refractories WORLDFORUM 4 (2012) [2] 77

1 Magnesia as a mineral

Magnesia (MgO) or the mineralogical term“periclase” was firstly synthesized by heatingof magnesium carbonate (MgCO3) in 1754[1]. In the 18th century magnesium carbonate,which is today known as magnesite, wascalled “magnesia alba”, and magnesium wasextended to the metal in the “magnesia alba”at the same time. The term magnesia derivedfrom a prefecture in Thessaly, Greece namedMagnisia (Μαγνησια), where magnesiumoccurs in form of carbonate rock accompaniedby oxides and carbonates of manganese andiron.The relative abundance of magnesium de-pends on the considered system. In the solarsystem, magnesium is the eighth most abun-dant element, constitutes about 16 % of theentire earth and approximately 2 % of theEarth’s crust respectively. The concentration of magnesium in seawater is about 0,13 %.Magnesium is a highly lithophilic element. Im-portant rock forming minerals of the earthcrust containing magnesium are dolomite,

about 2 trillion tonnes of magnesium in theoceans, and billions of tonnes in deposits ofdolomite, olivine, and magnesium-bearingevaporates [5]. Therefore, the amount of avail-able magnesia is enormous, still in the future.The application of magnesium and magnesiacomponents is manifold. The main consumerfor primary magnesium raw materials likemagnesite, brucite and bischofite are plastics,paper and chemical industry as well as the in-dustry for production of magnesium metal.Highly reactive caustic magnesia, produced

olivine, chlorites as well as the pyroxene andamphibole group minerals. High concentra-tions of magnesium oxide are present in mag-nesite, olivine, brucite and bitterns (bischofite,epsomite, carnallite). Today, more than 60magnesium containing minerals are known. Aselection of magnesium compounds of indus-trial importance is given in Tab. 1.For magnesia extraction, predominate sourcesare magnesite deposits of metasomatic orsedimentary origin with varying quality(coarse and fine crystalline magnesite), sea-water and brines. The more common dolomiteand olivine deposits are also used for synthet-ic production of magnesia. According to theU.S. Geological Survey (USGS), the worldmagnesium compounds annual productioncapacity was about 11,4 Mt in 2010, whereof~89 % is produced from natural magnesiterocks, and ~11 % is sourced from seawater orbrines [4]. A breakdown of the major worldmagnesite mine production and reserves bycountry is given in Tab. 2. This consumptionmay be compared with the currently identifiedglobal magnesite resources of ~12 bil-lion tonnes, several million tonnes of brucite,

Magnesia, an Essential Raw Material for Cement Kiln Refractories

J. Södje, H.-J. Klischat

Dedicated to Dr Peter Bartha on the occasion of his 75th birthday.

Magnesia (MgO) or the min-eralogical term “periclase” wasfirstly synthesized by heating ofmagnesium carbonate (MgCO3)in 1754. The article gives a sur-vey on the industrial use of mag-nesia as refractory material andan historical overview on the ap-plication of basic brick grades incement rotary kilns. The currentstresses on basic refractory lin-ings in cement rotary kilns areoutlined. Prospects for futureR+D work are given.

Tab. 1 Magnesium compound selection of industrial importance (Sources: CRC Handbook of Chemistry and Physics [2], and Pocket Manual RefractoryMaterials [3], d = decomposes)

Mineral FormulaDensity [g/cm3]

HardnessMohs

Melting Point [°C]

MgO Content[%]

Magnesite MgCO3 3,05 4–4½ 540d ~48

Dolomite CaCO3 · MgCO3 2,85 3½–4 750d ~22

Olivine (Mg,Fe)2SiO4 3,27–3,37 6½–7 1205–1890 max. 48

Magnesia/Periclase MgO 3,58 6–6 2840 ~99

Brucite Mg(OH)2 2,36 2½–3 350d ~69

Magnesium chloride MgCl2 2,32 714 ~42

Bischofite MgCl2 · 6H2O 1,59 1–2 116–118 ~20

Carnallite KCI · MgCl2 · 6H2O 1,60 1–2 300d ~14

Magnesium sulfate MgSO4 2,66 1127d ~33

Epsomite MgSO4 · 7H2O 1,68 2–2½ 150d ~16

Magnesium metal Mg 1,74 2½ 650

Johannes Södje, Hans-Jürgen Klischat Refratechnik Cement GmbH37079 GöttingenGermany

