AU2013251277A1 - Process for the preparation of pigment granules and the use thereof - Google Patents
Process for the preparation of pigment granules and the use thereof Download PDFInfo
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Abstract
The present invention relates to pigment granules and to a process for the preparation thereof and their use.
Description
H:\kxg\lnteroven\NRPortbl\DCC\KXG\5787394_l.doc-I/l 1/2013 - la This is a divisional of Australian Patent Application No. 2007201363, the entire contents of which are incorporated herein by reference. The present invention relates to pigment granules and a process for the preparation thereof and 5 their use. The processing of pigment granules requires milling of the pigments to give primary particles in order to achieve the optimum colour impression. The powders formed thereby produce a very large amount of dust and, owing to their finely divided nature, tend to adhere and stick in metering 10 units. In the case of toxicologically hazardous substances, it is therefore necessary during processing to take measures for avoiding danger to man and environment from dusts which form. However, even in the case of safe inert substances, such as, for example, iron oxide pigments, avoidance of dust pollution is increasingly being desired by the market. 15 Dust avoidance and improved metering based on good flow properties for achieving a qualitatively uniform colour impression on use in building materials and organic media is therefore the aim when handling pigments. This aim is achieved more or less by applying granulation processes to pigments. For example, pelletizing or spray granulation are used. In recent years, however, it has also been possible for briquetted and press granules increasingly to become established on the 20 market. These granules are now very successful commercially. In the case of pigments, the market requires in principle two conflicting properties when pigment granules are used: mechanical stability of the granule and good dispersing properties in the medium used. The mechanical stability is responsible both for good transport properties during transport 25 between manufacturer and user and for good metering and flow properties during the use of the pigments. It is produced by strong adhesive forces and depends, for example, on the amount of binder or on the pressure during moulding by pressing. On the other hand, the dispersibility is influenced by thorough milling prior to granulation (wet and dry milling), by the mechanical energy during incorporation (shear forces) and by dispersants which immediately reduce the 30 adhesive forces in the dry granules during incorporation into a medium. In the case of pigments, however, the use of larger amounts of dispersants is limited to owing to the auxiliary/pigment cost ratio. Moreover, a high proportion of auxiliaries results in a corresponding reduction in the colour strength or scattering power. Since the colour strength variations are generally ±5 %, for example when colouring building materials, the use of additives is also limited even if they simultaneously 35 act as adhesion promoters and dispersants. Furthermore, the additives must not change the performance characteristics of the end products, such as, for example, building materials, plastics and finishes, in a disadvantageous manner, for example the compressive strength or the setting behaviour in the case of concrete, -2 the compressive strength or abrasion resistance in the case of asphalt and the strength or the notched impact strength in the case of plastics, the elastic properties in the case of elastomers (polymers) and the rheological properties in the case of paints and finishes. According to the prior art, for example, spray granulation (spray drying by means of a disc or 5 nozzle) by the cocurrent or countercurrent method and pelletizing (mixer, fluidized-bed granulator, disc or drum) or compacting processes are suitable as production processes for pigment granules. Granulation by spray drying starts from pigment suspensions with the use of binders. Appropriate processes are described in various patents. Water-soluble binders are 10 predominantly used. Thus, organic substances, such as, for example, ligninsulphonates, formaldehyde condensates, gluconic acids and sulphated polyglycol ethers, are used as starting materials in DE 3 619 363 Al, EP 0 268 645 Al and EP 0 365 046 Al, while inorganic salts, such as, for example, silicate and phosphate, are used as staring materials according to DE 3 918 694 Al and US 5,215,583 Al. A combination of spray granulation and pelletizing 15 has also been described in EP 0 507 046 Al. In DE 3 619 363 Al and EP 0 268 645 Al, the use of a compacting process is excluded. EP 0 257 423 Al and DE 3 841 848 A l describe spray granulation with the use of polyorganosiloxanes as hydrophobic, lipophilic additives. The atomization drier mentioned generally leads to particle sizes which are too small and a large fine fraction. This means that a 20 substantial proportion of the material from the drier is not obtained as directly usable granules but is first retained in the filter as a fine fraction and then has to be recycled to the process. The hydrophobing aftertreatment leads in the case of spray-granulated products to granules which are very free-flowing but produce an extremely large amount of dust. EP 0 424 896 Al discloses the preparation of low-dust fine granules in a production run in 25 known intensive mixers. A low content of waxes in combination with emulsifier and wetting agents is used here by applying an aqueous dispersion. In general, water contents of 20 to more than 50% are obtained. These granules must first be dried and separated from oversize and undersize. DE 31 32 303 Al describes low-dust, flowable inorganic pigment granules which are mixed 30 with binders becoming liquid under the action of heat (40 to 60'C) and are granulated by a screen process with the use of a screening aid (pressure). About 10 to 20% of the throughput are obtained as a fine fraction of< 0. 1 mm.
-3 EP 0 144 940 Al discloses low-dust pigment granules which, starting from filter slurry, are mixed at 50 to 200'C with about 50% of water by addition of 0.5-10% of surface-active substances and additionally mineral oil or waxes which become liquid, up to the smear point. The process takes place in intensive mixers, and possibly subsequent granulation and 5 subsequent drying are also effected. Water is present in the end product in an amount of 10 to 15%, which is disadvantageous for incorporation into plastics. Other processes, too, are limited in their application. Owing to drop formation, spray granulation requires the use of readily flowable, i.e. low-viscosity, suspensions. For the drying process, it is therefore necessary to evaporate a larger amount of water than in the case of the 10 frequently usable fluidized-bed drying from highly pressed-out pigment filter pastes. This leads to higher energy costs. In the case of pigments prepared beforehand by calcination, spray granulation means an additional process step with high energy costs. Moreover, a larger or smaller proportion of fine material is obtained in the dust filter during the spray granulation which has to be recycled to the production. 15 DE 28 44 710 Al describes the granulation of pigments in a fluidized bed "uith granulating auxiliaries, dry pigment powder being sprayed with water Pelletizing frequently also has disadvantages. Starting from pigment powder, it can be carried out in mixers with high turbulence, by the fluidized bed process or by disc and drum granulation. Common to all these processes is that the binder requirement, generally water, is 20 high so that drying has to follow as an additional process step. Here too, granules of different sizes are obtained, particularly if insufficient binder is available for the amount of powder or the actual distribution is not optimum. A certain proportion of granules may then be too large, while on the other hand excessively small and therefore still dusting fractions are present. Classification of the granules formed with recycling of oversize and undersize is therefore 25 required. Disc granulation leads to a broad particle size spectrum of granules. Where this is undesirable owing to the poor dispersibility of particles which are too large, the granulation process has to be monitored by intensive monitoring by personnel and granule production has to be optimized by manual control of the amount of nuclei. Here too, classification with recycling of the 30 oversize and undersize is usually effected. DE 42 14 195 Al discloses a process for colouring asphalt with inorganic pigment granules, in which oils are used as binders. This is a simple granulation process.
