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Alternative Fuel for a Standard Diesel Engine

A Hull, I Golubkov, B Kronberg and J van Stam International Journal of Engine Research 2006 7: 51 DOI: 10.1243/146808705X30549 The online version of this article can be found at: http://jer.sagepub.com/content/7/1/51

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Alternative fuel for a standard diesel engine

A Hull1,3*, I Golubkov2, B Kronberg1,3, and J van Stam3 1Institute for Surface Chemistry, Stockholm, Sweden 2Agrofuel AB, St Goransgatan, Stockholm, Sweden 3Department of Physical Chemistry, Karlstads University, Karlstad, Sweden The manuscript was accepted after revision for publication on 28 April 2005. DOI: 10.1243/146808705X30549

Abstract: Alternative fuels have been developed for the commercial diesel products Mk1 and EN590. Appropriate additives were selected from a broad range of oxygenates including alcohols, acetals, ethers, esters, and nitrates by a process of systematic elimination. The resulting fuels called Biodiesel 15 meet all existing standards in force for diesel fuel, are stable, and have similar performance characteristics to standard diesel. Signicantly Biodiesel 15 is much cleaner than standard diesel with around 30 per cent or more reductions in particulate matter in the exhaust emissions. Carbon dioxide (CO ) emissions are much lower with Biodiesel 2 15 than with standard diesel products. Other regulated emissions are on a par with Mk1. The fuel consumption of Biodiesel 15 is 2 per cent lower than that of conventional Mk1. Keywords: alternative diesel fuel, oxygenates, diesel engine performance, diesel engine emissions, particulate emissions

1 INTRODUCTION Industry worldwide has a strong incentive to develop alternative motor fuels to protect the environment and adhere to tighter emissions requirements. In 1997 in Kyoto, representatives from 105 states signed the Kyoto Protocol [1], which is designed to reduce excess carbon dioxide (CO ) emissions produced 2 when burning oil, mineral gas, coal, and related products. The combustion of motor fuels adds considerably to the imbalance of CO in the atmosphere. Nitrogen 2 and sulphur oxides (NO and SO ) are also formed and x x cause the acidication of lakes and other fresh water supplies, aecting the vital functions of humans, animals, and vegetation. Finally, solid particles, which are the products of incomplete combustion, cause cancers in humans and animals. The use of motor fuel components derived from renewable raw materials, so-called biocomponents, enables a reduction of the harmful impact of burning fuel on the environment. Accordingly in 2003 the European Commission passed a directive [2] to
* Corresponding author: KTH Stockholm, Institute for Surface Chemistry, Box 5607, Stockholm, SE 114 86, Sweden. email: angelica.hull@surfchem.kth.se

member states promoting the use of biocomponents in motor fuel starting from 2005. The European Commission has also dened requirements on the amount of harmful pollutants in exhaust emissions of internal combustion engines, specically for SO , x NO , and particulates. x The stipulations of the directive are such that by 2010 the amount of harmful pollutants in exhaust emissions will reach an entirely new level. Clearly, reaching such a reduced level of harmful pollutants will require considerable investment from motor fuel producers. The existing inventory of vehicles and machinery with standard engines prevents the use of motor fuels consisting completely of biocomponents within the time frame set by the European Commission. So it is evident that in the years to come the role of mixed fuels produced partly from petroleum and partly from renewable raw materials will grow considerably. Gasolineethanol blends for spark ignition (SI) engines and diesel mixtures containing methyl ethers of higher fatty acids for use in diesel engines are examples of this type of fuel. The development and marketing of a diesel fuel containing biocomponents, a biodiesel, is complicated by the standards requirements [3] for diesel fuel, which impose substantial restrictions on potential
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fuel additives. First, a high ash point is required, which according to the requirements of the EU standard should be not lower than 55 C. This immediately rules out a wide variety of potential biocomponents as they are too volatile. Second, the distillation properties and cloud point set by the standard similarly rule out quite a number of readily available products produced from renewable raw material. Third, a marketable fuel must be stable and above all stable in the presence of water. Fourth, the performance of biodiesels must be similar to standard diesel and the emissions properties of biodiesels must be signicantly better than those of standard diesel. It is well known that replacing part of the hydrocarbons (HCs) in diesel fuel by oxygenates can provide satisfactory engine power and cleaner exhaust without modication of existing diesel engines [4, 5]. The feasibility and properties of mixtures of diesel fractions with pure ethanol was reported long ago [6]. However, the main problem of using lower alcohols is the tendency of the fuel mixtures to phase separate, especially in the presence of water and at temperatures below 0 C. The problem of water in diesel alcohol mixtures is solved in a number of patents [711], which include the use of surfactants. The problem of using lower alcohols in diesel fuel is solved by the creation of microemulsions stabilized by surfactants [12, 13]. Also, fatty acids and organic ethers have been added to the mixtures of diesel and the lower alcohols [14]. Besides being used as a replacement of the petroleum component of a diesel fuel, oxygenates have been proposed for increasing the cetane number and reducing harmful pollutants in exhaust emissions produced during the combustion of diesel fuel [1517]. Others report work on multicomponent oxygencontaining diesel fuels. These works report improved performance properties of such fuels and reductions in the level of harmful substances in the exhaust. This is to be expected given that multicomponent oxygen-containing diesel fuels ignite and combust better. The eect of biodiesel fuels comprising oxygen-containing additives on the emissions of various heavy-duty engines has been studied [18, 19]. Oxygenates of dierent molecular structure were selected for the evaluation. Results of the tests demonstrate that particulates emission depends directly on the oxygen content in the fuel. Reduction of particulates is accompanied by a small increase of NO emissions. Generally, addition of oxygenates to x the fuel decreases emissions of carbon monoxide (CO) and HCs. Unregulated emissions of aldehydes and ketones also decrease on addition of oxygenates.
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When peroxide cetane-boosting additives are added to fuel containing oxygenates the emissions prole is identical to the emission prole obtained for low-aromatic fuels. Reduction of particulates by 52 per cent as compared to the base fuel is reported [20] when using a mixture of 15 per cent dimethoxymethane and 85 per cent low-sulfur, low-aromatics diesel. However, dimethoxymethane has a tendency to evaporate from the fuel if special handling measures are not taken. Moreover, addition of 15 per cent dimethoxymethane to the HC base requires some modication of the fuel system of the engine. The eect on regulated and unregulated exhaust emissions produced by the addition to a standard diesel fuel of 20 per cent methyl esters of fatty acids has been studied [21, 22]. The resulting mixture was tested in standard engines of various types. It was demonstrated that the use of the mixed fuel results in a reduction of HC, CO, and particulates compared with a standard diesel fuel. At the same time the use of the mixed fuel results in an increase of NO x emission and fuel consumption when compared with a standard diesel fuel. The study of the polyaromatic hydrocarbons (PAH) and nitropolyaromatic hydrocarbons (NPAH) produced during the combustion of the mixed fuel demonstrated that the addition of 20 per cent methyl esters of higher fatty acids to a standard diesel fuel results in a lower emission of the PAH and NPAH compounds compared with a standard diesel. The objective of the studies [23, 24] was to select oxygenates as blending components in diesel fuel. Based on the analysis of several dozens of oxygencontaining compounds it has been demonstrated that only two can be used for formulating mixed diesel fuels. Despite all these developments, currently there is no fuel on the market containing more than 6 per cent of oxygenates that is suitable for operation in conventional diesel engines. Over the last ten years oxygen-containing diesels for conventional engines have been developed by the authors. A specic goal of the research was to obtain a fuel comprising at least 15 per cent of oxygenates. The fuel was to have physical/chemical properties and characteristics in use closely similar to the standards in force for diesel fuels. Moreover, any fuels developed in this way should have the additional advantage of signicantly lower exhaust emissions. The approach taken allows the oxygen-containing diesel to be used by the existing vehicle eet without modication or adjustment. The advantage of this approach is that vehicle users will not have to make additional investments in expensive engine
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modications or new engines. In addition, the use of the oxygen-containing compounds obtained from biomass meets all the requirements of the directive especially as regards the four diculties already mentioned. The main results of this development are presented in this paper.

