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Fuel 87 (2008) 11411147 www.fuelrst.com

Regulated and non-regulated pollutants emitted from two aliphatic and a commercial diesel fuel
Efthimios Zervas
*
Department of Environmental Engineering, Democritus University of Thrace, Vas. Soas 12, 67100 Xanhi, Greece Received 6 March 2007; received in revised form 14 June 2007; accepted 14 June 2007 Available online 18 July 2007

Abstract Two synthetic aliphatic fuels and a commercial one were used on a Diesel vehicle to study the impact on exhaust regulated and nonregulated emissions. The two aliphatic fuels decrease hydrocarbons (HC), carbon monoxide (CO) and particulate matter (PM) emissions comparing to the reference fuel (commercial fuel), but they slightly increase nitrogen oxides (NOx) emissions. Total particle number and particle size distribution are almost the same for the three fuels used on the New European Driving Cycle (NEDC), however some differences are observed on steady speeds. The two aliphatic fuels decrease the emission of particulate sulphates, of nitrous oxide (N2O), of carbonyl compounds and methane (CH4) comparing to reference fuel. Carbon dioxide (CO2) emissions of the three fuels are similar. 2007 Elsevier Ltd. All rights reserved.
Keywords: Diesel; Exhaust emissions; Non-regulated pollutants; FischerTropcsh; Aldehydes

1. Introduction During the previous years an important research of fuel eects on emissions took place on both gasoline and Diesel engines. Emissions of regulated pollutants but also nonregulated ones, such as carbonyl compounds [15], polycyclic aromatic hydrocarbons (PAHs, [6]) or organic acids [2] emitted from Diesel engines were studied from several authors. Due to increased importance given on the emissions of nano-particle, particle number and size distribution of Diesel exhaust gas are also reported in several studies [7,8]. Several works are referred to alternative Diesel fuels, such as bio-fuels [9,10] and synthetic ones, such as FischerTropsch fuels [1115]. Even if the number of works on alternative synthetic Diesel fuels, such as FischerTropsch, constantly increases during last years, most of these articles are focused on the

Tel.: +30 24510 79392. E-mail address: ezervas@env.duth.gr

emission of regulated pollutants. The published results are some times contradictory, especially the results of NOx emissions, where some authors report an increase using FischerTropsch fuels [12,13] or a decrease [11]. Such contradictory results exist also in the case of PM emissions [15]. The main reason is that these studies used dierent fuels, vehicles and experimental conditions [15]. Some works study the emission of total number and size distribution of nano-particles emitted from engines feed with FischerTropsch fuels [12]; however, there is a lack of information about the other non-regulated pollutants, such as carbonyl compounds, N2O, or methane. In this work, two synthetic aliphatic fuels and a commercial Euro3 one were used on a vehicle equipped with a Diesel engine operating on the New European Driving Cycle (NEDC) and on three steady speeds. Emissions of regulated and non-regulated pollutants, such as particle number, median particle diameter and particle size distribution, carbonyl compounds, N2O, methane, CO2, particulate sulphates and insoluble organic fraction (IOF) were measured. The regulated and non-regulated emissions of the three fuels were compared and discussed.

0016-2361/$ - see front matter 2007 Elsevier Ltd. All rights reserved. doi:10.1016/j.fuel.2007.06.010

