ARTICLE IN PRESS

Atmospheric Environment 41 (2007) 6236–6254

www.elsevier.com/locate/atmosenv

PM10, PM2.5 and PM1.0—Emissions from industrial

plants—Results from measurement programmes in Germany
C. Ehrlicha,, G. Nolla, W.-D. Kalkoff a, G. Baumbachb, A. Dreiseidlerb
a
Saxony Anhalt State Environmental Protection Agency, Reideburger Str. 47, D-06116 Halle, Germany
b
University of Stuttgart, Institute of Process Engineering and Power Plant Technology, Pfaffenwaldring 23,
D-70569 Stuttgart (Vaihingen), Germany
Received 8 December 2006; received in revised form 29 March 2007; accepted 29 March 2007

Abstract

Emission measurement programmes were carried out at industrial plants in several regions of Germany to determine the
fine dust in the waste gases; the PM10, PM2.5 and PM1.0 fractions were sampled using a cascade impactor technique. The
installations tested included plants used for: combustion (brown coal, heavy fuel oil, wood), cement production, glass
production, asphalt mixing, and processing plants for natural stones and sand, ceramics, metallurgy, chemical production,
spray painting, wood processing/chip drying, poultry farming and waste treatment. In addition waste gas samples were
taken from small-scale combustion units, like domestic stoves, firing lignite briquettes or wood.
In total 303 individual measurement results were obtained during 106 different measurement campaigns. In the study it
was found that in more than 70% of the individual emission measurement results from industrial plants and domestic
stoves the PM10 portion amounted to more than 90% and the PM2.5 portion between 50% and 90% of the total PM
(particulate matter) emission. For thermal industrial processes the PM1.0 portion constituted between 20% and 60% of the
total PM emission.
Typical particle size distributions for different processes were presented as cumulative frequency distributions and as
frequency distributions. The particle size distributions determined for the different plant types show interesting similarities
and differences depending on whether the processes are thermal, mechanical, chemical or mixed. Consequently, for the
groups of plant investigated, a major finding of this study has been that the particle size distribution is a characteristic of
the industrial process. Attempts to correlate particle size distributions of different plants to different gas cleaning
technologies did not lead to usable results.
r 2007 Elsevier Ltd. All rights reserved.

Keywords: PM10; PM2.5; PM1.0; Stationary source emission; Emission measurement; Fine particles; Cascade impactor; Particle size
distribution

1. Introduction

Corresponding author. Tel.: +49 345 5704500; The health impact of fine dust has been evaluated
fax: +49 345 5704505.
at international and EU level (Council Directive,
E-mail address: [email protected] 1999; The APHEA Project, 1996; WHO, 2006;
(C. Ehrlich). Second Position Paper on Particulate Matter, 2004).

1352-2310/$ - see front matter r 2007 Elsevier Ltd. All rights reserved.
doi:10.1016/j.atmosenv.2007.03.059
 ARTICLE IN PRESS
C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254 6237

According to recent epidemiological investigations Poland and others. Small wood-burning furnaces
fine and ultrafine dust particles in the ambient air were also investigated.
adversely affect human health so the European
commission adopted a directive (Council Directive, 2. Experimental investigations
1999) limiting the mass concentration of PM10 in
the ambient air; a proposed new European Directive 2.1. General
seeks to limit the PM2.5 mass concentration in
ambient air. It is expected, however, that at present, Aerodynamic diameter dae, used to represent
strict limit values cannot be met in all areas of particle dispersion in gases, is defined as the
Germany and Europe (Second Position Paper on diameter of a particle with the same sedimentation
Particulate Matter, 2004) and therefore further velocity in gases as spheres from material of the
emission reduction measures will be required. For density 1 g cm3.
the implementation of such air pollution abatement The reference method for sampling and measure-
measures better data on fine dust emissions are ment of PM10 concentration (as well as a provi-
necessary than currently available. The past legisla- sional procedure for sampling and measurement of
tion had required only the control of total PM the PM2.5 concentration) in ambient air is laid down
emissions and so our knowledge of fine dust (Council Directive, 1999/30/EC). The method is
emissions is poor. based on the inertial separation of the PM10 particle
The results from a number of specific measure- fraction and its subsequent gravimetric determina-
ment programmes being conducted by the German tion. In this study, PM10 (and PM2.5) dust emission
Federal Environmental Agency and the German fractionation was carried out using cascade impac-
states were intended to improve the knowledge of tors, i.e. the same separation principle as used in the
fine dust emissions from different industrial and ambient air method. Cascade impactors are rela-
other sources. The presented study is based on tively simple to use for in situ sampling and avoids
results of measurement programmes in Saxony- agglomeration effects that might distort the particle
Anhalt (Landesamt für Umweltschutz Sachsen- size distribution. Impactors fractionate suspended
Anhalt, 2001), Bavaria (Bayerisches Landesamt für dust particles into different size categories according
Umweltschutz, 2000), Saxonia (Sächsisches Land- to their inertia. The basic components of an
esamt für Umwelt und Geologie, 1999) and the impactor are a nozzle and an impaction plate.
Federal Environmental Agency (Baumbach et al., When accelerated in the nozzle those particles
1999; Dreiseidler et al., 2001). These programmes having sufficient inertia strike the impaction plate
included measurements at industrial plants where and are collected. A cascade impactor contains
total dust emissions are relevant or contain toxic several impactor stages and particles are segregated
materials such as heavy metals. Thus, for example, as a function of decreasing inertia, so that samples
investigations were carried out at combustion plants of decreasing aerodynamic particle size are obtained
(brown coal, heavy fuel oil, wood), cement produc- stage by stage. The particles not retained by any of
tion plants, glass production plants, asphalt mixing the impactor stages are collected in a backup filter
plants, processing plants for natural stones and downstream of the impactor stages. The particle
sand, ceramic industry plants, metallurgy, chemical mass collected is determined by weighing each stage
plants, spray painting plants, wood processing/chip before and after sampling; the material collected can
drying, poultry farming and waste treatment plants. be used, when required, for further analyses e.g. on
In total, 106 measurement campaigns were under- dust composition. A pre-separator is necessary if
taken and 303 individual measurements were made. there is a large proportion of coarse particles
The first results have already been presented 4PM10 (Lützke and Muhr, 1981).
(Baumbach et al., 1999; Ehrlich et al., 1999, 2000;
Bayerisches Landesamt für Umweltschutz, 2000; 2.2. Sampling techniques
Dreiseidler et al., 2001). PM measurements were
also carried out at a small stove burning different The measurement campaigns used eight- or six-
kinds of fuel briquettes; since burning brown coal stage Anderson Impactors, type Mark III (material:
briquettes on household fireplaces remains common stainless steel) and/or a six-stage Stroehlein type
practice in the new German federal states and in the STF 1 impactor (material: Titanium). Preliminary
new EU Member States like Czech Republic, investigations showed that under similar sampling
 ARTICLE IN PRESS
6238 C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

