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2013-01-1678
Published 04/08/2013
Copyright © 2013 SAE International
doi:10.4271/2013-01-1678
saefuel.saejournals.org
ABSTRACT
The focus of the present study was to characterize the fuel reactivity of high octane number fuels (i.e., low fuel
reactivity), namely gasoline, ethanol, and methanol when mixed with cetane improvers under lean, premixed combustion
conditions. Two commercially available cetane improvers, 2-ethylhexyl nitrate and di-tert-butyl peroxide, were used in the
study. First, blends of the primary reference fuels iso-octane and n-heptane were port injected under fixed operating
conditions. The resulting combustion phasings were used to generate effective PRF number maps. Then, blends of the
aforementioned base fuels and cetane improvers were tested under the same lean premixed conditions as the PRF blends.
Based on the combustion phasing results of the base fuel and cetane improver mixture, the effective PRF number, or
octane number, could be determined. In all three base fuels it was found that 2-ethylhexyl nitrate is more effective at
increasing fuel reactivity compared to di-tert-butyl peroxide. However, 2-ethylhexyl nitrate has a potential disadvantage
due its nitrate group, which can manifest itself as NOx emissions. The relationship between the fuel-bound nitrate group
and the engine-out NOx emissions was extensively characterized in the present study. It was also observed that methanol's
response to cetane improvers was better than that of ethanol, in spite of the fact that they have similar octane numbers in
their neat form. Once the reactivity of the base fuels was characterized, two mixtures of methanol and cetane improvers
were selected and compared to diesel fuel as the high reactivity fuel (i.e., direct injected) for RCCI combustion.
CITATION: Dempsey, A., Walker, N. and Reitz, R., "Effect of Cetane Improvers on Gasoline, Ethanol, and Methanol
Reactivity and the Implications for RCCI Combustion," SAE Int. J. Fuels Lubr. 6(1):2013, doi:10.4271/2013-01-1678.
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Reactivity Controlled Compression Ignition (RCCI) is a volume 2-ethylhexyl nitrate (EHN) as the high reactivity fuel
dual fuel partially premixed combustion concept developed for RCCI combustion. They made comparisons to gasoline/
by Kokjohn et al. [4]. In this strategy, a low reactivity fuel, diesel RCCI and found that more E10+EHN was required
such as gasoline, is premixed via port fuel injection (PFI) and compared to diesel fuel to achieve similar combustion
a high reactivity fuel, such as diesel fuel, is direct injected phasing. This suggests that diesel fuel is more reactive than
(DI) during the compression stroke. This process of in- E10 mixed with 3% by volume EHN. Kaddatz et al. also
cylinder fuel blending develops fuel reactivity gradients in showed that for RCCI operation with gasoline/diesel, if the
the combustion chamber. The stratification of fuel reactivity direct injection timings were sufficiently advanced, start of
results in a broad combustion event and reduced pressure rise injection command of −36° ATDC and earlier, the NOx
rates compared to fully premixed HCCI combustion. Using a emissions went to essentially zero. However, as the direct
suite of optical diagnostics Kokjohn has gone on to injection timings were advanced using E10+EHN as the high
demonstrate that RCCI is a chemically controlled combustion reactivity fuel, the NOx emissions converged to one-third of
process, similar to HCCI [5]. The direct injection events are the fuel-bound NO from the EHN. This potential
sufficiently early during the compression stroke that the peak disadvantage of using EHN as a reactivity enhancer will be
equivalence ratio at the start of combustion remains very lean discussed in detail in the present study.