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2. Experimental section A passenger car equipped with a 1.9 L Euro3 Diesel engine and a commercial Diesel oxidation catalyst (DOC) was used for these tests, which were performed on the NEDC following the ocial European regulations [16]. Complementary tests on three steady speeds of 50 km/h, 3rd gear, 50 km/h, 4th gear and 100 km/h, 5th gear, were also performed. Three dierent fuels were used for these tests: a reference fuel (commercial Euro3 Diesel fuel), named R and two synthetic aliphatic ones, named A and B. These fuels contain only parans and no aromatic or naphthenic compounds. Table 1 shows the main characteristics of these fuels. Fuel R is used rst, followed by fuel A and then by fuel B. Between each fuel, the fuel tank is completed emptied and cleaned. Fuel lters were also changed. Before each fuel test, the vehicle runs for 200 km with this fuel to eliminate possible memory eects. Analysis of regulated pollutants was performed according to European regulations [16]. Particle size distribution was determined on NEDC with an Electrical Low Pressure Impactor (ELPI) and on the three steady speeds with a Scanning Mobility Particle Sizer (SMPS). Particulate sulphates were extracted from particulate matter and analyzed by Ionic Chromatography (IC). N2O is analyzed by Gas Chromatography using Electron Capture Detection (GC/ ECD). Exhaust methane is analyzed by Gas Chromatography/Flame Ionisation Detector (GC/FID). Carbonyl compounds are collected in 2,4-di-nitro-phenyl-hydrazine (DNPH) solution in acetonitrile and the nal solution was analyzed by High Performance Liquid Chromatography using Ultra-Violet detection (HPLC/UV). Regulated
Table 1 Characteristics of the three fuels used (nm: not measured) Characteristic Density at 15 C (kg/m ) Viscosity at 40 C (mm2/s) Cetane number S content (mg/kg) Water content (mg/kg) Cold lter plugging point (C) Distillation curve (C) Initial point 5% 10% 20% 30% 50% 70% 80% 90% 95% Final point Residual (% vol.) Mono-aromatics (% vol.) Bi-aromatics (%, vol.) Total aromatics (%, vol.) H/C
3

pollutants were analyzed upstream and downstream the oxidation catalyst (engine-out and tail-pipe emissions), while only the tail-pipe emissions non-regulated pollutants were analyzed. More details about the methods used can be found elsewhere [1719]. 3. Results and discussion 3.1. General presentation of regulated pollutants emission Fig. 1 shows the tail-pipe emissions of the four regulated pollutants for the three fuels used. The two aliphatic fuels A and B emit signicant lower emissions of HC, CO and PM than the reference fuel, while they increase very slightly NOx emissions. Fuels A and B decrease HC emissions 68% and 71% respectively, CO emissions 71% and 76% respectively and PM emissions 34% and 28% respectively comparing to fuel R. The corresponding increases in NOx emissions are very low: 1.3% and 6.5%. However, these results are within the repeatability limits of NOx determination. 3.2. Analysis of HC, CO and PM emissions Some previous works report a decrease of HC, CO and PM exhaust concentration: using a reference and a hydrotreated fuel [2] or from the use of FischerTropsch fuels (a 5060% decrease for the three pollutants [11] and also on USA driving cycles [12]). However, another work reports an increase of 430% of CO and HC exhaust concentrations at high speed/load steady engine points and a decrease of 3077% at low speed/load using a Fischer Tropsch fuel [13], indicating that the impact of these fuels
0.5

R 832.0 2.78 52.8 206 nm 27 188 210 225

A 775.7 2.39 71.3 <1 23 28 160 186.2 199 219.2 236.2 264 290.7 305 322.8 335.2 344.3 1 0.2 <0.1 0.2 2.18

B 775.7 2.68 74.8 <10 16 6 189.2 206.6 213.2 227.4 241.7 271.6 302.9 318.9 337.3 349.3 359.9 1 <0.1 <0.1 <0.1 2.24
0.4

R A B

Exhaust emissions (g/km)

0.3

0.2

271

0.1

329 345 356 nm nm nm 1.92

HCeo

COeo /4

HCtp

COtp

NOx

PM

Fig. 1. Engine-out and tail-pipe emissions of the four regulated pollutants of the three fuels used (eo: engine-out, tp: tail-pipe, CO engine-out is divided by 4).