conditions both impactor types showed comparable sampling periods. All measurements took place
particle size distributions in a range from 0.6 to during the process was operated normally. For each
16 mm for the various processes tested. Both measurement campaign the flue gas conditions
impactors are heat resistant up to 850 1C. Perforated (waste gas velocity, static pressure, temperature
collecting plates and glass–fibre backup filters were and water vapour content) were determined.
used for the particle separation. The sample gas flow
suction rate was determined using thermal mass 2.4. Quality assurance
flow meters.
All measurements were performed according to
2.3. Sampling and measurement the quality assurance measures specified in EN ISO/
IEC 17025 (2005). Thus, all pollutant emissions
The sampling and measurement was carried out were measured with standardized measurement
in accordance with VDI 2066 Bl. 5 (1994). In methods (VDI guidelines, DIN, EN) and officially
contrast to the total dust emission measurements, approved measurement instruments were used for
however, the gas flow through an impactor must be the determination of gaseous components. All plant
kept constant at all points of the sampling grid to operating and measured parameters were carefully
provide constant separation conditions in the documented using standardized report guidelines.
impactor. The volumetric flow rate only depends
on the waste gas conditions and can be calculated 3. Results
with special computer programs. Hence one mea-
surement can only cover sampling points with Tables 1–4 list the plants investigated, the
similar gas velocity (maximum acceptable deviation performance characteristics pertaining during the
is 730%), if the flow is not that homogeneous sampling periods, the fuels used, and descriptions of
several measuring operations are required. The the gas cleaning equipment and final results of PM
sampling period should be chosen such that percentage and total dust content (Landesamt für
sufficient PM mass is collected on each impactor Umweltschutz Sachsen-Anhalt, unpublished; Bayer-
stage to permit weighing with the required accuracy isches Landesamt für Umweltschutz, 2000; Baum-
without overloading the stages. bach et al., 1999; Ehrlich et al., 2000; Landesamt für
First, the existing emission concentrations of Umweltschutz, 2001; Sächsisches Landesamt für
total dust (according to EN 13284-1 (2001)) had Umwelt und Geologie, 1999; Dreiseidler et al.,
been determined in order to be able to specify 2001).
the required sampling times and suction rates for
the impactor samplings. Thus, on the one hand 4. Discussion
overloading of the impactor stages was avoided
and on the other hand sufficient PM masses could 4.1. General
be ensured to allow weighing with adequate
accuracy. Since, for the industrial plants examined, In the framework of this article it is not possible,
the total PM concentrations were usually low at the to present all results from 106 emission measure-
tested industrial plants, very long sampling times ment campaigns (see Tables 1–4) as particle size
(up to 18 h and in extreme cases 52 h) had to be distributions in diagrams, therefore in the following
provided to obtain an adequate filter loading. section typical particle size distributions of emission
By contrast, the high PM concentrations arising samples were selected, presented and discussed.
from domestic fire places required sampling times Nevertheless all obtained results were presented
that were substantially shorter than the time taken and assessed in Section 4.7 (Figs. 8–11).
for the complete burn cycle of the batch of fuel It is common practice to plot size distribution
used. Investigations proved, however, that most data in such a way that a straight line results. This
of the particle load was emitted in the first third assists in more detail data analysis, e.g. for reading
of the combustion cycle and so the impactor of essential parameters like PM10, PM2.5 or PM1.0.
measurements were carried out at this time of This can be done if the distribution fits a standard
higher emission. law. In this study the best fit with the experimental
The operating conditions of each installation data was gained using the cumulative frequency
were determined and documented during the particle size distribution (D) according to Rosin,
Table 1
Measurement results for combustion plants