2 KEY RESULTS The research started with study of the stability of simple mixtures of alcohols and diesel fuel. Screening experiments on both cloud point and detection of phase separation were carried out. Mk1 diesel fuel together with ethanol, as well as another alcohol, were used in each experiment. The test results are shown in Table 1. It is not so much the exact values of the parameters which are of interest, but rather the trends which can be seen passing from light to heavier alcohols and increasing the amount of water present. The data from Table 1 show that the stability of the mixtures comprising ethanol and diesel increases when higher alcohols are added to the mixture. There are clear trends when higher alcohols are present in the mixture of ethanol and diesel so that some mixtures do not separate at signicantly reduced temperatures. This is shown by the sequence of mixtures 1 2 3 5 4. Another related trend shows how to accommodate some water in the mixture such as when 95 per cent by volume of pure ethanol is used instead of 99.9 per cent by volume of pure ethanol. Consider the sequence 6 8 15 14, for example,

to see this. The last mixture in this sequence contains about 0.3 per cent water, which is not negligible. Acetals, ethers, and esters are further potential biocomponents besides alcohols. So the study of reduced temperature stability was extended to include these in mixtures of diesel and alcohols. An inorganic ester, isopropyl nitrate, was also included. The results are the same as for the previous experiments on these mixtures and are presented in Table 2. The results are broadly similar to those in Table 1. An analysis of the experimental data shows that acetals, ethers, and esters also may increase the stability of dieselethanol mixtures at reduced temperatures, even in cases where a certain amount of water is present. The production of homogeneous mixtures of diesel and biocomponents stable at reduced temperatures is a considerable step towards obtaining alternative biodiesel. These mixtures can become a test fuel, however, only after testing their performance properties on a standard engine and after it is proved that they satisfy the requirements of the existing standards for diesel fuels. The preliminary tests were aimed at obtaining a fuel composition for conventional diesel engines with up to 15 per cent biocomponents. Swedish Mk1 diesel was chosen as a base for this fuel as it is the most environmentally advanced motor fuel in its class. The most favourable mixtures for lowtemperature stability were used as biocomponents including alcohols, ethers, esters of fatty and inorganic acids, and also acetals. Rapeseed oil ethyl ether was also added as a potential candidate.

Table 1 Results of stability tests for various blends of diesel motor fuel, ethanol, and higher alcohols
Temperature (C)
No.
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15

Composition
Mk1 : Et Mk1 : Et : 2-Propanol Mk1 : Et : 1-Butanol Mk1 : Et : 1-Pentanol Mk1 : Et : 1-Pentanol Mk1 : EtW Mk1 : EtW : 1-Propanol Mk1 : EtW : 2-Propanol Mk1 : EtW : 1-Butanol Mk1 : EtW : 1-Pentanol Mk1 : EtW : 2-Pentanol Mk1 : EtW : 1-Hexanol Mk1 : EtW : 1-Hexanol Mk1 : EtW : 1-Heptanol Mk1 : EtW : 1-Heptanol

Composition % wt
95 : 5 85 : 7.5 : 7.5 85 : 7.5 : 7.5 85 : 10 : 5 85 : 12 : 3 98 : 2 85 : 3 : 12 85 : 3 : 12 85 : 5 : 10 85 : 6 : 9 85 : 6 : 9 85 : 6 : 9 85 : 7 : 8 85 : 6 : 9 85 : 7 : 8

22
1 1 1 1 1 1* 1 1 1 1 1 1 1 1 1

10
1* 1* 1 1 1* 2 1* 1* 1 1 1* 1 1* 1 1*

37
2 2 1 1 2 2 2 2 2 1 2 1 1* 1 2

Key: Mk1=diesel motor fuel Mk1; Et=ethanol 99.9 per cent by volume; EtW=ethanol 95 per cent by volume; *=cloudy solution; 1=homogeneous solution; 2=two-phase mixture.

