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Keywords: Feldspathic fluxes are fundamental ingredients of many ceramic products, but little is known about the sources
Ceramics actually utilized by industry and the evolution over time. This paper reviews the sourcing of feldspathic raw
Feldspar materials over a long timespan (1971–2016) including viable substitutes (particularly recycled materials and
Flux end-of-life products). A large set of data was collected, critically assessed and elaborated to get an original
Material flows
insight into market dynamics. In addition, the technological value, based on composition and technological
Raw materials
properties of different fluxes, is referred to ceramic use and batch design. A detailed analysis of ongoing trends,
Waste recycling
mainly driven by the technological innovation in the ceramic tile industry, disclosed possible criticalities in the
medium-term supply of key raw materials, principally sodium feldspar from albitites. To mitigate this risk, three
actions are envisaged to improve the resource efficiency and sustainability of feldspathic fluxes: 1) full valor-
ization of primary deposits, 2) increasing recourse to alternative sources, 3) relaxing the technological con-
straints in ceramic applications.
https://doi.org/10.1016/j.resconrec.2018.02.027
Received 12 January 2018; Received in revised form 21 February 2018; Accepted 21 February 2018
0921-3449/ © 2018 Elsevier B.V. All rights reserved.
M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
Fig. 1. Distribution of the main mining districts of feldspathic raw materials currently in operation (Dondi, 2018).
through collection, critical assessment and elaboration of data from a 3. Sources of feldspathic raw materials
wide range of literature as well as statistical and industrial sources. The
goal is to get an insight into the dynamics that are taking place in the 3.1. Naturally-occurring raw materials
market of feldspathic raw materials, as dictated by changes in the de-
mand by the major end-users, firstly ceramic tiles and sanitaryware Feldspathic raw materials are mined from a wide range of deposits
industries. This is essential to draw future scenarios, which can be in different geological contexts (Fig. 1 and Table 1). In addition, fluxes
helpful to assess any risk for secure supply and plan sustainable actions are recovered from secondary sources too.
on both industrial sides: producers and end-users of feldspathic fluxes. The main sources are granitic suites, including acid differentiates
(pegmatites and aplites) and the corresponding extrusive and hypa-
byssal terms (rhyolites, porphyries). Leucogranites are the most im-
2. Methodological approach portant resources among granitoids. Relevant deposits are in operation
at: Spruce Pine, North Carolina, and Monticello, Georgia, United States
Data on the production of feldspathic materials were collected from (Potter, 2006); in the Serie dei Laghi, Piemonte, Italy (Grisoni and
the official statistics of each country, when accessible, integrated with Boriani, 1990); Montebras, Allier, France (Dudoignon et al., 1988);
general databases (Taylor et al., 2005; Brown et al., 2016a, 2016b; Lower Silesia, Poland (Ciesielczuk et al., 2008; Lewicka and
Reichl et al., 2015; USGS, 1971–2017; EC-RMIS, 2017) and information Wyszomirski, 2010); Jundiaí, Itupeva, Sorocaba and Mogi das Cruzes,
made available by mineral suppliers (ICerS, 1995–2016). For some São Paulo, Brazil (Motta et al., 1998; Motta, pers. comm.)
countries, a reverse estimation of the actual flux consumption was Pegmatites are the traditional source of feldspar and dozens of
carried out, based on the ceramic tiles production figures (Baraldi, aplito-pegmatitic fields are mined all over the World (Černý and Ercit,
2017), in order to check the declared feldspar outputs and get reliable 2005; Dill, 2015). The major districts are in:
and robust figures. This operation was performed for any ceramic ty-
pology, whose amount of flux is known on average, under the as- - India, Rajasthan (Joshi et al., 2014) and Andhra Pradesh (Sarkar,
sumption of reasonable values for bulk density and thickness of ceramic 2001).
tiles in order to convert the tile production (expressed in square meters) - Thailand, in the Ratchaburi, Ranong and Tak provinces
into mass of ceramic body (expressed in tons). (Suwimonprecha et al., 1993).
Additional information was gathered and elaborated to extract the - Argentina, in the Sierras Pampeanas (Galliski, 2009).
share attributable to different feldspar sources. This step was accom- - China, in Fujian (Yueqing et al., 1987) and Altaj Range in Xinjiang
plished country by country, through a careful evaluation of the litera- (Zhang and Chen, 2010).
ture (e.g., McLemore, 2006; Potter, 2006) including reports of national - Iran, particularly in the Sanandaj-Sirjan zone (Masoudi et al., 2002;
geological surveys and mining authorities (e.g., Coelho, 2009; Starý Khalaji et al., 2007).
et al., 2016; Indian Minerals Yearbook, 2017). However, an exhaustive - South Africa, in various areas of the country (Von Backstrom, 1976).
referencing goes beyond the scope of the present paper and the reader is - Portugal, in the north and centre of the country (Antunes et al.,
addressed to an extensive review of flux deposits (Dondi, 2018). 2013; Neiva et al., 2012).
A particular attention has been paid to fluxes that are in use as - Brazil, principally in Borborema-Seridó, Paraíba and Rio Grande do
substitutes of feldspars, with special care on recycled materials, such as Norte (Beurlen, 1995) and the Eastern Brazilian pegmatite province,
mining residues, waste glasses, and so on. Minas Gerais and Bahía (Bilal et al., 2001).
Although the whole set of data extends along the period 1971–2016,
the discussion has been focused on the last two decades (since 1994 The major deposits of ‘aplite’ are in the Shigaraki area, Shiga and
through 2016). Mie prefectures, Japan (Hirano and Sudo, 1994); Botro ai Marmi,
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M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
Table 1
Sources of feldspathic raw materials for the ceramic industry.
