Fuel Properties Effects on Current Diesel Vehicle Technology Emission

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1 Fuel Properties Effects on Current Diesel Vehicle Technology Emission L. Ntziachristos, Z. Samaras Laboratory of Applied Thermodynamics Aristotle University, Thessaloniki GREECE INTRODUCTION Great attention has been lately focused on the potential technical solutions to improve the exhaust emission characteristics of diesel engines. This is in part due to the increasing share of diesel passenger cars in the market, which benefit from lower CO 2 emissions than their gasoline counterparts, in an effort to meet greenhouse gas reduction targets [1]. Research spreads into three directions: reduction of in-cylinder pollutant formation, development of aftertreatment devices and improvement of fuel specifications. Directive 98/70/EC regulates fuel specifications for the automotive sector in Europe today. For diesel fuel, it provides maximum permissible limits for density, 95% distillation point, polycyclic aromatic hydrocarbons and sulphur content, as an outcome mainly of the EPEFE programme [2]. However, several other physical and chemical properties of the fuel, such as surface tension, viscosity, oxygen content etc., may influence the spray development and the combustion process in a diesel engine. Hence, there is a great interest to explore whether further reductions in diesel engine emissions may be achieved by adjusting fuel properties, which are left uncontrolled today by the relevant legislation. In this paper we examine the effects of a large fuel property matrix on the emission characteristics of a Euro 3 passenger car to identify the potential for further emission improvements of current technology vehicles. METHODS Fuel Matrix The fuel matrix consisted of 12 fuels, 9 of which were not oxygenated while three were oxygenated ones. Each fuel was blended with the target to change only one physical property to the rest. Obviously, it was not possible to change the physical properties of the fuels while not modifying their chemical character. Therefore, one should distinguish between chemical and physical effects on emissions. Table 1 provides a summary of the main fuel properties examined. In addition to the base fuel (REF), there are two fuels of decreasing surface tension (S- and S=) of variable density (D- and D+) and viscosity (V- and V+) and two fuels similar to the REF one but with different proportion of paraffins and naphthenes (P and N). The three oxygenated fuels were produced by blending the reference fuel with RME (ester) or diglyme (ether) to achieve different oxygen content. Vehicle and lab setup The vehicle tested was a Renault Laguna 1.9 dci equipped with a turbocharged common rail engine (max pressure 1350 bar) with exhaust gas recirculation (EGR) and two oxidation catalysts (pre-cat and main cat). This technology corresponds to the state of the art today for 1

2 diesel engines in passenger cars and was considered representative to explore the effect of fuel properties on today's vehicles. For this reason, we did not calibrate the engine parameters to different fuels. The vehicle was placed on the chassis dynamometer and was tested following a strict protocol which involved different driving cycles for conditioning with each new fuel and measurements over regulated and real-world cycles developed in the European Artemis project [3]. Two repetitions of a measurement day were performed with each fuel. Table 1: Fuel matrix and main properties. Acronym REF S- S= D- D+ V- V+ P N RME Digl.3 Digl.9 Paraffins, % w t Naphthenes, % w t Aromatics, % w t Density, 15 C, kg/m Distillation, C, 5% Distillation, C, 50% Distillation, C, 95% Cetane number Viscosity +40 C, mm 2 /s Surface tension + 20 C mn/m Heat of combustion, MJ/kg Compressibility, 60 bar, 20 C [10E-5 bar -1 ] C/H ratio Oxygen content, % w t, Sulfur content, ppm w t Sampling and Analysis All regulated pollutant measurements (CO, HC, NO x, PM) were conducted according to the legislation, sampling from a dilution tunnel (CVS). However, in order to obtain a more detailed look on the physical properties of the particles emitted, we utilized the sampling methodology and the system developed in the European Particulates project [4]. This system (Figure 1) consists of a porous dilutor where dilution occurs directly at the sampling tip at a nominal value of 12.5:1 to eliminate particle losses and decelerate aerosol activity downstream of the sampling point. Subsequent dilution stages further reduce particle concentration to levels within the range of the aerosol instrumentation. Silica gel Filter CPC SMPS or DMA/CPC Charcoal CONTROLLER SP UNIT ST ET EP DT CT Exhaust gas MFC Pressure regulators 3 bar Cooling agent Ejector dilutors Ageing chamber TD DC DGI Fig. 1 CO2 anal. (raw) On/off valve CVS CO2 anal. (dil) ELPI Bypass Trap Flowmeter Dilution Air Line Sample Line Pump Schematic of the sampling system used for exhaust aerosol sampling. 2

3 This sampling system allows the measurement of several particle properties. The numberweighted size distribution of solid particles was recorded with the ELPI sampling downstream of a thermodenuder, which removed volatile and semivolatile species. A CPC was used to record the total particle number concentration, including solid and non-solid particles. A diffusion charger (DC) was calibrated and used to monitor the total active surface of exhaust aerosol [5]. An SMPS provided the size distribution of the total aerosol over steady state tests and a gravimetric impactor (DGI) produced the mass-weighted size distribution, averaged over a test. Statistical Methods The results collected with all fuels for all pollutants and particle properties examined were analyzed with statistical methods to capture the important effects. All measurements were scrutinized with Analysis of Variance (ANOVA) to reveal the statistically significant fuel effects. This method examines the mean values of different samples to identify where true differences are established, given the variability of the measurements. Additionally, a Principal Component Analysis (PCA) was applied to demonstrate correlations between the fuel properties and the corresponding emissions. PCA formulates combinations of fuel variables (components) with which to correlate emissions. This allows reduction of a multidimensional correlation space to a fewer dimensions matrix, which improves understanding of the different associations between fuels and emissions. RESULTS Figure 2 provides an overview of the general emission performance with use of all fuels over the European legislated cycle (NEDC). Results are presented on a PM NO x chart which should be considered as the main tool in evaluating any diesel emission control measure. For reference, the type approval, Euro III and Euro IV diesel emission limits are also shown on the chart. Error bars correspond to different measurements Euro III 0.45 Digl Type approval D- ST- ST= NOx [g/km] 0.35 Digl.3 N V- D + REF V Euro IV RME 0.25 Fig PM [g/km] PM-NOx trade-off for different fuels examined over the regulated cycle. Solid blocks correspond to the emission standards of 2000 (Euro III) and 2005 (Euro IV) and the type approval value for the vehicle examined. Solid lines are a guide to the eye. 3

