2014-DONDI-Clays_and_Bodies_for_Ceramic_Tiles.pdf

Published on Applied Clay Science 96 (2014) 91-109.Copyright © 2014 Elsevier Ltd. All rights reserved. doi:10.1016/j.clay.2014.01.013 Clays and Bodies for Ceramic Tiles: Reappraisal and Technological Classification Michele Dondi, Mariarosa Raimondo, Chiara Zanelli Institute of Science and Technology for Ceramics (ISTEC - CNR), via Granarolo 64, 48018 Faenza, Italy Abstract The ceramic tile industry is a dynamic sector whose technological innovation and market trends have drawn a complex picture of products and processes. Raw materials have been deeply involved in such an evolution: the flexibility of current manufacturing cycles enables the use of a very wide range of clays, whose chemical and mineralogical composition, particle size distribution and ceramic properties were reappraised. The classical reference schemes are no longer able to properly describe and predict the role of clays in tilemaking. In order to fill this gap, an industry-oriented, technological classification of clay raw materials is proposed on the basis of chemical (Fe2O3 content) and mineralogical parameters (amount of phyllosilicates and carbonates) together with particle size (fractions <2 µm and >63 µm) and plasticity (methylene blue index and Atterberg plastic index). It firstly discriminates light-firing and dark-firing clays according to an iron oxide threshold of 3%. Light-firing clays are distinguished by the amount of kaolinite group minerals and plasticity in “kaolins” (high-grade, low-grade, and raw kaolins, kaolinitic loams) and “plastic clays” (ball clays, pyrophyllitic clays, white bentonites); the distinction of three classes of ball clays with increasing plasticity is envisaged. Dark-firing clays are classified according to coarse-grained fraction and amount of carbonates in carbonate-rich types (marly and carbonatic clays), red loams and red clays; these latter are furtherly differentiated by the relative abundance of clay minerals. Such a classification is essential to draw the guidelines for body formulation and to explain the criteria followed in the industrial practice for each category of ceramic tiles. Key properties are discussed to design batches for porous tiles, vitrified and semivitrified red stoneware, and vitrified light-firing bodies. Both the clay classification and the guidelines to body formulation are intended to provide up-to-date tools to assess the ceramic potential and correct use in tilemaking of clay materials, but they cannot substitute a throroughful technological characterization, adequately simulating the industrial processing. Key-words: body formulation; ceramic tiles; clay raw materials; technological properties. 1. Introduction The production of ceramic tiles is growing worldwide at a rate of ~300 million m2 per year and has already passed 10 billion m2 in 2012 (Baraldi, 2013; Stock, 2012). Such an impressive growth implies an increasing demand for raw materials, whose global consumption can be estimated around 230 million tons per year. The commercial success of ceramic tiles is due to a continuous increase of product quality from both technical performance and aesthetic appearance viewpoints. Such a quality improvement stems from the intensive product and process innovation that took place during the last decades and is now widespread in every tilemaking country (Nassetti, 1989; Corma, 2008). This innovation has completely renovated the manufacturing cycle by introducing technological revolutions like fast firing, which brought about drastic changes in raw materials and eventually gave rise to novel products (e.g., monoporosa and porcelain stoneware) and to the disappearence of classic tile types (e.g., majolica and calcareous earthenware). As a consequence, a paradigm shift occurred in the formulation of ceramic bodies and in the selection of raw materials (Fiori and Fabbri, 1985; Becker and Brenner, 1997; Dondi, 2003). From this standpoint, classical treatises on ceramic raw materials —set up with reference to a picture of manufacturing and products already obsolete— are no longer able to describe the current market or to assess the potential of a given clay in tilemaking (Harvey and Murray, 1997; Mitchell and Vincent, 1997; Diaz and Published on Applied Clay Science 96 (2014) 91-109. Copyright © 2014 Elsevier Ltd. All rights reserved. doi:10.1016/j.clay.2014.01.013 Torrecillas, 2002; McCuistion and Wilson, 2006) or to address the correct design criteria for batch formulation (Singer and Singer, 1963; Fabbri and Fiori, 1985; Fiori et al., 1989). The aim of this paper is to overview the technological evolution in the ceramic tile sector and its effects on product typologies through: (i) a reappraisal of composition and application of clay materials in tilemaking; (ii) the proposal of a clay classification for ceramic purposes; (iii) the review of compositional ranges for each type of ceramic tile with design criteria and guidelines for their batch formulation. Overall, the main objective is the study the chemical-mineralogical composition and technological behaviour that allows the evaluation of the applicability of the ceramic clays. 2. Experimental approach As a first step, a classification of ceramic tiles is outlined to introduce both terminology and basic concepts of tilemaking. Criteria followed in tile classification encompass standard prescriptions and commercial issues. Another fundamental aspect is the continuous change in technological and compositional features of ceramic tiles induced by process and product innovation. The evolution of both manufacturing technology and product types is reviewed in order to draw a picture of how the ceramic tile industry has been evolving during the last decades. Clay materials used in the industrial practice were selected in order to get a representative picture (1040 samples) of uses, technological features, and geographic provenance. The data sources for the clays here considered are summarized in Table I. For each clay, chemical and mineralogical composition (with rational calculation when quantitative data were not given) were considered together with particle size distribution, plasticity (Atterberg consistency limits and Methylene Blue Index, MBI) and technological behaviour in tilemaking (if available). In particular, MBI is able to summarize the overall technological performance of clays (Kelly, 1984; Chiappone et al., 2004): it can be measured at natural pH (MBIn) or in acidic conditions (MBIa at pH~4) according to ASTM C837. The body formulation of different types of wall and floor tiles was taken from literature sources about porous bodies (Escardino, 1992; Dondi et al., 1999; Bittencourt et al., 2001; Das et al., 2005; Sousa and Holanda, 2005) and vitrified bodies (Beltran et al., 1996; Motta et al., 2001; Mukhopadhyay et al., 2009; Zanelli et al., 2011a; Lassinanti Gualtieri et al., 2011; Lazaro et al., 2012) as well as from the industrial practice (SACMI, 1986 and 2001; Lorici and Brusa, 1991; Brusa and Bresciani, 1996; Sanchez et al., 1997). 3. Ceramic tile technology 3.1. Ceramic tiles: types and classification Ceramic tiles are classified by the ISO 13006 technical standard on the basis of water absorption: <3% (Group I), 3-10% (Group II) and >10% (Group III); groups I and II are divided in two subgroups each at the water absorption threshold of 0.5% and 6%, respectively (Fig. 1). The group code includes a letter which stands for the shaping technique: A for extrusion and B for pressing (Table II). In contrast, tile marketing is based on the end use: wall coverings (Group III and to a large extent IIb) and floorings (Groups I and IIa). Along with the end use, tiles are discriminated by the body colour (a different product value is assumed for coloured and colourless bodies). The resulting terminology is somehow related to the tilemaking technology and/or the ceramic material constituting the product, so creating a patchwork of names not easy to be understood (Table II). Figure 1 gives a picture of tile products, stemming from the above mentioned commercial and standard issues, by contrasting body colour (mostly depending on iron oxide concentration) and body compactness (expressed as typical values of water absorption). It can be seen that standard groups are not homogeneously populated neither as the number of products (much more in Groups III and I) nor in terms of body colour (Group II is essentially represented by red bodies, while in Group BIa there are exclusively colourless bodies). 