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Documente Cultură
DR ALY H. SHAABAN
HQ AIR FORCE CIVIL ENGINEERING
SUPPORT AGENCY
HQ AFCESAIRACO
TYNDALL AFB FL 324035323
. OTIC
AUGUST 1994
ELECTED
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Auoust 1994
4,
6. AUTHOR(S)
ALY H. SHAABAN; Ph.D.
a.
PERFORMING ORGANIZATION
REPORT NUMBER
ESL-TR-92-55
10. SPONSORING/ MONITORING
AGENCY REPORT NUMBER
j 13. ABSTRACT
This research effort Investigated the effects of anode depolarization and pulsed DC on the
performance of the water electrolytic process for hydrogen generation. An experimental
approach was Implemented using the FmO 1-LC electrolytic cell manufactured by ICI Chemical
& Polymers Company. The FmOH.C had a stainless steel cathode and platinum-cooled titanium
anode. Using a 10 percent by weight sulfuric acid as on electrolyte, the experimental results show
that significant Improvement in the performance of the water electrolysis Is feasible. The anode
depolarization process has the potential of Improving the water electrolysis performance up to
three limes that of the conventional water electrolysis. On the other hand, Using pulsed DC
caused current polarity reversal during the off period of the pulse. Placing a diode in the circuit
prevented the polarity reversal but allowed the electrolytic cell to maintain a DC voltage level of
2.3 volts. The results of pulsed DC are In conflict with those reported In the literature. A boslc
research program Is proposed to Investigate the effects of pulsed DC. anode depolarization with
the use of the state-of-the-art 3D ultramlcroelectrodes.
14.
SUBJECT TERMS
WATER ELECTROLYSIS
ANODE DEPOLARIZATION
SECURITY CLASSIFICATION
OF REPORT
UNCLASSIFIED
17
PULSED DC
HYDROGEN GENERATION
OF THIS PAGE
UNCLASSIFIED
20 LIMITATION OF ABSTRACT
'
'Jl
. j'J.':i
EXECUTIVE SUMMARY
A.
OBJECTIVES
The objective of lhis reseach is to document the performance of the electrolysis process
for hydrogen generation when pulsed DC and anode depolarization are used. The resulting data
were to be used in designing an efficient electrolytic cell that meets the Air Force needs.
B.
BACKGROUND
Hydrogen can play an important role in future energy systems because of the diversity of
its applications, the variety of ways in which it can be stored, its environmental advantages, and
the possibility of producing hydrogen using solar, nuclear, wind, hydropower, and other renewable
energy sources. The environmental impact of hydrogen as a source of energy is very favorable .
Signs of the world moving to the hydrogen economy are evident. The Euro-Quebec HydroHydrogen agreement will produce 20 million cubic feet of pure electrolytic hydrogen per day for
use as transportation fuel at Hamburg, Germany, and to fuel a hydrogen-powered version of the
European-made Airbus _aircraft.
The U.S. Department or Defense interest in hydrogen applications is growing fast. The
Army Research Office (ARO) obtained a 500-watt fuel cell design that weighs less than 10
pounds for individual soldier power. Currently, ARO is exploring the feasibility of using fuel cells
for power generation on the battlefield. The requirement is a small, light, and inexpensive
hydrogen supply device which could convert a readily available material to hydrogen of sufficient
purity to operate the fuel cells. If such a device can be engineered with efficiencies much higher
than those of existing methods, hydrogen would play a viable economic role in future Air Force
applications. These applications could include heat pumps; power generation; and fuel for
cooking, vehicles, and aircraft.
Water electrolysis is a simple process where electrical energy is converted to chemical
energy in the form of hydrogen. However, the very use of electrical energy is the major
disadvantage of the water electrolysis. Electrical energy Is relatively expensive, and efforts are
underway to maximize the efficiency of the water electrolysis process so that hydrogen can be
produced at levels competitive with the production of petroleum fuel.
C.
SCOPE
This research effort investigated the performance of water electrolysis using anode
depolarization and pulsed DC power. The research consisted of four major tasks: 1) develop a
laboratory experiment; 2) examine the anode depolarization effects; 3) examine the pulsed DC
power operation; and 4) examine the combined effects of pulsed DC and anode depolarization.