Granitoids GRA Coarse-grained plutonic rocks, rich in feldspars and oversaturated in silica (quartz > 20%). Fluxes Spruce Pine, USA; Montebras, France;
are mainly recovered from granites (particularly leuco-granites) with minor granodiorites, Strzeblow, Poland.
alkaligranites, and some trondhjemites.
Pegmatites PEG Very coarse-grained basement rocks, abundant in feldspar, which in most cases are acid Sierras Pampeanas, Argentina; Black
differentiates of granitoids (or syenoids). Fluxes come from all subtypes: plutonic pegmatites, Hills, USA; Kyrkoberget, Finland.
pseudo-pegmatites, meta-pegmatites and pegmatoids.
Aplites APL Differentiates of granitoid (or syenoid) rocks with a fine-grained texture. Some fluxes are Botro ai Marmi, Italy; Shigaraki, Japan;
commercialised as “aplites”, as they exhibit an (apparent) aplitic texture, e.g. due to rock Montpelier, USA.
alteration.
Acid volcanics and RHY Extrusive acid rocks (rhyolite, rhyodacite, dacite, comendite) including subvolcanic and Ahuazotepec, Mexico; Lozzolo, Italy;
subvolcanics hypabyssal types (porphyry). Fluxes are recovered from lavas, domes, pyroclastics (cinerite, tuff, Türkismühle, Germany.
ignimbrite, and perlite) and veins.
Nepheline syenites and NSP Silica-undersaturated rocks containing feldspars and feldspathoids (nepheline, leucite, etc). Fluxes Blue Mountain, Canada; Stjernøy,
phonolites are typically obtained as nepheline syenite or its extrusive equivalent nepheline phonolite, but also Norway; Lages, Brazil.
ultrapotassic rocks can be utilized.
Feldspathic arenites ARK Feldspathic sandstones and conglomerates (and the corresponding unlithified sediments). Fluxes Florinas, Italy; Carrascal del Río, Spain;
are mostly recovered from arkoses and subarkoses, with some lithic arkoses as well. Hirschau, Germany.
Metamorphics MET Metamorphic equivalents of previous deposits (e.g., gneiss, porphyroid, micaschist, quartzite) Itapeva, Brazil; Campo Largo, Brazil;
mostly in the greenschist facies. Fluxes are mainly obtained from phyllites and gneisses. Robilante, Italy.
Albitites ALB Metasomatic rocks formed through an albitization process that leads to the formation of almost Menderes, Turkey; Ottana, Italy;
monomineralic bodies (albite after plagioclase and K-feldspar) under the action of metamorphic Salvezines, France.
fluids.
Epithermal alterations EPI Hydrothermal alteration giving rise to peculiar rock types: porcelain stone, eurite, agalmatolite, Amakusa, Japan; Crocetta, Italy; Gusev,
pinite, toseki and roseki (in Japanese), dunzi or baidunzi (in Chinese) including episyenite and Russia.
sanidinite.
Alternative sources Low-melting minerals alternative to feldspars; end-of-life materials and byproducts, typically see Table 3
feldspar bearing or largely glassy, such as mining residues, waste glasses, and combustion ashes.
Tuscany, Italy (Loschi Ghittoni, 1972) and Montpelier, Virginia, United Deposits generated through low temperature hydrothermal (epi-
States (Potter, 2006). thermal) alteration provide a set of peculiar fluxes (e.g., eurite and
Acid volcanic and subvolcanic rocks, essentially rhyolites and por- pottery stone) characterized by a significant amount of low melting
phyries, are important sources of fluxes in Mexico, Ahuazotepec near minerals, such as sericite. Important deposits are in Japan for pottery
Puebla (Solana Lopez, 2012); Germany, across Saarland and Rheinland- stone, e.g. Amakusa and Taishu (Hirano and Sudo, 1994; Nakagawa and
Pfalz (Bornhöft and Kleeberg, 2012); Italy, in Piemonte (Quick et al., Matsuura, 1994) and in Italy for eurite at the Elba Island, Tuscany
2009), Tuscany (Viti et al., 2007) and Sardinia (Bornioli et al., 1994); (Maineri et al., 2003; Benvenuti et al., 2006).
Russia, Kostomuksha and Roza-Lampi, Karelia (Il’ina et al., 1999); There has been a rather balanced recourse to such different sources,
Turkey: Kireç, Bileçik (Kara et al., 2009) and Ilgin, Konya (Kayaci et al., as it stands out considering the cumulative production in the period
2010). 1971–2016 (Fig. 2A). Along with the main types (albitites, granites,
A few alkaline complexes with silica-undersaturated rocks are sup- pegmatites, and nepheline syenites), there is a significant contribution
plying the ceramic industry. Nepheline syenite come basically from: by all the other sources, which in many cases have a strong importance
Canada, Blue Mountain in Ontario (Payne, 1968); Norway, Lillebukt in locally, as for feldspathic sands, aplites, acid volcanics, phyllites and
the Stjernøy island close to the North Cape (Geis, 1979); Russia, Vish- epithermal alterations.