3.2. Ceramic tile manufacturing Ceramic tiles are currently manufactured by the wet or the dry route. A detailed description of tile manufacturing goes beyond the aims of the present paper. At any rate, a short outline of technology and its evolution is given hereafter (some relevant features are reported in Table II) with reference to the five basic steps (Various Authors, 2000-2008): Published on Applied Clay Science 96 (2014) 91-109. Copyright © 2014 Elsevier Ltd. All rights reserved. doi:10.1016/j.clay.2014.01.013 1) body preparation involving wet ball milling or dry grinding of raw materials and powder agglomeration by spray drying (wet route) or granulation (dry route); 2) tile shaping mostly by dry pressing, but also extrusion is used; 3) tile drying by fast cycles in vertical or horizontal driers; 4) tile glazing and decoration by a large set of technological solutions; 5) tile firing by fast cycles in roller kilns (rarely chamber or tunnel furnaces). Additional steps can be present, like end-of-line treatments (e.g., tile polishing, cutting or functionalization), while others may be shifted along the flow-chain (e.g., decoration can be performed during shaping). A key-point is the technological innovation that has deeply changed each processing step in the last six decades, as it can be appreciated in Figure 2: Body preparation has been since long time improving starting by the introduction of the wet route: replacing to a large extent conventional hammer mills (#1 in Fig. 2) and granulation (#6) by spray driers (#7) and ball mills with upgrading from discontinuous (#2) to continuous (#3) then to modular mills (#4). Significant improvement has been recently achieved in the dry route too, by developing versatile and more efficient roller and pendular mills (#5) as well as by granulation systems of new generation (#9). Tile shaping gained a great advantage by the adoption of hydraulic presses (#12) instead of mechanical ones (#11); the former have been continuously improved, getting more powerful and reliable machines able to produce even large size slabs. Novel shaping technologies (e.g. dieless pressing) entered in use especially focused on low thickness and large size, e.g. 3x1 m slabs 3 mm thick (#13). Extrusion (#10) has been recently revitalized to manufacture big slabs with novel wet technology (#8). Tile drying was converted from old-style chamber plants (#14) to vertical driers (#15) that in the last decade made progressively room for multichannel horizontal driers (#16) and even hybrid solutions, including infrared heating (#17). Tile glazing is still retaining conventional processes (application by bell, disk or doctor blade) that have been gradually automized and improved, gaining in control and quality, and enriched by dry applications; the introduction of digitalized systems is envisaged. Tile decoration moved from traditional screen printing to silicon roller printing and soluble salts, till the recent spreading of ink-jet printing. Fast firing is the trait of ceramic process that has been continuously improved by developing roller kilns (#20) that replaced tunnel furnaces (#18) and early kinds of fast firing plants, like plates or pegs kilns (#19). Roller kilns have gradually gained wider sections, turning multichannel (#21) and able to operate at higher temperatures (up to 1250°C). Further steps go towards hybrid furnaces, as those fed by methane and electricity (#22). 3.2. Evolution of ceramic bodies with technological innovation Technological innovation has strongly affected the use of raw materials, thus a look at the evolution of ceramic tile technology is fundamental to fully understand the changes occurred in bodies formulation along the last 60 years. Product and process innovation can be perceived through the historical evolution of ceramic tiles, mainly based on data from the Sassuolo district in Italy, that is leading the technological progress in this field (Fig. 3) and the Castellón district in Spain, besides some time lags (Corma, 2008). As a matter of fact, after the World War II a few types of ceramic tiles were on the market (Singer and Singer, 1963): essentially porous and glazed wall tiles (white body: calcareous earthenware; red body: majolica) while floor tiles were unglazed products mostly destined to industrial and outdoor applications: stoneware in its variants (red or white) manufactured by extrusion (klinker, rustic cotto) or dry pressing (red stoneware and fine stoneware). The main product innovation during the 1960s was the development of cottoforte, a glazed porous tile suitable for floorings, which switched the production towards floor tiles. The harsh energetic crisis during the 1970s compelled the ceramic industry to convert its process to a lower energy consumption, fostering the advent of fast firing in roller kilns, that turned step by step the whole tilemaking cycle into a new technology (involving wet milling > spray drying > dry pressing > fast drying and firing). Such a novel technology, besides being much more flexible and efficient from the energetic point of view, proved to be unable to process the classic body formulations (i.e., majolica, earthenware and stoneware) thus imposing drastic changes to batch compositions. This eventually gave rise, through an empirical approach, to new products: monoporosa (manufactured by fast single fire) and then birapida (by fast double fire) took the place of majolica or earthenware and are now dominating the field of porous tiles. As red monoporosa/birapida derived from majolica, white birapida arose from calcareous earthenware but, curiously enough, white monoporosa was developed starting from stoneware formulations. compositional or technological features (ICerS.. Dondi et al. may contain low amounts of illite-mica. it has rapidly got market shares to become now likely the most important tile product worldwide. involving properties like slip viscosity. ceramic bodies are distinguished in light-firing (from white to light brown) and dark-firing (from pink to dark brown) on the basis of colour after firing. By this way.2014. In the same period. Stentiford. Overall. may be classified under the same term. 1% Fe2O3). along with kaolinite.Published on Applied Clay Science 96 (2014) 91-109. such a threshold is somewhat related with technological properties: the iron content of a kaolin utilized to whiten a given body. Such a commercial success drew the implementation of the whole manufacturing route. Besides the general distinction between kaolin and ball clay (Harvey and Murray. on the other hand. although further components (feldspars.. smectite. As the use of ball clays. Among clay minerals. it often happens that similar raw materials be termed as “kaolin” or “ball clay” depending on the end-use. Al-oxyhydroxides and non plastic components (quartz. very different in composition and particle size.g.013 The evolution of floor tiles was more complicated (Reh. vermiculite and chlorite can be found in decreasing order of frequency. fusibility. By this way. introduced in a small amount to improve the green bending strength. At any rate. iron and aluminium oxyhydroxides. rock fragments. initially an unglazed floor tile for heavy traffic applications. is tolerable even if slightly exceeding the limit. is acceptable for values well below the limit (e.g. interstratified K/S. halloysite. clays used in light-firing and dark-firing bodies are fairly well discriminated by a Fe2O3 content of approximately 3% wt. Copyright © 2014 Elsevier Ltd. 5 and 6): >75% High-grade Kaolins (HK). particle size distribution and plasticity (Atterberg consistency limits and Methylene Blue Index).clay. instead of local red-firing clays. pore-forming ability and so on. percentage of quartz and other phyllosilicates (particularly pyrophyllite and expandable clay minerals: smectite + interstratified I/S). for instance. 4. 4. (Fig. low iron oxide clays (hence light-coloured after firing) are distinguished by the amount of kaolinite group minerals into the following classes (Figs. 1997) these terms are used quite freely for commercial purposes regardless genetic. 2003. organic matter) may be present. shaping. From the mineralogical point of view. feldspars. 2010). 1999. translucent). drying and firing) will be outlined in the following paragraphs. pyrophyllite. a single-fired glazed white stoneware was developed. First of all. turning to be the leading product in the 1990s. also illite. For this reason. superwhite.. compaction. drying sensitivity. sericite. Thanks to its outstanding technical performances.. Porcelain stoneware. has progressively gained aesthetic value by a wide range of decoration techniques with the creation of glazed porcelain stoneware and special body types (e. plasticity. .01. characterized by high to very high amount of kaolinite and/or halloysite. dickite. providing substantial improvements in body preparation. which are strictly connected with clay mineralogy and particle size distribution (Dondi. amount of kaolinite group minerals (kaolinite. All rights reserved. 2005). Bal and Fiederling-Kapteinat. hence their commercial classification. entailing the technological features of clays (rheological properties and behaviour during grinding. depends on the technological and appearence requirements of each kind of ceramic body: firstly the colour after firing and secondly the behaviour during the tilemaking process. Further distinctions. even if a certain role is played by further components (as TiO2 and CaO) that may turn the colour to yellowish or pinkish shades. the iron oxide content of a bentonite. a shift to white bodies occurred during the 1980s (Bertolani et al. 1986).1. doi:10.1016/j. 1991): first a single-fired glazed red stoneware was achieved by modifying unglazed stoneware and cottoforte batches (and it is still the reference product for semi-vitrified or vitrified red bodies). starting from fine stoneware formulations. 