Due to the lack of 6.1 funds, only the first task was completed while the second and third tasks
were partially accomplished.
iii
D.
RESULTS
The experimental results show that significant improvement in the performance of the
water electrolysis is feasible. Using sulfur dioxide as anode depolarizer dissolved in a 10 percent
by weight sulfuric acid anolyte has the potential of improving the process performance up to three
times that of the conventional water electrolysis. In the case of pulsed DC, the results are in
conflict with those reported in the literature, and further work is needed to settle the issue of using
pulsed DC in water electrolysis.
E.
RECOMMENDATIONS
This research offers many potential payoffs that would benefit the Air Force and other
branches of the United States Government. Given a clearer understanding of the electrolytic
process behavior at ionic level, advances are possible in the areas of electrode material and
design, depolarizers, and electrolytes. Therefore, a basic research program is recommended and
a new design based on the state-of-the-art ultramicroelectrode technology, is proposed. The use
of these three-dimensional electrodes will increase the contact time with the depolarizer material
which translate to larger hydrogen production. The hydrogen yield density is expected to be 1
to 2 order of magnitude greater than the conventional two-dimensional electrodes.
The overall
goal of the proposed research is to explicitly account for the characteristics of the double-layer
and the nature of the oxidation process at the anode in describing the electrolytic process
behavior under varied loading conditions.
iv
PREFACE
This report was prepared by the Air Force Civil Engineering Support Agency (AFCESA),
Research, Development, and Acquisition Division, Air Base Operability and Repair (RACO) and
Applied Research Associates (ARA). ARA efforts were performed under SETA Contract Number
F08635-C-88-0067.
The author wishes to express his gratitude to Mr Edgar Alexander for his interest in this
project and continuous encouragement and support during the course of this effort. The author
wishes to thank Dr Lany C. Muszynski for his help during the course of this effort and Mr Daniel
J. Weston for his contributions in setting up the experiment and the design of the electrical setup.
This report summarizes work done between June 1991 and November 1992. Mr Edgar
Alexander was the AFCESA Project Officer.
This report has been reviewed by the Public Affairs Office and is releasable to the National
Technical Information Service (NTIS). At NTIS, it will be available to general public, including
foreign nations.
This technical report has been reviewed and is approved for publication.
~::I
Frank P Gallagher Ill, Col, USAF
Director, Air Force Civil Engineering Laboratory
Eddr;-;,lexander,
Project Manager,
Chief, Airbase Operability and Repair Branch
Ao<~eesian
'------
7-*f.U./..JJ:k
Felix T. Uhlik, Lt. Col., USAF
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TABLE OF CONTENTS
Title
Section
INTRODUCTION . . . . . . . . . . . . . . . . . . . . . . .
A.
OBJECTIVES . . . . . . . . . . . . . .
B.
BACKGROUND . . . . . . . . . . . . .
C.
SCOPE . . . . . . . . . . . . . . . . . . .
.....
..
...
..
1
1
1
2
Ill
EXPERIMENTAL WORK . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .
A.
EXPERIMENT SETUP . . . . . . . . . . . . . . . . . . . . . . . . . . . .
B.
LABORATORY TEST SERIES ......................
1.
Baseline Test, Non-pulsed DC Power . . . . . . . . . . . .
2.
Pulsed DC Power. ..........................
3.
Baseline Anode Depolarization. . . . . . . . . . . . . . .
9
9
11
11
11
14
IV
15
15
32
32
32
32
II
REFERENCES ......................... .
BIBLIOGRAPHY
''."
......
'.'
Vii
. . . . . .
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....
..
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..... ......
...........
...........
...........
0.
,,
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....
....
....
....
.........
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....
...
6
8
30
33
33
35
36
37
"
.....
'
3
5
5
'
'
39
4'7
LIST OF FIGURES
Figure
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
Title
viii
Figure
25
Title
Experiment Setup Response For 50 Percent Duty Cycle and 40 kHz Pulse at 100 ccm
Hydrogen Yield. . ....
