1219

Proceedings of the Combustion Institute, Volume 28, 2000/pp. 12191225

INJECTION OF A H
2
O
2
/WATER SOLUTION INTO THE COMBUSTION
CHAMBER OF A DIRECT INJECTION DIESEL ENGINE AND ITS
EFFECT ON SOOT REMOVAL
BERTHOLD FRANZ and PAUL ROTH
Institut fu r Verbrennung und Gasdynamik
Gerhard-Mercator-Universita t Duisburg
47048 Duisburg, Germany
Hydrogen peroxide (H
2
O
2
) dissolved in water was injected into the combustion chamber of a direct
injection (DI) diesel engine at different crank angles. Its effect on the general combustion characteristics
was followed by crank angle (CA) resolved pressure and OHradiation measurements inside thecombustion
chamber. The inuence on soot mass in the exhaust gas ow was measured by the Bosch Smoke Number,
which is the standard measurement technique in internal combustion engine research. Additionally, the
concentrations of unburned hydrocarbons (HC) and nitric oxides (NO
x
) were recorded by a gas analyzer.
For both, the spray of H
2
O
2
/water and pure water, a clear decrease in soot emission was observed for
early injection at crank angles 40 CA 10 before top dead center (BTDC), which is associated
with an increase in the exhaust gas HC concentration. For these conditions, the soot removal is mainly an
effect of compressed air cooling, which increases the induction time of the diesel spray, thus resulting in
a shift toward more premixed combustion. At injection crank angles CA 10, the water and the H
2
O
2
/
water sprays show an opposite behavior with respect to the exhaust gas soot. The in-cylinder measurements
clearly show an increase of OH radiation during cycles with H
2
O
2
/water injection compared to the standard
engine conditions. The H
2
O
2
decomposition product OH inuences the chemistry of the in-cylinder soot
oxidation, which results in a decrease of the soot mass in the engine exhaust gas ow. Concentrations of
HC and NO
x
are not signicantly affected. The addition of pure water causes an increase in the exhaust
gas soot for spray injection crank angles CA 10.
Introduction
With increasing common interest in air pollution
and its effects on the environment and public health,
vehicle emissions are being subjected to increasingly
stringent exhaust gas regulations. With the introduc-
tion of a three-way catalytic converter, the emissions
from gasoline-fueled engines have been reduced sig-
nicantly. For diesel engines, a general strategy of
lowering soot and NO
x
emission is more complicated
and still in discussion. This is due to the interrelation
between the heterogeneous mixture formation and
self-ignition of the diesel combustion process. On
the one hand, long ignition delay times lead to a
more premixed combustion with low soot emission,
due to lean combustion. On the other hand, this pro-
cess amplies NO
x
formation because of increasing
combustion temperature. This sootNO
x
trade-off is
one of the major problems in diesel combustion de-
velopment.
One possibility to lower soot and NO
x
emission is
the addition of water during diesel combustion.
Since water/fuel emulsions have a lower cetane
number in comparison to conventional diesel fuel,
the ignition delay increases, resulting in lower soot
emission. The fuel-added water reduces the com-
bustion temperature and leads to a lower NO
x
for-
mation rate. A negative effect is the increase in the
emission of unburned hydrocarbons (HC), which is
strongly related to a longer ignition delay time and
an increased inuence of quenching effects [1,2]. A
very effective method of lowering NO
x
emission is
known as stratied waterfuel injection. Again, the
used water decreases local temperature peaks. De-
pending on the waterfuel stratication, a signicant
reduction of NO
x
emission is possible without any
effect on soot or HC [3,4]. The potential of this
method for reduction of soot and NO
x
is limited.
Independent from the method of the water addition,
the main effects are an increase in the ignition delay
time and a decrease in the mean combustion tem-
perature.