2004. tridymite and opal). other clays. 1995-2010). halloysite. they basically consist of phyllosilicates (mostly kaolinite) and silica phases (quartz and exceptionally cristobalite. we propose a classification based on the following criteria: iron oxide content.. thermal cycles. end-of-line treatments and particularly decoration. In practice. dickite). Ceramic clays: composition and classification The use of clays in tile manufacturing. This colour depends essentially on the iron oxide content. ensured several advantages. a new floor tile type was launched: the porcelain stoneware (Sanchez et al. Light-firing clays (LFC) Light-firing clays encompass several commercial types going under the general terms of kaolin and ball clay (including pyrophyllite and to some extent bentonite) each referring to a wide range of mineralogical and granulometric characteristics. polished. 4). titanium dioxide) each below 15%. interstratified I/S. 2012). The utilization of raw kaolins in tilemaking is not straightforward. This can be described as a compromise between coarse grain size and relatively high plasticity. Belarus (Levitskii et al. besides predominantly kaolinitic. Raw Kaolins (RK) are basically deeply kaolinized parent rocks (in case of primary deposits) that contain a lot of non plastic components (particularly rock fragments. However. being classified as Pyrophyllitic Clays (PC) or White Bentonites (WB) respectively. As a matter of fact. Ball Clays (BC) have an amount of kaolinite group minerals analogous to low-grade kaolins (although it can be below 50% in case of illite-rich materials). 1996) or Sinitsa and Dedovka. 2012). Examples of HK used in tilemaking are kaolins from Cornwall.1. 1998) and Piloni di Torniella. The distinction between low-grade kaolins and ball clays is here proposed in terms of plasticity (Fig.clay. Yanik.. Sergievich et al. illite.4. made up of quartz. Scott et al. Bordeepong et al. UK (Bristow. 1997.1. The addition of raw kaolin turns to be useful particularly when the distance from mine to tile factory is short. an abundant non plastic fraction.1. 2011). thanks to comparable amounts of kaolinite. Some sedimentary deposits utilized by the ceramic industry contain. the LK class defines clays with a rather low plasticity (MBIa <7.1. rock fragments) whose technological behaviour has to be balanced by the other clays and fluxes making up the body. chlorite). contain from low to significant amounts of illite and/or interstratified I/S along with an always important non plastic portion.. the technological behaviour is clearly different from that of HK. the technological performance of the materials higher in kaolinite and poor in feldspars and expandable clay minerals does not substantially differ from that of high-grade kaolins. these limits can be to some extent overcome by the occurrence of feldspars (enhancing fusibility and fostering sintering) and expandable clay minerals (improving plasticity). 4. Kitagawa and Köster. mainly consisting of quartz with some feldspars and sometimes carbonates. at least 40% in weight. Italy (Costa et al. the amount of phyllosilicates must be high enough to bestow a sufficient.. due to the increased non plastic fraction. Copyright © 2014 Elsevier Ltd. At any rate. Italy (Bertolani and Loschi Ghittoni. 1991) or some grades from Kütahya. 2011. Examples of LK used in tilemaking are kaolins from Santa Severa. However. Low-grade Kaolins (LK). 1971). interstratified I/S. RK may play as a sort of mix. 2012) and some grades from Muang Ranong. as the raw kaolins. All rights reserved.3. strongly affecting their technological behaviour. so presenting analogies with flint clays (Keller.1016/j. feldspars. Mexico (Guillén et al. As a matter of fact. Thailand (Worasith et al. 4. More refractory terms often need to be milled in order to exhibit a plastic behaviour. 6). the overall mineralogical composition of BC overlaps to a large extent those of kaolins (Fig. When the amount of kaolinite group minerals approaches 50%.. doi:10. 5). feldspars and mica). enhancing the formation of mullite and whiter shades during firing. 2011. but difficult to press and highly refractory. Germany (Keck. Raw Kaolins (RK).1. Viti et al. 4.01.2. quartz. Both raw kaolins and kaolinitic loams are characterized by a coarse-grained particle size distribution with often a significant sandy fraction (>25% over 63 µm). high-grade kaolins are easily dispersable in water. In any case. although their use is restricted to vitrified and porous bodies (usually in percentages larger than HK) being generally not utilized in engobes and glazes. These clay materials are here named kaolinitic loams due to their coarse grain size distribution. quartz and flux (feldspars. raw kaolins cannot fulfil ordinary requirements for ceramic clays. implying lower plasticity and confirming difficulties in pressing and sintering. although low. Light-firing clays poor in kaolinite and containing more than 20% of pyrophyllite or smectite constitute special cases..Published on Applied Clay Science 96 (2014) 91-109. For instance. etc.. 1996) and Bayern. 4. 1989. Kaolinitic Loams (KL) are sedimentary deposits where kaolinite is admixed with an abundant non plastic fraction (mainly quartz) frequently accompanied by other clay minerals (smectite. The behaviour of low-grade kaolins in the ceramic cycle is influenced by components associated to kaolinite in the plastic and non plastic fractions. Turkey (Kadir et al. Kaolinitic Loams (KL).. due to the frequent occurrence of expandable clay minerals together . Examples of RK used in tilemaking are raw materials from Romana (Ligas et al. In ceramic tile manufacturing. 2007) or Michoacán. plasticity on the raw kaolin to act as a clay material. HK are typically used in low amounts: a few percent in glazes and engobes (to thicken and stabilize suspensions) and no more than 10-15% in porous and vitrified bodies (unglazed porcelain stoneware and white birapida). especially due to their poor plasticity. so permitting to have a low cost. High-grade Kaolins (HK). so it is frequently disregarded.2014. 1991.5). 1993.013 50-75% 25-75% 25-50% <25% Low-grade Kaolins (LK). Ball clays are distinguished from raw kaolins (when kaolinite content is <50%) by their large particle fraction below 2 µm. 1995-2010). may affect significantly plasticity and behaviour during pressing and drying. 2010) and Argentina (Zalba. contain quartz.. interstratified K/S.e. 1986. feldspars and often kaolinite and/or illite or sericite. highly plastic. 2009).... these large sets of mineralogical and granulometric data reflect into wide ranges of technological properties of BC. although they are not always present. although the firing colour of the terms richer in iron is rather dark.. This picture allows to classify LFC according to the technological performance (Fig. high plasticity clays (12<MBI<16..g. There are many examples of BC used in tilemaking (Mc Cuistion and Wilson. Sardinia (Danasino and Di Primio. and lower refractoriness with respect to kaolins (Sánchez-Soto and Pérez Rodríguez. gibbsite. opal). quartz (0-60%) and feldspars (0-30%) concentrations. Further minerals (e. 2000. 2008). 1981. According to the classical definition “Ball clay is a fine-grained. 1979. 4. Dondi et al. These technological constraints make it preferable to have WB with not too much smectite and particularly with a moderate activity (i.013 with kaolinite. 1998).7.1016/j. Some clay materials used in ceramic tile production are characterized by the occurrence of pyrophyllite. RK). Examples of WB used in tilemaking are from Italy (Andreola et al. 1995). Pyrophyllitic clays can replace BC in many applications and are used in tilemaking especially in India (Das and Mohanty. Fig.. 2000). Naimo et al.. medium plasticity clays (7. Expandable clay minerals (mostly interstratified illite-smectite and sometimes smectite) are common components that can reach 25% and. White Bentonites (WB). Pyrophyllitic clays (PC). 1997) and Argentina (Alló and Murray. Germany (Marx and Hennicke. drying and firing. Argentina (Domínguez et al. 2011). regardless of compositional features. Ball Clays (BC).1. 5): low plasticity clays (MBI < 7. easier compaction.5<MBI<12. in ceramic tile production such a definition is stretched to cover a proper (or even a just acceptable) behaviour during wet milling. 2003). 2003 and references therein).clay. but preferably below 2%) are used in tilemaking as additives to enhance plasticity of too lean bodies. In reality.01. This kind of clay materials is commonly referred to as White Bentonites. 