-4 DE 196 38 042 Al and DE 196 49 756 Al describe inorganic pigment granules obtained from dry pigments, for example finished material, by mixing with one or more auxiliaries, compacting and further subsequent steps, such as comminution, screening and recycling of coarse and/or fine material. In the compacting step, compacting is effected with nip forces of 5 0.1 to 50 kN/cm. The granules obtained can be surrounded by an additional layer which serves for increasing the stability or as an aid in processing. In DE 4 336 613 Al and DE 4 336 612 Al describe inorganic pigment granules obtained from dry pigments, for example finished material, by mixing with binders, compacting and further subsequent steps, such as crushing on a screen granulator and subsequent pelletizing on a 10 rotating disc or in a rotating drum. In the compacting step, compacting is effected with nip forces of 0.1 to 15 kN/cm. The granules prepared according to the teaching of DE 196 38 042 Al, DE 196 49 756 Al, DE 4 336 613 Al and DE 4 336 612 Al contain only the auxiliary or the auxiliaries which were added in the first process step to the pigment powder. Even if the granule particles are 15 surrounded by an additional layer, they contain in their interior only the auxiliary or the auxiliaries which were added to the pigment powder in the first process step. The granule particles are composed in their interior of a homogeneous mixture of pigment and auxiliary or auxiliaries. However, it is known that auxiliaries which lead to very good dispersibility in an application medium on improvement of the product properties may be far less effective in 20 another application medium, and in certain circumstances even incompatibility may be observed. Thus, for example, strongly hydrophobic auxiliaries may be advantageous in the case of incorporation into plastics or asphalt, while they lead to difficulties in the case of incorporation into aqueous emulsion paints or in the preparation of aqueous slurries, since the granules are only very poorly wetted with water. For this reason, the granules prepared 25 according to the teaching of DE 19 649 756 Al, DE 4 336 613 Al and DE 4 336 612 Al are not simultaneously equally suitable for all application media. During the preparation, it would therefore have been necessary to add a plurality of auxiliaries which permit as good a processability as possible in all application media. This is not very expedient from the economic point of view and moreover the multiplicity of different additives may result in 30 mutual incompatibilities. If granules are prepared from pigment mixtures according to the teaching of DE 19 649 756 Al, DE 4 336 613 Al or DE 4 336 612 Al, a further disadvantage of these granulation processes is found. It is first necessary to prepare a mixture of the different pigments, which is then mixed with binders and other auxiliaries and further processed. It was therefore an object of the present invention to provide a process which avoids the -5 disadvantages described to date of compacting granulation when applied to inorganic or organic pigments and provides sufficiently stable, meterable, low-dust granules having good dispersibility in different application media. This object was achieved by pigment granules which consist of a pressed or briquetted core 5 and at least one outer layer applied by granulation, a) the core containing at least one organic or inorganic pigment or mixtures thereof and at least one auxiliary and b) the outer layer applied by granulation or the outer layers applied by granulation containing at least one - optionally pressed or briquetted - organic or inorganic pigment 10 or mixtures thereof and the outer layer applied by granulation or the outer layers applied by granulation containing in each case at least one auxiliary and c) in the outer layer applied by granulation or the outer layers applied by granulation, 1) at least one organic or inorganic pigment other than that in the pressed or briquetted core being present or 15 2) at least one auxiliary other than that in the pressed or briquetted core being present or 3) at least one organic or inorganic pigment other than that in the pressed or briquetted core being present and at least one auxiliary other than that in the pressed or briquetted core being present or 20 4) the identical organic or inorganic pigment or the identical organic or inorganic pigments being present with auxiliaries identical to those in the pressed or briquetted core, at least one of the pigments in at least one outer layer applied by granulation then, however, not being pressed and not being briquetted. In this way, it is possible to improve the pressed and briquetted granules and substantially to 25 optimize the preparation process since, independently of the subsequent application medium, a uniform pressed or briquetted core fraction can always be used. This uniform core fraction can be filled into suitable containers and temporarily stored or transported to another location where the subsequent further processing takes place. In the further processing, at least one outer layer comprising at least one pigment powder is applied by granulation to the uniform 30 core fraction in a further process step. The pigment powder comprising the core fraction and -6 that comprising the outer layer applied by granulation need not necessarily be identical. This is advantageous particularly in the preparation of granules from pigment mixtures since it is possible to dispense with the prior mixing of the individual pigments. Thus, various orange shades can be prepared, for example, by mixing iron oxide red and iron oxide yellow pigments 5 or various green shades can be prepared by mixing iron oxide yellow and phthalocyanine blue pigments. For the preparation of iron oxide orange granules, it is therefore possible either to apply an iron oxide red pigment as an outer layer to a compacted iron oxide yellow pigment (core fraction) by addition of said iron oxide red pigment by granulation or to apply an iron oxide yellow pigment as an outer layer to a compacted iron oxide red pigment (core fraction) 10 by addition of said iron oxide yellow pigment by granulation. Fig. 1 illustrates this principle. It shows the optical micrograph of iron oxide orange granules in which an iron oxide red pigment was applied as an outer layer (designated as "B" in Fig. 1) to a compacted and subsequently rolled iron oxide yellow pigment (core fraction - designated as "A" in Fig. 1) by granulation. For the preparation of the optical micrograph, the granule particles were cast in a resin and 15 ground. What is important in the case of the multistage process according to the invention is that, in the first step, a sufficiently cohesive homogeneous material is produced by addition of the auxiliary or of the auxiliaries to one or more organic or inorganic pigment powders. As a rule, mixers are used for this purpose but in individual cases it may also be advantageous to use a 20 mill. In the second step, pressing or briquetting once or several times is then effected. The core fraction is produced by a commninution step, such as, for example, screen granulation, and is optionally isolated by a separation step and can be rounded or coated. A separation step for isolating the core fraction is, however, not absolutely essential since the powder obtained in the comminution step can also be applied directly to the core fraction by granulation. The 25 substantial process step in the process according to the invention is subsequent rolling with addition of one or more organic or inorganic pigments or pigment mixtures, the pigment or the pigments or pigment mixtures being mixed with one or more auxiliaries before or during the addition so that at least one outer layer is also applied by granulation. The application of the outer layer(s) by granulation can be effected in a fluidized bed or in a fluid bed. The auxiliary 30 or auxiliaries used should permit as good processibility as possible 'in the respective application medium. A further advantage of the process according to the invention is, inter alia, that it is possible to start from dried and possibly milled pigment powder. This is particularly economical especially when the pigment is prepared by a dry synthesis - such as, for example, the 35 preparation of iron oxide red by calcination of iron oxide black or yellow. In spray granulation, -7 for example, further preparation of a slurry and thereafter an additional drying step are required. Moreover, removal of the water used for preparing the slurry by evaporation is very energy-consuming. Inorganic pigments used are preferably iron oxide, titanium dioxide, chromium oxide, zinc 5 oxide and rutile mixed-phase pigments and carbon black (carbon pigments). Organic pigments used are preferably azo, quinacridone, phthalocyanine and perylene pigments and indigoids. Inorganic pigments are preferably used. However, it is also possible to use fillers. Both inorganic and organic substances may be used as auxiliaries. Water, salts from the group consisting of the phosphates, phosphonates, carbonates, 10 sulphates, sulphonates, silicates, aluminates, borates, titanates, formates, oxalates, citrates, tartrates, stearates, acetates, polysaccharides, cellulose derivatives, such as, preferably, cellulose ethers or cellulose esters, phosphonocarboxylic acids, modified silanes, silicone oils, oils from biological cultivation (preferably rapeseed oil, soya bean oil, maize oil, olive oil, coconut oil, sunflower oil), refined paraffinic and/or naphthenic mineral oils, synthetically 15 prepared oils, alkylphenols, glycols, polyethers, polyglycols, polyglycol derivatives, ethylene oxide-propylene oxide copolymers, protein/fatty acid condensates, alkyl benzenesulphonates, alkyl naphthalenesulphonates, ligninsulphonates, sulphated polyglycol ethers, melamine/formaldehyde condensates, naphthalene/formaldehyde condensates, gluconic acid, polyacrylates, polycarboxylate ethers, polyhydroxy compounds, polyhydroxyamino 20 compounds or solutions or mixtures or suspensions or emulsions thereof are preferably used as auxiliaries. In the context of this invention, emulsifiers, wetting agents and dispersants are also considered to be auxiliaries. Preferably emulsifiers having HLB values of 7 to 40, in particular of 7 to 18, are suitable as 25 emulsifiers for use in building materials comprising aqueous systems, such as, for example, concrete, containing alkyl or acrylic radicals and hydrophilic intermediate and end groups, such as, for example, amides, amines, ether, hydroxyl, carboxylate, sulphate, sulphonate, phosphate, phosphonate, amine salt, polyether, polyamide or polyphosphate. The substances can be used individually or in combination, depending on their HLB value. 30 Preferably, alkyl benzenesulphonates, fatty alcohol sulphates, fatty alcohol ether sulphates, fatty alcohol ethoxylate, alkylphenol ethoxylate, branched and/or straight-chain alkane- or olefin-sulphonates, branched and/or straight-chain alkane- or olefin-sulphates and -8 sulphosuccinates are suitable as wetting agents. Preferably, ligninsulphonates, melaminesulphonates, naphthalenesulphonates, soaps, metal soaps, polyvinyl alcohols, polyvinyl sulphates, polyacrylamides, polyacrylates, polycarboxylate ethers, medium- and long-chain alkanesulphates or -sulphonates or 5 -sulphosuccinates and medium- and long-chain alkanephosphates or -phosphonates are used as dispersants. The auxiliaries can preferably be used in combination with further additives, such as, for example, antifoams, retention aids or fragrances. Preservatives in a concentration of 0.01 to 1% by weight, based on the weight of the pigment 10 granules, may also be added to the pigment granules, preferably during mixing. Formaldehyde eliminating compounds, phenolic compounds or isothiazolinone preparations may be mentioned as examples. The pigment granules preferably contain auxiliaries in a total amount of 0.001 to 10% by weight, particularly preferably of 0.01 to 5% by weight, very particularly preferably of 0.1 to 15 5% by weight, based on the total amount of the pigments. The pressed or briquetted core according to a) and the outer layer applied by granulation or the outer layers applied by granulation according to b) and c) preferably contain in each case an inorganic or in each case an organic pigment. The pressed or briquetted core according to a) and the outer layer applied by granulation or the 20 outer layers applied by granulation according to b) and c) preferably contain the same pigment, but at least one of the outer layers applied by granulation contains an auxiliary which differs in amount or type from that in the pressed or briquetted core according to a). The pressed or briquetted core according to a) and the outer layer applied by granulation or the outer layers applied by granulation according to b) and c) preferably contain the same pigment, 25 the pigment in at least one of the outer layers applied by granulation not being pressed and not being bniquetted. The pressed or bniquetted core according to a) and the outer layer applied by granulation or the outer layers applied by granulation according to b) and c) preferably contain in each case a plurality of inorganic pigments and/or in each case a plurality of organic pigments. 30 The pressed or bnquetted core according to a) and the outer layer applied by granulation or the -9 outer layers applied by granulation according to b) and c) preferably contain the same organic or inorganic pigments but at least one auxiliary which differs in amount or type from the core. The pressed or briquetted core according to a) and the outer layer applied by granulation or the outer layers applied by granulation according to b) and c) preferably contain the same 5 organic and/or inorganic pigments, the pigment in at least one of the outer layers applied by granulation not being pressed and not being briquetted. The pigment or the pigments which forms or form the outer layer applied by granulation according to b) and c) is or are preferably altogether not more than four times the weight, preferably not more than the same weight, based on the weight of the pressed or briquetted 10 core according to a). The pressed or briquetted core according to a) preferably contains auxiliaries other than those in the outer layer applied by granulation according to b) and c). The pressed or briquetted core according to a) is preferably coated once or several times with one or more auxiliaries. 15 The outer layer applied by granulation or the outer layers applied by granulation according to b) and c) are preferably in each case coated once or several times with one or more auxiliaries. Only the outermost of the outer layers applied by granulation according to b) and c) is preferably coated once or several times with one or more auxiliaries. 20 The inorganic pigment granules preferably have a bulk density in the range of 0.3 to 4.0 g/cm 3 , preferably in the range of 0.5 to 2.0 g/cm 3 , the pigment granules which contain carbon black or organic pigments preferably having a bulk density in the range of 0.1 to 2.5 g/cm 3 . Preferably at least 85% of the pigment granules have a particle size in the range of 80 to 25 3000 jm, preferably in the range of 100 to 1500 pm. The pigment granules preferably have a residual water content of less than 4% by weight, preferably less than 2% by weight. In the context of this invention, residual water is understood as meaning the residual moisture. The pigment granules preferably additionally contain preservatives, antifoams, retention 30 aids, antisettling agents and/or fragrances.
