Hydrometallurgy 108 (2011) 33–45

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Hydrometallurgy
j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / h yd r o m e t

Bauxite residue issues: I. Current management, disposal and storage practices

G. Power, M. Gräfe, C. Klauber ⁎
CSIRO Process Science and Engineering (Parker CRC), Light Metals National Research Flagship, PO Box 7229, Karawara WA 6152, Australia

a r t i c l e i n f o a b s t r a c t

Article history: Bauxite residue has been continuously produced since the inception of the alumina/aluminium industry in the
Received 19 August 2010 late nineteenth century. The global inventory of bauxite residue reached an estimated 2.7 billion tonnes in 2007
Received in revised form 1 February 2011 increasing at 120 million tonnes per annum. This growth highlights the urgency to develop and implement
Accepted 14 February 2011
improved means of storage and remediation, and to pursue large-volume utilization options of residue as an
Available online 24 February 2011
industrial by-product. This review looks at current management practices for disposal and amendment, and how
Keywords:
each unit process influences residue properties. Since 1980 the trend has been away from lagoon-type
Red mud impoundments towards “dry” stacking; this reduces the potential for leakage, reduces the physical footprint and
Bauxite residue improves recoveries of soda and alumina. Associated technical developments in residue neutralization are
Bayer process solids considered with possible future practices in residue disposal and how that might best integrate with future
Global residue inventory utilization. For example, hyperbaric steam filtration is an emerging technology that could discharge residue as a
BRDA engineering dry, granular material of low soda content. Such properties are beneficial to long term storage and remediation,
Dry-stacking but importantly also to future utilization. Although residue has a number of characteristics of environmental
Lagooning
concern, the most immediate and apparent barrier to remediation and utilization (improved sustainability) is its
Residue utilization
high alkalinity and sodicity. The sustained alkalinity is the result of complex solid-state and solution phase
BRaDD
Marine disposal interactions while its sodicity arises from the use of caustic soda (NaOH) for digestion. This is the first in a series of
four related reviews examining bauxite residue issues in detail.
Crown Copyright © 2011 Published by Elsevier B.V. All rights reserved.

1. Introduction
Bauxite residue and its appropriate management is of increasing
environmental concern. As the global demand for aluminium metal
continues in transportation, packaging and construction, from the
fabrication of fuselages and car parts to disposable containers and
various consumer durables, the legacy of nearly 120 years of alumina
extraction from bauxite ore is manifested as an estimated 2.7 billion -
tonnes (Bt) of hazardous material commonly referred to either as red
mud or bauxite residue. This amount is currently increasing by
approximately 120 million tonnes per annum (Mtpa). Storage locations
vary from purpose built, well-engineered containment areas through to
simply utilizing natural landscape depressions and the bottom of the
ocean (marine disposal). Despite the long-standing recognition of
bauxite residue as a problem, it has never been satisfactorily resolved. In
order to understand why this has arisen and to seek possible solutions
for better management, it is very useful to consider all aspects of
production, chemistry, residue value and barriers to utilization. This is
the first in a series of four reviews examining issues pertinent to bauxite
residue and its environmental impact (see also Klauber et al., 2011;
Gräfe et al., 2011; Gräfe and Klauber, 2011). Ultimately, the aim is to
⁎ Corresponding author. Tel.: + 61 8 9334 8060; fax: + 61 8 9334 8001.
E-mail address: craig.klauber@csiro.au (C. Klauber).
identify the technologies or practices for either the alternative use of
bauxite residues and/or improved storage practices.
2. Overview of bauxite residue management
2.1. History and future of bauxite residue
In order to appreciate the trends in both awareness and
perceptions of residue, the evolution of technologies, management
systems and the regulatory situation, it is worthwhile examining the
history of the alumina industry and the inevitable growth in the world
residue inventory and how it has been managed.
In 1885, Karl Josef Bayer moved from Brno (Czech Republic, then
Austro-Hungarian Empire) to St. Petersburg, where he joined the
Tentelev Chemical Plant to work on the dying of cotton fabrics using
pure aluminium hydroxide, which was a rare and expensive raw
material. By 1887 he had discovered that aluminum hydroxide could
be precipitated in crystalline form from a cold sodium aluminate
(NaAl(OH)4) solution, if a seed of aluminium hydroxide was used. On
July 17, 1887, the Imperial Patent Office of Germany issued patent
number 43977 “Verfahren zur Darstellung von Thonerdehydrat und
Alkalialuminat”.1 Shortly after, he discovered that the required NaAl
(OH)4 solution could be prepared by heating bauxite under pressure
1
Process for synthesis of aluminium oxide hydrate (gibbsite) and alkali aluminate.