25
Experiment Setup Response For 80 Percent Duty Cycle and 10 Hz Pulse at 100 ccm
Hydrogen Yield. . ...........
25
Experiment Setup Response For 80 Percent Duty Cycle and 500Hz Pulse at 100
ccm Hydrogen Yield. . . . . . . . . . . . . . . . . . . . . . . ................... , .
26
Experiment Setup Response For 80 Percent Duty Cycle and 1 kHz Pulse at 100 ccm
Hydrogen Yield. . .....................................
26
Experiment Setup Response For 80 Percent Duty Cycle and 5 kHz Pulse at 100 ccm
Hydrogen Yield. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27
Experiment Setup Response For 80 Percent Duty Cycle and 10 kHz Pulse at 100 ccm
Hydrogen Yield. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27
Experiment Setup Response For 80 Percent Duty Cycle and 25 kHz Pulse at 100 ccm
Hydrogen Yield. . . . . . . . . . . . . . . .
................
28
Experiment Setup Circuit Power Demands. . .. , ........
28
Electrolyzer Power Demands (power vs. duty cycle) . . . . . . . .
....
29
Electrolyzer Power Demands (power vs. frequency) . . . . . . . . . . . . . . . . . . . . . . . 29
Performance Characteristics of the ICI Electrolyzer With S02 Saturated Anolyte. . . 30
Anode Depolarized Hydrogen Generation Rate vs. Power Demand. . . . . . . . . . . . . 31
0
26
27
28
29
30
31
32
33
34
35
36
ix
SECTION I
INTRODUCTION
OBJECTIVES
The principal objective of this research is to examine the effects of pulsed DC power and
anode depolarization on the performance of the water electrolysis process. The resulting data
then to be used in the design of an efficient electrolytic machine that meets Air Force needs.
B.
BACKGROUND
Hydrogen can play an important role in future energy systems because of the diversity of
its applications, the variety of ways in which it can be stored, its environmental advantages, and
the possibility of producing hydrogen using solar, nuclear, wind, hydropower, and other renewable
energy sources. The ecvironmental impact of hydrogen as a source of energy is very favorable.
It bums cleanly and can be obtained from water with water vapor as its combustion product.
The present market for hydrogen is limited to food hydrogenation, ammonia, and
metallurgical processes. In the future, when the so-called hydrogen economy starts to take place,
energy will be a major hydrogen user market which will dwarf the present market Hydrogen
applications in energy areas range from consumption of hydrogen as a fuel (e.g. transportation
fuel, home heating and cooking, etc.) to closed cycle applications as in the metal hydrides heat
pump. Signs of the world moving to the hydrogen economy are evident The Euro-Quebec
Hydro-Hydrogen agreement [1] will produce 20 million cubic feet of pure electrolytic hydrogen per
day for use as transportation fuel at Hamburg, Germany, and to fuel a hydrogen-powered version
of the European-made Airbus aircraft.
Combined with other elements hydrogen can be found in abundance. For example, one
mole of water consists of one mole of hydrogen combined with half a mole of oxygen. Several
methods were devised to liberate hydrogen from hydrides. Water electrolysis is the commercially
applied process to obtain hydrogen from water at 99.99 percent purity. Water electrolysis is a
simple process where electrical energy is converted to chemical energy in the form of hydrogen.
However, the very use of electrical energy is the major disadvantage of the water electrolysis.
Electrical energy is relatively expensive and efforts are underway to maximize the efficiency of
the water electrolysis process so that hydrogen can be produced at levels competitive with the
production of petroleum fuel.
The U.S. Department of Defense interest in hydrogen applications is growing fast. The
Army Research Office (ARO) obtained a 500-watt fuel cell design that weighs less than 10
pounds for individual soldier power. Currently, ARO is exploring the feasibility of using fuel cells
for power generation on the battlefield. The requirement is a small, light, and inexpensive
hydrogen supply device which could convert a readily available material to hydrogen of sufficient
purity to operate the fuel cells. If such a device can be engineered with efficiencies much higher
than those of existing methods, hydrogen would play a viable economic role in future Air Force
applications. These applications could include heat pumps; power generation; and fuel for
cooking, vehicles, and aircraft.