No. Plant, maximum performance, fuel or basic input Samplings Performance during Dust separation Total dust in Mean value
material measurement period mg m3
(as thermal input) PM10 in % PM2.5 in % PM1.0 in %

Combustion plant/coal
1 Power plant, 180 MW, dry brown coal 3 180 MW ESP, scrubber 4.3 90.7 75.5 52.0

C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

2 Power plant, 146 MW, bcb limestone 3 114 MW ESP, FGD 4.6 92.0 74.0 47.7
3 Fluidized bed combustion, 119 MW, brown coal 3 114 MW ESP, FGD, NOx 14.4 97.0 65.7 25.5
4 Power plant, 1000 MW, pulverized hard coal 2 1000 MW ESP, FGD, NOx 0.9 88.4 69.2 51.3
5 Power plant, 1000 MW, pulverized hard coal 2 500 MW ESP, FGD, NOx 0.7 91.3 71.6 50.0

Combustion plant/heavy oil

ARTICLE IN PRESS
6 Combustion, 10 MW, heavy oil 3 5 MW Additive 44.4 98.0 81.9 64.3
7 Combustion, 10 MW, heavy oil 3 8.5 MW Additive 52.3 91.3 64.7 49.9
8 Combustion, 10 MW, heavy oil, urea 3 5 MW Additive, SNCR 56.7 97.1 77.5 55.8
9 Combustion, 10 MW, heavy oil, urea 3 8.5 MW Additive, SNCR 70.3 93.5 68.0 50.7
10 Combustion, 20 t h1 steam, heavy oil 3 9.7 t h1 steam SNCR 9.2 92.5 68.8 49.1
(output)
11 Combustion, 270 MW, heavy oil 3 270 MW NOx 45.8 87.1 71.1 63.2
12 Combustion, 270 MW, heavy oil 2 270 MW Additive, NOx 33.4 93.4 86.3 76.5
13 Combustion, 270 MW, heavy oil 2 200 MW NOx 26.8 96.5 88.9 76.3
14 Combustion, 270 MW, heavy oil 2 200 MW Additive, NOx 26.2 95.9 87.1 69.2

Combustion plant/wood
15 Grate firing, 1.4 MW, saw chips, saw dust 1 0.9 MW CC 194.0 98.6 70.4 49.0
16 Grate firing, 1.4 MW, saw chips, saw dust 1 1.3 MW CC 172.0 98.3 67.7 44.8
17 Grate firing, 0.8 MW, saw chips, saw dust 1 0.8 MW CC 251.0 98.3 62.6 36.0
18 Grate firing, 3 MW, hogged wood 1 1.3 MW CC 184.0 98.0 91.7 85.2
19 Underfeed stoker, 2.3 MW, rest of chipboards 3 1.3 MW Multi-CC 94.3 95.1 73.4 58.7
20 Grate firing, 1.1 MW, piece of wood, saw chips 1 1.0 MW CC 123.0 89.8 55.0 43.2
21 Grate firing, 2 MW, hogged wood, wood waste 1 1.5 MW ESP 27.0 89.2 67.1 62.4
22 Grate firing, 7.9-9.5 MW, wood, wood chips 1 5.8 MW ESP 23.0 73.5 53.6 46.3
23 Grate firing, 7.9-9.5 MW, natural gas, wood, chips 1 8.6 MW ESP 27.0 80.9 56.9 46.1
24 Grate firing, 15 MW, hogged and rest wood, chips 1 15 MW ESP 7.0 87.1 52.7 33.8
25 Grate firing, 1.5 MW, hogged wood 1 0.5 MW CGC, multi-CC 24.0 99.8 99.5 95.6
26 Grate firing, 1.5 MW, hogged wood 1 0.9 MW CGC, multi-CC 31.0 100.0 97.2 92.7
27 Power station, 31 t h1 steam, matured wood 3 27 t h1 steam CC, FF, NOx 19.9 80.2 31.4 13.8
(output)

6239
 6240
Table 2
Measurement results for cement, ceramic, glass industry

No. Plant, maximum performance, fuel or basic input Samplings Performance during Dust Total dust Mean value
material measurement period separation in mg m3
PM10 in % PM2.5 in % PM1.0 in %

Cement/furnaces
28 Rotary kiln, brown coal dust, waste oil 3 87 t h1 clinker (do) ESP horizontal 8.2 96.7 82.3 52.6
29 Rotary kiln, brown coal dust, waste oil 2 85 t h1 clinker (co) ESP horizontal n.m. 96.2 69.5 39.0
30 Lepol-kiln, raw meal, coal, waste oil, used tyre 6 41 t h1 clinker (do) ESP 15.1 92.4 50.1 39.2
31 Heat exchanger, raw meal, heavy oil, used tyre 6 118 t h1 clinker (do) ESP 2.3 99.4 75.2 42.9
32 Heat exchanger, raw meal, heavy oil, used-tyre 6 118 t h1 clinker (co) ESP 4.8 100.0 62.1 25.0