0304-386X/$ – see front matter. Crown Copyright © 2011 Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.hydromet.2011.02.006
34
140 Global residue production and inventory
residue production rate (Mtpa)
120 annual residue production
cumulative inventory
100
80
60
40
20
0 0
1900 1920 1940 1960 1980
year
Fig. 1. Global production rate and cumulative inventory of bauxite residue.
in concentrated caustic soda (NaOH) solution, a process that he
patented shortly after (Patent number 65604 issued by the German
Imperial Patent Office 31 January 1892). Bayer's two patents formed
that basis of the industrial process of extracting and synthesizing
gibbsite that now bears his name (Habashi, 1988).2
The potential for the Bayer process to provide alumina as feedstock
for the newly invented process for manufacturing aluminium metal
was quickly realized. By 1892 Bayer plants had been established in
England, France, Italy and Germany for this purpose. Between 1893
and 1910 two further Bayer plants were built in France and the
Pittsburgh Reduction Company (later Alcoa) built the first Bayer plant
in the USA at East St. Louis (Illinois). In the ensuing 30 years, more
plants were built in the USA, Germany, Great Britain, Japan and the
Soviet Union. Of these early plants, only the plant at Gardanne
(France) is still operating today.
From these beginnings the aluminium industry grew rapidly. From
6800 tonnes in 1900 the global production rate of aluminium metal
reached 1 Mtpa in 1940. The global inventory of bauxite residue at
that time can be estimated to have been approximately 22 Mt,
associated with production facilities that were small by today's
standards. The available literature up to that time makes little
mention of bauxite residue, other than to account for dealing with it
as part of the cost of production. It appears that neither the industry,
public nor governments viewed bauxite residue as an issue of social or
environmental importance.
Technology development and economies of scale have driven the
development of increasingly larger production facilities. By the 1980s,
1 Mtpa was the size of new plants being built in Australia and Brazil,
with plants in Spain and Ireland expanding beyond 1 Mtpa in the early
1990s. Today Alunorte (Barcarena, Brazil) is targeting a production of
6 Mtpa. By 1985 residue was being produced at a rate of approxi-
mately 48.5 Mtpa and the global inventory of residue neared the 1 Bt
mark. In 2007 the annual production of residue was an estimated
120 Mtpa and the global inventory had risen to over 2.6 Bt. Thus it
took approximately 90 years to generate the first billion tonnes of
residue, but only approximately 15 years to produce the second.
These figures suggest that 3 Bt will be exceeded between 2010 and
2015. Our estimates of the growth in the inventory and rate of
production of bauxite residue from 1900 to 2007 are shown in Fig. 1
and are based on alumina and aluminum metal production.
Where alumina production data is not directly available, the
annual production values have been inferred by applying a factor of 2
to the production values for aluminium metal. This factor is calculated
from the stoichiometric ratio of 1.9 plus an additional 0.1 to allow for
alumina being produced for non-metallurgical uses (0.08, Roskill,
2
The dates suggested by Habashi (1988) are incorrect as can be evidenced from the
original patents. The correct dates are presented here.
G. Power et al. / Hydrometallurgy 108 (2011) 33–45
3000
2008) and for dust and other losses in the conversion of the oxide to
the metal. Bauxite residue tonnage was then estimated by applying an
2500
overall ratio of 1.5 to the alumina production (Hamada, 1986). Factors
such as bauxite grade, alumina extraction efficiency and caustic losses
cumulative residue (Mt)
2000 will vary between refinery operations so a world average ratio value
of 1.5 should only be regarded as approximate.
1500
2.2. Need for a cohesive residue database: Development of BRaDD
1000
It appears to have been in the early 1980s, when the bauxite residue
inventory was approaching the 1 Bt level, that bauxite residue became
500
recognized as an issue of increasing environmental importance to the
future of the industry. In 1981, the United Nations Environmental
2000 Programme (UNEP) and the United Nations Industrial Development
Organization (UNIDO) jointly sponsored a workshop in Paris to examine
the environmental aspects of alumina production. Overviews of the
workshop, “Environmental Aspects of Alumina Production”, are
available as a UNEP pamphlet (United Nations Industrial Development
Organisation, 1985), and in a conference paper by (Hamada, 1986).
In 1986, The University of the West Indies and The Jamaica Bauxite
Institute conducted the first conference and workshop on bauxite
tailings in Kingston (Jamaica) co-sponsored by UNIDO and the
International Research Development Centre (IRDC) and major
producers of alumina and aluminium (Wagh and Desai, 1986). A
subsequent bauxite tailings workshop was held in Perth (Australia)
1992 under the sponsorship of the Australian bauxite and alumina
producers (Glenister, 1992).
Other useful sources of publications relating to bauxite residue
storage and disposal have been conference proceedings of the annual
Light Metals conferences of The Minerals, Metals and Materials
Society (TMS), the Alumina Quality Workshop held every 3 years in
Australia, and the International Committee for the Study of Bauxite,
Alumina & Aluminium (ICSOBA). In the general academic literature
(journal and conference proceedings) only a small number of
publications relating to bauxite residues and storage issues have
appeared. From the first publication in 1977 to date, there are about
90 papers (excluding pre-1990 conference proceedings and patents)
and CSA's Aluminium Industry Abstracts lists 220 publications since
1968 including patents, peer-reviewed journal articles, other articles
and conference proceedings.
Surveys of the accessible literature on residue revealed that the
various data domains placed a severe limitation on the ability to
collect, systematize and interrogate information on residue. A number
of key features are apparent:
1. Relevant information is scattered over many public domain sources:
journals, conference proceedings, patents, company reports, securi-
ties and exchange commission reports, newspaper articles, PhD and
MSc theses, and other miscellaneous sources. Much of the informa-
tion is not peer-reviewed, but is essential to construct an under-
standing of residue management.
2. Each source of information provides only a limited amount of
relevant data, and the data type is not consistent across publications.
3. The relevant information is published in a variety of languages,
principally Chinese, English, French, German, Portuguese, Russian
and Spanish.
4. The nature and scope of the information is owner and/or refinery
specific and not consistent in either form or content.
5. Each refinery has unique operating details with respect to bauxite
residue technologies, management and engineering practices.
6. The operating details of each refinery may or may not change in
any given year.
That is, for every refinery, a multifactorial data set propagates over
time, which must then be combined over all refineries in order to
provide a true reflection of technology, storage practices, engineering,
 G. Power et al. / Hydrometallurgy 108 (2011) 33–45 35

science, utilization options and chemistry relevant to bauxite residue. simplest method, the residue slurry from the washing circuit is
The absence of a means of collecting and managing information disposed directly into the sea, usually via a pipeline that takes the
on bauxite residue is a key impediment to elucidate knowledge slurry well offshore for discharge into the deep ocean. For lagooning
gaps about bauxite residue. This prompted the creation of an on-line the residue slurry from the washing circuit is pumped into land-based
database that would contain details on refinery practices on bauxite ponds. Such ponds may be formed within natural depressions using
residue storage, disposal, and technologies gathered from a wide dams and other earthworks to ensure secure containment. More
range of sources with an aim to provide a comprehensive resource recently the emphasis has been on dry disposal, namely “dry” stacking
through which data could be compared and analyzed in a variety of and dry cake disposal. “Dry” stacking is a misnomer as the residue is
ways. The database, known as the Bauxite, Residue and Disposal actually not dry at time of discharge. Each method has advantages and
Database (BRaDD), is publicly available to interested parties at no cost disadvantages that are summarized in Table 3.
(see Gräfe et al., 2009, 2010). BRaDD has been an essential enabling The main factors determining the choice of disposal method for
tool for the collation and interpretation of information required for a given refinery are local rainfall and topography and the land
this and the subsequent reviews in this series. It is hoped that later availability in the context of the grade and mineralogy of the bauxite
versions of BRaDD, with data input from the industry, will provide and the size of the refinery (which together determine the rate of
invaluable support to the development of a global strategy for the residue production) and of course legislative requirements. Secondary
future of bauxite residue management. factors that can influence choice are the economics of trucking versus
pumping to the BRDA. French and Japanese practices have historically
2.3. Bauxite residue production process: red side favoured disposal at sea as the best option on economic and
environmental grounds. North American practice has favoured land-
The success of the Bayer process is demonstrated by the fact that, based disposal in lagoons, even for refineries on the seaboard.
despite enormous technological advances and the need to process a The 1970s saw a major expansion of the alumina industry in
wide range of ore types, the basic chemistry and operational steps of a response to growth in primary aluminium production, resulting in a
modern Bayer plant are fundamentally the same as originally rapid growth in the production rate and global inventory of bauxite
described in Bayer's patents. In combination with the Hall–Héroult residue (Fig. 1) that in turn led to the construction of new refineries
process for smelting alumina to metal, it remains the only viable throughout the world. In particular, increasingly large refineries were
process for the production of the metal, a situation that is highly built in the major laterite regions of first Australia and then South
unusual, if not unique, in the history of metallurgical processes. The America. The distribution and timing of refineries are shown in Fig. 3.
chemical and physical nature of bauxite residue is determined by the Apart from a number of refineries that we have been unable to locate
nature of the bauxite and the effect that the Bayer process has on it.
Hence it is relevant to consider the main aspects of a modern Bayer
plant that affect residue properties.
The half of the Bayer plant that affects the properties of the residue
produced includes a series of unit processes that start with bauxite and
finish with bauxite residue; this is often referred to as the “red side”. A
contemporary Bayer plant's red side generally includes the unit
processes of bauxite milling, pre-desilication, digestion, clarification,
and counter-current decantation (CCD) washing (thickener series). A
further thickening and/or filtration step prior to residue discharge
(usually to a bauxite residue disposal area or BRDA) follows these unit
processes. A schematic of these basic steps is shown in Fig. 2. Each unit
process influences the chemical composition of the residues, as well as
their physical and mineralogical attributes and the way they behave
subsequently in the BRDA.
Bauxite residue management begins at the point of separation of the
green liquor from the solids remaining after digestion. This is usually
achieved in a thickener (also known as a settler) which separates
residues from saturated sodium aluminate (NaAl(OH)4) solutions. After
the green liquor has been separated, the residue underflow is transferred
to the counter-current decantation (CCD) washer trains where the
residues are washed in several stages in raked thickeners (settler-
washers) to recover NaOH and NaAl(OH)4 from the remaining entrained
liquor and from the solids that slowly release these constituents into
solution. After washing in the CCD train, the residue is usually filtered or
treated in a final thickener to increase the solids content prior to being
transported to the BRDA. Filtration is used in some plants currently, but
the majority of plants use thickeners for this purpose. The thickener may
typically be either a deep cone thickener (Alcan) or a superthickener
(Alcoa). The most important influences of each process in relation to
bauxite residue are summarized in Tables 1 and 2.

