EP2619153A1 - A grout composition - Google Patents

A grout composition

Info

Publication number
EP2619153A1
EP2619153A1 EP11776853.1A EP11776853A EP2619153A1 EP 2619153 A1 EP2619153 A1 EP 2619153A1 EP 11776853 A EP11776853 A EP 11776853A EP 2619153 A1 EP2619153 A1 EP 2619153A1
Authority
EP
European Patent Office
Prior art keywords
quantities
present
composition
bond
grout
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Withdrawn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
EP11776853.1A
Other languages
German (de)
French (fr)
Inventor
Luigi Perrino
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.)
Sika Technology AG
Original Assignee
Sika Technology 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 Sika Technology AG filed Critical Sika Technology AG
Publication of EP2619153A1 publication Critical patent/EP2619153A1/en
Withdrawn legal-status Critical Current

Links

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
    • 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
    • C04B28/02—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 hydraulic cements other than calcium sulfates
    • C04B28/04—Portland cements
    • 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
    • C04B20/00—Use of materials as fillers for mortars, concrete or artificial stone according to more than one of groups C04B14/00 - C04B18/00 and characterised by shape or grain distribution; Treatment of materials according to more than one of the groups C04B14/00 - C04B18/00 specially adapted to enhance their filling properties in mortars, concrete or artificial stone; Expanding or defibrillating materials
    • C04B20/10—Coating or impregnating
    • C04B20/1055—Coating or impregnating with inorganic materials
    • C04B20/1066—Oxides, Hydroxides
    • 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
    • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
    • C04B2111/00474—Uses not provided for elsewhere in C04B2111/00
    • C04B2111/00637—Uses not provided for elsewhere in C04B2111/00 as glue or binder for uniting building or structural materials
    • 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
    • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
    • C04B2111/00474—Uses not provided for elsewhere in C04B2111/00
    • C04B2111/00663—Uses not provided for elsewhere in C04B2111/00 as filling material for cavities or the like
    • C04B2111/00672—Pointing or jointing materials
    • 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
    • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
    • C04B2111/00474—Uses not provided for elsewhere in C04B2111/00
    • C04B2111/00663—Uses not provided for elsewhere in C04B2111/00 as filling material for cavities or the like
    • C04B2111/00698—Uses not provided for elsewhere in C04B2111/00 as filling material for cavities or the like for cavity walls
    • 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
    • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
    • C04B2111/60—Flooring materials
    • 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
    • C04B2111/00—Mortars, concrete or artificial stone or mixtures to prepare them, characterised by specific function, property or use
    • C04B2111/70—Grouts, e.g. injection mixtures for cables for prestressed concrete