It is known that most of the soot formed during
diesel engine combustion is also oxidized inside the
diesel combustion chamber [5]. This process is
strongly related to the presence of OH radicals,
which concentrations drop signicantly at crank an-
gles (CA) exceeding 40 CA after top dead center
(ATDC) [6,7]. A further soot oxidation seems pos-
sible if OH radicals are present during later parts of
diesel combustion. Roth et al. [8] have shown that
1220 COMBUSTION IN ENGINES
Fig. 1. Experimental setup: DI diesel engine equipped with an additional spray system for water or H
2
O
2
/water
injection.
lter-collected soot particles can very effectively be
burned if an H
2
O
2
/water solution is sprayed from
time to time into the exhaust gas ow of a diesel
engine. Born and Peters [9] have described experi-
ments where an H
2
O
2
/water solution is sprayed into
the combustion chamber of a diesel engine, resulting
in a signicant reduction of soot emission. Beside
the effect of lower soot emission, it would be of in-
terest to get more information about the effect of
water-dissolved H
2
O
2
on typical diesel combustion
parameters. The present paper is therefore focused
on soot removal as well as on the parameters of ig-
nition delay time, additional OH radical appearance,
and HC and NO
x
concentration. The question to be
answered is whether the observed drop in soot emis-
sion is primarily an effect of water addition or caused
by H
2
O
2
and/or its decomposition products. Exhaust
gas compounds such as soot, NO
x
, HC, and CO
2
are
routinely monitored during the present engine ex-
periments.
Experimental
A schematic view of the experimental setup is pre-
sented in Fig. 1. The engine is an air-cooled, single
cylinder, four stroke, direct injection (DI) diesel en-
gine with a maximum power output of 4.5 kW at
3000 rpm. The engine has a displacement of 380 cc
and a compression ratio of 1:18. It is operated
with conventional diesel fuel at 2000 rpm and full
load in all experiments. The crankshaft is connected
to an electronically controlled dynamometer.
The H
2
O
2
/water solution is injected by a second
injection system into the engine combustion cham-
ber. It is designed like a common-rail systeminorder
to optimize the accuracy of the injection timing. The
injector is placed beneath the diesel injector at the
edge of the piston bowl. The hydrogen peroxide so-
lution is stored in a tank pressurized by nitrogen be-
ing directly connected to the injector. During all ex-
periments, the injection pressure was set to 300 bar,
and 35% H
2
O
2
(of total mass) dissolved in water was
used. Except for the injector, which is made of car-
bon steel, the whole H
2
O
2
/water system was made
of stainless steel in order to minimize decomposition
of H
2
O
2
due to catalytic surface reaction. For the
same reason, the inner part of the injector is also
especially prepared with a coating. A programmable
Tektronix pulse generator with amplier was used to
operate the solenoid valve of the common-rail injec-
tor. To enable pre-top dead center (TDC) injection
of the H
2
O
2
solution, a trigger signal was set to 90
CA before top dead center (BTDC). The timing of
the H
2
O
2
/water injection system could be set with
an accuracy of 0.5 CA.
In order to perform time-resolved measurements
of combustion pressure and OH radiation, sensors
for TDC and CA were used, directly connected to
the crankshaft of the engine. The time resolution of
H
2
O
2
/WATER INJECTION INTO DIESEL COMBUSTION 1221
Fig. 2. Measured exhaust gas soot mass, HC, and NO
x
relative to reference engine conditions for water and
H
2
O
2
/water injection at different crank angles.
the CA sensor was 0.5 CA. The combustion pres-
sure was monitored by a water-cooled Kistler 6001
pressure transducer. The signals of the TDC sensor,
the CA sensor, and the pressure transducer were re-
corded by a Yokogawa digital oscilloscope. Since the
pressure records of DI diesel engines often have os-
cillations at maximum pressure, and during the rst
phase of expansion, a statistical procedure described
by Harndorf [10] was used to remove the oscillations
in a physically reasonable manner.
The optical setup for measuring OHradiationcon-
sists of four main parts: a window-like sapphire ber,
a one-in-two optical ber, two optical interference
lters, and two photomultipliers (PM). The sapphire
ber of 425 lm in diameter was cleaved into the
cylinder head above the center of the piston bowl.
The tip of the ber window protruded into the com-
bustion chamber to avoid soot deposition due to
thermophoresis. A specially designed one-in-two op-
tical ber was used to split the emission signal into
two equal parts. One PM was equipped with a nar-
row band interference lter of k 308 nm (5
nm), which corresponds to the optical A
2
R X
2
P
transition of OH. The second PMwas equippedwith
a narrow band interference lter of k 340 nm
(4.1 nm) to detect the thermal radiation of the
soot particles. The lters in the optical setup were
replaced by k 488 nm and k 633 nm narrow
band interference lters to allow two-color tempera-
ture measurements of the soot particles. The emis-
sion signals were again recorded as a function of the
CA and stored in a Yokogawa oscilloscope. Addition-
ally, a set of thermocouples was used to measure
intake and exhaust gas temperature of the engine.
