On the production of fired clay bricks from waste materials: A critical update

Construction and Building Materials 68 (2014) 599–610

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Review

On the production of fired clay bricks from waste materials: A critical update Sergio Neves Monteiro a,⇑, Carlos Maurício Fontes Vieira b a b

Military Institute of Engineering, IME, Materials Science Department, Praça General Tibúrcio, 80, Praia Vermelha, Urca, CEP 22290-270, Rio de Janeiro, RJ, Brazil State University of the North Fluminense Darcy Ribeiro – UENF, Av. Alberto Lamego 2000, CEP 28013-602, Campos dos Goytacazes, RJ, Brazil

h i g h l i g h t s  An up-to-date list of works on waste incorporation into clay ceramics is discussed.  Fuel-containing wastes may reduce energy to produce clay bricks to less than 1 kW h.  Brick production in Brazil uses mostly wood as fuel bringing neutral CO2 emission.  For the next 2 decades Brazilian bricks will be mainly fabricated by firing.  Thereafter geopolymerization might replace firing and cementing in brick production.

a r t i c l e

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Article history: Received 16 January 2014 Received in revised form 7 June 2014 Accepted 3 July 2014

Keywords: Clay ceramic Waste incorporation Firing energy Environmental emission Brazilian brick production Properties

a b s t r a c t Recently, the production of bricks from waste materials was reviewed by Zhang in Construction and Building Materials. The main focus was a division into three producing methods: firing, cementing and geopolymerization. Both firing and cementing methods were indicated to consume significant amount of energy and release large quantities of greenhouse gases. Based on these drawbacks and taking into account the need to protect clay resources, it was concluded that geopolymerization seems to be the trend to follow. Most of the reviewed works on the firing method, published since 1987, were related to wastes incorporated into clay ceramics. In the present work, starting from previous review articles, additional information was added to extend the knowledge, not covered by Zhang, on the incorporation of wastes into clay ceramics. The particular case of Brazil, in which large and easy to mine clay deposits support an extensive network of ceramic industries, is surveyed. Fuel containing wastes contribute to save in firing energy, while fluxing wastes improve the ceramic properties. At least for the next decades, clay ceramic incorporation seems to be the most realistic solution for recycling industrial wastes in countries, such as Brazil, with vast clay resources. Ó 2014 Elsevier Ltd. All rights reserved.

Contents 1. 2. 3.

4. 5.

Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Previous reviews on waste incorporated clay ceramics. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Recent works on waste incorporated clay ceramics. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.1. Fuel or organic wastes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3.2. Fluxing or inorganic wastes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Conclusions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

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1. Introduction ⇑ Corresponding author. Tel.: +55 21 2546 7042; fax: +55 22 2546 7049. E-mail addresses: [email protected] (S.N. Monteiro), [email protected] (C.M.F. Vieira). http://dx.doi.org/10.1016/j.conbuildmat.2014.07.006 0950-0618/Ó 2014 Elsevier Ltd. All rights reserved.

In a recent work, Zhang [1] presented a relevant state-of-the-art review on the utilization of waste materials to produce bricks. An

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extensive list of publications associated with several different types of wastes was introduced to the reader with corresponding summary of processing methods and main results. Zhang [1] divided the methods of brick production into 3 categories: firing, cementing and geopolymerization and these were discussed in terms of specific advantages and drawbacks. In particular the firing method, in most cases related to the conventional clay brick production, has the advantage of easy execution using well known and traditional procedures and equipments. By contrast, making bricks through firing, as pointed out by Zhang [1], has the drawbacks of consuming a significant amount of energy, on average 2.0 kW h, per brick, and release a large quantity of greenhouse gases, about 0.41 kg of CO2, quoting the work of Reddy and Jagadish [2]. Another environmental concern noted by the author was a shortage of clay in many parts of the world. This motivated countries such as China to start limiting the use of bricks made from clay. In conclusion, Zhang [1] indicated that the geopolymerization method, which is claimed to consumes much less energy and is associated with a smaller carbon footprint, seems to be the trend to follow. As a long term future prognostic, one cannot disagree on Zhang [1] conclusions. However, many aspects of his review work deserve a second opinion regarding the firing method. The reader should pay attention to two points in the present work. First, although Zhang’s proposal by its title ‘‘production of bricks from waste material’’ [1] may appear limited to specific process of fabrication of rectangular blocks, it certainly concerns to the recycling of wastes. Regardless the type of fired ceramic piece (brick, tile, pipe, block, etc.) the important point is the feasibility of incorporating a given waste. Results in terms of advantages and drawbacks to the fired ceramic, as compared to cementing and geopolymerization, were the main focus of Zhang’ review [1], not the shape of the product. A second point to be noticed is that a number of quoted articles in the present work is written in Portuguese. Far from trying to bring difficulty to the reader, the idea is of emphasize the waste incorporation into fired ceramic as a more relevant recycling procedure in Portuguese speaking countries. In particular, the reasons for Brazil will be further highlighted along this presentation. It will be shown that today, and for the next two decades, different from some other countries, the advantages strongly justify the recycling of wastes by incorporation into fired clay ceramic.

2. Previous reviews on waste incorporated clay ceramics Perhaps by considering beyond the scope of his review, Zhang [1] failed to quote previous review articles that are now worth mentioning. Indeed, in 1997 Dondi et al. [3,4] presented an earlier two parts review on the recycling of industrial urban wastes into clay ceramics for brick production. This review was based on a literature survey since 1977 covering works from selected countries such as Italy, UK, Spain, Germany and USA. Works from other countries were disregarded. The main focus of Dondi et al. [3,4] review was a classification of the wastes into 5 categories associated with the major characteristics, which affects the clay brick. These are: fuel; fly-ash; fluxing; plasticity reducing and plasticifying wastes. The reader might be particularly interested in several earlier references in the review of Dondi et al. [3,4], not mentioned by Zhang [1], presenting a substantial amount of information in terms of waste characterization, process parameters and properties of incorporated ceramics. More recently, an up-to-date review was presented by Vieira and Monteiro [5] on the incorporation of wastes into clay ceramics. In this later review, modifications were introduced in the original Dondi et al. [3,4] categories to allow a wider variety of wastes to be considered. Additionally to fuel and fluxing wastes, a more