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are not the same at each engine point. This last work reports a decrease of 1758% of PM emissions at all engine points. However, another author conducted experiments on a shock tube and showed that FischerTropsch fuels generally decrease PM missions comparing to a reference Diesel fuel; however, an increase is observed at high pressures [20]. A review study [15] reports than HC, CO and PM emissions generally decrease with the use of Fischer Tropsch fuels, however an increase of PM emissions is sometimes observed. It must be noted that dierent FischerTropsch fuels, dierent engines and dierent experimental conditions were used in these studies, so the obtained results cannot be compared very easily. It is reported that HC and CO emissions depend on the cetane number [21,22]. A higher cetane number reduces ignition delay and consequently the amount of fuel burned in the premixed combustion phase, leading to a reduction of air/fuel inconsistencies, resulting lower HC and CO emissions [13]. Other parameter is the aromatic content [23], which increases HC and CO emissions. As the two aliphatic fuels have higher cetane number and very low aromatic content, HC and CO emissions are expected to be lower than the commercial reference fuel, which is the case. Another parameter decreasing HC emissions is the distillation curve. A fuel with lower distillation curve has improved vaporisation and thus decreased wall wetting which leads to decreasing HC emissions [24]. This is the case of the two aliphatic fuels used in this study comparing to the reference one. The decrease of HC and CO tail-pipe emissions is due to a decrease of engine-out emissions (Fig. 1), indicating that the combustion of the two aliphatic fuels is dierent from the combustion of fuel R; however, the combustion temperature of the two fuels is similar, as NOx emissions does not change signicantly. It must be noticed that the decrease of HC and CO emissions is lower in the case of engine-out emissions than in the case of tail-pipe emissions. The decrease of HC engine-out emissions is 51% and 57% for the fuels A and B respectively comparing to 68% and 71% for the tail-pipe emissions. This statement indicates that the two aliphatic fuels emit dierent engine-out hydrocarbons, which are better oxidized on the oxidation catalyst leading to a higher decrease of tail-pipe total HC. The decrease of engine-out CO is 39% and 46% for the fuels A and B respectively, comparing to 71% and 76% decrease of tail-pipe emissions. This must be to a synergy between CO/HC conversions on the oxidation catalyst. As these fuels have dierent engine-out HC and CO emissions and dierent exhaust HC composition, the temperature on the oxidation catalyst will also be dierent, leading to dierent oxidation eciencies. Fig. 2 shows that there is a clear, almost linear, decrease between HC and CO emissions (engine-out and tail-pipe) and fuel H/C ratio. A very slight decrease is also observed with fuel H/C ratio in the case of PM emissions. The same decrease is already observed in the case of a spark ignition engine [25].

10

Exhaust concentration (g/km)

HC engine-out HC tail-pipe CO engine-out CO tail-pipe NOx tail-pipe PM tail-pipe

0.1

0.01 1.9 2 2.1 2.2 2.3

H/C fuel ratio

Fig. 2. HC, CO, NOx and PM emissions as a function of fuel H/C ratio.

3.3. Analysis of NOx emissions Fuels A and B increase slightly NOx emissions on the NEDC comparing to fuel R, but this increase is within the repeatability limits. Some older studies report that NOx emissions decrease with cetane number [21,23]; however, this is not always valid in newer vehicles and fuels [22]. No such tendency is found in our tests. NOx emissions depend on combustion temperature and oxygen concentration, which are inuenced by several parameters, such as fuel structure, injection timing, etc. [14]. Miyamoto et al. [26] correlated the H/C fuel ratio with NOx emissions when the ignition delay remained constant, and attributed the dierences in NOx emission to dierence of the heat release rate, however Szybist et al. [14] showed that this cannot be the main factor for NOx emissions. In our case, there is a slight increase in NOx emissions on NEDC with H/C ratio (Fig. 2); however, the three points used are not sucient for such a correlation. All previous works do not agree on the impact of FischerTropsch fuels on NOx emissions. Some works report a decrease of NOx emissions of 1525% on the NEDC using FischerTropsch fuels [11], or an increase of 214% at steady speed/load points [13] or an increase of 112% on USA driving cycles [12]. Szybist et al. [14] indicates than a FischerTropsch fuel has about 20% lower NOx emissions than a reference fuel at high engine loads, while at low loads this trend is inversed and an increase of up to 60% is observed. These dierences depend also on the injection timing. The same work reports that as they are dierences in injection timing due to the dierent compressibility of each fuel, NOx emissions are roughly the same in the case of high load if they are reported to the same injection timing. However, a 100% FischerTropsch fuel has lower NOx emissions than the other fuels studied.

