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Applied Energy
journal homepage: www.elsevier.com/locate/apenergy
h i g h l i g h t s
Blending butanol or pentanol with biodiesel changed the DPM characteristics.
The blends reduced EC and DPM emissions, but increased WSOC and OC fractions.
They reduced emissions of total particle-phase PAHs and also carcinogenic potential.
They showed different effects on counts of nanoparticles and lager particles.
a r t i c l e
i n f o
Article history:
Received 4 May 2015
Received in revised form 25 October 2015
Accepted 30 October 2015
Available online 18 November 2015
Keywords:
Diesel engine
Biodiesel
Higher alcohols
Particulate emissions
PAHs
a b s t r a c t
A systematic study was conducted to make a comparative evaluation of the effects of blending n-butanol
and n-pentanol with biodiesel at 10% and 20% by volume on engine performance and on the physicochemical characteristics of particulate emissions from a single cylinder, direct injection diesel engine.
The engine was operated at a constant engine speed and at three engine loads. Compared to biodiesel,
butanolbiodiesel blends lead to a maximum of 1.6% increase in the brake thermal efficiency (BTE)
and an increase in the brake specific fuel consumption (BSFC) by 1.93.9% at low and medium engine
loads. Pentanolbiodiesel blends result in an improvement in the BTE and a maximum of 2% increase
in the BSFC. Compared to biodiesel, both the blended fuels can reduce the particulate mass and elemental
carbon (EC) emissions, with butanol being more effective than pentanol. The blended fuels also show a
lower emission of total particle-phase polycyclic aromatic hydrocarbons (PAHs) and also a lower carcinogenic potential. However, the proportion of particulate-bound organic carbon (OC) and water-soluble
organic carbon (WSOC) are increased for the both blended fuels, especially for 20% butanol in blends.
The emissions of volatile and solid particles are reduced significantly in terms of their counts for both
kinds of blended fuels at medium and high engine loads, whereas the total particle counts for both
10% and 20% butanol in blended fuels are increased at low engine load due to a significant increase in
particles with diameter less than 15 nm.
2015 Elsevier Ltd. All rights reserved.
1. Introduction
Research on the use of sustainable and cleaner fuels in internal
combustion (IC) engines for both mobile and stationary applications continues to receive considerable attention because of the
motivation to reduce our dependence on conventional fossil fuels
and to mitigate environmental and health impacts [1]. Among
the proposed alternative fuels, biodiesel and alcohols are the most
widely investigated ones in diesel engines for reducing diesel fuel
consumption and toxic emissions [24]. Biodiesel is renewable,
nontoxic and readily biodegradable, has no aromatic compounds,
Corresponding author. Tel.: +65 65165135; fax: +65 67744202.
E-mail address: ceerbala@nus.edu.sg (R. Balasubramanian).
http://dx.doi.org/10.1016/j.apenergy.2015.10.173
0306-2619/ 2015 Elsevier Ltd. All rights reserved.
and possesses a high cetane number, high flash point and also
excellent lubricity performance [57]. It has been widely reported
that substantial reduction in hydrocarbon (HC), carbon monoxide
(CO) and diesel particulate matter (DPM) emissions can be
achieved through the application of biodiesel from various feedstocks in diesel engines [26]. Despite its many advantages, the
direct application of pure biodiesel, or the use of high percentage
of biodiesel in diesel blends may cause a poor atomization and
incomplete combustion, carbon deposits or clogging of fuel lines,
as well as thickening and gelling of the engine lubricating oil due
to its poor volatility and high viscosity [6,810]. These major drawbacks of biodiesel limit its proportion in diesel blends, typically
about 20% [10]. Apart from biodiesel, lower alcohols, mainly
methanol and ethanol, in combination with diesel fuel, have been
72
widely investigated for reducing the NOx and the particulate emissions [3,4]. However, some practical difficulties prevent their use
as fuels in diesel engines, such as reduced lower heating value
(LHV) compared to diesel fuel, miscibility and stability problems
when blended with diesel fuel, low cetane number, high autoignition temperature and poor lubricating properties [810].
