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2000-01-2206
1
COMPACT PLASMA BOOSTED REFORMERS rotation in order to minimize electrode erosion. The
hydrocarbon fuel and additional air are injected down-
Plasmatrons provide highly controllable, ohmic heating of stream from the electrodes. The mixture of hot air and
gases to elevated temperatures. At these temperatures, vaporized hydrocarbons enter the plasma reactor where
the gas is partially ionized. The increased temperatures, the reaction takes place.
ionization levels, and mixing provided by plasmatron
heating accelerate reformation of hydrocarbon fuels into Water inlet
hydrogen rich gas. The high temperatures can be used
for reforming a wide range of hydrocarbon fuels into
hydrogen-rich gas without using a catalyst. Thus, it is Plasmatron
possible to eliminate problems associated with catalyst Air inlet
use, such as narrow operating temperature, sensitivity to
fuel composition, poisoning, and response time limita-
tions.
By increasing the reaction rates, plasma heating could
Cathode
significantly reduce size requirements for effective
reforming, increase speed of response and increase fuel
flexibility. A wide range of operation is possible, from par- Anode
tial oxidation to steam reforming. The boosting of the
reaction rate would occur by creating a small high tem-
perature region (5000-10000 K) where radicals are pro-
duced and by increasing the average temperature in an
extended region.
Water outlet
The additional heating provided by the plasma can
ensure a sufficiently high number of chemically reactive Fuel/air/water
species, ionization states, and elevated temperatures for
the partial oxidation reaction to occur with negligible soot Figure 1. Plasmatron fuel converter device. Reaction
production and with a high conversion of hydrocarbon extension cylinder and heat exchanger are
fuel into hydrogen-rich gas. The effective conversion of not shown.
hydrocarbon fuel is aided by both the high peak tempera-
ture in the plasma and the high turbulence created by the Figure 2 shows a photograph of a microplasmatron with-
plasma. out a reaction extension cylinder, operating with air at
about 1.5 kW. The plasma jet is pointing vertically in the
The rapidly variable plasmatron parameters (energy
figure. During reforming operation, fuel and additional air
input, flow rate, product gas composition, etc.) make this
are injected downstream from the stainless steel flange
technology able to respond to the dynamic demands of
shown in Figure 2.
vehicles. It should be practical to instantaneously pro-
duce hydrogen-rich gas for use during cold startup. Figure 3 shows a microplasmatron fuel converter that
Throughout the driving cycle, rapid changes in hydrogen- includes a reaction extender and a heat exchanger. The
rich gas flow can be accommodated by variation of plas- heat exchanger can be used to simultaneously cool down
matron parameters. [8] the hydrogen-rich gas and to preheat the incoming air
and fuel. Preheating the air and fuel reduces the electri-
Figure 1 shows a diagram of a multi kilowatt plasmatron.
cal energy requirement to the plasmatron and increases
The device operates at atmospheric pressure, with air as
the hydrogen yield. Work is continuing in the develop-
the plasma forming gas. The plasmatron operates in DC
ment of a high efficiency, high temperature heat recuper-
mode. The plasmatron consists of a copper cathode with
ator. Simple calculations show that using preheat can
a hafnium tip, and a copper tubular anode [14]. The elec-
reduce the electrical power requirements to the plasma-
trodes are separated by an electrical insulator made out
tron by half.
of fiberglass (G-10). The cathode and anode are water
cooled, and this cooling represents a sink of energy. A typical microplasmatron fuel converter includes a steel
Measurements on the water temperature rise indicate tube 4-cm in diameter and 15-cm long. It is thermally
that the plasmatron is about 70–80% efficient. Hafnium insulated by fiberglass felt and steel screens. The
allows operation on air as the plasma forming gas. The samples of hydrogen rich gas are cooled down and ana-
hafnium tip has a high electron emissivity and relatively lyzed using gas chromatography (GC). Table 1 shows
long lifetime using a current less than ~100 A. the typical plasmatron range of operating parameters for
a DC arc device. Materials that could be used for various
The plasma arc ignites across the electrode gap. Air is
components of the plasma-boosted reformer are copper,
injected tangentially upstream from the electrodes to pro-
zirconium and molybdenum. Conversion efficiency, elec-
duce a vortex that elongates the plasma inside the tubu-
trode life, size, and weight are essential feasibility issues
lar anode. The anode root of the arc is in constant
and require detailed experimental investigation.
