Fuel Processing Technology 104 (2012) 343351

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Fuel Processing Technology

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Particulate matter and elemental emissions from a cement kiln

R.K. Gupta, Deepanjan Majumdar, J.V. Trivedi, A.D. Bhanarkar
Air Pollution Control Division, National Environmental Engineering Research Institute (Council of Scientic and Industrial Research), Nehru Marg, Nagpur 440 020, India

a r t i c l e

i n f o

Article history:
Received 9 September 2011
Received in revised form 6 June 2012
Accepted 8 June 2012
Available online 6 July 2012
Keywords:
Air pollution
Coal
Coke
Dispersion modelling
Metal
Particle size distribution

a b s t r a c t
Particulate matter emission from a stack attached to the kiln and raw mill in a cement plant was studied. Elemental (As, Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb and Zn) and ionic (Ca2+, NO3, SO42) composition and particle size distribution of stack particulates, principal raw materials and products were determined. The feed rates of raw meal were
found to be 144 and 18 t h 1 at cyclone and bag house inlets, respectively, while stack emission of the same
amounted to 86 kg h 1, indicating bag lter removal efciency of over 99%. Particle size distribution of stack particulates revealed that PM10, PM2.4 and PM1 had cumulative shares of 88%, 49% and 15%, respectively. Emission
load of various elements from the stack ranged from 0.001 (copper) to 1.69 (iron) kg h 1. Air quality modelling
indicated that maximum ground level concentrations of As, Pb, Ni, Cd and Cr were much lower than the prescribed ambient air quality standards in India and also the Health Guidelines of USEPA and others. Particle size
distribution and the elemental content of the raw materials, by-products and cement indicated that elemental
exposure is likely from fugitive emissions during improper material handling and transport.
2012 Elsevier B.V. All rights reserved.

1. Introduction
Cement is an essential binding material used in construction and is
produced worldwide. India is the second largest cement-producing
country in the world [1]. India had a per capita cement consumption
of only about 136 kg in 200607 while China, Japan and France had
about 660, 631 and 447 kg, respectively, while the world average was
estimated to be about 350 kg [2]. In 1996, around 115 large and about
300 small cement plants in India produced 76.2 million ton (MT) cement per year. While the total installed capacity for cement increased
by around 47 million ton from 17 to 64 million ton during 1970 and
1990, it increased by another 41 million ton to 105 million ton of
installed capacity in India within only 6 years between 1990 and 1996
[3]. Capacity utilization in cement sector has been at its highest only
after 19992000 when it reached 85% and even more after 200405.
In January 2007, it even went up to 100%, highest ever in India, guiding
it to the average of 94% for the nancial year [2].
There are four primary process routes in cement manufacturing:
dry, semi-dry, semi wet and wet processes. In the dry process, the raw
materials are ground and dried into a raw meal, which is fed to the
pre-heater or pre-calciner kiln, requiring lesser energy than wet process. Majority of cement kilns use dry process nowadays [4]. Wet process is an older technology, where raw materials, often with high
moisture, are ground in water to form a pumpable slurry, which is fed
directly into the kiln or rst into a slurry dryer. A greater amount of
heat per ton of clinker produced is needed for the wet process to

Corresponding author. Tel./fax: + 91 712 2249895.

E-mail address: ad_bhanarkar@neeri.res.in (A.D. Bhanarkar).
0378-3820/$ see front matter 2012 Elsevier B.V. All rights reserved.
doi:10.1016/j.fuproc.2012.06.007

evaporate the additional water, resulting into 40% more energy consumption [5].
Particulates and particulate bound metals and ions emitted from
various industrial sources are dispersed into the atmosphere due to atmospheric dynamics [6,7]. Possible link between occupational exposure
to particulates and metals and respiratory health has been discussed by
several researchers [8,9]. Health risk to communities around cement
plants has been also studied [10]. Moreover, pollutants emitted from cement plants, especially metals, get distributed in soils also and may
affect vegetation and enter food chain via crops and water [11]. Evidently,
human health can be indirectly affected through the intake of drinking
water, contaminated foodstuffs and skin absorption of chemicals from
contaminated soils apart from direct exposure to ambient dust generated
by stack emissions from cement plants.
The potential sources of fugitive particulate matter (PM) emissions
in cement plants include raw material handling, grinding, blending
and delivery, clinker storage, grinding, cement storage, bulk loading
and packaging of nal product, making cement industry a major emitter
of particulate matter [12]. Stationary emission sources in a cement plant
are the stacks attached to the raw mill, rotary kiln, coal mill, grate cooler, cement mill etc. Majority of particulates emitted from cement industry may range from 0.05 to 5.0 m in diameter [13]. In cement plants
without any dust control technology, 24% and 7% of the emitted particles were found to be lesser than 10 and 2.5 m, respectively, in a wet
process kiln, whereas in a dry process kiln, 42% and 18% of particulate
emissions were less than 10 and 2.5 m, respectively. In both wet and
dry process plants with dust control technology, about 85% of escaping
particles were less than 10 m in diameter, while in dry plants having
bag houses, about 45% of escaping particles was of b2.5 m diameter
[14]. Traditionally, combustible materials such as coal and oil are used

