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Fuel
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Department of Environmental Engineering, National Cheng Kung University, Tainan City 70101, Taiwan, ROC
Sustainable Environment Research Center, National Cheng Kung University, Tainan City 70101, Taiwan, ROC
Center for Combustion Energy and State Key Laboratory of Automotive Safety and Energy, Tsinghua University, Beijing 100084, China
d
Department of Mechanical Science and Engineering, University of Illinois at Urbana Champaign, IL 61801, USA
e
Department of Chemical Engineering and Materials Engineering, National Ilan University, Ilan City 26047, Taiwan, ROC
b
c
a r t i c l e
i n f o
Article history:
Received 7 October 2010
Received in revised form 15 November 2011
Accepted 17 November 2011
Available online 3 December 2011
Keywords:
Butanol
Biodiesel
NOx
PAHs
Carbon dioxide
a b s t r a c t
Three groups of n-butanoldiesel blends with 0, 0.5, and 1.0 wt.% water-content were investigated to
simulate the hydrated butanol produced by acetonebutanolethanol fermentation and a simple distillation treatment. Both 30-day standing and centrifugal test results showed that 15 wt.% n-butanol (BT)
was the minimum additive ratio to stabilize the 1.0 wt.% water content diesel blend, while those blends
that contained 0 or 0.5 wt.% water could remain as stable one-phase clear liquids by adding just 5 wt.%
BT. These stable diesel blends were further examined in a heavy-duty diesel-fueled engine generator
(HDDEG). Using BT-diesel blends increased the indicated specic fuel consumption (ISFC) because of
the lower heating value of n-butanol, while the micro-explosions that occurred could reduce the ISFC
when using 0.5 wt.% water-containing BT-diesel blends. NOx emissions increased with the increasing
BT content at a low additive ratio (515 wt.%), and reduced when adding a higher amount of BT
(>15 wt.%). PM, total-PAHs, and total-BaPeq emissions were all signicantly reduced when the increasing
BT additive ratio contained either 0, 0.5, or 1.0 wt.% water because of the lower sulfur and higher oxygen
fuel contents. On the other hand, the CO emission level went up with the addition of BT. Notably, the diesel blends with 0.5 wt.% water only slightly increased ISFC when low fractions of BT were added, i.e. 0.40%
and 0.81% ISFC increases with the addition of 5 and 10 wt.% BT, respectively. In addition, there were signicantly lower NOx, PM, Total-PAHs and Total-BaPeq, emissions with the blends than with regular diesel.
With the aim of achieving both good energy performance and less pollutant emissions, the 5 and 10 wt.%
BT additive with 0.5% water content blends were the most suitable for practical use in an HDDEG without
any engine modications or changes in controls.
2011 Elsevier Ltd. All rights reserved.
1. Introduction
Since Diesel invented the rst compression-ignition engine in
1892, both researchers and manufacturers have worked to make
such engines operate with greater thermal efciency, higher output power, and lower emissions of carbon monoxide (CO) and unburned hydrocarbon (HC). However, the sharply increasing price of
crude oil and dwindling reserves over the last few decades [1]
show the dangers of over-dependence on fossil fuels. Additionally,
the emissions of particulate matter (PM), sulfur dioxide (SO2),
Corresponding authors. Address: Department of Environmental Engineering,
National Cheng Kung University, Tainan City 70101, Taiwan, ROC. Tel.: +886 6 2757
575x65831; fax: +886 6 275 2790 (S-L. Lin).
E-mail addresses: cbmsgml@gmail.com (S.-L. Lin), wjlee@mail.ncku.edu.tw
(W.-J. Lee).
0016-2361/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2011.11.042
nitrogen oxides (NOx) and polycyclic aromatic carbons (PAHs) released when burning such fuels cause environmental and public
health problems [24], as well as being associated with global
warming due to the inuence of greenhouse gas (GHG) emissions,
especially carbon dioxide (CO2). Therefore, developing cleaner and
renewable energy sources has become a pressing concern.
Biodiesel and bioethanol are the two most popular renewable
and oxygenated fuels currently in use. As extracting fuel from
crops is more environmentally friendly and CO2 conservative than
petroleum processing, several processes have been developed to
transform neat vegetable oil into biodiesel with similar properties
to those of a regular diesel. The transesterication process is the
most practical one, with high production yields of around
8095% and the ability to signicantly decrease the viscosity of
neat vegetable oil [5]. In a study on biodiesel emissions, Scholl
and Sorenson [6] reported that CO, unburned HC, NOx, and smoke
365
2. Experimental section
2.1. Fuel preparations and stability tests
A premium diesel fuel (D100) produced by Chinese Petroleum
Corporation (CPC) was used as a base fuel in current study. Analytical-grade n-butanol (BT) obtained from J.T. Baker (>99.5% purity)
was utilized to simulate the bio-butanol produced by ABE fermentation. Additionally, to simulate the dehydrated butanol treated by
a simple distillation separation process after ABE fermentation, the
water contents were xed at 0.5 and 1.0 wt.%, while the butanol
additive fractions were varied from 5 to 10, 15, 20, and 25 wt.%.