- 10 The invention also relates to a process for the preparation of pigment granules, characterized in that a) one or more organic or inorganic pigments are mixed with one or more auxiliaries, b) this mixture is subjected to at least one pressing or briquetting step in order to obtain 5 scabs, c) these scabs are comminuted in at least one step to give nuclei and powder, dl) the nuclei are separated from the powder in that the fraction greater than 80 ym, preferably greater than 100 ym, serves as a core fraction and optionally (i) is subjected to a rounding step and/or 10 (ii) is coated with one or more auxiliaries, it being possible for step dl)(ii) also to take place before dl)(i) or it being possible for both steps to take place simultaneously, and the product obtained remaining in the production process while the other fraction is removed from the process or recycled, or 15 d2) the nuclei serve as a core fraction and the powder formed on comminution is applied completely to this core fraction by granulation by subsequent rolling, optionally one or more auxiliaries being added and it being possible for the product obtained and completely applied by granulation to be coated with one or more auxiliaries, e) and at least one outer layer being applied by granulation by subsequent rolling to the 20 product obtained with addition of one or more organic or inorganic pigments or mixtures thereof, (i) the organic or inorganic pigment or pigments or mixtures having been mixed beforehand with one or more auxiliaries and/or (ii) one or more auxiliaries being added during the subsequent rolling and/or 25 (iii) the organic or inorganic pigment or pigments or the mixture of organic or inorganic pigments and at least one auxiliary having been subjected beforehand to one or more pressing or briquetting steps, - I1 in order to obtain subsequently rolled granules and f) the granules subsequently rolled in this manner are optionally coated once or several times with auxiliaries. During pressing or briquetting (compacting, step b)), an important characteristic is the pressing 5 force (kN) per cm of roll width (nip force). During compacting between rolls, linear transmission of the pressing force is assumed since a pressing area cannot be defined and a pressure (kN/cm 2 ) therefore cannot be calculated. The pressing or briquetting step b) is preferably effected by means of a roll press or matrix press and at nip forces of 0.1 to 50 kN/cm, preferably of 0.1 to 20 kN/cm. 10 If a plurality of pressing or briquetting steps is effected, identical or different nip forces can be used. The use of different nip forces is particularly advantageous, for example, when the organic and/or inorganic pigments have a very low bulk density so that precompaction is effected in a first pressing or briquetting step. Preferably, a plurality of pressing or briquetting steps b) is effected directly in succession, 15 identical or different pressing or briquetting units being used and the pressing or briquetting steps being carried out at identical or different nip forces in the range of 0.1 to 50 kN/cm, preferably of 0.1 to 20 kN/cm. The compacting is preferably effected at low nip forces. The nip forces used are generally preferably in the bottom range of the commercially available apparatuses. Commercially 20 available apparatuses are, for example, the Pharmapaktor 200/50 from Bepex GmbH, Leingarten, Germany. The comminution in step c) can be effected by means of all commercially available comminution units, such as crushers, toothed rolls, rolls having friction apparatuses or screen granulators or screen-type mills, in which the material is pressed through a sieve (so-called 25 coarse grinder). The rotors, as are generally known, revolve or oscillate at a circumferential velocity of 0.05 m/sec to 10 m/sec, preferably 0.3 to 5 rn/sec. The distance between rotor and screen or perforated disc is 0.1 to 15 mm, preferably 0.1 to 5 mm, particularly preferably 1 to 2 mm. The comminution in step c) is preferably effected by means of a sieve as a comminution unit 30 having a mesh size of 0.5 to 4 mm, preferably of 1 to 2 mm.
- 12 Under certain circumstances, it is advantageous to carry out the comminution step c) several times in succession. For this purpose, a plurality of screen granulators or screen-type mills preferably with different mesh sizes of the sieve - can be connected in series. Preferably, a plurality of comminution steps c) by means of a sieve is effected directly in 5 succession, different mesh sizes of the sieve being used and, in the last comminution step, a sieve having a mesh size of 0.5 to 4 mm, preferably of 1 to 2 mm, being used. If a plurality of comminution steps c) is carried out directly in succession, different comminution units can also be combined with one another. Thus, for example, before the use of a screen granulator or a screen-type mill, a coarse cominution of the scabs by means of 10 roll or jaw crushers can first be effected. Inter alia, the particle size distribution of the comminuted product can be influenced thereby. Preferably, a plurality of comminution steps c) is effected directly in succession, different comminution units being used. Before the comminution in step c), the scabs from b) are preferably separated into two fractions, the coarse fraction in which at least 85 % of the particles are greater than 500 pm, 15 preferably greater than 600 pm, being fed to step c) and being comminuted in one or more steps and the fine fraction being fed to step dl) in order to be separated again into two or more fractions in step dl), separately from or together with the nuclei and the powder from step c), and to form the core fraction. The nuclei and powder of the comminuted product from step c) are preferably separated into 20 two fractions in step dl), the fine fraction smaller than 80 pm, preferably smaller than 100 pm, very particularly preferably smaller than 250 pm, being removed or recycled to the process and the coarse fraction greater than 80 pm, preferably greater than 100 pm, very particularly preferably greater than 250 pm, serving as a core fraction which is further converted in the process. 25 The nuclei and powder of the comminuted product from step c) are preferably separated into three fractions in step dl), the fine fraction and the coarse fraction being removed or recycled and the medium fraction in the range of 80 to 2000 pm, preferably in the range of 100 to 1500 pm, very particularly preferably in the range of 250 to 1000 pm, serving as a core fraction which is further converted in the process and optionally subjected to a rounding step and/or 30 additionally coated. The rounding step dl)(i) is preferably effected on a rotating disc (pelletizing disc), in a coating drum or in a rotating drum (pelletizing drum), in a screen unit or in a fluidized bed or in a fluid bed. Here, the dust fraction can be removed by suction or discharged in the fluidized bed with the air. The dust fraction can be recycled to the process - 13 at another point. After the comminution in step c), the removal of the fine fraction can also be omitted (step d2)). Instead, the nuclei formed in comminution step c) serve as a core fraction onto which the powder formed in the comminution step is completely applied by granulation by subsequent 5 rolling. The subsequent rolling step under d2) is preferably effected on a rotating disc (pelletizing disc), in a coating drum or in a rotating drum (pelletizing drum). Optionally, coating with one or more auxiliaries can also be effected thereafter. Before step e), the core fraction from step dl) is preferably separated into two fractions, the fine fraction or the coarse fraction being removed or recycled and the fraction in the range of 10 80 to 2000 pm, preferably in the range of 100 to 1500 jpm, being fed to step e). Before step e), the core fraction from step dl) is preferably separated into three fractions, the fine fraction and the coarse fraction being removed or recycled and the medium fraction in the range of 80 to 2000 pm, preferably in the range of 100 to 1500 Im, being fed to step e). In the subsequent pelletizing step e), one or more organic or inorganic pigments or mixtures of 15 organic and/or inorganic pigments, which were mixed beforehand with one or more auxiliaries, are added to the product obtained from the process steps described above and are applied by granulation by subsequent rolling. The subsequent rolling under e) is preferably effected on a rotating disc (pelletizing disc), in a coating drum or in a rotating drum (pelletizing drum). The auxiliary or auxiliaries used are chosen so that they permit good processability in the desired 20 application medium. The auxiliary or auxiliaries used in process step e) therefore need not necessarily be identical to the auxiliary or auxiliaries which was or were added in process step a). The same applies to the organic or inorganic pigment(s). In process step e), it may be entirely advantageous to use a pigment or pigments or a pigment mixture which is or are different to that of those in process step a). If a plurality of pigments is used in process step e), 25 it is unimportant whether they are added in succession or whether a mixture was prepared beforehand from the pigments and this mixture is added in step e). It is also unimportant whether a pigment mixture which contains one or more auxiliaries is prepared by first preparing the pigment mixture and then mixing this with one or more auxiliaries or by first mixing one or more pigments with one or more auxiliaries and finally mixing the pigments 30 already mixed with auxiliary or auxiliaries. Preferably, the organic and/or inorganic pigment(s) added in step e) is or are altogether not more than four times the weight, preferably not more than the same weight, based on the weight of the core fraction used in step e).