C.
SCOPE
This effort experimentally studied the performance of water electrolysis for hydrogen
generation under two concepts: (1) the depolarization of the anode using sulfur dioxide to
reduce/eliminate the anodic losses; and (2) the use of pulsed DC electric power instead of the
nonpulsed DC currently used.
The effort involved the development of a laboratory experiment which consisted of a series
of tests using the Fm01-LC electrolytic cell, manufactured by ICI Chemicals & Polymers. The
tests were divided into four series: (1) A nonpulsed DC power test set to determine the cell's
baseline performance; (2) Anode depolarization under nonpulsed DC power test set to determine
the cell baseline performance efficiency using sulfur dioxide as anode depolarizer; (3) A pulsed
DC power test set to determine the cell performance as a function of the pulsed energy
parameters; and (4) Anode depolarization under pulsed DC power test set. Due to cuts in 6.1
findings, only the first three were partially accomplished.
SECTION II
where the electrical energy is converted to chemical energy as hydrogen. The reaction at the
electrodes can be as follows:
a.
2H20
b,
2e-
H2
20W
(2)
ow ~ 1 0:z
2
+ H2 0 + 2e-
(3)
In this process water is consumed and only two electrons are involved in the dissociation
of one molecule of water. There are no side reactions in water electrolysis that could yield
undesirable products, so the process is clean and requires no extra separation or purification of
products.
The first law of thermodynamics for an open system states that :
Q- W = AH
(4)
w.
Ws = -nFE
where:
n
F
(5)
t:.H- Q
(6)
nF
For isothermal reversible process (no losses), Q is given as
(7)
Q,... = T t:.S
where T is temperature and .oS is the change in system entropy. Substituting Equation (7) into
Equation (6) results in the definition of the cell reversible potential below which neither hydrogen
nor oxygen can be generated.
= t:.H - Tt:.S
(8)
nF
(,;.H-T.oS) is the change in the system Gibbs free energy ,;.G . At standard conditions ( 25 'C and
1 atm ) ,;.H equals 68,320 callgmole and ,;.G equals 56,690 callgmole. Therefore, the cell
reversible potential equals to
E
ff1V
t:. G =
nF
56,690 a
2 (23,074)
1.23 volts
(9)
Because of the inefficiencies in the electrolysis process, the potential required to drive an
electrolysis cell at a practical hydrogen generation rate ( i.e. current, /, which is proportionate to
hydrogen generation) is higher than the cell reversible potential. In Equation (6), n and F are
constants, and for the same conditions of pressure, temperature, and electrolyte concentration,
91 is constant and Q will change as E changes. As the process becomes irreversible and
inefficient, Q decreases and eventually becomes negative where electric energy is wasted as
heat At the point where no heat need to be added to the cell ( Q=O ) and all energy needed is
supplied by electrical energy, the corresponding cell potential is called the thermoneutral voltage.
This potential is given by :
E-
t:.H
= --
nF
1.48 volts
(1 0)
However, current cell design requires operating voltages higher than the thermoneutral voltage.
At these operating voltages, part of the electrical energy is lost as heat which raises the cell
temperature and requires cell cooling.
The operating potential of an electrolyzer is given by:
E = E,...
Losses
(11)
(12)
----------------------------------------------------------------
where
6.H
'11 =
Etl>mm
ll.G + losses
(13)
Therefore, under ideal conditions (no losses or reversible process), the production of hydrogen
will take place with an efficiency of 120 percent, and at therrnoneutral conditions the cell efficiency
is 100 percent
Current electrolyzers are running at 75 percent efficiency. The exergy analysis of the
water electrolysis process shows the majority of the losses are caused by the cell internal design
and not external emission. To reach higher electrolysis efficiency, current research efforts are
devoted to optimizing cell design to reduce internal losses.
B.
