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Article history: Sustainable development efforts aimed at substantial reduction of carbon dioxide emissions focused
Available online 2 January 2018 research activities in this field, among others, on a partial or full replacement of Portland cement by
environmental more friendly alternatives. Calcined gypsum can be considered as one of possible options
Keywords: in that respect. However, although the environmental impact is an important issue, gypsum was
Calcined gypsum production analyzed only rarely and sufficiently accurate data are still missing. In this paper, a carbon footprint
Environmental assessment
analysis of two types of gypsum ranging from cradle to gate according to ISO 14067 is presented. The
Carbon footprint
inventory data based on primary data obtained from the producers of natural gypsum and flue gas
Natural gypsum
Flue gas desulfurization gypsum
desulfurization gypsum in the Czech Republic are completed by the emission factors obtained from the
literature survey. The results of the carbon footprint analysis show that the carbon dioxide emissions
related to the manufacturing of calcined gypsum from flue gas desulfurization gypsum are 105.3 kg of
carbon dioxide/t, i.e., 25.2% lower than for the application of natural gypsum. Calcination is identified as
the most harmful process from the point of view of carbon dioxide generation for both raw materials; it
is responsible for 55% and 72% of total carbon dioxide emissions for natural gypsum and flue gas
desulfurization gypsum, respectively. The obtained information is essential for further design and
development of new types of composites meeting the requirements of sustainable development better
than today’s mainstream solutions.
© 2018 Elsevier Ltd. All rights reserved.
https://doi.org/10.1016/j.jclepro.2018.01.002
0959-6526/© 2018 Elsevier Ltd. All rights reserved.
796
J. For t, R. Cerný / Journal of Cleaner Production 177 (2018) 795e802
the cement use (exposure to allergens, free crystalline silica, or factors, such as composition of the energy mix, fuel base,
hexavalent chromium) pose a serious risk as well (Moretti et al., manufacturing technologies and efficiency, the legal framework,
2017). Therefore, new strategies leading to limitations of negative and composition of the raw materials should be taken into account
impacts of cement production were formulated (Summbell et al., (De Wolf et al., 2017; Heidari et al., 2017).
2016) and new approaches aimed at progressive and advanced In this paper, the environmental assessment of calcined gypsum
techniques (Valderrama et al., 2012) or at the substitution of fuel production in the Czech Republic is presented. The analysis in-
base (Fyffe et al., 2015; Rovira et al., 2010) were developed lately. cludes two major sources of raw gypsum, namely natural gypsum
However, the barriers related to a longtime payback of invested and flue gas desulfurization (FGD) gypsum; the minor gypsum
capital, short-run decision, and mistrust to the application of un- sources, such as titanogypsum, phosphogypsum, or fluorogypsum,
proven technologies still present the main limits to the application are not considered. The carbon footprint related to calcined gypsum
of more efficient innovations in the cement industry (Chen, 2009; manufacturing is determined for both types of raw gypsum and
Pardo et al., 2011). compared with Portland cement. Contrary to some previous studies
Utilization of materials with lower energy demanding produc- published by other investigators, the calculations are based on
tion, which could partially replace Portland cement in binders, can primary data obtained from the particular producers, and the
be considered as one of the prospective ways towards mitigation of regional factors are taken into account.
environmentally harmful effects related to cement manufacturing
(Turk et al., 2015). Slag (Rosales et al., 2017), fly ash (Hannesson 2. Materials
et al., 2012), or sewage sludge (Pavlík et al., 2016) can be
mentioned as characteristic examples in that respect. Another 2.1. Natural gypsum
alternative can be found in a complete replacement of Portland
cement by a different material base, at least in some practical ap- Natural gypsum is the primary source for the production of
plications. Here, calcined gypsum or geopolymers belong to the sulfate binders in the country. The Koberice quarry located in the
most prospective solutions. northeast (Silesian) part of the Czech Republic represents its
The availability of raw gypsum on the market is relatively wide exclusive source. The beginning of mining dates back to 1965. The
at present, the main sources being natural gypsum quarried in area of quarry reaches 65 ha and the thickness of gypsum layer is
certain locations and various types of waste gypsum appearing as about 35 m. The raw material contains 60e85% of calcium sulfate
by-products of some industrial activities, e.g., flue-gas- dihydrate with an admixture of clay and small amount of anhydrite.
desulfurization-, phospho-, titano-, and boro-gypsum. However, A detailed composition of mined rock is given in Table 1. The gyp-
despite the long history of its use, gypsum finds currently only a sum was formed by sedimentation in a closed water bay. Initially,
limited application in the building industry, mostly in the form of together with fine particles, the gray-colored lower benches, which
plaster boards or interior plasters. Its potential for future applica- contain about 50% micro- and macro crystalline gypsum, gradually
tions is though much greater, e.g., as a material of load-bearing settled. Later, the upper level was characterized by coarser crystals
structures (Tesarek et al., 2007) or lightweight construction mate- with a higher gypsum content of up to 90%. The last layer, over-
rial with properties similar to cellular concrete (Vimmrov a et al., burden, is made up of only 60% by gypsum and the rest are clays,
2011). loess, and humus loams.