Definitions

  • the present invention relates to a grout composition, its use and the production process therefor.
  • the invention relates to a grout composition and use thereof for pointing purposes, especially for floorings and wall coverings made using ceramic slabs or tiles, natural stones or like products in substantially slab form.
  • the laying of ceramic slabs or tiles generally involves spreading, on the surface to be clad, a layer of mastic or other adhesive, and then applying the slabs or ceramic tiles on the layer.
  • the slabs or tiles are flanked to one another such as to realise a continuous covering.
  • the appearance of the finished cladding is therefore characterised by the presence of a plurality of slabs or ceramic tiles separated by a grid network of grout-filled spaces; the grout must therefore also exhibit aesthetic and functional characteristics which will last over time.
  • the lines filled with cement grout which remains porous to a certain extent and is therefore susceptible to some degree of water absorption, become home to microorganisms such as mould, bacteria or fungus, which cause unpleasant coloration and odours in the grout, as well as stains and even a deterioration in the actual grout.
  • An aim of the present invention is to obviate the above-cited drawback.
  • a further aim of the invention is to attain the objective in the ambit of a simple, rational and relatively inexpensive solution.
  • the invention makes available a grout composition comprising at least a bond and at least an inorganic anti-bacterial agent destined to be dispersed in the bond.
  • composition comprising a given substance X
  • composition comprising a given substance X
  • a composition comprising a given substance X
  • the antibacterial agent is therefore dispersed in the whole mass of the bond.
  • the action of the antibacterial agent is such as to inhibit the growth of bacteria, fungus or moulds; furthermore, as it is inorganic in nature, it does not wear away over time and maintains its antibacterial effect over the whole working duration of the grout.
  • the grout composition advantageously further comprises at least an inert material, for example exhibiting a granulometry comprised between 0.01 mm and 1 mm, which is also destined to be dispersed in the bond, with the aim of guaranteeing the grout qualities of high mechanical resistance to abrasion over time.
  • an inert material for example exhibiting a granulometry comprised between 0.01 mm and 1 mm, which is also destined to be dispersed in the bond, with the aim of guaranteeing the grout qualities of high mechanical resistance to abrasion over time.
  • the bond is selected from among hydraulic bonds, such as for example cement, hydraulic lime, aluminium cement, natural pozzolana materials, artificial pozzolana materials and the like;
  • the inert material is selected from among calcium carbonate, quartz and silicon sand or a mixture of the three above-named components.
  • the inorganic antibacterial agent is advantageously constituted by silver ions, preferably stabilised on glass support elements, or clay support elements or the like, known as carriers.
  • the silver ions are such as to inhibit growth of microorganisms, such as bacteria, mould and fungus, inasmuch as they bond to the cellular structure of the microorganisms such as to interact with the enzymatic synthesis.
  • microorganisms such as bacteria, mould and fungus
  • the silver ions intervene in the duplicating mechanism of the microorganisms' DNA, facilitating formation of species that are reactive to oxygen and which thus enable the grout to be kept clean.
  • the bond for example the cement, is preferably present in quantities comprised between 20% and 60%, the inert material is present in quantities of between 38% and 79.98%, while the silver ions are present in quantities of between 0.02% and 2%.
  • the grout composition advantageously further comprises a pozzolana additive in quantities comprised between 0% and 2%, which gives the compound better mechanical resistance and chromatic stability.
  • the pozzolana additive improves and contributes to the elimination of any efflorescence due to the presence of free lime in the cement constituting the bond.
  • the preferable pozzolana additives are microsilicates or amorphous silicates or metakaolins.
  • the grout composition of the invention further comprises a grip accelerator in quantities comprised between 0% and 1.5%.
  • the accelerator has the function of shortening grout drying times, once it has been laid.
  • Grip accelerators that can advantageously be used are aluminium sulphate or formiated lime.
  • the grout composition can comprise a fluidifier in quantities comprised between 0% and 0.5%, such as to reduce the water/bond ratio when it is prepared for laying, improving the mechanical resistance and the abrasive resistance.
  • the fluidifier can be an additive based on polycarboxylate ethers or melamine sulphonate.
  • composition of the invention can also comprise colorant pigments in quantities of between 0% and 5%,
  • the grout composition comprises titanium dioxides in quantities comprised between 0% and 3%, which improves the brilliancy and the chromatic effect of the grout.
  • composition of the invention further comprises a soluble copolymer in powder form in quantities comprised between 0% and 3%, which enables a reduction in water absorption of the grout after the grout has hardened, i.e. following laying.
  • the grout composition can further comprise cellulose ether in quantities comprised between 0 and 0.2% with the aim of improving the rheology of the grout, which translates into a greater applicability of the grout during the laying thereof, for example, in the spaces between the tiles.
  • composition of the invention can advantageously comprise a water- repellent in power form, in quantities comprised between 0% and 1 %, which enables a further reduction in the water absorption following hardening of the grout, once the grout has been laid.
  • Portland cement (white or grey) in class I 52.5 R present in quantities of 30%; quartz having a granulometry of between 0.1 and 0.3 mm and in a 40% quantity;
  • iron oxide pigment in a 0.5% quantity; titanium dioxide in a 1 % quantity;
  • silver ions stabilised on a carrier for example on glass supports, in a 0.15% quantity.
  • a further aspect of the present invention is the use of a grout composition as a space-filler in floors and wall coverings.
  • a no-less important aspect of the invention is a process for preparation of a composition of the invention, which comprises a stage of batching the weighted quantities, for example using scales, of the powders of the various above-listed components in accordance with, for example, the above- described recipe of the example.
  • the thus-batched powders are then loaded into a coulter or blade mixer for dry-mixing the powders.
  • the mixing can be performed for a few seconds; at the end of the mixing the composition is ready to be sent to a bagging machine such as to be packed in sacks.
  • the anti-bacterial grout it is sufficient to wet the grout with an appropriate quantity of water and mix it; when the paste thus-obtained has reached the desired consistency it is laid in such a way as to penetrate internally of the space to be filled, such as to fill it completely.
  • a rubber spatula or another tool of known type, can be used to lay the grout. Once the grout has been laid, when the grout starts to harden and grip, the spaces can be cleaned. For example a damp sponge can be wiped over the spaces such as to give the grout therein a substantially homogeneous conformation.