- 14 The organic and/or inorganic pigment(s) used in step e) is or are preferably different from the organic and/or inorganic pigment(s) which was or were used in process step a). In step e), an organic or an inorganic pigment is preferably added. In step e), preferably a plurality or organic and/or inorganic pigments are added in succession. 5 In step e), in particular a plurality of organic and/or inorganic pigments is added, these having been mixed with one another beforehand. The organic and/or inorganic pigment(s) used in step e) is or are preferably mixed beforehand individually or as a mixture with one or more auxiliaries. The granules obtained after step e) are separated, preferably before step f), into two fractions, 10 and only the fraction in which the particles are greater than 80 pm, preferably greater than 250 im, is fed to step f), while the fine fraction is removed from the process or recycled. The granules obtained after step e) are separated, preferably before step f), into three fractions, and only the fraction in which at least 85% of the particles are greater than 80 ym, preferably greater than 100 ym, or are in the range of 80 to 3000 ym, preferably in the range of 15 100 to 1500 im, is fed to step f), while the other fractions are removed from the process or recycled. One or more drying steps are preferably additionally effected. General description of the preparation process Mixing of the organic or inorganic pigment(s) with one or more auxiliaries, which is described 20 in step a), can be effected in conventional mixers. The number of units and unit types is known to the person skilled in the art. In individual cases, it may be advantageous also to use a mill for the mixing process. The same applies to the preparation of the mixture of pigment(s) and auxiliary or auxiliaries which is used in process step e). Before the comminution in step c), the scabs from b) can preferably be separated into two 25 fractions (intermediate step x) in order subsequently for the coarse fraction in which at least 85% of the particles are greater than 500 ym, preferably 600 Am, to be fed to step c) and to be comminuted in one or more steps, and the fine fraction is fed to step dl) in order to be separated again in step dl), separately from or together with the nuclei and the powder from step c), into two or more fractions and to form the core fraction.
- 15 Preferably, only the coarse fraction from intermediate step x) is comminuted in step c) while the fine fraction from intermediate step x) is separated into two or more fractions in step dl). The intermediate step x) can preferably be effected by classification or screening (mechanical separation). Screens, such as, for example, drum screens, oscillating screens and vibrating 5 screens, are preferably used. The nuclei and the powder of the comminuted product are preferably separated in d1) into two fractions, the fractions smaller than 80 pm, preferably smaller than 100 pim, very particularly preferably smaller than 250 pm, being removed or recycled to the process and the fraction greater than 80 pm, preferably greater than 100 pm, very particularly preferably greater than 10 250 jtm, serving as core fraction. The amount of the fine fraction is preferably 10 to 50% by weight, particularly preferably 10 to 30% by weight. The fine fraction is removed from the process and can be recycled to the process at another point. The fraction remaining in the process serves as a core fraction and is optionally rounded in a further step dl)(i) and/or coated with one or more auxiliaries in step dl)(ii). 15 The nuclei and the powder of the comminuted product are particularly preferably separated in step dl) into three fractions, the fine fraction and the coarse fraction being removed from the process or recycled to the process and the medium fraction in the range of 80 to 2000 im, particularly preferably in the range of 100 to 1500 pm, very particularly preferably in the range of 250 to 1000 pim serving as core fraction. The amount of the fine and coarse fraction is 20 preferably 10 to 50% by weight, particularly preferably 10 to 30% by weight. The fine and coarse fraction is removed from the process and can be recycled to the process at another point. The fraction remaining in the process serves as a core fraction and is optionally rounded in a further step dl)(i) and/or coated with one or more auxiliaries in step d1)(ii). The rounding step under dl) can be carried out with removal of the dust fraction. The rounding 25 step dl)(i) can be effected on a rotating disc (pelletizing disc), in a coating drum or in a rotating drum (pelletizing drum), in a screen unit or in a fluidized bed or in a fluid bed. Here, the dust fraction can be removed by suction or discharged in the fluidized bed with the air. The dust fraction can be recycled to the process at another point. Particularly preferably, the nuclei of the comminuted product from step c) serve, without 30 separation into a plurality of fractions in step d2), as the core fraction and the powder of the comminuted product from step c) is completely applied to the core fraction by granulation by subsequent rolling, one or more auxiliaries optionally being added and it being possible for the completely granulated product obtained to be coated with one or more auxiliaries.
- 16 The subsequent rolling and complete granulation of the comminuted product in step d2) are preferably carried out on a rotating disc (pelletizing disc) or in a coating drum or in a rotating drum (pelletizing drum). Before process step e), it may be advantageous to carry out a further intermediate step y) in 5 which a desired particle size fraction is separated from the product stream. Preferably, only the fraction in the range of 80 to 2000 jim, very particularly preferably in the range of 100 to 1500 jim, is fed to process step e) while the fine and/or coarse fraction are removed from the process or recycled to the process. The intermediate step y) may be advantageous when the comminuted product from step c) was fed to step d2). 10 Before step e), the core fraction from step dl) is preferably separated into two fractions, the fine fraction or the coarse fraction being removed or recycled and the fraction in the range of 80 to 2000 pm, in particular in the range of 100 to 1500 pm, being fed to step e). Before step e), the core fraction from dl) is preferably separated into three fractions, the fine fraction and the coarse fraction being removed or recycled and the medium fraction in the 15 range of 80 to 2000 pm, in particular in the range of 100 to 1500 pm, being fed to step e). The intermediate step y) can preferably be effected by classification or screening (mechanical separation). Screens, such as, for example, drum screens, oscillating screens and/or vibrating screens, are preferably used. The subsequent rolling in step e) is preferably effected on a rotating disc (pelletizing disc) or in 20 a coating drum or in a rotating drum (pelletizing drum). The organic or inorganic pigment(s) used in process step e) needs or need not be identical to the organic or inorganic pigment(s) described under step a). In the preparation of mixed colours, the choice of different pigments is even particularly advantageous. The granules obtained after step e) can preferably also be coated in step f) once or several 25 times with one or more auxiliaries. The coating of the pigment granules serves for increasing the stability or as an aid in processing. This layer can be produced by application of inorganic salts in solution, of polyols or waxes of polyethers, polycarboxylates, polycarboxylate ethers or cellulose derivatives, preferably carboxymethylcellulose. 30 After process step e), it may be advantageous to carry out a further intermediate step z) in - 17 which a desired particle size fraction is separated from the granules obtained. Preferably, the fraction greater than 80 4m, preferably greater than 100 pm, or the fraction in the range of 80 to 3000 urn, preferably in the range of 100 to 2500 pm, or particularly preferably in the range of 250 to 1500 ulm, is separated off and is fed to step f). Oversize and/or undersize can be 5 removed from the process or recycled. Optionally, it may be advantageous to carry out the intermediate step z) also after step 0. The granules obtained after step e) are preferably separated before step f) into two fractions and only the fraction in which the particles are greater than 80 plm, particularly greater than 250 pm, is fed to step f) while the fine fraction is removed from the process or recycled. 10 The granules obtained after step e) are preferably separated before step f) into three fractions and only the fraction in which at least 85% of the particles are greater than 80 jam, and particularly greater than 100 pim, or are in the range of 80 to 3000 jam, in particular in the range of 100 to 1500 prm, is fed to step 0 while the other fractions are removed from the process or recycled. 15 The intermediate step z) can preferably be effected by classification or screening (mechanical separation). Screens, such as, for example, drum screens, oscillating screens and/or vibrating screens, are preferably used. The recycling of oversize and/or of undersize separated off to the process can be effected at various points. It is dependent, inter alia, on which auxiliaries were added, whether one or 20 more pigments are used for the total process and whether mixing of the auxiliaries or pigments via the recycling of oversize and undersize is desired or not. However, the person skilled in the art will without doubt recognize that process step in the process according to the invention which is ideal for this application and in which recycling of the oversize and/or undersize separated off is particularly advantageous. When recycling the oversize, it may be 25 advantageous if it is comminuted after being separated off and before being recycled. The process according to the invention can be applied not only to inorganic and/or organic pigments but also to fillers. The invention also relates to the use of the pigment granules for colouring building materials, such as concrete, cement mortar, renders and asphalt, and for colouring organic 30 media, such as finishes, plastics and colour pastes, and for the preparation of emulsion paints and slurries.
- 18 The pigment granules are preferably mixed with the building materials in an amount of 0.1 to 10% by weight, based on cement, or, in the case of asphalt, based on the total mixed material. The pigment granules are preferably first suspended in water and then mixed with the 5 building materials. The pigment granules are preferably mixed with the organic media. The organic media are preferably plastics. The plastics are preferably thermoplastics, thernosetting plastics and/or elastomers. The pigment granules are preferably mixed with liquid plastics. 10 The organic media are preferably polymers having rubber-elastic properties. The organic media are preferably powder coating materials. The pigment granules are preferably mixed with the emulsion paints. The subject of the present invention arises not only out of the subject of the individual patent claims but also out of the combination of the individual patent claims with one 15 another. The same applies to all parameters disclosed in the description and any desired combinations thereof. The invention is explained in more detail with reference to the following examples, without there being any intention to limit the invention thereby.