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Table 2 Results of stability tests for various solutions of diesel motor fuel, ethanol, higher alcohols, acetals, ethers, esters, and nitrates
Temperature (C)
No.
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15

Composition
Mk1 : Et : Methylal Mk1 : 2-Propanol : Methylal Mk1 : Et : Diethyl ether Mk1 : Et : Dibutyl ether Mk1 : Et : Butylethyl ether Mk1 : Et : Ethyl acetate Mk1 : Et : Butyl acetate Mk1 : Et : IPN Mk1 : Et : DBE : IPN Mk1 : Et : BA : IP Mk1 : Et : BA : IP : IPN Mk1 : EtW : Bt Mk1 : EtW : Bt : BA Mk1 : EtW : Bt : BA : IPN Mk1 : EtW : Bt : DBE : IPN

Composition % wt
90 : 5 : 5 90 : 5 : 5 80 : 10 : 10 80 : 10 : 10 80 : 10 : 10 80 : 10 : 10 80 : 10 : 10 75 : 15 : 10 75 : 15 : 9 : 1 80 : 10 : 5 : 5 79 : 10 : 5 : 5 : 1 85 : 6 : 9 80 : 6 : 9 : 5 78 : 6 : 9 : 5 : 2 78 : 6 : 9 : 6 : 1

22
1 1 1 1 1 1 1 1 1 1 1 1 1 1 1

10
1* 1 1 1 1* 1 1 1 1 1 1 1* 1 1 1

37
2 2* 1* 2* 2 1 1 1* 2 2 1 2 2* 1 1

Key: BA=butyl acetate; Bt=1-butanol; DBE=dibutyl ether; Et=ethanol 99.9% by volume; EtW=ethanol 95% by volume; IP=2-propanol; IPN=isopropyl nitrate; Mk1=diesel motor fuel Mk1; *=cloudy solution; 1=homogeneous solution; 2=two-phase mixture.

The rst tests were performed on a benchmark engine at Miljoverkstaden, Skovde, Sweden. During these tests various fuel compositions were tested on a standard Volvo TD61 GS engine with a nominal power of 140 kW to determine the performance properties of the diesel test mixtures, namely power output and torque. From the results of the rst tests mixtures were selected which contained up to 15 per cent biocomponent and 85 per cent diesel fuel Mk1 and provided the necessary power output and torque in a standard engine (that is not less than 95 per cent of the corresponding properties on the same engine for Mk1 diesel fuel). Additionally, the results were used to ne tune the biodiesel compositions for a second round of tests on the same engine. The test results are shown in Figs 1, 2, 3, and 4 and in Table 3.

Fig. 2 Power curve of the Volvo TD61 GS engine with a nominal power of 140 kW for blended fuels of Mk1 diesel and various oxygenates according to the fuel compositions given in Table 3, as indicated in the legend

Fig. 1 Power curve of the Volvo TD61 GS engine with a nominal power of 140 kW for blended fuels of Mk1 diesel and various oxygenates according to the fuel compositions given in Table 3, as indicated in the legend
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Fig. 3 Torque curve of the Volvo TD61 GS engine with a nominal power of 140 kW for blended fuels of Mk1 diesel and various oxygenates according to the fuel compositions given in Table 3, as indicated in the legend
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Table 3 Summary of test results for diesel mixtures containing oxygenates compounds. Tests performed on a heavy-duty Volvo TD61 GS engine, nominal power 140 kW
Performance properties of the engine at 2000 r/min
No.
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20

Composition
Mk1 Mk1 : Et : Bt Mk1 : Et : Pt Mk1 : EtW : Pt Mk1 : EtW : Hx Mk1 : EtW : Hp Mk1 : Et : DEE Mk1 : Et : EtA Mk1 : Et : BA Mk1 : Et : IPN Mk1 : Et : Bt : BA : IPN Mk1 : EtW : Bt : BA Mk1 : EtW : Bt : BA : IPN Mk1 : EtW : Bt : DBE : IPN Mk1 : RME Mk1 : Et : Bt : RME Mk1 : Et : Bt : RME Mk1 : EtW : Bt : RME Mk1 : EtW : Bt : RME : IPN Mk1

% by volume
100 85 : 7.5 : 7.5 85 : 10 : 5 85 : 6 : 9 85 : 6 : 9 85 : 6 : 9 80 : 10 : 10 80 : 10 : 10 80 : 10 : 10 75 : 15 : 10 79 : 10 : 5 : 5 : 1 80 : 6 : 9 : 5 79 : 6 : 9 : 5 : 2 79 : 6 : 9 : 6 : 1 95 : 5 95 : 1.5 : 1 : 2.5 90 : 5 : 3 : 2 90 : 3.5 : 3 : 3.5 79 : 6 : 9 : 5 : 1 100

Power (kW)
114 107 106 110 111 111 104 103 103 102 103 105 106 107 112 113 113 110 110 115

Torque (Nm)
547 510 508 525 532 532 503 500 500 492 502 506 508 510 534 536 535 525 529 547

Key: BA=butyl acetate; Bt=1-butanol; DBE=dibutyl ether; DEE=diethyl ether; Et=ethanol 99.9% by volume; EtA=ethyl acetate; EtW=ethanol 95% by volume; Hx=1-hexanol; Hp=1-heptanol; IPN=isopropyl nitrate; Mk1=diesel motor fuel Mk1; Pt=1-pentanol; RME=rapeseed oil methyl ether.

