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.

Tab. 1 Magnesium compound selection of industrial importance

Magnesia (MgO) or the min- (Sources: CRC Handbook of Chemistry and Physics [2], and Pocket Manual Refractory
Materials [3], d = decomposes)
eralogical term “periclase” was
Density Hardness Melting MgO Content
firstly synthesized by heating of Mineral Formula
[g/cm3] Mohs Point [°C] [%]
magnesium carbonate (MgCO3) Magnesite MgCO3 3,05 4–4½ 540d ~48
in 1754. The article gives a sur- Dolomite CaCO3 · MgCO3 2,85 3½–4 750d ~22
vey on the industrial use of mag- Olivine (Mg,Fe)2SiO4 3,27–3,37 6½–7 1205–1890 max. 48
nesia as refractory material and Magnesia/Periclase MgO 3,58 6–6 2840 ~99
Brucite Mg(OH)2 2,36 2½–3 350d ~69
an historical overview on the ap-
Magnesium chloride MgCl2 2,32 714 ~42
plication of basic brick grades in
Bischofite MgCl2 · 6H2O 1,59 1–2 116–118 ~20
cement rotary kilns. The current Carnallite KCI · MgCl2 · 6H2O 1,60 1–2 300d ~14
stresses on basic refractory lin- Magnesium sulfate MgSO4 2,66 1127d ~33
ings in cement rotary kilns are Epsomite MgSO4 · 7H2O 1,68 2–2½ 150d ~16
outlined. Prospects for future Magnesium metal Mg 1,74 2½ 650
R+D work are given.
olivine, chlorites as well as the pyroxene and about 2 trillion tonnes of magnesium in the
amphibole group minerals. High concentra- oceans, and billions of tonnes in deposits of
1 Magnesia as a mineral tions of magnesium oxide are present in mag- dolomite, olivine, and magnesium-bearing
Magnesia (MgO) or the mineralogical term nesite, olivine, brucite and bitterns (bischofite, evaporates [5]. Therefore, the amount of avail-
“periclase” was firstly synthesized by heating epsomite, carnallite). Today, more than 60 able magnesia is enormous, still in the future.
of magnesium carbonate (MgCO3) in 1754 magnesium containing minerals are known. A The application of magnesium and magnesia
[1]. In the 18th century magnesium carbonate, selection of magnesium compounds of indus- components is manifold. The main consumer
which is today known as magnesite, was trial importance is given in Tab. 1. for primary magnesium raw materials like
called “magnesia alba”, and magnesium was For magnesia extraction, predominate sources magnesite, brucite and bischofite are plastics,
extended to the metal in the “magnesia alba” are magnesite deposits of metasomatic or paper and chemical industry as well as the in-
at the same time. The term magnesia derived sedimentary origin with varying quality dustry for production of magnesium metal.
from a prefecture in Thessaly, Greece named (coarse and fine crystalline magnesite), sea- Highly reactive caustic magnesia, produced
Magnisia (Μαγνησια), where magnesium water and brines. The more common dolomite
occurs in form of carbonate rock accompanied and olivine deposits are also used for synthet-
by oxides and carbonates of manganese and ic production of magnesia. According to the Johannes Södje, Hans-Jürgen Klischat
iron. U.S. Geological Survey (USGS), the world Refratechnik Cement GmbH
The relative abundance of magnesium de- magnesium compounds annual production 37079 Göttingen
pends on the considered system. In the solar capacity was about 11,4 Mt in 2010, whereof Germany
system, magnesium is the eighth most abun- ~89 % is produced from natural magnesite
dant element, constitutes about 16 % of the rocks, and ~11 % is sourced from seawater or Corresponding author: H.-J. Klischat
entire earth and approximately 2 % of the brines [4]. A breakdown of the major world E-mail: hklischat@refra.com
Earth’s crust respectively. The concentration magnesite mine production and reserves by
of magnesium in seawater is about 0,13 %. country is given in Tab. 2. This consumption Keywords: magnesite, magnesia, cement
Magnesium is a highly lithophilic element. Im- may be compared with the currently identified rotary kiln, lining concept, refractory wear
portant rock forming minerals of the earth global magnesite resources of ~12 bil- resistance
crust containing magnesium are dolomite, lion tonnes, several million tonnes of brucite,