general category of property affecting wastes embodied the earlier proposed fly-ash, plasticity reducing and plasticifying waste categories. The consideration of a category such as fuel wastes in both reviews [3–5] enables an important distinction of residues with heat power enough to sensibly contribute to a saving in the ceramic processing and reduce the fired clay brick embodied energy. Several works investigated the incorporation of oily residues from industry and petroleum operations [6–16]. These works reported practical advantages such as the increase in processing speed, reduction in equipment wear, enhancement of mechanical properties and saving in fuel consumption. Blast furnace sludge was included as fuel waste because it still has a significant amount, up to 25%, of coke [17,18]. Sludge from pulp and paper making industry, also considered as a fuel waste, contributed to a saving in energy during the firing stage of incorporated clay ceramics [19,20]. The category of fluxing wastes, discussed in Vieira and Monteiro review [5], comprised industrial residues that would form low melting temperature phases and thus improve the linear shrinkage, water absorption and mechanical strength of clay ceramics. These are the sludge from ornamental rock processing [21–30], glassy residues [31–37], and flux-containing residues [38–40]. The general category of wastes, without heat power or fluxing action, that affect the ceramic properties encompass distinct industrial types. As in the first two categories, several works failed to be reviewed by Zhang [1]. These works investigated the following types of wastes: spent ceramic powder, also known as grog or chamotte [41–48], water treatment sludge [49–55], steel slag [56–61], ashes [62–69], electrolytic/galvanic sludge [70–76], catalyst reject [77], textile industrial slurry [78], metallurgical smelting sand rejects [79,80], tannery sludge [81], construction/demolition leftover [82,83]. 3. Recent works on waste incorporated clay ceramics After Vieira and Monteiro review [5], many other works were dedicated to the incorporation of wastes into clay ceramics. Zhang [1] listed 8 papers in a more recent period after 2008 up to 2012 but several additional ones might deserve to be reviewed. These recent additional papers will be also chronologically listed. However, as a general classification, they are divided into two categories regarding the type of incorporated waste: (3.1) fuel or organic and (3.2) fluxing or inorganic. To shorten the summary of each paper, both the amount of incorporation (wt%) and processing/firing temperature (°C) will be shown inside parenthesis. Whenever available, changes in the microstructure and properties will be indicated. 3.1. Fuel or organic wastes Pinheiro and Holanda [84] investigated clay ceramics (uniaxially pressed/800–1000 °C) incorporated (up to 30 wt%) with encapsulated petroleum waste. The authors showed that for 30 wt% incorporation in firing at 1000 °C, the linear shrinkage decreases (3.6%), the water absorption decreases (16.5%) and the compressive strength also decreases (8.2 MPa). As for the structure, no incorporated ceramic showed surface stains and black core defects that might result from the petroleum waste. These results justify the petroleum waste incorporation as a technically adequate procedure, which causes less environmental impact. Hajjaji and Khalfaoui [85] investigated the effects of oil shale addition (up to 20 wt%) into clay ceramic (extruded/700–1075 °C). The results showed that the oil shale addition lead to development of anorthite and diopside and a drastic decrease of the ceramic glassy phase. SEM microstructures revealed shrinkage and weak cohesion

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between the glassy phase and anorthite, probably responsible for the occurrence of annular empty spaces. The authors found that the ceramic properties experienced a marked change up to 12 wt% addition because of the glassy phase, but remained practically unchanged for higher additions, with water absorption around 15% and bending strength at about 30 MPa, due to calcium silicates formation. Qi et al. [86] conducted different experiments to evaluate the microstructure and properties of ultra-lightweight ceramic pellets (sintering/950–1160 °C) produced from mixtures of clay and dehydrated sewage sludge (up to 90 wt%). In special, the authors considered the optimum condition to be 20–30 wt% sludge addition associated with a preheating at 400 °C for 20 min and firing at 1150 °C for 10 min, which resulted in a ceramic with 0.331 g/cm3 of density. This particular, ultra-lightweight clay ceramic, displayed a cellular structure and water absorption of 5.3 wt%. A bloating phenomenon was found by SEM to be associated with gaseous bubbles. Toxic metal leaching values below the detection limit were considered suitable for practical civil engineering. Eliche-Quesada et al. [87] studied the production of clay bricks (uniaxial press molded/950 °C) incorporated with different industrial wastes: urban sewage sludge (15 wt%), malt bagasse (2.5 wt%), brewing sludge (5 wt%), olive mill wastewater (6.5 wt%), and coffee ground (3 wt%) residues. The authors found that each type of waste has a distinct effect on the incorporated clay brick. For instance, water absorption increased to above 35% and the compressive strength decreased by a maximum of 19% when sewage sludge, brewing sludge and bagasse were incorporated. The incorporation of coffee grounds and olive mill wastewater was even more beneficial by showing similar compressive strength together with 19% improvement in thermal conductivity in comparison with pure clay bricks. Microstructural study by SEM showed that the incorporation of brewing sludge as well as the bagasse increased the open porosity, while the coffee grounds and olive wastewater increased the closed porosity and micropores. Teixeira et al. [88] reported on the incorporation (up to 30 wt%) of a sludge, generated in a Brazilian water treatment plant, into clay ceramics (uniaxially pressed/850–1200 °C). The chemical and mineralogical composition of the sludge varied according to the month of its production. The properties of the incorporated ceramics were impaired with respect to pure clay ceramic. The flexural strength decreased to 8 MPa for 20% sludge incorporation at 1150 °C. However, the authors concluded that the sludge can be incorporated into clays up to 10 wt% and fired at temperatures lower than 1000 °C to produce hollow bricks. Firing above this temperature permits up to 20 wt% of incorporation to produce not only bricks but also roof tiles. Devant et al. [89] analyzed the possibility of improving the fabrication and properties of sewage sludge (up to 23.8 wt%) incorporated red clay ceramics (extruded/980 °C) by adding (16.7 wt%) forest waste into the binary mixture. Considering a ternary pseudo diagram, the authors found the optimal ternary mixture to be 10 wt% sludge, 10 wt% forest waste and 80 wt% clay. A clay body with such composition would have a compressive viscosity of 96 kP/cm2, thermal conductivity of 0.31 W/m K and porosity of 59.4%. This mixture met the technological limit for an extrudable material and the resulting ceramic would present a relatively high compressive strength with low thermal conductivity, suitable for building construction. Leaching and outgassing tests favor the environmental aspects associated with the production of sludge and forest waste incorporated clay ceramics. Raut et al. [90] reviewed 18 specific works on the production of bricks both of fired clay and dried cement, incorporated with industrial and agricultural solid wastes. Regarding the fired clay bricks incorporated with organic wastes, of interest in this section, only the recent works of Mucahit and Sedat [91], using paper processing residues (up to 30 wt%) added to bricks