Fig. 4 Torque curve of the Volvo TD61 GS engine with a nominal power of 140 kW for blended fuels of Mk1 diesel and various oxygenates according to the fuel compositions given in Table 3, as indicated in the legend

The control fuel is shown in each diagram. The control fuel is included twice, by way of compositions 1 and 20 (see Table 3) to check that there was no change in the engine during the tests. From the results of the initial tests those compositions containing 15 per cent of biocomponent and 85 per cent of Mk1 diesel fuel that showed at least 95 per cent of the power and torque of Mk1 were selected. These compositions can be regarded as candidate fuels for pilot tests only after passing emissions tests. These tests were performed at MTC,
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Jordbro, Sweden in two stages. First, exhaust emissions were tested on a light-duty vehicle [25]. Second, simultaneous testing of the exhaust emissions, power, and torque was carried out on a heavy-duty engine [26]. Again Mk1 was used as a control. The rst stage of the exhaust emissions tests at MTC consisted of screening tests of a large number of candidate compositions, the performance properties of which had already been determined. Screening tests were performed on two cars, rst the VW Golf CL Diesel, model year 1993, with a mileage of about 115 000 km and with a standard diesel engine D1-WO3-92 produced by VW. The second car was the Audi A6 1.9 TDI, model year 1998, with a mileage of about 47 000 km and with a standard diesel engine produced by Audi. Testing of the exhaust emissions of the oxygen-containing diesel mixtures selected in the screening tests was performed in accordance with the test cycle EU 2000 NEDC (new European driving cycle) on the VW Passat TDI car, model year 1997, with a mileage of about 87 000 km and with a standard diesel engine 2D1-WDE-95 produced by VW. Figure 5 shows the details of the NEDC. Each day was the start of a new test cycle. The tests were performed according to the normal procedure, starting with a cold engine start (20 C) for test mixture 1 in Table 4. After some idle and engine
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Table 4 Performance properties of various fuel compositions based on Mk1

Performance properties
No.
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24

Compositions of the alternative fuel test mixtures

Mk1 100 Mk1 94.9 Mk1 89.9 Mk1 88.2 Mk1 83.2 Mk1 95 Mk1 90 Mk1 90 Mk1 85 Mk1 84.7 Mk1 89.7 Mk1 95 Mk1 95 Mk1 90 Mk1 90 Mk1 85 Mk1 89.9 Mk1 95.7 Mk1 95.7 Mk1 85 Mk1 85 Mk1 85 Mk1 84.8 Mk1 100

CO (g/km)
0.012

HC (g/km)
0.026 0.056 0.046 0.069 0.097 0.055 0.043 0.069 0.058 0.069 0.068 0.029 0.035 0.037 0.049 0.052 0.050 0.039 0.042 0.049 0.046 0.047 0.045 0.034

NO x (g/km)
0.757 0.810 0.770 0.906 0.886 0.819 0.819 0.893 0.813 0.886 0.898 0.707 0.601 0.676 0.670 0.668 0.670 0.618 0.624 0.651 0.696 0.706 0.636 0.575

CO 2 (g/km)
154.6 151.8 140.2 154.0 151.5 144.8 142.0 140.5 145.9 149.0 147.9 148.1 142.0 154.5 146.8 147.5 146.9 143.9 143.6 145.6 143.7 142.4 148.6 142.3

PM (g/km)
0.049 0.044 0.040 0.037 0.037 0.047 0.043 0.035 0.036 0.035 0.033 0.047 0.047 0.044 0.042 0.039 0.041 0.045 0.044 0.041 0.045 0.039 0.037 0.047

Fc (l/100 km)
5.986 5.982 5.539 6.189 6.100 5.609 5.614 5.626 5.853 6.016 5.956 5.744 5.662 6.103 5.858 5.897 5.846 5.637 5.631 5.794 5.652 5.733 5.939 5.653

Et 2.1 Et 2.1 Et 5.5 Et 5.5 Et 2.5 Et 2.5 Et 5 Et 5 Et 5.2 Et 5.2 RME 5 Et 1 Et 2 EH 4.6 EH 4.6 Et 3.4 EtW 2.2 EtW 2.2 EtW 3 B 2.5 B 2.3 Et 2

IP 1.4 IP 1.4 DB 3.2 DB 3.2 BA 1.5 BA 1.5 BA 1.5 BA 1.5 BA 3.1 BA 3.1 IP 0.7 IP 1.4 DAE 5.4 DAE 5.4 IP 0.7 BA 1.3 EHA 1.3 B 5 DB 5 EH 3.1 DB 3.6

B 1.2 B 1.2 IP 1.4 IP 1.4 IP 0.5 IP 0.5 IP 0.5 IP 0.5 IP 1 IP 1 B 0.6 B 1.2 RME 5 IPN 0.7 IP 0.4 IP 0.4 IPN 0.4 EHA 7.5 DB 4.6 B 3.2

IPN 0.5 IPN 0.5 B 1.2 B 1.2 IPN 0.5 IPN 0.5 IPN 0.5 IPN 0.5 IPN 1 IPN 1 IPN 0.2 IPN 0.4

0.015 RME 5 IPN 0.5 IPN 0.5 RME 5 DB 2.5 DB 2.5 RME 5 0.018 0.023 RME 5 0.026 0.018 0.017 0.025 RME 5 0.024 0.035 0.027 0.019 RME 2.5 RME 5 0.035 0.024 0.038 0.046

BA 2 IPN 0.4 IPN 0.4 DB 1.6 RME 5 IPN 0.2

RME 3.3

0.044 0.032 0.039

EHA 5

0.047 0.043 0.043

RME 6.2

0.055 0.043

Key: B=n-butanol; BA=butyl acetate; DAE=diisoamyl ether; DB=dibutyl ether; EH=2-ethyl-1-hexanol; EHA=2-ethyl hexyl acetate; Et=ethanol 99.9% by volume; EtW=ethanol 95% by volume; IP=isopropanol; IPN=isopropyl nitrate; Mk1=diesel motor fuel Mk1; RME=rapeseed oil methyl ether.

stop during the change of the particle lter this was followed by testing of test mixtures 1 to 24 with a warm engine start. After cleaning the fuel system with a new fuel, to ush the fuel used in the previous test, a new particulate lter was attached and the EU 2000 cycle was performed again. Measurements of the regulated emissions were performed according to a well-known test procedure (93/59/EEC, 1993) using the Horiba 9000 system. The test results are shown in Table 4.
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The second stage of the MTC tests was carried out on compositions selected from the rst stage. In some cases, minor corrections based on the results were made to the compositions. The test engine at the second stage was a heavy-duty Volvo D7 C290 Euro 2 equipped with Garret, nominal power 213 kW. The engine was run on the test compositions, simultaneously measuring exhaust emissions and performance properties. As before these were compared with the corresponding properties of standard
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Fig. 5 Schematic representation of the MTC EU 2000, NEDC driving cycle

Fig. 8 Torque produced at dierent percentage load at an engine speed of 2200 r/min. Data from the MTC test cycle according to ECE R49 for the compositions given in Table 5, as indicated in the legend

Mk1. The test cycle used was ECE R 49. The various features of the cycle are shown in Fig. 6. The test results are presented in Figs 7, 8, 9, and 10, and in Table 5.