(i.e., equivalence ratio < 0.5). This results in sequential The impact of cetane improvers on fully premixed HCCI
autoignition events beginning at the regions of highest fuel combustion has previously been investigated as well. Mack et
reactivity and progressing down the reactivity gradient. In al. [9] demonstrated the effect of adding DTBP to blends of
addition, Kokjohn has shown that flame propagation plays an ethanol and diethyl ether during HCCI combustion. They
indistinguishable role during the combustion process due to found that the addition of DTBP did not elongate the heat
the very lean equivalence ratios [5]. release nor did it allow for stable retardation of the
The majority of RCCI combustion research conducted to combustion phasing. However, they found that the
date has used port injected gasoline and direct injected diesel combustion did advance by approximately 3° CA for 3%
fuel [6]. There are potential disadvantages of a combustion DTBP in ethanol. Eng et al. [10] studied the effect of adding
strategy that requires two different base fuels (e.g., two fuel DTBP to gasoline during HCCI operation with the goal of
tanks). However, considering that RCCI combustion only extending the low load limit. They found that from 0 to 2%
requires that a fuel reactivity gradient be present in the DTBP addition, the low load limit was reduced by 23%.
combustion chamber, it has been proposed to use port However, from 2% to 15% DTBP addition the low load limit
injected low reactivity fuel and direct inject the same low was only reduced by an additional 10%. This data suggests
reactivity fuel mixed with a small percentage of a cetane that DTBP added to gasoline exhibits a very non-linear
improver to serve as the high reactivity fuel. With this behavior in terms of increasing the gasoline's reactivity. In
approach, the vehicle would require a single fuel tank (i.e., both of the aforementioned studies on HCCI combustion with
the low reactivity fuel, such as gasoline) and an additive tank, cetane improvers (i.e., [9, 10]) it was discussed that the
which would need to be roughly the same size as a diesel effects of ignition promoters are currently not totally
exhaust fluid (DEF) tank, depending on the additive doping understood. There is some evidence that suggests the ignition
level [7]. Thus, the main goal of the present study was to promoting effect is due simply to a temperature increase,
characterize the potential of low reactivity fuels, namely stemming from low temperature heat release. However, other
gasoline, ethanol, methanol, and blends of the alcohols and researchers argue that the effect is chemical in nature and due
gasoline when mixed with cetane improvers to understand to the fact that chain propagating and chain branching
how they will perform as the high reactivity fuel during RCCI reactions are accelerated by the decomposition of the cetane
operation. improver. The present study supports the latter chemical
effect.
Previous Research with Cetane Improvers Of course, the effect of cetane improvers on diesel fuel
EHN & DTBP under mixing limited conditions (i.e., high equivalence ratios)
has been studied extensively. Schwab et al. [11] studied the
Splitter et al. [7] were among the first to investigate the
effect of EHN and DTBP on two different diesel fuels. Figure
aforementioned concept on a heavy duty diesel engine, in
which they port injected gasoline and direct injected gasoline 1 illustrates their findings, in which regardless of the cetane
mixed with small amounts of di-tert-butyl peroxide (DTBP). number of the base fuel, as the cetane improvers are added,
the cetane number increase (i.e., reactivity increase) is more
They found that RCCI combustion could be achieved by
rapid with EHN than with DTBP.
mixing as little as 2% by volume DTBP into the direct
injected gasoline. Kaddatz et al. [8] conducted similar
research on a light duty diesel engine. Considering that the
majority of pump gasoline in the United States today has
been blended with up to 10% ethanol by volume (i.e., E10),
Kaddatz et al. investigated using E10 mixed with 3% by
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Characterizing High Octane Number Fuels Figure 3. Predicted equivalence ratio distribution from
CFD simulations with 85% premixed gasoline and 15%
Mixed with Cetane Improvers direct injected diesel fuel.