3. Storage practices, engineering and science

3.1. Development of disposal methods
Prior to the 1970s, there were only two disposal methods in
general use, marine discharge and lagooning. Marine discharge is the
Fig. 2. Schematic of a general Bayer process “red side”, highlighting those processes
affecting the disposal and storage of bauxite residues. The right arrows for the counter-
current wash train (e.g. 1–5) indicate the flow of wash water opposite to the flow of
residue. The final residue preparation stage may be a deep cone type thickener (5),
superthickener (e.g. 6) or a filter. Some refineries practice a variety of pre-disposal
neutralization amendments.
36 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
Table 1
Bayer plant unit processes affecting bauxite residue characteristics relevant to disposal and storage.
Plant process
Bauxite milling
Pre-desilication
Digestion
Settling
Washing
Final thickening or filtration
in China, we believe this distribution map accurately accounts for the
majority of global alumina production. This rapid expansion coincided
with increasing environmental awareness. Regulation in the devel-
oped world from the 1970s onwards led to the development of new
approaches to residue management.
Table 4 shows residue disposal methods used for 17 refineries for
which information could be found for each of the years nominated.
These 17 refineries accounted for 44% of the 76 million tonnes of
alumina produced globally in 2007 (U.S. Geologic Survey, 2008).
Noteworthy is the consistent trend away from marine disposal to
land-based disposal, and from wet to “dry” disposal methods. In 1965,
one third of the refineries considered were disposing of residue by
marine dumping, and the other two thirds were impounding it in
lagoons. In the 1970s research into alternatives led to the develop-
ment of “dry” stacking methods. The subsequent increase in the
number of plants using “dry” stacking, and the conversion of a number
of refineries from wet to dry disposal, reflects its emergence as the
favoured option for residue disposal (Banerjee, 2003; Cooling, 1989)
and certainly the preferred practice in the construction of new
refineries. By 1985 43% of the refineries were using “dry” stacking,
growing to 70% by 2007. As noted in Table 3 it has the particular
advantages of reducing the land area required for residue storage,
minimizing the potential for liquor release to the surrounding
environment and also maximizing the recovery of liquor (and
entrained value) to the refinery. One serious drawback however is
the increased risk of fugitive dust requiring mitigation methods.
3.2. Marine disposal
The 1981 UNEP/UNIDO workshop concluded that “disposal
[of bauxite residue] into rivers has been strongly discouraged and
Table 2
Bayer digest variables.
Hudson (1987).
Main Al mineral Gibbsite
Al(OH)3
Temperature (°C) 104–145
Pressure (atm) 1.0–3.0
NaOH (M) 8.9–3.6
Effects relevant to disposal and storage
• Sets the effective particle size distribution and specific surface area of bauxite particles for digestion
• Particle size and surface area are key factors in determining physical properties
(e.g. Settling rates, mud rheology) and chemical properties (e.g. Adsorption of flocculants, organics and
metal ions, dissolution rates of minerals and precipitates)
• Introduces sodium alumino-silicates (desilication products or DSP) to the residue
• High temperature, high pressure environment which alters the elemental and mineralogical make-up
of the original bauxite particles into bauxite residues
• Nature of the bauxite dictates temperature, pressure and NaOH concentrations (see Table 2)
• Introduces large amounts NaOH to the solids increasing their ph, alkali and Na+ content
• Al is solubilized and removed from the solid phase
• Mineral transformation reactions occur: less stable minerals dissolve and re-precipitate; other minerals
undergo solid-state dehydration reactions which convert them to more stable mineral phases
• Conducted in high volume raked settlers
• Slurry is mixed with chemical additives to promote settling and to clarify the overflow liquor
• Bauxite residue is separated from the green liquor
• Conducted in high volume raked washers
• Flocculants added to achieve required underflow densities
• Recovery of NaOH and NaAl(OH)4 in the remaining liquor of the residues to be returned to the main
Bayer process liquor
• Underflow of the last washer is optimized according to the disposal method
• Increases solids density to meet storage or disposal requirements
• Further flocculant or filtration aid added
• Additional washing
marine disposal regarded as a last resort where suitable land disposal
is not available” (United Nations Industrial Development Organisation,
1985). This appears to reflect the opinion of the majority of companies
involved in alumina refining. There has been a shift away from direct
marine or river disposal as noted in Table 4. To our knowledge no new
refineries were built after 1970 that employ marine disposal. Presently
only 2–3% of global alumina production results in marine disposal of
residue.
Residue from the Gramercy plant in Louisiana was disposed into
the Mississippi River until 1974, at which time a transition was made to
lagooning. The operating company (Kaiser) voluntarily removed
residue from the river and relocated it to land-based lagoons. Effort
was also directed towards dewatering and treating the residue to enable
the creation of useful products in order to limit the requirements for
additional area for residue disposal (Kirkpatrick, 1996).
Plants in Japan are restricted in relation to land area available for
disposal of residues, and so have historically marine discharged.
Responses to find beneficial uses for residue (e.g. as a supplement to
cement manufacture) have proved insufficient. Other approaches to
minimize residue have been to maximize the imported bauxite grade
and to directly import smelter feed “hydrate” (International Maritime
Organization, 2005). Japan made a commitment in 2005 to the
International Maritime Organization that disposal of bauxite residue
to the sea would be discontinued by 2015. The country reported that
in the previous 5 years residue had been disposed to the sea at two
locations at a total rate of 1.0 Mtpa. Environmental impact assess-
ments at both sites concluded no impact on water quality and marine
organisms in the water column in the region of sedimentation but some
differences in the nature of the seabed between the dumping sites and
control sites, i.e. only limited impact was reportedly observed. It was
intended that further monitoring campaigns would be carried out every
2 to 3 years (International Maritime Organization, 2005).
The plants at Gardanne in France and Viotia in Greece that still use
marine dumping are actively pursuing alternatives (Martinet-Catalot
et al., 2002). Dauvin (2010) summarizes the most recent impact
assessments for the Cassidaigne canyon. It is noteworthy that as of
Boehmite 2010 only 0.18 Mt (dry weight) will be discharged at Gardanne and
γ-AlOOH they (along with Japan) will cease all marine discharge by 2015. A
200–232 study of the discharge from the Viotia plant into the Gulf of Corinth
6.0 showed that an extensive deposit has been formed close to the point
5.0–3.6
of discharge from a pipeline at a depth of 100 m. The residue also
 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
Table 3
Summary of the advantages and disadvantages of the four residue disposal methods.
Advantages
Marine disposal
No land required for storage
No closure and rehabilitation of storage areas
No impacts associated with land-based storage (dusting, contamination
of surface and ground waters, and leaching of toxic metals)
Lower capital and operating costs than for land-based disposal methods
No additional thickening or filtration of the slurry prior to disposal
Does not return impurities to the Bayer plant liquor
Lagooning (low wt% solids)
Lowest capital cost land-based disposal method
No additional thickening or filtration of the slurry prior to disposal
Dust potential minimized by maintaining a supernatant liquor layer
Does not return impurities to the Bayer plant liquor
“Dry” stacking (48–55 wt.% solids)
Land area required for storage is minimized
Structures required for secure containment are minimized
Soda and alumina values in the liquor are returned to the Bayer plant
Potential for leakage to groundwater is minimized
Risk of surface water contamination is lowered by smaller area of open
contaminated water and returning runoff to the Bayer plant
Rapid de-liquoring assists area management, including rehabilitation
Hazards associated with open caustic lakes are minimized
Recovery of solids for alternative uses is facilitated
Dry cake disposal (N 65 wt.% solids)
Land area required for storage is minimized
Collapse risk of a raised mound or impoundment is minimized
Soda and alumina values in the liquor are returned to the Bayer plant
which reduces the need for washing stages
Low leakage risk to groundwater due to the low pore volume
Environmental and safety hazards associated with the presence of open
caustic lakes are avoided
Residue can be recovered by standard earthmoving equipment
Rehabilitation and closure are facilitated by the ability to landscape the
deposit and by its low alkali content
extends over the sloping shelf of the sea floor and into an abyssal plain to
a depth of 860 m at distances of up to 17 km from the point of discharge.
The main mechanism of transport of the residue from the shelf to the
abyss was found to be by gravitational flow triggered by seismic events,
which are common in the region (Varnavas et al., 1986).
3.3. Lagooning
The residue slurry from the washing circuit is pumped into land-
based impoundments. In the absence of suitable natural topography,
ponds may exist as fully fabricated structures, generally excavated
into the existing land. In either case, best practice is to line the ponds
with sealants to minimize liquor leakage to the underlying ground
and ground water. The linings vary in relation to both the materials
used and the complexity of the construction. The simplest is a single
layer of compacted clay which separates the residue from the original
soil or rock of the storage area, but the integrity of such layers cannot
generally be guaranteed (Thomas et al., 2002). Additional security can
be achieved by the use of multiple layers featuring impermeable
plastic or geo-membrane materials to form a seal between the residue
and the supporting clay or other layer beneath. Minimizing the
hydrostatic pressure by removing liquor by decanting and in some
cases by also under-draining the deposit further contributes to the
reliability of the seal (Cooling, 1989). Storage problems can be further
mitigated by neutralizing the slurry prior to discharge, for example by
37
Disadvantages
Covering of sea-bed and destruction of associated ecosystem
Potential for release of toxic metals to marine environment
Increased turbidity of seawater due to dispersion of original residue and the
formation of colloidal magnesium and aluminium compounds
Unknown effects on ecosystems and food chains
Increasing community/regulatory pressure to discontinue the practice
Loss of soda and alumina values with entrained liquor
Provision of substantial areas of land
Long term planning and funds for closure and rehabilitation
Loss of soda and alumina values with entrained liquor
If not neutralized:
Poorly compacted highly alkaline residue and highly alkaline lake
Range of hazards (risk of contact of humans and wildlife with caustic liquor and
residue, and contamination of surface and ground waters)
Costly engineering to prevent catastrophic failure of impoundments
Difficult to close and rehabilitate because of large amounts of caustic liquor —
possibility of an indefinite legacy
Sufficient areas of land for storage
Planning and funds allocation for long-term closure
Additional stage of thickening or filtration prior to discharge.
Liquor impurities are returned to the Bayer plant (process impacts)
“Dry” stack surfaces are subject to fugitive dust lift-off and mitigation processes
may be required (e.g. sprinklers)
Difficult to achieve in areas of high rainfall and low net evaporation
Significant compaction density hinders the establishment of vegetation
Provision of sufficient areas of land for storage
Long term planning and funds for closure and rehabilitation
Installation and operation of a filtration plant capable of handling entire
residue production
Liquor impurities are returned to the Bayer plant (process impacts)
Surfaces are subject to dust lift-off so that mitigation processes may be required
mixing with seawater or by the addition of mineral acids (e.g.
sulphuric acid).
Lagooning is the simplest land-based disposal method, but due to the
low solids content is also the most dependent on good engineering
practice for the residue containment. The increased risk with low solids
containment is tragically demonstrated by the impoundment wall
collapse at the Ajka Timföldgyár alumina refinery in October 2010
(Enserink, 2010). Effective low solids in an impoundment area can also
arise from high rainfall events.
3.4. “Dry” stacking
“Dry” stacking is a significantly different disposal concept and could
more generically be termed thickened tailings disposal (TTD). Unlike
lagooning residue at a low solids level, the residue slurry from the washing
circuit is thickened to a paste (in the initial range of approximately 48 to
55% solids) prior to discharge. The paste is thixotropic, and so is amenable
to pumping and pipeline transport. Upon discharge from the pipe it
will flow down a slope without segregating or settling to form layers of
uniform thickness at an angle of repose in a range of 2° to 6° (in non-
freezing conditions). The residue deposit is built into a stack by
discharging the paste progressively in thin layers that are allowed to
dewater and air-dry before being overlain with the next layer. Upon
standing, the paste consolidates (with liquor decant) to a density of 62 to
65% solids, with a final dry density around 70% and an accompanying
38 G. Power et al. / Hydrometallurgy 108 (2011) 33–45