4 The usual PM NO x trade-off is also observed in the case of the fuel matrix. There are very few fuels that can give concurrent reductions in both pollutants over the reference fuel and none non-oxygenated one that can give differences outside the variability of the measurements. It is obvious that the solid line, along which lie all fuels, is almost vertical to the line that connects the two emission standards. This means that approaching the Euro IV targets by changing fuel specifications only is not possible without tuning the engine parameters. Moreover, ANOVA identified no statistically significant differences between the non-oxygenated fuels. Oxygenated fuels were found to consistently bring reductions to PM and to increase NO x (ether fuels) as oxygen content increased. This was further verified by ANOVA. The positive effect of oxygenated fuels on PM was extended to all particle properties, including total number and surface. The solid particle distributions measured led to the conclusion that this is due to a reduction in the volume of accumulation mode particles. This is consistent with a chemical mechanism for soot suppression when carbon-oxygen bonds are present [6]. Table 2 provides a summary of the effect of different fuel properties on the main gaseous pollutants, fuel consumption and particle properties, recorded over different driving cycles. Significant effects are only seen for the highly oxygenated fuels, despite the relatively large change of conventional diesel properties. This indicates that current technology is not much sensitive to diesel fuel properties, excluding the addition of oxygen in the fuel. Table 2: Summary of the fuel effect on diesel exhaust emissions. Arrows designate increase in emissions when the value of a property increases ( ) and vice versa ( ). Fuel Matrix NO x PM CO 2 Fuel Consumption Active Surface Solid Total Surface tension 13% 10% 3% 2% n/a 10% Density 15% 20% 15% 5% 10% Viscosity both fuels reduced NO x up to 10% 20% 15% 15% 10 % RME -13% -12% 2% 5% 10% Diglyme 25% 55% 10% 50% 35% 25% The fuel matrix was built in order to try to isolate the effect of different physical properties on emissions. However, this was achieved by blending different chemical components (except of surface tension reduction which was achieved by using an additive). Hence, it was not possible to identify whether a positive effect originated from changing the shape of the diesel spray or by inhibiting the chemical mechanism of pollutant formation. To separate between the two, we utilized the PCA to examine how the chemical character of the fuel is associated with pollutant emissions. This is demonstrated in Table 3 where the same convention to Table 2 is followed. Table 3 delivers several messages. The most important is that NO x emission is sensitive to the fuel chemical character and in particular to the paraffins / naphthenes ratio, with NO x increasing in the same trend with this ratio. PM was found less affected by the chemical character and mainly paraffin increase and tri+-aromatic decrease led to significant reductions of particles. The same trends were confirmed by aerosol measurements, with all particle properties increasing with the aromaticity of the fuels (and partially with di- 4

5 naphthenes). On the other hand, increasing fuel aromaticity seemed to improve fuel efficiency. Table 3: Qualitative effect of fuel chemical character on diesel exhaust emissions. Property NO x PM CO 2 Fuel Consumption Active Surface Solid Total Mono-aromatics Di-aromatics Tri+-aromatics Poly- aromatics Total aromatics Total paraffins Total naphthenes Mono-naphthenes Di-naphthenes Tri-naphthenes C/H ratio CONCLUSIONS This study showed that a current passenger car, equipped with an advanced common rail injection engine, seems to be rather insensitive to the physical properties and the chemical character of diesel fuels. Effects of physical properties and chemical composition are found in the ±10% range for PM and NO x, when engine calibration is not modified for different fuels. Oxygen content can however significantly reduce PM with limited effect on tailpipe CO 2 and a moderate increase of NO x and fuel consumption. The decrease of PM emission was followed by a decrease in the volume of accumulation mode particles, which would be consistent with a chemical suppression of soot formation by oxygen-fuel bonds. NO x emissions were found more sensitive to the chemical character rather than the physical properties of the fuel. Emission levels increased as the ratio of paraffins / naphthenes was also increased. Finally, the fuels studied seem to generally follow a PM NOx trade-off pattern which designates that concurrent fulfilment of more strict NO x and PM emission standards may not be possible with tuning of the fuel properties only. REFERENCES 1. ACEA: Monitoring of ACEA s commitment on CO 2 emission reductions from passenger cars, Final Report available at Brussels, Belgium (2003). 2. ACEA and EUROPIA: European programme on emissions, fuels and engine technologies. Final Report, Brussels, Belgium, p. 650 (1996). 3. ARTEMIS: Assessment and Reliability of Transport Emission Models and Inventory Systems, Internet reference at (2004). 4. Ntziachristos, L., Giechaskiel, B., Pistikopoulos, P., Samaras, Z., et al.: SAE World Congress, Detroit, USA, SAE Paper (2004). 5. Ntziachristos, L., Giechaskiel, B., Ristimäki, J., Keskinen, J.: J. Aerosol Sci., accepted 6. Kitamura, T., Ito, T., Senda, J., Fujimoto. H.: JSAE Review, 22: 139 (2001). 5

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