refractories WORLDFORUM 4 (2012) [2] 77

Tab. 2 World Magnesite Mine Production and Reserves of Magnesite, breakdown by sumed heat-treated magnesia is processed for
countries [× 103 Mt] (Source: USGS, January 2012 [5], e = estimated) refractory production.
Mine Production However, magnesium is an important element
Reserves
2010 2011e in the physiology of the biosphere, too. Life
Australia 86 90 95 000 would not be thinkable without magnesium.
For instance, one of the most important bio-
Austria 202 200 15 000
logical processes for life on Earth is the pho-
Brazil 115 115 160 000
tosynthesis. This process requires chlorophyll
China 4040 4100 550 000 which enables the formation of carbon hy-
Greece 86 90 30 000 drates from carbon dioxide and water in sun-
India 95 100 6 000 light. The central ion of chlorophyll is magne-
North Korea 43 45 450 000 sium, and a lack of magnesium leads to re-
duction in chlorophyll formation finally result-
Russia 346 350 650 000
ing in the disease of “chlorosis”. For human
Slovakia 187 190 35 000 beings, magnesium is a very important min-
Spain 133 130 10 000 eral to promote health. It enhances many en-
Turkey 288 300 49 000 zyme-related processes (formation of energy
Other countries 141 159 390 000 from blood sugar, effective nerve and muscle
functioning, formation of bones, teeth, etc.).
World total (rounded) 5760 5900 2 500 000
2 Application of magnesia
Tab. 3 Important binary refractory compounds of magnesia for refractories
(Source: Pocket Manual Refractory Materials [3])
The first industrial use of magnesia as refrac-
Chemical Compound Mineral Name Density [g/cm3] Melting Point [°C]
tory material is linked to the evolution of the
MgO · Al2O3 Spinel 3,58 2135 steel industry during the Industrial Revolution
MgO · CaO Doloma 2,88 2370 (eutectic) in the second half of the 19th century. Magne-
MgO · Cr2O3 Picochromite 4,42 2350 sia was firstly used in blast furnaces in Austria
MgO · Fe2O3 Magnesio ferrite 4,20 1730 (MF + liquid)
in the period between 1852 and 1859 as re-
fractory material [6]. However, rubbles of un-
MgO · SiO2 Enstatite 3,18 1557
burnt magnesite were probably earlier applied
2MgO · SiO2 Forsterite 3,13 1890 in facile blast furnaces. Since the 1940s, mag-
0,2MgO · 0,8ZrO2 MgO stab. zirconia – ~2100 (eutectic) nesia brick grades like magnesia and magne-
sia chromite as well as dolomite bricks are in-
between 700 and 1000 °C in rotary or mul- nesia, produced in rotary or shaft kilns be- stalled in the hot sections of cement rotary
tiple-hearth furnaces, is utilized in different tween 1500 °C and 2300 °C is used for high kilns [7, 8].
products including special cements (Sorel ce- quality basic refractories. Fused magnesia, In the current technology of steel and cement
ment), animal feed, fertilizers, rubber, gas- produced in electric arc furnaces at tempera- production being the worldwide largest con-
scrubbing equipment, chemical processing tures >2800 °C, is mainly used for basic car- sumer of refractories, magnesia is the most
(so-called “Milk of Magnesia”), medicinal and bon/graphite bricks for the steel industry. important raw material for linings in steel-
pharmaceutical products, etc. Sintered mag- More than four-fifths of the annually con- making vessels (converter, ladles, etc.) and in
the cement kiln system (rotary kiln, hot sec-
tions of the static systems (arch of the kiln
hood)).
The decisive advantage for application of
magnesia is not only its melting point of
2840 °C which is the highest of all usable re-
fractory oxides on an industrial scale, but also
a high chemical resistance to basic melts and
alkalis. 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 the
physical properties of magnesia (Tab. 3).
Therefore, the physical properties of magnesia
Fig. 1 Refractory lining concepts in cement rotary kilns up to the 1940s bricks, such as chemical resistance, thermal

78 refractories WORLDFORUM 4 (2012) [2]

expansion, thermal conductivity, thermal
shock resistance, flexibility and hot mechani-
cal strength can be modified and adapted to
specific requirements with a certain addition
of spinel types (chromium ore, MA spinel, her-
cynite, pleonaste, galaxite) as well as with zir-
conia, forsterite and graphite. This variety of
usage resulted in various brick grades known
today like magnesia chromite bricks, magne-
sia spinel bricks, magnesia hercynite bricks, Fig. 2 Refractory lining concept in cement rotary kilns up to the 1980s
magnesia pleonaste bricks, magnesia galaxite
bricks, magnesia zirconia bricks, magnesia
carbon bricks, doloma bricks and a magnesia
forsterite brick as currently latest develop-
ment [9–23].