As mentioned previously, the main goal of this work was
to characterize low reactivity fuels mixed with cetane
improvers to evaluate how well they will perform as the high Figure 2 also shows the resulting apparent heat release
reactivity fuel during RCCI operation. First, an experiment rate (AHRR) for this mid-load operating condition. Figure 3
representative of the thermodynamic conditions experienced shows the equivalence ratio distribution in the combustion
by the directed injected fuel during RCCI combustion needed chamber at −18° ATDC predicted by CFD simulations using
to be selected. Figure 2 shows a representative RCCI KIVA3V. As can be seen, the background equivalence ratio
operating condition in which 85% of the total fuel is from the premixed gasoline is 0.3. The direct injected diesel
premixed gasoline and the remaining 15% is direct injected fuel provides some equivalence ratio stratification, with a
diesel fuel. The diesel was injected using a double injection peak equivalence ratio in the chamber of 0.5. The majority of
strategy with the first injection at −61° ATDC and the second the direct injected fuel exists at an equivalence ratio between
at −41° ATDC. 0.32 and 0.34, which is nearly the background equivalence
ratio. Thus, a lean, premixed combustion experiment would
serve as a representative operating condition for the high
reactivity fuel during RCCI operation.
Objectives
The main focus of the current study was to investigate
RCCI combustion in a light duty engine using a single low
reactivity fuel, mainly alcohols, and the low reactivity fuel
mixed with cetane improvers to serve as the high reactivity
fuel. This concept has been demonstrated previously by
Splitter et al. [7] and Kaddatz et al. [8], but the amount of
cetane improver used was arbitrarily chosen. In this study, the
reactivity of the base fuels (i.e., gasoline, ethanol, methanol,
and alcohol/gasoline blends) was characterized when mixed
with cetane improvers EHN and DTBP. The goal was to
understand how the base fuel's reactivity changes and if these
low reactivity fuels could be utilized as high reactivity fuels
Figure 2. Typical RCCI injection strategy and for RCCI combustion when mixed with cetane improvers.
subsequent AHRR operating with gasoline & diesel fuel.
SINGLE CYLINDER LIGHT DUTY
DIESEL ENGINE LABORATORY
The experiments were carried out on a light duty, four-
stroke diesel engine based on the General Motors 1.9L
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platform. Table 1 shows the engine and fuel injector Multiple combustion strategies were investigated in this
specifications and Figure 4 provides a schematic of the single study, namely HCCI and RCCI. HCCI operation was
cylinder engine laboratory. With a bore of 82.0 mm and achieved with two port fuel injectors mounted in the intake
stroke of 90.4 mm this engine is representative of a light duty runner. The point of fuel injection is approximately 30 cm
automotive diesel engine with four valves per cylinder driven upstream of the intake valves. For RCCI operation, the low
by dual overhead cams. A stock four-cylinder head is reactivity fuel was delivered through the same port fuel
installed atop a single cylinder block with only the valves for injectors and the high reactivity fuel was delivered with a
cylinder #2 activated by the cams. centrally mounted common rail injector.
Engine controls and data acquisition were handled
Table 1. GM 1.9L Single Cylinder Engine Specifications through National Instruments LabView software. A Kistler
6125A pressure transducer in series with a Kistler 4010
charge amplifier was used to measure the in-cylinder
pressure. A shaft encoder with 1440 pulses per revolution
was used, which supplies a resolution of 0.25 crank angle
degrees. For each operating point 300 consecutive cycles of
cylinder pressure data were acquired. Each individual cycle's
pressure data was smoothed using a Fourier series low-pass
filter with a Gaussian roll-off function having a transmission
of 100% from 0 to 1600 Hz and dropping to 1% at 6720 Hz.
Once filtered, the collected cycles were ensemble averaged to
yield a representative cylinder pressure trace, which was used
to calculate the apparent heat release rate (AHRR) and, in
turn, determine combustion phasing. The AHRR is
essentially the chemical heat release rate minus the heat loss
rate to the combustion chamber walls and is given by
(1)
From the AHRR, the accumulated heat release can be
determined. The combustion phasing was calculated to be the
crank angle at which the accumulated heat release had
reached 50% of its maximum, denoted as CA50.