Corresponding author: H.-J. Klischat

E-mail: hklischat@refra.com

Keywords: magnesite, magnesia, cement

rotary kiln, lining concept, refractory wear

resistance

78 refractories WORLDFORUM 4 (2012) [2]

between 700 and 1000 °C in rotary or mul-tiple-hearth furnaces, is utilized in differentproducts including special cements (Sorel ce-ment), animal feed, fertilizers, rubber, gas-scrubbing equipment, chemical processing(so-called “Milk of Magnesia”), medicinal andpharmaceutical products, etc. Sintered mag-

nesia, produced in rotary or shaft kilns be-tween 1500 °C and 2300 °C is used for highquality basic refractories. Fused magnesia,produced in electric arc furnaces at tempera-tures >2800 °C, is mainly used for basic car-bon/graphite bricks for the steel industry.More than four-fifths of the annually con-

sumed heat-treated magnesia is processed forrefractory production.However, magnesium is an important elementin the physiology of the biosphere, too. Lifewould not be thinkable without magnesium.For instance, one of the most important bio-logical processes for life on Earth is the pho-tosynthesis. This process requires chlorophyllwhich enables the formation of carbon hy-drates from carbon dioxide and water in sun-light. The central ion of chlorophyll is magne-sium, and a lack of magnesium leads to re-duction in chlorophyll formation finally result-ing in the disease of “chlorosis”. For humanbeings, magnesium is a very important min-eral to promote health. It enhances many en-zyme-related processes (formation of energyfrom blood sugar, effective nerve and musclefunctioning, formation of bones, teeth, etc.).

2 Application of magnesia for refractories

The first industrial use of magnesia as refrac-tory material is linked to the evolution of thesteel industry during the Industrial Revolutionin the second half of the 19th century. Magne-sia was firstly used in blast furnaces in Austriain the period between 1852 and 1859 as re-fractory material [6]. However, rubbles of un-burnt magnesite were probably earlier appliedin facile blast furnaces. Since the 1940s, mag-nesia brick grades like magnesia and magne-sia chromite as well as dolomite bricks are in-stalled in the hot sections of cement rotarykilns [7, 8].In the current technology of steel and cementproduction being the worldwide largest con-sumer of refractories, magnesia is the mostimportant raw material for linings in steel-making vessels (converter, ladles, etc.) and inthe cement kiln system (rotary kiln, hot sec-tions of the static systems (arch of the kilnhood)).The decisive advantage for application ofmagnesia is not only its melting point of 2840 °C which is the highest of all usable re-fractory oxides on an industrial scale, but alsoa high chemical resistance to basic melts andalkalis. Additionally, it forms high-melting binary compounds with the oxides Al2O3, CaO,Cr2O3, Fe2O3, and ZrO2, which can be tolerat-ed as subsidiary components in certain pro-portions or may be desirable for modifying thephysical properties of magnesia (Tab. 3). Therefore, the physical properties of magnesiabricks, such as chemical resistance, thermal

Tab. 2 World Magnesite Mine Production and Reserves of Magnesite, breakdown bycountries [× 103 Mt] (Source: USGS, January 2012 [5], e = estimated)

Fig. 1 Refractory lining concepts in cement rotary kilns up to the 1940s

Mine Production 2010 2011e Reserves

Australia 86 90 95 000

Austria 202 200 15 000

Brazil 115 115 160 000

China 4040 4100 550 000

Greece 86 90 30 000

India 95 100 6 000

North Korea 43 45 450 000

Russia 346 350 650 000

Slovakia 187 190 35 000

Spain 133 130 10 000

Turkey 288 300 49 000

Other countries 141 159 390 000

World total (rounded) 5760 5900 2 500 000

Tab. 3 Important binary refractory compounds of magnesia (Source: Pocket Manual Refractory Materials [3])

Chemical Compound Mineral Name Density [g/cm3] Melting Point [°C]

MgO · Al2O3 Spinel 3,58 2135

MgO · CaO Doloma 2,88 2370 (eutectic)

MgO · Cr2O3 Picochromite 4,42 2350

MgO · Fe2O3 Magnesio ferrite 4,20 1730 (MF + liquid)

MgO · SiO2 Enstatite 3,18 1557

2MgO · SiO2 Forsterite 3,13 1890

0,2MgO · 0,8ZrO2 MgO stab. zirconia – ~2100 (eutectic)

refractories WORLDFORUM 4 (2012) [2] 79

expansion, thermal conductivity, thermalshock resistance, flexibility and hot mechani-cal strength can be modified and adapted tospecific requirements with a certain additionof spinel types (chromium ore, MA spinel, her-cynite, pleonaste, galaxite) as well as with zir-conia, forsterite and graphite. This variety ofusage resulted in various brick grades knowntoday like magnesia chromite bricks, magne-sia spinel bricks, magnesia hercynite bricks,magnesia pleonaste bricks, magnesia galaxitebricks, magnesia zirconia bricks, magnesiacarbon bricks, doloma bricks and a magnesiaforsterite brick as currently latest develop-ment [9–23].