The soot amount in the exhaust gas was measured
by a conventional AVL smoke meter. Its analog out-
put was connected to a PC equipped with an analog/
digital interface. Exhaust gas concentrations of HC,
NO
x
, and CO
2
were detected by a Pierburg ame
ionization detector (FID), an Eco-Physics chemo-
luminescence NO
x
meter, and a Pierburg infrared
CO
2
meter, respectively.
Results
In a rst series of experiments, the inuence of
H
2
O
2
/water solution injected at different crank an-
gles on soot mass, HC, and NO
x
concentration was
studied. The amount of the H
2
O
2
solution was al-
ways 40% of the fuel volume. In all cases, the diesel
fuel was injected at CA 10. To separate the
expected H
2
O
2
effect from that of water, experi-
ments were also conducted with pure water injec-
tion. The results of these experiments are shown in
Fig. 2. In all three graphs, the measured soot mass,
HC, and NO
x
concentration relative to the condi-
tions without any additional injection (reference
condition) are shown as a function of the injection
time scaled in degrees of CA relative to TDC. Num-
bers greater than 1 indicate an increase of the re-
spective property; numbers lower than 1 stand for a
reduction in soot mass, HC, or NO
x
. The statistical
scatter of the experimental data is illustrated by error
bars. Pure water injection is indicated by squares;
H
2
O
2
/water injection is indicated by circles. It is
very clear at rst view that the results obtained are
very sensitive to the injection crank angle. The upper
diagram in Fig. 2 illustrates that an injection of water
at CA 40 reduces the soot mass by about 20%,
whereas H
2
O
2
/water injection causes a decrease of
only about 3%. If the injection is set to CA 20,
the difference between water and H
2
O
2
/water in-
jection disappears. For injection very close to the
diesel injection at CA 10 and for TDC, the
soot mass exceeds the value obtained at the refer-
ence condition. This trend proceeds for pure water
addition with decreasing tendency for increasing in-
jection crank angle. To the contrary, the injection of
H
2
O
2
/water solution at CA 5 causes again a
decrease in the soot emission of the engine, which
is optimal at CA 10. For very late injection,
CA 40, no signicant change in soot mass
could be observed, independent in whether water or
H
2
O
2
/water was injected.
The results of additional spray injection on the HC
and NO
x
concentration in the diesel exhaust gas are
1222 COMBUSTION IN ENGINES
Fig. 3. In-cylinder crank-angle-resolved pressure mea-
surements for water and H
2
O
2
/water spray injection at CA
40 and CA 30.
Fig. 4. In-cylinder crank-angle-resolved pressure mea-
surements for water and H
2
O
2
/water spray injection at CA
20 and CA 10.
shown in the middle and lower part of Fig. 2. At
injection CA 0, the HC concentration increases
signicantly and the NO
x
concentration is lowered.
These effects are stronger for pure water spray than
for H
2
O
2
/water solutions. For injection CA 0, the
effects disappear, and the measured exhaust gas con-
centrations are very similar to those obtained with-
out any spray addition.
In a further series of experiments, the pressure in
the combustion chamber of the diesel engine was
measured as a function of the crank angle for spray
injection conditions previously described. Since
combustion differs from cycle to cycle, a number of
100 cycles was always recorded for each injection
time and statistically evaluated. Stronger effects on
the measured pressure records from the spray injec-
tion time were only obtained for injection at CA0.
Figs. 3 and 4 show typical measured pressure pro-
les as a function of the crank angle for the reference
conditions without any additional spray (solid lines)
and for spray injection at CA 40 and CA
30 (Fig. 3) and CA 20 and CA 10
(Fig. 4), both for pure water addition (dasheddot-
ted lines) and H
2
O
2
/water addition (dashed lines).