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(compressed/1100 °C) and Kadir et al. [92], incorporating cigarette butts (10 wt%) into clay bricks (pressed/1050 °C), need to be quoted. As for the latter [92], the reader should pay attention to the incorrect authors’ names and journal quotations in Raut et al. [90] reference number [2]. Cusidó and Soriano [93] studied the valorization of waste water treatment plants sludges by pelletizing through a ceramization process (sintering/1050 °C) to obtain a material, Pellexpended™, similar to expanded clay used as construction material. Although not incorporated into a clay matrix, the pelletizing is associated with a firing process to recycle a worldwide common waste as a clay-like product. The authors claimed to have developed a new lightweight material with open porosity of 62% and low thermal conductivity of 0.9–1.2 W/m K. Leaching tests revealed, after firing, undetectable amounts of hazardous metal, with the exception of vanadium. Toxicity tests also showed negative results. Firing emissions were found surprisingly lower than those for clay bricks incorporated with sewage sludge. The authors also concluded that the ceramization of the sludge pellets is a promising valorization technique worth considering from both economical and technological perspectives. Dias et al. [94] characterized a blast furnace sludge for clay ceramic fabrication. Thermal analysis was conducted up to 1025 °C at a heating rate of 10 °C/min under air. The authors found that the sludge has a high content of coke and its combustion generates enough heat to sensibly contribute to the ceramic firing process. Fig. 1 shows the differential scanning calorimetric (DSC) and thermogravimetric (TG) curves for the sludge. In this figure, the energy associated with the DSC exothermic peak at 725 °C was calculated as 6.648 kJ/kg, which corresponds to a saving in fuel for the ceramic firing. Gas analysis indicate that CO, CO2, NO and SO2 were emitted from 450 to 1150 °C. It was recommended that sludge incorporation should be restricted to less than 10 wt% to avoid excess of acid gaseous emission to the atmosphere. Cusidó and Cremades [95] investigated the environmental effects of using clay bricks (extruded/1050 °C) incorporated (up to 60 wt%) with sewage sludge. Additionally, ceramic coating, ceramic mixtures of sludge-forest residue-clay as well as ceramics incorporated with paper industry sludge were also investigated. Based on leaching, outgassing and offgassing tests, the authors concluded that contents of sludge seem to have no influence on the environmental characteristics of structural clay ceramics for building materials. The inert capacity of these ceramics comes from the partial vitrification of most heavy metals. These lighter and more thermal-acoustical insulating materials could be used, up to 25 wt% of sludge incorporation, without restrictions other

Fig. 1. DSC and TG curves for the blast furnace sludge. Reproduced with permission from [94].

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than the regulation of technical properties required by each country. Herek et al. [96] characterized clay ceramic bricks (extruded/ 900 °C) incorporated (up to 20 wt%) with textile laundry sludge. The results showed that the sludge incorporation impaired the main properties by decreasing the bending strength (3.05 MPa) and increasing the water absorption (26%). Leaching and solubilization tests indicated that sludge incorporated ceramics are inert with respect to the Brazilian environmental norm. Images by SEM showed that the pore size increased with the amount of laundry sludge. The authors concluded that the addition of textile wastewater sludge into clay ceramic bricks is advantageous as it recycles a hazardous residue in a secondary raw material. De la Casa et al. [97] reported on clay bricks and masonry (extruded/1000–1050 °C) incorporated (up to 16 wt%) with twophase olive mill waste, known in Spain as ‘‘alperujo’’. The authors found a saving in fuel due to the ‘‘alperujo’’ energy input above 1000 kJ/kg for 12 wt% incorporation. A higher porosity was observed by SEM with pores of greater size from the combustion of organic matter. They concluded that the incorporation causes no problem to the processing stages of extrusion, drying and firing. After firing the water absorption increased (12.05%), while the bending strength decreased (11.6 MPa). Moreover, valorization of the ‘‘alperujo’’ could be achieved in facing clay bricks incorporated with lower amounts and in masonry units for amounts above 6 wt%. These latter are either equivalent to the traditional masonry units or exhibit lower thermal conductivity. Eliche-Quesada et al. [98] investigated the valorization of residues from biodiesel production by incorporation into porous clay bricks (mold-pressed/1050 °C). Two distinct types of residues were separately added to clay: spent earth from biodiesel filtration (up to 20 wt%) and glycerin (up to 15 wt%). The results indicated that both residues incorporations decreased the compressive strength (25 MPa) and increased the water absorption (23%), but still keeping values within those required by the European standards. Thermal conductivity was found to decrease (0.09 W/m K) in both residues incorporated bricks. The incorporation increased open porosity as observed by SEM and produced larger pores. The authors concluded that the biodiesel residues are suitable as secondary raw material in clay ceramic brick production. The same research group of Eliche-Quesada et al. [99] studied a variety of wastes, some with organic content, sawdust (up to 10 wt%), others organic–inorganic, spent earth from oil filtration (up to 30 wt%) and compost (up to 30 wt%) and another inorganic, marble residue (up to 20 wt%) incorporated into clay bricks (uniaxial pressing/950 and 1050 °C). The results showed for the two firing temperatures a tendency of the bulk density to decrease (1.5–1.6 g/cm3); the apparent porosity to increase (37–45%); water absorption to increase (24–31%) and compressive strength to decrease (10– 35 MPa) for the highest percentage of incorporation depending on the waste. SEM analysis showed at 1050 °C a more compact and better-developed microstructure with nearly spherical and isolated pores. The authors concluded that it is possible to obtain ceramic bricks with 5 wt% sawdust; 10 wt% compost as well as 15 wt% of both spent earth from oil filtration and marble residue, within standards for bricks and mechanical properties similar to clay bricks without incorporated wastes. Kizinievicˇ et al. [100] analyzed the incorporation (up to 40 wt%) of a sludge waste, from a water treatment plant in Lithuania, into clay ceramic products (manually formed/1000–1050 °C). A mixture of 60–65% clay and 35–40% sand was used as ceramic matrix. After 5 wt% of sludge incorporation, both linear shrinkage (17.5%) and the water absorption (28.8%) increased. As for the compressive strength (14 MPa) and density (1.34 g/cm3), both decreased above 5 wt% incorporation. In addition of changing the technological properties the sludge, mostly composed of Fe2O3, acts as a pigment that dyes the clay ceramic with a more intense red color. As for the