3 Application of basic brick grades

in cement rotary kilns
(historical overview)
Due to the changes in burning and kiln system
technologies the refractory linings have
undergone continuous modifications over the
more than 100-year history of cement rotary
kilns. Fireclay bricks and high alumina bricks
in the hottest section were primary used until
Figs. 3, 4 Refractory lining concepts in cement rotary kilns between the mid of 1980s
the 1940s (Fig. 1). and the 1990s.
Afterwards, basic brick grades like magnesia [Fig 3 (top): rotary kiln with 4-stage preheater,
bricks and magnesia chromite bricks were ap- Fig. 4 (below): rotary kiln with 4-stage preheater and precalcination AS]
plied for the first time in the burning section.
However, magnesia bricks could not compete
with the performance of magnesia chromite
bricks due to their poor structural flexibility.
Dolomite bricks were installed in the burning
zone at the same time, but this brick grade
exhibits sensibilities to CO2, sulphur and
humidity [24].
The further development of high performance
rotary kilns with increasing capacity and
higher specific thermal cross sectional loads
meant that magnesia chromite bricks, like
PERILEX® 80, now became essential in the
main basic kiln sections (burning zone,
Fig. 2).
In the mid-seventies, chromite-free magnesia Due to the environmental impact of alkali tially started in the 1980s, the wear of the
spinel bricks were firstly tested in the coating- chromate the demand for chromite-free basic refractory lining in cement rotary kilns
free transition zones in Japanese cement ro- bricks in the cement industry increases. Con- changed significantly. Massive salt infiltra-
tary kilns [25]. The application of magnesia sequently, the refractory industry introduced tions mostly with other wear factors be-
spinel bricks started in Germany in the early new chromite-free basic brick grades with came more and more evident, apart from
eighties [10]. In this connection, ALMAG® 85 modified structural properties and enhanced mechanical/thermomechanical loads, ther-
became the most popular magnesia spinel physical characteristics [12, 14–17]. mal/thermochemical influences, thermal
brick for cement rotary kilns. Figs. 3 (rotary overload and redox burning conditions,
kiln with 4-stage preheater) and 4 (rotary kiln 4 Current stresses on basic Fig. 5. In summary more than 60 % of post-
with 4-stage preheater and pre-calcination refractory linings in cement mortem analyses indicate salt loads com-
AS) broadly show lining concepts with rising rotary kilns bined with other stresses. Regarding more
use of magnesia spinel brick grades between With the implementation of secondary fuels than 1500 post-mortem analyses within the
the mid of 1980s and the 1990s [26]. as energy source for cement burning, ini- last ten years (2001–2011), the wear types

refractories WORLDFORUM 4 (2012) [2] 79

 overheating of bricks occurs, and depending
on the oxygen partial pressure elemental
carbon condensation in deeper horizons of
the lining may take place. Fundamental signs
of 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 may
deposit in lower horizons of the lining in a
temperature range below ~600 °C (Fig. 8).
Carbon deposits in form of soot on the inter-
Fig. 5 Percentages of various wear factors acted upon basic refractory bricks in rotary nal shell are also observed. Damage to the
kiln systems, based on numerous post-mortem analyses [27] brickwork by extensive spallings may occur
with this so-called carbon disintegration.
Due to the associated process conditions in-
cluding the increasing use of secondary fuels
and raw materials within the last years, an in-
creasing incorporation of volatile compounds
into the system is detectable (alkali, sulphur,
chloride compounds, and traces of heavy
metal elements). These compounds have the
affinity to form various salt compounds which
condensate in the lining mainly in the lower
and upper transition zones of the kiln (LTZ,
UTZ, Fig. 9). While previously principally single
salts, such as sylvine, arcanite, and anhydrite,
were determined in the structure of the bricks,
the condensation of mixed salts is currently
determined in used bricks to a greater extent.
Fig. 6 Relative distribution of wear influences on basic refractory bricks in cement
Calcium langbeinite, langbeinite, syngenite as
rotary kilns within the last ten years
well as aphthitalite are the mainly determined
mixed 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 sulphur
rich fuels, such as pet coke. The excessive sul-
phur which cannot be bonded by alkalis may
thermochemically react with the basic refrac-
tory lining. The so-called silicate corrosion
takes place. The silicates, which are present in
traces in the magnesia and the magnesia
itself are corroded, and form anhydrite and
magnesia containing silicates (merwinite,
monticellite, forsterite). Although this wear
mechanism is known since the mid of 1980s
Fig. 7 Thermally overloaded basic bricks taken from the lower burning zone.
[28], it can be even detected macroscopically
Bleached horizons indicate temporarily reducing operating conditions
today due to the high sulphur concentrations
of silicate corrosion, redox and carbon dis- Reducing and/or redox operating conditions in the system. A texture with small and wavy
integration increasingly appear besides are mostly linked to a not optimum combus- pores is the typical sign of this wear in an ad-
massive loads by volatile components tion of the utilized secondary fuels. These con- vanced stage (Fig. 10). The refractoriness and
(salts, and heavy metals), thermal/thermo- ditions are mainly locally limited to kiln sec- the structural flexibility of the basic brick are
chemical stresses and mechanical/thermo- tions where coarse fuel material is burning reduced.
mechanical influences (Fig. 6). directly on the lining. As a consequence, local