In the crank angle range of interest (CA 10 to
CA 25), the measured pressure varies between
40 and 70 bar. It is clear from Fig. 3 that water in-
jection, and to a minor extent H
2
O
2
/water injection,
shifts the pressure increase to later crank angles, re-
sulting in an increase of the ignition delay time by
about 2 CA. This effect seems to vanish for later
injection times (Fig. 4). The maximum shift in the
ignition delay time in the case of H
2
O
2
/water injec-
tion is about 1 CA. For crank angles CA 0, no
systematic difference between standard engine
operation and additional spray injection was ob-
served. The largest difference in maximum combus-
tion pressure is less than 2 bar.
Besides the pressure measurement inside the die-
sel engine combustion chamber, OH emission was
recorded as a function of the crank angle. The aim
was to demonstrate whether the H
2
O
2
decomposi-
tion product OHleads to an additional light emission
signal. While the pressure is nearly homogeneously
distributed inside the combustion chamber, the light
emission in general and also the OH emission at a
certain wavelength are locally distributedproperties,
which are known to be affected by many optical and
thermochemical quantities. The optical window and
the ber optic are designed and positioned such that
radiation is collected from the center of the piston
bowl with an opening angle of 12 (see Fig. 1). There
is agreement in the combustion engine community
that the value of such emission measurements lies
more in the crank angle behavior than in the abso-
lute height. The crank angle resolved radiation mea-
sured at k 308 nm in the wavelength range of Dk
5 nm is a mixture of spectral OH radiation and
H
2
O
2
/WATER INJECTION INTO DIESEL COMBUSTION 1223
Fig. 5. In-cylinder crank angle resolved OH emission
for various conditions without and with spray addition.
Fig. 6. In-cylinder temperature measurements at differ-
ent crank angles.
quasi continuum radiation, mainly from the parti-
cles. The OH radiation curves shown in Fig. 5 for a
crank angle range of CA 3 to CA 30
were obtained from the total radiation at 308 nm,
from which the thermal radiation of the particles
measured beside the OH band was subtracted. Like
the in-cylinder pressure measurements, each curve
in Fig. 5 was obtained by signal averaging of 100
cycles and normalization to a maximum value of 1.
The curve with closed circles indicates the results
for standard engine operation conditions. At about
1 CA, radiation is detectable, reaching a maxi-
mum value at CA 10. If pure water is injected
at CA 20, both the rst radiation and the max-
imum radiation is shifted by 0.5 CA compared to
the previous case. The OH radiation curve obtained
with H
2
O
2
/water injection at CA 20 does not
differ from the one at standard engine conditions,
which is not plotted in this gure. For water injec-
tion at CA 10, the rst appearance and the
maximum radiation are not different from the radi-
ation at standard engine operation conditions. The
most obvious trend can be seen for H
2
O
2
/water in-
jection at CA 10, where the OH radiation
curve is shifted by DCA 1.5 CA compared to the
standard engine operation condition. This remark-
able effect coincides with the observed maximum
soot mass reduction in Fig. 2 for those conditions.
Measurements of the crank-angle-dependent
temperature prole during standard engine opera-
tion were performed by applying the two-color par-
ticle radiation spectroscopy. Regarding the spacial
resolution of such measurements, the same restric-
tions apply as in the case of OH emission measure-
ments. In Fig. 6, the mean particle surface tem-
perature, obtained from 100 individual combustion
cycles, which is assumed to be equal to the mean gas
temperature, is shown with high crank angle reso-
lution. Under the present conditions, the maximum
temperature is T 1950 K at CA 7, decreas-
ing to about T 1650 K at CA 34. Very simi-
lar mean temperature proles were obtained in the
case of H
2
O
2
/water injection. The almost unchanged
temperature prole in the case of H
2
O
2
/water in-
jection can be caused by two combined effects: the
energy being required for spray evaporation is com-
pensated by the exothermicity of the gas phase H
2
O
2
decomposition and/or by the heat release of the het-
erogeneous reaction of soot and OH.
