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Properties of gasoline-ethanol-methanol ternary fu

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Egyptian Journal of Petroleum 28 (2019) 371–376
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Egyptian Journal of Petroleum
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Full Length Article
Properties of gasoline-ethanol-methanol ternary fuel blend compared
with ethanol-gasoline and methanol-gasoline fuel blends
Manal Amine ⇑, Y. Barakat
Processes Design & Develop Department, Egyptian Petroleum Research Institute, Cairo, Egypt
a r t i c l e
i n f o
Article history:
Received 14 February 2019
Revised 4 August 2019
Accepted 26 August 2019
Available online 14 September 2019
Keywords:
Distillation curve
Azeotrope formation
Ternary and binary fuel blends
a b s t r a c t
Two binary sets of gasoline-methanol (GM) and gasoline-ethanol (GE) blends along with two other ternary sets of gasoline-methanol-ethanol (GME) blends were formulated comprising single and dual alcohol.
ASTM-D86 distillation, vapor pressure, and octane number were measured. Also, distillation curves were
constructed for each blend and the influence of azeotrope formation was discussed. The obtained results
reveal that distillation curves of gasoline blends, comprising from 5 to 15 vol% methanol, display a more
significant decrease in distillation temperature than gasoline-ethanol blends. Also, more decrease in distillation temperature is observed by increasing the rate of blended alcohol. At equal rates of blended alcohol, the distillation curve of ternary fuel (GE5M5) is positioned in between distillation curves of binary
fuel blends GM10 and GE10. More acceptable vapor pressure is achieved in ternary GEM fuels containing
7.5–15.0 vol% of dual alcohol, the same rate in GM blends increases vapor-lock tendency. At equal alcohol
content, GEM blends give a higher octane number than GE one.
Ó 2019 Egyptian Petroleum Research Institute. Production and hosting by Elsevier B.V. This is an open
access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
1. Introduction
Climate change and petroleum fuel depletion are the most significant problems that the world is facing today so great efforts for
discovering environmentally friendly and renewable sources of
energy have increased around the world. As the transportation sector shares with huge amounts of global emissions, it is important
that the alternative fuel is of lower exhaust emissions.
1.1. Octane boosting additives
Straight run gasoline requires the addition of many additives,
one of them is the octane booster as gasoline often has low octane
rating and cannot satisfy the requirements of the modern engines.
Compounds of tetraethyl lead (TEL) were used as significant octane
boosters as they raise the octane number by about ten times [1].
However, TEL compounds have a dangerous impact on human
health [2] so its addition was banned in almost all countries [3].
Alcohols and ethers are the most commonly used oxygenated additives in gasoline to assist in octane rating boost and provide better
combustion quality. Methyl tertiary butyl ether (MTBE) was used
as one of the most significant additives for enhancing gasoline
Peer review under responsibility of Egyptian Petroleum Research Institute.
⇑ Corresponding author.
E-mail address: manalamine2030@gmail.com (M. Amine).
octane number. MTBE was favorable because it is not as sensitive
to water as other additives and does not increase the volatility of
the fuel blend [4]. However, MTBE showed a serious problem as
it contaminates groundwater and strongly thought as a health risk
threat [5,6]. At present, alcohols are the most common renewable
additives used as octane promoters in gasoline fuel [7]. The addition of alcohol such as ethanol or methanol to gasoline can
enhance air quality because it improves fuel combustion. Alcohol
is considered as another source of oxygen in the combustion process as it contains an oxygen atom in its chemical composition.
