EP2903762A2 - Herstellung eines zusatzes eines turbinenbauteils mit mehreren materialien - Google Patents

Herstellung eines zusatzes eines turbinenbauteils mit mehreren materialien

Info

Publication number
EP2903762A2
EP2903762A2 EP13852362.6A EP13852362A EP2903762A2 EP 2903762 A2 EP2903762 A2 EP 2903762A2 EP 13852362 A EP13852362 A EP 13852362A EP 2903762 A2 EP2903762 A2 EP 2903762A2
Authority
EP
European Patent Office
Prior art keywords
powder
layers
laser
component
laser energy
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP13852362.6A
Other languages
English (en)
French (fr)
Inventor
Ramesh Subramanian
Michael Ott
Dimitrios Thomaidis
Alexandr Sadovoy
Jan Münzer
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Siemens AG
Original Assignee
Siemens AG
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Siemens AG filed Critical Siemens AG
Publication of EP2903762A2 publication Critical patent/EP2903762A2/de
Withdrawn legal-status Critical Current

Links

Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F7/00—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression
    • B22F7/02—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite layers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F10/00—Additive manufacturing of workpieces or articles from metallic powder
    • B22F10/30—Process control
    • B22F10/36—Process control of energy beam parameters
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F5/00—Manufacture of workpieces or articles from metallic powder characterised by the special shape of the product
    • B22F5/009—Manufacture of workpieces or articles from metallic powder characterised by the special shape of the product of turbine components other than turbine blades
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F5/00—Manufacture of workpieces or articles from metallic powder characterised by the special shape of the product
    • B22F5/04—Manufacture of workpieces or articles from metallic powder characterised by the special shape of the product of turbine blades
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F7/00—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression
    • B22F7/06—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite workpieces or articles from parts, e.g. to form tipped tools
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
    • B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
    • B23K26/00—Working by laser beam, e.g. welding, cutting or boring
    • B23K26/34—Laser welding for purposes other than joining
    • B23K26/342—Build-up welding
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B28—WORKING CEMENT, CLAY, OR STONE
    • B28B—SHAPING CLAY OR OTHER CERAMIC COMPOSITIONS; SHAPING SLAG; SHAPING MIXTURES CONTAINING CEMENTITIOUS MATERIAL, e.g. PLASTER
    • B28B1/00—Producing shaped prefabricated articles from the material
    • B28B1/001—Rapid manufacturing of 3D objects by additive depositing, agglomerating or laminating of material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B28—WORKING CEMENT, CLAY, OR STONE
    • B28B—SHAPING CLAY OR OTHER CERAMIC COMPOSITIONS; SHAPING SLAG; SHAPING MIXTURES CONTAINING CEMENTITIOUS MATERIAL, e.g. PLASTER
    • B28B1/00—Producing shaped prefabricated articles from the material
    • B28B1/008—Producing shaped prefabricated articles from the material made from two or more materials having different characteristics or properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C64/00—Additive manufacturing, i.e. manufacturing of three-dimensional [3D] objects by additive deposition, additive agglomeration or additive layering, e.g. by 3D printing, stereolithography or selective laser sintering
    • B29C64/10—Processes of additive manufacturing
    • B29C64/141—Processes of additive manufacturing using only solid materials
    • B29C64/153—Processes of additive manufacturing using only solid materials using layers of powder being selectively joined, e.g. by selective laser sintering or melting
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B33—ADDITIVE MANUFACTURING TECHNOLOGY
    • B33Y—ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3-D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3-D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
    • B33Y10/00—Processes of additive manufacturing
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01D—NON-POSITIVE DISPLACEMENT MACHINES OR ENGINES, e.g. STEAM TURBINES
    • F01D5/00—Blades; Blade-carrying members; Heating, heat-insulating, cooling or antivibration means on the blades or the members
    • F01D5/12—Blades
    • F01D5/28—Selecting particular materials; Particular measures relating thereto; Measures against erosion or corrosion
    • F01D5/288—Protective coatings for blades
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F10/00—Additive manufacturing of workpieces or articles from metallic powder
    • B22F10/20—Direct sintering or melting
    • B22F10/28—Powder bed fusion, e.g. selective laser melting [SLM] or electron beam melting [EBM]
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F12/00—Apparatus or devices specially adapted for additive manufacturing; Auxiliary means for additive manufacturing; Combinations of additive manufacturing apparatus or devices with other processing apparatus or devices
    • B22F12/50—Means for feeding of material, e.g. heads
    • B22F12/53—Nozzles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B22—CASTING; POWDER METALLURGY
    • B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
    • B22F2999/00—Aspects linked to processes or compositions used in powder metallurgy
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01D—NON-POSITIVE DISPLACEMENT MACHINES OR ENGINES, e.g. STEAM TURBINES
    • F01D5/00—Blades; Blade-carrying members; Heating, heat-insulating, cooling or antivibration means on the blades or the members
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F05—INDEXING SCHEMES RELATING TO ENGINES OR PUMPS IN VARIOUS SUBCLASSES OF CLASSES F01-F04
    • F05D—INDEXING SCHEME FOR ASPECTS RELATING TO NON-POSITIVE-DISPLACEMENT MACHINES OR ENGINES, GAS-TURBINES OR JET-PROPULSION PLANTS
    • F05D2230/00—Manufacture
    • F05D2230/30—Manufacture with deposition of material
    • F05D2230/31—Layer deposition
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P10/00—Technologies related to metal processing
    • Y02P10/25—Process efficiency
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/24—Structurally defined web or sheet [e.g., overall dimension, etc.]
    • Y10T428/24479—Structurally defined web or sheet [e.g., overall dimension, etc.] including variation in thickness
    • Y10T428/24521—Structurally defined web or sheet [e.g., overall dimension, etc.] including variation in thickness with component conforming to contour of nonplanar surface
    • Y10T428/24545—Containing metal or metal compound

