Egyptian Journal of Petroleum 28 (2019) 371–376 Contents lists available at ScienceDirect Egyptian Journal of Petroleum journal homepage: www.sciencedirect.com 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 . However, TEL compounds have a dangerous impact on human health  so its addition was banned in almost all countries . 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: [email protected] (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 . 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 . 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 . 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/). 372 M. Amine, Y. Barakat / Egyptian Journal of Petroleum 28 (2019) 371–376 and cold engine starting . 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 . 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 . 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 . 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 . 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 . 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  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.  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.  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 373 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 . 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. 374 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 . ASTM-D323 is not applicable for measuring the vapor pressure of alcohol-gasoline blends because of trace amounts of water present in the test . 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 . 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 . 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 . 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 . 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 375 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 . 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  while methanol’s blending octane values are nominally 129-134 research octane number (RON) and 97-104 motor octane number (MON) . 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 . 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 . 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 . 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. 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