C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

33 Rotary kiln, brown coal dust, raw meal 2 334 t h1 clinker (do) ESP 3.5 95.5 78.2 41.6
34 Rotary kiln, brown coal dust, raw meal (1 mill) 4 325 t h1 clinker (co) ESP 7.1 89.9 56.4 25.4
35 Rotary kiln, brown coal dust, raw meal (2 mills) 2 287 t h1 clinker (co) ESP 12.9 90.9 49.2 24.5

Cement/cooler fabric filter

36 Grate cooler, clinker 3 72 t h1 clinker FF 3.4 43.3 3.8 1.2

ARTICLE IN PRESS
37 Gate cooler, clinker 3 72 t h1 clinker FF 21.1 23.6 2.6 0.6

Cement/cooler ESP, CC
38 Clinker cooler, raw meal, coal, waste oil, used tyre 6 41 t h1 clinker (co) ESP, multi-CC, CC 15.3 98.0 64.5 23.2

Glass industry/bath
39 Manufacture batch glass, cullet, batch, natural gas 6 223 t d1 Lime-sorption, ESP 3.0 95.3 53.5 21.2
40 Manufacture of flat glass, cullet, batch, natural gas 6 508 t d1 FGD (lime), ESP 5.1 93.2 44.8 23.7
41 Manufacture of goblets and beakers, bath, cullet, batch, 3 46 t d1 FF 0.8 93.4 53.3 37.7
natural gas

Glass industry /treatment

42 Manufacture of goblets and beakers, treatment, cullet, 2 46 t d1 FF 0.2 83.9 49.5 41.7
batch

Asphalt mix plant

43 Asphalt mix plant, asphalt granulate, oil 6 150 t h1 FF 19.0 93.1 29.2 8.3

Manufacture of porcelain/press
44 Isostatic compression press, porcelain substance 4 400 piece h1 FF 0.1 94.9 57.4 38.3

Treatment natural stone, sand

45 Crusher plant, lime stone, dolomite 3 600 t h1 FF 1.2 69.2 14.2 5.0
46 Screening plant, lime stone, dolomite 3 225 t h1 FF 10.9 59.2 5.9 1.2
47 Sand conditioning, natural sand 3 30 t h1 FF 6.2 68.7 11.9 2.9
48 Sand drying, cinder sand, heavy oil 1 30 t h1 FF 28.3 87.3 18.9 6.0
49 Preparation of ceramic raw materials, loam, clay, 3 Full load FF 0.8 80.4 34.4 16.5
porosity material

Tunnel oven ceramic industry

50 Oven (without additive), loam, clay, gas 1 Full load 5.3 93.9 85.0 79.7
51 Oven (with additive), loam, clay, gas, lime 3 Full load 3.4 95.4 88.6 84.9
 C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254
Table 3
Measurement results for metallurgy, chemical plants, spray painting and others

ARTICLE IN PRESS
No. Plant, maximum performance, fuel or Samplings Performance during Dust Total dust Mean value
basic input material measurement period separation in mg m3
PM10 in % PM2.5 in % PM1.0 in %

Metallurgy/melt
52 Converter, brass scrap, copper dross, cokey 3 59 t charge1 FF 2.4 96.3 76.3 51.3
53 Aluminium-remelt heat, natural gas, al-scrap 2 Without Reactor (lime), FF 0.2 98.5 72.0 35.8
information
54 Cupola, iron-scrap, coke, limestone 4 6.4 t h1 FF 7.1 87.9 43.8 19.8
55 Induction furnace, iron casting plant, iron-scrap 4 2.4 t h1 FF 0.4 77.4 48.6 18.1
56 Cupola, iron-scrap, coke 6 15 t h1 CC, scrubber, 58.3 95.4 88.1 72.4
57 Electric arc furnace, iron/steels scrap, aggregates 3 100 t h1 FF 4.6 96.1 58.1 24.6
58 Cupola, iron/steels scrap, cokey 1 16 t d1 FF 0.2 96.2 75.8 64.4

Metallurgy /drying, cooling

59 Drying plant, aluminium chips 2 1.8 t h1 Afterburning, FF 1.0 95.4 46.1 20.3
60 Drying plant, aluminium-chips 2 1.5 t h1 Afterburning, FF 0.4 98.4 52.9 32.8
61 Tunnel to cooling castings, castings, water 2 No information No information n.m. 94.6 42.7 23.2
62 Rotary screen, casting transport, castings 6 150 t/month FF 25.4 81.8 28.4 9.5

Metallurgy, treatment
63 Sand conditioning, pit-iron sand, betonite, coal dust 6 27–30 t h1 ESP 21.4 74.0 15.5 1.4
64 Sand conditioning wet casting, sand, betonite 2 20 t h1 FF 0.6 86.8 36.2 21.2
65 Treatment, moulding sand, consumable material 2 FF 4.1 91.9 39.7 20.6

Chemical plants/drying, furnace

66 Flow dryer A fabrication of acrylonitrile fibre, acrylonitrile 4 800 kg h1 CC, water injection 16.9 91.4 62.1 50.9
67 Flow dryer B fabrication of acrylonitrile fibre, acrylonitrile 6 800 kg h1 CC, water injection 8.9 83.9 48.6 17.4
68 Fertilizer dryer, fertilizer, heavy oil, carbon-monoxide 6 450 t d1 FF, packed scrubber 13.3 96.3 33.4 n.m.