- 19 I. Description of the methods of measurement used A. Determination of the dispersibility for building materials The determination of the dispersibility for building materials is effected in cement mortar by colonmetric measurement of prisms produced using white cement and having the following 5 data: Cement-quartz sand ratio 1:4, water-cement value 0.35, level of pigmentation 1.2%, based on cement, mixer used from RK Toni Technik, Berlin, with 5 1 mixing bowl, design 155 1, speed 140 rpm, batch 500 g of cement. After a mixing time of 40 s, 55 s, 70 s, 85 s and 100 s, samples of (300 g) of the mixture are 10 taken in each case and test specimens (5 x 10 x 2.5 cm) are produced therefrom under pressure (pressing force 114 kN for 2 seconds). Hardness of the test specimens: 24 hours at 30'C and 95% relative humidity with subsequent drying for 4 hours at 60*C. Colorimeter measurement via Dataflash* 2000 Datacolor International, 4 measuring points per stone. The mean values obtained are compared with the values of a reference sample. The colour difference AEab* and 15 the colour strength (reference sample = 100%) (DIN 5033, DIN 6174) are assessed. In the context of this application, the following colorimetric abbreviations and calculations are used, as known from the CIELAB system: * a* corresponds to the red-green axis with Aa* = a* (sample) - a* (reference) * b* corresponds to the yellow-blue axis with Ab* = b* (sample) - b* (reference) 20 0 L* corresponds to the lightness with AL* = L* (sample) - L* (reference). " A Eab* corresponds to the colour difference, where (AE3b*) 2 = (AL) + (Aa*) 2 + (Ab*) 2 , i.e. AEab* =[ (AL) 2 + (Aa*) 2 + (Ab*) 2 ]A, For the relative colour strength in %, the following equations apply: (K/S)sample Relative colour strength in % (K/S)rerence 100 25 - 20 (1 -p*)2 K/S = 2 -p* Y/100 - ro P 1 - ro - r 2 (0 - Y/100) where ro = 0.04 and r 2 = 0.6 and Y is the tristimulus value (lightness). The calculation is effected on the basis of DIN 53234. 5 The dispersibility is designated as good at a colour difference up to 5% relative to the reference sample and a colour difference AEab* of not more than 1.5 units. B. Determination of the dispersibility for asphalt The determination of the dispersibility in asphalt was effected according to the following method: the pigment powder or pigment granules is or are mixed in a heatable laboratory 10 mixer (Rego mixer) together with a road construction bitumen of the type B 80 (commercial product from Shell AG) and additives for 60 seconds at 180 0 C. Test specimens are produced with the mixture according to Marshall ("The Shell Bitumen Handbook, Shell Bitumen U.K., 1990, pages 230-232). Differences in the shade of the Marshall bodies compared with a predetermined comparative sample of pigment powder are assessed colonmetrically by 15 comparison of the red values a* (Minolta Chromameter II, standard illuminant C, CIELAB System, DIN 5033, DIN 6174). Differences in the a* values of less than 0.5 unit are not visibly distinguishable. C. Determination of the dispersibility for plastics The determination of the dispersibility in plastics is effected on the basis of DIN EN 13900-2: 20 Pigment and fillers - dispersing methods and assessment of the dispersibility in plastics, part 2, Determination of the colouristic properties and ease of dispersion in plasticizer-containing polyvinyl chloride (PVC-P) moulding material by two-roll milling. The pigment or pigment granules to be tested is or are dispersed at 160 ± 5'C in the form of a lightened mixture comprising pigments and a titanium dioxide white pigment powder (Tronox* R-FK-2; Tronox* 25 R-FK-2 is a commercial product of Tronox Incorporated) in the weight ratio = 1:5 on a mixing roll mill in PVC. The mill hide obtained is divided and one half is then subjected to high shear forces by rolling at room temperature. The ease of dispersion DHpvc.,, which indicates the -21 percentage increase in the colour strength after rolling at room temperature, is a measure of the dispersibility in the case of coloured pigments. The colour strength of the cold-rolled PVC hide is fixed at 100% as a reference and is determined according to the abovementioned formulae. The ease of dispersion DHPVC-P is then calculated according to (F 5 DH Pvc-P = 100 * cold-rolled sample _ Fhot-rolled sample ) Here, Fhot 0 led sample is the colour strength value of the hot-rolled test specimen and Fcold.rolled sample is accordingly the colour strength value of the cold-rolled test specimen. The abovementioned formulae are applicable for the calculation of the colour strength, ro being 0.05325 and r 2 being 0.65 in the case of testing in plastics. 10 In the determination of the dispersibility in plastics, the colour difference AEab* between hot and cold-rolled PVC hide is additionally determined. For the calculation of AL*, Aa*, Ab* the formulae mentioned above and known from the C[ELAB system are applicable. Here, cold rolled PVC hide also serves as reference. A readily dispersible pigment or pigment granules is or are already completed dispersed at low shear forces, whereas higher shear forces are 15 necessary to aid rolling at low temperature for completely dispersing a pigment which is difficult to disperse. The following is therefore applicable: the greater the ease of dispersion and the smaller the colour difference AEab*, the more readily is the pigment dispersible. Particularly in the case of granules the dispersibility is very important since the granule particles first have to be broken up and are then dispersible in a plastic. This dispersibility of 20 coloured pigments or granulated coloured pigments is designated as good at an ease of dispersion of not more than 10% and at a colour difference AEab* of not more 1.5 units in the test method described above. D. Determination of the dispersibility of emulsion paints The dispersibility of coloured pigments in emulsion paints is determined by means of 25 dissolvers. The test medium is an emulsion paint based on a PVA dispersion (vinyl acetate/vinyl versatate) having a pigment volume concentration of 55% (pigment/filler ratio 40/60). Following incorporation of the pigment, 180 g of white emulsion paint are initially introduced and then 6.0 g of the coloured pigment to be tested are sprinkled in with stirring (Tronox* R-KB-2/coloured pigment weight ratio = 5:1; Tronox* R-KB-2 is a commercial 30 product of Tronox Incorporated). The following dispersing conditions are established using a dissolver disc (diameter 4 cm): - 22 10 min 1000 rpm (2.1 m/s) 20 min 2000 rpm (4.2 m/s) 10 min 4500 rpm (9.4 m/s) After the individual dispersing times, coats having a wet film thickness of 150 p.im (gap height 5 of the coating knife) are prepared and are dried at room temperature. After the drying, the coats (coating films) are peeled off using a sharp-edged object, with the result that the undispersed pigment particles appear as dots or stripes (specks) at the surface. The dispersing energy to be applied to the granules is assessed using a rating scale from level 1 to 5: Level 1: no specks 10 Level 2: a few specks Level 3: moderate number of specks Level 4: many specks Level 5: very many specks Good dispersibility is present only at the rating levels I and 2; from level 3, the rating for the 15 dispersing energy applied is insufficient. E. Determination of the self-plasticization of slurries In the preparation of slurries, 300 g of water are initially introduced and the pigment powder or pigment granules to be tested is or are introduced at room temperature without further additions of additives ("self-plasticization") with stirring by means of a dissolver disc having a 20 diameter of 3.5 cm at about 1500 rpm until a suspension having a solids content of 70% by weight is achieved. If a viscosity value of more than 1000 mPa-s is obtained for this starting slurry with a Brookfield viscosimeter with the use of the Brookfield measuring spindle no. 4 and at a speed of 100 rpm, the solids content is reduced in steps of 5% by weight by adding water until a viscosity value of less than 1000 mPa-s is established. If, on the contrary, the 25 starting slurry having a solids content of 70% by weight has a very low viscosity, its solids content is increased in steps of 5% by weight by adding pigment powder or pigment granules until the maximum solids content which still permits a viscosity value of less than 1000 mPa-s is achieved. During use in practice, the slurries having a viscosity up to 1000 mPa-s are considered to be capable of being handled (pumpable and meterable) without problems. 24 -23 hours after preparation of the slurry, the viscosity is measured again with the Brookfield viscosimeter with the use of spindle no. 4 and at a speed of 100 rpm. An increase in the viscosity to above 1000 mPa-s is undesired. In the preparation of slurries from pigment particles or pigment granules, as high a solids content as possible in combination with as low a 5 viscosity as possible is desirable. Pigment granules are therefore all the more suitable for the preparation of slurries ("self-plasticization") if the slurry prepared has as low a viscosity as possible at as high a solids content as possible. F. Determination of the determination of the flow behaviour The flow behaviour of the pigment granules is determined by measuring the efflux time 10 through a funnel of 100 ml volume having a 6 mm orifice, on the basis of ASTM test to D 1200-88. The present invention is explained in more detail below with reference to examples without these examples constituting a limitation. The granules from Examples 1, 3 and 5 were prepared by processes which correspond to the prior art and serve as a comparison. 15 II. Comparative Example 1 50 kg of iron oxide red Bayferrox* 160 (commercial product from Lanxess Deutschland GmbH) were mixed with 1.5% of polypropylene glycol (average molecular weight about 2000) in a mixer for 15 minutes. The mixture was pressed on a 200/50 compactor (from Bepex, Leingarten) at around 15 kN (3 kN/cm) and then comminuted on a crusher (from Frewitt, 20 Fribourg, Switzerland) having a screen of 1.25 mm mesh size. The comminuted product was screened over a screen having a mesh size of 250 pm. The oversize fraction was about 77%. For testing in the various media, in each case the fraction from 315 ptm to 1250 Ptm was used (Comparative Example 1). The results of the investigation of the granules from Comparative Example I are summarized 25 in Table 1. III. Example 2 The Bayferrox* 160 described above was mixed with the following auxiliaries for 15 minutes in a mixer: I. 1.5% of polypropylene glycol (average molecular weight about 2000) -24 U. 3.0% Texapon* 842 (Texapon* 842 is an aqueous solution of sodium octylsulphate containing around 30% of active substance, commercial product from Cognis Deutschland GmbH & Co. KG) M. 3.0% of a 30% strength aqueous polyethylene glycol solution (average molecular 5 weight about 20 000) IV. 2.0% of a 45% strength aqueous solution of ammonium ligninsulphonate In each case 1.0 kg of the fraction from Example 1 screened over 250 im was introduced into a granulating pan having a diameter of 70 cm and an inclination of 530 and was rolled for about 3 minutes at 34 rpm. In each case 0.5 kg of the 10 a) abovementioned mixture I. b) abovementioned mixture F. c) abovementioned mixture M. d) abovementioned mixture IV. was introduced in the course of about 3 minutes uniformly into the rotating granulating pan, 15 and the total sample was then further rolled for another 4 minutes (Examples 2a to 2d). For testing in the various media, in each case the fraction from 315 Pm to 1250 Pm was used in order always to compare the same particle sizes with one another. The results of the investigation of the granules from Examples 2a to 2d are summarized in Table 1. 