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R.K. Gupta et al. / Fuel Processing Technology 104 (2012) 343351

as fuels in cement manufacturing but favourable conditions in the kiln

allow the usage of alternative fuels like exhausted motor oil, spent solvents, paint residues, plastics, scrap tyres, efuent treatment plant
(ETP) sludge, heavy metal-containing sludges etc. [11,1522]. Clinker
manufacturing also can utilize variety of raw materials, most of which
could make up for chemical deciencies of the primary limestone
feed. Although many of these supplementary materials are mined products, wastes are also potentially suitable, especially when they are
found cheap. Some materials contribute both oxides and energy, e.g.
deinking sludge from recycling and shredder nes from paper plants.
Some of these materials offer process advantages; for example, certain
aluminum smelter by-products (pot liners, catalysts) not only contribute alumina, but also sufcient uorine or calcium uoride to act as a
ux [23]. Fly ash and bottom ash from coal-red power plants, as well
as ferrous slags, are consumed in large quantities as supplementary silica, alumina, and lime sources for clinker. Pozzolans and similar
cementitious extender materials may also be added to produce blended
cements and masonry cements. Waste products used as extenders
include some types of y ash, GGBFS (ground granulated blast furnace
slag), burnt rice husk ash, CKD (cement kiln dust), burnt clays
(metakaolin) and silica fume [14]. Heavy metal emissions from cement manufacturing are common, since metals may be present in
both raw materials and conventional fuels [24]. A relevant study [24]
identied raw material feed as the principal source of metal input and
also indicated contribution from fuel, e.g. coal.
Particulate and associated metal emissions from cement plants may
have serious environmental and health implications. Especially, considering the lack of information on the extent of emissions of particulates
and metals from cement plants, it was deemed important to estimate
particulate emission rates along with their size distribution and metal
emission loads from cement industry. The tested null hypothesis or theory of this experiment was as follows: particulate matter and associated
metal emissions from cement plants do not pose any signicant environmental and health risk and so may be exempted from estimation
and detail scientic insight. So, the present study was undertaken in a
state of the art cement manufacturing plant in India to estimate particulate matter emission including its particle size distribution from the
common stack of a raw mill and rotary kiln, one of the most important
stationary sources in a cement plant, and also to understand its potential risk on human respiratory health as particle size is an important indicator of possible respiratory risks associated with particulates. Metal
and cation/anion content in raw materials and stack emission were
also determined to estimate metals/ionic emission loads and understand risks of metal exposure in likely events of fugitive emissions.
Further, elemental concentrations (e.g. As, Cd, Cr, Ni and Pb) in the
ambient air in the vicinity of the plant was predicted by using an
USEPAdeveloped dispersion model and these results were compared
with regulatory standards on ambient air quality followed in India
and also with USEPA and others Health Guidelines.
2. Materials and methods
2.1. Background of the cement plant
The selected cement plant is located in India and is one of the largest indigenous producer and exporter of cement. This plant has two
rotary kilns for clinker production each having an installed capacity
of 5200 metric tons per day (TPD) and total cement production capacity of the plant is about 60346187 metric tons per day (TPD).
Coal, pet coke and ETP sludge (as an alternative fuel) are used as
fuels in the proportion of 11:85:4. The ETP sludge is collected from
the clariers in an efuent treatment plant of a textile mill located
in the region. The general properties of fuels are presented in
Table 1. Dry raw milling is practiced in the selected plant where the
raw materials are dried using the excess heat generated by the rotary
kiln. For raw meal preparation, limestone, bauxite, laterite/red ochre

Table 1
Characteristics of fuels used in kiln.
Parameter

Imported coal

Pet coke

Alternative fuela

Sulphur (%)
Ash (%)
Gross caloric value (kcal kg1)
Moisture (%)

0.650.72
14.9015.35
65006650
7.6010.10

6.307.0
0.50.7
81508350
4.808.10

1.84
35.48
1570
11.88

ETP sludge.

are mixed in 5:1:1 proportion and fed to a grinder for crushing and
grinding and subsequently transferred to a cyclone separator wherefrom the separated materials are stored in a silo for subsequent delivery to the rotary kiln. The materials emanating from the cyclone
separator are driven off through a bag lter to the stack for release
to atmosphere. The materials collected in the bag house are recycled
to the silo. For clinker production, the raw mill is fed to a preheater
heated by the excess heat generated by the rotary kiln for thermal
conditioning and then to the rotary kiln for combustion along with
mixture of pulverized coal and coke as fuel delivered from the coal
mill. Clinker is produced under high temperature in the rotary kiln
from raw mill (mixture of iron ore e.g. laterite/red ochre, limestone
and bauxite) at a temperature of about 1400 1450 C. The ue gas
from rotary kiln is sent to the bag lter before its discharge into atmosphere through stack. A schematic diagram of the entire cement
manufacturing process in the selected plant is presented in Fig. 1.

2.2. Sampling
Samples of raw materials viz. limestone, laterite, red ochre, coal +
coke, gypsum, y ash were collected from their stockpiles and the grinding mill located within the plant premises. Dry samples were collected
from various points within the stockpiles by a stainless steel spatula
and composite samples of each were prepared by combining these samples. The composite samples were stored in zip locked plastic bags and
stored for analysis. The ne materials collected by the cyclone and bag
lter attached to the raw mill were also collected in zip locked plastic
bags by opening the dust removal attachment at the bottom of the systems and allowing the dust to freely fall in the bags. All the collections
and measurements were carried out during normal plant operations in
2009.