In a last series of experiments, the compression
ratio of the diesel engine was changed from 1:18
toward 1:19.5. The reason for this modication was
to increase the mean, crank-angle-dependent tem-
perature of Fig. 6 to higher values. The volume ow
of the diesel fuel used was slightly adjusted such that
the soot mass emission was the same as compared
to the standard engine conditions. The increase in
the compression ratio causes an increase in the max-
imum combustion pressure from 68 to 75 bar and
increases in the exhaust temperature by 60 K. The
effect of the crank angle injection timing of the
H
2
O
2
/water spray on the measured soot mass in the
exhaust gas ow is shown in Fig. 7 in the same co-
ordinates as used in Fig. 2. The curve with circles
indicates the results which have already been de-
scribed in Fig. 2; the curve with squares shows the
inuence of the increased compression ratio. The
general structure of both curves is similar, but the
soot removal effect is higher for the increased com-
pression ratio, that is, higher mean temperature and
pressure. Furthermore, the crank angle interval, in
which H
2
O
2
/water injection has a lowering effect on
soot mass emission, is increased from 40 CA up
to 60 CA.
1224 COMBUSTION IN ENGINES
Fig. 7. Comparison of measured exhaust gas soot mass
as a function of the crank angle injection of H
2
O
2
/water
for two engine compression ratios.
Discussion
The injection of pure water and H
2
O
2
/water so-
lution into the combustion chamber of a diesel en-
gine at different times clearly shows signicant ef-
fects on soot formation/removal and on HC and
NO
x
. The different experimental information ob-
tained from in-cylinder and exhaust gas measure-
ments is discussed according to the spray injection
crank angle.
Injection Crank Angle 40 CA to 20 CA
Under these conditions, the spray enters the com-
bustion chamber before the fuel is injected at CA
10. The temperature inside the combustion
chamber is below 1000 K, that is, the spray evapo-
rates but the thermal decomposition of H
2
O
2
is very
slow. As a consequence of the spray evaporation, the
temperature slightly decreases, resulting in an in-
crease in the ignition delay time (see Fig. 3) and thus
in intensied premixed combustion. This nally
leads to the observed decrease in the soot emission
of the engine. This effect is more clear in the case
of pure water injection, because H
2
O
2
under these
conditions is expected to slightly contribute to the
early soot formation compared to the case of pure
water. The observed increase in the HC concentra-
tion is in agreement with the results of Velji et al.
[11].
Injection Crank Angle 10 CA to 5 CA
In this crank angle range, the soot emission of the
engine is above that of the reference condition. The
effect is more clear for water injection than for
H
2
O
2
/water injection. The in-cylinder pressure
measurements reveal that the water spray does not
signicantly inuence the ignition delay time. The
measured OH radiation also shows no difference
compared to engine reference operation conditions.
It is most likely that the additionally injected spray
interferes with the diesel fuel spray (CA 10).
The observed slight difference in water or H
2
O
2
/
water sprays might be a result of differences in spray
penetration and characteristics caused by differ-
ences in density, viscosity, and surface tension. Born
and Peters [9] report a reduction in soot emission
for this spray timing range. This indicates that syn-
chronous injection of diesel fuel and water spray may
cause both an increase and a decrease in soot emis-
sion depending on the particular injection condi-
tions.
Injection Crank Angle 10 CA to 40 CA
For this CA range, spray injection causes different
effects on soot emission, depending on whether wa-
ter or an H
2
O
2
/water solution is used. The soot
emission of the engine is clearly reduced by H
2
O
2
/
water injection, with the highest efciency at CA
10. Under these conditions, the mean gas tem-
perature is about 1950 K, which leads to a very fast
thermal decomposition of H
2
O
2
[12] and in turn to
the observed increase in OH radiation (see Fig. 5).
It is therefore very clear that the water-dissolved
H
2
O
2
and not the water itself is responsible for this
soot reduction effect. As described by v. Gersumand
Roth [13] in their shock tube experiments, the re-
action probability for surface oxidation of soot by
OH is very high. The simultaneously observed re-
duction in soot and increase in OH radiation indi-
cates that this is also a signicant process in the pres-
ent oxidation of soot during diesel combustion,
which is also reported by Cavaliere et al. [14]. For
injection crank angles up to CA 40, a reduc-
tion of the soot mass in the diesel exhaust gas with
decreasing tendency was observed. This trend can
be explained by the decrease in the in-cylinder mean
gas temperature (see Fig. 6) toward 1600 K, which
results in a less effective thermal decomposition of
H
2
O
2
into OH radicals. This interpretation is further
conrmed by the soot mass results obtained from
the engine with higher compression ratio (see Fig.