nevogorsk in Southern Urals (Nedosekova et al., 2009). Its extrusive However, the current picture is substantially altered by the out-
equivalent (nepheline phonolite) is mined principally in: Brazil, Lages standing increase in the output of albitites, which ensures around 37%
in Santa Catarina (Aumond and Scheibe, 1996); Germany, Brenk in the of the present flux demand worldwide. Apart pegmatites, which slightly
Eifel (Bornhöft and Kleeberg, 2012); Czech Republic, Zelenický vŕch, grew their share, the remaining sources see their slices shrink in the
Northern Bohemia (Pazdernik, 1997). global pie: moderately for granites and feldspathic arenites, but con-
Fluxes of sedimentary origin are obtained from feldspathic arenites, sistently for the remaining fluxes (Fig. 2B).
mainly arkoses. The countries where this source is largely exploited are: A completely different perspective is offered by considering the
Italy, Loiano Formation in the northern Apennines (Bertolani et al., number of mines in operation. Two thirds of deposits under exploitation
1984); Sassarese-Logudoro in Sardinia (De Carlo et al., 1990) and are in pegmatitic fields, while the mines active on albitites and granites
Fossanova, Latium; Spain, Carrascal del Río and Río Pirón, Segovia sum up to about 9% and 7%, respectively, of the total number. All the
(Sánchez Muñoz and García Guinea, 1992); Germany, Hirschau- other sources have shares below 5% (Fig. 2C). This implies a different
Schnaitterbach in Bavaria (Dill et al., 2016); Unites States, in California, size of mines (Table 2): much larger for albitites (on average 129
Arkansas, and Idaho (Potter, 2006). thousand tons per year) than for pegmatites (mean output 10 thousand
Metamorphic and metasomatic rocks are extensively utilized by the tons per year). The other sources have a mean production per mine
ceramic industry, especially albitites and phyllites. The largest albitite comprised between approximately 23 and 74 thousand tons per year.
deposits are in the Menderes massif in southwestern Turkey (Çakır, The recourse to the different sources of fluxes, all along the period
2005; Uygun and Gümüşçü, 2000). Further big mining districts are in 1994–2016, is pictured in Fig. 3. Despite some annual fluctuations, like
central Sardinia, Italy (Palomba, 2001; Castorina et al., 2006) and those in correspondence of the economic recession in 2008–2013, a
eastern Pyrenées, France (Boulvais et al., 2007; Poujol et al., 2010). general trend clearly stands out.
Phyllites are essentially mined in Brazil (Biondi and Marczynski 2004; The classic sources based on granitoids and acid differentiates
de Andrade et al., 2008) with the major deposits in São Paulo (Itapeva (pegmatites, aplites, granites, porphyries) denote a declining relative
and Pirapora do Bom Jesus), Paraná (Campo Largo) and Minas Gerais importance, since their contribution to the global market of fluxes went
(Igarapé). from ∼60% (in the early 1990s) down to the current ∼40%. Other
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M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
Fig. 2. Contribution of the various sources to the total output of feldspathic fluxes: (A) cumulative production in the period 1971–2016 and (B) year 2016. Number of mines in operation
in the last decade for each source (C).
Table 2
Estimated outputs and number of mines operating on feldspathic fluxes.
Sources Output (thousand tons) Number of operating mines Mean output per mine
(2016) (1000 t per year)
1971–2016 2007–2016 2016
fluxes – like feldspathic arenite, nepheline syenite, phyllite and pottery 3.2. Secondary raw materials
stone – suffered a less accentuated (relative) contraction, since their
share passed from ∼30% (early 1990s) to the present ∼25%. It was the Along with primary deposits, ceramic fluxes are collected from al-
outstanding growth in albitite production, which increased from ∼10% ternatives sources as well. The idea to substitute feldspar in ceramic tile
(early 1990s) to ∼40% nowadays, to revolutionize the international bodies by non-conventional fluxes goes back at least to the 1970s.
market (Fig. 3). Nevertheless, a detailed review of these attempts goes beyond the scope
of this paper. Thus, only feldspar substitutes that actually went on
Fig. 3. Relative importance of the different sources of ceramic fluxes in the period 1994–2016. Abbreviations as in Table 1.
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M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
Table 3
Fluxes used in ceramic tilemaking as alternative to feldspathic materials.
Alternative minerals rocks containing low melting components that can act as flux, like sericite, volcanic epithermal alterations (Table 1) talc, diopside,
glass, and so on. chlorite, dolomite.
Mining residues quarry dumps of ornamental stones. granite, gneiss and quartzite dumps.
tailings from processing of feldspathic rocks and ornamental stones. granite fines, granite and quartzite cutting and
polishing sludges.
End-of-life products secondary raw materials from the selective recovery of municipal wastes. waste glasses from: bottle, PC-TV screen, lamp and
vial.
Processing wastes residues of ceramic manufacturing, as fired scraps and wastewater or grinding sludges. porcelain stoneware or vitreous china scraps and
grinding sludges.
mainly outcome of combustion processes, like municipal waste incinerator ashes and stabilized municipal waste incinerator ash, wood ash.
biomass-based thermal power plant ashes.
production are here considered. They can be reconducted to the four Another source of secondary raw materials is the manufacture of
sources in Table 3. vitrified ceramics, such as porcelain stoneware tiles and vitreous china
The market relevance of fluxes alternative to feldspathic materials is sanitaryware, which generates both fired scraps and processing sludges,
rather differentiated: from raw materials widely utilized by the ceramic e.g. from wastewater treatment or grinding operations. The ceramic
industry to secondary materials seldom in use. Alternative low-melting industry can cannibalize such residues, being to a large extent glassy, in
materials – like sericite featuring epithermal alterations or natural glass partial replacement of conventional fluxes (Rambaldi et al., 2007b;
in volcanic rocks – are constituents of well-known fluxes, such as pot- Nandi et al., 2015; Tarhan et al., 2017).