6241
69 Spray dryer for drying resin, liquid condensation resins 6 0.65 m3 h1 FF 2.6 78.3 15.3 3.3
 6242
Table 3 (continued )

No. Plant, maximum performance, fuel or Samplings Performance during Dust Total dust Mean value
basic input material measurement period separation in mg m3
PM10 in % PM2.5 in % PM1.0 in %
1
70 Rotary dryer (bentonite), natural gas, podsol 3 2th FF 4.7 76.7 32.1 11.1
71 Run around dryer (bentonite), natural gas, podsol 3 3 t h1 CC, ESP 79.8 96.7 63.9 21.3
72 Milling dryer (bentonite), natural gas, bentonite, soda 6 9 t h1 ESP 3.3 95.2 49.9 11.8
73 Low-shaft electric arc furnace (manufacture of silicium), coal, 6 3.2 t h1 FF 1.2 92.8 45.4 24.9
charcoal, coke, chips

Chemical installations

C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

74 Urea prill processing, urea 2 45 t h1 80.0 97.0 68.5 15.5
75 Urea prill processing, urea 4 25 t h1 45.0 91.7 61.4 38.3
76 Fluid catalytic cracker carbon-monoxide, vacuum gas oil 6 160 m3 h1 Multi-CC, ESP 21.0 97.1 71.4 26.4
77 Fluid catalytic cracker, wax distillate, refinery residuals 6 100 t h1 ESP 2.7 90.2 57.7 19.3

Spray painting
About 400 kg d1

ARTICLE IN PRESS
78 Spray painting of automobiles, organic solvents 3 Venturi-washer 0.6 97.6 82.8 30.6

Wood working/shaving dryer

79 Rotating drum dryer, shavings 4 58 MW CC, FF 28.7 90.9 66.7 52.3
80 Chipping dryer, shavings, gas or oil 2 Full load ESP 2.1 99.2 92.8 87.5

Poultry farming
81 Floor keeping, fryer 6 14500 animals 6.2 60.6 8.2 1.0
82 Battery keeping, laying hen 4 15700 animals 3.1 36.5 2.7 0.4

Utilization of waste material

83 Old growth shredder, lumber, wood, timber waste 4 30 t h1 FF 4.5 92.6 16.7 11.5
Table 4
Measurement results for small-scale firing units

No. Plant, maximum performance, fuel or basic input Samplings Performance during Dust Total dust in Mean value
material measurement period separation mg m3
(as thermal input) PM10 in % PM2.5 in % PM1.0 in %

Small-scale firing units/coal

84 Household stove, 6 kW, LAUBAG-bcb (after cooling) 3 6 kW Without 20.5 93.4 85.4 76.6

C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

85 Household stove, 6 kW, LAUBAG-bcb (before 2 6 kW Without 13.2 91.6 84.1 75.7
cooling)
86 Household stove, 6 kW, MIBRAG-bcb (after cooling) 3 6 kW Without 56.4 95.9 83.5 63.8
87 Household stove, 6 kW, MIBRAG-bcb (before cooling) 3 6 kW Without 80.6 90.5 80.5 63.1
88 Household stove, 6 kW, Polish bcb (after cooling) 2 6 kW Without n.m. 95.8 80.8 65.0

ARTICLE IN PRESS
89 Household stove, 6 kW, Polish bcb (before cooling) 2 6 kW Without 66.2 93.5 77.0 63.3
90 Household stove, 6 kW, Bashkirian bcb 3 6 kW Without 147.8 91.3 80.8 70.6
91 Household stove, 6 kW, MIBRAG-bcb 3 6 kW Without n.m. 94.0 85.6 75.4

Small-scale firing units/wood

92 Firing plant, 175 kW, chips 1 177 kW CC 24.3 93.5 84.4 80.0
93 Firing plant, 175 kW, chip board 1 139 kW CC 75.1 98.5 86.2 79.8
94 Firing plant, 150 kW, chips 1 148 kW Without 23.2 95.1 72.1 66.9
95 Firing plant, 150 kW, chips 1 43.4 kW Without 22.3 99.6 93.8 86.9
96 Firing plant, 150 kW, joinery residues 1 133 kW Without 119.9 74.2 57.8 52.7
97 Firing plant, 150 kW, coloured pencil residues 1 112.5 kW Without 33.7 71.3 43.7 39.0
98 Firing plant, 450 kW, log wood 1 416.5 kW Multi-CC 56.7 100 96.5 89.0
99 Firing plant, 450 kW, log wood 1 273 kW Multi-CC 55.1 98.0 79.7 63.1
100 Small-scale firing unit, 9 kW, log wood beech 1 9.4 kW Without 78.0 98.9 95.8 92.8
101 Small-scale firing unit, 9 kW, log wood beech 1 7.5 kW Without 54.0 98.2 90.2 70.9
102 Small-scale firing unit, 9 kW, log wood pine 1 8.2 kW Without 47.0 98.9 95.2 91.8
103 Small-scale firing unit, 9 kW, log wood pine 1 6.8 kW Without 85.0 99.2 97.6 94.1
104 Chimney stove, 6 kW, log wood beech 1 5.7 kW Without 98.0 99.7 98.4 87.3
105 Chimney stove, 6 kW, log wood beech 1 4.1 kW Without 104.0 97.8 95.5 86.6
106 Pellet stove, 8.5 kW, wood pellets 1 8.0 kW Without 17.0 99.0 95.3 92.9

do ¼ direct operation, co ¼ compound operation, bcb ¼ brown coal briquette, SNCR ¼ selective non-catalytic reduction, ESP ¼ electrostatic precipitator.
n.m. ¼ no measurement, FGD ¼ flue-gas desulphurization, CGC ¼ chimney gas condensation, FF ¼ fabric filter, CC ¼ cyclone, NOx ¼ NOx removal.