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Ceramic Engineering (AREA)
  • Inorganic Chemistry (AREA)
  • Materials Engineering (AREA)
  • Structural Engineering (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Curing Cements, Concrete, And Artificial Stone (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

A grout composition comprising at least a bond, a peculiarity of which consists in its comprising at least an inorganic antibacterial agent destined to be dissolved in the bond.

Description

A Grout Composition
TECHNICAL FIELD
The present invention relates to a grout composition, its use and the production process therefor.
In more detail, the invention relates to a grout composition and use thereof for pointing purposes, especially for floorings and wall coverings made using ceramic slabs or tiles, natural stones or like products in substantially slab form.
BACKGROUND ART
It is known to clad floors and/or walls of a building or the like by means of laying flooring panels. The most common solutions use ceramic slabs or tiles for the purpose.
The laying of ceramic slabs or tiles generally involves spreading, on the surface to be clad, a layer of mastic or other adhesive, and then applying the slabs or ceramic tiles on the layer. The slabs or tiles are flanked to one another such as to realise a continuous covering.
Although slabs or ceramic tiles are reciprocally laid adjacent to one another, they also remain separated from one another by spaces, of varying narrowness, sometimes known as fugues.
These spaces are subsequently filled using a special grout, for example a cement, which form a sort of grid-structure that remains visible when the cladding operation is complete.
The appearance of the finished cladding is therefore characterised by the presence of a plurality of slabs or ceramic tiles separated by a grid network of grout-filled spaces; the grout must therefore also exhibit aesthetic and functional characteristics which will last over time.
Often, however, the lines filled with cement grout, which remains porous to a certain extent and is therefore susceptible to some degree of water absorption, become home to microorganisms such as mould, bacteria or fungus, which cause unpleasant coloration and odours in the grout, as well as stains and even a deterioration in the actual grout.
DISCLOSURE OF INVENTION An aim of the present invention is to obviate the above-cited drawback.
A further aim of the invention is to attain the objective in the ambit of a simple, rational and relatively inexpensive solution.
These aims are attained by the characteristics of the invention as described in the independent claims. The dependent claims delineate preferred and/or especially advantageous aspects of the invention.
BEST MODE FOR CARRYNG OUT THE INVENTION
In particular, the invention makes available a grout composition comprising at least a bond and at least an inorganic anti-bacterial agent destined to be dispersed in the bond.
In the following, the terms "comprising" , "including" and "constituted", for example a composition "comprising" a given substance X, can mean that it is entirely constituted by the substance X or that it can include other additional substances, for example substance X plus Y.
The antibacterial agent is therefore dispersed in the whole mass of the bond. The action of the antibacterial agent is such as to inhibit the growth of bacteria, fungus or moulds; furthermore, as it is inorganic in nature, it does not wear away over time and maintains its antibacterial effect over the whole working duration of the grout.
The grout composition advantageously further comprises at least an inert material, for example exhibiting a granulometry comprised between 0.01 mm and 1 mm, which is also destined to be dispersed in the bond, with the aim of guaranteeing the grout qualities of high mechanical resistance to abrasion over time.
In a preferred embodiment, the bond is selected from among hydraulic bonds, such as for example cement, hydraulic lime, aluminium cement, natural pozzolana materials, artificial pozzolana materials and the like; the inert material is selected from among calcium carbonate, quartz and silicon sand or a mixture of the three above-named components.
The inorganic antibacterial agent is advantageously constituted by silver ions, preferably stabilised on glass support elements, or clay support elements or the like, known as carriers. The silver ions, as mentioned, are such as to inhibit growth of microorganisms, such as bacteria, mould and fungus, inasmuch as they bond to the cellular structure of the microorganisms such as to interact with the enzymatic synthesis. In substance, by preventing the energy production of the enzymes, the growth of the microorganisms is inhibited, and the microorganisms cannot reproduce.
Furthermore, the silver ions intervene in the duplicating mechanism of the microorganisms' DNA, facilitating formation of species that are reactive to oxygen and which thus enable the grout to be kept clean.