20 Table 1 shows that Comparative Example I and Example 2a behave very similarly in all performance characteristics tested. Thus, no significant improvement in the formed characteristics is detectable as a result of the straightforward application by granulation of an outer layer which contains an additive identical to that in the compacted core. The granules from Examples 2b to 2d on the other hand show substantial advantages over 25 Comparative Example 1 and Example 2a) in at least one performance characteristic. Thus, the sample from Example 2b is substantially better dispersible in building materials: a final colour strength of 99%, based on the powder used, is reached after only 55 s. The granules from Comparative Example 1 give a colour strength of 96% only after a mixing time of 85 s, and the -25 granules from Example 2a) show a mere colour strength of 94% after a mixing time of 85 s. On incorporation into emulsion paint or in the preparation of slurries, the sample from Example 2b shows no substantial differences from Comparative Example 1 and Example 2a. The dispersibility in asphalt meets the requirements. 5 In the case of self-plasticization, the granules from Example 2c permit a 5% higher solids content than Comparative Example I and Example 2a. With regard to their dispersibility in building materials, the granules from Example 2d are comparable with those from Example 2b and are thus rated better than Comparative Example 1. However, on incorporation into a slurry, the granules from Example 2d additionally permit a 10 very high solids content of 75% in combination with a very low viscosity. IV. Comparative Example 3 50 kg of iron oxide red Bayferrox* 110 (commercial product from Lanxess Deutschland GmbH) were mixed with 1.0% of Walocel* CRT 30 P (commercial product from Wolff Cellulosics GmbH & Co. KG) in a mixer for 15 minutes and then homogenized by means of a 15 Bauermeister mill having a 1 mm screen insert. The homogenized product was pressed on a 200/50 compacter at about 5 kN (1 kN/cm) and then comminuted on a crusher having a screen of 1.25 mm mesh size. The comminuted product was screened over a screen having a mesh size of 250 tim. The oversize fraction was about 87%. For testing in the various media, in each case the fraction from 315 pm to 1250 im was used (Comparative Example 3a). 20 A part of the comminuted product from Comparative Example 3a were introduced, without prior screening, into a granulating pan having a diameter of 70 cm and an inclination of 53* and was rolled discontinuously for about 10 minutes at about 35 rpm. The rolled material was screened over a screen having a mesh size of 250 pm. The oversize fraction was about 94%. For testing in the various media, once again the fraction from 315 jIm to 1250 Im was used in 25 order always to compare the same particle sizes with one another (Comparative Example 3b). The results of the investigation of the granules from Comparative Examples 3a and 3b are summarized in Table 1. V. Example 4 The Bayferrox* 110 powder used in Example 3 was mixed in a mixer with the following 30 additives in the course of 15 minutes: -26 I. 5.0% of a 20% strength aqueous solution of a partly hydrolysed polyvinyl alcohol having a low molecular weight II. 3.0% of an about 35% strength aqueous solution of a polycarboxylate ether II. 3.0% of an about 30% strength aqueous solution of a polyacrylate 5 In each case 1.0 kg of the screened material (fraction > 250 prm) from Comparative Example 3a was then introduced into a granulating pan having a diameter of 70 cm and an inclination of 530 and was rolled for about 3 minutes at about 34 rpm. In each case 0.5 kg of the a) abovementioned mixture I. b) abovementioned mixture [I. 10 c) abovementioned mixture III. was introduced uniformly in the course of about 3 minutes into the rotating granulating pan and then the total sample was further rolled for another minutes (Examples 4a to 4c). For testing in the various media, in each case the fraction from 315 jim to 1250 ptm was used in order always to compare the same particle sizes with one another. 15 The results of the investigation of the granules from Examples 4a to 4c are summarized in Table 1. Table 1 shows that Comparative Examples 3a and 3b are disadvantageous in all performance characteristics tested, with the exception of the dispersibility in plastics. The dispersibility in building materials is insufficient since, even after a mixing time of 100 s, only final colours 20 strength of 91% and 88%, respectively, result, therefore the granules are not yet completely dispersed. Thus, no significant improvements in the performance characteristics are found as a result of the straightforward application by granulation of an outer layer which consists of compacted fine fraction and contains an additive identical to that in the compacted core. The granules from Comparative Example 3a also show unsatisfactory behaviour in the self 25 plasticization. A slurry prepared with a solids content of 60% has a relatively low viscosity but thickens to a very great extent in the course of a day and finally, with a viscosity > 1700 mPa-s, can no longer be handled. The granules from Examples 4a to 4c on the other hand show substantial advantages over the comparative examples in at least one performance characteristic. Thus, the granules from -27 Example 4a are substantially better dispersible in building materials: a final colour strength of 97%, based on the powder used, is achieved even after a mixing time of 70 s. However, the granules from Example 4a are not suitable for the preparation of a slurry. On the other hand, the granules from Examples 4b and 4c show different behaviour. On 5 incorporation into building materials, they achieve a colour strength of only 90% and 91%, respectively, after a mixing time of 100 s and are therefore identical to the two comparative examples, the granules from Examples 4b and 4c are very suitable for self-plasticization. With the granules from Example 4b, it is possible to prepare a suspension having a solids content of 60%, which can also be used without problems after storage for one day, and granules from 10 Example 4c even permit a solids content of 65%. VI. Comparative Example 5 For the preparation of an iron oxide orange mixture, Bayferrox* 920 and Bayferrox* 110 are mixed in a weight ratio of 3:2 in a mixer. 1.5% of a 45% strength aqueous solution of polyethylene glycol (average molecular weight about 4000) are added to this mixture in a 15 mixer and mixed for a further 15 minutes. The mixture was pressed on a 200/50 compacter at about 16 kN (3 kN/cm) and then comminuted on a crusher having a screen of 1.5 mm mesh size. The comminuted product was introduced in 1.0 kg portions into a granulating pan having a diameter of 70 cm and an inclination of 530 and rolled at about 35 rpm until the fine fraction had been completely applied by granulation. 20 For testing the various media, once again the fraction from 315 Pm to 1250 jIm was used in order always to compare the same particle sizes with one another (Comparative Example 5). The orange starting mixture described above, before addition of the polyethylene glycol solution, served in the investigation of the dispersibility in building materials as a reference for the colour strength. The results of the investigation of the granules from Comparative Example 25 5 are summarized in Table 2. VI. Example 6 1.5% of a 45% strength aqueous solution of polyethylene glycol (average molecular weight about 4000) were added to 20 kg of iron oxide yellow Bayferrox* 920 from Example 5 in a mixer and mixed for 15 minutes. The mixture was pressed on a 200/50 compacter (from 30 Bepex, Leingarten) at about 16 kN (3 kN/cm) and then comminuted on a crusher (from Frewitt, Fribourg, Switzerland) having a screen of 1.5 mm mesh size. The comminuted product - 28 was screened over a screen having a mesh size 250 ptm. The Bayferrox* 110 powder used for Example 5 was mixed in a mixer with the following auxiliaries for 15 minutes: I. 4.0% of a 25% strength solution of sodium caprylate (solvent water:ethanol 1:1) 5 II. 3.0% of an about 30% strength aqueous solution of a polyacrylate M. 3.0% of an about 30% strength aqueous polyethylene glycol solution (average molecular weight about 20 000) In each case 0.6 kg of the abovementioned compacted, comminuted and screened Bayferrox* 920 granules was introduced into a granulating pan having a diameter of 70 cm and an 10 inclination of 53' and rolled at about 34 rpm. Thereafter, in each case 0.4 kg of the a) abovementioned mixture I. b) abovementioned mixture H. c) abovementioned mixture III. was introduced uniformly in the course of about 3 minutes into the rotating granulating pan by 15 forcing the powder through a screen of 0.5 mm mesh size (Examples 6a to 6c). For testing in the various media, in each case the fraction from 315 pm to 1250 pm was used. The results of the investigation of the granules from Examples 6a to 6c are summarized in Table 2. The granules from Comparative Example 5 cannot be satisfactorily dispersed in building 20 materials. Even after a mixing time of 100 s, a colour strength of only 80%, based on the orange starting mixture used, is obtained. The granules from Examples 6a to 6c on the other hand show substantially improved dispersibility. Vfii. Example 7 The following powder mixtures were prepared in a mixer: 25 I. the Bayferrox* 920 powder used in Example 6 for the preparation of the pressed core, with 3.0% of an about 35% strength aqueous solution of a polycarboxylate -29 ether U. a 9:1 mixture of the Bayferrox* 920 powder used in Example 6 for the preparation of the pressed core and a phthalocyanine blue pigment (Bayplast* Blue, commercial product from Lanxess Deutschland GmbH) with 3.0% of a 5 45% strength aqueous polyethylene glycol solution (average molecular weight about 4000). The amount stated in each case below for the compacted, comminuted and screened Bayferrox@ 920 granules described in Example 6 was introduced into a granulating pan having a diameter of 70 cm and an inclination of 530 and rolled at about 34 rpm. Thereafter, in each 10 case the amount stated below of the abovementioned mixture I. or H. was introduced uniformly in the course of about 3 minutes into the rotating granulating pan by forcing the powder or the powder mixtures through a screen of 0.5 mm mesh size. a) 0.6 kg of the compacted, comminuted and screened Bayferrox* 920 granules and 0.4 kg of the mixture I. 15 b) 0.8 kg of the compacted, comminuted and screened Bayferrox* 920 granules and 0.2 kg of the mixture H. c) 0.6 kg of the compacted, comminuted and screened Bayferrox* 920 granules and 0.4 kg of the mixture 11. For testing the various media, in each case the fraction from 315 prm to 1250 im was used. 20 The results of the investigation of the granules from Examples 7a to 7c are summarized in Table 3.