6243
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6244 C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

Rammler, Sperling and Bennet (RRSB) (Batel, too: Y ¼ dR/d(log d) (R is the cumulative residue
1964). distribution, R ¼ 1–D) (Batel, 1964).
The RRSB function is well suited for particle
distributions arising from comminution processes, a 4.2. Coal-fired thermal power plants
common basic processes in a variety of the plants
investigated in this study. Another illustration Fig. 1(a) and (b) show the particle size distribu-
method is the depiction of the frequency distribu- tions of the emissions from various types of
tion (Y) over the PM diameter, which has been used pulverized coal-fired thermal power plants. In

99
90
cumulative frequency distribution [%]

50

20

10
5 Plant-No.
1
2
3
1 4
5
0.5

0.2 0.4 1 2 4 6 8 10 20
aerodynamic particle diameter d [ µm]

1.7

1.5

1.3
frequency distribution [-]

1.1

0.9
Plant - No.
0.7 1
2
0.5 3
4
5
0.3

0.1

0.1 0.5 1 5 10
aerodynamic particle diameter d [µm]

Fig. 1. (a) PM size distributions of thermal power plants (brown coal firing), RRSB cumulative frequency distribution; plant numbers
according to Table 1. (b) PM size distributions of thermal power plants (brown coal firing), frequency distribution; plant numbers
according to Table 1.
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C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254 6245

general a bi-modal particle size distribution appears shifted to around 2 mm (compared to 0.5–0.8 mm for
in the combustion processes (Szpila et al., 2003). the other coal combustion processes), the second
The density distribution in the Fig. 1(b) shows two maximum occurs around 6 mm for the fluidized bed
modes, one in the submicrometer range (0.5–0.8 mm) combustion. The shift of the fine-grained mode to a
and the other in the coarse range (5–10 mm). more coarser grain is probably related to an
In the flue gases of the fluidized bed combustion interaction of the bed material with the ash
(plant No. 3) the maximum of the fine portion is components (Szpila et al., 2003).

1.2

1.1
Plant -No.
1.0 6
7
0.9 8
frequency distribution [-]

9
0.8 10
11
0.7 12
13
0.6
14
0.5

0.4

0.3

0.2

0.1

0.1 0.5 1 5 10
aerodynamic particle diameter d [ µm]

Fig. 2. PM size distribution in flue gases of heavy oil firings, frequency distribution; plant numbers according to Table 1.

1.5
Plant-No.
28 do
29 co
frequency distribution [-]

30 do
31 do
1.0
32 co
33 do
34 co
35 co

0.5

0
0.1 1 5 10
aerodynamic particle diameter d [ µm]

Fig. 3. PM size distribution in flue gases of cement factories, frequency distribution; plant numbers according to Table 2.
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6246 C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

4.3. Heavy fuel oil firings measurement method; the coarser mode lies here
within the range of 2–3 mm.
The heavy fuel oil-fired combustion plants
investigated (Fig. 2) also show a bi-modal particle 4.4. Cement factories
size distribution. Here, the fine mode is strongly
shifted to the ultrafine range (smaller than 0.1 mm) Fig. 3 represents the particle size distributions in
and so it is not completely covered by the the clean gas of cement kilns. The large to very large

99
90
cumulative frequency distribution [%]

50

10

Plant - No.
36
1 37
38
0.5

0.4 1 2 4 6 8 10
aerodynamic particle diameter d [ µm]

2
frequency distribution [-]

1.5

1
Plant - No.
36
37
0.5 38

0
0.1 0.5 1 5 10 50
aerodynamic particle diameter d [ µm]

Fig. 4. (a) PM size distributions of cement clinker cooler plants, RRSB cumulative frequency distribution; plant numbers according to
Table 2 (plant Nos. 36 and 37: unexpected but proved results). (b) PM size distribution in flue gases of cement clinker cooler plants,
frequency distribution; plant numbers according to Table 2 (plant Nos. 36 and 37: unexpected but proved results).
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C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254 6247

portion (o3 mm) in the flue gas of the two rotary of particles from mechanical processes (e.g. raw
kilns (plant Nos. 28, 30, 31, 33) in direct (do) or mills) are contained in the flue gas and thus the fine
compound (co) operation is clearly to be seen. mode of 0.5 mm also shifts to 1.5–2 mm.
Moreover a little coarser particle size distribution Measurements show (Fig. 4(a) and (b)) that while
can be recognized in the compound operation (plant emitting lower concentrations of total PM (see
Nos. 29, 32, 34, 35). The bi-modal distribution Table 2), cement plants with grate cooler plants and
typical for thermal processes, is again well identifi- baghouse filters (plant Nos. 36 and 37) have a more
able. The compound operation means that portions pronounced coarse particle size fraction than that of