However, problems could happen such as phase separation in fuel
blend but this problem could be solved by the addition of cosolvents [8–10]. Also, corrosion problems could happen to metallic
parts of the fuel system [11]. Among the most critical problems
created as a result of adding alcohol is the increase in fuel volatility
[12,13]. Most of the problems caused by adding alcohol could be
avoided by using low concentrations of alcohol or by adding
another co-solvent. Rather than directly displacing gasoline with
methanol or ethanol, an improved approach would involve the
use of a limited amount of high octane fuel (methanol or ethanol)
to enable the engine to be more efficient in its use of gasoline fuel,
which has considerably higher energy density. This so-called
Octane-on Demand concept, therefore, combines the high energy
density and widespread availability of oil-derived fuels with the
superior octane quality of methanol or ethanol, while reducing
the problems associated with energy density, phase separation
https://doi.org/10.1016/j.ejpe.2019.08.006
1110-0621/Ó 2019 Egyptian Petroleum Research Institute. Production and hosting by Elsevier B.V.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
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M. Amine, Y. Barakat / Egyptian Journal of Petroleum 28 (2019) 371–376
and cold engine starting [14]. This system assisted vehicles to operate at high severity conditions, while still utilizing the comparatively low octane quality gasolines. This system reduced the
necessity to produce large quantities of high octane gasoline. Morganti et al. examined the optimum way to leverage the most
widely available high octane fuels to improve the performance
and environmental impact of light-duty vehicles. A comprehensive
set of engine data was presented for a regular grade E10 gasoline
and a high octane E30 gasoline. These fuels were compared with
the Octane-on Demand concept in a high compression ratio engine
with moderate levels of boosting. The results proved that the
Octane-on Demand concept afforded lower specific CO2 emissions
to the E30 gasoline, with up to a 10% improvement in specific fuel
consumption; Octane-on-Demand engines that are calibrated to
operate at peak efficiency afforded no significant benefits over
higher octane gasolines with mid-levels of ethanol, e.g. E30. The
most promising Octane-on-Demand calibration strategy offered
considerable benefits over the high octane E30 gasoline. For all
operating conditions, the specific CO2 emissions were comparable
or lesser than the E30 gasoline, while the specific fuel consumption
was reduced by up to 10%. [15,16].
1.2. Methanol as a fuel
Methanol is often favored over ethanol as a biofuel primarily
because of the number of different production resources for
methanol, which can be manufactured from renewable energy
sources such as gasification of wood, agricultural by-products,
and municipal waste, as well as fossil fuel feedstocks like coal
and natural gas [17]. Methanol is a promising alternative fuel as
it can be blended with gasoline [18,19]. China is the biggest country in methanol production. It was even beyond half the global
total production capacity [20]. At the beginning of 2011, China
started the program in which the M85 (85% methanol-gasoline
blend) and M100 (pure methanol) were applied in spark-ignited
engines, and took Shanghai City and Shaanxi Provinces as the
pilots. In the Program, the annual consumption of methanol as
vehicle fuel in 2011 was about 2.3 million tons, which saved
almost 1.05–1.24 million tons of gasoline [21].
China is rich in coal which is regarded as a significant feedstock
for methanol production. Methanol is easily produced from gasified coal. This has led to the construction of mega methanol plants
in China. Dependence of China on imported oil has encouraged the
use of methanol as an alternative fuel in many provinces particularly those rich in coal. Also, the low cost of methanol has led to
adulteration of gasoline in such provinces. As a result, China governorate established various regional and national methanol fuel
standards. Also, methanol-gasoline flex-fuel vehicles were developed. Pure M100 vehicles are also available, and the current
researches are attempting to understand how new regulations
should evolve regarding to the exhaust emissions of such vehicles
[22]. Methanol is also produced from natural gas which is composed primarily from methane. The natural gas is converted to a
syngas gas which is a mixture of CO, CO2, and H2. This mixture is
then converted to methanol at conditions 250–300 °C, and pressure, 5–10 MPa, using CuO/ZnO/Al2O3 catalyst [23].
Literature comprises lots of works studied the characteristics
and performance of alcohol–gasoline blends, e.g., ethanol–gasoline
blends and methanol–gasoline blends. It can be recognized from
the literature that ethanol or methanol–gasoline blends can successfully decrease the pollutant exhaust emissions, compared to
the neat gasoline [24,25].