40 wt% sludge incorporation, SEM observation showed a total open porosity of 44.5%. Barbieri et al. [101] reported on a preliminary study of valorization of agricultural biomass wastes by incorporation into clay bricks. These wastes were grape seeds (5 and 8 wt%), cherries seeds (5 and 8 wt%), sawdust (5 wt%), and sugarcane ash (5 wt%), separately incorporated into clay ceramics (uniaxial pressing/950–1000 °C). The authors concluded that grape and cherries seeds as well as the sawdust incorporation bring an energetic support during their combustion in the firing stage. The sugarcane ash incorporation of 5 wt% improves the mechanical properties (28 MPa) due to its high silica content (61%), which acts as filler and reduces the clay body plasticity. Any of these biomass wastes incorporated in an amount of 5 wt% changes slightly the technological properties. The sawdust promotes the highest water absorption (20%). This might permit to obtain bricks with insulating characteristic. 3.2. Fluxing or inorganic wastes Lafhaj et al. [102] presented results on the incorporation of NovosolÒ processed river sediments from the north region of France (up to 45 wt%) into clay bricks (extruded/1010 °C). For bricks incorporated with 45 wt% of treated (phosphate added and 650 °C calcinated) sediments, the plasticity index decreased (10.55), while the water absorption increased (40%) and the strength decreased (25.58 MPa). Based on these properties and the French standards for freezing and thawing resistance as well as efflorescence and heavy metal leaching, the authors concluded that 35 wt% incorporation seems to be the most effective one. Montero et al. [103] investigated the addition (up to 35 wt%) of calcium carbonate sludge, obtained from stone industry, into clay ceramic tiles (uniaxial pressing/975–1050 °C). The main advantages of this addition were the cost reduction and the possibility of recycling a sludge whose disposal increases everyday in Spain. After firing, it was observed the appearance of white nodules accompanied by small chips or craters. The authors concluded that these tiles could be applied as construction materials despite the increase in water absorption (35.2%) and decrease in the bending strength (5.0 MPa). In another work of the same group, Montero et al. [104] investigated the addition of marble residue (up to 35 wt%) and sewage sludge (up to 10 wt%) into clay ceramic tiles (uniaxial pressing/975–1050 °C). It was found that these wastes react easily with clay providing a better sintering of the ceramic. The authors concluded that, although impairing both water absorption (41%) and bending strength (4.9 MPa), the selection of the adequate sewage sludge or marble residue content into the clay ceramic body permits to attend the usual standards applied to construction materials. Acchar et al. [105] studied the recycling of a spent catalyst reject, generated by the Brazilian petroleum industry, through its incorporation (20 wt%) into red clay products (extruded/700– 1150 °C). By firing at 1150 °C, the ceramic flexural strength reached 12 MPa while the water absorption was 5% with 10% of porosity. Large quartz grains and significant amount of pores were observed by SEM. The results of technical properties suggested that the reject incorporation constitutes a valid effort to environmental amelioration. Torres et al. [106] reported on the incorporation (up to 40 wt%) of two types of natural granite stone cutting and polishing sludges into bodies composed of two distinct clays to produce roof tiles (extruded/950–1050 °C). The results of 10 wt% incorporation provided excellent properties associated with less than 6% of water absorption and 38 MPa for bending strength. SEM/EDS results confirm the existence of Fe particles and high degree of homogeneity in the granite sludge incorporated microstructure. The authors indicated that the sludges can be used to replace natural non-plastic raw material in traditional clay ceram-

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ics fabrication. This will contribute to preserve non-renewable natural resources, while minimizing the negative environmental impact due to the sludges disposal. Cultrone and Sebastian [107] evaluated the technical properties of clay bricks (solid molded/800 and 1000 °C) pure or added with 5 wt% of fly ash. The addition of fly ash particles led to a reduction in the density (2.53 g/cm3) of bricks and improvement in their durability. Vitrification effects shown by SEM were less evident in incorporated bricks with high carbonate content. The texture of bricks with and without fly ash was found the same. Moreover, less decay was caused by salt crystallization in the structural pores. The authors concluded that this addition could have practical implications as a mean of recycling fly ash and achieving cost saving in brick production. Chen and Lin [108] studied the incorporation of sewage sludge ash (up to 50 wt%) and nano-SiO2 particles (up to 3 wt%), as strengthening additives, into clay ceramics (uniaxial pressing/1000 and 1100 °C). Results indicated that the water absorption (12%) of the incorporated (porcelain) clay ceramic was reduced at 1100 °C. With the nano-SiO2 addition, the bending strength was increased (8 MPa) at 1000 °C, while the linear shrinkage decreased ( 0.5%) and water absorption increased (20%). A tendency of precipitates to morph from fine to coarse was revealed by SEM as the firing temperature increased. Based on these results, the authors concluded that the nano-SiO2 particles contributed to improve the ceramic properties. Christogerou et al. [109] studied the introduction (up to 15 wt%) of boron wastes from Turkey boron ore processing into clay ceramics (pressed/800–950 °C). The authors indicated that up to 900 °C and 5 wt% of waste introduction the incorporated ceramic showed comparable properties with those of the pure (neat) clay ceramic used as reference. At a firing temperature of 950 °C the ceramic properties were improved. The water absorption was reduced (12%) and the bending strength increased (24.5 MPa). The porosity remained high with a cloud of pores widespread in a glassy matrix. It was concluded that the use of boron waste is feasible in small percentages (<5 wt%). Loryuenyong et al. [110] investigated the incorporation (up to 45 wt%) of recycled glass waste, from structural glass walls, into clay bricks (mold formed/1000–1200 °C). The results indicated that, with proper amount of waste and firing temperature, clay bricks with suitable properties could be obtained. In particular, a compressive strength as high as 41 MPa and water absorption as low as 2% were achieved from bricks with 15 wt% waste fired at 1100 °C. With 45 wt% of waste, the water absorption increases and the strength is significantly reduced. New cristoblalite and albite phases at 1100 °C were observed by SEM to increase with glass waste incorporation. These bricks with up to 30 wt% waste were able to meet the minimum requirements, even for some load-bearing structures. Maschio et al. [111] compared the properties of an incinerated paper mill sludge (up to 60 wt%) mixed with glass cullet (up to 40 wt%) both neat and incorporated (70–90 wt%) into clay ceramics (uniaxially pressed/1100–1140 °C). The results indicated that clay ceramics incorporated with 70 wt% of 60/40 mixture of sludge/cullet fired above 1120 °C display a stable sintering process associated with good hardness (5.7 GPa) and strength (54 MPa). These ceramics showed by XRD analysis a structure with free quartz, anorthite and diopside. Therefore, they might be suitable for the industrial production of tiles. Lin and Luo [112] investigated the incorporation (up to 50 wt%) of a catalyst waste into clay ceramics (uniaxial pressing/900–1200 °C) to produce pavement tiles. The authors indicated that the water absorption (20%) and the porosity (30%) of the clay ceramics increased with the amount of waste while the loss on ignition decreased. Hardness of both the neat and waste incorporated clay ceramics strongly depends on the amount of waste and firing temperature. It was concluded that the