2
The microplasmatron used in the engine experiments
described in the following section is shown in Figure 3.
The plasmatron is followed by a reaction extension cylin-
der, a simple heat exchanger (not cooled for the present
experiments), and a gas-to-water heat exchanger, used
to cool the reformate.
Steel 130
110
Secondary in Plasmatron
extender cylinder plas matron heat losses
100 heat losses Referred to
(heat exchanger)
90
electrical energy
related to electrical energy
80
3
of the system makes up for the decreased residence microplasmatron device used in the engine experiments
time. Figure 6 shows the composition of the reformate for described in the following section. During the engine
diesel as the fuel, as a function of the oxygen to carbon experiments, the unit operated at 270 W.
ratio. The hydrogen concentration is relatively constant.
The low current microplasmatron consists of a central
Microplasmatron fuel converters have substantial electrode, an insulator, and a tubular grounded electrode.
dynamic range. The lower power is determined by the The air-fuel mixture is introduced into the gap between
maximum voltage capability of the power supply (the volt- the electrodes creating a plasma discharge with charac-
age increases with decreasing current), while the highest teristics similar to those of a glow discharge (500–1000 V,
power is determined by erosion of the electrodes. It is 20-100 mA). The reaction is created by intimate contact
expected that a dynamic range of a factor of 10 is possi- of the air-fuel mixture with the discharge from the plasma
ble without substantial modification to the plasmatron and propagates through the reaction extension cylinder.
device. This is sufficient to provide the required change
in throughput for conventional engines. For hybrid vehi- ENGINE EXPERIMENTS
cles, with engines operating at constant or near constant
conditions, the plasmatron fuel converter would operate Microplasmatron reforming experiments were conducted
at near constant conditions, with air/fuel/power manage- using a production in-line four-cylinder SI gasoline-fueled
ment requirements that are much simpler than for con- engine (1995 General Motors Quad-4) at Oak Ridge
ventional drive. National Laboratory (ORNL). The Quad4 has a 2.3-L
displacement, 9.2-cm bore, 8.5-cm stroke, and compres-
Dependence of diesel converion to light hydrocarbons on air/fuel ratio
820 kJ/mol diesel
sion ratio of 9.5. This engine is port-fuel-injected and
no preheating does not utilize a turbocharger or exhaust gas recircula-
100%
tion. The engine was coupled to a 130-kW (175-hp)
90%
Diesel to light hydrocarbons conversion
70%
speed and load control. Engine control management
60% was carried out with a TEC-II control system (Electromo-
50% tive, Inc.) The TEC-II provided access to all calibration
40% parameters (base fuel curve, enrichment, and spark
30% advance) for proper engine operation. The TEC-II control
20%
allows the user to set a desired air/fuel ratio. It can also
10%
adjust the fuel automatically to maintain stoichiometric
0%
0.40 0.50 0.60 0.70 0.80 0.90 1.00 1.10 1.20 1.30 air/fuel ratio by monitoring the exhaust gas oxygen.
Oxygen to Carbon ratio
20 R EACTION
18 EXTENSION
16
CYLINDER
H2
14
Volume fraction (%)
CO
12
CO2
10
CH4
8
C2H4
6 C2H2
4
2
G ROUND ELECTRODE
0
0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.3
Oxygen to Carbon ratio
I NSULATOR
LOW CURRENT MICROPLASMATRON DEVICE
4
Along with engine operating parameters and in-cylinder the 1500 rpm condition. The maximum reformate flow
pressure, engine out regulated emissions (CO, HC and rate was determined by heat removal limitations of the
NOx) and PM were measured at each operating point. plasmatron reactor. Bench top tests are being conducted
Total mass concentration and rate of PM was measured in the laboratory to remove this limitation.
with a Tapered Element Oscillating Microbalance (TEOM,
R and P Co. Model 1105). A scanning mobility particle RESULTS AND DISCUSSION
sizer (SMPS, TSI, Inc.) measured PM size and number.