2003 and 2008)— with on the whole higher values with respect to LK. Santa Cruz. carbonates) are sometimes present in low amount. Piedmont (Fiori and Fabbri. from a few percent up to 80% wt. pyrophyllite. 2011b). Other components include iron oxyhydroxides (usually below 2%. volcanic glass and rock fragments. PC are usually claystones of different origin that.. Cravero et al. In practice. 1998. extremely high plasticity occurs only in bentonites among ceramic raw materials. Mukhopadhyay et al.. Clays with a high amount of smectite (frequently over 50% wt. doi:10.6. being roseki in Japan and Korea (Matsuda et al. Quite complex mineralogical assemblages are common: smectite together with other phyllosilicates (interstratified I/S and less frequently kaolinite or illite). LK.1-0. typically kaolins: HK. These limits are traceable to the technological behaviour in tilemaking and differ from established reference schemes (Polidori.7% range). Since pyrophyllite has a different technological behaviour with respect to kaolinite. chlorite. some raw materials going under the term “ball clay” exhibit a rather coarse grain size with the silty fraction over 50% (Fig. illite (0-60%). 4.1. 2009). entailing plasticity and behaviour during compaction. Higashi. Copyright © 2014 Elsevier Ltd. Dristas and Frisicale. Zanelli et al. Ukraine (Fiederling-Kapteinat et al. mainly kaolinitic sedimentary clay. feldspars.2014. BC1). However. silica phases (quartz. though their maximum tolerable amount is constrained by rheological properties during wet milling and spray-drying (smectite induces a sharp increase of slip viscosity and thixotropy) as well as by drying sensitivity (Andreola et al.1. 2009. 2004. The use of WB in tilemaking is substantially addressed to increase the mechanical strength of unfired bodies. the higher grades of which fire to a white or near white colour” (Wilson. and very high plasticity clays (16<MBI<30.. 2006): clays from Westerwald. Such a peculiar composition turns KL a rather versatile raw material. 2000). 2005. Petrick et al. Mukhopadhyay et al. As a consequence. BC3 and some WB).. tridymite. even if slightly higher amounts may be tolerated) and organic or carbonaceous matter (commonly in the 0. Greece (Christidis and Scott. Examples of KL used in tilemaking are Italian clays from Lozzolo.5. BC used in tilemaking plot over almost the entire Kaolinite−Illite−Quartz+Feldspar ternary diagram (Fig. All rights reserved.5. along with pyrophyllite. Ball clays are characterized by a wide range of MBIa —going from 8 to 40 meq/100g (Wilson. 6) and a relatively low iron content (Fe2O3 at max 6%. Particle size distribution is in most cases fine-grained with the clay fraction over 50% and frequently over 75%. cristobalite. Ca-exchanged terms). an outstanding range of compositions and technological properties goes under the commercial term of “ball clay” (ICerS. pressing and sintering. 6) implying wide ranges of kaolinite (20-80%). Overall. 1987) and Florinas. Donbass. that can be addressed to vitrified bodies up to 20-25%. 7). . it is convenient to classify as Pyrophyllitic Clays (PC) the raw materials with a significant amount of pyrophyllite (>20%) as they present commonly lower loss on ignition. 2009). BC2)...Published on Applied Clay Science 96 (2014) 91-109. 1998. 4. 9).2014. Spain: for example the Mas Vell (MC) and Araya (CC) clays (Bastida and Beltran. From the mineralogical point of view.. Particle size distribution can span from silty clays to clay silts and loams. etc). where different types of phyllosilicates (commonly illite. • The degree of lithification may affect. . smectite. 8): 4. feldspars and rock fragments (up to 40%). particle size distribution and technological behaviour. MC and CC are overall characterized by the most complex mineralogical composition among ceramic clays. All rights reserved. in the body formulation for wall tiles. 1997. which play a complex role during firing. carbonates below 10% and a coarse-grained fraction below 25%.. Dagounaki et al. doi:10. interstratified terms and chlorite. these criteria allow to distinguish the iron-rich clays in the following classes (Fig.013 4. as of new crystalline phases (e. RC are commonly complex mixtures where 3 to 5 groups of clay minerals (kaolinite. Dondi. being classified as clay or loam depending on the degree of milling (Alló et al. 1997). 2008). therefore the behaviour during shaping and sintering. the higher the amount of clay that can be used. implying that RC can contain a non plastic portion up to 70% (Fig. It discriminates easily sintered (selfsintering or vitrifying) clays from more refractory ones.2. The phyllosilicates-to-quartz+feldspars ratio can vary greatly. interstratified IS and chlorite is within 20%. or more properly the critical temperature at which sintering begins to run by viscous flow of the amorphous phase formed at high temperature. the amount of chlorite or expandable clay minerals is always below 20%. Dark-firing clays (DFC) Red-firing clays are commonly gathered in a single category. These thresholds define an extremely wide space. • Prevalently illitic red clays (RC2) where illite-mica terms are over 50% of phyllosilicates and the amount of smectite.. In order to fill this gap. Meseguer et al.2. thermal and moisture expansion. amount and type of phyllosilicates (the terms richer in expandable clay minerals are not suitable for the wet route). a classification is here proposed in terms of phyllosilicate assemblages (Fig.clay. Red Clays (RC) practically include every iron-rich clay material with Fe2O3 over 3%. A lower threshold is here proposed at 10% carbonates (calcite+dolomite) to define the field of marly clays. 1992.. and minor components depending on the origin of clay deposits (organic matter. with the <2 µm fraction ranging from 20% to 80% wt. so implying a very wide variation range in terms of mineralogical composition. amount of carbonates. 1986. A strongly lithified material (e. However. plagioclase. 1992. and making the production of net-shaped tiles feasible (Billi et al. • The so-called ‘fusibility’.2.Published on Applied Clay Science 96 (2014) 91-109. However.2. the maximum amount of a given clay depends primarily on its content in calcite and dolomite: the lower the carbonates percentage. sometimes pyrophyllite and vermiculite) coexist in the same raw material (Fig. carbonates (up to 50%). plasticity by Atterberg consistency limits (MBI values are just seldom available for DFC). From the granulometric viewpoint.. 9). both particle size distribution and plasticity. For this reason. 4. 8): • predominantly kaolinitic red clays (RC1) where kaolinite group minerals represent over 50% of the total of phyllosilicates. Overall. Marly Clays (MC) and Carbonatic Clays (CC). MC range from silty clays to clay silts with a low sandy fraction (Fig. Although to a certain extent arbitrary. 10).01. no distinctions are practiced in the industrial production beyond that of Red Clays. DFC consist predominantly of phyllosilicates (from 35% to over 90%) associated with quartz (up to 50%). coarse-grained fraction (>63 µm). it is proposed also an upper threshold at 30% of carbonates that define carbonatic clays whose use is generally restricted as a minor component in monoporosa and especially birapida tiles. chlorite. 10). 1999). depending on the milling process. entailing the formation of a smallsized porosity. pyroxene. The criteria followed in the classification of DFC are: iron oxide content (the 3% Fe2O3 threshold already mentioned for LFC). sulphides. Furthermore. sulphates.g. iron oxyhydroxides (up to 15%). 9) spread in different way over the silty and sandy fractions (Fig.. this threshold actually discriminates clay materials whose main use is in wall tiles. and melilite) controlling firing shrinkage. that as a consequence reflects into different technological behaviours. 2011b) or the Ranzano Fm in Sassuolo for MC (Billi et al.. Sanchez et al. particularly in the case of monoporosa technology.g. a shale) may change significantly its ceramic behaviour according to its grain size distribution. both in terms of mineralogical composition and particle size distribution. illite. Copyright © 2014 Elsevier Ltd.1016/j.. Besides this complicated compositional picture. the main parameters considered in the industrial practice are: • the occurrence of carbonates. carbonates and quartz are all present in significant amounts (Fig. smectite plus minor kaolinite and interstratified terms). Typical carbonate-bearing clays used in tilemaking are from Castellón.1. Calcite and dolomite are common constituents of many ceramic clay materials and their amount spans from absent to over 40%. that usually include up to a dozen different raw materials. feldspathoids. forming a liquid phase at high temperature that allows to densify the ceramic body by a viscous flow. 1). Argentina. highly fusible. stabilizing suspensions (in the wet route). particularly relevant are the following: − water absorption to fit the window of acceptance for each class (Fig. R3 are mostly silty clays. the following key properties are particularly stressed: − rheological properties of slips. About the behaviour during the tilemaking process. flux and filler in order to dump any fluctuation in composition and technological properties. with expandable clay minerals sometimes present.1016/j. All rights reserved. Dondi. providing a coarse-grained structure (so-called skeleton) contrasting deformations during drying and firing. The clay fraction is frequently a mix of illite.clay. The technical performances refer to the prescriptions of international standard ISO 13006 for each tile typology. It is common in the industrial practice to use more than one source of clay. thus it is strictly connected with key properties of each typology of ceramic tiles. though chamotte or other sand types are sometimes used. 2009).g. the most common filler is quartz sand. . but sericite. with moderate plasticity in case of chlorite-rich terms (Carretero et al. 2006). RL are typically utilized in the manufacture of rustic tiles. doi:10.g. other additives are pigments. Bertolani and Loschi Ghittoni.. in Tuscany and Piedmont. 