3 Application of basic brick gradesin cement rotary kilns (historical overview)

Due to the changes in burning and kiln systemtechnologies the refractory linings have undergone continuous modifications over themore than 100-year history of cement rotarykilns. Fireclay bricks and high alumina bricksin the hottest section were primary used untilthe 1940s (Fig. 1). Afterwards, basic brick grades like magnesiabricks and magnesia chromite bricks were ap-plied for the first time in the burning section.However, magnesia bricks could not competewith the performance of magnesia chromitebricks due to their poor structural flexibility.Dolomite bricks were installed in the burningzone at the same time, but this brick grade exhibits sensibilities to CO2, sulphur and humidity [24]. The further development of high performancerotary kilns with increasing capacity and higher specific thermal cross sectional loadsmeant that magnesia chromite bricks, likePERILEX® 80, now became essential in themain basic kiln sections (burning zone, Fig. 2).In the mid-seventies, chromite-free magnesiaspinel bricks were firstly tested in the coating-free transition zones in Japanese cement ro-tary kilns [25]. The application of magnesiaspinel bricks started in Germany in the earlyeighties [10]. In this connection, ALMAG® 85became the most popular magnesia spinelbrick for cement rotary kilns. Figs. 3 (rotarykiln with 4-stage preheater) and 4 (rotary kilnwith 4-stage preheater and pre-calcinationAS) broadly show lining concepts with risinguse of magnesia spinel brick grades betweenthe mid of 1980s and the 1990s [26].

tially started in the 1980s, the wear of therefractory lining in cement rotary kilnschanged significantly. Massive salt infiltra-tions mostly with other wear factors be-came more and more evident, apart frommechanical/thermomechanical loads, ther-mal/thermochemical influences, thermaloverload and redox burning conditions,Fig. 5. In summary more than 60 % of post-mortem analyses indicate salt loads com-bined with other stresses. Regarding morethan 1500 post-mortem analyses within thelast ten years (2001–2011), the wear types

Due to the environmental impact of alkalichromate the demand for chromite-free basicbricks in the cement industry increases. Con-sequently, the refractory industry introducednew chromite-free basic brick grades withmodified structural properties and enhancedphysical characteristics [12, 14–17].

4 Current stresses on basic refractory linings in cement rotary kilns

With the implementation of secondary fuelsas energy source for cement burning, ini-

Fig. 2 Refractory lining concept in cement rotary kilns up to the 1980s

Figs. 3, 4 Refractory lining concepts in cement rotary kilns between the mid of 1980sand the 1990s. [Fig 3 (top): rotary kiln with 4-stage preheater, Fig. 4 (below): rotary kiln with 4-stage preheater and precalcination AS]

80 refractories WORLDFORUM 4 (2012) [2]

of silicate corrosion, redox and carbon dis-integration increasingly appear besidesmassive loads by volatile components(salts, and heavy metals), thermal/thermo-chemical stresses and mechanical/thermo-mechanical influences (Fig. 6).

Reducing and/or redox operating conditionsare mostly linked to a not optimum combus-tion of the utilized secondary fuels. These con-ditions are mainly locally limited to kiln sec-tions where coarse fuel material is burning directly on the lining. As a consequence, local

overheating of bricks occurs, and dependingon the oxygen partial pressure elemental carbon condensation in deeper horizons ofthe lining may take place. Fundamental signsof thermal overload are wavy, concave sur-faces or surfaces, which appear to have melt-ed and solidified (Fig. 7).Significant low oxygen partial pressure acti-vates the Boudouard reaction[CO2+C<->2CO].

Due to presence of CO in a reducing atmos-phere on the hot side, elemental carbon maydeposit in lower horizons of the lining in atemperature range below ~600 °C (Fig. 8).Carbon deposits in form of soot on the inter-nal shell are also observed. Damage to thebrickwork by extensive spallings may occurwith this so-called carbon disintegration.Due to the associated process conditions in-cluding the increasing use of secondary fuelsand raw materials within the last years, an in-creasing incorporation of volatile compoundsinto the system is detectable (alkali, sulphur,chloride compounds, and traces of heavy metal elements). These compounds have theaffinity to form various salt compounds whichcondensate in the lining mainly in the lowerand upper transition zones of the kiln (LTZ,UTZ, Fig. 9). While previously principally singlesalts, such as sylvine, arcanite, and anhydrite,were determined in the structure of the bricks,the condensation of mixed salts is currentlydetermined in used bricks to a greater extent.Calcium langbeinite, langbeinite, syngenite aswell as aphthitalite are the mainly determinedmixed salts, in addition to alkali chlorides. In recent years, an excessive amount of sul-phur (SO2/SO3) in the kiln atmosphere is de-tectable due to the increasing use of sulphurrich fuels, such as pet coke. The excessive sul-phur which cannot be bonded by alkalis maythermochemically react with the basic refrac-tory lining. The so-called silicate corrosiontakes place. The silicates, which are present intraces in the magnesia and the magnesia itself are corroded, and form anhydrite andmagnesia containing silicates (merwinite,monticellite, forsterite). Although this wearmechanism is known since the mid of 1980s[28], it can be even detected macroscopicallytoday due to the high sulphur concentrationsin the system. A texture with small and wavypores is the typical sign of this wear in an ad-vanced stage (Fig. 10). The refractoriness andthe structural flexibility of the basic brick arereduced.