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catalyst waste might be incorporated up to 10 wt% in pavement tiles. Sokolar and Smetanova [113] reported on the incorporation (70 wt%) of fly ash from brown coal into clay ceramic tiles (uniaxially pressed/1000–1150 °C). The authors indicated that fly ash milling to 63 lm improved the sintering ability of the fly ashadded clay body. A 1.3 wt% of deflocculant/fluxing agent increased the green body flexural strength and decreased the water content. The fired tiles with milled fly ash displayed lower water absorption (8%) at 1150 °C and higher flexural strength (34.1 MPa). A more dense microstructure of deflocculated tiles was observed by SEM. Fly ash-incorporated clay bodies can be frost resistant with water absorption above 10% due to positive pore size distribution. Andreola et al. [114] reported on the incorporation (up to 20 wt%) of cleaned cathode ray tube glass, from dismantled TV and PC, into clay ceramics (press sintered/1210 °C). The glass waste replaced both feldsphatic and inert components need to improve a traditional clay ceramic body. The obtained incorporated ceramics showed main properties, water absorption (15%) and strength (10%) similar to commercial ceramic materials used in floor and wall tiles. Machado et al. [115] investigated the incorporation (up to 90 wt%) of an electric arc furnace steel dust, which contains high amounts of iron and zinc as well as significant amounts of lead, chromium and cadmium, into structural clay ceramics (mold compressed/800 and 1100 °C). For the maximum 90 wt% incorporation and 1100 °C firing, significant changes are observed in the water absorption (7.5%), porosity (23.8%), density (3.19 g/cm3), linear shrinkage (11.5%) and bending strength (0.44 MPa). Structural analysis by XRD indicated formation of diopside due to Ca and Mg in the steel dust. The authors indicated that, up to 20 wt% of dust, the incorporated clay ceramic may be used for brick and roof tile production with a limited risk of cadmium contamination. Hojamberdiev et al. [116] investigated the utilization of a muscovite granite waste added (up to 30 wt%) to a clay-type of matrix (uniaxially pressed/800–1150 °C) containing kaolin (60–65 wt%) together with grog (up to 10 wt%), bentonite (0–5 wt%) and loess (0– 10 wt%). The authors concluded that the waste resembles conventional non-plastic materials and can be beneficially used in the production of both flooring and facing tile ceramics. The flooring ceramic tile sample containing 30 wt% waste and fired at 1150 °C showed higher bending (32.04 MPa) and compressive (54.24 MPa) strengths in association with a favorable lower water absorption (3.66%). SEM and XRD analyses revealed small acicular mullite crystals embedded in glassy matrix. Both types of tile ceramics satisfied the standards and could be industrially used as a low cost raw material. Furlani et al. [117] reported on the characterization of distinct clay matrices (uniaxially pressed/1040–1140 °C) incorporated with a waste composed of a fixed 60/40 ratio of incinerated paper mill sludge and glass cullet. This fixed composition waste was incorporated in amount up to 90 wt% into the clay. The authors observed that the ceramics containing kaolin in their matrices displayed the best flexural strength (43 MPa) and Vickers hardness (5.1 GPa) overall behavior. The best properties of incorporated ceramics, using red or yellow clays as matrices, were obtained on products fired above 1080 °C. Ceramics with 60 wt% waste showed by SEM prismatic elongated structures attributed to diopside, akermanite or augite. A certain amount of vitreous phase was also observed. Both the ceramic performance and optimum temperatures are affected by the type and amount of clay added. Sokolar and Vodoka [118] studied the influence of two distinct (brown coal and fluidized) fly ashes addition (60 wt%), on the technical properties of clay ceramics (uniaxially pressed/1080 °C). The authors found that 60 wt% incorporation of the fluidized fly ash reduces

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the firing shrinkage ( 3%) while increasing the ceramic porosity (44.4%). Moreover, the water absorption increased (30.3%) and the bending strength decreases (8.9 MPa). A higher volume of pores was observed by SEM. In conclusion, it is possible to use a maximum of 20 wt% of fly ash and still meet the requirements for ceramic tiles. As for the environmental impact, the fluidized fly ash addition dramatically increases the content of SO2 in the flue gases during the ceramic firing. El-Maghraby et al. [119] used natural granite (up to 35 wt%) sieved to 200 mesh to completely replace fluxing and inert components of a clay ceramic (uniaxially pressed/1220 °C). The authors showed technical advantages in terms of reduction in water absorption (2.47%) and increasing bending strength (31.81 MPa) with higher granite content of 35 wt%. Based on SEM observations, the authors suggested that the increase in strength is related to coarse needle-like secondary mullite. Both environmental and economical advantages confirmed the feasibility of granite addition into a clay ceramic formulation. In the aforementioned important review paper of Raut et al. [90], the recent work of Caroline et al. [120] on recycled slag of welding flux (10 wt%) incorporation into clay bricks deserves to be quoted in this section. Pedroti et al. [121] conducted an assessment of clay ceramics (press molding/850 and 1050 °C) incorporated with variable amounts (0–100 wt%) of granite wastes. An investigation was conducted with experimental design using the Simplex method for all possible waste mixtures with two distinct, ‘‘weak’’ and ‘‘strong’’, clays. It was found that the incorporation of 17 wt% of waste gave the highest strength (30 MPa) in association with the lowest water absorption (15%) for mixtures rich in ‘‘strong’’ clay fired at 1050 °C. Moreover, it was suggested that new heating systems might reduce emissions that impact human health. Machado et al. [122] studied the incorporation (up to 50 wt%) of a sheelite residue, from ore mining, into clay ceramics (uniaxial compaction/850–1000 °C). Results with 50 wt% incorporation and firing at 1000 °C indicated water absorption (22%) below the standard and bending strength (6 MPa) within the norm.

The authors indicated the possibility of using a maximum of 30 wt% of residue for clay brick production. Vieira et al. [123] evaluated a clay ceramic (uniaxial pressing/ 1050 °C) incorporated (20 wt%) with powder waste from the sintering plant of a steel-making industry. As compared to the neat clay ceramic, the waste incorporation increased the amount (11%) and average size (1 lm) of the porosity and introduced structural defects such as microcracks observed by SEM. The authors suggested that the inert nature of the waste as well as its different coefficient of thermal expansion with respect to the clay matrix be responsible for the additional structural defects that could impair the technical properties. Silva et al. [124] investigated the incorporation (up to 20 wt% of ashes), resulting from the incineration of elephant grass, into clay ceramics (uniaxial pressing/850 °C). The authors indicated that the particle size of the ash is coarser than the convenient size for incorporation. The ashes are mainly composed of quartz and calcium compounds that sensibly reduced the linear shrinkage (13%) but, up to 20 wt%, did not change the water absorption (26%) and bending strength (4 MPa). It was concluded that the firing temperature of 850 °C is not enough to provide consolidation of the ceramic microstructure, as observed by SEM. Caldas et al. [125] reported on the incorporation (up to 10 wt%) of a flat glass waste (glass cullet) into clay ceramics (press molded/ 850 and 1050 °C). The authors found that the microstructure of both neat clay and 10 wt% cullet incorporated ceramics did not present significant differences. However, glass particles observed by SEM indicated the possibility of fluxing action. Indeed, firing at 1050 °C of the incorporated ceramic is associated with microstructural evidences of vitrification. Moreover, optical-dilatometry images, Fig. 2, show that the glass cullet has a softening point at 810 °C from which viscous flow allows ceramic pores to be penetrated and closed as a glassy phase. Partial vitrification of a 10 wt% incorporated ceramic, Fig. 3, can be attributed to a fluxing behavior of the cullet forming glassy phase (white arrow), which might improve the material technical properties .