Fig. 9 Power produced at dierent percentage load at an engine speed of 1320 r/min. Data from the MTC test cycle according to ECE R49 for the compositions given in Table 5, as indicated in the legend

Fig. 6 Schematic representation of the MTC test cycle according to ECE R 49

Fig. 10 Power produced at dierent percentage load at an engine speed of 2200 r/min. Data from the MTC test cycle according to ECE R49 for the compositions given in Table 5, as indicated in the legend

Fig. 7 Torque produced at dierent percentage load at an engine speed of 1320 r/min. Data from the MTC test cycle according to ECE R49 for the compositions given in Table 5, as indicated in the legend
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The biodiesel compositions which were selected at the second stage containing up to 15 per cent biocomponent and 85 per cent Mk1 diesel were tested at the SGS and Saybolt laboratories in Stockholm and Gothenburg according to standard methods to check
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Table 5 Test results for the alternative fuel test mixtures comprising oxygenates and diesel Mk1
Combustion properties
ID
1 2 3 4 5

Fuel compositions
Mk1 100 Mk1 85 Mk1 85 Mk1 85 Mk1 85

CO (g/kWh)
0.48

HC (g/kWh)
0.25 0.26 0.26 0.25 0.26

NO x (g/kWh)
6.07 6.05 6.12 6.20 6.11

CO 2 (kg/kWh)
0.69 0.68 0.68 0.69 0.68

PM (g/kWh)
0.046 0.045 0.044 0.046 0.041

Fuel (g/kWh)
209.1 211.3 213.2 213.1 214.0

Power (kW)
86.3 84.1 83.9 84.1 83.5

Bt 2.5 Bt 2.3 EH 4.6 EtW 3

DB 5 EH 3.1 DAE 5.4 Bt 5

EHA 7.5 DB 4.6 RME 5 IPN 0.4

0.47 RME 5 DB 1.6 EHA 5 0.45 0.44 0.45

Key: Bt=1-butanol; DAE=diisoamyl ether; DB=dibutyl ether; EH=2-ethyl-1-hexanol; EHA=2-ethyl hexyl acetate; EtW=ethanol 95% by volume; IPN=isopropyl nitrate; Mk1=diesel motor fuel Mk1; RME=rapeseed oil methyl ether

compliance with the requirements of the Swedish standard [27]. The test results are shown in Table 6. An analysis of the test results obtained at SGS and Saybolt shows that not all diesel mixtures comprising 15 per cent biocomponent and 85 per cent Mk1 with good performance properties can be used in Sweden. Lower alcohols and symmetric ethers of these alcohols, acetals and esters of the lower alcohols, and lower fatty acids cannot be recommended for further testing, even though they improve the combustion and exhaust emissions, because of their low ash point and consequent non-compliance with the standards for diesel fuel. New, previously unknown combinations of HCs and oxygen-containing compounds have been dened, providing the required diesel fuel performance properties and less harmful emissions. The major principle for the selection of these combinations

is that the oxygen-containing components to be mixed with the HC base fuel should include at least two compounds having at least four dierent oxygen-containing functional groups. Regarding the oxygen-containing components, higher alcohols and the corresponding ethers and acetals are recommended. For the esters one of the constituent compounds, either the alcohol or the fatty acid, can be lower, in the sense of fewer carbon atoms, and the second compound higher. In addition to those already mentioned, organic nitrates, peroxide compounds, and epoxides are recommended as oxygen-containing compounds. Such oxygenates in mixtures with HC diesel fractions provide the alternative fuel with the required performance properties, compliance with the standards requirements, and emission of combustion gases that contain fewer harmful pollutants.

Table 6 Properties of the alternative fuel test mixtures in comparison to standard Mk1 diesel
Fuel ID corresponding to Table 5
Property
Density 15C (kg/m3) Cetane number Cold lter, plugging point (CFPP) (C) Distillation initial boiling point (C) 95% distills at (C) Flash point (C) Sulphur content (mass) (mg/kg) Aromatic HCs content (% vol.); polycyclic (mass) (% wt.) Lubricity (mm)

Method
ASTM D-4052 EN ISO 5165 EN 116: EN ISO 3405 SS-EN 22719: ASTM D5453 SS 155116 IP391: 1995 ISO 12156

Standard for Mk1

820 max. 800 min. 51 min. 26 max. 180 min. 285 max. 56 min. 10 max. 5 max. 0.024 max. 460 max.