No doubt that the incorporation of methanol in ethanolgasoline blends can lower the cost of gasoline-alcohol fuel especially in non-agricultural countries which do not have feedstock
for ethanol production. However, the impacts of Gasoline-etha
nol–methanol blends are rarely investigated; there were very few
literatures regarding such ternary blend. Elfasakhany [26] examined the performance and exhaust emission of such ternary blend
and he found that when the vehicle was fueled with gasolineethanol-methanol blends, the carbon monoxide and unburned
hydrocarbons emissions concentrations were significantly
decreased compared to the neat gasoline. Turner et al. [27] investigated the effect of Gasoline-ethanol–methanol blends on CO2 and
NOx emissions. They applied different blend concentrations of
ethanol/methanol and they indicated that the ternary fuel blends
can reduce the CO2 and NOx emissions than the neat gasoline. Sileghem et al. [17] examined the effect of two different rates of
ethanol–methanol–gasoline blends on CO and NOx emissions.
They found that the ternary fuel blends reduce the NOx emission
than the neat gasoline but higher than the neat methanol. In addition, ternary fuel blends can yield less CO emissions than the binary fuel blends (methanol–gasoline or ethanol–gasoline) within
definite conditions of the engine speed. Results also showed that
ternary fuel blends afford less NOx than ethanol–gasoline blends
but they produce more NOx than the methanol–gasoline blends.
In the present study, we aim at studying gasoline-ethanol–metha
nol blends (GEM blends) at rates (5–15 vol% for the total alcohol
in the fuel blend). The volatility criteria (Distillation profile and
Vapor pressure) for the ternary fuel blends are compared with
those of the binary fuel blends; ethanol–gasoline and methanol–
gasoline blends and that of the neat gasoline at similar rates of
the total alcohol in the fuel blends Furthermore the influence of
the ternary fuel blends on octane rating is examined and compared
with that of the neat gasoline and that of the binary fuel blends.
2. Material and methods
2.1. Fuel blend formulation
Four groups of fuel blends were formulated from gasoline, ethanol and/or methanol. Gasoline was supported by Cairo Petroleum
Company-Mostorod Refinery. Absolute ethanol (99.9%) was purchased from CARLO ERPA while methanol (>99% purity) was purchased from SCHARLAU Chemical Company. The composition and
designation of the fuel blends were summarized in Table 1.
2.2. Fuel properties measurements
The Distillation curves of the fuel blends were constructed
according to ASTM-D86 while their vapor pressures were measured by automated Setavap 2 Vapor Pressure Tester according to
ASTM-D5191 Standard test method for the vapor pressure of
petroleum products. Research octane number was measured by
ZX-101XL – Portable Near-Infrared Octane/Cetane Analyzer.
3. Result and discussion
3.1. Distillation curve
The distillation curve is constructed from T (temperatures)
points on the y-axis and E (percent evaporated) points on the
x-axis. T10, T50, or T90, are the temperatures at which 10%, 50% or
90% by volume of fuel distilled [12,28]. From distillation profile,
some specific characteristics of gasoline fuel performance could
be evaluated. For example T10, the front-end volatility, it must be
low enough to facilitate starting in cold weather and adjusted in
hot weather to avoid vapor-lock formation. T50, the mid-range
volatility, must be adjusted to provide rapid warm-up, to attain
smooth running and to conserve carburetor from icing. T90, the
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M. Amine, Y. Barakat / Egyptian Journal of Petroleum 28 (2019) 371–376
Table 1
Designation and composition of fuel blends.