In the interior laminas of an electrolyte, the net charge is zero. This is because the
solvent dipoles are in random orientation and equal distribution of positive and negative charges
exists. For the ion discharge to take place, the electrical charge on the electrode has to be
matched by an opposite charge in the electrolyte across the electrode-electrolyte interface where
a potential difference arises. Therefore, upon applying an electrical field, the electrical forces
operating at the electrode-electrolyte interface give rise to another arrangement of solvent dipoles
and charged species. A net orientation of solvent dipoles and a net or access charge on a lamina
parallel to the electrode are established. The existence of two oppositely charged layers gave
rise to the term double-layer. The term double-layer is used to describe the arrangement of
charges and orientated dipoles constituting the interphase region at the boundary of the
electrolyte. Figure 1 shows the electrified interface in the double-layer concept The charge and
discharge of the double-layer could play a role in improving the performance of water electrolysis .
C.
The thermodynamic analysis of water electrolysis indicates that the electrical energy
required for a practical dissociation rate can be reduced if the number of electrons involved in the
reaction (Equation 6) is maximized and the losses that increase the cell potential (Equation 11)
are minimized. The activation overpotential is one of these losses and represents the energy
required to overcome the surface potential barrier which retards the ionic discharge processes
to the electrodes. The activation overpotential is largely at the anode [2] and represents most of
the losses in the electrolyzer cell. In order to enhance the ionic discharge, and thus the hydrogen
evolution rate, we must diminish the energy barrier at the anode. However, diminishing the anode
overpotential by using catalysts [3] while keeping oxygen evolution is expensive and will not
reduce the cell potential below the reversible potential of 1.23 volts.
-------------------------------Anode
Layer 1
Figure 1 :
If the oxygen el01ution is replaced by another anodic reaction that takes place at lower
potential than that of oxygen, then the cell potential (Equation 6) would be reduced. This process
is called anode depolarization. Further, if the new anodic reaction involves more electrons, then
the reversible potential, E.... and hence the cell potential, E, would be reduced dramatically.
Another likely approach to enhance ion discharge [4] would be a modification to the
conventional electrolysis process and would involve assisting the electrochemical reaction by
supplying either part or all of the energy required to overcome the surface potential barrier by
using some energy form other than DC electric energy. In this area Brookhaven National
Laboratory (BNL) [5] identified the utilization of heat and electricity in water vapor electrolysis,
while Gutmann and Murphy [4] suggested the use of pulsed DC.
One major disadvantage in water electrolysis is the use of electricity as raw energy. If the
electricity is produced by a thermal conversion of coal or oil, the Camet limitation is applied,
thereby limiting the process's overall efficiency. Renewable energy such as solar/photovoltaic,
wind power, and hydroelectric power are attractive raw energy sources for water electrolysis. The
use of solar energy in water electrolysis for hydrogen production has been studied in laboratory
settings using a poly crystalline Si photovoltaic 100 W generator [6]. During the same period it
has been demonstrated on a practical scale at an existing 350 kW photovoltaic site in Saudi
Arabia [7]. This link between photovoltaic power and electrolysis eliminated the complex power
conditioning interface required when AC electric energy is used and, in tum, eliminated the losses
encountered in converting AC to DC.
1.
Anode Depolarization
as depolarizers because their use injects an increasing amount of C0 2 into the atmosphere.
Other anode depolarizers suggested by Gutmann and Murphy [4] are NO, which
can be obtained from stack gases, and sea water. In the case of sea water, the expected anodic
product is chlorine. The industrial production of chlorine by brine electrolysis is a large industry
and involves sophisticated technologies. Adaptation of these technologies could yield efficient
electrolyzers for hydrogen production. One advantage of the anode depolarization process is that
instead of oxygen evolution at the anode there will be some valuable by-products that can be sold
and further reduce hydrogen production costs.
2.
Pulsed DC Power
Using a mechanically interrupted DC power supply, Bockris et. al. [14, 15] reported
two phenomena in 1952. Immediately upon application of voltage to an electrochemical system,
a high but short-lived current spike is observed. When the applied voltage is disconnected,
significant current continues to flow for a short time. They explained the first phenomenon as a
double-layer capacitance-charging transient, followed by the electrochemical discharge of the first
ionic layer, giving rise to the current, then replenished by the ionic mass transport from the bulk
of the electrolyte. The second phenomenon is due to ions in the double-layer facing the electrode
being discharged in the_absence of the externally applied field.