CHARACTERIZATION OF HIGH
OCTANE NUMBER FUELS MIXED
WITH CETANE IMPROVERS
Engine Operating Conditions & Reference
Combustion Phasing Maps
As mentioned previously, the RCCI direct injection
strategy creates equivalence ratio and octane number
stratification in the combustion chamber. In Figure 3 it was
shown that the equivalence ratio distribution just prior to
ignition remains lean (equivalence ratios < 0.5). Therefore,
lean fully premixed HCCI combustion was chosen as the
strategy to study the impact of cetane improvers on high
octane number fuels. The engine operating conditions that
were used to create the reference maps is shown in Table 2.
Figure 4. GM 1.9L Single Cylinder Engine Laboratory These engine operating parameters were fixed throughout the
study regardless of the base fuel, and two different
equivalence ratios were investigated: 0.26 and 0.3.
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(2)
Limits were set on the peak pressure rise rate and the
coefficient of variation (COV) of engine load (i.e., indicated
mean effective pressure, IMEP), at 10 bar/deg. and 10%,
respectively. Thus, at a given intake temperature, the most
advanced combustion phasing produced a peak pressure rise
rate of 10 bar/deg. and the most retarded phasing had a COV
of IMEP approaching 10%. These combustion phasing results
with primary reference fuels will serve as references to
Figure 7. Indicated specfic NOx emissions as a function
determine the effective PRF # of the base fuels mixed with
of the PRF # at an equivalence ratio of 0.3
cetane improvers.
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Table 3. Physical and chemical properties of the liquid fuels tested using HCCI combustion
intake temperatures used for the reference fuels and gasoline. instantaneously, allowing the data to be collected in a timely
At the far right (i.e., 100% alcohol-in-gasoline) are the intake manner.
temperatures used for neat ethanol and neat methanol. The
data points in between show the various gasoline/alcohol Gasoline/EHN Mixtures
blends investigated in this study, all with a unique intake Figure 11 shows the combustion phasing results for
temperature requirements. The intake temperatures outlined gasoline/EHN mixtures at an equivalence ratio of 0.26. It can
in Figure 10 where used for both equivalence ratios be seen that as the percentage of EHN in gasoline is
investigated here. These two intake conditions will be increased, the combustion phasing advances considerably.
referred to throughout the study as ∼60°C and ∼90°C. Also, as expected, as the intake temperature is increased the
The base fuels under investigation were tested in the same combustion phasing advances as well. Figure 11 is shown as
manner as the primary reference fuels. The engine operating an example, but regardless of the base fuel or cetane
conditions were shown in Table 2 and the intake temperatures improver the trends remain the same. Therefore, for the sake
are shown in Figure 10. Again, dual fuel HCCI combustion of brevity plots of the combustion phasing for every base fuel
was achieved via the use of two port fuel injectors. However, will not be shown.
instead of fueling with the primary reference fuels, one port The combustion phasing results can be used to derive an
injector was supplied with the neat base fuel and the other effective PRF # by referring back to the primary reference
with the base fuel aggressively mixed with a cetane improver fuel maps shown in Figure 5 and Figure 6. The resulting
(i.e., 10 to 15% cetane improver depending on the base fuel). effective PRF # for the gasoline/EHN mixtures is shown in
Using this approach, the global in-cylinder mixture of base Figure 12, where the results for both equivalence ratios and
fuel and cetane improver could be varied nearly two intake temperatures are plotted. As can be seen, the
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effective PRF # displays no observable dependence on the temperatures investigated. The standard RON and MON tests
equivalence ratio. are conducted at intake temperatures of 52°C and 149°C,
respectively [13]. The results shown in Figure 12 utilized
intake temperatures between those used in RON and MON
testing. As expected, the trend line shown in Figure 12
intersects the vertical axis (i.e., neat gasoline) at an effective
PRF # between the RON and MON of the gasoline, at
approximately PRF 92. This observation is important because
it provides confidence for the current experimental
investigation. From this point onward, whenever the
gasoline/EHN data is presented, it will be a combination of
the data from both intake temperatures.
Figure 13 shows the NOx emissions results for the data
points in Figure 12. For reference, the fuel-bound NO2 and
one-third of the fuel-bound NO2 are also shown on the plot.