tery stone (Hirano and Sudo, 1994; Nakagawa and Matsuura, 1994), Some municipal wastes, such as stabilized incinerator ashes
eurite (Maineri et al., 2003; Benvenuti et al., 2006) or some rhyolite (Andreola et al., 2001; Rambaldi et al., 2010; Schabbach et al., 2012)
(Bornioli et al., 1994; Kayaci et al., 2010). have been experimented as secondary raw materials by the ceramic tile
Further industrial minerals are sometimes employed in ceramic industry and in a few cases entered in use for a while. Their extremely
batches, but in low amount, as a sort of sintering promoter, like talc high fusibility, particularly in case of biomass combustion ashes from
(McCarthy et al., 2006), diopside (Azarov et al., 1995; Kuzmickas et al., thermal power plants, makes them good candidates as fluxes, but sev-
2013), dolomite (Ke et al., 2013), chlorite-bearing rocks (Biasini et al., eral technological hindrances are still to be overcome prior any gen-
2003) and basic igneous rocks (Kelling et al., 2000). eralised utilisation. As a matter of fact, there are problems in handling
Feldspathic materials can be obtained from quarry dumps, instead and storage (due to hygroscopicity and reactivity with moisture), slip
of freshly mined rocks, with environmental benefit and slope stabili- rheological behavior (boost in viscosity) and high iron content (darker
zation as well (Dino et al., 2012). This source – mostly residing on colour after firing).
granite (Bozzola et al., 1995a 1995b), gneiss (Souza et al., 2010), and
quartzite dumps (Dino et al., 2005) – is important for some ceramic 4. Technological value
districts. Further mining residues − such as tailings from granite (Eddy,
1972; Hojamberdiev et al., 2011) or pegmatite (Pereira Leite et al., Ceramic batches are designed to fulfil several technological re-
2014) beneficiation – have been proposed and perhaps found some quirements, which involve both the behavior during processing and the
local utilisation in the ceramic industry. An extensively investigated product performance (Singer and Singer, 1963; Dondi et al., 2014). In
case is that of sludges from cutting and polishing of ornamental stones, order to ensure the desired properties, different types of raw materials
particularly granite (Acchar et al., 2006; Aguiar et al., 2014; Gadioli have to be utilized, each playing a specific role in the manufacturing
et al., 2012; Hernández-Crespo and Rincón, 2001; Menezes et al., 2002, steps (Table 4).
2005, 2008; Segadães et al., 2005; Torres et al., 2004, 2007). However, The technological role of fluxes in ceramic bodies mainly consists in
they have not found a generalised use yet, because of technological forming a liquid phase during firing by melting alkali feldspars, sericite
problems connected with contaminants introduced during the proces- and further minerals. This phenomenon can involve also other phases,
sing, especially steel dust (after grinding media) and lime (added as like quartz, giving rise to eutectic-like melts (Becker et al., 1999). Such
sludge thickener). a liquid phase fills at high temperature the original porosity of unfired
The use of end-of-life products, essentially glassy materials from bodies and promotes densification by viscous flow (Cambier and
municipal waste sorting, is a target since a long time (Brown and Leriche, 1996; Zanelli et al., 2018). Finally, the liquid turns into a
Mackenzie, 1992). In the last decade, it turned into a common practice vitreous phase during cooling, so embedding fillers and ensuring the
in some supply chain of the ceramic tile industry (Bozzola et al., 2012). technical performance of the ceramic product (Sánchez et al., 2006,
A successful option consists in adding a few percent of waste glass to a 2010). The sintering kinetics mostly depends on the viscosity and sur-
feldspathic raw material in order to improve its fusibility (Carbonchi face tension of the liquid phase, which in turn is function of the che-
et al., 2003). The positive impact of recycling is strengthened when we mical composition of glass (Zanelli et al., 2011). For this reason, the
are dealing with a waste-of-waste, i.e. a residue of processing to recover chemical composition of fluxes is a key point to predict their techno-
a secondary raw material for the glass industry (as in the case of bottle logical behavior and effects during sintering.
glass sorting). The end-of-life products currently utilized in ceramic
manufacturing encompass glasses of various origin and composition: 4.1. Composition and technological properties of primary fluxes
- soda-lime container glass (Matteucci et al., 2002; Rambaldi et al., The fluxes coming from the various sources are characterized by
2007a; SASIL, 2009). their own composition for a combination of different factors: from
- BaO- and SrO-rich glass from PC-TV screen (Raimondo et al., 2007; petrologic and mineralogical traits to the yield during beneficiation
Andreola et al., 2010). treatments. An averaged chemical and mineralogical composition,
- borosilicate vial glass (Andreola et al., 2016). calculated as a touchstone for commercial fluxes, can be used to com-
- different glasses from various types (incandescence, neon glow, fluor- pare different sources (Table 5). Granitoids and acid differentiates
escence, and led) of lamps (de Araújo et al., 2014; Kim et al., 2016). usually provide mixed Na-K fluxes with a more or less abundant quartz.
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Table 4
Basic technological roles of the components of a ceramic tile batch.
Plasticity provider forming a stable water suspension (slip); allowing a proper compaction during pressing; bestowing ball clay, red clay, marly clay, kaolin.
mechanical strength on unfired tiles; precursor of mullite (kaolinite-bearing).
Flux forming a liquid phase at high temperature; allowing the body densification by viscous flow; creating a feldspathic fluxes, talc, Li-minerals,
vitreous phase embedding fillers. dolomite, glasses.