2.3. Stack and duct emission monitoring

Stack and duct monitoring was undertaken at various points to estimate the quantity material feed to various sections and also to measure
nal emission through the stack of kiln 1. Measurement of the raw
mill feed rate into the cyclone inlet, subsequent feed rate of outgoing
raw mill from cyclone into the bag lter inlet and emission of particulates from the combined stack of kiln and raw mill were carried out
by collecting particulate samples and determining parameters like air
temperature, pressure, velocity and ow rate within the material transfer lines at the selected sampling points by a stack monitoring kit. For
the sampling of particulate matter, Indian Standard Method for Air Pollution [25], which is similar to the USEPA method 5 [26], was used. All
the particulate samplings were carried out isokinetically for suitable
periods under normal operational conditions. Particulate matter concentrations were estimated by gravimetric analysis of particulate collection thimbles and subsequently the feed/emission rates (kg h 1) of
particulates were determined. The particles collected in thimbles were
analyzed for metals, ions and particle size distribution. Total particle inow concentration was measured at three points viz. cyclone inlet, bag
lter inlet and kiln stack outlet.

R.K. Gupta et al. / Fuel Processing Technology 104 (2012) 343351

345

Fig. 1. Schematic diagram of cement production and stationary sources in the selected cement plant.

2.4. Analysis of particulate matter

Raw materials and the particulate matter sample collected from the
stack were analyzed for particle size distribution by a Particle Size
Analyzer (CILAS 1180, Cilas). Total particulate matter emitted from
the stack was gravimetrically determined after conditioning glass bre
thimble for 24 h in a desiccator before and after sampling. Further,
heavy metal content in these samples was analyzed by an Inductively
Coupled Plasma Emission Spectrometer (JY-24, Jobin Yvon) as per
USEPA Method IO-3.4 [27]. Anions and cations in particulate samples
were analyzed in an Ion Chromatograph (Dionex 3000, Dionex Corporation) as per standard operating procedure [28]. Blank thimble samples
were also processed for background compensation using similar procedures for metals and anions/cations.

2.5. Impact of emissions of cement plant on ambient air quality around

its vicinity
USEPA-developed Gaussian plume dispersion based Industrial
Source Complex (ISC3) model, which can be used for single or multiple
source emissions, was used for predicting 24-hourly average ground
level concentration (GLC) inuenced by stack emissions from the kiln
stack. The details of the ISC3 model are documented elsewhere [29].
Daily surface meteorological data with respect to wind speed and direction and ambient temperature recorded in the area during study period
was used in the modelling exercise. The atmospheric stability classes
(PasquillTurner) have been computed using Turner's classication
[30]. By using source characteristics, emission rates and meteorological
data as input parameters, dispersion modelling was carried out for

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R.K. Gupta et al. / Fuel Processing Technology 104 (2012) 343351

Table 2
Emission and input rate of particulates from various transit points and kiln stack.

80

Temperature
(C)

Flow rate
(Nm3 h 1)

Particulate conc.
(mg Nm 3)

Entry/emission rate
(kg h 1)

70

Cyclone inlet
Bag house
inlet
Kiln stack
outlet

72
78

739417
269909

194599
65801

143890
17760

60

80

552736

155.3

85.8

estimating GLCs of selected metals (As, Cd, Cr, Ni and Pb) within 10- km
radial distance around the plant under study. Prediction of GLCs was
carried out for winter season as air pollutant dispersal is least in this
season. Further, isopleths of 24-hourly average GLCs were prepared.

Cumulative Share (%)

Sampling
point

71.2

Coal + Coke
Cement
Fly ash

57.9
50.8

50

37.0

38.2

40
30

23.2

22.0

13.4

20

8.0
2.1

10

0.5

0.8

0
0.1

2.4

10

Particle Size (m)

3. Results and discussion

Fig. 2. Cumulative share of various particle size groups in raw material and products.

3.1. Particulate feed rate and emissions

3.2. Particulate size distribution

Particulate size distributions of coal+ coke, y ash and cement revealed that a sizeable portion of the total particulate comprised of
PM0.1, PM1.0, PM2.4 and PM10, making them potentially harmful for
human health (Fig. 2). Ground coal + coke and y ash had higher

proportion in all particle size groups than cement. Proportion of PM1

was appreciably high in both coal+ coke and y ash, indicating signicant chances of health complications in cases of exposure. In ay ash,
over 50% proportion was on PM2.4, making it extremely harmful for
human health during possible exposure in handing and transport. For
coal+ coke, beyond 38% was PM2.4, which also could pose signicant
health risks in the coal and coke handling areas and coal mill. Particulate
size distribution in stack emission is presented in Fig. 3. The cumulative
shares of PM0.1, PM1.0, PM2.4, and PM10 emitted from kiln stack were 2.1,
15.3, 48.6, and 87.6%, respectively. In another study, Baroutian et al. [7]
reported similar trend in size distribution of particles from a kiln stack.
The population densities of particles in the stack emission were 0.07,
1.39, 1.08, and 5.70% for PM0.1, PM1.0, PM2.4 and PM10, respectively. Results of particulate size distribution are in agreement with results
reported in some other studies [14,33], indicating that about 85% of particles escaping from stack in the cement plant are less than 10 m in diameter and 45% of escaping particles was of b2.5 m diameter.
Particulates escaping through the stack with such size distribution indicated to potentially harmful consequences due to plume dispersion in
the areas within about 510 km radius around the plant.
3.3. Elemental compositions of particulate matter
Samples of raw materials and nished products were analyzed for
their elemental concentration (Table 3). Similarly, the concentration of a
few cations/anions and several metals were estimated in particulates collected from cyclone inlet, bag house inlet and the kiln stack (Table 4). In
general, Fe and Ca had higher concentration followed by nitrate and
100

Cumulative share (%)

Population density (%)

80
70

60
3

50
40

30
20

10
0

0
0.1

1
2.4
Particle Size (m)

10

Fig. 3. Particle size distribution in stack emission.