1
811 52.7 35 190.5 280.5 51 3 4.2 0.5 307

2
808.9 55 36 123.5 282.0 37 >2 3.8 >0.5 388

3
812.6 54.8 34 147.0 314.0 42 >2 3.9 >0.5 420

4
813.5 53.3 34 182.0 302.0 56 >2 3.7 0.5 406

5
811.5 57.2 35 78.0 279.0 26 3 4.7 >0.5 458

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According to current opinion on the nature of the combustion of oxygenated diesel fuels, it can be supposed that the discovered combination of the oxygen-containing components with the HC base fuel, which successfully combines a high content of bound oxygen and the necessary caloric value of HCs, provides favourable conditions in the combustion chamber of a diesel engine. The results of such combustion are the performance properties and the exhaust emissions of the new alternative fuel obtained. A patent application [28] valid in more than 60 countries of the world was led based on the results of the work performed. In some countries, including Sweden, the patent has already been granted. Certain compositions of the alternative diesel fuels were selected for further testing, including the study of the long-term reliability of performance in a standard engine. These tests are the closest possible approach to real-life working conditions. The eld tests were performed together with Svenska Lantmannen within the framework of a joint com pany, Agrofuel AB, which has been created specically for introducing alternative oxygen-containing biodiesel fuels to the market. One of the candidates, an alternative fuel to be called Biodiesel 15, comprising 15 per cent biocomponent and 85 per cent standard diesel, was selected for further testing. The alternative fuel compositions used were a mixture of the base diesel and biocomponent. The biocomponent is a specically selected combination of the oxygen-containing compounds originating from biomass and four dierent functional oxygencontaining groups. The base for the alternative fuel is either a standard Mk1 diesel or a standard European EN590 diesel, which when mixed with the biocomponent are compliant with the diesel fuel standards. The tests on Biodiesel 15 were performed on a standard six-cylinder engine Volvo DH10A285 with a nominal power of 210 kW. The data presented in Figs 11 to 14 show that replacing 15 per cent by volume of the HC base fuel by the biocomponent oxygenates eectively has no inuence on the performance properties of a heavy-duty engine compared to the operation of the same engine with a conventional EN590 or Mk1 fuel [29]. Figure 15 shows the dierence in the exhaust emissions and fuel consumption of a conventional diesel engine Volvo DH10A285 operating on reference and test fuels. The reference fuel used is 100 per cent diesel fuel comprising HCs, either EN590 or Mk1. The test fuel used is the diesel fuel Biodiesel 15 comprising 85 per cent by volume of either EN590 or Mk1
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Fig. 11 Comparison of the torque produced by a Volvo DH10A-285 engine with Mk1 and Biodiesel 15 based on Mk1

Fig. 12 Comparison of the torque produced by a Volvo DH10A-285 engine with EN590 and Biodiesel 15 based on EN590

Fig. 13 Comparison of the power produced by a Volvo DH10A-285 engine with Mk1 and Biodiesel 15 based on Mk1

and 15 per cent by volume of the blend comprising several oxygen-containing compounds obtained from biomass. Figure 15 shows that the test fuel is characterized by reduced net emissions of basically all harmful pollutants in the exhaust. The particulate matter reductions of 37 and 28 per cent for the Biodiesel 15 versions of EN590 and Mk1 respectively are highly interesting, especially since Mk1 is currently recognised as the most advanced and environmentally safe diesel fuel in the world. The reduction
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Fig. 14 Comparison of the power produced by a Volvo DH10A-285 engine with EN590 and Biodiesel 15 based on EN590

of net CO emissions is about 14 per cent compared 2 with that of both EN590 and Mk1. This substantial reduction results from the amount of CO which is 2 recycled through the biocomponent in the biosphere. The fuel consumption increases less than 2 per cent compared to that of the reference fuel [29]. The Volvo DH10A285 engine mounted on a test bench was disassembled and inspected by the engine specialists before and after the tests with Biodiesel 15. The engine specialists did not make any remarks in any of the tests.

Fig. 15 Comparison of the relative changes in emissions and fuel consumption of the Volvo DH10A-25 engine when using Biodiesel 15 versions of the standard diesel fuels EN590 and Mk1. The test cycle is ESC (European steadystate cycle), 13 mode type, Directive 1999/ 96/EC

Table 7 shows the specication of Biodiesel 15 in comparison to the requirements of the standards for the European grade EN590 and Swedish Mk1. The data from Table 7 show that the novel diesel fuel comprising up to 15 per cent by volume of biocomponents is within the requirements of the standards in force.

Table 7 Comparative properties of Biodiesel 15 and standard EN 590 and Mk1 fuels
Diesel fuel properties included in the standard
Density at 15 C (kg/m3)

Method
ASTM D-4052 ISO 3675 : 1998 ASTM D-613 ISO 165 : 1998 ASTM D-2500 EN 23015 : 1994 IP309 EN 116 : 1997 ASTM D-130 ISO 160 : 1987 ASTM D-86 ISO3405 : 1998

EN590 standard
845 max. 820 min. 51 min. 16 max. 26 max. 1

EN590 based Bio-diesel 15

Mk1 standard
820 max. 800 min.

Mk1 based Bio-diesel 15

808

836 51 min. 52.2 36 38 1 180 min. 180 280 63 16 max. 26 max. 1 36 38 1a 51.5

Cetane number Cloud point (C) CFPP (C) Copper strip corrosion (by scale) Distillation initial boiling point (C) evaporates at 180 C (%) 95% evaporated at (C) Flash point (C)

10 max. 340 max. SS-ISO 2719 EN 22719: 1993 ASTM D-2274 ISO 12205:1996 ASTM D4928-89m ISO 2937:1996 SS-EN ISO 4260 SS-EN ISO 14596 : 1998 SS155116 IP 391 : 1995 SS-EN ISO 12156-1 55 min.

5 325 62

285 max. 56 min.

Oxidation stability (g/m3) Water content (mass) (mg/kg) Sulphur content (mass) (mg/kg)

25 max. 25 max. 200 max. 350 max. 10 156 47 5 max. 0.024 max. 460 max. 200 max. 10 max.

152 2

Aromatic HCs content (volume) (%) polycyclic (mass) (%) Lubrication (mm)

11 max. 460 max.