4. but in proper amounts they may be added practically to every type of red tile bodies in total or partial replacement of filler (Kayaci et al. 2002) to high plasticity of the smectite-rich grades. − bending strength of unfired tiles that must be high enough (usually >4 MPa) to withstand wet glazing and mechanical stress of screen printing (this latter requirement can be relaxed in case of non contact decoration. − porosity and linear shrinkage that must match the target after a proper firing schedule. kaolinite).. and further raw materials are utilized too. Body formulation is focused on both technological behaviour and technical performance of finished products. for RC1 (Cravero et al. Brazil (Christofoletti and Moreno. glaze appearance. that affect dramatically the efficiency of milling and spray drying (Andreola et al. e. feldspars and rock fragments. opacifiers and sintering promoters.Published on Applied Clay Science 96 (2014) 91-109. In tilemaking..g. quite fusible but with a poor to moderate plasticity.013 • Mixed types like illite-chlorite red clays or illite-smectite red clays (RC3) where the amount of chlorite and/or expandable clay minerals associated to illite is over 20% of the total of phyllosilicates. four basic ingredients are necessary: − Clay. 1996.. for example. 1997). Red loams are exploited. by inkjet printing). Technological innovation has been increasing the flexibility of tilemaking processes. Spain (García-Tomás et al. 2005) and various red shales from the Sassuolo district in Italy (Fiori. − absence of bulk or surface defects (black core. during firing clay acts as flux (e. 1982a and 1982b. Villar and Chulilla clays from Castellón. ensuring the plasticity necessary for shaping.. 5. Spain. 1999). the plastic behaviour is also heavily affected by the amount of non plastic component. in the wet route. − Additives. 1995). Motta et al. Bastida et al. − Filler. Examples of red clays used in tilemaking are those from Neuquén. 2010). − Flux. etc). For all types. illite) or mullite precursor (e. Illite-rich RC2 terms are in many cases silty clays.3. Such a peculiar composition turns RL especially suitable for extruded products and not surprisingly they are extensively used in the manufacturing of heavy-clay products (Fabbri and Dondi. 1996. Italy (Malesani..01. Fig. Bastida and Beltrán.2.. Copyright © 2014 Elsevier Ltd. planarity. Red Loams (RL) represent substantially a special case of red or marly clays with an abundant coarsegrained fraction (over 25% >63 µm. and bestowing mechanical strength on unfired tiles. 1992. 10). 1986 and 1990) as well as in the Teruel basin. for RC2 (Bastida. and for RC3 the Corumbataí Fm... 2004. so allowing the preparation of ever more complex batches. kaolinite and chlorite. Different technological behaviours are expected for these red clay types: the RC1 grades richer in kaolinite are rather plastic and refractory (somehow approaching the definition of fireclay) besides significant amounts of sandy fraction are frequent. 1986). like a pore-forming agent which develops porosity during firing and fosters sintering by surface diffusion (role frequently carried out by carbonates). This sandy component typically consists of quartz. Ceramic bodies: formulation and design criteria In the design of body recipes for ceramic tiles.2014. feldspars are the typical flux. P3: by introducing Ca or Ca-Mg raw materials different from carbonates. by controlling both CTE (
20-400°C typically in the 6. González-García et al. As porous bodies are always glazed. 1998 and 1999. Although there is no emphasis on colour for RMP and RBR. 1995. carbonates in monoporosa bodies are constrained to 7-12% wt (at most 15%). UPS). route 3 opens a wide range of solutions in terms of alkaline-earth oxidesbearing raw materials: wollastonite. it will cause defects (pinholes). 1999. RBR and RMP typologies). However.. for simplicity sake. − coefficient of thermal expansion (CTE) that ensures the body-glaze thermodilatometric matching. the expected colour of fired body is white for WMP and especially WBR (Fe2O3 of the batch is usually <1%. All rights reserved. account must be taken that multipurpose bodies are sometimes designed by the industry: a single batch can be formulated to produce two different typologies (e. drying and firing shrinkages must be very low. Kara et al. diopside. 5. calcite thermal decomposition occurs. with conspicuous advantages in terms of cost and productivity. 2011. due to the fast firing cycle. In any case. Filler is privileged . BIII or BIIb. at most 2% wt dry-basis). In these cases. never exceeding 1 cm/m. semi-vitrified and vitrified red bodies (GRS).. that is 15 MPa. 2010). special care is needed to ensure the body-glaze thermodilatometric matching.013 − modulus of rupture and resistance to deep abrasion according to each class (Table II). Serra et al. ii) fostering the gas permeability (lower bulk density of unfired tile by lower load at the press) and iii) limiting the carbonate amount of the batch..Published on Applied Clay Science 96 (2014) 91-109.01. It implies that MC have to be within ~60% of RMP batches (much less in the case of CC) with some RC together with filler or RL to control gas permeability (Kayaci et al. BIIa or BIb) just changing the processing parameters (Brusa and Bresciani. This overall target is easier accomplished with calcium-rich bodies that promoting the formation of Ca-Mg silicates (plagioclase. Monoporosa technology allows to fire at the same time body and glaze. roughly corresponding to BIII. 2008 and 2009.1. at rather high temperatures and may overlap glaze melting. Hajjaji and Mezouari. route P2 is followed to get RMP and RBR tiles. 2013. 1996. There are three main routes to design proper porous bodies (Tables III and IV): P1: by using carbonate-bearing clays (MC and CC).2014. GPS. respectively. pyroxene. synthetic silicates (including frits and glass-ceramic systems). but when neither calcite nor dolomite are available (or large size.. As a consequence. Route P1 is commonly adopted for red bodies.1. P2: by adding calcite or dolomite to the batch.clay. melilite. For this purpose. − resistance to moisture expansion in order to prevent damages to floorings and wallings (Hall and Hoff. Dondi et al.. Furthermore. White bodies are always manufactured by route P2. However. 2010). Porosity is constrained by the minimum bending strength required.1. Trindade et al. Industrial firing schedules are typically running at 1000-1140°C of maximum temperature with 30-45 minutes cold-to-cold. only when no suitable carbonate-bearing clay is available. 2001. Porous bodies are designed to get net shape tiles. doi:10. Kacim and Hajjaji. vitrified light-firing bodies (GWS. etc) during firing result stronger and more stable to moisture than low calcium bodies even with a high porosity.5-8. BII and BI classes of the ISO 13006 standard. Copyright © 2014 Elsevier Ltd. 5.. In order to prevent pinholes. high quality WMP tiles have to be produced without carbonates).1016/j. the body colour after firing is an important commercial aspect. 2012). if CO2 released from CaCO3 breakdown passes through a melted glaze.g.. the kinetics of calcite (or dolomite) breakdown has to be accelerated by: i) reducing the carbonate particle size. 2003.. Porous tiles produced by the wet route (particularly white bodies as well as many red monoporosa plants) preclude the use of raw materials with abundant expandable clay minerals (BC3 and some RC3 and MC cannot be utilized as main components).1%). A detailed description of phase transformations occurring during the thermal treatment of carbonatic clays and porous bodies can be found in the literature (Dondi et al.. the Fe2O3 content of fired bodies is usually from 4 to 6% (at maximum 8% wt).0 MK-1 range) and moisture expansion (recommended <0. 