Fuel Designation
Composition
G
GE5
GE7.5
GE10
GE12.5
GE15
GM5
GM7.5
GM10
GM12.5
GM15
GE5M2.5
GE5M5
GE5M7.5
GE5M10
GE2.5M5
GE7.5M5
GE10M5
Gasoline (Vol%)
Methanol (Vol%)
Ethanol (Vol%)
Total (Vol%)
100
95
92.5
90
87.5
85
95
92.5
90
87.5
85
92.5
90
87.5
85
92.5
87.5
85
0
0
0
0
0
0
5
7.5
10
12.5
15
2.5
5
7.5
10
5
5
5
0
5
7.5
10
12.5
15
0
0
0
0
0
5
5
5
5
2.5
7.5
10
100
100
100
100
100
100
100
100
100
100
100
100
100
100
100
100
100
100
200
G
GE5
GE7.5
GE10
GE12.5
GE15
180
160
Temperature,°C
tail-end volatility, should be adjusted enough to afford good fuel
economy and to protect the engine from deposits formation.
When alcohols were blended with gasoline, especially the
shorter chain alcohols, methanol and ethanol, the blend displays
decreases in distillation temperatures and does not act as an ideal
mixture, because of the formation of a near-azeotropic mixture
[12,29,30].
In distillation curves for methanol or ethanol-gasoline blends
(Figs. 1 and 2), the distillation temperature increases until the
first10% has been recovered. Subsequently, there is a substantial
plateau area where the distillation temperature increases slowly.
Following the plateau area, the temperature increases rapidly
again and approaches, the gasoline distillation curve. Nearazeotropic behavior is observed in the plateau region, but by complete distilling the alcohol, the near-azeotropic mixture is removed
and the distillation temperature increases toward that of the
140
120
100
80
60
40
20
0
0
10
20
30
40
50
60
70
80
90
100
Evaporated volume%
Fig. 2. Distillation curves for ethanol-gasoline blends.
Temperature,°C
150
140
G
130
GM5
120
GM7.5
110
GM10
100
GM12.5
90
GM15
80
70
60
50
40
30
20
10
0
0
10
20
30
40
50
60
70
80
90
100
Evaporated volume%
Fig. 1. Distillation curves for gasoline-methanol blends. Where G is gasoline free of
alcohol, GM5 is gasoline contained 5% of methanol and GM15 is gasoline contained
15% of methanol.
remaining gasoline hydrocarbons [29]. In the case of gasolinemethanol blends, the impact of the near-azeotropic mixture is
more significant than that of gasoline-ethanol blends. It’s obvious
from the figures that the effect increases with increasing the rate
of alcohol.
Gasoline-ethanol-methanol blends were found to have the
same trend as the binary fuel blend (gasoline-ethanol or
gasoline-methanol blends). Distillation temperatures were found
to increase gradually until the first10% has been recovered. Subsequently, there is a substantial plateau region where the distillation
temperature increases slowly. Following the plateau region, the
temperature increases rapidly again and approaches, the gasoline
distillation curve (as shown in Figs. 3 and 4). Fig. 5 compares the
distillation curves of the fuel blends containing 10 vol% of alcohol,
the ternary fuel blend was found to lie approximately in the middle
position between those of the single-alcohol fuel blends (gasolinemethanol blends and gasoline-ethanol blends) containing the same
total alcohol volume concentration. From the obtained results of
investigating the distillation curves, we can conclude that using
the ternary blend is much better than using gasoline-methanol
blends as it diminishes the significant impact of the single methanol blending.
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M. Amine, Y. Barakat / Egyptian Journal of Petroleum 28 (2019) 371–376
200
160
180
140
G
GE10
Temperature,°C
140
120
Temperature, °C
G
GE5
GE5M2.5
GE5M5
GE5M7.5
GE5M10
160
100
120
GM10
100
GE5M5
80
60
80
40
60
20
40
0
20
0
20
40
60
80
100
Evaporated volume %
0
0
10
20
30
40
50
60
70
80
90
100
Evaporated volume %
Fig. 5. Distillation curves of neat gasoline compared with gasoline-methanol,
gasoline-ethanol, and gasoline-ethanol-methanol blends containing 10 vol% of
alcohol.
