an increase in the dimensional stability of the textile sheet.
• the depth of the dentures in the range of 1 mm to 10 mm, preferably in the range of 2 mm to 5 mm.
• Dents with a depth in the above range are easy and cost-effective to manufacture. In addition, they lead only to a low mechanical stress and plastic deformation during the forming of the textile fabric, so that it has a good mechanical stability.
• the noble metal wire is made of a platinum metal or an alloy thereof.
• the noble metal-containing wire is made of precious metal or it contains a significant proportion (> 50 wt .-%) of precious metal.
• the noble metal is a platinum metal.
• platinum metal is understood to mean the elements osmium, iridium, platinum, ruthenium, rhodium, palladium. Platinum metals are suitable for use in catalysts.
• the catalyst comprises a plurality of textile fabrics arranged one behind the other, the indentations of adjacent fabrics being offset from each other.
• the textile fabrics have an upper side with concavely curved indentations and a lower side with convexly outwardly curved indentations, and if the textile fabrics are arranged one behind the other such that the upper side and underside of the textile fabrics face one another.
• the top and bottom can differ in their dimensional stability in the direction of flow and in the opposite direction. If the upper and lower sides of the textile fabrics face one another, then the fabric has approximately the same mechanical stability both in the flow direction and in the opposite direction. As a result, the catalyst has no preferred direction; it can be installed in both directions in a reactor. At the same time by the opposite arrangement, a compact arrangement of the fabric is obtained, which contributes to a high dimensional stability and a uniform flow through the catalyst.
• the textile fabric has openings whose opening width is less than 500 ⁇ , preferably in the range between 5 ⁇ and 300 ⁇ .
• FIG. 1 shows a first embodiment of the catalyst according to the invention with a textile fabric in a plan view in a schematic
• FIG. 2 is a photographic representation of a textile fabric according to the invention
• FIG. 3 is a schematic representation of a second embodiment of the catalyst according to the invention with a plurality of textile fabrics arranged one behind the other and offset from one another, and FIG. 3
• Figure 4 shows a third embodiment of the catalyst according to the invention with several consecutively arranged textile fabrics, the top and bottom opposite to each other in a schematic representation.
• FIG. 1 shows a top view of a first embodiment of the catalyst according to the invention, to which the reference numeral 1 is assigned overall.
• the catalytic converter 1 comprises 25 catalyst networks arranged one after the other and offset from one another, of which only the uppermost catalytic converter network 2 is shown in FIG.
• the catalyst nets not shown in FIG. 1 are designed like the catalyst net 2.
• the catalyst net 2 is a textile fabric in the form of a knitted fabric, which is produced by machining a noble metal-containing wire 3.
• the noble metal-containing wire 3 is made of a platinum-rhodium alloy (95/5). manufactures and has a wire diameter of 76 ⁇ .
• the catalyst net 2 has a weight per unit area of 7.3 g / dm 2 .
• the mesh openings are identified by the reference numeral 7.
• the catalyst network is a textile fabric in the form of a fabric having a mean mesh size of 236 ⁇ .
• the catalyst net 2 is provided with a three-dimensional secondary structure. It has a beulGermanieri surface which is hydraulically generated with a liquid pressure medium using a shaping Stützele- element.
• Suitable support element for example, a spiral, polygons, rings or discs.
• the catalyst net 2 has a honeycomb structure by stringing together hexagonal indentations.
• the individual indentations 4 are curved in the direction below the plane of the drawing; they are strung together in two spatial directions x, y.
• Adjacent dentures 4 are separated by a peripheral zone 5.
• the edge zone 5 is flat and has a width of about 2 mm.
• the indentations 4 have a hexagonal basic shape.
• the area of the denting in the projection on the network level 6 is about 3 cm 2 .
• the depth of the denting is about 2.5 mm.
• Catalyst 1 is suitable for the production of nitric acid by the Ostwald method.
• nitric acid presentation it is passed through by an ammonia / oxygen mixture (catalytic combustion of ammonia). The following reaction takes place:
• FIG. 2 shows a photograph of the catalyst network according to the invention, to which the reference number 20 is assigned overall.
• the catalyst network 20 is a knitted fabric made of a platinum / rhodium (95/5) wire with a wire diameter of 76 ⁇ .
• the knitted fabric has a vault-structured surface, which was produced by pressure effect on the knitted fabric with the aid of a sinusoidal support element.
• a vault-structured, honeycomb-shaped surface is formed by self-organization, so that the catalyst network 20 has a high mechanical stability.