Population density (%)

90
Cumulative share (%)

General stack/duct parameters, particulate matter feed rate and emissions at various sampling points are reported in Table 2. The ow rate of
air carrying raw meal into the cyclone was 739,417 Nm3 h 1 while the
ow entering bag house inlet was 269,909 Nm3 h 1. The concentration
of raw meal in the cyclone inlet air was as heavy as 194.6 g Nm 3. As
raw meal is the major raw material for cement, it is fed in huge quantity
to cyclone for onward transmission to the rotary kiln via preheater. The
raw meal feeding rate was calculated to be almost 144 t h 1 from raw
mill to the cyclone, while about 18 t h 1 of it entered bag house, constituting a major proportion of raw meal entering in the preheater for further delivery to rotary kiln. The particulate concentration and emission
from the kiln stack were about 155 mg Nm 3 and 86 kg h 1, respectively, implying that only 0.48% of particulate was released though the stack
after getting ltered in the bag lter, indicating a bag lter removal efciency of about 99%. The values of particulate emission from kiln stack
in this study were consistent with the Adana Cement Plant studied by
Ekinci et al. [31], having a cement production capacity of 245 t h 1
(PM emission: 86 kg h 1), similar to the one reported in the present
study (~250 t h 1). Central Pollution Control Board (CPCB) [32] of
India has promulgated a particulate emission limit of 250 mg Nm 3 for
Indian Cement plants having more than 200 TPD capacity with a note
that a more stringent standard of maximum 150 mg Nm 3 was applicable for larger plants on case to case basis. Taking this scenario into consideration, the particulate concentration in the rotary kiln stack emission
marginally exceeded the standard of 150 mg Nm 3 promulgated by
CPCB. Since the extent of emission was found to be just beyond the regulatory guideline or standard, the industry has to think of its strategy to
bring it down within the limit to escape sanctions by state pollution control body. Emission monitoring and proper maintenance of the bag lter
should be undertaken on regular basis apart from seriously considering
replacement of fabric lters frequently for improved performance.
Concentration of CO2, CO, NOx and SO2 in the ue gas emanating from
the kiln stack was also measured by permanently installed gas sensors.
Average concentrations of CO2, CO, NOx and SO2 in the kiln stack emission
were 16.1%, 222.6 mg Nm 3, 1127 mg Nm 3 and 3.8 mg Nm 3, respectively, and these values were similar to an earlier report done for cement
kilns [49]. These concentrations amounted to emissions of 160.1 Mt h 1
of CO2 and 123, 623 and 2.1 kg h 1 emissions of CO2, CO, NOx and SO2,
respectively.

R.K. Gupta et al. / Fuel Processing Technology 104 (2012) 343351

347

Table 3
Metal/ion contents in raw materials and nished products.
Metal/ion concentration (mg g1)

Material

Coal + Coke
Gypsum
Fly Ash
Laterite
Redochre
Limestone
Clinker
Cement

Ca2+

NO3

SO42

As

Cd

Co

Cr

Cu

Fe

Mn

Ni

Pb

Zn

NA
NA
NA
0.42
1.42
5.18
NA
NA

NA
NA
NA
1.39
1.64
1.77
NA
NA

NA
NA
NA
0.01
0.07
1.54
NA
NA

0.06
0.12
0.59
0.01
0.04
0.28
0.86
0.84

0.17
0.08
0.09
0.03
0.01
0.09
0.21
0.19

0.02
0.03
0.03
0.06
0.03
0.04
0.17
0.15

0.02
0.01
0.04
0.03
NA
0.02
0.06
0.06

0.01
0.01
0.03
0.01
0.03
0.01
0.05
0.04

1.86
2.50
4.12
10.6
6.59
6.65
35.38
28.38

0.39
0.07
0.11
0.44
NA
0.75
0.55
0.62

0.16
0.03
0.03
0.02
0.01
0.04
0.08
0.07

0.04
0.13
0.12
0.03
0.04
0.16
0.31
0.29

0.02
0.03
0.06
0.01
0.02
0.04
0.10
0.10

NA, not analyzed.