Fig. 3. Distillation curves of neat gasoline and gasoline-ethanol-methanol blends of
varied proportions of methanol.
150
140
G
130
GM5
Temperature, °C
120
GE2.5M5
110
100
GE5M5
90
GE10M5
80
70
60
50
40
30
20
10
0
0
10
20
30
40
50
60
70
80
90
100
Evaporated volume %
Fig. 4. Distillation curves of base gasoline and GEM blends of varied proportions of
ethanol.
3.2. Vapor pressure
Vapor pressure is the most important parameter of gasoline as
gasoline burns in its vapor state. Vapor pressure indicates the existence of adequate light fraction that evaporates at low temperatures. The vapor pressure of gasoline is most often measured
according to American Society for Testing and Materials ASTMD323 [31]. ASTM-D323 is not applicable for measuring the vapor
pressure of alcohol-gasoline blends because of trace amounts of
water present in the test [32]. In the present study, the vapor pressure of the fuel blends was measured according to ASTM-D5191
(equivalent to European method EN 13016-1) which involved
additional automation, smaller sample volumes, and greater
precision.
Vapor pressure is an important factor in controlling evaporative
emissions. Limits for the maximum vapor pressure of gasoline are
legally mandated in some regions to control air pollution [31].
When the vapor pressure of gasoline is low, an engine may have
to be cranked a long time before it works especially in winter
months. When the vapor pressure of the fuel is very low, an engine
may not work at all. Vapor pressure differs from winter to summer
seasons; the normal range is 7 psi to 15 psi according to ASTMD4814. High values of vapor pressure usually result in better performance for a cold start, but low values in summer are better to
avoid the tendency to vapor lock especially at high operating temperatures or high altitudes [31].
When blending methanol or ethanol with gasoline, the fuel
blend distilled at lower temperatures and does not behave like
an ideal mixture, because of the formation of a near-azeotropic
mixture [12,29,30]. The non-ideal mixtures also have higher vapor
pressures than would be predicted by Raoult’s law [33]. This effect
is particularly noticeable at a low concentration of alcohols
because the blend has a vapor pressure higher than either the
gasoline or the alcohol alone.
This non-ideal behavior of ethanol-gasoline and methanolgasoline blends is a result of molecular interactions between the
gasoline components and methanol or ethanol molecules. The ideal
behavior of vapor pressure of an ideal mixture would follow
Raoult’s law Eq. (1):
P¼
X
PiMi
ð1Þ
where P is the vapor pressure of the mixture, Pi the vapor pressure
of component i and Mi is the mole fraction of component i.
While the non-ideal mixture often represented through the use
of non-unity activity coefficients for each component, ci, as shown
in Eq. (2):
P¼
X
ciPiMi
ð2Þ
when methanol or ethanol or both is added to gasoline in
increasing amounts, the hydrogen bonding between alcohol molecules are increasingly weakened and the alcohol molecules start to
act as a low molecular mass component and the gasoline-alcohol
interactions change and the alcohol escape from the blend in the
form of vapor [13]. The non-polar hydrocarbon molecules in gasoline hinder the intermolecular hydrogen bonding between the
polar methanol or ethanol molecules, and the methanol or ethanol
interferes with molecular interactions between the gasoline hydrocarbon molecules [34–36]. These interfering with intermolecular
bonding let the respective molecules to escape easily from the
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M. Amine, Y. Barakat / Egyptian Journal of Petroleum 28 (2019) 371–376
93
92
91
90
RON
liquid in the form of vapor leading to increase vapor pressure. Fig. 6
illustrates that the extent of the increase in vapor pressure is less
pronounced with ethanol than methanol. This is due to the lower
vapor pressure and lower polarity of ethanol. This figure indicates
also that the dual alcohol blending into gasoline has a moderate
impact on the vapor pressure as the curves of the two groups of
GEM blends studied here lie in the middle position between curves
of the single alcohol blends depending on the rate of methanol
addition in the fuel blend. GEM blends of a higher percent of
methanol are not adequate to the summer period.