- 30 0 C0 v, 0 0 0 0 C 0 00 ( A COD - ~00 00 \ 0 O 0 nC 00 V) C) 0 0 CO0 U, '0 a Ca 0 C..> C) ._ _ _ _ _ _ _ _ _ _ _ 7- -E. C0 ~ - - 5 CC cu CIO~ CL -/ CL .- - 0 C CD c5 6. cC, CsC ON 00C% C ~ 0C7,. 00 - C; 0 5 6 6 6 : Om mu ca m0 m 03N ' N N ( x0 k u u -31 Table 2 Residual Efflux time Dispersibility in building material moisture Is] 1%I Colour strength [%] / Colour difference mixing time [s]; AEab*; Reference: Reference: Starting starting power mixture Comparative n.d. 44 80 / 100 3.2 Example 5 Example 6a 0.1 44 96/85 1.0 Example 6b 0.1 36 97 / 70 0.9 Example 6c 0.1 39 99 / 85 1.0 Table 3 Residual Efflux Dispersibility in plastic - Self-plasticization moisture time [%] [s} Ease of AEab*; Solids Viscosity Viscosity dispersion Reference: content after after one HDpvc-p cold-rolled [%] preparation day [%] PVC hide [mPa-s] [mPa.s] Example 7a 1.3 42 n.d. n.d. 30 870 840 Example 7b 0.9 42 2 0.5 n.d. n.d. n.d. Example 7c 0.9 36 3 0.7 n.d. n.d. n.d. 5 "n.d." in Tables I to 3 denotes "not determined". Fig. I shows an optical micrograph of iron oxide orange granules in which a compacted iron oxide yellow pigment serves as the core fraction (designated "A" in Fig. 1) on which an iron oxide red pigment (designated as "B" in Fig. 1) was applied as an outer layer by granulation. The granule particles are embedded in a resin and ground.
- 32 Throughout this specification and the claims which follow, unless the context requires otherwise, the word "comprise", and variations such as "comprises" or "comprising", will be understood to imply the inclusion of a stated integer or step or group of integers or steps but not the exclusion of any other integer or step or group of integers or steps. The reference in this specification to any prior publication (or information derived from it), or to any matter which is known, is not, and should not be taken as an acknowledgment or admission or any form of suggestion that that prior publication (or information derived from it) or known matter forms part of the common general knowledge in the field of endeavour to which this specification relates.
Claims (53)
1. Pigment granules, characterized in that they consist of a pressed or briquetted core and at least one outer layer applied by granulation, a) the core containing at least one organic or inorganic pigment or mixtures thereof 5 and at least one auxiliary and b) the outer layer applied by granulation or the outer layers applied by granulation containing at least one - optionally pressed or briquetted - organic or inorganic pigment or mixtures thereof and the outer layer applied by granulation or the outer layers applied by granulation containing in each case at least one auxiliary 10 and c) in the outer layer applied by granulation or the outer layers applied by granulation, 1) at least one organic or inorganic pigment other than that in the pressed or briquetted core being present or 15 2) at least one auxiliary other than that in the pressed or briquetted core being present or 3) at least one organic or inorganic pigment other than that in the pressed or briquetted core being present and at least one auxiliary other than that in the pressed or briquetted core being present or 20 4) the identical organic or inorganic pigment or the identical organic or inorganic pigments being present with auxiliaries identical to those in the pressed or briquetted core, at least one of the pigments in at least one outer layer applied by granulation then, however, not being pressed and not being briquetted. 25
2. Pigment granules according to Claim 1, characterized in that iron oxide, titanium dioxide, chromium oxide, zinc oxide, rutile mixed-phase pigments and carbon black (carbon pigments) are used as inorganic pigments.
3. Pigment granules according to Claim 1, characterized in that azo, quinacridone, phthalocyanine and perylene pigments and indigoids are used as organic pigments. - 34
4. Pigment granules according to one or more of Claims I to 3, characterized in that water, salts from the group consisting of the phosphates, phosphonates, carbonates, sulphates, sulphonates, silicates, aluminates, borates, titanates, formates, oxalates, citrates, tartrates, stearates, acetates, polysaccharides, cellulose derivatives, such as, in 5 particular cellulose ethers or cellulose esters, phosphonocarboxylic acids, modified silanes, silicone oils, oils from biological cultivation (in particular rapeseed oil, soybean oil, maize oil, olive oil, coconut oil, sunflower oil), refined paraffinic and/or naphthenic mineral oils, synthetically prepared oils, alkylphenols, glycols, polyethers, polyglycols, polyglycol derivatives, ethylene oxide-propylene oxide copolymers, protein/fatty acid 10 condensates, alkyl benzenesulphonates, alkyl naphthalenesulphonates, ligninsulphonates, sulphated polyglycol ethers, melamine/formaldehyde condensates, naphthalene/formaldehyde condensates, gluconic acid, polyacrylates, polycarboxylate ethers, polyhydroxy compounds, polyhydroxyamino compounds or solutions or mixtures or suspensions or emulsion thereof are used as auxiliaries. 15
5. Pigment granules according to one or more of Claims I to 4, characterized in that the pigment granules contain auxiliaries in a total amount of 0.001 to 10% by weight, in particular of 0.1 to 5% by weight, based on the total amount of the pigments.
6. Pigment granules according to one or more of Claims I to 5, characterized in that the pigment or pigments which forms or form the outer layer applied by granulation 20 according to b) and c) is or are altogether not more than four times the weight, in particular not more than the same weight, based on the weight of the pressed or briquetted core.
7. Pigment granules according to one or more of Claims I to 6, characterized in that the pressed or briquetted core according to a) and the outer layer applied by granulation or 25 the outer layers applied by granulation according to b) and c) contain in each case an inorganic or in each case an organic pigment.
8. Pigment granules according to Claim 7, characterized in that the pressed or briquetted core according to a) and the outer layer applied by granulation or the outer layers applied by granulation according to b) and c) contain the same pigment, but an auxiliary 30 differing in amount or type from the pressed or briquetted core according to a) is present in at least one of the outer layers applied by granulation.
9. Pigment granules according to Claim 7, characterized in that the pressed or briquetted core according to a) and the outer layer applied by granulation or the outer layers - 35 applied by granulation according to b) and c) contain the same pigment, the pigment in at least one of the outer layers applied by granulation not being pressed and not being bniquetted.
10. Pigment granules according to one or more of Claims 1 to 6, characterized in that the 5 pressed or briquetted core according to a) and the outer layer applied by granulation or the outer layers applied by granulation according to b) and c) contain in each case a plurality of inorganic pigments and/or in each case a plurality of organic pigments.
11. Pigment granules according to Claim 10, characterized in that the pressed or briquetted core according to a) and the outer. layer applied by granulation or the outer layers 10 applied by granulation according to b) and c) contain the same organic or inorganic pigments but at least one auxiliary differing in amount or type like the core.
12. Pigment granules according to Claim 10, characterized in that the pressed or briquetted core according to a) and the outer layer applied by granulation or the outer layers applied by granulation according to b) and c) contain the same organic and/or inorganic 15 pigments, the pigment in at least one of the outer layers applied by granulation not being pressed and not being bniquetted.
13. Pigment granules according to one or more of Claims I to 12, characterized in that auxiliaries other than those in the outer layer applied by granulation according to b) and c) are present in the pressed or briquetted core according to a). 20
14. Pigment granules according to one or more of Claims I to 13, characterized in that the pressed or briquetted core according to a) is coated once or several times with one or more auxiliaries.
15. Pigment granules according to one or more of Claims I to 14, characterized in that the outer layer applied by granulation or the outer layers applied by granulation according to 25 b) and c) are in each case coated once or several times with one or more auxiliaries.
16. Pigment granules according to one or more of Claims I to 15, characterized in that only the outermost of the outer layers applied by granulation according to b) and c) is coated once or several times with one or more auxiliaries.
17. Pigment granules according to one or more of Claims I to 16, characterized in that the 30 inorganic pigment granules have a bulk density in the range of 0.3 to 4.0 g/cm 3 , in particular in the range of 0.5 to 2.0 g/cm 3 , and in that the pigment granules which - 36 contain carbon black or organic pigments preferably have a bulk density of 0.1 to 2.5 g/cm 3 .
18. Pigment granules according to one or more of Claims 1 to 17, characterized in that at least 85% of the pigment granules have a particle size in the range of 80 to 3000 pam, in 5 particular in the range of 100 to 1500 pm.