Although several approaches have been attempted to resolve or
alleviate the problems, there are still some challenges when applying these lower alcohols into practical applications. For example,
on the one hand, immiscibility can be overcome by using emulsifiers to form a micro-emulsion with methanol or ethanol [9,10],
or by directly injecting them into the air intake [11]; both of these
alcohols could be combined with the preheating of intake air to
improve ignition and vaporization [9,10]. However, these processes require either skilled technical expertise, or complex engine
hardware modifications making these options unattractive for
practical applications. On the other hand, blending diesel with
methanol or ethanol with certain stabilization additives and cetane
enhancers seems to be preferred because of its simplicity with no
need to modify the existing engine. However, the percentage of
alcohols in diesel blends is usually restricted to 510%, and additives could be costly [9]. The use of higher alcohols such as butanol
and pentanol blended with diesel fuel in diesel engines has
recently drawn considerable research attention due to higher miscibility with diesel [1217]. However, the fuel properties such as
lubricity, viscosity, and cetane number of higher alcoholsdiesel
blends still need to be improved [12].
Blending of biodiesel with both lower and higher alcohols can
simultaneously overcome the above-mentioned disadvantages of
biodiesel and alcohols and has therefore been extended to their
application in diesel engines [5,710,1821]. For example, biodiesel and alcohols are miscible to some extent without any need
for an emulsifier or a co-solvent. In the blended fuels, the lower
viscosity and higher volatility of alcohols compensates for these
opposite properties in biodiesel. Likewise, the lower cetane number of alcohols could be improved with the simultaneous use of
the higher cetane value of biodiesel. Meanwhile, with the increased
amount of oxygen content in blends, complete fuel combustion can
be achieved. Extensive research has recently been carried out on
the use of various methanolbiodiesel and ethanolbiodiesel
blends in diesel engines [5,7,9,21]. From those previous studies,
it has become clear that methanol and/or ethanol blended with
biodiesel decreases NOx and DPM emissions while there are mixed
results in terms of CO and HC emissions depending on the relative
proportion of methanol or ethanol used as well as the engine operating conditions. Recently, Laza et al. [8] and Kumar et al. [18]
revealed that fuel properties such as lubricity, viscosity and cetane
number can also be improved by blending higher alcohols with
biodiesel. These blended fuels were more suitable for applications
in diesel engines than methanolbiodiesel or ethanolbiodiesel
blends. Subsequently, Tosun et al. [19] compared the effects of
blending 20% methanol, ethanol and butanol by volume with peanut methyl ester on fuel properties, engine performance, and
exhaust emissions. They concluded that butanolbiodiesel blends
showed higher engine power and torque, higher reductions of CO
emissions than both methanolbiodiesel blends and ethanolbiodiesel blends. Meanwhile, Yilmaz et al. [10], Kumar et al. [18]
and Rakopoulos [20] explored the effects of butanolbiodiesel
blends on diesel engine performance and exhaust emissions,
respectively. These studies revealed the beneficial effects of using
various blends of butanol with diesel fuel on CO, smoke and DPM
emissions at various engine loads.
There has been no systematic investigation on the quality of
engine emissions when being fueled with pentanolbiodiesel
blends, to the best of our knowledge. Meanwhile, the effect of
blending biodiesel with both butanol and pentanol on the physical
73
Properties
ULSD
Biodiesel
n-Butanol
n-Pentanol
Chemical formula
C (wt.%)
H (wt.%)
O (wt.%)
Sulfur content (mg/kg)
Lower heating value (MJ/kg)
Heat of evaporation (kJ/kg)
Density (kg/m3)@15 C
Viscosity (mPa s)@40 C
Cetane number
Flash point (C)
Boiling point (C)
Ignition temperature (C)
86.6
13.4
<10
42.5
250290
827
2.86
52
71
210235
200220
78
12
10
3.1
39.1
300
884
4.36
58
170
338
C4H9OH
64.9
13.5
21.6
33.1
585
810
2.22
17
35
117
343
C5H11OH
68.2
13.6
18.2
34.7
308
814
2.88
20
49
138
300
background air and in the diluted exhaust [11], using a nondispersive infrared analyzer (MRU VarioPlus, Germany, 0.5% accuracy). This measurement was done for every test, and all data presented in this article have been dilution-corrected to represent
engine-out conditions.