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1E+015
R A B

PM number (dN/dlogDP, 1/km)

The same correlation is not valid in the case of low load. More examples of works using FischerTropsch fuels and their impact on exhaust emissions can be found in a review study [15]. It must be noticed that fuel is not the only parameter, as engine and experimental conditions used also inuence NOx emissions. 3.4. Particle number and size distribution on the NEDC Fig. 3 shows the total particle number, determined by ELPI, emitted on the NEDC from the three fuels used. It is clearly shown that the two aliphatic fuels emit the same particle number as the reference one. This gure shows that the dierence on particulate mass emissions between the two aliphatic fuels and the reference one cannot be explained by a dierence on the emitted particle number. The size distribution of the exhaust particles emitted from the three fuels is very similar (Fig. 4). This statement indicates that the dierence on the emitted particulate mass is apparently due to small dierences of the upper size fraction of emitted particles. The mass corresponding to these big particles is very high comparing to the mass of smaller particles [27] and a small dierence on the emitted number can lead to important particulate mass dierence. It must be noted that ELPI repeatability is very low at these particle sizes [17,18]. As fuels A and B have lower sulphur content, it is expected that they will have lower nucleation-mode particle emissions, as sulphates enhance the formation of these particles [13]. This is not the case in our tests, as the three fuels have the same particle size distribution, indicating that sulphates are not the only source of nano-particles nucleation and other sources, as HC condensation, are also responsible for the nucleation. Schaberg et al. [13] reports that sulphates can be formed on the oxidation catalyst even with
5E+014

1E+014

1E+013

1E+012

1E+011

1E+010

1E+009 0.001 0.01 0.1 1 10

Dp ( m)
Fig. 4. Particle size distribution on the NEDC from the three fuels used. ELPI measurements.

fuels with very low sulphur content. It is also reported that signicant reduction on PM emission can be observed when the sulphur fuel content decreases from 3000 to 500 ppm, but this decrease is very low as sulphur content approaches zero [28]. Another work reports that a FischerTropsch fuel emits a lower particle size distribution than a reference fuel on USA driving cycles [12] and especially at the region of smaller particles. 3.5. Particulate mass, particle number and size distribution on steady speeds A more detailed investigation about particle emissions is curried out on three steady speeds: 50 km/h, 3rd gear, 50 km/h 4th gear and 100 km/h 5th gear. Fig. 5, bottom curves, shows that the decrease of PM emissions from the use of fuels A and B on the NEDC is mainly due to high speed of 100 km/h, 5th gear. At the speed of 50 km/h, 3rd gear, reference fuel emits lower PM emissions than the other two fuels: 3.5% lower than fuel A and much lower (40%) than the emissions of fuel B. However, looking closer to the repeatability limits of PM measurement, which is about 30% [17,18], the change of fuel A is not signicant, while fuel B clearly emits higher PM emissions than fuel R. Keeping the same vehicle speed and changing gear (50 km/h, 4th gear), PM emissions decrease for the three fuels. The PM emissions of fuel R are 30% lower in this case than the rst steady point. Both aliphatic fuels emit now lower PM emissions than fuel A: 34% and 22% for the fuels A and B respectively, which are at the lower limits of repeatability measurements. In the case of the high speed of 100 km/h, 5th gear, PM emissions increase 54% in the case of fuel R comparing to the rst

Total particle number (1/km)

4E+014

3E+014

2E+014

1E+014

0 R A B

Fig. 3. Total particle number emitted on the NEDC from the three fuels used. ELPI measurements.

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120

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Median diameter (nm)

R A B

80

40

5E+014

4E+014

3E+014 2E+014 1E+014 0.04

Exhaust PM

0.03 0.02 0.01 0 50/3 50/4 100/5

Fig. 5. Bottom bars: PM emission on three steady speeds from the three fuels used. Middle bars: total particle number emitted on three steady speeds from the three fuels used (ELPI measurements). Upper bars: median diameter of the particles emitted on three steady speeds from the three fuels used (SMPS measurements). 50/3: 50 km/h, 3rd gear, 50/4: 50 km/h, 4th gear, 100/5: 100 km/h, 5th gear.