The positive effects of gypsum application in construction on Material processing starts in the quarry by mining of the raw
the environment were recognized already years ago, but mostly it material and ends after the production of gypsum hemihydrate
was on a general level only. For instance, Guo and Shi (2008) (Fig. 1). Gypsum extraction methods are based on the utilization of
concluded that the production of gypsum is less demanding on stall mining procedures, such as drilling and rock blasting.
energy inputs due to the lower temperature of raw material calci- Exhausted materials are consequently loaded on trucks and taken
nation, and the carbon dioxide emissions related to the raw ma- away to the first stage of screening to remove mudstone and other
terial decomposition are also reduced. Suare z et al. (2016) referred undesirable content. Afterwards, the material is crushed, finely
to significant savings achieved by the utilization of waste gypsum. grounded, and placed into the stock, where it is naturally pre-dried.
The lower decomposition temperature accompanied with After a certain time period, depending on the intensity of the
decreased energy consumption was used by Ling and Kwan (2016) mining, the material is moved by the belt conveyors toward the
as a supporting fact of their research. calcination furnace using natural gas as fuel. Currently, the
The analyses of the environmental impact of gypsum produc- modernized kiln with utilization of the residual waste heat pro-
tion published to date were relatively rare and mostly suffered from vides about 5e10% fuel consumption savings compared to the
the lack of primary data. Jimene z-Rivero and García-Navarro (2016) outdated kiln used in the previous period. The fired gypsum is
in one of the very few studies on gypsum life cycle used therefore further moved by belt conveyors, milled to fine particles and moved
generic data derived from the case studies on similar building to the final storage. Currently, the production of natural gypsum is
materials. The problems related to the absence of primary data
were though noticed also for the most frequently analyzed building
materials, such as concrete (Dong et al., 2015). The results on the Table 1
Mineralogical and oxide composition of the natural gypsum rock.
evaluation of environmental impact of Portland cement found in
the scientific literature can serve as another example in that Component Amount (mass %)
respect, they varied from 662 kg (Deja et al., 2010) to 950 kg (Ali CaSO4$2 H2O 60e80
et al., 2011) of CO2/t. Dong et al. (2015) assigned the lack of pri- CaSO4 <0.5
mary data on concrete partially to the unwillingness of industrial Water <10
Loss of ignition <16
subjects to provide real data about environmental impacts of their
SiO2 8e16
main operating activity. However, some more objective factors, SO3 28e37
such as purity of the raw material, used technology, transportation, CaO 24e36
and other regional particularities (Zhang and Wang, 2016) can play MgO 0.2e1
an important role as well. Therefore, in order to provide a Al2O3 <1
Fe2O3 <1.6
comprehensive overview of environmental impacts, the local
J. For t, R. Cerný / Journal of Cleaner Production 177 (2018) 795e802 797
lower, as compared to the previous decades, which is due to the about 140 C. This dose of thermal energy is going into the absorber,
increasing use of industrial gypsum. The annual production of where desulfurization itself takes place. The absorber is a vertical
natural gypsum in this quarry varies from 20 to 25 thousand tones. vessel with a circular cross section of ~15 m in diameter and
30e40 m in height. At the top, there are placed 3e4 shower planes
2.2. Flue gas desulfurization gypsum formed by a pipe network with special limestone suspension
nozzles. It contains very pure (98%) and finely ground
FGD gypsum represents one of the major sources for calcined (d ¼ 0.09 mm) limestone which is converted to an aqueous sus-
gypsum manufacturing on a world scale (Lee et al., 2011). It can be pension with 25% CaCO3 before use. The flue gases are introduced
perceived as a waste product formed during combustion of coal. If into the middle portion of the so-called absorption zone, the rising
the coal has a high sulfur content, it is released during high tem- ones are washed with a “spray” absorption agent and the reaction
perature combustion and forms a part of flue gas in the form of of SO2 and CaCO3 takes place. Purified exhaust gases at 60 C leave
sulfur dioxide. Efforts to mitigate the negative impact of coal the absorber back to the heat exchanger, where they are reheated to
combustion on the environment result in desulfurization of the flue 95 C to be fed into the chimney. The resulting suspension is
gases in power stations and heating plants in large quantities. accumulated at the bottom, where the oxidation air is being
Desulfurization is carried out in a dry way by fluid combustion in injected. A part of the absorber serves also as an indicator of
such a way that limestone or dolomite is fed to the fuel and the composition. The pH value reveals if the mixture still contains some
desulfurization process takes place already in the boiler (Fig. 2). The remaining limestone; in that case the sludge is introduced again
hot combustion gases are first separated from solid particles in the into the device (Guo and Shi, 2008). The produced gypsum has
electrostatic precipitator and with an initial temperature of 180 C excellent properties. It is characterized by large compact crystals
enter the regenerative heat exchanger where they are cooled to and high chemical purity (98%). The final humidity is about 10%.
