WO2005092816A2 - Utilisation de compositions de poudres polymeres redispersibles dans l'eau dans des materiaux de construction d'argile - Google Patents

Utilisation de compositions de poudres polymeres redispersibles dans l'eau dans des materiaux de construction d'argile Download PDF

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Publication number
WO2005092816A2
WO2005092816A2 PCT/EP2005/002544 EP2005002544W WO2005092816A2 WO 2005092816 A2 WO2005092816 A2 WO 2005092816A2 EP 2005002544 W EP2005002544 W EP 2005002544W WO 2005092816 A2 WO2005092816 A2 WO 2005092816A2
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WO
WIPO (PCT)
Prior art keywords
clay
acrylate
use according
copolymers
vinyl
Prior art date
Application number
PCT/EP2005/002544
Other languages
German (de)
English (en)
Other versions
WO2005092816A3 (fr
Inventor
Hermann Lutz
Alois Sommerauer
Klaus Bonin
Original Assignee
Wacker Polymer Systems Gmbh & Co. Kg
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 Wacker Polymer Systems Gmbh & Co. Kg filed Critical Wacker Polymer Systems Gmbh & Co. Kg
Priority to EP05715922A priority Critical patent/EP1725507A2/fr
Publication of WO2005092816A2 publication Critical patent/WO2005092816A2/fr
Publication of WO2005092816A3 publication Critical patent/WO2005092816A3/fr
Priority to IN4829CHN2014 priority patent/IN2014CN04829A/en

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Classifications

    • 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
    • C04B24/00—Use of organic materials as active ingredients for mortars, concrete or artificial stone, e.g. plasticisers
    • C04B24/24—Macromolecular compounds
    • C04B24/26—Macromolecular compounds obtained by reactions only involving carbon-to-carbon unsaturated bonds
    • C04B24/2641—Polyacrylates; Polymethacrylates
    • 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
    • C04B28/00—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements
    • C04B28/001—Compositions of mortars, concrete or artificial stone, containing inorganic binders or the reaction product of an inorganic and an organic binder, e.g. polycarboxylate cements containing unburned clay
    • 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
    • C04B2103/00—Function or property of ingredients for mortars, concrete or artificial stone
    • C04B2103/0045—Polymers chosen for their physico-chemical characteristics
    • C04B2103/0057—Polymers chosen for their physico-chemical characteristics added as redispersable powders
    • 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
    • C04B2103/00—Function or property of ingredients for mortars, concrete or artificial stone
    • C04B2103/0045—Polymers chosen for their physico-chemical characteristics
    • C04B2103/0066—Film forming polymers