217 wt.% (0.5/25.51/6) water-containing butanol blends were
investigated in the current study. The hydrated butanoldiesel
blends were prepared by adding the specic ratios of water into
the pure n-butanol, and then blending the hydrated butanol with
a conventional diesel by employing a lab-scale 1-L mixer with
3000 rpm for 15 min. The premixed products were then homogenized in an ultrasonic tank at 40 kHz and 120 W ultrasonic power
output for 15 min. The products were then tested for their stability.
The stability of the diesel blends was examined by two gravitational and centrifugal tests. In the gravitational test, the appearance of each diesel blend was recorded after standing for 30 days
at 25 C to determine the one-month-storage stability. Furthermore, a centrifugal stability test was conducted at 5000 rpm for
15 min to predict the stability changes of diesel blends after longer
term storage. After the two stability tests, the four levels of the
phase appearances of the blended fuels formed an empirical index
of stabilities: (a) one-phase clear liquid; (b) one-phase liquid crystalline; (c) two-phase liquid crystalline; (d) two-phase clear liquid.
The order of stability is (a) > (b) > (c) > (d), so that an unstable
blend will transform its appearance from (a) to (d) over time.
366
Table 1
Recovery rates and compositions of acetone butanol ethanol solution using C. acetobutylicum and/or C. beijerinckii in ABE fermentation.
References
Acetone
Butanol
Ethanol
1
1
1
gL
wt.%
gL
3.326.12
5.327.4
5.20
4.024.1
3.74
4.60
25.343.6
29.236.1
29.5
22.032.2
31.3
23.0
8.2412.8
11.946.4
11.9
13.456.2
7.40
14.1
ISFC V=Pt mL kW
1
IE Pt=VH %
1
2
where V represents the fuel consumption (mL) during each sampling time, P stand for the power generated (kW) by the dieselfueled engine generator with 110 V, t represents the sampling time
(h) and H stands for the heating value of each diesel blend.
Table 2
Specications of the tested diesel fueled engine.
Specications
Manufacturer
Type
Bore Stroke
Displacement volume
Rated engine speed
Output power
Torque
Ignition system
Injection type
Injection timing
Injection pressure
Lubrication system
Cooling system
wt.%
gL
55.773.9
61.169.5
67.6
63.273.6
62.0
70.5
0.000.51
0.32.1
0.50
0.61.1
0.79
1.30
Total ABE
wt.%
g L1
wt.%
0.002.74
1.272.82
2.80
1.234.60
6.62
6.50
12.219.2
17.775.9
17.6
18.281.3
11.9
20.0
100
100
100
100
100
100
367
lines of the 21 PAH compounds ranged from 0.995 to 0.999. Additionally, the results showed the average recovery (n = 3) of individual PAHs by NIEA A730.70C was 80114%. Analysis of eld blanks,
including glass-ber lters and cartridges, showed all PAH levels
were less than the DL.
The 21 individual PAHs were divided into low-molecular
weights (LM-PAHs containing two- and three-ring PAHs), midmolecular weights (MM-PAHs containing four-ring PAHs), and
high-molecular weights (HM-PAHs containing ve- to seven-ring
PAHs) due to their different physical and chemical properties.
The total-PAH data in the exhaust of a diesel-fueled engine was
the sum of the 21 individual PAHs. The overall toxicity was dened
as the sum of Benzo[a]pyrene equivalent (total BaPeq), which was
each PAH concentration multiplied by its toxicity equivalent factor
(TEF).
Table 3
Blending processes and stability tests of WBTD blends.
Blends
W0.5
BT25W0.5
BT20W0.5
BT15W0.5
BT10W0.5
BT5W0.5
BT25W1
BT20W1
BT15W1
BT10W1
BT5W1
BT6W0.6
BT7W0.7
BT8W0.8
BT9W0.9
n-Butanol (wt.%)
0.0
25
20
15
10
5
25
20
15
10
5
6
7
8
9
Water (wt.%)
0.5
0.5
0.5
0.5
0.5
0.5
1.0
1.0
1.0
1.0
1.0
0.6
0.7
0.8
0.9
Blending processes
Stability tests
Water/butanol (wt.%)
After stirring
After ultrasonic
After 30 days
Centrifuge
2-Clear
O
O
O
O
O
O
Bubbles (1%)
O
2-crystalline
2-crystalline
1-crystalline
1-crystalline
1-crystalline
2-crystalline
2-Emulsion
O
O
O
O
O
O
O
O
2-emulsion
2-emulsion
1-emulsion
1-emulsion
1-emulsion
2-emulsion
2-Clear
O
O
O
O
O
O
O
O
2-emulsion
2-emulsion
1-emulsion
1-emulsion
1-emulsion
2-emulsion
2-Clear
O
O
O
O
O
O
O
O
2-clear
2-clear
2-clear
2-clear
2-clear
2-clear
2.0
2.5
3.3
5.0
10
4.0
5.0
7.0
10
20
10
10
10
10
368
Table 4
Fuel properties of each diesel blend.