Fig. 2. Optical-dilatometry results for the glass waste. Reproduced with permission from [125].

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Gadioli et al. [126] studied the incorporation (up to 30 wt%) of granite waste, generated by an ornamental stone industry, into clay ceramics (uniaxial pressing/1050 °C) for rustic wall tile production. The authors indicated that the water absorption (13%) remained constant and below the standards, while the linear shrinkage (6%) and bending strength (8%) decreased with 30 wt% waste incorporation. Quartz particles from the waste were considered as possibly causing the reduction in strength. In spite of changes in properties, all formulations up to 30 wt% of waste attended the Brazilian standards for rustic wall tiles. Altoé et al. [127] investigated the degradation by salt spray of red clay ceramic (press-molding/650–850 °C) incorporated (up to 10 wt%) with ornamental rock waste. For ceramics incorporated with 10 wt%, the water absorption (22%) was above the standard but the flexural strength (2 MPa) was within the norm, even after degradation by salt spray. A statistical Weibull analysis indicated that 5 wt% waste incorporated ceramics fired at 850 °C were considered by the authors as more suitable than the neat clay ceramic for use in red bricks subjected to degradation by marine environment. Pérez-Villarejo et al. [128] investigate the recycling of ashes from a biomass incinerator by incorporation (up to 50 wt%) into clay bricks (press-molded/950 °C). Although for 50 wt% incorporation the water absorption was increased (30%) and the compressive strength decreased (14%), bricks with ash content up to 20 wt% met the European Union standards. SEM observation showed, with increasing amount of ash, an increase in open porosity as a result of the connection of macropores. The authors concluded that incorporating ashes into clay ceramics reduces both environmental problems and total cost of raw material. He et al. [129] studied the effect of a red mud incorporation, generated in the Bayer process of alumina production, incorporated (up to 80 wt%) into clay ceramics (press molded/1000–1100 °C). An increase in the ceramic density and linear shrinkage as well as decrease in water absorption were obtained with increasing amount of red mud incorporation. Indeed, for 80 wt% incorporation and firing at 1050 °C, a marked change occurred in density (1.85 g/cm3), linear shrinkage (28% and water absorption (10%). The compressive strength increased up to 40 MPa for 20 wt% of red mud incorporation. Based on SEM observation, this was attributed to the formation of glassy phases from fluxing agents in the red mud at higher fired temperatures. However, incorporation beyond 40 wt% decreased the strength by limiting the formation of glass phase. The optimum parameters for production of common clay bricks were 20 wt% incorporation and firing at 1050 °C for 2 h. Pérez-Villarejo et al. [130] studied the incorporation (up to 90 wt%) of a red mud, derived from a aluminum industry in Spain, into clay ceramics (uniaxial force/950 °C). Neat clay and pure red

mud were also studied. The authors claimed that the ceramic technical properties display interesting values. In particular, the compressive strength of about 45 MPa for the neat clay ceramic decreased to 15 MPa for 12 wt% incorporation, Fig. 4, but then increased up to an amazing 70 MPa for 90 wt% red mud incorporation, although the pure fired red mud strength was only 45 MPa. Adding the red mud to the clay ceramic structure, up to 50 wt% and firing at 950 °C for 1 h, improved the properties: strength (52.54 MPa), water absorption (21%) and shrinkage (0.46%), due to the production of a great amount of vitreous phase in the microstructure, as analyzed by SEM. In fact, the optimal proportion of mud to clay was found to be 50 wt%. Arsenovic et al. [131] investigated the possibility of using the sludge from hot dip galvanizing Serbian plants (3 and 6 wt%) incorporated into clay bricks (extruded/870–1020 °C). As main results, the authors found that the compressive strength increases (31 MPa at 1020 °C) with firing temperature but decrease with 6 wt% incorporation (13.5 MPa at 870 °C). The water absorption decreases (7.8 at 1020 °C) but increases (13.7% at 870 °C) with 6 wt% incorporation. SEM analysis revealed that the addition of the sludge decreases the bond ability of the mixture, while increasing the brick porosity. It was concluded that the bricks showed satisfactory mechanical and toxic elements leaching characteristics. Eliche-Quesada et al. [99], an already presented work in Section 3.1, also studied the incorporation of a fluxing inorganic waste obtained from marble residue (up to 20 wt%) incorporated into clay bricks (uniaxial pressing/950 and 1050 °C). TGA/DTA analysis showed, in addition to an initial 2.6% loss of moisture, a residue weight loss of 43% associated with a strong decomposition of CaCO3 into CaO and CO2. A 20 wt% addition of marble residue reduces the brick bulk density (1.87–1.69 g/cm3) at 950 °C and the compressive strength (80–50 MPa) at 1050 °C. SEM observation showed open porosity at 950 °C in contrast with a more closed porosity and denser microstructure at 1050 °C. Lin et al. [132] investigated the incorporation (up to 30 wt%) of a solar panel glass waste into clay bricks (sintered/700–1000 °C). The results indicated that increasing the amount of waste improved the main brick properties by decreasing the water absorption (10%) and increasing the compressive strength (29.4 MPa). In fact, bricks containing 30 wt% of waste fired at 1000 °C met the Chinese standards for first-class brick. The salt crystallization and wet-dry tests showed that the waste incorporation had high beneficial effects by increasing the brick durability. The authors concluded that the waste is suitable for the partial replacement of clay in brick production. Mymrine et al. [133] investigated the joint incorporation of oil-contaminated diatomite residue (25–35 wt%), galvanic sludge (20–25 wt%) and glass waste (5–20 wt%) into a red clay ceramic (uniaxially pressed/950–

Fig. 3. SEM micrograph of a 10 wt% cullet incorporated clay ceramic fired at 1050 °C. Reproduced with permission from [125].

Fig. 4. Variation of the clay ceramic compressive strength with red mud incorporation. Reproduced with permission from [130].