steady speed. In this high speed, a clearly signicant decrease is observed between fuel R and the two aliphatic fuels: a 53% and 51% decrease of PM emissions for fuels A and B respectively comparing to fuel R. However, as in the case of NEDC measurements, total particle numbers at these steady speeds do not follow particulate mass measurements. Fig. 5, middle curves, shows a decrease of particle number emitted from the two aliphatic fuels comparing to fuel R at the two low speeds of 50 km/h. This decrease is lower in the case of fuel B than in the case of fuel A and is outside or at the lower limits of repeatabil1E+014

ity. At the high speed of 100 km/h, 5th gear, the opposite trend is observed: fuels A and B emit higher particle numbers than fuel R, however, these values are within the repeatability limits. Schaberg et al. [13] reports the opposite trend: a decrease of total particle number using a Fischer Tropsch fuel at high speed/load steady engine operation points and an increase at low ones. However, fuels and engine used are not the same and a direct comparison is not evident. The median diameter of these measurements, determined by SMPS, is shown at the upper part of Fig. 5. For the three steady speeds, there is no signicant dierence between the median diameters of the three fuels. Median diameter is 9297 nm in the case of the rst steady speed and decrease to 5156 nm and 5361 nm, respectively, at the second and third point. Fig. 6 shows that, at the three steady speeds, there is no signicant dierence between the particle size distributions of the three fuels. These distributions were determined by ELPI and remain within the repeatability of this instrument. SPMS measurements also show no signicant dierence, as the dierences on the particle size distributions remain within the repeatability limits. Schaberg et al. [13], reports that a FischerTropsch fuel has lower number of particles less than 50 nm than a reference one due to the lower sulphur content of this fuel, however this result is not conrmed here. The results of our study show that there is no possible to correlate the particulate mass and particle number on NEDC measurements or steady speeds. A previous work also showed that such a correlation is not evident [27]. These results show that these three fuels must not be compared only on the NEDC as the trends of each fuel on each steady point are completely dierent. This statement indicates that much work is still necessary to nd out the real world emissions of alternative fuels. 3.6. Emissions of non-regulated pollutants on the NEDC Fig. 7 shows the emissions of the other non-regulated pollutants on the NEDC. It is clearly shown that two aliphatic fuels have signicantly lower emission of particulate
1E+014
R A B

Particle number

emissions (g/km)

(1/km)

Particle number (dN/dlogDp, 1/km)

Particle number (dN/dlogDp, 1/km)

Particle number (dN/dlogDp, 1/km)

R A B

1E+014

R A B

1E+013

1E+013

1E+013

1E+012

1E+012

1E+012

1E+011

1E+011

1E+011

1E+010

1E+010

1E+010

1E+009

50 km/h, 3rd gear

0.001 0.01 0.1 1 10

1E+009

50 km/h,4th gear
0.001 0.01 0.1 1 10

1E+009

100 km/h, 5th gear

0.01 0.1 1 10

0.001

Dp ( m)

Dp ( m)

Dp ( m)

Fig. 6. Particle size distribution on three steady speeds from the three fuels used. ELPI measurements.

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16 R A B 12

E. Zervas / Fuel 87 (2008) 11411147

SO4 N2O Form Acet Total IOF

CO2

CH4

Fig. 7. Emissions of non-regulated pollutants on the NEDC from the three fuels used. Form: formaldehyde, acet: acetaldehyde, total: total carbonyl compounds, N2O and SO4 in lg/km, formaldehyde, acetaldehyde, total carbonyls and CH4 in mg/km, CO2 in g/km/10, IOF in %.

sulphates than the reference one. This is due to the very low sulphur content of the two aliphatic fuels: lower than 10 mg/kg against 206 mg/kg in the case of the reference fuel. The two aliphatic fuels also decrease the emission of N2O comparing to the reference fuel. The R fuel emits 9.7 lg/km while the A and B fuels 7.7 lg/km and 6.3 lg/ km, respectively. It must be noticed that the repeatability of this measurement is 27% and the above decreases: 20% and 35%, respectively, for fuels A and B comparing to fuel R, are quite at the lower limits of repeatability. The order of magnitude of N2O emissions is quite similar to another study [5], which reports 816 lg/km of N2O using a commercial fuel. Another work using a FischerTropsch fuel on USA driving cycles [12] reports a decrease of 38% of N2O comparing to the emissions of a reference fuel on FTP; however the emissions on the US06 and Highway driving cycles are similar between reference and Fischer Tropsch fuels. The two aliphatic fuels also show a signicant decrease on the emission of carbonyl compounds comparing to fuel R. While this last one emits 14.5 mg of total carbonyl compounds per km, the A and B fuels emit only 4.5 and 1.6 mg/ km, which corresponds to a decrease of 69% and 89%. Naturally, this decrease is also signicant in the case of the two rst aldehydes, formaldehyde and acetaldehyde. Fuel R emits 8.4 and 4 mg/km of HCHO and CH3CHO respectively, while the emissions of the two aliphatic fuels A and B are as low as 2.7 and 0.8 mg/km, respectively, in the case of fuel A and 1.2 and 0.6 mg/km, respectively, in the case of fuel B. Other works also reports a decrease in exhaust concentration of carbonyl compounds using a reference and a hydro-treated fuel [2], or from the use of a FischerTropsch fuel on the USA driving cycles [12]. It