The fuel-bound NO2 was calculated assuming that one NO2
Figure 11. Combustion phasing (CA50) results for molecule is removed from each EHN molecule in the fuel
gasoline/EHN mixtures at an equivalence ratio of 0.26 mixture. As can be seen in the Figure, the engine-out NOx
emissions track fairly well with one-third of the total fuel-
bound NO2. This is consistent with the findings of Ickes et al.
[15] under diesel low temperature combustion operation with
diesel fuel/EHN mixtures.
Dec et al. [14] pointed out that gasoline autoignition Figure 13. Indicated specific NOx emissions as a
chemistry is not sensitive to the equivalence ratio at low function of the EHN percentage in gasoline during lean
intake pressure conditions (i.e., less than ∼2.0 bar intake HCCI combustion.
pressure). Thus, considering the intake pressure used in the
current study was sufficiently low at 1.1 bar, it is expected
that the ignition timing of the gasoline would be relatively Ethanol/EHN Mixtures
independent of equivalence ratio. Additionally, the effective Figure 14 shows the effective PRF # for ethanol/EHN
PRF # of the gasoline/EHN mixtures is not sensitive to the mixtures under lean, HCCI combustion operating conditions.
intake temperature. This is expected because the gasoline Just as with gasoline, the effective PRF # is not sensitive
used in this study has a relatively low fuel sensitivity (i.e., to the mixture equivalence ratio. However, contrary to
RON minus MON), as can be seen in Table 3. The reason gasoline, the effective PRF # is very sensitive to the intake
conventional gasoline displays relatively low fuel sensitivity temperature. This is consistent with the fuel sensitivity (i.e.,
is because gasoline is mainly composed of paraffin RON minus MON) of ethanol as shown in the fuel property
compounds, which is the same class of hydrocarbon as the table, Table 3. As mentioned previously, it is expected that
primary reference fuels. Thus, they display similar chemical the alcohol fuels would have higher fuel sensitivity than
behavior. However, the small amount of fuel sensitivity that gasoline because they are a different class of hydrocarbon
the tested gasoline does have is not captured in the current compared to the reference fuels and gasoline.
study because of the relatively small range of intake
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Methanol/EHN Mixtures
Figure 16 shows the effective PRF # for methanol/EHN
blends. Trend wise, the results are very consistent with those
observed with ethanol/EHN mixtures. Again, a polynomial fit
was created for the data collected at the ∼90°C (i.e.,
Tin=113°C) intake condition and then applied to ∼60°C (i.e.,
Tin=82°C) data because data at low EHN percentages was
unattainable at the colder intake temperature. The sensitivity
of the effective PRF # to intake temperature is significant,
just as it was with ethanol.
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response curves for EHN and DTBP have vastly different enhanced at a faster rate compared to ethanol. Previous
slopes, and therefore are converging very rapidly. research has demonstrated that both ethanol and methanol act
as inhibitors of low temperature combustion chemistry [17,
18]. The results shown in Figure 21 and Figure 26 suggest
that ethanol is a stronger inhibitor, resulting in less reactivity
enhancement from the cetane improvers studied here. The
chemical reasons for this are not understood and currently
under investigation using detailed chemical kinetics
modeling.
Figure 25. Effective PRF # of methanol blended with Figure 27. Indicated specific NOx emissions as a
EHN and DTBP during HCCI combustion function of the DTBP percentage in all three base fuels
during lean HCCI combustion
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Alcohol/Gasoline Blends Mixed with not allow for less cetane improver to be used to achieve a
given reactivity level.
Cetane Improvers
IMPLICATIONS OF ALCOHOLS
MIXED WITH CETANE IMPROVERS
FOR RCCI COMBUSTION
A main goal of the present study was to characterize the
potential of low reactivity fuels to serve as high reactivity
fuels for RCCI combustion when mixed with cetane
improvers. The characterization presented above suggests
that:
Figure 28. Effective PRF# for gasoline/ethanol blends 2. However, methanol's response to the cetane improvers
mixed with EHN at an intake temperature of ∼90°C. is much more rapid than ethanol's, thus requiring less additive
to achieve a given reactivity level.