1990. by identifying three broad categories: porous bodies (WBR. talc. 2001. whose final dimensions are the same of the mould used for pressing. WMP. so preventing crazing defects. Porous bodies Porous bodies (water absorption >10%) are addressed to wall tiles that are manufactured by either the monoporosa technology (fast single firing) or the birapida technology (fast double firing) for both coloured bodies (RMP and RBR) and white bodies (WMP and WBR). The criteria of body formulation will be outlined. Jordán et al. 2006). Pardo et al. RBR batches came from majolica formulations: they are based on 60-80% marly clays corrected by some red clays. so still make use of kaolins.1016/j. Vieira and Monteiro. BIIa or BIIb classification.01. WBR bodies exhibit both a higher kaolin-to-ball clay ratio and larger amounts of filler with respect to WMP batches (Fig. olivine) and feldspars (with development of a more or less abundant vitreous phase). Copyright © 2014 Elsevier Ltd. 11 and RMP1-2 in Table IV) while RL is preferred in Spanish-style batches (Fig. along with floorings. Hematite crystallization from Fe-oxyhydroxides is a distinctive feature of these bodies (Hajjaji et al. 2008. WMP bodies were derived from stoneware batches and for this reason their formulation may contain low-grade kaolins and kaolinitic loams. This large set of products goes under the commercial name of red stoneware with its variants (glazed. WBR derived from calcareous earthenware batches. Pyrophyllite-bearing batches are often fluxed by wollastonite without carbonates (e. respectively).. 2004). All rights reserved. etc) with firing schedules that must be as faster (best 40 minutes or less) and as colder (best 1170°C or less) as possible. Red stoneware is nowadays produced by the dry route more frequently than by the wet route (Motta et al. beyond some convergency of requirements: e. 2009. semi-porous bodies with water absorption 6-10% (BIIb) are addressed. Therefore. 5. expandable clay minerals should be avoided in the wet route (recommended <5% in the batch) as coarse-grained clay materials should not be utilized in the dry route (limiting particularly the silty fraction that is little affected by dry milling). unglazed. in alternative. 11).Published on Applied Clay Science 96 (2014) 91-109. 12). 2012). mechanical strength. 5.2. It is almost always glazed. In fact.2014. although percentages over 20% (that were common in the traditional majolica and calcareous earthenware industry) are not recommended.g. The main concern in the design of red stoneware bodies is to fit the standard target (water absorption.1. Batches were changed by introducing some flux (to improve sintering kinetics) and some filler (to contrast black core and pyrodeformation) in order to make it possible the fast firing rates (Fabbri and Fiori. As the body is first fired without glaze. The strategies of formulation differ from rustic to glazed tiles. 2010). Vitrified red stoneware was developed from the traditional unglazed stoneware by adjusting the technological behaviour of red clays to the requirements of fast single firing (Fig. Red stoneware is manufactured by fast single firing at 1120-1180°C of maximum temperature in 20 to 50 minutes cold-to-cold. If CC are utilized. red clays are corrected with a filler (Table IV). On the other hand. Sánchez et al. Generally speaking.. the following criteria are applied in the industry to formulate red stoneware bodies (Table IV): . along with ball clays or pyrophyllitic clays. as there is no gas permeability requirement. Birapida technology was developed to overcome the technological constraints of monoporosa. to wall coverings. only rustic tiles and some low porosity tiles for outdoor applications (BIb) are unglazed. Mineralogical transformations occurring during the firing of low porosity red bodies are generally simpler than those of carbonate-bearing batches. Khalfaoui and Hajjaji. and these latter from semi-vitrified to vitrified bodies. Firing shrinkage must be within 6 cm/m (BII) or 9 cm/m (BIb) as firing deformations must be kept under strict control. large amounts of filler and sometimes fluxes.. in fact. Batches for rustic tiles are simple and often entirely made up of red loam with plasticity suitable for extrusion (Fabbri and Dondi.. Trindade et al. 5..2.g. is the higher amount of MC and the often lower percentages of filler and flux (Fig. Body colour varies from light red to dark brown (when MnO2 is added to prevent black core) as Fe2O3 amount is usually in the 3-7% range (at maximum 9% wt). spinel. 2011. 11 and RMP3). 11). 2002. 1990). 1999. Jordán et al. Vitrified and semi-vitrified red bodies Vitrified and semi-vitrified red-firing bodies are utilized for floor tiles that fall in the BIb and BIIa classes (water absorption 0. highly plastic clays are tolerated in low amounts in both wet milling (as they increase the slip viscosity) and dry cycle (they are difficult to moist by granulation).2. WBR4 in Table III).1. 1985. 12 and WMP3-4 in Table III). rustic) regardless of the BIb. the amount of carbonates in the batch can be higher than 12-15%. making simpler —besides the additional cost of a second fire— the production of porous tiles.. The main distinction between RBR and RMP bodies.. they essentially entail the breakdown of clay minerals (with formation of new crystalline phases: mullite and less frequently sanidine. Sometimes rustic tiles are processed by slow single firing of heavy-clay industry (Table II).5-3% and 3-6%. Different properties are expected for bodies processed by the wet or the dry route. doi:10.013 in Italian-style bodies (Fig. with little filler or RL. For this purpose it is useful to have a certain quartzous skeleton (typically 20-30%) which also helps to get the correct CTE (7-8 MK-1). a higher amount of RC is necessary. together with significant amounts of filler and fluxes (Fig.clay. 2008). abrasion..2014. with most technical properties depending on the interplay of residual porosity and phase composition. The firing transformations occurring to LFC and light-coloured bodies are the subject of several studies (Aras. 2004). due to their higher water absorption. slip rheological properties (milling and spray-drying). Semi-vitrified red stoneware has overall a batch composition close to that of the vitrified bodies.. 2007. with bodies containing some carbonates. often plastic and refractory red clays (like kaolinitic types RC1) can be used up to 30%. 5. frost. 2003. 2003. fluxes (7% sodic feldspar) and fillers (10% quartz sand) but appeal to then uncommon raw materials like . along with richer in iron. GWS bodies are typically fired at 1160-1190°C for 35-50 min cold-to-cold to get water absorption in the 1-3% range. 2004. Mukhopadhyay et al. illite and/or chlorite to be ‘self-sintering’ (like many RC2 and RC3 clays) can be used in large amounts (35-65%) being adjusted by adding filler.1% (although standard limit being <0. These large sized tiles require a special body formulation with particular care in the choice of clay raw materials and additives. 17. Lassinanti Gualtieri et al. respectively. Boschi.. Porcelain stoneware tiles can be either glazed or unglazed and are usually fired at 1190-1240°C for 50-70 min to fulfil the market requirement of water absorption ~0. Thus. Zanelli et al. plasticity and compressibility (pressing) and bending strength (glazing and decoration) are the key points for clay raw materials (Bougher.. Bastida et al. 2011. potassic. as they directly affect amount and composition of the vitreous phase. A compromise is necessary to match the slip requirements in terms of viscosity and thixotropy (recommending low amount of smectite and interstratified IS) with the needs of plasticity and strength (satisfied by a relatively high percentage of expandable clay minerals). 2008. since the specific surface area created by milling is the driving force of sintering. Glazed White Stoneware was first developed in the early 1980s by SACMI’s body No. Carbajal et al.. Copyright © 2014 Elsevier Ltd. usually below 20%. 2013. clay is kept to a minimum: its role is essentially restricted to govern the technological behaviour before firing. Brazil (Masson et al. 2008). Jordan et al. doi:10.g. 5. like fluxes (sodic.. 2009 and 2010).. BIIb tiles are easier to be produced. 2007. their amount is 25-40%). whose fast densification rates make it crucial the control on firing shrinkage (recommended <7 cm/m) and pyroplastic deformation. In particular. The clay contribution during firing is mainly that of mullite precursor (kaolinite. that can be provided by either calcite-bearing RC (which may contain up to 10% carbonates) or a minor amount of MC to be added to carbonate-free RC (i.1. This objective is achieved through viscous flow sintering.. The outstanding innovation in porcelain stoneware technology has led to the production of large slabs (up to 360x120 cm2) as very thin (0. Ferrari and Gualtieri. 5.. Dondi et al.5 cm) tiles and their combination (large and thin slabs) by uniaxial pressing. 1996. dieless pressing. whose formulation clearly represents a rupture from previous schemes: limited use of conventional clays (25% BC). particle size distribution is stressed. 