99
90
cumulative frequency distribution [%]

50

Plant - No.
10
84
85
86
87
1 88
89
0.5 90
91

0.4 1 2 4 6 8 10
aerodynamic particle diameter d [ µm]

2.0

1.8

1.6
frequency distribution [-]

1.4 Plant - No.

84
1.2
85
1.0 86
87
0.8 88
89
0.6 90
91
0.4

0.2

0
0.05 0.1 0.5 1 5 10 50
aerodynamic particle diameter d [ µm]

Fig. 5. (a) PM size distributions of small firing plants using brown coal briquettes, RRSB cumulative frequency distribution; plant
numbers according to Table 4. (b) PM size distribution in flue gases of small firing plants using brown coal briquettes, frequency
distribution; plant numbers according to Table 4.
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6248 C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

the plant with grate cooler and electrostatic raw gas PM concentrations in the clinker cooler
precipitator (plant No. 38). According to the (plant No. 38) are usually relatively low, defects in a
information supplied by the Research Institute of filter tube do not necessarily lead to high emission
the Verein Deutscher Zementwerke e.V. (1998) the concentrations. Furthermore it is documented in
reason for these coarse particles in the waste gases literature (Lützke and Muhr, 1981) relating to
of the plant Nos. 36 and 37 could be that porous baghouse filters that the dust quality may be
sites in the filter medium or leaks may, in addition, dependent on the interactions of the particles
allow coarser particles to pass the filter. Since the with the filter cake and associated agglomeration

99
90
cumulative frequency distribution [%]

50 Plant - No.
92
93
94
95
10 96
97
98
99
100
101
1 102
103
104
105
106

0.4 1 2 6 8 10
aerodynamic particle diameter d [ µm]

2.0
Plant - No.
1.8 92
93
1.6 94
95
96
frequency distribution [-]

1.4 97
98
1.2 99
100
1.0 101
102
103
0.8 104
105
0.6 106

0.4

0.2

0.1 0.5 1 5 10
aerodynamic particle diameter d [ µm]

Fig. 6. (a) PM size distributions of wood combustion plants, RRSB cumulative frequency distribution; plant numbers according to
Table 4. (b) PM size distribution in flue gases of wood combustion plants, frequency distribution; plant numbers according to Table 4.
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C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254 6249

phenomena, and thus coarser particles have been 4.5. Small-scale firing units
found in the clean gas.
These unexpected results of plant No. 36 were Figs. 5(a), (b), 6(a) and (b) typify the particle size
confirmed by repeated measurements taken half a distributions in the flue gases of small combustion
year later. The new data, at the same plant, also plants. The particle size distributions of the 9 kW
showed a further coarsening in the particle size furnaces fired with log wood (beech, spruce) (see
distribution (plant No. 37). Thus, the mean PM10 plants No. 100–103 in Figs. 6(a) and (b)) showed a
portion changed from 45% to 22%, in the mean greater proportion of fine particulates (see Table 4)
time the total dust content in the flue gas had also than briquette-fired plants of a similar capacity
increased from 3.4 to 21.1 mg m3. (plants No. 84–91 in Figs. 5(a) and (b)). The fine

1.4

1.2
frequency distribution [-]

1.0

0.8

0.6 Plant - No.

81
0.4 82

0.2

0.1 0.5 1 5 10
aerodynamic particle diameter d [ µm]

Fig. 7. PM size distribution in waste gases of poultry farming plant, frequency distribution; plant numbers according to Table 3.

circa 70 % of all PMx individual measurements

100
90
PM10
80
PMx - portion in %

70
60
50 PM2.5

40
30 PM1.0
20
10
0
0 50 100 150 200 250 300
sample number

Fig. 8. Schematic depiction of the PMx fraction of individual measurements—in descending order.
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6250 C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

particulate fraction, which extends into the ultrafine 4.6. Poultry farming plant
range, cannot be completely collected using the
measuring technique used here (VDI 2066 Bl. 5, Fig. 7 shows the PM size distributions of
1994). These fine and ultrafine particles are formed emissions from a poultry farm. The emissions from
from volatile exhaust components that condense eight barnstables with 14.500 broilers per stable
during cooling in the exhaust duct and deposit on were determined. Here the predominant influence
the surfaces of existing fine particles (such as soot) on PM formation is mechanical particle resuspen-
or form new particles. In the case of biomass sion rather than any thermal process. As might
combustion, wood in this case, volatile alkali therefore be expected the resultant distribution
compounds such as potassium salts are also present shows more coarse particles and is not bi-modal.
(Nussbaumer, 2003). The measurement results show that 50% of the
Wood combustion plants with larger capacity particles are larger than 10 mm (see Table 3).
(175 kW, plant Nos. 92–99, Figs. 6(a) and (b))
show distinctly coarser PM distributions. Here, it 4.7. Comparison of plant groups
would seem that coarser mineral ash com-
ponents carried away by highflow caused of the It is difficult to define PM10, PM2.5 and PM1.0
suction ventilators thereby enhancing the ‘‘coarse’’ profiles that are abatement technology specific.
mode. There are too many factors that might influence

Fig. 9. Portion of PM10 for all investigated plant groups.