The first stage diluter was only used to cool the sampling gas
temperature below 52 C for particulate sampling. DPM emissions
from the first-stage diluter were collected onto 47 mm Teflon filters (Pall Life Sciences) and pre-combusted (650 C for 12 h)
47 mm quartz fiber filters (Whatman, USA), by using two MiniVol particulate samplers (Air metrics Ltd.; 5 L/min flow rate),
respectively. Particles collected on the Teflon filters were used
for gravimetric analysis, and for WSOC analysis, while those
collected on quartz fiber filters were processed for subsequent
OC/EC and PAHs analysis. Before and after sampling, the filters
were allowed to equilibrate in a humidity-controlled chamber at
a constant temperature and humidity (24 1 C, 30 8% RH), and
weighed using a microbalance (Sartorius MC5, accuracy of 1 lg)
for quantifying total particulate mass emissions. After being
weighed, the filters were kept in glass petri dishes and stored
under refrigeration at 20 C for the subsequent analysis.
The number concentrations and size distributions of volatile
and solid particles in the secondary dilution stage were measured
by a Fast Mobility Particle Sizer (FMPS, Model 3091, TSI Incorporated, USA) in the size range of 5.6560 nm. In this setup, two
diluters were used in series, with the first stage being heated by
a surface heater to 190 C in order to minimize thermophoretic
deposition. For the online measurement of the solid particle number concentrations, a thermodenuder (TD, Dekati Ltd) was placed
in-line between the secondary stage diluter and the FMPS. In the
TD, the volatile compounds of the particles were vaporized by
heating the sample aerosol, and were then gradually cooled and
adsorbed onto active charcoal so that they did not re-condense
onto the remaining solid particles. The temperature in the heating
section of the TD was maintained at 265 C. The TD diffusion losses
were estimated using the method of Surawski et al. [24] and the
diffusion loss-corrected particle size distributions are presented
in this article.
2.3. Carbon analysis
A DRI Model 2001A Thermal/Optical Carbon Analyzer (Atmoslytic Inc., Calabasas, CA, USA), following the IMPROVE TOR (thermal
optical reflection) protocol was used to quantify OC and EC fraction
of particles. In this method, eight carbon fractions can be defined
including OC1-OC4, OP and EC1-EC3. The method details, including
heating program and the determination of each carbon fractions
were described in [25]. For the measurement of water-soluble
74
25% Load
BSFC (g/kW.h)
520
a,b,c
a,b,c
a,c a,b,c
a
50% Load
BSFC
40
75% Load
a,b
a,b
c a,b,c
a,b,c a,b
c
a,c
a
a,c a,b a
390
35
BTE
30
a a,c a,c a a
25
260
130
a,b,c a,c
a a,c
a,c
BTE (%)
650
20
15
0
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
Test Fuel
Fig. 1. Brake specific fuel consumption (BSFC) and brake thermal efficiency (BTE).
a
Significantly different from the diesel fuel (p < 0.05); bSignificantly different from
the biodiesel (p < 0.05); cSignificantly different between butanolbiodiesel blends
and pentanolbiodiesel blends with the same proportion of them in blends
(p < 0.05).
addition of butanol and pentanol to biodiesel can result in the oxygen enrichment, the higher flame speed, the improved spray characteristics [1,7], and the longer ignition delay associated with their
lower cetane number [20], which could enhance the combustion
process and therefore increase BTE. On the other hand, the higher
latent heat of evaporation of butanol could lower the combustion
temperature and reduce the BTE, especially at lower engine load
with high proportion of them in blends. Compared to butanol,
pentanol has lower latent heat of evaporation, and is therefore less
affected by the variation of combustion temperature. The integrated result shows that the butanol addition only slightly
increased the BTE at high engine loads with 20% butanol addition,
while the pentanol addition shows a slight increase in the BTE for
all tested conditions. Overall, the results on the engine performance indicate that pentanoldiesel blends show less variations
in BSFC and a slightly higher BTE, and are therefore more suitable
for applications in diesel engines compared to butanoldiesel
blends.