1.5 396

4.2 0.02 382

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The homogeneity and stability of Biodiesel 15, which is a homogeneous solution without surfactants, was investigated by storing a sample of the fuel in a warehouse in Sweden under normal atmospheric conditions for two years. Regular analysis of the extracted samples demonstrated that the fuel properties did not suer any changes violating the standard. The alternative fuel Biodiesel 15 as developed was tested on a four-cylinder engine Valmet 420 DSG with a nominal power of 46 kW mounted on a test bench at the research institute VTT, Finland. The test was carried out over a prolonged period of operation of 500 h. Additionally, at the Statoil research centre in Norway the performance of a fuel pump in a test bench study lasting 1000 h was checked. Both the Valmet 420 DSG engine and the fuel pump, mounted on test benches, were disassembled and inspected by engine specialists before and after the tests of the new fuel. An analysis of the data obtained [30] showed that the new fuel does not have any negative eects on the performance of the engine and the fuel pump. The alternative fuel Biodiesel 15 has also been tested in winter conditions in the northern part of Sweden with ambient temperatures below 20 C. Two forest machines harvester Valmet 901 (ID2350) equipped with a standard four-cylinder engine Valmet 420 DWRE with a nominal power of 84 kW and forwarder Valmet 860 (ID4673) equipped with a standard six-cylinder engine Valmet 620 DS with a nominal power of 118 kW were operated on the new fuel. The operation of the machines on the alternative fuel Biodiesel 15 during more than two months did not cause any diculties and according to the drivers and operators was in no way dierent from the operation of the machines on standard diesel fuels. According to the opinion of the specialists inspecting the internal condition of the engines of the Valmet forest machines before and after operating on Biodiesel 15 there was no change in the engine conditions [31]. Positive results from the various tests of Biodiesel 15 enabled the start of eet testing in municipality buses in Sala, Sweden. The eet test lasted for a period of more than one year. There were 16 buses comprising 15 commuter buses and one service bus running on Biodiesel 15. The 16 buses included: four Scania L94UB, model year 2001 buses; two Scania CN113 City, model year 1997 buses; three Scania CN113 Forort, model years 1994 and 1995 buses; one Volvo D10LE City, model year 2001 bus; three Volvo B10M Forort, model year 1999 buses; two Volvo B10M Forort, model year 1993 buses; and one
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service bus, model year 1996. The mileage of all 16 buses during the entire period of the eet test amounted to 772 750 km. The operation of these 16 buses on the new alternative fuel was controlled throughout the whole eet test in accordance with the program Falttest av Agrodiesel 15 [32] developed by the Institute for Jordbruksoch miljoteknik and coordinated with the oil company Statoil and the engine producers Volvo and Scania. During the whole test period there were no negative remarks from the drivers, service personnel, or passengers regarding the operation of Biodiesel 15. In addition, the composition of the exhaust emissions from two of the buses were regularly tested in the specialised centre AVL MTC AB [33]. These two buses were a sixcylinder engine Volvo DH10A285EC96 installed in the Swedish municipal bus Volvo B10M Forort Euro 2, model year 1999, licence plate number HAA 177, and a six-cylinder engine Scania DC 902 Variant BO1 installed in the Swedish municipal bus Scania L94UB Euro 3, model year 2001, licence plate number RUR 880. The exhaust emissions tests demonstrated a reduction of particulates content during the operation of the new fuel, with a particularly large reduction in the small particulates. Other regulated exhaust emissions from the Volvo and Scania bus engines during the operation on Biodiesel 15 were on the same level as the exhaust emissions from the same engines operating on a standard Swedish Mk1 diesel fuel, apart from CO of course, which is much lower 2 than for Mk1. The Volvo DH10A285EC96 and Scania DC 902 Variant BO1 engines installed on the buses were inspected with endoscopes before and after the tests. The engine specialists did not make any remarks during any of the inspections. Measurements of the fuel consumption of all 16 buses during the whole period of the eet test during 20032004 showed that the consumption of Biodiesel 15 was 2 per cent lower than the consumption of standard Swedish Mk1 diesel by the same 16 buses during the identical period during 20022003, prior to the eet test. The biocomponents in Biodiesel 15 are produced from grain and other agricultural crops using approved technology. There is much set-aside land in Europe and European countries are interested in the development of agriculture since it provides additional jobs and helps maintain the countryside. In Nordic countries the raw material for producing biocomponents can be wood. The production of Biodiesel 15 is a simple blending of the base fuel and the biocomponents. The storage and handling of Biodiesel 15 is identical to Mk1.
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3 CONCLUSIONS A systematic approach to the problem of developing alternative fuels for standard diesel products has been used. The objectives were broadly intended to meet all the existing standards in force for diesel fuel, to be suitable for the existing inventory of diesel engines, and to extend the use of alternative oxygencontaining biodiesel fuels in diesel engines. These objectives have been fully met. In summary, the new alternative fuel contains 15 per cent of oxygenates, which can be produced both from petroleum and biomass. It completely satises all the properties of the standards in force for diesel fuel. It can be used in conventional diesel engines. It does not require any modications to the engine construction or in the materials used in the engine. A major benet of the alternative fuels presented in this paper is a substantial reduction in the amount of particulate matter in the engine exhaust with reductions of 37 per cent for Biodiesel 15 based on EN590 and 28 per cent for Biodiesel based on Mk1. The new alternative fuels can be recommended for operation in conventional diesel engines. Long-term tests show that the fuel is highly stable. Use of the fuel in 16 municipal buses in Sala, Sweden over a period of a year resulted in a 2 per cent reduction in fuel consumption. Finally, use of the alternative fuel containing 15 per cent oxygen-containing HCs obtained from biomass for operation in the existing inventory of conventional diesel engines would help to reduce considerably, by more than 15 per cent, the net emission of CO to 2 the atmosphere compared with operating the same engines on mineral-sourced fuel.

The authors are also grateful to SCA, who took part and provided forestry machines for the real-life tests, and also to the community of Sala, who took part and provided buses for the eet test of the fuel. Financial support from Swedish Energy Agency (Energimyndigheten), the European Commission, and Swedish Biofuels AB for carrying out parts of this work is gratefully acknowledged. The authors would also like to express deep gratitude to Tatiana Marandzheva of Tuchov Most, Kjell Lindqvist of Agroil AB, Kenneth Alness and Johan Berg of Svenska Lantmannen (SLR), Bjarne Lindberg, Bengt Tornblom of Statoil AB, Anders Laveskog of AVL MTC AB, Paivi Aakko and Marten Westerholm of VTT, and Rolf Berg of Befri Konsult for their substantial contribution to the accomplishment of this work.