Fig. 3. World map showing the distribution of alumina refineries based on establishment date (before or after 1970), closed or unknown.

increase in shear strength. Shear strengths of 20 kPa or more may be
reached (Nikraz et al., 2007). The consolidation occurs as the solids settle
and liquor is removed by a combination of decantation and surface
evaporation. Modern designs also include under-draining to facilitate the
consolidation process. The process is designed such that the dried paste
becomes substantially self-supporting so that it can be safely stacked to
considerable heights within containment bunds, minimizing the physical
footprint of the disposal area (Cooling, 1989). As with lagooning the
hazards associated with alkalinity may be reduced by neutralization but
any changes to paste rheology need to be considered.
Methods for disposing of residue with prior de-liquoring were
pioneered in Germany with a view to minimizing the land required
for disposal and maximizing the return of soda and alumina to the
refinery. The term “dry stacking” appears to have been first used to
describe the process developed at the Ludwigshafen plant in the
1970s (Anon, 1982; Pohland et al., 1981; Pohland and Tielens, 1983,
1986). Residue slurry from the washing stage was filtered on drum
filters that discharged a cake at about 55% solids by weight. The cake
was fluidized by mechanical agitation for pumping to the drying area
where it formed a mound with a shallow angle of repose (approx-
imately 5°). The deposition schedule was managed to optimize
surface drying while minimizing dusting potential. It was found that:
• The residue consolidates to about 62–67% solids, enabling it to be
traversed by machinery minimizing the requirements of the
containment dykes
• Degree of fluid decant was minimal, and rainwater could be
collected and either discharged to the environment or returned to
the Bayer plant according to purity
• Material compacts on standing to become highly impermeable
(permeability in the order of 10−9 cm/s), removing the necessity to
line the disposal area to prevent seepage of impurities into the
underlying soil and ground water
A similar system was developed and implemented by Alcan at the
Arvida plant in Canada (Paradis, 1992, 1993; Robinsky, 1982). In this
case special thickeners were developed to produce a residue of
sufficient solids density to behave as a non-segregating slurry. This led
to the development of the Alcan Deep Cone Thickener, a new
technology for producing densities of over 50% solids suitable for

Table 4
Storage practices at 17 refineries (representing 44% of global alumina production in 2007) for which information is available over the period 1965–2007.