Filler acting as skeleton that helps to control the tile shrinkage during drying and firing; damping pyroplastic quartz, silica sand, quartz-feldspathic
deformations by increasing the body viscosity at high temperature. fluxes, chamotte.
Additive modulating single issues of the technological behavior, e.g., slip rheology, green density, dry bending deflocculant, binder (bentonite), whiting
strength, firing shrinkage, pyroplasticity, colour after firing. (zircon, calcite).
Table 5
Averaged composition of commercial fluxes from primary sources.
Granitoids Pegmatites Aplites Acid volcanics and Nepheline syenites Feldspathic Metamorphics Albitites Pottery stones
subvolcanics and phonolites arenites (phyllites) and eurites
n 58 120 32 25 24 84 19 43 53
SiO2 73.11 69.12 70.87 74.28 58.13 83.99 69.01 68.88 74.48
TiO2 0.06 0.06 0.14 0.12 0.19 0.09 0.55 0.22 0.17
Al2O3 15.14 17.32 17.02 14.24 22.45 8.74 18.40 18.30 16.50
Fe2O3 0.32 0.19 0.29 0.81 0.76 0.32 1.99 0.26 0.63
MgO 0.11 0.14 0.22 0.28 0.29 0.17 1.03 0.87 0.27
CaO 0.74 0.55 0.88 0.56 1.06 0.64 0.21 0.91 0.48
Na2O 4.17 4.18 5.15 1.93 8.63 1.26 0.39 9.12 0.87
K2O 5.21 7.63 4.57 5.81 6.72 3.89 4.44 0.51 3.71
L.o.I. 0.67 0.60 0.75 1.98 1.46 1.03 3.94 0.79 2.61
Total 99.53 99.79 99.89 100.01 99.68 100.12 99.93 99.87 99.73
Plagioclase 39 38 48 19 33 14 4 82 10
K-feldspar 31 45 27 34 40 23 – 3 –
Nepheline – – – – 23 – – – –
Sericite – – – – – – 38 – 31
Quartz 27 14 21 39 – 60 45 11 51
Accessories 3 3 4 7 4 3 13 5 8
Fusibility very low to low to high low to high very low to low very high very low to low low to medium high low to medium
medium
Nevertheless, pegmatites allow a selective mining, by which potassic high amounts of iron and alkaline-earth oxides, as typically seen for
(and sometimes sodic) feldspar can be recovered. Fluxes mined from basic rocks (e.g., basalts).
acid volcanic rocks – and especially porphyries – are characterized by
K > Na and a high amount of silica minerals.
Such a potassic signature is found in fluxes obtained from arenites as 4.2. Composition and technological properties of secondary fluxes
well, where orthoclase is typically prevailing over plagioclase, together
with a very high percentage of quartz. Also phyllites, eurites and pot- In general, fluxes obtained from alternative sources exhibit a com-
tery stones are in general predominantly potassic and rich in quartz, but pletely different composition with respect to conventional feldspathic
here the main alkali source is frequently sericite. Albitites represent the materials (Table 6). Exception is made of some mining residues, and
main source of sodic feldspar (Na ≫ K) with a low amount of quartz. particularly those recovered from dumps of ornamental stones, which
Nepheline syenites and phonolites provide quartz-free, mixed Na-K have chemical and mineralogical features analogous to granitoids, and
fluxes with a more or less significant amount of nepheline. consequently a rather low fusibility.
A specific technological behavior, notably in terms of fusibility, can Overall, waste glasses constitute a class with a great compositional
be associated to these compositional features (Table 5) and can be variance, due to the wide range of applications (container, screen,
graphically expressed by contrasting the softening and melting tem- lamp, vial, etc) each requiring its own glass performance and chemistry.
peratures (Fig. 4): Compared to feldspathic fluxes, waste glasses usually have a low per-
centage of alumina and a high amount of alkaline and alkaline earth
- very high fusibility is exhibited by quartz-free and feldspathoid- oxides. In addition, some types contain elements – like barium, stron-
bearing fluxes, remarkably rich in feldspars, like nepheline syenites tium and boron – that in primary fluxes are present just in traces. Such
and phonolites; chemical features bestow on these secondary fluxes an extremely high
- high fusibility is characteristic of quartz-poor and feldspar-rich fusibility, with softening and melting temperatures comparable to ba-
fluxes, particularly when sodic terms are prevailing, as in albitites salts in Fig. 4 and even lower. These characteristics render the waste
and some pegmatites and aplites; glass an ideal additive, playing as sintering promoter, but turn difficult
- medium to low fusibility is found for quartz-poor fluxes, based on its introduction in large amount into a ceramic batch in replacement of
mixed Na-K feldspars or sericite, as happens with most pegmatites, feldspathic materials.
aplites, phyllites and some granitoids; Ceramic scraps are perfectly compatible with primary fluxes, of
- low to very low fusibility is observed when fluxes have large amount course, being in origin a mixture of feldspars, quartz and clay minerals.
of quartz and mixed feldspars, especially with a potassic signature, Consequently, these wastes are richer in alumina and poorer in alkalis
like in the case of many granitoids, acid volcanics and arenites; than many feldspathic materials. Their technological behavior is similar
- extremely high fusibility occurs just in case of low-silica fluxes with to quartz-rich, mixed Na-K fluxes and characterized by a low fusibility.
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Fig. 4. Fusibility chart (modified after Dondi et al., 2001) of feldspathic fluxes from different sources, based on softening and melting (half-sphere) temperatures, as measured by hot-
stage microscopy.