REFERENCES
1 Kyoto Protocol to the United Nations Framework Convention on Climate Change, United Nations, Kyoto, Japan, 1997. 2 EU Commission Directive Proposal for a Directive of the European Parliament and of the Council on the promotion of the use of biofuels for transport, Brussels, 7 November 2001, Nr COM(2001) 547 nal. 3 Standard for diesel fuel EN590 Svensk Standard SS-EN 590. Automotive fuels Diesel Requirements and test methods, 31 March 2000 (Swedish Institute for Standards). 4 Mathur, H. B., Babu, M. K. G., and Reddy, B. P. Eect of methanol supplementation on exhaust emissions from swirl chamber diesel engine. Indian Inst. Technol. J. Thermal Engng., 1982, 2(3), 6372. 5 Johnson, R. T. and Stoer, J. O. Performance of stabilized diesel fuels containing alcohols and water in single and multicylinder direct injection engines. SAE Special Publications, 1983, S.P. 542, pp. 91104 (Society of Automotive Engineers, Warrendale, USA). 6 Wrage, K. E. and Goering, C. E. Technical feasibility of diesohol. Trans. ASAE, 1980, 13381343. 7 Baker, A. S. Block or graft copolymers and their use as surfactants. UK Pat. Application GB 2 002 400 (23 June 1978). 8 Oppenlaender, K., et al. Verwendung von Polyathern und Acetalen auf der Basis von Methanol und/oder Athanol als Dieselkraftstoe sowie diese Komponenten enthaltende Dieselkraftstoe. European Pat. A1 0 014992 (20 February 1980). 9 Baker, A. S. Emulsifying agents. UK Pat. Application GB 2 115 002 (1 February 1982). 10 Sweeney, W. M. and Herbstman, S. Method of extending hydrocarbon fuels including gasolines and fuels heavier than gasoline. US Pat. 4 356 001 (26 October 1982).
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ACKNOWLEDGEMENTS The authors would like to express their appreciation to Agro Oil AB, which provided part of the nancing for this project and organized its realization. The authors are also grateful to Statoil AB for taking part in the realization of this project. The assistance of AVL MTC AB was appreciated for the extensive tests carried out and for permission to reproduce Figs 5 and 6. The valuable assistance of VTT Technical Research Centre of Finland, SGS Sweden AB, Saybolt Sweden AB, and Miljoverkstaden, Skovde is also acknowledged. The authors would like to express their gratitude to the Swedish Institute for Jordbruks och miljoteknik, which developed the programme and organized the eet test of the fuel developed.
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11 Guibet, J. C., Born, M., and Vandecasteele, J. P. Utilisation de melanges desters alkyliques dacides gras derives dhuiles vegetales dans des compositions combustibles pour moteurs Diessel. France Pat. F 2 498 622 (30 July 1982). 12 Schwab, A. Diesel fuel aqueous alcohol microemulsions. US Pat. 4 451 265 (29 May 1984). 13 Craig, D. et al., Additives enabling blending of polar and non-polar fuel components. PCT Application WO 98/56878 (17 December 1998). 14 Killick, R. W. and Wrigley, P. R. Fuel blends. PCT Application WO 95/02654 (26 January 1995). 15 Sweeney, W. M. Diesel fuel containing cyclohexane and oxygenated compounds. US Pat. 4 378 973 (5 April 1983). 16 Seemuth, P. D. Diesel fuel composition. US Pat. 4 522 630 (11 June 1985). 17 Cunningham, L. J. Fuel compositions with enhanced combustion characteristics. US Pat. 5 405 417 (11 April 1995). 18 Liotta, F. J. and Montalvo, D. M. The eect of oxygenated fuels on emissions from a modern heavy-duty diesel engine. SAE paper 932734, 1993. 19 McCormick, R. I., Ross, J. D., and Graboski, M. S. Eect of several oxygenates on regulated emissions from heavy-duty diesel engines. Environ. Sci. Technol., 1997, 31, 11441150. 20 Sirman, M. B., Owens, E. C., and Whitney, K. A. Emissions comparison of alternative fuels in an advanced automotive diesel engine. SAE paper 2001-01-2048, 2000. 21 Sharp, C. A., Howell, S. A., and Jobe, J. The eect of biodiesel on transient emissions from modern diesel engines. Part 1 Regulated emissions and performance. SAE paper 2000-01-1967, 2000. 22 Sharp, C. A., Howell, S. A., and Jobe, J. The eect of biodiesel on transient emissions from modern

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diesel engines. Part 2 Unregulated emissions and chemical characterization. SAE paper 2000-01-1968, 2000. Natarajan, M., et al. Oxygenates screening for advanced petroleum-based diesel fuels: Part 1. Screening and selection methodology for the oxygenates. SAE paper 2001-01-3631, 2001. Gonzalez, M., et al. Oxygenates screening for advanced petroleum-based diesel fuels: Part 2. The eect of oxygenate blending compounds on exhaust emissions. SAE paper 2001-01-3632, 2001. Emission tests. Results from testing oxygenated diesel fuels 124. MTC AB Research report, Svenska Technoferm AB, Sweden, 1999. Emission tests. Results from testing oxygenated diesel fuels with Mk1 as reference in a Volvo D7 engine. MTC AB Research report, Svenska Technoferm AB, Sweden, 1999. Standard for Mk1 diesel fuel. Svensk Standard SS 15 54 35 Dieselbrannolja av miljoklass 1 och 2 for snabbgaende dieselmotorer, 2001 (Swedish Institute for Standards). Golubkov, A. and Golubkov, I. Motor fuel for diesel gas-turbine and turbojet engines. PCT Application WO 01/18155 A1 (15 March 2001). Testing of Biodiesel 15 on a test-bench engine. VTT Research report, Agrofuel AB, Sweden, 2000. Testing of Biodiesel 15 on a test-bench engine. VTT Research report, Agrofuel AB, Sweden, 2001. Feltforsk Biodiesel 15. PKS report, Statoil Nordisk Energi, Norway, 2001. Falttest av Agrodiesel 15, JTI Uppdragsrapport, Institutet for Jordbruks-och miljoteknik, Sweden, 2004. Emissions from two buses fueled with Agrodiesel 15 and EC1 Diesel fuel. Summary report, AVL MTC AB, Sweden, 2004.

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