Startup date Refinery 1965 1975 1985 2007

1959 Kirkvine Lagoon Lagoon Lagoon Lagoon

1963 Kwinana Lagoon Lagoon “Dry” stack “Dry” stack
1965 Aluminium de Grece Sea disposal Sea disposal Sea disposal Sea disposal
1967 Queensland Alumina Ltd Lagoon Lagoon Lagoon
1972 Alcoa Alumino S.A. Lagoon Lagoon “Dry” stack
1972 Gove Alumina Lagoon Lagoon “Dry” stack
1972 Pinjarra Lagoon “Dry” stack “Dry” stack
1973 VAW Stade Unknown “Dry” stack “Dry” stack
1973 Eurallumina Lagoon Lagoon Lagoon
1980 San Ciprian “Dry” stack “Dry” stack
1983 Aughinish “Dry” stack “Dry” stack
1983 CVG Bauxilum Lagoon Lagoon
1984 Worlsey Alumina “Dry” stack “Dry” stack
1984 Wagerup Lagoon “Dry” stack
1987 Dhamanjodi “Dry” stack
1995 Alunorte Barcarena “Dry” stack
2005 Yarwun “Dry” stack
 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
the production of thickened tailings without the need for filtration
(Peloquin and Simard, 2002). In 1996 Alcan entered into a license
agreement with EIMCO for the further development and marketing of
Deep Cone thickeners. According to EIMCO (now FLSmidth Minerals)
there are over 50 Alcan Deep Cone thickeners now operating in
alumina plants, and the technology has been deployed to other
industries including copper and lead/zinc processing (Emmett and
Klepper, 1991; Emmett et al., 1992). Thickener performance issues are
reviewed by Farrow et al. (2000).
The National Aluminium Company (NALCO) plant at Orissa, India,
applied the Alcan technology (Banerjee, 2003; Das et al., 2003) to
replace the original wet disposal method and they simply refer to it as
TTD. The system was installed as part of a major plant expansion from
0.8 to 1.575 Mtpa. The existing wet disposal method would not have
been capable of supporting the projected residue production over the
ensuing 20 plus years, because of limitations on the availability of
suitable land area and environmental concerns associated with wet
disposal. The alternative of dry cake disposal was also considered, but
was rejected, primarily on grounds of capital and operating costs.
Concerns related to the safety and environmental aspects of trucking
the material in hilly terrain were also cited (Banerjee, 2003). In
addition to the “dry” stacking advantages outlined in Table 3, the TTD
system was seen to have additional advantages in relation to wet
storage of reduced earthquake and erosion risks and lower energy
consumption and pipeline requirements.
The rheological properties of bauxite residues vary widely
between plants and successful “dry” stacking requires an understand-
ing of the rheology (Farrow et al., 2000; Sofra and Boger, 2002) as
slurries are thixotropic and their flowability increases with the
amount and manner of mixing energy applied (Pashias and Boger,
1996). For example, slurry that has been allowed to settle to 50%
solids will be firm and seemingly un-pumpable, but if sufficient
mixing energy is introduced, the viscosity is decreased as the pore
liquids create a network enabling the slurry to be pumped. Without
sustained energy input it will slowly revert back to a firm condition.
These flow behaviour changes occur without the solids density of the
material changing. The key rheological parameters for slurry thickening
Fig. 4. Schematic of Alcoa dry-stacking method for bauxite residue disposal.
Redrawn from Alcoa (2005a).
39
and transport design, and for spreading behaviour and slope formation
prediction are yield stress and viscosity as a function of solids content
and the shear and compression history of the material (Green and Boger,
1997; Sofra and Boger, 2002). The particle size distribution is also
important (Doucet, 1999) as is the nature and rates of the chemical
additives (in particular flocculants and flowability aids).
These principles have also been successfully applied at the MOTIM
plant in Hungary, where the residue is filtered on vacuum drum filters
to 50% solids, fluidized by high-intensity stirring, and then pumped to
the residue storage area where it is stacked in layers to dry. After
drying times between 80 days (summer) and 160 days (winter), the
solids content rises to around 65%, at which point the material can be
mechanically spread using conventional earth-moving machines
(Solymar et al., 2002).
Alcoa determined that underflow densities in the region of 50 wt%
solids were sufficient as the starting point for a “dry” stacking system
provided with underdrainage for efficient de-liquoring (Cooling, 1989)
of the deposited residue and return of the recovered liquor to the Bayer
plant. The required solids density was achieved in a specially designed,
large diameter (90 m) thickener (a “superthickener”) and associated
rake system developed in collaboration with EIMCO (Marunczyn and
Laros, 1992, 1993). As the raking loads would exceed the capability of
any centre-drive design, a peripheral traction drive was employed
(Emmett and Klepper, 1991). Between 1985 and 1992, Alcoa imple-
mented at its Western Australian refineries a stacking system in which
residue is deposited into rectangular cells on a rotational basis to assist
drying and reduce the land area. It was found that final densities
of ~ 70 wt.% solids are achievable, although the time required was not
reported (Cooling and Glenister, 1992). A schematic of this system is
shown in Fig. 4. At 70 wt.% the shear strength of the stack is N 30 kPa (i.e.
high structural integrity) and not only is the storage volume
requirement reported to be about 60% of that required for lagooning,
but greater impoundment heights are more easily constructed. Further
under-drainage may be introduced progressively as the stack is built.
Some mechanical ploughing of the surface is required to optimize drying
rates, and water sprinklers are used on an as needs basis to mitigate
fugitive dust lift-off. Fig. 5 shows a satellite image of the Pinjarra residue
40 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
Fig. 5. Google Earth™ image of Pinjarra refinery and residue area in 2006. Captions inferred from Pinjarra long term residue management plan (Alcoa, 2005b). GOOGLE is a
trademark of Google Inc.
area (the labeling of the areas is according to the Pinjarra long term
residue plan (Alcoa, 2005b). This residue management has since been
deployed to other operations including those in Suriname, Spain, and Pt
Comfort Texas (Alcoa, 2001). It should be noted that the storage volume
advantage over lagooning may be operationally relevant for a time, but
the final compaction of the solids in a lagooned impoundment would be
similar to dry disposal. Issues such as yield stress values and
permeabilities at a given weight% solids must also be considered in
the context of residue particle size distributions, shape and mineralogy.
For example, Jamaican residues settle to considerably lower% solids than
other residues (Roach et al., 2001) but exhibit similar viscosities, leading
to the conclusion that comparisons of residue behaviour should be made
on a volume/volume basis and not% solids.
3.5. Dry cake disposal
Dry cake disposal refers to the practice of mechanically removing
as much water as possible from the residue to produce a dry cake with
a solid's content of N 65 wt% prior to disposal. The special case of dry
cake disposal is not always specified as such in available information
and “dry” stacking tends to be used to encompass both high wt% solids
methods. The dry cake is not pumpable, so is generally moved to the
disposal area by conveyors or trucks. There is no significant further
de-liquoring once the residue has been delivered to the storage area
and these factors distinguish it from “dry” stacking. Similarly to the
other methods, any hazards associated with entrained alkalinity can
be further reduced by washing or neutralizing the cake on the filters.
Filtration on vacuum drum filters followed by dry cake disposal has
been applied successfully in practice, for example at the Hindalco
plant at Renukoot (Shah and Gararia, 1995).
It is not possible to achieve a dry cake by means of thickening alone,
and so a filtration stage is required. Vacuum filtration is not generally
satisfactory for this purpose, as it is limited in the available pressure drop
across the filter cake to b 0.75 bar (Oeberg and Steinlechner, 1996). This
is insufficient to overcome the capillary resistance inside the pores of the
residue to fully de-liquor the cake. By using pressure filtration it is
possible to achieve differential pressures in the order of 6 bar which is
sufficient to fully de-liquor. The non-thixotropic nature of this cake is
fundamental to the success of the process. It means that the cake can be