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C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254 6251

particle size distributions and a limited number of ing to the levels of PM1.0, PM2.5 and PM10 portion
data is available to test possible relationships. The at the total dust. The result is shown in Fig. 8. It is
emitted PM spectra from the industrial processes evident that the majority of the plants investigated
tested showed a great variety. The most important emit dust with a high portion of fine particles; for
factor appeared to be whether the main process is more than 200 of the 303 individual measurements
thermal, mechanical or a mixed process. It is well (70%) the PM10 fraction accounted for greater than
known from the scientific and technical literature 90% of the total dust emitted.
that ultrafine particles (smaller than 0.1 mm) are Further evaluations were made of the individual
formed in thermal processes, due to sublimation or plant groups investigated, the results were arranged
condensation. On the other hand, particles formed according to the order given in the Annex of the
by mechanical processes can be expected to be IPPC-Directive (Council Directive, 1996) the re-
larger than 1 mm. In addition to these factors, the spective PM10, PM2.5 and PM1.0 values are repre-
particle size distributions in the exhaust gas of sented in box whisker diagrams—see Figs. 9–11.
combustion plants can also be influenced by: the A box indicates the range of the 25 and 75 percentile
firing and/or flue gas cleaning technologies, the fuel of the measured values and the biggest and smallest
type and the operating conditions (load/capacity) value of the measurement are indicated with a cross,
during the PM sampling period. The results a () indicates the 50 percentile.
(individual measurements) from all the plants tested Fig. 9 shows a PM10 portion in the total dust of
within the programme have been arranged accord- 490% for many plant groups (flagged area in

Fig. 10. Portion of PM2.5 for all investigated plant groups.

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6252 C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254

Fig. 9). Exceptions are: Grate cooler plant with stone and sand processing, poultry farming plant,
baghouse filters with the explained problems, drying, cooling, processing, recycling of waste,
natural stone and sand processing, poultry farming asphalt mixing plant exhibit low PM1.0 fraction of
plant. 0–30% (flagged area in Fig. 11). The third group,
The picture is different for the PM2.5 fraction of covering the small combustion plants (wood, brown
total dust emitted by the groups of plant under coal briquette), chip dryers and tunnel furnaces,
investigation: For most of the plant groups the exhibit very high levels of PM1.0 ranging from 60%
PM2.5 portion ranges between 50% and 90% to more than 90% of total dust.
(flagged area in Fig. 10). A PM2.5 portion of
2–50% has been determined for the more mechan- 5. Conclusion
ical processes such as natural stone and sand
processing, poultry farming plant, drying, cooling, For more than 70% of the individual emission
processing, recycling of waste and asphalt mixing measurements carried out at the industrial plants
plant. and at the domestic stoves, the PM10 portion
A different picture also results for the PM1.0 accounted for more than 90% of the emitted dust.
portion in the total dust too and three groupings The PM2.5 portion moves predominantly between
can be distinguished: For the thermal processes the 50% and 90% of the total dust. For the thermal
PM1.0 portion lies between 20% and 60% of the industrial processes the PM1.0 portion lays between
total dust. The mechanical processes such as natural 20% and 60% of the total dust.

Fig. 11. Portion of PM1.0 for all investigated plant groups.

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C. Ehrlich et al. / Atmospheric Environment 41 (2007) 6236–6254 6253

99.9
99.0 heavy oil

90.0 stove,lignite

cumulative frequency distribution [%]

wood briquette
combust.
50.0

Large combust. plant

10.0 chemical
5.0
cement

1.0
0.5 natural stone
poultry
RRSB - Diagram

0.1
0.5 1 5 10
aerodynamic particle diameter d [ µm]

Fig. 12. Schematic comparison of typical particle size distributions in the waste gases of thermal (- - - -) (wood combustion, lignite
briquette combustion, heavy oil combustion and large combustion plants), mechanical (      ) (poultry farming, natural stone
processing) and mixed processes (——) (cement factories, chemical plants).

The particle size distributions determined for determined emission factors for PM10, PM2.5 and
different plants can be clearly differentiated accord- PM1.0 are necessary. A contribution to that can be
ing to whether the emitting source is thermal, given by this article. Experimental determined emis-
mechanical or mixed as well chemical processes, sion factors for PM10, PM2.5 and PM1.0 are also very
see Fig. 12. Thermal processes according to Fig. 12 useful for establishing and revising of the ‘‘National
are small-scale firing units using wood or lignite Emission Ceilings Directive’’ of the European Com-
briquettes as fuel and large combustion plants mission (Directive, 2001/81/EC, 2001) regarding the
(heavy oil, coal); mechanical processes are natural Emission of primary particle fractions.
stone and poultry farming and mixed processes in
this context are chemical plants and cement Acknowledgment
factories.
Consequently, for the groups of plant investi- The authors wish to thank the Bavarian Environ-
gated, a major finding of this study has been that the mental Protection Agency and the Saxonian En-
particle size distribution is a characteristic of the vironmental and Geological Agency for taking their
technical process. Attempts to assign particle size measurement results.
distributions, of different plant, to different gas
cleaning technologies did not give usable results.
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