Definitions

  • the invention relates to the use of water-redispersible polymer powder compositions containing one or more film-forming polymers, one or more protective colloids and, where appropriate, antiblocking agents in clay building materials, in particular clay dry mortars.
  • Earth building materials have been used as building materials for many centuries, especially for building houses.
  • Loam is not a standardized building material and has a different composition depending on the place of discovery, which is generally a mixture of clay, silt (fine sand) and sand, which can also contain coarser components such as gravel, crushed stone or stones, and their proportion of clay is about 10 to 30% by weight.
  • the advantages of earth building materials are their easy availability, simple processing, their high moisture storage effect (pleasant indoor climate) and their ecological advantages (reusability).
  • Building materials based on clay are therefore increasingly used today in the form of wet mortars, but increasingly also in the form of dry mortars in interior construction, e.g. used for plastering the walls (basic and decorative plasters) but also in connection with wooden constructions as filler material, or as adobe and wall paints.
  • Other areas of application of earth building materials are soil sealing, for example in landfills, and in dam construction.
  • the object of the invention was to improve the mechanical strength and water resistance of earth building materials, in particular dry clay mortars. In addition, the processability of the earth building materials should remain guaranteed.
  • the invention relates to the use of water-redispersible, emulsifier-free polymer powder compositions containing one or more film-forming polymers, one or more protective colloids and, where appropriate, anti-blocking agents in clay building materials.
  • Suitable film-forming polymers are those based on one or more monomers from the group comprising vinyl esters, (meth) acrylic esters, vinyl aromatics, olefins, 1,3-dienes and vinyl halides and optionally other monomers copolymerizable therewith.
  • Suitable vinyl esters are those of carboxylic acids with 1 to 12 carbon atoms.
  • Vinyl acetate is particularly preferred.
  • Suitable monomers from the group of acrylic acid esters or methacrylic acid esters are esters of unbranched or branched alcohols having 1 to 15 carbon atoms.
  • Preferred methacrylic acid esters or acrylic acid esters are methyl acrylate, methyl methacrylate, ethyl acrylate, ethyl methacrylate, propyl acrylate, pro- pyl methacrylate, n-butyl acrylate, n-butyl methacrylate, t-butyl acrylate, t-butyl methacrylate, 2-ethylhexyl acrylate.
  • Methyl acrylate, methyl methacrylate, n-butyl acrylate, t-butyl acrylate and 2-ethylhexyl acrylate are particularly preferred.
  • Styrene, methylstyrene and vinyltoluene are preferred as vinyl aromatics.
  • the preferred vinyl halide is vinyl chloride.
  • the preferred olefins are ethylene, propylene and the preferred dienes are 1,3-butadiene and isoprene.
  • auxiliary monomers can also be copolymerized. 0.5 to 2.5% by weight of auxiliary monomers are preferably used.
  • auxiliary monomers are ethylenically unsaturated mono- and dicarboxylic acids, preferably acrylic acid, methacrylic acid, fumaric acid and maleic acid; ethylenically unsaturated carboxamides and nitriles, preferably acrylamide and acrylonitrile; Mono- and diesters of fumaric acid and maleic acid such as the diethyl and diisopropyl esters and maleic anhydride, ethylenically unsaturated sulfonic acids or their salts, preferably vinylsulfonic acid, 2-acrylamido-2-methyl-propanesulfonic acid.
  • pre-crosslinking comonomers such as polyethylenically unsaturated comonomers, for example divinyl adipate, diallyl maleate, allyl methacrylate or triallyl cyanurate, or post-crosslinking comonomers, for example acrylamidoglycolic acid (AGA), methyl acrylamide methyl NMA (methylolamide), (MAGMEamide), Methylol methacrylamide, N-methyl olallyl carbamate, alkyl ethers such as the isobutoxy ether or ester of N-methylol acrylamide, N-methylol methacrylamide and N-methylolallyl carbamate.
  • AGA acrylamidoglycolic acid
  • MAGMEamide methyl acrylamide methyl NMA
  • Methylol methacrylamide N-methyl olallyl carbamate
  • alkyl ethers such as the isobutoxy ether or ester of N-methylol
  • Epoxy-functional comonomers such as glycidyl methacrylate and glycidyl acrylate are also suitable.
  • silicon-ciumfunktionelle comonomers such as acryloxypropyltri (alkoxy) - and methacryloxypropyltri (alkoxy) silanes, vinyltrialkoxysilanes and vinylmethyldialkoxysilanes, with alkoxy groups at ⁇ example as ethoxy and ethoxypropylene glycol ether radicals can be contained.
  • Monomers with hydroxyl or CO groups for example methacrylic acid and acrylic acid, may also be mentioned.
  • rehydroxyalkyl esters such as hydroxyethyl, hydroxypropyl or hydroxybutyl acrylate or methacrylate, and compounds such as diacetone acrylamide and acetylacetoxyethyl acrylate or methacrylate.
  • transition temperature is in general a glass ⁇ Tg of ⁇ 40 ° C, preferably -10 ° C to + 25 ° C results.
  • the glass transition temperature Tg of the polymers can be determined in a known manner by means of differential scanning calorimetry (DSC).
  • DSC differential scanning calorimetry
  • Tgn the glass transition temperature ⁇ in Kelvin of the homopolymer of the monomer n. Tg values for homopolymers are listed in Polymer Handbook 2nd Edition, J. Wiley & Sons, New York (1975).
  • Homopolymers or copolymers which contain one or more monomers from the group consisting of vinyl acetate, vinyl esters of ⁇ -branched monocarboxylic acids having 9 to 11 carbon atoms, vinyl chloride, ethylene, methyl acrylate, methyl methacrylate, ethyl acrylate, ethyl methacrylate, propyl acrylate, propyl methacrylate, n -Butyl acrylate, n-butyl methacrylate, 2-ethylhexyl acrylate, styrene included.
  • Copolymers with vinyl acetate and ethylene are particularly preferred; with vinyl acetate, ethylene and a vinyl ester of ⁇ -branched monocarboxylic acids with 9 to 11 carbon atoms; with n-butyl acrylate and 2-ethylhexyl acrylate and / or methyl methacrylate; with styrene and one or more monomers from the group of methyl acrylate, ethyl acrylate, propyl acrylate, n-butyl acrylate, 2-ethylhexyl acrylate; with vinyl acetate and one or more monomers from the group consisting of methyl acrylate, ethyl acrylate, propyl acrylate, n-butyl acrylate, 2-ethylhexyl acrylate and optionally ethylene; with 1,3-butadiene and styrene and / or methyl methacrylate and optionally further acrylic acid esters; where the mixtures mentioned may
  • polymers of the abovementioned compositions which still contain 0.1 to 5% by weight, based on the total weight of the polymer, of monomer units which are derived from one or more comonomers from the group comprising ethylenically unsaturated mono- and dicarboxylic acids, such as Acrylic acid, methacrylic acid, fumaric acid and maleic acid; ethylenically unsaturated carboxamides and nitriles such as acrylamide and acrylonitrile; Monoesters of fumaric acid and maleic acid, as well as maleic anhydride, ethylenically unsaturated sulfonic acids or their salts, preferably vinylsulfonic acid, 2-acrylamido-2-methyl-propanesulfonic acid.