3.2. DPM and carbonaceous matter emissions
In this study, the particulate mass emissions, and carbonaceous
matter in particles, including EC, OC, and WSOC were determined,
based on which the ratios of OC/EC and WSOC/OC were calculated.
As shown in Fig. 2, for each fuel, the EC emission factor sharply
increases while the OC and WSOC emission factors generally
decreases with an increase in engine load, resulting in the
decreased OC/EC ratios with engine load. Compared to diesel fuel,
the EC emission factors for biodiesel decrease by 51.3%, 50.3% and
43.1% from low to high engine load. Both the butanol and pentanol
addition to biodiesel result in a further decrease in the EC emissions for all tested conditions. Similar results in smoke or particulate mass reduction were reported for methanolbiodiesel and
ethanolbiodiesel blends [3,5], and for butanolbiodiesel blends
[18,19]. Moreover, with the same proportion of butanol or pentanol in blends, the EC emission reduction for butanolbiodiesel
blends is generally higher than that obtained from pentanolbiodiesel blends, especially at higher engine load with a higher proportion of them in the blended fuels, as shown in Fig. 2(a). For
example, compared to B100, the reduction of EC emission factors
at different proportions of butanol in the blends is 28.555.4%,
28.654.2% and 11.438.7%, respectively from low to high engine
load. However, for pentanolbiodiesel blends, the corresponding
decreases are 23.739.2%, 21.623.5% and 7.19.8%, respectively.
These findings reveal that butanol has higher potential to inhibit
soot emissions than pentanol.
The variation of OC emissions was different from that of EC,
which seems to be associated with the engine load, the type of
alcohols used and the proportion of them in blended fuels. At
low engine load, the OC emissions for biodiesel and for its blends
with alcohols show no significant differences from those for the
diesel fuel. At medium and high engine loads, the OC emission factor for biodiesel is slightly lower than that for diesel fuel. Meanwhile, when compared to B100, the OC emission factors for
B80Bu20 and B80P20 are further reduced by 8.0% and 6.9% at medium engine load, and by 4.7% and 11.4% at high engine load, respectively. The results reveal that the blending of higher proportion of
butanol or pentanol with diesel is effective at reducing OC emissions at higher engine load. It is further observed that at high
engine load, the OC emission factor for B90Bu10 is slightly lower
than that of B90P10, while the OC emission factor for B80Bu20 is
slightly higher than that of B80P20. In other cases, the same proportion of butanol and pentanol in blended fuels results in a similar
emission level of OC.