2007. 2006. Hajjaji et al. 2008. 2006. the cottoforte approach. 2000.01.e. to the point that in several cases the same body can be used to produce BI or BII tiles just modifying the firing cycle.2. The flexibility in body formulation turned it possible —and in many cases necessary— to combine two or more of the above criteria. Light-coloured vitrified bodies are designed to fit the water absorption target by firing schedules achievable with roller kilns.3 cm) to very thick (2. Vitrified light-coloured bodies Light-coloured bodies are utilized to manufacture vitrified (BIb) and highly vitrified (BIa) floor tiles that correspond to commercial types Glazed White Stoneware (GWS) and Porcelain Stoneware. chemical. with a few exceptions (Melchiades et al.Published on Applied Clay Science 96 (2014) 91-109. GRS5 in Table IV). pyrophyllite) or additional flux in case of illite and interstratified IS (Lee et al..2.. complying all standard requirements in terms of mechanical. Motta et al. However. − red loams (RL) frequently have enough coarse-grained fraction to replace simultaneously filler and clay (when employed.3.1016/j.3. or extrusion (Raimondo et al. stain and thermal shock resistance. 2011a). especially the vitreous phase (Gualtieri. It happens for instance with some terms of the Corumbataí Fm that constitute the whole batch of the BII production in the Santa Gertrudes district. Lee et al. 2011a) also concerning their effect on the properties of tiles (Bakr.. 610% water absorption).013 − fine-grained. mixing different types of red clays and even different kinds of filler and flux. Zanelli et al. − raw materials that naturally contain enough feldspars. Gualtieri.clay. 2010). 2010). A distinctive treat of semi-vitrified tiles is the chance to have bodies based on a single clay able to fulfil all technological requirements (feasible for the rather large window of acceptance: e..5%).. Being the more refractory (and expensive) component in light-coloured vitrified bodies. commonly within 20% each. All these products are manufactured by the wet route. 2011.. as they need the addition of both flux and filler. All rights reserved. alkaline-earth and their combination) are strongly concerned. joined to the flexibility of tilemaking process. typical recipes in the Sassuolo (Italy) and Castellón (Spain) districts are reported in Table III. − Non plastic raw materials are more abundant than the clay component.013 low-grade kaolin (8%) and especially “eurite” (50%) that is a sericite-feldspar flux. This classification is in full agreement with the industrial practice. they are classifiable as medium (BC1) or to high (BC2) to very high plasticity (BC3) implying that not all the Ukrainian ball clays exhibit high plasticity (LK and BC1 terms should be blended with more plastic terms). it can be even lower in special products: e. Porcelain stoneware bodies may contain additives with different purposes: e. 1986).g. may be used if their iron content is low (e. Cretaceous clays from the Oliete-Teruel basin. − chance to utilize unconventional fluxes with some clay component (e.Published on Applied Clay Science 96 (2014) 91-109.2. All rights reserved. ensuring fusibility.01. the use of BC2 with some BC3 is recommended for large sized and/or thin tiles.. in particular: Miocene clays from the Donbass basin. − priority to multipurpose raw materials (e. KL. 5. PSW2 and PSW4 in Table III): − the Fe2O3 amount of the body (0. late Paleozoic clays from Argentina. BC1). PC) are utilized together with highly plastic additives (BC3 or WB). sedimentary kaolins from Mississippi.2014. 2004. The UPS typology was developed starting from recipes inspired to porcelain: not a case if early batches did large use of kaolins and limited amounts of fluxes (i. However. especially in UPS batches.15%. bodies more suitable for fast firing were formulated during the 1990s and their basic criteria are still valid. are not considered here. 2011b. <1%). offer many degrees of freedom in body formulation. pigments and opacifiers for through-body decoration of UGS.e. 6. − Multipurpose raw materials are well tolerated. like anorthitebased.. In contrast.3.5%. GPS bodies exhibit higher iron contents. they pertain to light-firing clays and plot into the field of ball clays according to their particle size distribution and kaolinite content (Fig.. skeleton and some plasticity (SACMI. Along with typical UGS and GPS recipes. superwhite or translucent UPS.g. Copyright © 2014 Elsevier Ltd. RK). USA. within this threshold.g. unconventional types with some clay component. Fiederling-Kapteinat. 12): − Fe2O3 amount of the body in between 1% and 2%. As their iron oxide is at most 1. as Ukrainian clays are addressed to porcelain stoneware production (normally 10-30% of the batch) and secondarily to white-firing . Tennessee and Texas. 2004). − clay:non plastic raw materials ratio around 50%:50%.. The samples characterized by Galos (2011a) are here taken into account as representative of ceramic clays coming from different mines in the Donbass district. like RK. LK. Porcelain Stoneware represents the top quality floor tiles with the best technical performances and aesthetic appearance. though with little adjustments for the GPS typology (e. Zanelli et al. carbonates. glass-ceramic frits. Ukrainian clays are reknown in ceramic tile production for their plasticity and technological properties (Bal and Fiederling-Kapteinat. basic criteria to design GWS batches are (Fig. Spain. together with a pyrophyllite-based batch. 2005) to the point they are frequently considered a benchmark for high quality ball clays (Galos. raw granite acting as both flux and filler). PSW1 in Table III).g. batches distinguished essentially by the recourse to special fluxes and additives. both UPS and GPS can be used in wall coverings and ventilated façades too. etc) to fasten densification kinetics. low plasticity clays (KL. As an example. Depending on their MBI. − preferred use of clays with low to medium plasticity (LK.g..clay. particularly if they contribute to lower cost and iron oxide average content of the batch. 2011b). − Although conventional fluxes predominate. plasticizers (from WB to organic and hybrid binders) especially for large size and/or thin tiles.g. From that moment the doors have been opened for an extensive use of unconventional raw materials that. Ukraine. In this framework. 13). doi:10.1016/j. − Clays with medium to high plasticity (BC1 and BC2) are preferred. Worked examples The classification here proposed will be applied to some representative examples of clay raw materials for the ceramic industry. 30-35% of plastic component in superwhite bodies (Tenorio Cavalcante et al. the clay:non plastic ratio usually ranges from 40%:60% to 45%:55%. Mesozoic to Tertiary clays from Tunisia.7% on average) must be lower than 1.. sintering promoters (talc. Table III reports an example of pyrophyllite-based body. 2008). mineralogical. 2008. thus classifiable as LFC. 7. Late Paleozoic clays from Tandilia. Strategies of batch formulation like RMP3 and RBR2 can be envisaged. The iron-rich clays are rather coarse-grained. Copyright © 2014 Elsevier Ltd. 13). defining RC2 and RC3 types (Fig. 2010). these LFC find application in bodies where they play simultaneously the role of filler and plastic component: e. The classical terminology for ceramic tiles and related reference schemes for raw materials are no longer useful to describe and predict the role of clays in tile manufacturing and must be upgraded... Overall. Jeridi et al. these clays are in many cases classified as KL or LK.Published on Applied Clay Science 96 (2014) 91-109. (1996)— offers a wide range of composition and particle size distribution. Argentina. due to the low plasticity of these raw materials.. The case-study of the Oliete-Teruel basin in Spain —taking as example the clays characterized by GarcíaTomás et al. Iron oxide widely fluctuates from 1% to 9%. their particle size and kaolinite amount spread from RK to HK with most samples in the field where LK and BC overlap (Fig. particle size distribution and ceramic behaviour— is currently utilized in tilemaking. All rights reserved. Jeridi et al.. A wide set of ceramic clays from Tunisia were recently investigated encompassing Triassic (Medhioub et al. According to their relatively low amount of kaolinite and fraction <2 µm. 1997).. and the clay mineralogy.. Another clay with 15% pyrophyllite is likely classifiable as LK. Sedimentary kaolins from southeastern USA are here represented by data taken from Wilson (1998).. 2011). 14). It allows a more efficaceous and complete evaluation of clay resources (including valuable types not always considered among industrial minerals) along with a realistic assessment of technological potential of clays.clay. The remaning clays are predominantly kaolinitic and so attributable to the RC1 type (Fig.g. 2008. 14). 1997). Jurassic (Hajjaji et al.013 bodies for porous tiles. 