CARB Phase II certification grade gasoline was used for Figures 8 and 9 show the Coefficient of Variation of the
engine and plasmatron operation. The gasoline equiva- gross Indicated Mean Effective Pressure (COV of IMEP)
lent air/fuel ratio was measured with a universal exhaust as a function of equivalence ratio for the two operating
gas oxygen (UEGO) sensor (Horiba MEXA 110) in the conditions. Both cases of baseline operation (without
exhaust stream. Therefore during reformate addition, the reformate addition) and the case with reformate addition
reported equivalence ratio from the UEGO sensor is are shown in the figures. The equivalence ratio in these
higher (richer) than the actual equivalence ratio because figures has been determined from the exhaust gas com-
of the effect of burning both gasoline from the engine and position. The presence of hydrogen in the engine sub-
reformate from the microplasmatron on the UEGO sen- stantially reduces the COV of IMEP, even at the 2300 rpm
sor. condition, when the reformate addition is a small fraction
of the total fuel.
The microplasmatron was operated with a constant gaso-
line throughput of 0.25 g/s. The reformate was cooled
10.0
down to room temperature by a low-pressure shell-in-
9.0 Baseline Hydrogen Assist
tube heat exchanger. The composition of the microplas-
8.0
matron output was continuously monitored using a con-
7.0
ventional tailpipe emissions monitor (Horiba MEXA 554).
6.0
H2 16% NA
5.0
N2 60% NA
4.0
HC by FID (ppm C3) NA 260-410
3.0
Experiments were conducted at two engine operating 2.0
conditions: the first one at 2300 rpm and 4.2 bar brake 1.0
mean effective pressure (BMEP); and the second one at 0.0
1500 rpm and 2.6 bar BMEP. Maximum brake torque 1.10 1.00 0.90 0.80 0.70 0.60
(MBT) spark timing was defined for both operating condi- Equivalence Ratio
tions at stoichiometric conditions with the engine in Figure 9. COV of IMEP as a function of exhaust
closed-loop control mode. Once the MBT spark timing equivalence ratio (2300 rpm, 4.2 bar BMEP).
was defined for each condition, spark timing remained
fixed as air/fuel ratio was increased with the engine in Figures 10 and 11 show the NOx emissions as a function
open-loop control mode. BMEP was also kept constant of the COV of IMEP. The plots illustrate the reduction of
as air/fuel ratio was increased. NOx emissions within acceptable levels of cycle-to-cycle
Reformate was introduced into the engine via the intake combustion variations (3 to 5% COV of IMEP). The NO x
manifold downstream of the throttle. The overall hydro- concentration decreases with the reformate addition for a
gen addition was relatively small, being about 4% of fuel given COV of IMEP, even with relatively small reformate
heating value at the 2300 rpm condition and about 9% at addition. At a COV of 5%, NOx is reduced by a factor of
5
about a hundred by the addition of plasma boosted Use of the microplasmatron caused a relatively small
reformer generated hydrogen at 1500 rpm engine opera- decrease in thermal efficiency (see Figures 16 and 17).
tion. Higher reformate addition may be necessary, espe- Thermal efficiency was degraded because of the fuel that
cially for the higher load cases. The plasma-boosted is reformed and the microplasmatron electrical power
reformer is presently being modified to provide increased consumption. When the proportion of plasmatron output
hydrogen generation. is higher (e.g., the 1500 rpm engine condition), the effi-
ciency penalty is reduced at lower equivalence ratios due
30.0 to improved combustion stability.
Baseline Hydrogen Assist
25.0
12.0
Baseline Hydrogen Assist
20.0
NOx (g/kW-hr)
10.0
15.0
8.0
HC (g/kW-hr)
10.0
6.0
5.0
4.0
0.0
0.0 2.0 4.0 6.0 8.0 10.0 2.0
COV IMEP (%)
0.0
Figure 10. NOx emissions as a function of the COV of
0.0 2.0 4.0 6.0 8.0 10.0
IMEP (1500 rpm, 2.6 bar BMEP). COV IMEP (%)
The corresponding concentration of hydrocarbons is Figure 12. Hydrocarbon emissions as a function of the
shown in Figures 12 and 13, for the 1500 and 2300 rpm COV of IMEP (1500 rpm, 2.6 bar BMEP).