Definitions

  • This invention relates to additive layer manufacturing, and particularly to making multi-material metal/ceramic gas turbine components by selective laser sintering and selective laser melting of adjacent powder layers of different materials.
  • Selective layer additive manufacturing includes selective laser melting (SLM) and selective layer sintering (SLS) of powder beds to build a component layer by layer to achieve net shape or near net shape.
  • SLM selective laser melting
  • SLS selective layer sintering
  • a powder bed of the component final materia! or precursor material is deposited on a working surface.
  • Laser energy is selectively directed onto the powder bed following a cross sectional area shape of the component, thus creating a layer or slice of the component, which then becomes a new working surface for a next layer.
  • the powder bed is conventionally spread over the working surface in a first step, and then a laser defines or "paints" the component sectional area on the bed in a following step, for example by raster scanning.
  • a related process often referred to as micro-cladding, deposits a powder onto a component via a moving nozzle or other delivery device.
  • a laser concurrently melts the powder at the deposit point, thus forming a bead of material on the component as the delivery device moves. Successive passes can build a layer or layers of material for repair or fabrication of a component.
  • FIG. 1 is a sectional view of a prior art gas turbine blade.
  • FIG. 2 Is a sectional view of a powder delivery device forming adjacent powder layers on a working surface.
  • FIG. 3 is a sectional view of laser beams melting and sintering adjacent powder layers.
  • FIG 4 shows a pattern of scan paths for powder delivery and/or laser delivery parallel to non-linear sectional profiles of a component
  • FIG 5 shows an alternate scan pattern with parallel linear paths.
  • FIG 6 shows scan paths that are normal, or approximately normal, to the walls of the component.
  • FIG 7 shows a second slice being formed on a first slice of the component.
  • FIG 8 shows adjacent powder layers deposited at different thicknesses.
  • FIG 9 shows an interlocking interface between adjacent materials.
  • FIG 10 is a flow chart showing aspects of an embodiment of the invention.
  • the inventors have devised a method for additive manufacturing of a component having multiple adjacent materials of different properties. It produces a net shape or near net shape with strong bonding of the adjacent materials, including metal to ceramic. This is especially beneficial in fabricating gas turbine components such as superalloy blades and vanes with ceramic thermal barrier coatings. Such airfoils are difficult to fabricate, because they have complex shapes with serpentine cooling channels lined with turbulators and film cooling holes.
  • FIG 1 is a transverse sectional view of a typical gas turbine airfoil 20 with a leading edge 22, trailing edge 24, pressure side 26, suction side 28, metal substrate 30, cooling channels 32, partition walls 34, turbulators 38, film cooling exit holes 38, cooling pins 40, and trailing edge exit holes 42.
  • the exterior of the airfoil substrate is coated with a ceramic thermal barrier coating 44.
  • a metallic bond coat 45 may be applied between the substrate and the thermal barrier coating.
  • Turbulators are bumps, dimples, ridges, or valleys within the cooling channels 32 that increase surface area and mix the fluid boundary layer of the coolant flow.
  • FIG 2 shows a process and apparatus for delivering first 48, second 50, and third 52 adjacent powder layers onto a working surface 54A in respective first, second, and third section area shapes of first, second, and third adjacent final materials in a given section plane of a component.
  • the first powder layer 48 may be a structural metal delivered in the area shape of an airfoil substrate 30 as shown in FIG 1.
  • the second powder layer 50 may be a bond coat delivered adjacent the first powder 48 in the area shape of a bond coat 45 on the substrate (FIG 1 ).
  • the third powder layer 52 may be a thermal barrier ceramic delivered adjacent the second powder in the area shape of the thermal barrier coating 44 (FIG 1 ).
  • An interface 58 between the first and second powder layers may be delivered so as to form an overlap zone 57 that provides a material gradient transition between the two adjacent powder layers 48, 50.
  • An interface 58 between the second and third powders 50, 52 may be delivered so as to form an engineered mechanical interlock such as interleaved fingers projecting alternately from the second and third powders (later shown).
  • the powder delivery device 60 may have one or more nozzles 62 delivering powder spray 64 to a focal point 66.
  • the powder delivery device 60 may incorporate multi-axis movements 61 relative to the working surface 54A, so that the nozzle can follow non-linear sectional profiles in a given horizontal plane, can move to different planes or distances relative to the working surface 54A, and can deliver powder at varying angles.
  • the axes may be implemented by motions of the work table 55 and/or the powder delivery device 60 via tracks and rotation bearings under computer control.
  • Powder delivery parameters such as nozzle translation speeds, mass delivery rates, and spray angles may be
  • the powder may be compacted and stabilized by means such as electromagnetic energy and/or mechanical or acoustic vibration prior to laser heating.
  • the powder may be wetted with water, alcohol, lacquer or binder prior to or during spraying so it holds a desired form until the laser melts or sinters it into a cohesive slice of the component.
  • flux material may be included with the powder materials to facilitate the cladding process.
  • FIG 3 shows a process and apparatus for melting and/or sintering different powder layers 48, 50, 52 with respective different laser energies.