2011b) in both porous and vitrified bodies up to 20% (RL) and up to 30% (RC1). However.. 1996. Both kaolins and ball clays can be widely utilized in tilemaking (Bougher. two samples plotting in the BC field can be actually defined medium plasticity ball clays on the basis of their Atterberg plastic index (Fig. Cretaceous (Felhi et al. These DFC are currently used (Meseguer et al. GPS and UPS bodies (for instance GWS3 and PSW5 in Table III). with half of samples below 3%. 2012. respectively. entailing the addition of some filler to compensate the rather fine-grained distribution.. 1996) the former in lower amount (especially in WMP and GWS batches) while the latter as the main clay component of light-firing formulations. Overall. doi:10.. Samples with the lowest plasticity and the highest kaolinite percentage are classified as RK-LK and HK. Lombardo. 2008) and Tertiary units (Felhi et al. Common features are their iron amount over 3% (DFC) and their particle size distribution mostly ranging from silty clays to clayey silts.. The remaining sample is a pyrophyllite-bearing illitic red clay (RC2). GWS1 and PSW4 batches (Table III).. These raw materials appear to be well suited for porous tiles (Azzouz et al. This picture is in agreement with current industrial use: PC (and LK) are components of GWS. particularly when large slabs have to be manufactured or if it is necessary to improve plasticity of other clay components. they present iron oxide content within light-firing clays.01.1016/j. readily transferable to the ceramic . This technological evolution has directly entailed raw materials: a really wide spectrum of clays —with an outstanding range of chemical and mineralogical composition. that discriminates MC and RC. The main distinctive parameters are the amount of carbonates. the MBI values of the other samples indicate ball clays with medium plasticity (BC1) plus two high plasticity samples (BC2) and one smectite-bearing sample of very high plasticity (BC3). with half of samples with a sandy fraction over 25% (thus classified as red loams). 13). Conclusions Ceramic tile manufacturing is a dynamic industrial sector where market trends and technological innovation have created a complex picture of products and processes. the RC2 clay can be used in GRS batches. 2003). 2011) whose bodies make use of at the same time of MC and RC (that are present in all the geological units). that however depends on the milling degree (Alló et al. A new and industry-oriented classification has been proposed on the basis of simple chemical. Hachani et al. granulometric and rheological parameters of clay materials. their use must be balanced with high plasticity clays like BC2 or BC3 (Sánchez et al. Half of samples characterized by Zalba (1979) have enough pyrophyllite (20-33%) to be described as PC and a sufficiently low iron oxide (<2%) to be used in light-firing bodies.2014. particularly for porcelain stoneware. are distinguished by high rather amounts of pyrophyllite associated with kaolinite and illite (Dristas and Frisicale. The criteria to properly design the batches for wall and floor tiles have been revised. 1997. W. World production and consumption of ceramic tiles. 55. both clay classification and body formulation criteria here proposed cannot substitute a thoroughful technological characterization of ceramic raw materials.. 103.S. Simpang Pulai.. Clay Sci. K. 11591164. J. trying to highlight the key properties for each category of ceramic bodies. Cl. Argentina. 2006. Proc.. Sci.clay. 303-310. Interceram... Qatar Univ. doi:10. Clay Sci.Y. Ceram.A. Precambrian yellow illitic clay from La Siempre Verde pit. 35. Appl. Aras. Almohandis. Gimenez.. Hadi. 119. E. Cravero. 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Typologies of ceramic tiles (acronyms from Table II) according to body colour (mostly depending on the iron oxide content) and compactness (expressed by water absorption) and their classification in agreement with ISO 13006 standard.Published on Applied Clay Science 96 (2014) 91-109. 1016/j.2014. Technological innovation in the main tilemaking stages (see text for explanation of numbered fields). 2. Copyright © 2014 Elsevier Ltd. .013 Fig. All rights reserved.01.Published on Applied Clay Science 96 (2014) 91-109.clay. doi:10. 2014.clay.01.Published on Applied Clay Science 96 (2014) 91-109.1016/j. doi:10. Evolution of typologies of ceramic tiles with technological innovation. 3. . All rights reserved. Copyright © 2014 Elsevier Ltd.013 Fig. . doi:10. 5. Classification of light-firing clays according to their amount of kaolinite group minerals and clay fraction as well as their Methylene Blue Index at pH~4 (MBIa) or Atterberg Plastic Index.clay.1016/j. All rights reserved. Copyright © 2014 Elsevier Ltd.Published on Applied Clay Science 96 (2014) 91-109. 4. Content of phyllosilicates and iron oxide in clays whose declared use is in dark-firing and light-firing bodies.01. Fig.2014.013 Fig. Particle size distribution of light-firing clays for ceramic tiles. 7. All rights reserved.1016/j. . Fig.013 Fig.2014. 6.Published on Applied Clay Science 96 (2014) 91-109.01. Mineralogical composition of light-firing clays for ceramic tiles. Copyright © 2014 Elsevier Ltd.clay. doi:10. Published on Applied Clay Science 96 (2014) 91-109.2014. Fig.1016/j. Copyright © 2014 Elsevier Ltd. doi:10. Classification of dark-firing clays according to their coarse-grained fraction. 8. amount of carbonates and clay minerals. 9. All rights reserved.01. Mineralogical composition of dark-firing clays for ceramic tiles.013 Fig.clay. . 01.clay. 11.Published on Applied Clay Science 96 (2014) 91-109. . Particle size distribution of dark-firing clays for ceramic tiles. Fig.1016/j. 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All rights reserved.) 30-45 min 40-50 (b.) 30-50 min (b.clay.5 BIa AI Resistance to deep abrasion mm3 Typical firing schedule maximum temperature duration cold-to-cold °C 960-1050 (biscuit) 940-980 (glaze) 1040-1060 (biscuit) 960-980 (glaze) 1030-1140 (biscuit) 1030-1150 1100-1150 (biscuit & glaze) time 30-40 h (b. Shaping: P=pressing.Published on Applied Clay Science 96 (2014) 91-109. & g. L=light-firing body.) 12-14 h (g. Copyright © 2014 Elsevier Ltd.013 Table II. basic requirements and firing schedule of ceramic tiles. Class Tile typology (ISO (commericial name) 13006) glaze Water absorption shaping Body type body colour Tile features Modulus of Tile type (acronym) rupture % wt. Classification.) 12-14 h (g. E=extrusion. doi:10.) majolica D P G MAJ calcareous earthenware L P G CEW red birapida D P G RBR white birapida L P G WBR red monoporosa D P G RMP 1070-1100 35-50 min white monoporosa L P G WMP 1100-1140 40-50 min rustic cotto D E(P) U RUS 17.1016/j. .01. MPa BIII POROUS >10 AIII SEMI POROUS 6-10 BIIb AIIb SEMI VITRIFIED 3-6 BIIa 0. Glaze: G=glazed tile.5-3 BIb AI VITRIFIED HIGHLY VITRIFIED <0.5 649 40-70 h cottoforte D P G CFO 18 540 950-1000 980-1060 (biscuit) 960-980 (glaze) 38-40 h (b. U=unglazed tile.) 35-40 h (b.) red stoneware D P G GRS 18 (BIIb) 22 (BIIa) 30 (BIb) 540 (BIIb) 345 (BIIa) 175 (BIb) 1120-1160 20-50 min klinker L E U KLK 23 275 1100-1200 40-70 h red stoneware D P U URS 30 175 980-1000 42-45 h white stoneware L P G GWS 30 175 1170-1200 35-50 min porcelain stoneware L P G GPS 40-60 min porcelain stoneware P(E) U UPS 175 1190-1220 L 35 1200-1230 45-75 min 15 no prescription (BIII) 2365 (AIII) Body colour: D=dark-firing body. clay. doi: 10.Published on Applied Clay Science 96 (2014) 91-109 Copyright © 2014 Elsevier Ltd. All rights reserved.2014. clay raw materials (% wt) Tile typology White Monoporosa White Birapida Glazed Stoneware Porcelain Stoneware HK-LK WMP1 WMP2 WMP3 WMP4 WBR1 WBR2 WBR3 WBR4 GWS1 GWS2 GWS3 PSW1 PSW2 PSW3 PSW4 PSW5 KL-RK 20-30 20-40 10-20 10-20 10-20 15-35 0-10 10-20 0-20 0-20 35-45 12-18 0-10 0-20 10-15 10-20 10-20 10-15 15-25 0-20 0-20 10-20 0-20 BC 50-75 30-40 30-50 20-30 20-30 20-30 15-45 30-50 10-15 10-35 0-30 12-18 27-32 30-40 10-30 0-20 PC 25-40 20-40 20-40 other components (% wt) porefiller flux forming 10-15C 10-40 0-10 7-10C 15-25 5-10 C 8-12 0-20 5-20W 0-20 10-20 20-30 5-10 30-40 30-40 10-20 W 5-20 5-10 25-35 10-15 30-45 10-30 35-50 30-40 12-18 27-32 5-10 42-48 5-15 45-55 5-15 40-50 0-10 40-50 Pore-forming agent: C=carbonates (calcite and/or dolomite). Examples of batch formulation for dark-firing bodies. Table IV.01.1016/j. clay raw materials (% wt) Tile typology Red Monoporosa Red Birapida Glazed Red Stoneware Rustic Cotto MC RMP1 RMP2 RMP3 RMP4 RMP5 RBR1 RBR2 RBR3 RBR4 GRS1 GRS2 GRS3 GRS4 GRS5 RUS1 RUS2 CC 50-60 20-40 35-45 20-25 15-20 70-80 60-70 20-40 5-15 RC 10-20 30-50 40-50 40-60 40-60 10-20 20-30 40-50 60-80 65-80 60-80 60-70 90-100 65-80 RL other components (% wt) porefiller flux forming 15-20 0-10 20-40 0-10 15-25 0-20 20-50 7-12 0-20 0-20 0-20 10-20 20-40 10-20 0-20 0-20 0-20 0-20 0-20 10-25 0-10 10-15 0-20 0-20 100 70-90 Pore-forming agent: C=carbonates (calcite and/or dolomite) 36 15-20 10-30 .013 Table III. Examples of batch formulation for light-firing bodies. W=wollastonite.