Blends
Density
Kinetic viscosity
Heating value
D
B5
B10
B15
B20
B25
B5W0.5
B10W0.5
B15W0.5
B20W0.5
B25W0.5
B15W1
B20W1
B25W1
0.830
0.829
0.828
0.827
0.826
0.825
0.830
0.829
0.828
0.827
0.826
0.829
0.828
0.827
4.152
3.191
3.241
3.292
3.342
3.393
3.180
3.231
3.281
3.332
3.382
3.270
3.321
3.372
41.66
41.23
40.80
40.37
39.94
37.86
41.02
40.59
40.16
39.73
37.65
39.96
39.53
37.44
Fig. 1. ISFC (a) and IE (b) of three different water content groups of tested diesel
blends.
Fig. 2. Nitrogen oxide emissions (a) and exhaust gas temperatures (b) of three
different water content groups of tested diesel blends.
369
the highest NOx producer with the pure BT-diesel blend (BT20).
The reason why the changing blended ratio emitted the highest
NOx concentration was that the existence of 0.5 wt.% water provided extra latent heat and retarded the ignition time, so that it
partially approached low-temperature combustion and inhibited
thermal NOx formation [45]. The exhaust temperatures when
using BT20 (539 K) and BT15W0.5 (540 K) were almost the same,
as shown in Fig. 2b, and this could be the critical factor with regard
to thermal NOx formation. Additionally, the 1.0 wt.% water content
BT-diesel blends were too unstable in 5 and 10 wt.% BT ratios to
test in the engine. Thus in the group with 1.0 wt.% water,
BT15W1 had the highest NOx emissions and this was reduced to
the overall lowest NOx emissions of 65 ppm in the three groups
of diesel blends, 35.5% lower than that of D100, by adding
25 wt.% BT to the blends. Consequently, the 1.0 wt.% water content
could effectively cool the combustion system and inhibit thermal
NOx formation; however, the signicantly higher ISFC of BT25W1
is a major obstacle to practical use. On the other hand, BT5W0.5
had a minimal ISFC increase (+0.44%) and also a signicant NOx
reduction (22.5%), and thus might be a more suitable alternative
diesel blend. Since the injection timing was xed in this HDDEG,
the increasing NOx levels by using low BT additive ratios could
not be avoided because of their higher oxygen content. Tests of
retarding injection timing are suggested in future studies, because
the retarded injection will provide a more premixed air condition
and absorb more heat from the compression stroke. NOx emissions
are thus expected to be reduced with the lower peak temperature
in the cylinder; however, the increase in ISFC will then become another problem. Low levels of BT addition are thus the better choices
when retarding the injection timing, because of their lower increase in ISFC.
3.4. PM and CO emissions
Particulate matter (PM) is a harmful pollutant with regard to
the respiratory system and generally forms by three modes: (1)
nucleation, (2) accumulation/condensation, and (3) coalescence.
In the current study, the amount of n-butanol added had a positive
effect in reducing PM (Fig. 3a). These trends could be due to the
increasing oxygen contained in the BT additive, which further enhanced the oxidation reactions, as supported by the results of a
ethanol-diesel blend investigation conducted by Lapuerta et al.
[46]. Additionally, the decrease in sulfur content of the diesel
blends when adding more sulfur-free additive (n-butanol) could
also inhibit the formation of sulfuric acid, which has been reported
to form PM by accumulating or condensing on the soot or metallic
ash in exhaust gas at a lower temperature than with the in-cylinder conditions [4749]. The PM emissions of the highest BT containing blends (BT25, BT25W0.5, and BT25W1) were 94, 52, and
88 mg Nm3, representing 31.2%, 61.9%, and 35.4% reductions from
that of D100 (135 mg Nm3), respectively. According to the above
sulfur-altered mechanism, BT25W1 should have the lowest PM
level instead of BT25W0.5. This unexpected result might be caused
by the micro-explosion mechanism, which could reduce the formation of nuclei (soot) and enhance the ISFC at the same time
[4244]. Nevertheless, the sulfur content of the tested diesel was
less than 50 ppm, which would lower the effect of the sulfur-altered mechanism to reduce PM, and the regulations regarding sulfur content are now becoming stricter, e.g. a limit of 10 ppm sulfur
came into effect in Europe in 2011. Thus, the mechanism of microexplosions dominates the PM reductions for different water additive ratios. Unfortunately, the PM emissions increased again by
increasing the water content to 1 wt.%, which might be because
the cooling effect retarded the soot oxidization and promoted the
condensation pathway to form PM. Consequently, 0.5 wt.% water
addition is a more efcient approach to reducing PM.