  • the substrate superalloy powder 48 and the bond coat powder 58 may be melted with first and second laser energies, and the ceramic thermal barrier powder 52 may be sintered with a third laser energy that only partly melts the ceramic particles.
  • the different laser energies 69A, 69B may be provided by a single laser emitter 68A with variable output, or by multiple laser emitters 68A, 68B with different outputs for different powder layers.
  • the laser emitter may incorporate multi-axis movement 70 relative to the working surface 54A, so that it can follow non-linear sectional profiles in a given plane, can move to different planes or distances relative to the working surface 54A, and can position and direct a laser beam for desired angles and spot sizes.
  • FIG 4 shows a pattern of paths 72 that follow the non-linear sectional shape profiles 73, 74, 75 of the component 20.
  • the powder delivery focus 66 of FIG 2 may be controlled to follow such paths.
  • Such a scan pattern 72 parallel to the sectional shape profiles allows the powder type to be changed for each powder layer 48, 50, 52.
  • the laser energy 69A-B may also follow non-linear scan paths such as 72 of FIG 4. This path type minimizes the number of changes in laser intensity for different powder materials.
  • a first laser energy may be directed to follow a contour of the sectional shape 73 of the first powder layer 48
  • a second laser energy may be directed to follow a contour of a sectional shape 74 of the second powder layer 50
  • a third laser energy may be directed to follow a contour of a sectional shape 75 of the third powder layer 52.
  • the laser may be cycled off as it passes over areas intended to remain as voids in the formed component, such as film cooling holes 38.
  • FIG 5 shows an alternate scan pattern with parallel linear paths 74 for the laser energy.
  • FIG 6 shows paths 76 that are normal, or approximately normal, to the walls of the component. Patterns 74 and 76 may require laser intensity changes at each crossing of the interfaces 56, 58 for the different powder layers in addition to off/on cycling for the voids 38.
  • the spacing of scans 72, 74, 76 depends on the laser beam width or spot size at the powder surface. Multiple laser emitters may be used together to produce a wider swath to reduce the number of scans.
  • the laser beam(s) may be adjusted in width by changing the distance of the emitter from the working surface, and/or the beam may be adjusted In size and shape by adjustable lenses, mirrors, or masks to better define small, sharp, or curved elements of the component such as fillets, without decreasing the scan spacing and spot size.
  • FIG 7 shows a first solidified slice 74 of the component providing a new working surface 54B on which to apply powder layers 48, 50, 52 for a second slice 76 of the component.
  • FIG 8 shows powder layers 48, 50, 52 delivered at different heights depending on their respective process shrinkages to achieve a final uniform slice thickness.
  • the powders of the first 48 and second 50 adjacent layers may be deposited in the overlap zone 57 such that the powders overlap in a gradient material transition.
  • the overlap width may be at least 0.2 mm for example.
  • the powders of the second 50 and third 52 adjacent layers may also be deposited in an overlap zone 77 such that the powders overlap in a gradient material transition.
  • the overlap widths may be at least 0.2 mm or 0.4 mm or up to 1 mm or up to 2 mm. for examples.
  • FIG 9 shows an interface between the second 50 and third 52 layers formed with engineered interlocking features 80 there between, such as interleaved profiles that form 3D interlaced fingers projecting alternately from the bond layer 50 and the ceramic layer 52.
  • interlocking mechanical interface may be provided instead of, or in addition to, a gradient material zone 77 as shown in FIG 8.
  • Fissures 82 may be formed in the ceramic layer 52 for operational strain relief by cycling the laser energy off/on as it scans the ceramic layer 52.
  • Hollow ceramic spheres 84 may be included in the material of the ceramic layer 52 to reduce thermal conductivity. Inclusion of hollow ceramic spheres in the thermal barrier layer 52 permanently reduces its thermal conductivity, since the sphere voids are not subject to reduction by operational sintering.
  • FIG 10 is a flow chart of a method 84 showing aspects of an embodiment of the invention, including the following steps:
  • step 92 Repeating from step 86 with successive section planes to fabricate the component by selective layer additive manufacturing.
  • nano-scale ceramic particles can reduce the sintering temperature of the ceramic layer by as much as 350 °C in some embodiments. This can facilitate co-sintering and bonding of the metal and ceramic layers. Temperature reduction occurs particularly when the ceramic powder comprises at least 2% and up to 100% by volume of particles being less than 100 nm average diameter, and it especially occurs with particles less than 50 nm average diameter. The present method allows sintering by only partially melting such nano-particles. This is not possible when applying a ceramic coating with thermal spray technologies, because it tends to fully melt the smaller particles.
  • Nickel-based superalloys used in high temperature gas turbine components are often strengthened by a gamma prime precipitant phase within a gamma phase matrix.
  • the properties of these superalloys that make them durable in high-temperature environments also make them difficult to fabricate and repair.
  • they can be fabricated and joined to adjacent layers of different materials, including ceramics, by the method described herein. Casting of gas turbine blades having serpentine channels with turbulators and film cooling exit holes is difficult and expensive.
  • the present method reduces cost while more fully joining the different material layers, it allows a complete multi-material component such as a turbine blade to be fabricated in one process, instead of casting a superalloy blade, then coating it in a separate process, such as thermal spray.