readily discharged from the filter by air blow-back or mechanical means,
and can then be transported to the disposal area by truck or conveyor
where it can be stacked with a minimum of additional treatment in
relatively simple containment facilities (Kainuma et al., 1979; Oeberg
and Steinlechner, 1996; Steinlechner et al., 1996).
Recent trials of BOKELA hyperbaric filtration technology have been
successfully demonstrated using a Bokela Hi-Bar® at the pilot plant
scale at the Aluminiumoxid Stade (Germany) plant (Bott et al., 2002).
This trial demonstrates the possibility of a marked improvement in the
removal of fluids and salts from bauxite residue in which solids contents
of N 75% can be achieved with the application of steam in the filter. This
filtration method produces soda contents as low as 3 g/kg as compared
to 6 to 12 g/kg by vacuum filtration. The resulting cake is described as
“extremely dry and well washed … with a crumbly, sandy-like and non-
sticky consistency and a low soda content” (Bott et al., 2002). Similar
results were also achieved by Maschinenfabrik Andritz at the CVG plant
in Venezuela (Oeberg and Steinlechner, 1996).
Producing a residue with these characteristics greatly simplifies
handling and storage requirements, reduces the potential for environ-
mental impact, and broadens the options for rehabilitation and/or reuse
of the material. A number of these advantages were previously
demonstrated by Nippon Light Metals at their Tomakomai works
(Kainuma et al., 1979). Given that the technology has been demon-
strated at a plant scale, the challenge is to develop it as an economically
attractive alternative to current methods, and then to deploy it to
existing and future plants.
3.6. Bauxite residue amendment
Except for dry cake disposal bauxite residue is discharged as a slurry
or paste whose high alkalinity (pH N 11) and high sodium content
 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
favours particle dispersion. In addition, the solids in the slurry contain a
high proportion of fine, silt- to clay-sized particles. The combination of
these chemical and physical factors creates significant difficulties in the
handling, storage and remediation or utilization of bauxite residue. For
long-term storage or utilization of the residue, it may be necessary to
release liquor to the surrounding environment. This will generally
require it to be neutralized in some way and diluted prior to discharge.
The pore fluids remaining in the stack will generally also need to be
diluted and/or neutralized. Solid alkalinity can also have a profound
effect on attempts to neutralize the pore water and is a major factor to be
considered in any evaluation of possible future storage or utilization
scenarios. The need to amend bauxite residue grew with the rapid
growth of industry output and increasing levels of environmental
awareness and regulation.
Although significant general progress has been made with the
advent of “dry” stacking, it is reasonable to conclude that pressure
filtration, washing and at least partial pH neutralization would remain
essential to any long term disposal solution. However, pressure filtration
in particular is costly and its implementation without regulatory
incentive is unlikely. The key to successful amendment is the complex
chemistry, this is treated in detail in part three of this review series
(Gräfe et al., 2011).
3.6.1. Alkalinity of bauxite residue
The object of the digestion step of the Bayer process is to dissolve
aluminium-containing minerals while minimizing the dissolution of
other mineral phases. This is achieved in a strongly alkaline solution at
temperatures above 100 °C (mostly in the range 145 to 250 °C), so
that minerals such as gibbsite (Al(OH)3) and boehmite (γ-AlO(OH))
are dissolved to produce [Al(OH)4]− (aluminate) ions in solution,
according to the following reactions:
− −
AlðOHÞ3ðsÞ þ OH ⇔½AlðOHÞ4 ðaqÞ
− −
γ  AlOðOHÞðsÞ þ OH þ H2 O⇔½AlðOHÞ4 ðaqÞ
The bauxite residue is then separated from the main liquor stream
and washed to recover soda and alumina. The resulting residue
contains pore water that is considerably more dilute (by a factor of at
least 10) than the main Bayer plant liquor, but is nevertheless highly
alkaline. If this residual solution is then neutralized, aluminium
hydroxides will re-precipitate. The nature of the precipitates depends
on the method and conditions of precipitation, but will generally
include Al(OH)3 and/or AlOOH.
The chemistry of the residue slurry is thus determined by the
interactions between the bauxite and the plant liquor during digestion,
followed by the changes that occur after the bulk solids are separated
from the digest liquor and progressively washed (usually CCD) to
remove sodium hydroxide, aluminate and carbonate. During the
washing process various chemicals are added, most notably flocculants
to settle the residue and clarify the solution for return to the Bayer liquor
circuit, and lime to remove carbonate ions from the liquor by
precipitation of CaCO3 and replacement of carbonate by hydroxide
ions in solution, in a process called “causticization”, nominally:
2− −
CaO þ CO3 þ H2 O→CaCO3ðsÞ þ 2OH
This produces pH buffers in the form of calcium carbonate, tricalcium
aluminate (TCA, stoichiometric formula Ca3Al2(OH)12) and calcium-
aluminate carbonate (hydrocalumite, stoichiometric formula Ca4Al2
(OH)12.CO3.6H2O).
Apart from the intended solubilization of aluminium species, there
are a number of other reactions that occur during and prior to digestion.
One of the most important is the solubilization of phyllosilicate minerals
(clays), e.g. kaolinite Al4Si4O10(OH)8. The dissolution of these minerals
results in aluminate and silicate ions in solution. The digester discharge
41
liquor, which is the solution produced by the digestion process, also
contains Na+ ions in high concentration. As a result, the liquor becomes
unstable with respect to a range of sodium alumino-silicates, in
particular sodalite3 and/or cancrinite.4 These sodium alumino-silicate
solids that form during pre-desilication and pre-digestion are collec-
tively referred to as “desilication products” or DSPs because they remove
silica, sodium and hydroxide ions from solution by incorporation. DSP is
a form of solid alkalinity, stable while the solution is alkaline, but
decomposing in neutral to acid solutions, releasing sodium, hydroxide,
aluminate and silicate ions into solution. In this way the DSPs act as
significant solid alkaline pH buffers.
A number of side reactions can occur between the added lime and
the aluminate ions in the Bayer solution. The exact reactions and the
nature of the products depend on conditions, but the general
reactions may be illustrated by the formation of hydrated calcium
aluminate and aluminate carbonate as follows (Rosenberg et al.,
2004):
− −
3CaðOHÞ2 þ 2½AlðOHÞ4  þ nH2 O→Ca3 Al2 ðOHÞ12 :nH2 OðsÞ þ 4OH
− 2− −
4CaðOHÞ2 þ 2½AlðOHÞ4  þ CO3 þ nH2 O→½Ca2 AlðOHÞ6 2 :CO3 :nH2 OðsÞ þ 4OH
Alkaline solids can also be formed with other anions such as
phosphate, zincate and titanate, and with other cations such as
magnesium and potassium.
Both the quantity and forms of alkalinity must be taken into
account in any process for neutralizing the residue. For example, the
amount of carbonate in solution determines the buffering capacity of
the solution above pH 10. In the region of neutral pH additional
buffering is provided by (solid) aluminium hydroxides, and if
significant carbonate is present, also by sodium alumino-carbonates,
in particular dawsonite (NaAl(OH)2CO3).
3.6.2. Seawater remediation
Apart from direct marine disposal, such as has been practiced at
Gardanne since the very early days of the industry (Martinet-Catalot
et al., 2002), the first example of onshore remediation of residue by
mixing with seawater appears to be at the Queensland Alumina refinery.
In this case seawater was used as a transport fluid for pumping it to
disposal lagoons in order to conserve fresh water (Hanahan, 2004).
Remediation by neutralization was a consequence, but not the primary
aim of seawater use.
By adding seawater, hydroxide, carbonate and aluminate ions are
removed from solution by reaction with Mg2+ and Ca2+ ions to form
alkaline solids, in particular hydrotalcite (Mg6Al2(CO3)(OH)16·4(H2O))
and calcite (CaCO3). This buffers the solution in the range of pH 8 to 9.
It has been shown that the phosphate adsorption capacity of the
solids is substantially increased by seawater neutralization (Hanahan,
2004), and that the solids have a high trapping capacity for trace
metals (McConchie et al., 2002). These features are useful in relation