The results from this study indicate that biodiesel and higher
alcoholsbiodiesel blends are more effective in inhibiting EC
75
400
75% Load
50% Load
25% Load
EC
320
240
a
160
a,b,c
a,b,c
a,b,c
a,b,c
80
a
a,b,c
a,b,c
a,b,c
a,b,c
a,b,c
a,b,c
a,b,c
a,b,c
(b)
OC Emission Factor (mg/kW.h)
(a)
900
25% Load
OC
b
720
540
a a a
360
a a,c
50% Load
WSOC
a
a
a
a
150
100
aa a a
a
a a
a,b,c
a,c
50
75% Load
a,b
200
1200
25% Load
1000
800
50% Load
DPM mass
600
a,b,c
a,b,c
a,b,c
a,b,c
200
0
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
75% Load
(f)
0.40
25% Load
75% Load
50% Load
OC/EC
WSOC/OC
0.32
a,b
a,b
WSOC/OC
a a
OC/EC
400
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
50% Load
a,b,c
27
Test Fuel
45
36
75% Load
a,b,c
a,b,c
a,b
a,b
Test Fuel
25% Load
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
(d)
25% Load
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
Test Fuel
250
a,b,c
a,b,c
a,b,c
18
a,c
a,b,c
a,b,c
180
Test Fuel
(e)
a,b a,b
(c)
75% Load
50% Load
a,b
0.24
a a
a,b,c
a,b,c
a,b
a
a,b,c
a,b,c
0.16
a,b,c
9
a
a,b a,b
a,b,c
0.08
a,b,c
a,b
a a,b
a,b,c
0.00
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
Test Fuel
Test Fuel
Fig. 2. Emission of carbonaceous species (a) EC (elemental carbon), (b) OC (organic carbon), (c) WSOC (water-soluble organic carbon), and (d) DPM (diesel particulate matter)
mass, and the ratios of (e) OC/EC and (f) WSOC/OC. aSignificantly different from the diesel fuel (p < 0.05); bSignificantly different from the biodiesel (p < 0.05); cSignificantly
different between butanolbiodiesel blends and pentanolbiodiesel blends with the same proportion of them in blends (p < 0.05).
76
77
a
b
c
MMW-AHs
HMW-PAHs
Total-PAHs
Total-BaPeq
55.3 13.4
13.1 5.6a
6.8 2.2a,b
5.9 1.5a,b
4.8 0.3a,b
4.4 1.0a,b
414.5 66.9
341.3 31.4
291.4 20.7a,b
305.1 38.4a
140.2 20.3a,b,c
233.1 25.0a,b,c
21.3 4.6
5.0 1.8a
2.6 0.8a,b
2.4 0.5a,b
1.5 0.2a,b
1.6 0.3a,b
25% load
D100
B100
B90Bu10
B90P10
B80Bu20
B80P20
103.8 24.8
25.9 11.2a
18.1 4.0a,c
42.1 6.5a,b,c
20.4 9.3a,c
34.4 10.2a,c
255.5 28.7
302.2 14.6a
194.6 14.5a,b,c
257.0 30.4b,c
114.8 10.7a,b,c
194.3 13.8a,b,c
50% load
D100
B100
B90Bu10
B90P10
B80Bu20
B80P20
68.4 13.4
22.0 5.1a
12.5 1.6a,b,c
34.5 5.9a,b,c
15.0 4.9a,c
23.9 5.0a,c
255.1 14.2
260.0 17.7
145.1 17.4a,b,c
223.4 11.4a,b,c
87.6 7.4a,b,c
158.8 17.1a,b,c
17.3 3.9
8.6 1.9a
3.1 0.5a,b
2.7 0.4a,b
2.5 0.2a,b
2.7 0.5a,b
340.9 31.5
290.6 24.7
160.8 19.5a,b,c
260.5 17.6a,b,c
105.0 12.4a,b,c
185.4 22.5a,b,c
10.0 2.2
3.4 0.6a
1.4 0.2a,b
1.4 0.2a,b
1.1 0.1a,b
1.3 0.2a,b
75% load
D100
B100
B90Bu10
B90P10
B80Bu20
B80P20
80.3 7.4
21.2 4.1a
16.6 1.5a,c
33.6 2.5a,b,c
24.5 1.7a,c
31.0 4.2a,b,c
384.0 11.3
338.2 7.6a
237.6 8.0a,b,c
266.6 14.5a,b,c
181.9 13.6a,b,c
221.6 13.4a,b,c
12.1 1.6
6.9 1.2a
5.1 0.9a,b,c
3.9 0.4a,b,c
5.1 0.8a,b,c
3.4 0.2a,b,c
476.4 20.3
366.3 12.9a
259.3 10.4a,b,c
303.8 17.5a,b,c
211.4 16.1a,b,c
256.0 17.8a,b,c
6.6 0.7
3.1 0.4a
2.2 0.3a,b
2.2 0.2a,b
1.8 0.3a,b
1.5 0.1a,b
(a)
5x10
25% Load
4x10
3x10
2x10
1x10
D100
B100
B90Bu10
B90P10
B80Bu20
B80P20
0
10
100
Diameter (nm)
7
6.4x10
4.8x10
3.2x10
1.6x10
(b) 8.0x10
50% Load
D100
B100
B90Bu10
B90P10
B80Bu20
B80P20
0.0
10
100
Diameter (nm)
(c)
2.0x10
75% Load
1.6x10
1.2x10
8.0x10
4.0x10
D100
B100
B90Bu10
B90P10
B80Bu20
B80P20
0.0
10
100
Diameter (nm)
Fig. 3. Volatile (without TD) PN (particle number) size distributions.