GE-Blends
88
GEM-Blends of varied E
3.3. Octane number
87
Octane number is a term used to estimate the antiknock performance. It is the ability of the gasoline fuel to resist knocking as it
burns in the combustion chamber. Research and motor octane
numbers (RON, MON) represent the main quality features of the
gasoline, as they give a specific indication of the anti-knocking performance of the fuel. The higher the octane number the better the
gasoline resists detonation and the smoother the engine runs [37].
Incorporation of ethanol or methanol in gasoline promotes the
octane number of the fuel blends [38–40] as the RON of ethanol
was usually indicated to be about 109 and the MON approximately
90 [40] while methanol’s blending octane values are nominally
129-134 research octane number (RON) and 97-104 motor octane
number (MON) [41]. Furthermore, the autoignition chemistry and
charge cooling have a significant effect on the research octane
number (RON) of ethanol/gasoline blends. While gasoline is fully
vaporized before entry into the engine in a standard RON test, significant charge cooling is observed for blends with high ethanol
content, with the presence of a near-saturated and potentially
two-phase air-fuel mixture during induction [42]. As obvious from
Fig. 7, the research octane number (RON) of ethanol-gasoline or
methanol-gasoline blends increases as the rate of the added alcohol in fuel blends increases. A small percentage of ethanol or
methanol can, therefore, lead to a disproportional increase in the
octane number. The obtained results are in agreement with the
findings of other researchers [43]. Literature suggested that the
base fuel composition plays an important role in this non-linear
blending behavior of alcohol [44–47]. To this end, base fuels with
lower octane numbers provided a greater increase in the RON with
10% ethanol addition [47]. In GEM blends the effect of the dual
alcohols on the octane ratings is similar to that of the single alcohol. As the rate of the dual alcohol increase, the octane number
increase. The impact of dual alcohol on octane number depends
on the proportion of the added methanol in the fuel blend; the
86
14
GM-Blends
89
GEM-Blends of varied M
5
7.5
10
12.5
15
Total alcohol, vol%
Fig. 7. Comparison of the Measured Research (RON) octane numbers for GEM
blends with single alcohol blends.
GEM blends of higher methanol content are higher in octane number as indicated from Fig. 7. Fig. 7 also compares the research
octane numbers of GEM blends with those of methanol-gasoline
blends and ethanol-gasoline blends containing the same rate of
alcohol. Higher octane rating can easily be achieved through
proper formulations of ternary gasoline blend (GEM) than binary
ethanol one.
4. Conclusion
Binary and ternary gasoline blends, comprising from 5 to 15 vol
% alcohol, display a significant decrease in distillation temperature than alcohol-free gasoline.
The distillation curve of ternary gasoline blends (GEM) is positioned in between the binary GM at the bottom and GE at the
top.
Dual alcohol blending into gasoline (GEM), reduces the vapor
pressure severity of single methanol blending.
Higher octane rating can easily be achieved through proper formulations of ternary gasoline blend (GEM) than binary ethanol
one. We found that GE5M10 blends are higher in octane number than ethanol-gasoline blends (GE15) by approximately 1
point.
From the obtained results, GEM blends are highly recommended than gasoline-ethanol blends and gasoline-methanol
blends. GEM is more economic than GE blends and reduces
the vapor pressure severity of single methanol blending.
12
Vapor pressure, psi
Declaration of Competing Interest
10
The authors declare that they have no known competing financial interests or personal relationships that could have appeared
to influence the work reported in this paper.
8
GM-Blends
6
GEM-Blends of varied M
4
GEM-Blends of varied E
2
GE-Blends
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0
0
2.5
5
7.5
10
12.5
15
17.5
Total alcohol, vol%
Fig. 6. Vapor pressures of binary blends compared with ternary blends.
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