  • ethylenically unsaturated mono- and dicarboxylic acids such as Acrylic acid, methacrylic acid, fumaric acid and maleic acid
  • the film-forming polymers are prepared by the emulsion polymerization process or by the suspension polymerization process in the presence of protective colloids, preferably by the emulsion polymerization process, the polymerization temperature generally being 40 ° C. to 100 ° C., preferably 60 ° C. to 90 ° C., and at the copolymerization of gaseous comonomers such as ethylene can also be carried out under pressure, generally between 5 bar and 100 bar.
  • the polymerization is initiated using the water-soluble or monomer-soluble initiators or redox initiator combinations which are customary for emulsion polymerization or suspension polymerization. Examples of water-soluble initiators are sodium persulfate, hydrogen peroxide and azobisisobutyronitrile.
  • Examples of monomer-soluble initiators are dicetyl peroxydicarbonate, dicyclohexyl peroxydicarbonate, dibenzoyl peroxide.
  • the initiators mentioned are generally used in an amount of 0.01 to 0.5% by weight, based on the total weight of the monomers.
  • Combinations of the initiators mentioned in combination with reducing agents are used as redox initiators.
  • Suitable reducing agents are, for example, sodium sulfite, sodium hydroxymethanesulfinate and ascorbic acid.
  • the amount of reducing agent is preferably 0.01 to 0.5% by weight, based on the total weight of the monomers.
  • regulating substances can be used during the polymerization.
  • regulators are usually used in amounts of between 0.01 and 5.0% by weight, based on the monomers to be polymerized, and are metered in separately or premixed with reaction components.
  • examples of such substances are n-dodecyl mercaptan, tert. -Dodecyl mercaptan, mercaptopropionic acid, mercaptopropionic acid methyl ester, isopropanol and acetaldehyde. No regulating substances are preferably used.
  • Suitable protective colloids are partially saponified or fully saponified polyvinyl alcohols; polyvinylpyrrolidones; polyvinyl; Polysaccharides in water-soluble form such as starches (amylose and amylopectin), celluloses and their carboxymethyl, methyl, hydroxyethyl, hydroxypropyl derivatives; Proteins such as casein or caseinate, soy protein, gelatin; lignin; synthetic polymers such as poly (meth) acrylic acid, copolymers of (meth) acrylates with carboxyl-functional comonomer units, poly (meth) acrylamide, polyvinylsulfonic acids and their water-soluble copolymers; Melamine formaldehyde sulfonates, naphthalene formaldehyde sulfonates, styrene maleic acid and vinyl ether maleic acid copolymers.
  • Partially saponified or fully saponified polyvinyl alcohols are preferred.
  • Partially saponified polyvinyl alcohols with a degree of hydrolysis of 80 to 95 mol% and a Höppler viscosity in 4% aqueous solution of 1 to 30 mPas are particularly preferred (Höppler method at 20 ° C., DIN 53015).
  • postpolymerization can be carried out using known methods to remove residual monomers, for example by postpolymerization initiated with a redox catalyst. Volatile residual monomers can also be removed by distillation, preferably under reduced pressure, and, if appropriate, with the passage or passage of inert entraining gases such as air, nitrogen or water vapor.
  • the aqueous dispersions thus obtainable have a solids content of 30 to 75% by weight, preferably 50 to 60% by weight.
  • the dispersions are dried, if appropriate after the addition of protective colloids as a spraying aid, for example by means of fluidized-bed drying, freeze drying or spray drying. The dispersions are preferably spray dried.
  • Spray drying is carried out in conventional spray drying systems, and atomization can be carried out by means of single-, two- or multi-component nozzles or with a rotating disc.
  • the outlet temperature is generally selected in the range from 45 ° C. to 120 ° C., preferably 60 ° C. to 90 ° C., depending on the system, the Tg of the resin and the desired degree of drying.
  • the viscosity of the food to be consumed is adjusted via the solids content in such a way that a value of ⁇ 500 mPas (Brookfield viscosity at 20 revolutions and 23 ° C.), preferably ⁇ 250 mPas, is obtained.
  • the solids content of the dispersion to be evaporated is> 35%, preferably> 40%.
  • the spray aid is used in a total amount of 0.5 to 30% by weight, based on the polymeric constituents of the dispersion.
  • the total amount of protective colloid before the drying process should be at least 1 to 30% by weight, based on the polymer content; 5 to 20% by weight, based on the polymer content, are preferably used.
  • Suitable protective aids are, for example, the protective colloids already mentioned. No other protective colloids are preferably used as polyvinyl alcohols as a spray aid.
  • the powder obtained can be equipped with an antiblocking agent (antibacking agent), preferably 1 to 30% by weight, based on the total weight of polymeric constituents.
  • antiblocking agents are calcium carbonate or magnesium carbonate, talc, gypsum, silica, kaolins such as metakaolin, silicates with particle sizes preferably in the range from 10 nm to 10 ⁇ m.
  • hydrophobic finishing one or more hydrophobizing agents from the group comprising fatty acids and fatty acid derivatives and organosilicon compounds can be added to them before the dispersions are dried. Suitable compounds for this are listed, for example, in DE-A 10323205.
  • the clay building materials modified according to the invention are suitable for use as clay base plasters, clay decor plasters and clay paints, preferably for interior walls and ceilings, but also for exterior walls and damp rooms; as a clay mortar for laying clay bricks, for example to fill out timber frameworks, as a clay filler for floors / walls / ceilings; and as clay building adhesives.
  • the clay building materials modified according to the invention are also advantageous in the production of clay moldings in order to impart greater resistance and strength to them, for example for clay / clay figures, clay / clay bricks, extruded clay moldings.
  • dispersion powders coating the clay mortar with dispersion powders results in an extreme increase in the mechanical strength values (bending tensile strength, compressive strength, adhesion), which go far beyond what is known in other building material systems and mortars based on cement, gypsum or calhydrate.
  • dispersion powders with a hydrophobic effect it is surprisingly not only possible to massively reduce water absorption, but also to achieve very good water and moisture resistance, so that such products are also suitable for outdoor use.
  • the redispersion powders were tested in the following clay formulation:
  • the clay mortar was applied to clay bricks using a template (50 mm diameter, 10 mm thick). After the mortar had hardened, metal tie rods were glued to the clay mortar to be tested after 27 days with epoxy resin adhesive in order to carry out the adhesive tensile test.
  • the adhesive pull values were determined in accordance with DIN 18156 in each case after the abovementioned storage with a pull-off device from Herion with a load increase rate of 250 N / s.
  • the measured values in N / mm 2 represent mean values from 5 measurements.
  • the adhesive tensile strengths were determined after 2 storage conditions:

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  • Chemical & Material Sciences (AREA)
  • Ceramic Engineering (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Dispersion Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Paints Or Removers (AREA)
  • Processes Of Treating Macromolecular Substances (AREA)
  • Curing Cements, Concrete, And Artificial Stone (AREA)

Abstract

L'invention concerne l'utilisation de compositions de poudres polymères redispersibles dans l'eau, exemptes d'émulsifiants, contenant un ou plusieurs polymérisats filmogènes, un ou plusieurs colloïdes protecteurs et éventuellement des agents antiadhérents, dans des matériaux de construction d'argile.
PCT/EP2005/002544 2004-03-18 2005-03-10 Utilisation de compositions de poudres polymeres redispersibles dans l'eau dans des materiaux de construction d'argile WO2005092816A2 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
EP05715922A EP1725507A2 (fr) 2004-03-18 2005-03-10 Utilisation de compositions de poudres polymeres redispersibles dans l'eau dans des materiaux de construction d'argile
IN4829CHN2014 IN2014CN04829A (fr) 2004-03-18 2006-09-18

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102004013468.5 2004-03-18
DE200410013468 DE102004013468A1 (de) 2004-03-18 2004-03-18 Verwendung von in Wasser redispergierbaren Polymerpulver-Zusammensetzungen in Lehmbaustoffen

Publications (2)

Publication Number Publication Date
WO2005092816A2 true WO2005092816A2 (fr) 2005-10-06
WO2005092816A3 WO2005092816A3 (fr) 2006-06-15