4.3. Fluxes in ceramic batch design at a relatively low temperature (1180–1220 °C, as in the case of por-
celain stoneware and fine stoneware) it is necessary to increase the flux
Fluxes are introduced in the various ceramic batches in different percentage to 45–65% (favored are sodic terms). Furthermore, felds-
amount: from a few percent up to 60% and over (Fig. 5). The quantity pathic raw materials are sometimes used in porous and/or red-firing
of flux depends on the characteristics of finished products: porous, bodies as well, despite the low firing temperature (1050–1150 °C) at
semi-vitrified or vitrified bodies, and engobes or glassy coatings which a dual role is played: filler and to a minor extent fluxing.
(Sánchez et al., 1990; Galán and Aparicio, 2006; Dondi et al., 2014). Therefore, fluxes play a key-role in vitrified products (porcelain,
These features are somehow related to the sintering temperature, which vitreous china, porcelain stoneware, fine stoneware) where the che-
in turn is function of the amount and physical properties at high tem- mical composition of raw materials determines the firing behavior and
perature of the liquid phase (Becker et al., 1999, Conte et al., 2018). basic technological properties, like the sintering kinetics and pyr-
Vitrified bodies, like porcelain and vitreous china, are fired at high oplasticity (Buchtel et al., 2004; Zanelli et al., 2011; dos Santos
temperature (≥1300 °C) and require a moderate amount of flux Conserva et al., 2017). Nevertheless, the industrial use of fluxes is
(15–30%, preferentially potassic). In order to get highly vitrified bodies changing upon the driving force of environmental sustainability and
Table 6
Composition of commercial fluxes from alternative sources.
Granite dump Gneiss dump Container glass PC TV screen Fluorescent lamp LCD screen Porcelain Vitreous MWIBA MWIBA
(ICerS, (Souza et al., (ICerS, glass (Andreola glass (Andreola glass (Kim stoneware scrap china scrap (Schabbach (Rambaldi
1995–2016) 2010) 1995–2016) et al., 2010) et al., 2016) et al., 2016) (Rambaldi et al., (Tarhan et al., 2012) et al., 2010)
2007b) et al., 2017)
SiO2 75.90 66.43 71.60 61.23 68.89 60.10 64.06 74.29 47.40 34.22
TiO2 0.02 0.83 0.07 0.35 – – 0.48 0.40 0.75 1.54
ZrO2 – – – 0.91 – – 1.10 0.19 – –
B2O3 – – – – – 10.30 – – 0.56 –
Al2O3 11.10 17.26 2.40 2.56 2.29 16.80 16.54 21.44 9.95 13.46
Fe2O3 0.19 3.70 0.35 0.10 0.08 0.03 0.50 0.90 4.38 5.73
MgO 0.40 0.32 2.00 0.76 3.00 0.44 4.63 0.29 2.91 4.67
CaO 2.70 2.23 9.70 1.13 5.16 7.60 1.40 0.52 18.80 35.58
ZnO – – – 0.18 – – – – 0.34 0.26
SrO – – – 8.84 0.07 4.20 – – – –
BaO – – – 10.03 0.95 0.48 – – – –
PbO – – – – – – – – 0.31 0.32
Na2O 5.20 1.01 12.70 8.27 17.75 – 4.43 0.09 – 2.29
K2O 4.00 7.49 1.00 5.56 1.62 – 2.05 0.99 – 1.68
P2O5 – – – – – – – – 1.26 –
SO3 – – – – – – – – 1.01 –
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M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
Fig. 5. Amount of flux (weight percent) introduced in industrial batches for various ceramic products.
technological innovation. In the latest years, the ceramic industry is addition, the recent trend is outlined as production in the last decade
increasingly demanding for fluxes with high fusibility, because they and difference between 2007 and 2016 (plus/minus).
allow to move towards a sustainable manufacturing through a double Gathering all data, the global output of feldspathic raw materials
action: sums up to 28.779 million tons in 2016: a figure distinctly greater than
the total elaborated by different databases, which range from 22.7
- ensure a lower temperature and a shorter time of firing in order to million tons (USGS, 1971–2017) to 26.2 million tons (Brown et al.,
reduce the energy consumption per unit of finished product; 2016b) or 26.8 million tons (EC-RMIS, 2017). This is to a certain extent
- enable the use of other fluxes with low or very low fusibility, justified by the inclusion of alternative fluxes, particularly pottery stone
available locally and/or at a lower price, in order to improve the and phyllite.
resource efficiency. The evolution of the global production highlights a continuous
growth over time (Fig. 7A) but for some strong fluctuations occurred in
The substantial role played by innovation in varying the use of raw the last decade, most in charge of albitite suppliers (Fig. 7B). They are
materials is here exemplified by trends occurring in the Sassuolo- essentially linked to market dynamics in the Mediterranean countries in
Scandiano district, which has the technological leadership for ceramic correspondence with the economic recession in the period 2008–2012.
tiles (Fig. 6). Within this sector, porcelain stoneware is continuously Such a general increment in the production of feldspathic raw materials
gaining market share, especially with the present traction towards ever took place according to three main trends:
larger sizes, reaching 120 × 240 cm up to 180 × 480 cm each slab
(Raimondo et al., 2010). The bodies utilized for such large slabs require 1) A slight increase, at the average rate of +162 thousand tons per
a high amount of fluxes (preferentially sodic to improve the sintering year, occurred along two decades (1971–1990). The ongoing model
kinetics) and a lower filler-to-flux ratio (to minimize the risk of cooling was substantially based on the flux consumption by domestic
defects). This trend is inducing a growing demand for fluxes from al- ceramic and glass industries, with the exception of some products
bitites that reverberate in the international market, since all the other with a significant export share (potassic feldspar and nepheline
ceramic tile districts are starting to manufacture porcelain stoneware syenite).