operating conditions, respectively. Decreases in HC
emissions of about 20-30% are possible. Larger effects 12.0
could be possible with the additional of increased Baseline Hydrogen Assist
amounts of hydrogen rich gas. 10.0
showed very low values for both the baseline and refor-
mate addition cases. Figure 14 shows the relative mass 6.0
emissions decrease from the baseline stoichiometric
case. Although the TEOM was approaching its lower 4.0
sensitivity limits, the trend is still clear; decreasing equiv-
alence ratio leads to lower PM mass emissions. In addi- 2.0
30.0
Baseline Hydrogen Assist
25.0
20.0
NOx (g/kW-hr)
15.0
10.0
5.0
0.0
0.0 2.0 4.0 6.0 8.0 10.0
COV IMEP (%)
Figure 14. Relative PM emissions as a function of
Figure 11. NOx emissions as a function of the COV of equivalence ratio (1500 rpm, 2.6 bar BMEP).
IMEP (2300 rpm, 4.2 bar BMEP).
6
DISCUSSION
dN/dlogDp (#/cc) 6000
The addition of reformate stabilized engine operation
0.71 P under lean fueling, resulting in lower NO x emissions.
4500
Similar results should be obtainable with reformate addi-
3000 0.83 P
tion at high EGR levels. The exhaust gas has a larger
heat capacity than air (due to the higher concentration of
1500 1.0 P tri-atom molecules in the exhaust gas), and therefore
1.0 NOx reduction with EGR should be larger than with air
0
5.42 11.9 [1]. Tests are being planned to investigate the effects of
26.4 58.2 EGR with reformate addition.
128.
Dp (nm) In a similar fashion to other reformer concepts such as
those used for reforming ethanol [12,13], the plasma-
boosted reformer is also ideally suited for cold-start con-
ditions, due to the rapid response time of the microplas-
Figure 15. Particle size distribution for four different
matron. The time of microplasmatron operation without
equivalence ratios (designated by labels) at
preheat and with a high fraction of fuel to the device is
1500 rpm, 2.6 bar BMEP. P designates
limited to cold start and is thus very small. During cold
hydrogen assist. Note the overall numbers
start, a high fraction of the fuel would be converted into
are very low.
hydrogen-rich gas. As soon as the catalyst is warmed
up, the fraction of processed fuel would be decreased.
40
35
Onboard generation of hydrogen-rich gas using a
plasma-boosted microreformer could provide important
30 new opportunities for significantly reduced emissions. A
compact plasma boosted reformer was successfully inte-
grated with a gasoline engine on an engine test stand. SI
25
engine experiments were carried out to determine the
effect of reformate addition on emission and efficiency.
20
NOx emissions reduction of two orders of magnitude was
1 .1 0 1 .00 0.90 0.80 0.70 0 .6 0 obtained. The plasma boosted microreformer operated
E qu iva le nc e R atio reliably for the relatively long duration of the experiments
(>6 hours per day), operating on gasoline. Additional
Figure 16. Engine thermal efficiency as a function of
effort is required to decrease the electromagnetic noise,
equivalence ratio (1500 rpm, 2.6 bar BMEP).
as well as to better integrate the microplasmatron fuel
converter with the engine. The rapid response, as well
40 as the robustness to fuel characteristics and ambient
B a selin e H yd roge n A ss ist temperature, makes the plasma-boosted microreformer
suitable as a fuel converter for a variety of onboard appli-
T he rm a l E ffic ie n cy (% )
35
cations.
30 ACKNOWLEDGMENTS
7
REFERENCES 8. D.R. Cohn, A. Rabinovich, C.H. Titus and L. Brom-
berg, Near Term Possibilities for Extremely Low
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damentals, McGraw Hill, 1988. eration of Hydrogen, Int. J Hydrogen Ener 22 715
(1997).
2. Breshears, R., Cotrill, H. and Rupe, T., Partial Hydro-
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Development, Ann Arbor, MI Oct (1973). Generation Technology for Vehicular Applications, J.
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