19. Pigment granules according to one or more of Claims 1 to 18, characterized in that the pigment granules have a residual water content of less than 4% by weight, in particular less than 2% by weight.
20. Pigment granules according to one or more of Claims I to 19, characterized in that the 10 pigment granules additionally contain preservatives, antifoams, retention agents, antisettling agents and/or fragrances.
21. Process for the preparation of pigment granules according to one or more of Claims 1 to 20, characterized in that a) one or more organic or inorganic pigments are mixed with one or more 15 auxiliaries, b) this mixture is subjected to at least one pressing or briquetting step in order to obtain scabs, c) these scabs are corminuted in at least one step to give nuclei and powder, dl) the nuclei are separated from the powder in that the fraction greater than 80 ym, 20 in particular greater than 100 ym, serves as a core fraction and optionally (i) is subjected to a rounding step and/or (ii) is coated with one or more auxiliaries, it being possible for step dl)(ii) also to take place before dl)(i) or it being possible for both steps to take place simultaneously, and the product obtained 25 remaining in the production process while the other fraction is removed from the process or recycled, or d2) the nuclei serve as a core fraction and the powder formed on comminution is -37 applied completely to this core fraction by granulation by subsequent rolling, optionally one or more auxiliaries being added and it being possible for the product obtained and completely applied by granulation to be coated with one or more auxiliaries, 5 e) and at least one outer layer being applied by granulation by subsequent rolling to the product obtained with addition of one or more organic or inorganic pigments or mixtures thereof, (i) the organic or inorganic pigment or pigments or mixtures having been mixed beforehand with one or more auxiliaries and/or 10 (ii) one or more auxiliaries being added during the subsequent rolling and/or (iii) the organic or inorganic pigment or pigments or the mixture of organic or inorganic pigments and at least one auxiliary having been subjected beforehand to one or more pressing or briquetting steps, in order to obtain subsequently rolled granules and 15 f the granules subsequently rolled in this manner are optionally coated once or several times with auxiliaries.
22. Process according to Claim 21, characterized in that the pressing or briquetting step b) is effected by means of a roll press or matrix press and at nip forces of 0.1 to 50 kN/cm, in particular 0.1 to 20 kN/cm. 20
23. Process according to Claim 21, characterized in that a plurality of pressing or briquetting steps b) is effected directly in succession, identical or different pressing or briquetting units being used and the pressing or briquetting steps being carried out at identical or different nip forces in the range of 0.1 to 50 kN/cm, in particular of 0.1 to 20 kN/cm.
24. Process according to Claim 21, characterized in that, in step c), the comminution is 25 effected by means of a sieve having a mesh size of 0.5 to 4 mm, in particular of I to 2 mm, as a comminuting unit.
25. Process according to Claim 21, characterized in that a plurality of comminution steps c) by means of a sieve is effected directly in succession, different mesh sizes of the sieve being used and, in the last comminution step, a sieve having a mesh size of 0.5 to 4 mm, 30 in particular of 1 to 2 mm, being used. - 38
26. Process according to Claim 21, characterized in that a plurality of comminution steps c) is effected directly in succession, different comminution units being used.
27. Process according to Claim 21, characterized in that, before the comminution in step c), the scabs from b) are separated into two fractions, the coarse fraction, in which at 5 least 85% of the particles are greater than 500 pm, in particular greater than 600 pm, is fed to step c) and comminuted in one or more steps and the fine fraction is fed to step dl) in order to be separated again into two or more fractions in step dl), separately from or together with the nuclei and the powder from c), and to form the core fraction. 10
28. Process according to Claim 21, characterized in that the nuclei and powder of the comminuted product from step c) are separated into two fractions in step dl), the fine fraction smaller than 80 sm, in particular smaller than 250 im, being removed or recycled to the process and the coarse fraction greater than 80 ym, in particular greater than 250 im, serving as a core fraction. 15
29. Process according to Claim 21, characterized in that the nuclei and powder of the comminuted product from c) are separated into three fractions in step dl), the fine fraction and the coarse fraction being removed or recycled and the medium fraction in the range of 80 to 2000 ym, in particular of 250 and 1000 pm, serving as a core fraction.
30. Process according to Claim 21, characterized in that, before step e), the core fraction 20 from step dl) is separated into two fractions, the fine fraction or the coarse fraction being removed or recycled and the fraction in the range of 80 to 2000 pm, in particular in the range of 100 to 1500 pm, being fed to step e).
31. Process according to Claim 21, characterized in that, before step e), the core fraction from step dl) is separated into three fractions, the fine fraction and the coarse fraction 25 being removed or recycled and the medium fraction in the range of 80 to 2000 tm, in particular in the range of 100 to 1500 pim, being fed to step e).
32. Process according to Claim 21, characterized in that the organic and/or inorganic pigment(s) added to step e) is or are altogether not more than four times the weight, in particular not more than the same weight, based on the weight of the core fraction used 30 in step e).
33. Process according to Claim 21, characterized in that the organic and/or inorganic -39 pigment(s) used in step e) is or are different from the organic and/or inorganic pigment(s) which was or were used in process step a).
34. Process according to Claim 21, characterized in that an organic or an inorganic pigment is added in step e). 5
35. Process according to Claim 21, characterized in that a plurality of organic and/or inorganic pigments is used in succession in step e).
36. Process according to Claim 21, characterized in that a plurality of organic and/or inorganic pigments is added in step e), these having been mixed with one another beforehand. 10
37. Process according to Claim 21, characterized in that the organic and/or inorganic pigment(s) used in step e) is or are mixed beforehand individually or as a mixture with one or more auxiliaries.
38. Process according to Claim 21, characterized in that the granules obtained after step e) are separated into two fractions before step f), and only the fraction in which the 15 particles are greater than 80 ym, in particular greater than 250 pm, is fed to step f), while the fine fraction is removed from the process or recycled.
39. Process according to Claim 21, characterized in that the granules obtained after step e) are separated into three fractions before step f), and only the fraction in which at least 85% of the particles are greater than 80 Am, in particular greater 100 ym, or are in the 20 range of 80 to 3000 Am, in particular in the range of 100 to 1500 Im, is fed to step f) while the other fractions are removed from the process or recycled.
40. Process according to Claim 21, characterized in that the rounding step dl) (i) is effected on a rotating disc (pelletizing disc), in a coating drum or in a rotating drum (pelletizing drum), in a screen unit or in a fluidized bed or in a fluid bed. 25
41. Process according to Claim 21, characterized in that the subsequent rolling step under d2) is effected on a rotating disc (pelletizing disc), in a coating drum or in a rotating drum (pelletizing drum).
42. Process according to Claim 21, characterized in that the subsequent rolling step under e) is effected on a rotating disc (pelletizing disc), in a coating drum or in a rotating drum 30 (pelletizing drum). -40
43. Process according to one or more of Claims 21 to 42, characterized in that one or more drying steps are additionally effected.
44. Use of the pigment granules according to Claims 1 to 20 and of the pigment granules prepared by the process according to Claims 21 to 43 for colouring building materials 5 such as concrete, cement mortar, renders and asphalt, and for colouring organic media, such as finishes, plastics and colour pastes, and for the preparation of emulsion paints and slurries.
45. Process for colouring building materials with the pigment granules according to Claims I to 20 and the pigment granules prepared by the process according to Claims 10 21 to 43, characterized in that the pigment granules are mixed with the building materials in an amount of 0.1 to 10% by weight, based on cement or, in the case of asphalt, based on the total mixed material.
46. Process for colouring building materials with pigment granules according to Claims 1 to 20 and the pigment granules prepared by the process according to Claims 21 to 43, 15 characterized in that the pigment granules are first suspended in water and then mixed with the building materials.
47. Process for colouring organic media with pigment granules according to Claims 1 to 20 and the pigment granules prepared by the process according to Claims 21 to 43, characterized in that the pigment granules are mixed with the organic media. 20
48. Process according to Claim 47, characterized in that the organic media are plastics.
49. Process according to Claim 48, characterized in that the plastics are thermoplastics, thernosetting plastics and/or elastomers.
50. Process according to one or more of Claims 47 to 49, characterized in that the pigment granules are mixed with liquid plastics. 25
51. Process according to Claim 47, characterized in that the organic media are polymers having rubber-elastic properties.
52. Process according to Claim 47, characterized in that the organic media are powder coating materials.
53. Process for colouring emulsion paints with pigment granules according to Claims 1 to 30 20 and the pigment granules prepared by the process according to Claims 21 to 43, -41 characterized in that the pigment granules are mixed with the emulsion paints.
Priority Applications (1)
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AU2013251277A AU2013251277A1 (en) | 2006-04-10 | 2013-11-01 | Process for the preparation of pigment granules and the use thereof |
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DE102006017109.8 | 2006-04-10 | ||
AU2007201363A AU2007201363A1 (en) | 2006-04-10 | 2007-03-28 | Process for the preparation of pigment granules and the use thereof |
AU2013251277A AU2013251277A1 (en) | 2006-04-10 | 2013-11-01 | Process for the preparation of pigment granules and the use thereof |
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AU2007201363A Division AU2007201363A1 (en) | 2006-04-10 | 2007-03-28 | Process for the preparation of pigment granules and the use thereof |
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AU2013251277A1 true AU2013251277A1 (en) | 2013-11-21 |
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AU2013251277A Abandoned AU2013251277A1 (en) | 2006-04-10 | 2013-11-01 | Process for the preparation of pigment granules and the use thereof |
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