to revegetation of bauxite residue areas, and for creating various re-
use products (Tillotson, 2006).
Seawater is also used to neutralize the decant liquor from ponding
operations prior to discharge. Neutralization by simply mixing the
decant liquor with seawater results in the formation of white colloidal
precipitates which have the potential to produce contamination
downstream of the discharge point (Baseden and Grey, 1976). At the
Gove refinery, hydrotalcite, calcium carbonate and calcium oxalate
were identified as the main components of such precipitates along
with trace amounts of other salts (Anderson et al., 2008).
Further research led Alcan Gove to develop a seawater treatment
method for decant water to meet stringent standards of purity for
3
Na6[Al6Si6O24]·[2NaOH,Na2SO4]·nH2O.
4
Na6[Al6Si6O24]·2[CaCO3]·nH2O.
42 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
discharge to the environment (Haggard and Smith, 2002). The purity
parameters of particular interest are pH, turbidity and trace metals. In
addition to meeting the designated water quality criteria, ecological
toxicity testing was done to provide additional confirmation that the
treated water was safe for discharge to the marine environment. It was
found that a two-stage treatment was required in order to meet the
design performance requirements, particularly in relation to vanadium
levels. The first stage of the process is the mixing of the decant water
with a six-fold excess of heated seawater (waste cooling water from the
plant evaporators) to form the hydroxide precipitates. The resulting
suspension is then mixed with residue slurry and treated with
flocculants in a thickener to produce a clarified overflow stream for
discharge. Continuous flow (bench scale) trials confirmed that the
required performance parameters can be met with this design, which
has been proposed for implementation at Gove (Anderson et al., 2008).
Successful implementation of this technology would be a significant
milestone in the development of seawater neutralization technology. It
would be the first use of a Deep Cone thickener as a mixer to produce
overflow water suitable for direct discharge and would eliminate the
need of a labyrinthine discharge channel required to provide residence
time necessary for formation and sedimentation of precipitates.
3.6.3. Mineral acid remediation
There are few examples in the literature of neutralization of bauxite
residue by mineral acids and whilst addressed in general terms by
McConchie et al. (2002), no examples are given. The authors point out
that large quantities of acid would need to be available at low cost,
opining that this is unlikely to be the case for alumina refineries
generally. It is also noted that residue neutralized by mineral acid
contains no residual (solid) alkalinity, and so would not be useful as a
starting material for the range of applications envisaged by those
authors. In addition it does not improve the physical properties of the
material, both of which occur if either seawater or carbon dioxide is used
for neutralization.
It has been reported that sulphuric acid is used as a supplementary
neutralizing agent at the Yarwun refinery (Queensland, Australia) due
to (pipeline) limitations in seawater supply (Sturt, 2008). The
performance of sulphuric acid was assessed in terms of its ability to
reduce the level of aluminate in the discharge liquor. It was found that
the mineral acid was significantly less effective in removing aluminate
from solution because it relies on the precipitation of aluminium
hydroxide, whereas if seawater is used the solid phase formed is
hydrotalcite which is less soluble at the target pH of 8.5.
No references were found in the open literature concerning the
neutralization of bauxite residue decant waters with mineral acids in
a specific refinery context. Such a practice would be expected for some
refineries in order to meet discharge license requirements. This would
result in the formation of colloidal and/or gelatinous precipitates
(primarily aluminium hydroxides and hydroxy-carbonates) requiring
a clarification process prior to discharge.
3.6.4. Carbon dioxide remediation
A process for reacting bauxite residue with gaseous carbon dioxide
was piloted by Alcan for the Saramenha Ouro Preto refinery in Brazil
in 1983 (Versiani, 1983). The concept has since been developed by
Alcoa as a means of reducing the pH of the slurry prior to “dry”
stacking (Cooling et al., 2002). Extensive laboratory and pilot-scale
testing was carried out by Alcoa between 1991 and 1996. This was
followed by small-scale field trials in which several mixing devices
were tested. Carbonated residue was deposited in layers so that its
longer term behaviour could be studied in a “dry” stacking operation.
The optimum rate of CO2 addition was found to be 25 kg CO2 per m3 of
residue slurry, at a slurry density of 48% solids. It was demonstrated
that a pH of 9 could be achieved in the carbonated residue. The pH of
the leachate collected from the under-drainage system remained
steady at around 10.5 over an extended period, while the pH of the
leachate from a non-carbonated drying bed was consistently greater
than 13. On the basis of these trials, full scale residue carbonation
capability was implemented at the Kwinana refinery in 2000 (Cooling
et al., 2002).
Prior to neutralization, residue slurries are highly alkaline. The pH
of the slurry is generally in the region of 13, equivalent to an OH−
concentration of 0.1 M. Introducing CO2 to the solution causes rapid
neutralization according to the following reaction:
− −
CO2ðgÞ þ OH →HCO3 ðaqÞ
This reaction causes the pH to drop rapidly until buffering by the
carbonate/bicarbonate equilibrium becomes apparent below a pH of
10. At that pH solid hydroxides begin to form, creating additional
buffering as they equilibrate with the ions in solution.
The Alcoa trials demonstrated that it was possible to achieve a pH
as low as 8.5 by reacting residue slurry with CO2 under pressure
(Cooling et al., 2002). However, after the CO2 overpressure was
removed, the pH would slowly rise until a final pH of about 10.5 was
reached. This rise was explained by those authors and by Smith et al.
(2003) as being due to the dissolution of alkaline solid phases that
become soluble in this pH range, for example TCA. As noted, TCA is
present in bauxite residue as a result of the use of lime in the Bayer
process for control of carbonate levels in the liquor (Rosenberg et al.,
2004) and as an aid to settling and filtration (Whittington, 1996).
Dissolution of TCA results in the release of OH− ions to the solution,
thus raising the pH. This is accompanied by the formation of new solid
phases, including calcium carbonate (calcite), sodium aluminium
hydroxyl-carbonate (dawsonite) and aluminum hydroxide (gibbsite),
possibly according to the following equations:
− þ
Ca3 Al2 ðOHÞ12 þ 3HCO3 ðaqÞ þ 4Na →3CaCO3 þ 2AlðOHÞ3 þ 3H2 O
þ −
þ4Na þ 3OH
− þ
2Ca3 Al2 ðOHÞ12 þ 10HCO3 ðaqÞ þ 4Na →6CaCO3 þ 4NaAlðOHÞ2 CO3
−
þ10H2 O þ 6OH
Due to the buffering effects of these reactions, the pH can be expected
to stabilize in the region of 10.5. These observations are consistent with
recent work by Khaitan et al. (2009a), who also observed that the
amount of TCA present is a major factor in determining the carbon
sequestration capacity of a bauxite residue (Khaitan et al., 2009b).
Alcoa found that carbonation of residue affects the physical prop-
erties of the material as well as its chemical composition. Carbonated
residue dries more rapidly than uncarbonated residue, possibly because
of the elimination of surface crusting and improved cracking behaviour
that provides more effective surface area for evaporation. It was also
found that the mechanical strength of the residue was enhanced by
carbonation. The combination of these effects results in a significant
reduction in the drying time required to reach a target minimum
strength to ensure long-term stability, which in turn reduces the
required cycle time for drying and improves the utilization of the
residue drying area. Some of the perceived benefits of carbonation of
residue have been summarized (Cooling et al., 2002) as:
• Reduces risk to containment seal material (clay or synthetic) and
therefore reduced risk of groundwater contamination
• Improves quality of drainage water
• Provides a sink for greenhouse gasses
• Reduces risk of future classification of the residue as a hazardous waste
• Facilitates development of productive uses for the residue in the future
CO2 supply is a key issue to be considered in relation to carbonation