7). Although the higher pressure is known to inhibit
H
2
O
2
decomposition, the higher temperature will
support thermal decomposition. Overall, the in-
creased in-cylinder temperature supports the ther-
mal decomposition of H
2
O
2
and increases the pool
of OH radicals available for soot surface oxidation.
On the other hand, the injection of pure water re-
duces, according to Fig. 5, the observed OH emis-
sion and increases consequently the soot mass in the
exhaust gas. Water injection at later crank angles is
more and more unimportant for the in-cylinder
chemistry of soot removal or formation.
H
2
O
2
/WATER INJECTION INTO DIESEL COMBUSTION 1225
Conclusions
Pure water and water-dissolvedhydrogenperoxide
were injected at different crank angles into the com-
bustion chamber of a DI diesel engine, which was
always operated at the same conditions of 4.5 kW
and 2000 rpm. Two main effects were observed:
1. At early injection crank angles of 40 CA
20, a reduction in the exhaust gas soot mass was
found for both sprays. This is mainly a cooling
effect during the engine compression phase by
water, which increases the ignition delay time of
the diesel combustion and intensies premixed
combustion.
2. At injection crank angles of 10 CA
40, water and H
2
O
2
/water sprays show opposite
effects. On the one hand, the experiments clearly
show that the water-dissolved H
2
O
2
thermally de-
composes under these conditions, increasing the
OH radical pool in the combustion chamber. As
a consequence, soot particles are more effectively
oxidized, resulting in a reduction of the soot mass
in the exhaust gas. On the other hand, the injec-
tion of pure water under these conditions has no
reduction effect.
Acknowledgments
The work was supported by the German Science Foun-
dation. The authors would like to thank the Motorenfabrik
Hatz for donating the diesel engine and for extensive tech-
nical support. Special thanks to Mr. Ellwanger from the
DaimlerChrysler Corporation for placing different types
of common rail injectors at our disposal.
REFERENCES
1. Binder, K., Mineralo ltechnik, Vol. 12, Beratungsge-
sellschaft fu r Mineralo l-Anwendungstechnik mbH,
Hamburg, 1992, pp. 419.
2. Ladommatos, N., Parsi, M., and Knowles, A., Fuel
75(1):814 (1996).
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Y., and Nagae, Y., in Twentieth International Congress
on Combustion Engines, CIMAC, London, 1993, pp.
120.
4. Kohketsu, S., Mori, K., Sakei, K., Nagawa, H., and
Oda, Y., in Thirteenth International Combustion En-
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Formation in Combustion, Springer-Verlag, Berlin,
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6. Eichlseder, H., Rechberger, E., and Staub, P., inFu nfte
Tagung, Arbeitsprozess des Verbrenungsmotors, AVL,
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10. Harndorf, H., in Zweite Indizier Symposium, AVL,
Darmstadt, Germany, 1996.
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Twenty-First International Congress on Combustion
Engines, (CIMAC), Interlaken, 1995, pp. 119.
12. Baulch, D. L., Cobos, C.J., and Cox, R. A., J. Phys.
Chem. Ref. Data 21(3) pp. 411429 (1992).
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COMMENTS
Cary Presser, NIST, USA. How would the characteristics
(quality) of H
2
O
2
/H
2
O spray inuence soot formation pro-
cesses in the DI diesel engine? What was the degree of
mixing between the H
2
O
2
/H
2
O spray and the diesel spray?
Authors Reply. During the present series of experi-
ments, we did not vary the characteristics of the H
2
O
2
/
water spray. The injection pressure was always 300 bar, the
nozzle used has ve orices of 110 lm each, and the mean
droplet size of the spray was less than 2 lm. Both injection
systems spray from different external positions into the
center of the piston x-bowl. The injection of the diesel
spray always started at 10 CA; the duration was about
10 CA. The timing of the H
2
O
2
/water spray was varied
between 40 CA and 70 CA with a spray duration of
also about 10 CA. For comparable spray times of both
systems, we observed some interference. The degree of
mixing of both sprays was not studied in detail.