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1100 °C). The results showed that a relatively high bending strength of 22.9 MPa was obtained for a combined mix of 30 wt% diatomite residue, 20 wt% sludge, 20 wt% glass waste and 30 wt% clay ceramic fired at 1100 °C. Microstructural observation by SEM revealed porosity and glass-like surfaces. Moreover, the transformed glassy phases explained the very low lixiviation and solubility of heavy metals from the ceramic structure. The authors concluded that, up to 25 wt%, the rejects of oily diatomite and galvanic sludge, which has a total heavy metal content over 60%, can be used in combination with glass waste and clay for producing an environmentally friendly ceramic to be applied as an economically attractive construction material. Acchar et al. [134] evaluated the incorporation (up to 20 wt%) of untreated coffee husk ashes, rich in alkaline and alkaline-earth metals as flux, into clay ceramic tiles (uniaxially pressed/1100– 1200 °C). The authors indicated that ceramics incorporated with about 10 wt% ashes and fired near 1180 °C presented technical properties, linear shrinkage (6%), water absorption (2%) and flexural strength (24 MPa), that fall within the range specified by the Brazilian standards for floor tiles. SEM analysis revealed spherical isolated pores and typical morphology of mullite needles and leucite crystals. It was concluded that the ashes can advantageously replace feldspars as fluxing agents with the potential to reduce not only natural clay consumptions but also industrial production and landfill costs as well as disposal area requirements. Stathopoulos et al. [135] investigated the stabilization of an electric arc furnace dust by its incorporation (2.5 and 5.0 wt%) into clay ceramics (extruded/850–950 °C). The results showed that the dust addition increased the compressive strength from 2.8 MPa, for neat clay ceramic, to 3.3 MPa, for the 5 wt% dust incorporated ceramic. EDS/SEM microstructural analysis revealed the contribution of Zn-rich particles to the clay ceramic. In addition, the amount of heavy metals leached from pilot scale clay blocks was within the European regulatory limits. A 5 wt% incorporation could provide a high utilization potential for the Greek annual dust generation in the industrial sector of clay block production. Vieira et al. [136] investigated the incorporation of an electric arc furnace dust, collected from an integrated steel plant in Argentina, into red clay ceramics (uniaxial pressing/850 °C). The incorporation was performed in amounts of up to 20 wt% separately mixed with two types of clays, one from Argentina and another from Brazil. The dust was found to act as a non-plastic material, which could adjust the workability of the mixture. The water absorption (14% Brazil and 10% Argentina) and diametral compression (12 MPa Brazil and 7 MPa Argentina) were not significantly affected by the incorporation. The authors attributed the differences between both ceramics, processed from Argentinean and Brazilian clays, to the comparatively higher amount of SiO2 in the Argentinean one. They indicated to be technological feasible to recycle the dust up to 20 wt% into red ceramics fabricated from both types of clays. Quijorna et al. [137] characterized the sintering behavior of a slag obtained from electric arc furnace dust to investigate its potential as a clay substitute in ceramic processes. This so-called Waelz slag, named after the commercial Waelz process for recovering volatile hazardous metallic wastes, was uniaxially pressed and fired at temperatures in the range of 850–1050 °C. In general, an increase of the firing temperature promotes densification and decreases the open porosity (14%), while maintaining an almost constant shrinkage ( 26%) and density (2.5 g/cm3). An effective sintering of the slag started around 950–1000 °C by viscous flow of fluxing compounds producing a glassy phase, which contributes to the fixation of heavy metals. Indeed, at 1050 °C, SEM images show the formation of liquid phase that bonds the grains. Above 950 °C, a weight gain related to gaseous emissions was observed. Firing of the slag affects not only its physical properties but also

its leaching behavior and gaseous emissions through the release of volatile compounds. De la Casa and Castro [138] used washed olive pomace ashes (5 and 10 wt%) to replace clay in bricks manufacture (extruded/1000– 1050 °C). After firing, the bricks with 10 wt% of ash presented a decrease in linear shrinkage (1.5–0.9% at 1050 °C); increase in water absorption (8–14% at 1000 °C); decrease in bulk density (2.0–1.79 g/cm3 at 1025 °C) and decrease in bending strength (19.9–9.4 MPa at 1050 °C). It was also found that lighter masonry units formed with 10 wt% incorporation of washed olive pomace ashes feature a decrease in thermal conductivity (0.84–0.68 W/ m K) and a fired bending strength (10.2 MPa), which is high enough for low density clay masonry.

4. Discussion It is unquestionable the relevance of Zhang’s review article [1] as a contribution to the practical recycling of wastes by incorporation into ceramic pieces (bricks) used as construction and building materials. Zhang’s main points of concern – limited commercial bricks with waste, the method for producing bricks from waste materials, the potential contamination from the used waste, the absence of standards, and the slow acceptance of waste-added bricks by industry and public – are shared by most researchers working on this subject. It is also shared Zhang’s statement that for wide production and application of waste-added bricks, further research and development is needed. As for the government policy and public education, these are relevant points but still open to questions. In many countries, the role played by the market forces should also be considered. Certainly in the case of China, a governmental authority and disciplined public education would favor the adoption of measurements aligned with the country’s interest. There, it could effectively be a greater acceptance of waste-added bricks by both the industry and the end consumer. Moreover, in order to protect its clay resource and the environment, China could defacto limit the use of fired clay bricks. In this case, the cementing and geopolymerization methods of producing construction bricks might in a short time substitute firing, as preconized by Zhang [1]. On the contrary, countries like Italy, Spain, India, Brazil, leading – after China – the world production of clay ceramics for building construction, face different conditions. For instance, in the case of Brazil, the annual production of clay items (blocks, roof tiles, bricks, stoneware pipes, pots, ornamental ware and house utensils) is estimated to be around 180 million tons [139]. The country’s official reserves of common clay amount to 3.7 billion tons. Therefore, at the current consumption, it would take more than 20 years to exhaust the Brazilian clay deposits. From an environmental point of view, this is not only a short time but also a reason for concern regarding soil degradation associated with clay mining. Indeed, the adverse effects of quarrying such as damages to landscape and disposal of related wastes are now punishable by law. For the Brazilian economy the fired clay ceramic industry has been a traditional sector for employment and building construction. Today, the cost of a common 200  200  100 mm hollow clay brick is very low (0.15 US dollars apiece). As the clay deposits are depleted and the environmental legislation enforced, this price will eventually raise and other materials/methods of brick fabrication might, in a long term, prevail in Brazil. The production method, which was the core subject of Zhang’s review [1], deserves to be critically discussed for its implication in future and ongoing research work. A realistic scenario in Brazil indicates that other industrial methods such as cementing and geopolymerization for brick, tile and block production are not competing against fired clay ceramic, both today and within the next