Fig. 3. Emissions of particulate matter (a) and carbon monoxide (b) of three
different water content groups of tested diesel blends.
370
Table 5
PAH emission concentration of water-containing butanoldiesel blends.
a
b
c
d
e
D100
(n = 2)
BT5W0.5
(n = 2)
BT10W0.5
(n = 2)
BT15W0.5
(n = 2)
BT20W0.5
(n = 2)
BT25W0.5
Mean
TEFsa
Nap
AcPy
Acp
Flu
PA
Ant
FL
Pyr
CYC
B(a)A
CHR
B(b)F
B(k)F
B(e)P
B(a)P
PER
IND
DBA
B(b)C
B(ghi)P
COR
P
LM-PAHsb
P
MM-PAHsc
P
HM-PAHsd
Total PAHs
Total BaPeqe
72.5
7.81
3.73
20.7
249
9.19
12.6
31.6
0.82
1.25
1.26
1.33
1.68
0.06
0.17
0.02
0.12
0.03
0.06
0.07
0.02
363
48.9
2.24
415
1.14
69.0
7.01
3.35
19.5
232
8.19
10.9
30.0
0.78
1.15
1.18
1.24
1.60
0.06
0.15
0.01
0.11
0.02
0.06
0.05
0.02
339
45.3
2.08
387
1.05
68.2
6.81
3.00
19.3
229
8.57
10.5
29.7
0.79
1.16
1.18
1.25
1.61
0.05
0.15
0.02
0.09
0.02
0.05
0.05
0.02
335
44.6
2.07
382
1.05
66.8
6.73
2.72
19.1
216
5.76
10.0
29.0
0.81
1.18
1.22
1.11
1.66
0.05
0.16
0.02
0.04
0.02
0.05
0.04
0.02
317
43.4
2.08
363
1.00
65.8
6.13
2.36
18.9
211
5.19
10.1
27.5
0.76
1.02
1.11
1.05
1.56
0.05
0.15
0.01
0.03
0.02
0.04
0.04
0.02
309
41.6
1.92
353
0.94
59.1
5.82
2.16
17.2
190
4.74
8.37
25.3
0.79
1.07
1.17
1.06
1.62
0.04
0.14
0.01
0.03
0.02
0.04
0.04
0.02
279
37.8
1.96
319
0.91
0.001
0.001
0.001
0.001
0.001
0.010
0.001
0.001
0
0.100
0.010
0.100
0.100
0
1.000
0
0.100
1.000
0
0.010
0
(3) NOx emissions were inversely related to the exhaust temperatures with higher BT additions (1525 wt.%), while
BT20, BT15W0.5, and BT15W1 had the maximum NOx emissions in the 0, 0.5, and 1.0 wt.%-containing blends, respectively. The major mechanism of NOx reduction was the
lower combustion temperature [56] achieved by adding BT
and water.
(4) The 0.5 wt.% water content showed a dramatic reduction of
ISFC from pure and 1.0 wt.% BT addition, which is explained
by the fact that the micro-explosions could provide better
atomization and moderate the ISFC of low-heating value
BT-diesel blends.
(5) The ISFC of BT5W0.5 (495 mL kW1 h1) and BT10W0.5
(497 mL kW1 h1) did not substantially increase from that
of D100 (493 mL kW1 h1). In addition, they reduced NOx
by 22.5% and 16.5%, PM by 41.1% and 44.9%, total-PAHs by
6.67% and 7.92%, and total-BaPeq by 7.91% and 7.78%, respectively, compared to those of regular diesel. In order to consider both energy performance and pollutant emissions,
the 5 and 10 wt.% BT additives with 0.5% water content were
the two most suitable blends for practical use in an HDDEG.
Nevertheless, butanol additive can be utilized by applying
bio-processes that can reduce CO2 emissions over a products life cycle, and which are more environmentally friendly
than those associated with petro-diesel.
Acknowledgments
This research was supported in part by the National Science
Council in Taiwan, Grant Number NSC 98-2621-M-006-007. The
authors also thank Professor S.J. Chen, Dr. S.W. Li, Mr. J.H. Tsai,
Mr. Y.C. Liu, Ms. L.P. Chang, and Mr. S.S. Chang for their insightful
discussions and great help in the experimental work.
371
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