• the arch structure of the catalyst network has indentations 21 lined up in two spatial directions.
• the individual indentations 21 are curved in the direction below the plane of the drawing; they are strung together in two spatial directions x, y.
• Adjacent indentations 21 are separated from one another by an edge zone 22.
• the edge zone 22 has a width of about 2.5 mm.
• the indentations 21 In a projection onto a network plane 23 defined by the edge zone 22, the indentations 21 have a rounded polygonal basic shape.
• the area of one of the indentations 21 in the projection onto the network plane 23 is approximately 2 cm 2 .
• the depth of the denting is about 3 mm.
• FIG. 3 shows an embodiment of a catalyst 30 according to the invention with six catalyst nets 31 a-f in cross-section.
• the catalyst 30 is suitable for the production of hydrocyanic acid by the Andrussow method; it is flowed around in the hydrogen cyanide production of a gaseous ammonia-methane-air mixture.
• the flow direction is perpendicular to the network plane of the catalyst networks 31 a-f and is shown by the arrows 32, 33.
• the catalyst networks 31 af each have an upper side 34 a-f and a lower side 35 a-f. For the sake of simplicity, only the upper sides 34a, 34f and the lower sides 35a, 35f are shown in FIG.
• the top sides 34a-f have indentations 36, the bottom sides 35a-f show the indentations 36 corresponding bulges 37.
• the catalyst networks 31 af are arranged one behind the other, that in each case the top of a first network and bottom of the subsequent, second Net opposite.
• FIG. 4 shows in cross-section a further embodiment of a catalyst 40 according to the invention with six catalyst networks 41 af.
• the catalyst 40 is suitable for the production of nitric acid by the Ostwald method; it is flowed around in the nitric acid production of a gaseous ammonia-oxygen mixture.
• the flow direction is perpendicular to the network plane of the catalyst networks 41 af and is shown by the arrows 42, 43.
• the catalyst networks 41 a-f each have an upper side 44a-f and a lower side 45a-f. For the sake of simplicity, only the upper sides 44e, 44f and the lower sides 45e, 45f are shown in FIG.
• the topsheets 44a-f have concave inwardly arched indentations 46 of hexagonal ground structure; the lower surfaces 45a-f show convex raised bulges 47 corresponding to the indentations 46.
• the catalyst nets 41a-f are arranged one behind the other in such a way that the upper side of a first network and upper side of the second network following it are opposite each other.
• the PtRh5 catalyst nets in the reference reactor 1 were flat and were stacked.
• the catalyst package consists of five networks of PtRh without vault structure and a location Kanthai network.
• the catalyst package in reactor 2 consists of four layers of PtRh5 catalyst network with a vault structure, completed by a layer of Kanthai net. Adjacent catalyst networks were arranged one above the other so that the bulges were in one another, as shown in Fig. 4.
• the kanthai network of both network packets fulfills a function, which is not essential for the present invention, of separating the respective catalytic networks from the underlying carrier.
• test results include the catalyst efficiency of the catalyst (yield of NO in%), the nitrous oxide content of the reaction gas (in ppm by weight), the pressure loss across the catalyst bed (in mmH 2 O) and the temperature ,
• the test series were each prepared for an ammonia load of 8 and 12 tN / m 2 d.
• the result of the test shows that the catalyst efficiency for the package of catalyst nets with a vault structure is 0.9% or 1, 1% higher than in the case of a package of catalyst nets without a vault structure. In this area of technology, this represents a significant and economically significant increase. It is attributed to the fact that in a vault structure, the probability of contact of a reactant with the catalyst surface is relatively larger and therefore contributes to a more effective catalysis.

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• 2013
  • 2013-02-21 DE DE102013101749.5A patent/DE102013101749A1/de not_active Ceased
• 2014
  • 2014-02-20 EP EP14708501.3A patent/EP2958672A1/de not_active Withdrawn
  • 2014-02-20 RU RU2015139857A patent/RU2015139857A/ru unknown
  • 2014-02-20 CN CN201480009654.9A patent/CN105073251B/zh not_active Expired - Fee Related
  • 2014-02-20 BR BR112015020034A patent/BR112015020034A2/pt active Search and Examination
  • 2014-02-20 US US14/769,324 patent/US9757720B2/en not_active Expired - Fee Related
  • 2014-02-20 WO PCT/EP2014/053327 patent/WO2014128216A1/de active Application Filing

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