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Figure 37. AHRR results over a sweep of the ratio of Figure 38. Engine-out NOx emissions as a function of
high to low reactivity fuel using neat methanol and the port fueling percentage for three different high
methanol mixed with 12% DTBP reactivity fuel compositions
The lack of combustion phasing control is also thought to Table 4. Engine performance and emissions results for
be a consequence of the large amount of charge cooling that the different high reactivity fuel compositions
is expected with direct injected methanol. Essentially,
wherever the high reactivity methanol/cetane improver
mixture targets in the combustion chamber will be cooled
significantly, counteracting the increase in reactivity from the
EHN and DTBP. Thus, the net effect is nearly no change in
the combustion phasing as the global amount of cetane
improver is increased or decreased.
Figure 38 shows the engine-out NOx emissions as a
function of the port fueling percentage for the different high
reactivity fuel compositions. When diesel fuel is used as the
high reactivity fuel, the NOx emissions are low if more than
∼92% of the total fuel is port injected neat methanol. As was
the case with the direct injection timing sweep, the NOx
emissions when operating with methanol/DTBP are very low
regardless of the port fueling percentage. When
methanol/EHN was used as the high reactivity fuel, the NOx
emissions were again higher. However, as concluded The major issue with the methanol/cetane improver
previously, if 0.3 mg or less of EHN were injected per cycle, mixtures remains, which is the inability to control the
the NOx emissions stemming from the fuel-bound nitrate combustion phasing to a large extent. This disadvantage is
group remain below 0.3 g/kW-hr. summarized in Figure 39. The error bars shown in the figure
Table 4 shows the engine performance and emissions are calculated from the standard deviation of the CA50 at
results for select cases which utilized the three different high each operating point over a 300 cycles. As can be seen, the
reactivity fuel compositions studied here. As can be seen methanol/cetane improver mixtures are unable to vary
from the table, the methanol/cetane improver mixtures combustion phasing despite large changes in the port fueling
performed just as well as diesel fuel. However, the peak percentage. However, when diesel fuel is utilized as the high
pressure rise rates produced by the methanol/cetane improver reactivity fuel, a large amount of combustion phasing control
mixtures were higher, suggesting that the in-cylinder is experienced.
gradients in fuel reactivity are not as large as those produced
when diesel fuel is used.
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ACKNOWLEDGMENTS
The authors gratefully acknowledge the support of this
work by the United States Department of Energy (DOE) and
the Princeton Combustion Energy Frontier Research Center
(CEFRC). Additionally, the authors would like to thank the
United Wisconsin Grain Producers, LLC for donating the
ethanol fuel used in this study.
DEFINITIONS/ABBREVIATIONS
Φ - Equivalence Ratio
AHRR - Apparent Heat Release Rate
ATDC - After Top Dead Center
CA - Crank Angle
CA50 - Crank Angle of 50% Fuel Burned
CFD - Computational Fluid Dynamics
COV - Coefficient of Variation
DEF - Diesel Exhaust Fluid
DI - Direct Injection
DTBP - Di-Tert Butyl Peroxide
E10 - 90% Gasoline/10% Ethanol by Volume
E50 - 50% Gasoline/50% Ethanol by Volume
E85 - 15% Gasoline/85% Ethanol by Volume
EHN - 2-EthylHexyl Nitrate
HCCI - Homogeneous Charge Compression Ignition
IMEP - Indicated Mean Effective Pressure
IVC - Intake Valve Closure
M50 - 50% Gasoline/50% Methanol by Volume
MON - Motored Octane Number
NO - Nitrogen Oxide
NO2 - Nitrogen Dioxide
NOx - Nitric Oxide Emissions
PFI - Port Fuel Injection