sulphate. Among the elements of environmental concern, As, Cd, Cr, Ni

and Pb showed higher concentration in the stack emissions. The results
indicate that only a small amount of elements associated with particles
were emitted through the stack (Table 4). In general, majority of the elements were captured by the bag lter, indicating removal efciency to the
tune of 99%. Amongst all the elements, Ca had the highest concentration
in cyclone and bag house followed by Fe. Bhanarkar et al. [34] also
reported higher concentration of Ca and Fe at ESP inlet in coalred
power plant. As the raw meal consisted of primarily limestone, laterite/
redochre in the proportion of 5:1, the dominance of Ca and Fe was justied in the raw mill entering cyclone and bag house inlets. Dominance
of Ca and Fe was also observed in the raw materials (Table 3), but Ca emission via particulate matter through the stack was well below that of Fe, indicating that probably most of the Ca was associated with larger sized
particulates which were retained by cyclone and bag house. Notably, concentration of SO42 and NO3, which were much lower than Ca2+ in the
feeds to cyclone and bag house, had higher mass emissions from stack
(Table 4). Sulphates and AsCa compounds are produced due to mineral
transformation that occur during coal combustion and increased from cyclone inlet to stack y ash as a result of reaction between CaO and gaseous
products such as SOx [35].
The mass feed rate or emission rate of a few cations/anions and several metals was estimated for cyclone inlet, bag house inlet and the kiln
stack (Table 5). The input rates of As, Cd, Cr, Cu, Ni, Pb and Zn were
29.99, 15.7, 5.7, 2.07, 8.84, 31.5 and 11.8 kg h 1, respectively, of which
only 0.020, 0.008, 0.003, 0.001, 0.003, 0.019 and 0.007 kg h 1 were emitted from stack, indicating that only a small quantity of these elements
from the fuel/raw materials was emitted and that the bag lter capture
most of the elements. The total emission rate of toxic elements (As, Cd,
Cr, Ni and Pb) was 0.053 kg h 1. Ratios of output and input indicated
that only minor amounts of most elements were emitted from the

Table 4
Concentration of cations/anions and metals from various discharge points.
Ion/
metal
Ca2+
NO3
SO42
As
Cd
Cr
Co
Cu
Fe
Mn
Ni
Pb
Zn
a

Concentration (g Nm 3)
Cyclone inlet air

Bag lter inlet air

Kiln stack

1066796
223441
78875
38653
16661
7164
7164
2666
847374
78473
7497
41486
15495

523461
109934
36767
13266
5130
1120
2064
707
241507
24941
2417
13502
2771

349
649
573
37
14.6
4.9
15.4
2.1
3062
76
5.1
34
13.5

Efciency in removing respective ions/metals.

Bag lter
efciencya
(%)
99.93
99.41
98.44
99.72
99.71
99.56
99.25
99.71
98.73
99.70
99.79
99.75
99.51

stack. Arsenic was emitted at a rate of 0.07% of input feed, followed by

Pb, Cd and Cr, and most of these elements are volatilized during combustion and expected to be enriched with ne particles, but the extent of enrichments depends on the post-combustion transformations [36]. The
total emission rate of other elements was 1.80 kg h 1. There is little concern about the toxicity of these elements. Majority of these emissions in
these elements are related to Fe, Mn and Co (1.74 kg h 1) with Fe having
the highest emission (1.69 kg h 1). Schuhmacher et al. [10] studied a cement plant having a clinker production capacity of ~4110 TPD, similar to
one in the present study (~5200 TPD). However, unlike the other cement
plant [10], the cement plant in this study used only coal/pet coke and bag
lter as the particulate control device. There are differences in particle
types/metals emitted from these two cement plants (Table 5).
Several researchers have reported increased emissions of PM and
metals with increasing amounts of alternative fuels viz. waste tyres
[15,16,21,17], sewage sludge [18,11], waste oils [19,17], refusederived fuel (RDF) [20], and solid recovered fuel (SRF) [37] when used
in cement plants. However, the characteristics of metal emissions depend on the alternate fuel used for co- processing. Pegg et al. [21]
showed that class I and II metal emissions were high with the use of
tyre as supplemented fuel with coal and reported an increase in Zn
emissions with use of tyre as alternate fuel with coal and pet coke
[17]. It was attributed to the presence of zinc oxide in tyres as part of
the rubber vulcanization [21]. Conesa et al. [15] reported increased
emissions of Ni and Pb in stack emissions when tyres were fed as fuel.
The behavior of the metals in cement kiln was found to be inuenced
by the feeding point of these materials, i.e. when tyres were fed at the
end of gas trajectory, i.e. the volatilizing metals emanating from tyres
had too low residence time in the kiln to be absorbed by the cement,
and when sewage sludge was fed to the other side of the furnace at
the point of maximum temperature, it resulted in a higher residence
time of the volatiles produced [15]. However, Giugliano et al. [38] inferred that the metal emissions did not appear to have any relationship
with the fuel substitution practices when authors conducted tests with
constant mass feed ratios of tyre chips to conventional pulverized petroleum coke ranging from 0.25 to 0.7 in cement production. The applied fuel replacement ratios ranged between 16 and 36% in terms of
total heat input (3780% in terms of the precalciner heat load), with a
tyre chip having lower heating value (LHV) of 6500 kcal kg 1 to
7150 kcal kg 1. Authors indicated that emissions of even the most volatile elements in tyres (Pb and Zn) were not increased, which were
partially attributed to the fabric lter [39]. Amand and Leckner [18]
tested co-combustion of pre-dried sewage sludge and mechanically
dewatered sludge in circulating uidized bed (CFB) with coal or
wood as base fuel. They found that all mercury was volatilized, but
some Cd remained in the bed, especially during operation with
coal. Instead, Hg and Cd were enriched in the y ash, Hg mostly in
the bag lter, whereas Cd was rather evenly distributed between
secondary cyclone and bag lter. Manganese which is known to be
less volatile in coal combustion showed an even distribution in the