3. Methods
Mining
The environmental assessment of gypsum manufacturing in the
Czech Republic was done using the calculation of carbon footprint
in accordance with ISO 14067 (2013), where technical specification
of carbon emissions is given. This document is based on ISO 14040 Transportation
(2006), 14044 (2006), 14020 (2000), and 14025 (2006) standards
which are often used for the environmental product declaration
and assessment of the environmental impact. Carbon labeling ac-
cording to ISO 14067 (2013) provides a modern and improved Milling and storage
analysis, as compared to PAS 2050 (2011) or WRI/WBCSD: The GHG
protocol (2011).
Based on ISO 14067 (2013), the application of carbon footprint
methods in this paper was done in the following steps: Calcination
Table 2 Table 5
Life cycle inventory of calcined gypsum production: natural gypsum as raw material. Comparison of cumulative carbon footprint of calcined gypsum production (cradle
to gate).
Process description Energy consumption Fuel type
per ton Process description Fuel type CO2 emissions/t of gypsum
Separation and dewatering 24.3 kWh Electricity Table 5 shows the cumulative carbon footprint of calcined
of FGD gypsum gypsum production from natural gypsum and FGD gypsum.
Transport to storage 6.3 kWh Electricity Apparently, while the total greenhouse gas emissions related to the
Transport to the calcination 2.1 kWh Electricity
kiln from storage
processing of natural gypsum were 140.7 kg CO2/t of produced
Calcination 63 kg Mixture of fossil calcined gypsum, for FGD gypsum they were 25.2% lower. This
and alternative fuels difference could be assigned, in general, to easier processing
Homogenization and 15.4 kWh Electricity technologies of FGD gypsum.
transport to the final
Fig. 5 presents the share of the particular manufacturing stages
storage
on total carbon dioxide emissions. The highest environmental in-
fluence could be assigned to the calcination of gypsum in the kiln
(more than 50%), for both natural gypsum and FGD gypsum as raw
Emissions related to the calcination of raw gypsum at temper-
materials. Burning of a substantial amount of natural gas during
atures up to 180 C in the rotary calcination kiln powered by natural
this process can be perceived as a significant factor generating
gas were determined on the basis of the environmental declaration
greenhouse gas emissions and damaging the ozone layer. Taking
of the particular kiln from its producer. Provided data were further
into account the previous studies of various authors, the combus-
discussed with the kiln maintenance and recalculated according to
tion of fossil fuels is also accompanied with other negative exter-
the real natural gas consumption during the manufacturing process
nalities, such as production of formaldehyde, benzene, and other
of calcium hemihydrate with calcination temperature about 150 C
substances (Jiaqiang et al., 2017; Zhang et al., 2018).
as the main product, namely about 57.3 kg CO2/GJ.
For natural gypsum as the raw material, the second most sig-
The secondary emission related to the usage of the electricity
nificant environmental burden was mining from the quarry. The
grid was calculated on the basis of the knowledge of the Czech
use of various machinery powered mainly by diesel fuel partici-
energy mix with the dominant share of combustion of fossil fuels
pated in the greenhouse gases (GHGs) production by about 15%.
and nuclear power plants. The secondary production of carbon
Crushing and separation of raw materials posed the third most
dioxide emissions generated by consumption of electricity from the
energy demanding process accompanied with excessive GHGs
grid were estimated on the basis of the of the WNA Report (2010) in
emissions, having only a slightly lower share than mining.
relation to the Czech electricity mix. Thus, the carbon dioxide
On the other hand, for FGD gypsum dewatering of the material
emissions coming from electricity consumption were determined
obtained from the desulfurization procedure and its separation
as the weighted average of particular energy sources, namely
from the other residual compounds was the second most important
49.3 kg CO2/GJ. The Czech national energy mix used for electricity
process from an environmental point of view. The energy expended
production is given in Table 4.
here depended on the employed technology (hydrocyclones, in-
dustrial centrifugas, and belt filters); the process was responsible
for ~13% of cumulative amount of carbon dioxide. However, hereby
formed calcium sulfate dihydrate with up to 10% of water had a
Table 4 significantly lower demand on homogenization, as compared to
Czech energy mix. natural gypsum processing.
Energy source Share [%]
Mining and crushing were thus responsible for the major part of
differences between the carbon dioxide emissions related to
Renewable 10.11
manufacturing of calcined gypsum from natural gypsum and FGD
Sun 2.77
Wind 0.63 gypsum.