Landscapes

  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Mechanical Engineering (AREA)
  • Materials Engineering (AREA)
  • Optics & Photonics (AREA)
  • Physics & Mathematics (AREA)
  • Composite Materials (AREA)
  • Ceramic Engineering (AREA)
  • Automation & Control Theory (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • Powder Metallurgy (AREA)
  • Turbine Rotor Nozzle Sealing (AREA)
  • Laminated Bodies (AREA)
  • Laser Beam Processing (AREA)
  • Other Surface Treatments For Metallic Materials (AREA)
EP13852362.6A 2012-10-08 2013-10-07 Herstellung eines zusatzes eines turbinenbauteils mit mehreren materialien Withdrawn EP2903762A2 (de)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
US201261710995P 2012-10-08 2012-10-08
US201261711813P 2012-10-10 2012-10-10
US14/043,037 US20140099476A1 (en) 2012-10-08 2013-10-01 Additive manufacture of turbine component with multiple materials
PCT/US2013/063641 WO2014107204A2 (en) 2012-10-08 2013-10-07 Additive manufacture of turbine component with multiple materials

Publications (1)

Publication Number Publication Date
EP2903762A2 true EP2903762A2 (de) 2015-08-12

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ID=50432877

Family Applications (1)

Application Number Title Priority Date Filing Date
EP13852362.6A Withdrawn EP2903762A2 (de) 2012-10-08 2013-10-07 Herstellung eines zusatzes eines turbinenbauteils mit mehreren materialien

Country Status (7)

Country Link
US (1) US20140099476A1 (de)
EP (1) EP2903762A2 (de)
JP (1) JP2016502589A (de)
CN (1) CN104684667A (de)
IN (1) IN2015DN02324A (de)
RU (1) RU2015116240A (de)
WO (1) WO2014107204A2 (de)

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