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R.K. Gupta et al. / Fuel Processing Technology 104 (2012) 343351

Table 5
Emission and input rate of cations/anions and metals and comparison with other studies.
Ion/
metal

Input through coal + coke

(kg h 1)b

Ca2+
NO3
SO42
As
Cd
Cr
Co
Cu
Fe
Mn
Ni
Pb
Zn

86.0
21.2
3.6
1.3
3.4
0.4
0.4
0.1
37.9
8.0
3.3
0.8
0.3

Feed/emission rate (kg h 1)

Cyclone inlet

Bag lter inlet

Kiln stack

789
165.2
58.3
28.69
12.3
5.30
5.30
1.97
626. 6
58.0
5.54
30.7
11.5

141.3
29.67
9.92
3.58
1.38
0.30
0.56
0.19
65.2
6.73
0.65
3.64
0.75

0.193
0.359
0.317
0.020
0.008
0.003
0.009
0.001
1.692
0.042
0.003
0.019
0.007

Annual
emissions
(ton y 1)a

Percent
emission (%)

1.69
3.14
2.77
0.18
0.07
0.02
0.07
0.01
14.83
0.37
0.02
0.16
0.07

0.02
0.19
0.51
0.07
0.05
0.05
0.15
0.06
0.25
0.06
0.03
0.06
0.06

Kiln stack
emissiond,e
(kg h 1)
NA
NA
NA
0.00199
0.00399
0.00529
NA
NA
NA
NA
0.00860
0.04392
0.02585

NA, not available.

a
Considering 24 365 operation.
b
Calculated from coal/coke feed rate.
c
Calculated as a ratio of kiln stack emission and input (coal/coke input + cyclone inlet inputs) expressed as percentage.
d
Converted to kg h 1 from g s 1 as taken from [10].
e
Volumetric ow rate: 425,000 Nm3 h 1; PM emission: 33.156 kg h 1.

ashes in the boiler system during co-combustion with coal, but it was
enriched in the nest y ash during co-combustion of wood and
sludge.
Cutting oils originating from metal working uids may carry Co,
Ni and Cr which are used as binders in cutting tools and grinding
wheels [40], Pb (from leaded steel), Zn (from galvanized steel), Hg
and Cu (from cast and ductile irons) [41]. Cutting oils may sometimes carry a lighter load of heavy metals than waste oils in general.
The absence of volatile heavy metals from the indicative composition
of cutting oils positively affects their potential injection to the cement kilns [19]. RDF usually has a higher content of Sb, Hg, Cd, As,
Pb, Cu, Cr and Zn than pet coke, but sometimes coal can also present
large amounts of Hg, Co, Cd and Tl [20]. Based on these data and the
transfer factors (TF to waste gas for cement kilns), a simulation has
been performed on the effect of the use of RDF instead of coal and
pet coke (50% of caloric substitution has been assumed) on the
emissions of a cement kiln. They found that substitution of pet coke
with RDF had a negative impact (increase) on heavy metal emissions, particularly Hg, whereas a positive effect was expected if RDF
was used instead of coal. SRF is another alternative fuel made from
nonhazardous household wastes and is more homogeneous and
less contaminated than the generic RDF [42], though its caloric
value is much lower than petroleum coke. It was tested with petroleum coke, tyres and meat-bone meals in cement industry [36].
Their nding reveals that Zn and Mn emissions were highest when
SRF was used as Zn and Mn were high in SRF and probably these
metals were not being satisfactorily xed in the cement kiln.
Achternbosch et al. [43] found an increase in the trace element (antimony, cadmium, and zinc) concentration in cement due to the
use of waste as an input material. Also, Pb and Co concentrations increased in the cement but were less pronounced. The authors indicated that contrary to trace elements from raw materials, trace
elements from fuels underwent an additional resistance in the heat
exchanger/rotary kiln system, as a result of which their probability
of being emitted was much smaller. Oil well-derived drilling waste
and an electric arc furnace slag, tested on both laboratory and industrial scale, have proved to able replacements of limestone in part and
clay in the Portland clinker manufacture [44]. This feature is very interesting from an environmental point of view due to the related
reduced kiln thermal input and CO2 emission. No signicant differences are observed for the metal content in emissions where these
materials were used.