large slabs. 2) A fast growth observed in the period 1991–2005, at the average
pace of +546 thousand tons per year. It was essentially driven by
the mounting demand from ceramic tiles makers, depicted in Fig. 7A
5. Trends in the production of feldspathic raw materials
in terms of tonnage of raw materials utilized in their batches. Such
an expansion was made possible by the increasing productive ca-
Information on the production of feldspathic materials and alter-
pacity, at a similar rate, of pegmatites, granites, arenites, and par-
native fluxes, arranged country by country, is provided in Table 7.
ticularly albitites; the other sources exhibit a steady output or just a
Along with the estimated output in 2016, the cumulative amount in the
slight increment in the same period (Fig. 7B). This situation marks
period 1971–2016 is indicated together with the peak production. In
an enlargement of the international market of feldspathic raw ma-
terials, dominated by the albitite exportation from Turkey, and the
set-up of a stable supply chain to the major tile-making districts,
especially Sassuolo-Scandiano in Italy.
3) A booming output in the last decade, at the average rate of +777
thousand tons per year. It is still well correlated with the increasing
demand from the ceramic industry (Fig. 7A) and justified by the
worldwide diffusion of the production of porcelain stoneware tiles
(whose batches contain the largest amount of fluxes, see Fig. 5) prior
basically restricted to Italy. At variance with the previous trend,
such a further growth has been fundamentally implemented through
an expansion in the capacity of albitite producers (and to a minor
extent of pegmatite suppliers) since the other sources show just a
Fig. 6. Raw materials used in ceramic tiles manufacturing: estimation since 1990 and limited production increment or even a diminution since 2006, as
prediction to 2020 of the average batch in the Sassuolo-Scandiano district (Italy). for arenites and aplites (Fig. 7B).
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M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
Table 7
World production of feldspathic fluxes (and alternatives).
country output 2016 peak production cumulative 1971–2016 last decade 2007–2016 plus/minus (2016)–(2007)
Fig. 8 depicts how such changes in the flux demand affected the important developments concerning pegmatites (+130%), feldspathic
extractive capacity of each source over the last two decades, i.e. cov- arenites (+105%), granitoids (+100%) and phyllites (+95%). A minor
ering the trends 2 and 3 above described. Along with the outstanding increment is registered for nepheline syenites (+60%) and acid vol-
growth in the production from albitite deposits (on average 340,000 canics (+30%), whilst the output of aplites and epithermal alterations
tons more every year, about 400% of increment) there are also appears to be in contraction (−25% and −50%, respectively).
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M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
Fig. 7. Trends in the production of feldspathic raw materials and alternative fluxes: global output in the period 1971–2016, compared with the demand from the ceramic tile industry (A);
contribution of the different flux sources in the period 1994–2016 (B).
The ranking of the most important producers of feldspathic raw Italy, China, Brazil, Indonesia, India, Thailand, Iran and Spain) ensure
materials is shown in Table 8, where the top 25 countries are listed for ∼70% of the global demand. These countries rank also first in the list of
the cumulative output in the period 1971–2016 and in the last decade the major tile makers, thus corroborating the overwhelming role of
(2007–2016). It is significant that the nine major producers (Turkey, ceramic manufacturers on the flux market in most countries. However,
Fig. 8. Variation in the production of feldspathic fluxes from various sources occurred along the last two decades: difference in tonnage (A) and as percent of the 1996 output (B).
Table 8
Top 25 countries producing feldspathic materials and alternatives fluxes in comparison with the production of ceramic tiles.
Country Flux output 1971–2016 (tons × 1000) Country Flux output 2007–2016 (tons × 1000) Country Ceramic tiles 2007–2016 (million m2)
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Fig. 9. Cumulative curves of the contribution of the ten biggest mining districts, for each source, to the global production. Districts are arranged along the x-coordinate from 1 (the largest
output) to 10 (the tenth output) in order of decreasing production. The corresponding output (y-coordinate) is expressed as percentage of the total production for every flux source. Period
1971–2016 (left) and the situation based on the 2016 data (right).
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M. Dondi Resources, Conservation & Recycling 133 (2018) 191–205
In contrast, no significant risk is apparently associated with the proper processing (Bozzola et al., 1995a, b). This can be done also
concentration of suppliers for pegmatites, since the output of the big- for mining activities not targeted to ceramic fluxes, as the case of
gest ten fields sum up to only ∼45% of the demand, as a consequence quarry dumps of ornamental stones (Dino et al., 2012). A key point
of the large number of mines in operation. This figure turns into ∼80% towards a full exploitation of deposits is the difficult compromise
in the case of aplites. between extractive practices and mineral treatments on one side and
Other sources fall in an intermediate situation: 80% of the global the market requirements for by-products on the other side. The
demand is ensured by the five biggest mining districts for feldspathic minimum goal is preventing untolerable contamination for ceramic
arenites and by the seven more productive sites for granitoids. fluxes.