The bond, for example the cement, is preferably present in quantities comprised between 20% and 60%, the inert material is present in quantities of between 38% and 79.98%, while the silver ions are present in quantities of between 0.02% and 2%.
All the indicated values are percentages (%) in weight, in reference to the total weight of the composition.
The grout composition advantageously further comprises a pozzolana additive in quantities comprised between 0% and 2%, which gives the compound better mechanical resistance and chromatic stability.
Further, the pozzolana additive improves and contributes to the elimination of any efflorescence due to the presence of free lime in the cement constituting the bond.
The preferable pozzolana additives are microsilicates or amorphous silicates or metakaolins.
The grout composition of the invention further comprises a grip accelerator in quantities comprised between 0% and 1.5%.
The accelerator has the function of shortening grout drying times, once it has been laid.
Grip accelerators that can advantageously be used are aluminium sulphate or formiated lime.
Further, the grout composition can comprise a fluidifier in quantities comprised between 0% and 0.5%, such as to reduce the water/bond ratio when it is prepared for laying, improving the mechanical resistance and the abrasive resistance.
The fluidifier can be an additive based on polycarboxylate ethers or melamine sulphonate.
The composition of the invention can also comprise colorant pigments in quantities of between 0% and 5%,
Additionally, the grout composition comprises titanium dioxides in quantities comprised between 0% and 3%, which improves the brilliancy and the chromatic effect of the grout.
The composition of the invention further comprises a soluble copolymer in powder form in quantities comprised between 0% and 3%, which enables a reduction in water absorption of the grout after the grout has hardened, i.e. following laying.
The grout composition can further comprise cellulose ether in quantities comprised between 0 and 0.2% with the aim of improving the rheology of the grout, which translates into a greater applicability of the grout during the laying thereof, for example, in the spaces between the tiles.
The composition of the invention can advantageously comprise a water- repellent in power form, in quantities comprised between 0% and 1 %, which enables a further reduction in the water absorption following hardening of the grout, once the grout has been laid.
Example
An example of a cement malt is prepared starting with the following composition:
Portland cement (white or grey) in class I 52.5 R present in quantities of 30%; quartz having a granulometry of between 0.1 and 0.3 mm and in a 40% quantity;
calcium carbonate having a granulometry of 40 m and in a 25.5% quantity; amorphous silicon in a 1 % quantity;
calcium formiate in a 1 % quantity;
melamine sulphonate in a 0.1 % quantity;
iron oxide pigment in a 0.5% quantity; titanium dioxide in a 1 % quantity;
a powder resin based on vinyl acetate/ethylene copolymer in a 0.5% quantity; hydroxyethyl cellulose in a 0.03% quantity;
silane in a 0.2% quantity;
silver ions stabilised on a carrier, for example on glass supports, in a 0.15% quantity.
A further aspect of the present invention is the use of a grout composition as a space-filler in floors and wall coverings.
A no-less important aspect of the invention is a process for preparation of a composition of the invention, which comprises a stage of batching the weighted quantities, for example using scales, of the powders of the various above-listed components in accordance with, for example, the above- described recipe of the example.
The thus-batched powders are then loaded into a coulter or blade mixer for dry-mixing the powders.
The mixing can be performed for a few seconds; at the end of the mixing the composition is ready to be sent to a bagging machine such as to be packed in sacks.
To lay the anti-bacterial grout, it is sufficient to wet the grout with an appropriate quantity of water and mix it; when the paste thus-obtained has reached the desired consistency it is laid in such a way as to penetrate internally of the space to be filled, such as to fill it completely.
A rubber spatula, or another tool of known type, can be used to lay the grout. Once the grout has been laid, when the grout starts to harden and grip, the spaces can be cleaned. For example a damp sponge can be wiped over the spaces such as to give the grout therein a substantially homogeneous conformation.
Finally the grout is left to dry and any residues thereof on the ceramic tiles or slabs removed.
After just a few hours the silver ions will already be performing their antibacterial action, as mentioned herein above. The invention is not limited to the above-described examples, and variants and improvements may be brought thereto without its forsaking the ambit of the following claims.