of residue. The carbonation technology applied at Kwinana requires
concentrated CO2 as the raw material to be mixed with the residue
 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
slurry. The Kwinana alumina plant is located within an industrial
complex that includes an ammonia plant which produces pure CO2 as a
by-product, this is supplied to the residue area by a dedicated pipeline
(Cooling et al., 2002). Such examples of industrial synergy are rare, so
alternatives need to be considered if carbonation is to be applied more
generally. One alternative is to extract CO2 from flue gasses associated
with the alumina refinery. The level of CO2 in such flue gasses is
generally in the order of 10%, so a concentration process in which it is
separated from the other gasses (mainly nitrogen) is needed. The
current best technologies for capturing and concentrating CO2 from flue
gasses are based on amine scrubbing (Simmonds et al., 2003). This
requires the installation of a significant additional operation to an
already complex alumina plant, and carries the potential for amine
emissions. A promising amine-free alternative is based on carbonation
of residue liquor by contacting it with flue gasses in a high-efficiency
scrubber. The carbonated solution is then recirculated with residue
solids to carbonate the overall residue (Guilfoyle et al., 2005).
3.6.5. Sulphur dioxide remediation
The reaction of SO2 with residue has been developed as a means of
scrubbing SO2 from flue gasses. The technology utilizes the reaction of
SO2 with the sodium alumino-silicates in the residue to produce
sulphites that can be removed by oxidation by air (Yamada et al.,
1979a,b). The process was patented by the Sumitomo Aluminium
Smelting Co (Yamada et al., 1979b), and has been used at a number of
sites, including the Eurallumina plant (Sardinia, Italy; Fois et al.,
2007). The process is aimed at the removal of SO2 from gas streams
and the amount of residue neutralized is minor in relation to the total
of amount of residue produced. Reaction of bauxite residue with SO2 is
therefore an example of a beneficial use for bauxite residue, but it
does not appear to be a potential treatment for large quantities of
residue. Although not believed to be in use it is worth noting that a
process using SO2 to recover soda and alumina values form residue
has been patented (Cresswell et al., 1987).
4. Conclusions
Bauxite residue has been continuously produced since the
inception of the alumina/aluminium industry in the late nineteenth
century. We have estimated that the global inventory of bauxite
residue reached 1 billion tonnes in 1985, 93 years since the estab-
lishment of the first Bayer process plant. This inventory grew to 2 Bt
by 2000, a doubling time of only 15 years. The inventory was almost
2.7 Bt by 2007, growing at 120 million tonnes per annum. The
prospect of an ever decreasing doubling time, and an inventory of 4
Bt possibly before 2015, highlights the urgency of the need to develop
and implement improved means of storage and remediation, and to
pursue large-volume utilization options. Despite the size of the
industry and the residue problem, it is surprisingly difficult to
Table 5
Summary of the key knowledge gaps concerning management, disposal and storage practices for bauxite residue and areas of suggested research.
Knowledge gap
Economic technology to reduce the alkali and soda levels of bauxite residue.
Understanding the residue fundamentals of solid alkalinity and surface equilibria;
ion exchange, leaching and neutralization.
Detailed worldwide bauxite residue inventory knowledge (historical and current);
production, characteristics and disposal/storage practice.
Is dry disposal the best technical answer to residue disposal?
BRDA closure technology that improves on simple capping and re-vegetation.
Quantification and validation of carbon sequestration potential of
residue carbonation
Methods for direct carbonation of residue by stack gas carbon dioxide.
43
accurately gauge the volume and nature of current residue output,
let alone the very substantial legacy material in impoundment. Very
little useful information is in the public domain. We have established
an online database framework to try and address this problem — the
Bauxite, Residue and Disposal Database (BRaDD). BRaDD has been an
essential enabling tool for the collation and interpretation of
information required for this and the associated three reviews in
the series. With further programming refinements, and with data
input from the industry, BRaDD should be an invaluable tool in the
development of a global strategy for the future of bauxite residue
management.
Prior to 1980, most of the inventory of bauxite residue was held in
lagoon-type impoundments. This storage method has a number of
disadvantages, in particular the large areas of land required and the
potential for leakage of caustic liquors to the environment. Since 1980
the trend has been towards “dry” stacking in bunded areas that are
lined with a variety of natural and synthetic barrier materials.
Improved methods for thickening and washing of the residues prior
to storage, and recovery of decant water during storage, have been
developed to increase the recovery of valuable soda and alumina to
the Bayer process plants and to also minimize the potential for
leakage to the surrounding environment.
The current trend in residue storage practice is towards increasing
use of “dry” stacking as the preferred technology, and further research
to optimize this technology is appropriate. Hyperbaric steam filtration
is an emerging technology that produces a dry, granular residue of low
soda content. Such properties are beneficial to long term storage,
remediation, and utilization. Support for the development and
implementation of hyperbaric filtration as a potential breakthrough
technology is warranted.
A range of methods has been employed to neutralize both residue
and decant waters. The most established methods to date involve
either mixing with seawater to precipitate hydroxide, carbonate
and aluminate ions with magnesium and calcium, or with carbon
dioxide to produce calcium carbonate and calcium alumino-carbonates.
Neutralization with mineral acids is less successful due to the
influence of solid hydroxides in the residue and the deleterious effects
that this method of neutralization has on the physical properties of
the residue.
The most important barrier to remediation, utilization and long
term sustainability of bauxite residue management is its high
alkalinity and sodicity. The alkalinity of bauxite residue is a result of
complex solid-state and solution phase interactions. A better
understanding of these interactions is required to support progress
in the development of sustainable bauxite residue management and
re-use options, so ongoing research on the chemistry and technology
of residue neutralization is required. Based on this review of bauxite
management practices a set of knowledge gaps and research priorities
are summarized in Table 5.
Research project
Development of alternate processes, e.g. economically viable hyperbaric steam filtration.
Fundamental residue chemistry investigations of ion exchange, leaching and
neutralization.
Release of key residue information from industry practitioners into public domain
forums, e.g. BRaDD database.
Investigation of the relative long-term environmental impact risks of “dry” stacking,
dry cake disposal, seawater and carbonation methods.
Technology to reduce alkali and soda levels within existing BRDA locations.
Fully understanding long term CO2 equilibria as a function of residue composition and the
role of direct carbonation compared to natural absorption processes with time.
Development of methods for direct carbonation of residue by stack gas carbon dioxide.
44 G. Power et al. / Hydrometallurgy 108 (2011) 33–45
Acknowledgements
This project received funding from the Australian Government as
part of the Asia-Pacific Partnership on Clean Development and
Climate. The views expressed herein are not necessarily the views
of the Commonwealth, and the Commonwealth does not accept
responsibility for any information or advice contained herein. The
support of the CSIRO Light Metals National Research Flagship and the
Parker CRC for Integrated Hydrometallurgy Solutions (established and
supported under the Australian Government's Cooperative Research
Centres Program) is gratefully acknowledged. The authors gratefully
acknowledge Dave Pang for the development of the BRaDD interface.
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