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EP (1) EP1725507A2 (fr)
CN (1) CN100497235C (fr)
DE (1) DE102004013468A1 (fr)
IN (1) IN2014CN04829A (fr)
WO (1) WO2005092816A2 (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006063729A1 (fr) * 2004-12-15 2006-06-22 Wacker Polymer Systems Gmbh & Co. Kg Procede de stabilisation de surfaces produisant de la poussiere
CZ307890B6 (cs) * 2018-03-22 2019-07-24 ÄŚeskĂ© vysokĂ© uÄŤenĂ­ technickĂ© v Praze Nepálená hlína s regulovaným smrštěním
CN116514471A (zh) * 2023-03-21 2023-08-01 上海隧港建筑材料有限公司 一种防冻抗裂混凝土

Families Citing this family (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CZ302139B6 (cs) * 2008-10-23 2010-11-10 Claylab S.R.O. Nepálená hlína stabilizovaná polymery
DE102008044395A1 (de) 2008-12-05 2010-06-10 Wacker Chemie Ag Dränbeton-Zusammensetzung
CA2741255C (fr) * 2010-06-15 2013-05-14 Dow Stade Producktions Gmbh & Co. Ohg Compositions de poudre de polymere redispersible preparees a partir de latex a base de styrene et de butadiene pour des formulations de melange sec
CN102070924B (zh) * 2010-12-19 2012-11-07 陈新云 木质防火门多功能饰面涂层
ITRE20110015A1 (it) * 2011-03-08 2012-09-09 Matteo Brioni S R L Composizione di un impasto per rivestimento di superfici
JP6034873B2 (ja) * 2011-10-28 2016-11-30 ダウ グローバル テクノロジーズ エルエルシー 再分散性ポリマー粉末の内部添加剤としてのポリウレタン粉末の使用
AT512883B1 (de) * 2012-04-18 2017-09-15 Edmund Kern Hubert Getrockneter, ungebrannter, diffusionsfähiger, wasserresistenter und frostresistenter, ökonomischer, ökologischer Mergel und/oder Ton und/oder Lehm und/oder Mischformen davon
WO2014052033A1 (fr) * 2012-09-28 2014-04-03 Rohm And Haas Company Mélanges de poudres de polymère redispersibles pour une utilisation dans des formulations de mélange à sec
WO2018148929A1 (fr) * 2017-02-17 2018-08-23 Wacker Chemie Ag Utilisation d'une dispersion aqueuse de polymère pour la liaison interfaciale entre des matériaux poreux polymères

Citations (2)

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Publication number Priority date Publication date Assignee Title
DE19921815A1 (de) * 1999-05-11 2000-11-16 Basf Ag Verwendung von polysulfidfreien Zubereitungen als Zusatz zu Baumaterialien auf Basis von Lehm oder Ton
EP1420033A1 (fr) * 2002-11-14 2004-05-19 Wacker Polymer Systems GmbH & Co. KG Dispersions aqueuses de polymères stabilisés par un colloide protecteur et poudres redispersables dans l'eau

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19921815A1 (de) * 1999-05-11 2000-11-16 Basf Ag Verwendung von polysulfidfreien Zubereitungen als Zusatz zu Baumaterialien auf Basis von Lehm oder Ton
EP1420033A1 (fr) * 2002-11-14 2004-05-19 Wacker Polymer Systems GmbH & Co. KG Dispersions aqueuses de polymères stabilisés par un colloide protecteur et poudres redispersables dans l'eau

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006063729A1 (fr) * 2004-12-15 2006-06-22 Wacker Polymer Systems Gmbh & Co. Kg Procede de stabilisation de surfaces produisant de la poussiere
US7288581B2 (en) 2004-12-15 2007-10-30 Wacker Polymer Systems Gmbh & Co. Kg Process for the stabilization of dusting surfaces
CZ307890B6 (cs) * 2018-03-22 2019-07-24 ÄŚeskĂ© vysokĂ© uÄŤenĂ­ technickĂ© v Praze Nepálená hlína s regulovaným smrštěním
CN116514471A (zh) * 2023-03-21 2023-08-01 上海隧港建筑材料有限公司 一种防冻抗裂混凝土
CN116514471B (zh) * 2023-03-21 2024-05-07 上海隧港建筑材料有限公司 一种防冻抗裂混凝土

Also Published As

Publication number Publication date
EP1725507A2 (fr) 2006-11-29
IN2014CN04829A (fr) 2015-09-18
DE102004013468A1 (de) 2005-10-13
CN1934051A (zh) 2007-03-21
CN100497235C (zh) 2009-06-10
WO2005092816A3 (fr) 2006-06-15

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