3.4. Environmental assessment of emitted elements

3.4.1. Stack emissions
As no metal emission limits for cement industry have been prescribed
by Regulatory Authorities in India, results of this study were compared
with Turkish Environmental Standards, which has classied several elements relevant to cement industry [12] into non-carcinogenic class I
(encompassing Cr, Cd, Pb and Ni determined in this study), II
(encompassing Zn and Co determined in this study) and III
(encompassing Cu and Ca determined in this study). While Co and Cr
are also classied under class II for carcinogenic elements, they
only apply to carcinogenic compound formation. Arsenic has been
classied under carcinogenic class II element as arsenic trioxide, a
carcinogenic compound relevant to cement industry. Iron (Fe) has
not been included in any classication. Calcium and magnesium oxides are listed in the class III of non-carcinogenic trace elements, although their concentrations are quite high in the solid materials
handled in cement plants [12]. As per Turkish Air Quality Protection
Regulation (AQPR) [45], concentration or emission of none of the
metals reported in this study exceeded the prescribed safe limits.
From the regulatory perspective available in Turkey, the metal emission
from this cement plant can be considered as safe for environment and
health. European Commission [46] has prescribed an emission limit
value of 0.5 mg m 3 for Sb+ As + Pb + Cr+ Co + Cu+ Mn + Ni + V in
cement kilns practicing co-incineration. In this work, total heavy
metal emissions (excluding Sb and V) were 0.175 mg Nm 3 which
was within EU standards. USEPA [47] has promulgated emission
standards for various metals for existing and new stationary sources
for cement kilns. Separate standard has been prescribed for semivolatile (Pb + Cd) and low volatile metals (As + Be+ Cr). The emission
of Pb+ Cd in this study was found to be lower than the USEPA prescribed emission limit of 330 g dscm 1. In India, though no emission
standards have been specied for cement industry, a set of standards
exist for common hazardous waste incinerators which prescribes limiting concentrations of 0.05 mg Nm 3 (2 h) for Cd + Th and Hg and its
compounds, while a limiting concentration of 0.5 mg Nm 3 (2 h) has
been prescribed for Sb + As+ Pb + Co+ Cr+ Cu + Mn+ Ni+ V and
their compounds [48]. While comparing with these standards, total
heavy metal emissions (excluding Sb, V) from this cement plant are
lower than the permitted value. If annual emissions are considered in
the light of 24 365 operation, 14 t Fe would be emitted to the atmosphere with all other metals falling below 1 t (Table 5). Sulphate and

R.K. Gupta et al. / Fuel Processing Technology 104 (2012) 343351

349

Table 6
Predicted maximum concentration of various metals in ambient air at the vicinity of the cement plant vis a vis ambient air quality and health guidelines.
Metals

As
Cd
Cr
Ni
Pb
a
b
c
d

Emission
rate from
stack (kg h 1)

Maximum predicted
ground level
concentration
(ng m 3)

Background concentration
around cement industry
[54] (ng m 3)

Ambient air concentration

around cement industry
[54] (ng m 3)

CPCBa, [50] standards

(ng m 3)

0.020
0.008
0.003
0.003
0.019

0.58
0.23
0.09
0.09
0.55

120
850
800
240

120490
11206840
7104310
2401230

20
500

ATSDRb, [52]

USEPAc, [51]

OEHHAd, [53]

10
300
90

1500

15
20
200
14

Central Pollution Control Board, India.

Agency for Toxic Substances and Disease Registry, Georgia: Minimum risk level (MRL)/Reference concentration (RfC) values.
US Environmental Protection Agency, USA: National Ambient Air Quality Standard for lead. US EPA has not developed an MRL/REL/RfC for lead.
Ofce of Environmental Health Hazard Assessment, California: Reference exposure level (REL).

nitrate would be emitted at around 3 t per year. But since all these elements/ions are plant nutrients and have low mammalian toxicity, their
emissions may not be as hazardous as other toxic metals to the receiving environment in the short run.
3.4.2. Impact of stack emissions on ambient air quality
The maximum values of predicted GLCs of selected metals along
with their point of occurrence within 10 km radius around the plant
were obtained through air quality modelling by ISC3 model (Table 6).
The maximum predicted concentrations of As, Cd, Cr, Ni and Pb were
0.58, 0.23, 0.09, 0.09 and 0.55 respectively likely to be observed at
1.7 km distance in southwest direction. The modelling results presented
in table mainly focused on the maximum predicted concentrations of
the selected elements, since the latter were the most signicant vis a
vis the regulatory standards. Results indicated that concentration of all
the selected elements (As, Cd, Cr, Ni and Pb) emitted from the cement
plant were lower than the Indian National Ambient Air Quality Standard
promulgated by CPCB [50] as well as Health Guidelines of USEPA [51]
and other sources ATSDR [52] and OEHHA [53].
The ground level concentrations predicted by the model were also
compared with some reported ambient concentrations of the same
around cement plant in India [54] (Table 6). The background and ambient concentrations are the concentration values at the upwind and
downwind sites within 10 km of the cement plant reported in Sharma
and Parvez [54]. In light of these earlier reports, the predicted concentrations of elements in the vicinity of this plant were well within the range
of published data and can be termed as low. The predicted GLCs for As in
the form of isopleths are presented in Fig. 4. The pattern of isopleths of

other metals was similar, although the values differed in magnitude marginally. The model predictions indicated that the maximum concentration of metals would occur primarily in the south western direction in
the winter season under the prevailing wind conditions. Maximum impact of pollutants was observed within about 45 km distance in the
southwest direction as northeast was the predominant wind direction
observed in the area in that season. Hence, it is important to monitor regularly the levels of pollutants in the zone of maximum impact.