Fig. 5 Percentages of various wear factors acted upon basic refractory bricks in rotarykiln systems, based on numerous post-mortem analyses [27]

Fig. 6 Relative distribution of wear influences on basic refractory bricks in cement rotary kilns within the last ten years

Fig. 7 Thermally overloaded basic bricks taken from the lower burning zone. Bleached horizons indicate temporarily reducing operating conditions

Baymag

82 refractories WORLDFORUM 4 (2012) [2]

If the salt loaded brickwork is additionally ex-posed to strong reducing or varying redox atmosphere, condensation of alkali sulphite(K2SO3) and alkali sulphides (K2S, K2S3) be-sides alkali sulphates (K2SO4) occurs. Duringkiln stops these strongly hygroscopic saltseasily draw moisture from air, and a typicalH2S smell is perceivable, especially during re-

the demands placed on the refractory lininghave intensified. The main causes of this trendare the increasing use of secondary fuels andraw materials, the increased capacity and en-ergy input of the plants and additionallyadopted combustion modules.Regarding these conditions, the elongation of the zones in the rotary kiln installed with basic brick grades is indispensable(Fig. 12).Additionally, following essential demands areplaced upon the basic refractory products toreduce or prevent the before mentioned wearphenomena from the refractory side:• minimisation of infiltration and corrosion of

refractory components• optimisation of the structural texture by

higher flexibility and high structuralstrength

• optimisation of the thermochemical andthermal resistance.

Within the last ten years, successes relating toincreased wear resistance and lifetime exten-sion of refractories were already achievedwith the development of basic bricks withlower apparent porosity and higher structuralstrength combined with increased structuralflexibility, like the AF-product ALMAG® AF. Initial positive trials of these brick grades werealready carried out at the turn of the millen-nium.For higher mechanically loaded kiln sections,like tire areas, basic brick grades with in-creased chemical resistance combined withexcellent structural flexibility were also devel-oped within the last years, like the magnesiaspinel brick grade ALMAG® A1.For the burning zone, which temporarily suf-fers operational thermal fluctuations due tothe use of different secondary fuels, thermo-chemically reinforced concepts combined with

moval of bricks from the lining. Fig. 11 showssuch loaded used bricks with differentlycoloured salt efflorescences on the surfaces.

5 Conclusion and prospect

From the selected examples of wear phenom-ena it is clear that, in spite of the optimisationof the process technology of cement plants,

Fig. 8 Thermally loaded bricks including hot face clinker melt infiltration and condensa-tion of elemental carbon at the cold face side (left/right: black horizons). The sample inthe middle is the re-oxidized counterpart from right: the condensated carbon is burnedout and the bleaching vanishes.

Fig. 9 Salt and heavy metal infiltrations in different horizons of basic bricks: LTZ (left)= mainly alkali sulphate salts, UTZ (in the middle: mainly alkali chloride and alkali sul-phate salts; right: lead sulphite (PbS), and alkali chloride and alkali sulphate salts)

Fig. 10 Type of silicate corrosion due toexcessive sulphur in the kiln atmosphere

Fig. 11 Used bricks exposed to reducing atmosphere including salt condensations andefflorescences

easier coating formation behaviour are ap-proaching solutions, like magnesia pleonastebrick grades. Additionally, the magnesiapleonaste and magnesia forsterite brick gradesare alternative solutions for the burning zone re-garding innovative cost/performance-orientedchrome-free brick grade developments.Although recent years have seen the develop-ment of a particular market for secondary fuels of uniform quality in terms of fraction andcalorific value to meet the requirements of thecement industry, the process control of a cementplant will continue to remain a challenge in thefuture due to changing fuel usage.Therefore, the optimisation of the infiltration andcorrosion resistance combined with optimisedstructural flexibility as well as the thermochemi-cal and thermal resistance of the refractory prod-ucts will continue to be the focus of major de-velopment work from the refractory industryside.

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Fig. 12 Current refractory lining concept in cement rotary kilns with pre-calcination

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