Claims

Claims
1 ) . A grout composition for pointing, comprising at least a hydraulic bond comprising portland cement in quatities comprised between 20% and 60%, at least an aggregate material, suitable for being dispersed in the bond in quantities comprised between 38% and 79.98%, at least an inorganic antibacterial agent destined to be dissolved in the bond, a pozzolanic additive in a quantity of not above 2%, characterised in that the antibacterial agent comprises silver ions stabilised on support elements made of glass or clay and in quantities comprised between 0.02% and 2% (all the percentages are in weight in reference to a total weight of the composition).
2) . The composition of claim 1 , wherein the inert material is selected from among calcium carbonate, quartz and silicate sand.
3) . The composition of claim 1 , characterised in that it further comprises: a grip accelerator in quantities of not more than 1.5%;
a fluidifier in quantities of not more than 0.5%;
colorant pigments in quantities of not more than 5%;
titanium dioxide in quantities of not more than 3%;
a copolymer, dispersible in powder, in quantities of not more than 3%;
cellulose ether in quantities of not more than 0.2%;
a water-repellent in powder form, in quantities of not more than 1 %;
(all the percentages are expressed in weight comparison to a total of the composition).
4) . The composition of claim 3, wherein
the bond is Portland cement present in quantities of 30%;
the inert materials comprise quartz having a granulometry of between 0.1 and 0.3 mm in a 40% quantity and calcium carbonate having a granulometry of 40 μητι and in a 25.5% quantity;
the pozzolanic additive is amorphous silicon present in a 1 % quantity;
the grip accelerator is calcium formiate present in a 1 % quantity;
the fluidifier is melamine sulphonate present in a 0.1% quantity;
the colorant pigments are iron oxide pigments present in a 0.5% quantity; the titanium dioxide is present in a 1 % quantity;
the dispersible copolymer is a powder resin based on vinyl acetate/ethylene copolymer, present in a 0.5% quantity;
the cellulose ether is hydroxyethyl cellulose present in a 0.03% quantity;
the water-repellent is silane, present in a 0.2% quantity;
the silver ions are stabilised on carriers, for example on support elements, present in a 0.15% quantity;
(all the percentages are expressed in weight comparison to a total of the composition).
EP11776853.1A 2010-09-23 2011-09-22 A grout composition Withdrawn EP2619153A1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
ITRE2010A000074A IT1402120B1 (en) 2010-09-23 2010-09-23 COMPOSITION OF MALTA.
PCT/IB2011/002198 WO2012038810A1 (en) 2010-09-23 2011-09-22 A grout composition

Publications (1)

Publication Number Publication Date
EP2619153A1 true EP2619153A1 (en) 2013-07-31

Family

ID=43739076

Family Applications (1)

Application Number Title Priority Date Filing Date
EP11776853.1A Withdrawn EP2619153A1 (en) 2010-09-23 2011-09-22 A grout composition

Country Status (3)

Country Link
EP (1) EP2619153A1 (en)
IT (1) IT1402120B1 (en)
WO (1) WO2012038810A1 (en)

Cited By (1)

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CN113135681A (en) * 2021-03-16 2021-07-20 华中科技大学 Permeable inorganic antibacterial solution and preparation method thereof

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CN104876491A (en) * 2015-05-22 2015-09-02 营口象圆新材料工程技术有限公司 Mortar used for phenolic foam insulation board construction
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113135681A (en) * 2021-03-16 2021-07-20 华中科技大学 Permeable inorganic antibacterial solution and preparation method thereof
CN113135681B (en) * 2021-03-16 2022-06-28 华中科技大学 A kind of permeable inorganic antibacterial solution and preparation method thereof

Also Published As

Publication number Publication date
IT1402120B1 (en) 2013-08-28
WO2012038810A1 (en) 2012-03-29
ITRE20100074A1 (en) 2012-03-24

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