Water 1.15 The total share of transportation between particular production
Biomass 5.57 stages counted for natural gypsum processing only 8%, for FGD
Fossil 59.53 gypsum even less, and it was minor compared to the others. This
Lignite 43.91
Black coal 6.97
fact could be assigned in the case of natural gypsum to building the
Natural gas 8.4 whole manufactory in a close neighborhood of the quarry, for FGD
Others 0.25 gypsum to the absence of transportation from the quarry. The ho-
Nuclear 30.36 mogenization of calcium sulfate hemihydrate and transportation to
800
J. For t, R. Cerný / Journal of Cleaner Production 177 (2018) 795e802
160
Homogenization and
transport to the final
140
storage
Calcination
120
kg CO2/t of gypsum
60
Crushing
40
Transportation to the
20 separator and crusher
0 Gypsum quarring
NG FGD
Fig. 5. Comparison of carbon footprint of natural gypsum (NG) and FGD gypsum production.
the storage had a share of about 7e8% for both natural gypsum and geographically specific data was very important for the analyses
FGD gypsum processing. presented in this paper. This was obvious, e.g., in a comparison with
Summarizing the results of the environmental assessment, the the study of Lee et al. (2011) where the calculation of the envi-
utilization of FGD gypsum is in the conditions of the Czech Republic ronmental footprint of gypsum industry in the USA was presented.
beneficial and the need for the replacement of natural gypsum is The substitution of natural gypsum by FGD gypsum resulted, ac-
obvious. However, in many countries the production of FGD gyp- cording to Lee et al. (2011), in huge cumulative energy savings on
sum is significantly limited and moreover, according to the the national level when the USA energy mix was considered. The
worldwide carbon dioxide emissions restrictions (Desai et al., calculations in this paper performed for the Czech energy mix
2015), the operation of power plants based on the combustion of showed significantly lower savings.
fossil fuels with excessive sulfur content can be restricted in the The comparison of the environmental impact of calcined gyp-
mid or long-time horizon. The consideration about carbon dioxide sum with Portland cement as the most frequently used binder in
taxation in relation to the fulfillment of restriction targets became the building industry clearly favors both calcined gypsum binders
more actual in near future (Thao and Du, 2015). Implementation of analyzed in this paper. While carbon dioxide emissions related to
the tax pricing as an instrument for moderation of carbon dioxide the production of calcined gypsum were 140 kg CO2/t for natural
emission can significantly increase prices of many materials, thus gypsum and 105 kg for FGD gypsum as raw material, the CO2
decrease their utilization (Sathre and Gustavsson, 2007; He et al., emissions at Portland cement production varied from 662 to 950 kg
2015). of CO2/t (Table 6), depending on the regional and technological
As the main regional factors related to the environmental factors, such as the purity of raw materials, manufacturing tech-
assessment of calcined gypsum production in the Czech Republic, niques, transport distances, used fuel base, and different national
the used machinery, the purity of the raw material, and in partic- energy mixes.
ular the composition of the electricity mix, could be considered. Considering the ambitious carbon dioxide emission targets of
The major share of the electricity comes in the Czech Republic from the European Union and the contribution of cement industry to the
combustion of fossil fuels (60%), mostly lignite. Nuclear power total CO2 emissions, the application of calcined gypsum as an
plants contribute with about 30%, and the rest, i.e., only 10%, is alternative binder in some applications in the building industry can
supplied by the renewable power plants, despite the high sub- be perceived as a promising option (Lee et al., 2016; Vasconcelos
ventions for alternative and renewable energy sources. The com- et al., 2015; Baspinar and Kahraman, 2011). Apparently, gypsum is
bustion of lignite is accompanied with excessive carbon dioxide not able to provide an efficient solution for such a wide range of
emission, as compared to the other sources, even with other fossil applications as cement but many promising possibilities of gypsum
fuels. Whilst production of 1 kWh from combustion of natural gas is utilization were already found during the last decades (Degirmenci,
responsible for ~0.2 kg CO2, the combustion of lignite produces 2008; Garg and Jain, 2010; Zhou et al., 2012). The environmental
~0.36 kg CO2 per kWh (WNA Report, 2010). Compared to the other impact of calcined gypsum manufacturing, which can be at least
sources of energy, the coal combustion energy plants are 10 times five to six times (for natural gypsum and FGD gypsum as raw ma-
more harmful to the environment than nuclear power plants and terials, respectively) lower than for Portland cement, gives a clear
about 50 times than renewable energy sources from the carbon evidence of the great potential of calcined gypsum binders from the
dioxide production point of view (WNA Report, 2010). Therefore, sustainability point of view.
the collection of regionally focused inventories and other
J. For t, R. Cerný / Journal of Cleaner Production 177 (2018) 795e802 801
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