ng/m3

0.55

0.45

3.4.3. Fugitive emissions

In cement plants, fugitive emissions of raw materials and cement dust
may be appreciable and can cause ill health by skin contact, eye contact, or
inhalation. Risk of injury depends on duration and level of exposure and
individual sensitivity. Cement may contain hazardous substances like
crystalline silica (quartz), lime, gypsum, nickel, cobalt, and chromium
compounds [55]. Silica dust and metals are known to cause potentially
dangerous human health complications and so cement dust can be an important pathway to potential human exposure. Metal content in raw materials and cement (Table 3), analyzed for understanding the risks of
exposure via fugitive emissions during transfer, handling, storing and
packaging activities, indicated that although metal content was found to
be low to moderate, long time exposure to the fugitive dust emanating
from these materials might cause health problems due to metals apart
from the ne particulates [56]. The particle size distribution of
coal +coke, y ash and cement revealed that a sizeable portion of the
total particulate comprised of PM0.1, PM1.0, PM2.4, and PM10 making
them potentially harmful for human health. Ground coal +coke and y
ash had higher proportion of PM0.1, PM1.0, PM2.4, and PM10 than cement.
As cement is crushed in cement mill from gravely clinker, it is coarser in
nature than ground coal +coke and y ash. Expectedly, y ash had the
highest proportion of ne particulates but fortunately lesser amount of
y ash is handled by the plant for cement production, while coal and
coke are handled in much more quantity and cement production is also
much higher than y ash handled. So, there may be enough scope of
long term exposure through fugitive emissions of coal/coke, y ash
along with cement and proper care must be taken to arrest their fugitive
emissions.

0.35

4. Summary and conclusions

0.25

The particulate matter and associated elemental content (Ca 2 +,

SO42, As, Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb and Zn) of the principal
raw materials, products, combustion material from the kiln stack in
a cement plant were determined. Among the elements of environmental concern (As, Cd, Cr, Ni, Pb), As, Cd and Pb showed higher concentration in stack emitted particles. The particulate and particle
bound elemental emissions from the stack were found to be within
safe limits and the emission control system attached to rotary kiln is
found to be efcient. The rates of emissions of elements associated
with particles are very low. Ratios of output and input indicate that
only minor amounts of most elements are emitted from stack. No

10
N

8
Distance in North Direction, (km)

Health guidelines (ng m 3)

-2
-4

0.15

-6
0.05
-8
-10
-10

-8

-6
-4
-2
0
2
4
6
Distance in East Direction, (km)

10

Fig. 4. Predicted isopleths for 24-hourly average GLC of arsenic.

NO3,

350

R.K. Gupta et al. / Fuel Processing Technology 104 (2012) 343351

emission standards have been specied for cement industry in India

and so when compared with the regulatory standards in Turkey, EU
and USEPA the metal emission from this cement plant can be considered as safe for environment and health. While comparing with the
Indian standards exists for common hazardous waste incinerators,
total heavy metal emissions (excluding Sb, V) from this plant are
within the prescribed limit. The model-predicted GLCs of As, Cd, Cr,
Ni and Pb in the ambient air were much lower than the corresponding
regulatory standards in India and the Health Guidelines of USEPA and
others. The predicted concentrations of these elements in air were
found low compared to the ambient concentrations around cement
plant in India as reported in literature. Maximum impact of pollutants
was observed at 45 km distance in the southwest direction which is
the most predominant wind direction in the study area, and requires
regular monitoring in the zone of maximum impact. However, there
may be long term concerns from fugitive emissions of raw materials
and byproducts, but as such no standards are there for metals in
raw materials for the purpose of understanding the risk in cases of fugitive emissions. The particle size distribution indicates the presence
of ne particulates in emissions and raw materials and there may
be considerable exposure to these. So, environment management system should be made robust to safeguard workers from heavy exposure from ne particulates and associated metals.
The Industry has installed bag lter for particulate control in the raw
mill + kiln stack which was found to have high efciency of above 98%
which can be considered excellent under existing conditions. But, during monitoring, particulate emission was found to be beyond the prescribed upper limit and so a serious rethinking on the bag lter
performance has to be done immediately. Regular maintenance and replacement of the bag lters in quick succession may be considered
along with the possibility of going for more efcient type of fabric lters.
Due consideration may be given to another possible particulate control
option viz. cyclone followed by electrostatic precipitator, which will
need substantial input of power but will also be able to separate high
amount of particulate emissions from the industry.
Further, to control kiln emissions in cement manufacturing that uses
conventional or alternative fuels and raw materials one would require
precise control of processes. Particular attention is needed for control in
fuel quality (specically with regard to particle size, homogeneity and
ammability) and to the use of best combustion practices. Control of
proper dose, feeding point and burner technology will also be important
to maintain smooth kiln operating conditions [57]. Available carbon capture and storage (CCS) technologies may be considered to capture carbon
from CO2 emissions, provided any of them is proved to be economical for
this single plant. Barker et al. [58] have studied the techno-economical
feasibility of post-combustion CO2 capture and oxy-combustion CO2 capture for modern dry cement plants. Oxy-combustion offered the lowest
cost solution for CO2 capture for newly built cement plants but authors
recommended in-depth R&D to address of technical issues for successful
deployment of this technique. Cost was estimated to be about 40/ton of
CO2 avoided for a 1 Mt/y for a European cement plant and 23/Mt of CO2
avoided for a 3 Mt/y plant in Asia. The costs estimated for a postcombustion capture was found to be much higher at 107/Mt CO2 for a
1 Mt/y European cement and 59/t for a 3 Mt/y Asian plant. The authors
opined that use of alternative solvents and integration with an adjacent
power plant could substantially reduce the cost. Bosoaga et al. [49] have
discussed the efcacy and advantages of calcium looping cycle as a
novel tool for carbon capture which can utilize heat released during carbon capture for generating steam.
Acknowledgements
The authors are grateful to Director NEERI, Nagpur for constant
guidance and encouragement and Head, Air Pollution Control Division, NEERI, for his kind approval and permission to submit the
manuscript.

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