must be noted that formaldehyde and acetaldehyde decrease with H/C fuel ratio also in the case of a spark ignition engine [19]. Formaldehyde is the major carbonyl compound as it corresponds to 5260% of total carbonyl compounds, while acetaldehyde to 2737% [5]. There is no clear tendency between aliphatic and reference fuels for those percentages. Total aldehydes correspond to about 43% of total HC in the case of R and A fuels, but this percentage falls to only 17% in the case of fuel B. A previous study [3] reports that, for dierent vehicles tested on FTP, the ratio formaldehyde/acetaldehyde remains always constant and around 7/3, which is 2.33. In our case, the ratio HCHO/CH3CHO is 2.1, 2.2 and 1.4 for the fuels R, A and B, respectively. The IOF percentage of the emitted particles of the three fuels is exactly the same: 9%, indicating that the mechanism of IOF formation is independent of fuel composition and depends more on phenomena linked to combustion. Fig. 7 shows that the CO2 emissions of the three vehicles are practically the same. However, other authors report a decrease of CO2 emissions using a FischerTropsch fuel comparing to a reference one ([13], but only on steady engine operation points, [12] or the USA driving cycles). Methane emission is lower in the case of aliphatic fuels than in the case of the reference one, as it decreases from 9 mg/km in the case of R fuel to 7.5 and 7 mg/km in the case of fuels A and B, respectively. Another study reports similar exhaust concentrations of methane: 69 mg/km, using a Euro3 commercial fuel [5]. The corresponding decrease is 16% and 22% for the fuels A and B, respectively, relatively to fuel R. These values are lower than the corresponding decrease of the tail-pipe emissions of total HC (68% and 71% for the fuels A and B, respectively), indicating that the decrease of total HC emissions corresponds mainly to heavier HC. For this reason, exhaust methane corresponds to 27% of total HC emissions in the case of fuel R, while this percentage increases to 71% and 73% in the case of fuels A and B, respectively. A previous work [2] reports also a decrease in methane concentration, but an increase of its percentage in total HC using a reference and an hydro-treated fuel; however, Schubert et al. [12] reports a decrease of methane emissions from the use of a FischerTropsch fuel comparing a reference one but only on the FTP, while the emissions on the Highway and US06 driving cycles remain the same. 4. Conclusions Two synthetic aliphatic fuels and a commercial Euro3 one were used on a vehicle equipped with a Diesel engine operating on the New European Driving Cycle (NEDC) and on three steady speeds. Emissions of regulated and non-regulated pollutants of the three fuels were measured and compared. The obtained results show a signicant decrease of tailpipe HC and CO emissions of the two aliphatic fuels comparing to the reference one, of the order of 70%. The emis-

Exhaust emissions

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sions of PM are also decreased of the order of 30%; however there is slight increase (16%) of NOx emissions. There is an almost linear decrease between HC and CO emissions and fuel H/C ratio. The emissions of PM show also a very slight decrease with fuel H/C ratio, while NOx emissions a slight increase. Total particle number of the NEDC and particle size distribution is almost the same for the three fuels used. PM emissions of the two aliphatic fuels are lower than the reference fuel at the high speed of 100 km/h, 5th gear, while the trend is opposite at lower speeds. There is no correlation between PM and particle number at these steady speeds. For the three steady speeds, there is no signicant dierence between the median diameters and the size distributions of the three fuels. The two aliphatic fuels have signicantly lower emission of sulphates than the reference one due to their lower sulphur content. The two aliphatic fuels also decrease the N2O emissions comparing to the reference fuel by 20 35%, carbonyl compounds emissions by 6989%, and methane emissions by 1622%. Particulate IOF percentage and CO2 emissions of the three fuels are very similar. References
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