9.0
7.2
a,b,c
75% Load
Dp>100 nm
Dp=50-100 nm
Dp=15-50 nm
Dp<15 nm
a,b,c
a
5.4
50% Load
25% Load
a,c
b,c
a
a
a,b,c
a,c
a,b,c
a,b,c
3.6
a,b,c
a,b,c a,b,c
a,b,c
1.8
0.0
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
78
Test Fuel
Fig. 4. Size-segregated volatile particle number emissions and GMD (geometric
mean diameter). aSignificantly different from the diesel fuel (p < 0.05); bSignificantly different from the biodiesel (p < 0.05); cSignificantly different between
butanolbiodiesel blends and pentanolbiodiesel blends with the same proportion
of them in blends (p < 0.05).
35.9 1.3
29.9 1.0
21.2 1.6
22.3 1.4
17.7 0.6
19.4 0.8
a
a,b,c
a,b,c
a,b,c
a,b,c
50% load
75% load
56.0 1.8
46.2 1.6a
44.6 1.7a,b
44.6 0.8a,b
43.4 1.5a,b
43.9 0.7a,b
74.4 2.7
59.3 1.8a
57.4 1.5a,b,c
58.3 1.6a,b,c
54.3 1.9a,b
54.6 2.3a,b
79
Acknowledgements
20
50% Load
75% Load
References
6
16
Solid PN
5
Solid PA
4
3
a,b,c
a,b,c a,b,c
a,c
a
1
a,c
a,b
a,b
a,b,c
a,b,c
a a,ba,b a,b,c
a,b,c
a a,c a a,b
a a,b,c
a,b,c a,ba,b
12
a a,ba,ba,ba,b
25% Load
0
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
B80P20
B80Bu20
B90P10
B90Bu10
B100
D100
Fuel Type
Fig. 5. Solid PN (particle number) and solid PA (particle area) concentrations.
a
Significantly different from the diesel fuel (p < 0.05); bSignificantly different from
the biodiesel (p < 0.05); cSignificantly different between butanolbiodiesel blends
and pentanolbiodiesel blends with the same proportion of them in blends
(p < 0.05).
4. Conclusions
The following major conclusions were drawn from this preliminary study.
(1) Compared to biodiesel, butanolbiodiesel blends show a
maximum of 1.6% increase in the brake thermal efficiency
(BTE) and a 1.93.9% increase in the brake specific fuel consumption (BSFC) at low and medium engine loads. Pentanolbiodiesel blends result in an improvement in the
BTE and a maximum of 2% increase in the BSFC.
(2) Compared to biodiesel, both the blended fuels can effectively
reduce the elemental carbon (EC) and particulate mass emissions, with butanol being more effective than pentanol. The
blended fuels also reduce OC emissions at higher engine
loads with higher proportion of them blends. However, the
blends increase the OC and WSOC fraction in particles, especially for 20% butanol in the blended fuels at low engine
load.
(3) Compared to biodiesel, the addition of both butanol and
pentanol show lower emissions of total particle-phase PAHs
and also lower carcinogenic potential.
(4) Both of the blended fuels can effectively reduce in the total
volatile number emissions at medium and high engine loads.
The reduction of the total particle counts is mainly caused by
the reduction of solid particle emission in the cylinder, and
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