80 refractories WORLDFORUM 4 (2012) [2]

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 the demands placed on the refractory lining
have intensified. The main causes of this trend
are the increasing use of secondary fuels and
raw materials, the increased capacity and en-
ergy input of the plants and additionally
adopted 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 are
placed upon the basic refractory products to
Fig. 8 Thermally loaded bricks including hot face clinker melt infiltration and condensa-
reduce or prevent the before mentioned wear
tion of elemental carbon at the cold face side (left/right: black horizons). The sample in
phenomena from the refractory side:
the middle is the re-oxidized counterpart from right: the condensated carbon is burned
out and the bleaching vanishes.
• minimisation of infiltration and corrosion of
refractory components
• optimisation of the structural texture by
higher flexibility and high structural
strength
• optimisation of the thermochemical and
thermal resistance.
Within the last ten years, successes relating to
increased wear resistance and lifetime exten-
sion of refractories were already achieved
with the development of basic bricks with
lower apparent porosity and higher structural
strength combined with increased structural
flexibility, like the AF-product ALMAG® AF.
Initial positive trials of these brick grades were
already carried out at the turn of the millen-
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-
nium.
phate salts; right: lead sulphite (PbS), and alkali chloride and alkali sulphate salts) For higher mechanically loaded kiln sections,
like tire areas, basic brick grades with in-
If the salt loaded brickwork is additionally ex- moval of bricks from the lining. Fig. 11 shows creased chemical resistance combined with
posed to strong reducing or varying redox such loaded used bricks with differently excellent structural flexibility were also devel-
atmosphere, condensation of alkali sulphite coloured salt efflorescences on the surfaces. oped within the last years, like the magnesia
(K2SO3) and alkali sulphides (K2S, K2S3) be- spinel brick grade ALMAG® A1.
sides alkali sulphates (K2SO4) occurs. During 5 Conclusion and prospect For the burning zone, which temporarily suf-
kiln stops these strongly hygroscopic salts From the selected examples of wear phenom- fers operational thermal fluctuations due to
easily draw moisture from air, and a typical ena it is clear that, in spite of the optimisation the use of different secondary fuels, thermo-
H2S smell is perceivable, especially during re- of the process technology of cement plants, chemically reinforced concepts combined with

Fig. 10 Type of silicate corrosion due to Fig. 11 Used bricks exposed to reducing atmosphere including salt condensations and
excessive sulphur in the kiln atmosphere efflorescences

82 refractories WORLDFORUM 4 (2012) [2]

 easier coating formation behaviour are ap-
proaching solutions, like magnesia pleonaste
brick grades. Additionally, the magnesia
pleonaste and magnesia forsterite brick grades
are alternative solutions for the burning zone re-
garding innovative cost/performance-oriented
chrome-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 and
calorific value to meet the requirements of the
cement industry, the process control of a cement
plant will continue to remain a challenge in the
future due to changing fuel usage.
Therefore, the optimisation of the infiltration and
Fig. 12 Current refractory lining concept in cement rotary kilns with pre-calcination
corrosion resistance combined with optimised
structural flexibility as well as the thermochemi-
cal and thermal resistance of the refractory prod- [2] CRC Handbook of Chemistry and Physics, 80th Edi- [6] Zednicek, W.: Periclase, a remarkable and essential
ucts will continue to be the focus of major de- tion, 1999/2000 mineral for refractory ceramics. Radex-Rundschau
velopment work from the refractory industry [3] Routschka, G.: Pocket Manual Refractory Material, (1985) [4] 651–695
side. 3rd Ed., Essen 2008 [7] Hotz, G.; Bartha, P.: Stand der feuerfesten Zustel-
[4] U.S. Geogical Survey (USGS): 2010 Minerals Year- lung von Drehofenanlagen. ZKG International 28
References book, Magnesium compounds [Advance Release] (1975) [6] 236–240
[1] Black, J.: De humore acido a cibis orto et magnesia [5] U.S. Geogical Survey (USGS): Mineral Commodity [8] Bartha, P.: Mineralogische-chemische Veränderung
alba. Ph. D. Thesis, Edinburgh 1754 Summaries, January 2012 an Dolomitsteinen während des Einsatzes in Ze-

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 mentdrehöfen. ZKG International 25 (1972) [8] [15] Klischat, H.-J.; Weibel, G.; Bartha, P.: Entwicklungs- [22] Jansen, H.; Grosse Daldrup, H.; Subramaniam Mu-
359–364 stand chromerzfreier Magnesiasteinsorten für die thu Kumar: Latest developments of refractory linings
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E 277–E 280 CN-Special Refractories, Vol. 6 (1999) 3 on Refractories, Aachen 1983, 204–225

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