Nevertheless, while the present supply of fluxes from sediments appears 2. Increasing recourse to alternative sources: non-feldspathic, low-
to be improved, thanks to an offer that is wider than in the whole period melting minerals (like sericite) and particularly secondary raw ma-
1971–2016, the production of fluxes from granitoids is currently con- terials (waste glasses, ceramic scraps). The ceramic industry can
centrated in a fewer mining districts with respect to the past. play as an efficient converter of problematic materials (waste-of-
waste, i.e. residues of the waste management chain) into valuable
6. Discussion and conclusive remarks and safe products (Andreola et al., 2016). Nonetheless, the barrier
for a large-scale use of end-of-life products as ceramic fluxes is either
Approximately 575 million tons of feldspathic raw materials have technological or logistic. The former is the small amount allowed by
been globally mined since 1971, in large part to feed the ceramic and current ceramic technology and product specifications, e.g. a few
glass industries. This task was accomplished through a balanced re- percent of waste glass in a porcelain stoneware body (Matteucci
course to a wide range of feldspar sources in different geological con- et al., 2002; Raimondo et al., 2007). The latter is the limited amount
texts. From this standpoint, the supply chain of ceramic fluxes has de- of suitable wastes actually available: for instance, ceramic scraps
monstrated a rather high efficiency in the exploitation of resources, must be just a few percent of the production of an efficient tile-
considering that alternatives have already entered in the industrial making plant. On the other hand, end-of-life (and especially waste-
practice, including secondary raw materials. of-waste) materials are produced in volumes that are usually a
However, the present production for feldspathic materials, close to minor fraction of the flux demand. For example, the waste glass
29 million tons per year, is just the latest step of a trend increasing at collected in northern and central Italy is around 1 million tons per
the pace of 0.78 million tons per year in the last decade (that is more year, 80% of which is sorted as secondary raw material for the
than the output of the tenth major producer in 2016). Even if feldspars container glass industry. Approximately 200,000 tons per year of
are the main constituents of the Earth’s crust, this continuous growth waste-of-waste undergo a beneficiation process that allows re-
should create some concern, taking into account that the flux market is covering annually further 160 thousand tons for glassmakers and
dominated by demand of ceramic tiles manufacturers, whose produc- about 35,000 tons for the ceramic industry (SASIL, 2009). This
tion is rapidly increasing, being now demographically-driven. amount represents only 0.7% of the present consumption of felds-
Technological innovation in the ceramic tile sector is globally pathic materials by the Sassuolo-Scandiano district, thus waste glass
shifting the production towards two parallel targets: porcelain stone- can act just as a sintering promoter and not a realistic flux substitute
ware and other vitrified products (whose batches contain a high per- in a large-scale application.
centage of fluxes) and ever-larger sizes achieved by new technologies 3. Relaxing the technological constraints in ceramic applications: a
(which require high-quality fluxes, i.e. high fusibility and low amount large part of the potential feldspathic resources is nowadays over-
of chromophores). Thus, it is expected that the market will progres- looked because of its insufficient fusibility and/or untolerable
sively move towards fluxes with high or very high fusibility and a low amount of iron and titanium oxides, which are responsible for a dark
amount of iron oxide. Nowadays, these fluxes represent almost half of colour of fired products. The use of raw materials with a scarce
the market (i.e., 37% albitites, 6.5% nepheline syenite, plus a fraction fusibility is currently made possible by the addition of low-melting
from pegmatites) but have limited (or unknown) reserves. fluxes: by this way, large amounts of granites or feldspathic arenites
The complementary part of the market is constituted by fluxes with are directly employed together with albitites in Europe (Lewicka
medium to very low fusibility (and often not so scarce in chromo- and Wyszomirski, 2010). However, the main challenge for ceramists
phores) mainly recovered from granitoids, feldspathic sands, aplites, is how to develop Fe-rich bodies that could be suitable for vitrified
pegmatites, acid volcanics, and phyllites. These raw materials are in tiles, overcoming known problems (excessive firing deformations,
many cases believed to occur with large reserves (or at least resources). narrow sintering range, bloating, defects in glazes, etc).
It is crucial to underline that most of these fluxes are successfully uti-
lized in ceramic batches only together with fluxes of high fusibility. In fact, In conclusion, ongoing trends suggest drawing a future scenario to
it is the availability of low melting fluxes (like sodium feldspar) that test the security of supply of feldspathic raw materials. This is parti-
enables a large-scale utilisation of quartz-rich, mixed Na-K feldspathic cularly needed for albitites and nepheline syenites: first, because they
materials (like those coming from granites, arenites and so on). Thus, are the two sources that suffer for the highest dependence from a few
these latter sources, despite their local abundance, cannot satisfactorily mining sites. Second, as they play the role of key raw materials, thus
substitute albitites or nepheline syenites. turn essential for a large part of the production of ceramic tiles and
In addition, account must be taken that most ceramic fluxes are sanitarywares (and consequently their demand is likely to grow fur-
products with a relatively low value added. Indeed, current prices range ther). Unfortunately, accessible data on reserves are insufficient to at-
roughly from ∼40 €/ton (acid volcanics and arenites) up to > 200 tempt any reliable prediction of the medium-term availability of
€/ton (potassic feldspar) on the international market. For this reason, it feldspathic raw materials. Based on the few data published, present
is not pragmatic to conceive complex and expensive mineralurgical reserves might last for two or three decades at the present rate of
treatments to obtain large amounts of high-grade feldspar from sources consumption. More critical appears the situation of albitites, con-
as granitoids, arenites, aplites, or acid volcanics. sidering that a genetic model for this kind of deposit is lacking, while it
In order to mitigate the risk for a secure supply stemming from the should be useful to address the search for alternatives to currently
increasing demand for feldspathic raw materials, three strategies should exploited deposits.
be put in practice: Finally, more resources are necessary for R&D activities to fill the
knowledge gaps on feldspathic raw materials and their substitutes.
1. Full valorization of flux deposits: residues from mining of felds- Specific efforts should be particularly spent:
pathic rocks can be converted into marketable by-products by
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