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few decades. Whatever the method and the country, the incorporation of waste should be pursued as an important contribution to save natural clay and protect the environment. However, some points presented and discussed by Zhang [1], especially the drawbacks of high energy consumption, and large footprint associated with the firing method need to be re-examined. As aforementioned, Zhang [1] indicated that a fired clay brick is known on average to have an embodied energy of approximately 2.0 kW h and release about 0.41 kg of CO2 [1,2]. The change in these parameters due to the incorporation of waste was not discussed by Zhang [1]. Actually, considering the relatively small sample of 25 reviewed articles by Zhang [1] on the firing method, only the work of Sengupta et al. [140] made a comment regarding the reduction of process fuel associated with the incorporation of sludge from an Indian petroleum effluent treatment plant. In a communication paper, not reviewed by Zhang [1], the same Indian research group [141] indicated that the calorific value of the dried sludge is 18,213 kJ/kg. In principle, depending on the incorporated amount, this could sensibly reduce the energy consumed for fired ceramic production. Numerous other articles [6–20,84–102] investigated the incorporation of wastes with a carbonaceous content, which might provide a sensible energetic contribution to the ceramic process. For instance, Eliche-Quesada et al. [87] indicated that the high heating value of the bagasse from beer brewing was 19,045 kJ/kg. Even sludges from steelmaking industry [94] with 6648 kJ/kg, Fig. 1, could help in reducing the energy consumed for fired clay ceramic production. Therefore, one may expect that a brick incorporated with fuel-containing waste would require less than 2 kW h for its fabrication. A comparative analysis of clay brick embodied energy needs to be discussed in terms of weight rationalized values as presented in most technical works [142–149]. For instance, Manfredini and Sattler [148] indicated a minimum of 0.291 kW h/kg, which would correspond to 0.48 kW h for a reference clay brick with 1.65 kg. Just for comparison, using his same average brick with Zhang’s [1] indication of 2.0 kW h, then a much higher rationalized value of 1.21 kW h/kg is obtained. As a consequence, it is also possible to fabricate fired clay bricks with much lower embodied energy than that for a cement brick, with 1.5 kW h/kg, as indicated by Zhang [1]. In the particular case of Brazil, the reader should be informed of two special industrial characteristics. First, the production of a common clay brick is usually carried out at firing temperatures as low as 600 °C [150]. Second, most firing fuel, 97% [139], is from biomass. A preference exists for reforestation wood, which is much cheaper than any fossil fuel. Thus, at least in Brazil, a fired clay brick requires a minimum of 0.30 kW h/kg [148]. Moreover, the mixture of steelmaking wastes with clay (a common practice in the state of Minas Gerais) is reported to save 30% in volume of biomass (wood) as firing fuel [149]. Consequently, the incorporation of fuel-containing waste could result in a brick requiring much less than 1 kW h. As aforementioned, this is lower than the energy of 1.5 kW h [1] to produce 1 kg of a Portland cement brick of concrete. It is important to mention that cement is normally fabricated in kiln rotary type of furnaces with limited technical possibility of reducing the energy consumption by using wood as fuel. The reported lower values for fired bricks [143–150] might also be equivalent to the energy to produce a geopolymer brick. Such latter energy has not yet been fully calculated. As for the release of greenhouse gases, the typical Brazilian case of firing clay ceramics using wood as fuel corresponds to a neutral emission of CO2. Indeed, the CO2 emitted during firing is compensated by a similar amount absorbed during the growth of the tree. Regarding the environmental requirements, two situations deserve to be discussed. First, the release during firing of toxic elements that may exist in the waste. Numerous recent works

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[86,93,95,105,112,115,118,129–131,133,135,137] investigated the incorporation of wastes containing toxic elements as well the corresponding impact to the environment. Both drawbacks and advantages were reported. In some cases a toxic compound in the waste may be decomposed during firing and then emitted to the atmosphere as a dangerous pollutant. For example, Sokolar and Vodova [118] reported that the incorporation of CaSO4 containing ashes from a Czech Republic power plant increases the SO2 content to over 4000 ppm in the flue gases during firing above temperatures around 860 °C. Heavy metals containing wastes may also represent a source of contamination through leaching of fired ceramics exposed to an aggressive ambient. For instance, Quijorna et al. [137] indicated that the sintering of a slag from electric arc furnace, with potential as clay substitute in fired ceramics, although reducing the leaching behavior of Zn, Pb and Ba, increase that of Cr and Mo. By contrast, the firing of waste-incorporated clay ceramics could also improve both the environmental requirements and the technical properties. For example, in the work of Caldas et al. [125] flux-containing wastes contribute to form lower temperature glassy phases, Fig. 2, that may retain toxic elements inside an environment-inert ceramic structure, Fig. 3. In the work of Mymrine et al. [133], the combination of a galvanic sludge (60.2 wt% of heavy metals) with glass waste resulted in an inert clay ceramic after incorporation. Indeed, leaching and solubilization tests failed to detect, within the precision of 0.05–0.1 mg/L, any heavy metal extraction out of the ceramic structure. As for the technical properties, from relatively lower up to higher amounts, waste incorporation can improve the linear shrinkage, water absorption and mechanical strength. The example of red mud incorporation in the work of Pérez-Villarejo et al. [130] confirms this improvement up to 90 wt%, Fig. 4, due to the formation of a glassy phase. As a final remark, it is worth mentioning a relevant point regarding geopolymerization. For countries without facilities which exist in Brazil, such as huge clay deposits and extensive reforestation areas, it is acceptable that geopolymerization might be the adequate method to produce bricks. However, geopolymerization is restricted to wastes containing solid aluminosilicate materials like metal processing slag, red mud, fly and bottom ashes as well as mining tailing, stone processing sludges and grog (brick wastes). By contrast, many fuel-containing wastes, such as water treatment plant sludge, biomass, petroleum residues, blast furnace dust and paper mill sludge are not appropriated for geopolymerization. A significant amount of these fuel-containing wastes, especially those with relatively high carbonaceous content, are already being incorporated by Brazilian fired clay ceramic industries [145– 149]. Therefore, one should not expect in a near future any practical contribution of geopolymerization in the Brazilian production of bricks for building construction. 5. Conclusions  An extensive list of articles on the incorporation of wastes in fired clay ceramics has been presented, as a critical update, in complement to the recent review by Zhang [1].  It is shown that the particular case of Brazil, different than that of China, the production of construction building clay pieces (bricks, tiles, blocks) by firing is, and probably will be for the next two decades, more advantageous than cementing or geopolymerization.  The incorporation of fuel-containing waste, in association with a relatively low firing temperature of 600 °C, a common practice in many ceramic industries in Brazil, contribute to reduce the embodied energy to produce a clay brick to much less than the average of 2 kW h indicated by Zhang [1].

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 The prevalent use of reforestation wood as the main fuel for firing clay ceramics in Brazil results in a neutral CO2 emission. This is environmentally better than the case of cementing or geopolymerization that are currently not technically prepared to use biomass as the main source of energy.  The firing method applied to the incorporation of flux-containing wastes allows for glassy phase formation, which encapsulates toxic elements and may render the clay ceramic environmentally inert.

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