In 1984, Ghoroghchian and Bockris [23] designed a homopolar generator to drive
an electrolyzer on pulsed DC voltage. They concluded that the rate of hydrogen production would
be nearly twice as much as the rate for DC. Their conclusion was in agreement with the earlier
works of Tseung and Vassie [24] and Jasem and Tseung [25]. In these earlier works [24,25] they
attributed the increase in hydrogen and oxygen evolutions to an improvement in electrolyzer mass
transfer. lbl [26] also has shown that the application of short high-voltage pulses yields the
highest possible electrolysis current. He concluded that pulsing affects the surface state of the
electrodes. During conventional electrolysis, film of the gas bubbles forms on the electrode,
raising its resistance overpotentiaL Pulsed voltage will eliminate the resistance overpotential of
the gas bubbles. Viswanathan et. al. [29] showed that the thickness of the pulsating double-layer
(they termed it as diffusion layer) is a function of the characteristics of pulsed DC. Further,
pulsing action on electrochemical systems could give rise to the ionic vibration potentials. A more
drastic effect is to be expected if pulsed power is applied at frequencies resonating with the
dominant ionic discharge components. Thus, one of the methods for enhancing the ionic
exchange is the pulsed electrolysis.
The use of pulsed DC for electrochemical reactions, especially in electroplating,
is not new. In 1955 Robotron Corporation obtained a patent for "High Voltage Electroplating"
using pulsed power [28]. In 1966 Popkov [29] further substantiated the advantage of using pulsed
current. Avila and Brown [30] reviewed and confirmed the advantages of pulse plating on the
quality of gold plating for integrated circuitry use, while Bockris and Kita [31] obtained a reduction
in energy requirement by a factor of two. Pulsed electrolysis was also used in battery charging
by Wagner and Williams [32] and Bedrossian and Cheh [33]. In pulsed DC related work, Savage
and Thomtron [34] established that pulsed DC has advantages over continuous DC as reaction
promoter in gas phase synthesis. They attributed the enhancement to the higher mean electron
energies.
--------------------
SECTION Ill
EXPERIMENTAL WORK
EXPERIMENT SETUP
To quantify the effects of pulsed energy and anode depolarization on the performance of
the water electrolysis process, an experimental effort was initiated. The effort involved developing
a laboratory experiment. The laboratory effort consisted of a series of tests using the Fm01-LC
electrolytic cell, manufactured by ICI Chemicals & Polymers, and rated at 38 gram of
H,JKAmp.Hour.
The laboratory setup is shown in Figures 2, 3 and 4. It consists of an electrolyzer setup,
electrolyte make-up water system, pH control, nonpulsed DC and pulsed DC power supply
sources. The electrolyzer setup includes an electrolytic cell (Figure 3) model Fm01-LC, rated at
38 gram of H2/KAmp.Hour, and manufactured by ICI Chemicals & Polymers Company. The
anolyte and catholyte compartments are separated by a Du Pont 324-Naflon"" membrane. The
anolyte and the catholyle are pumped through the corresponding compartment so that the anolyte
and catholyte are separate except for ionic exchange through the membrane. The electrolyzer
has a stainless steel cathode and a platinum-coated titanium anode which were placed 3
millimeters apart. Each electrode has a projected area of 64 square centimeters. Throughout
the experiment a 10 percent by weight sulfuric acid solution was used as the electrolyte.
!FLOWMETER!
Electrode
Gasket
Spacer
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Separator
Gasket
Spacer
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Electrode
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Feed Allolyte
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Figure 3
Figure 4:
10
The key electronic equipment (Figure 4) used in this experiment included the following:
Industrial Equipment Co. power amplifier POWERTRAN model 2000 SHF-1-l<A, (The
POWERTRAN was modified to remove the output transformer to allow it to operate from DC to
70 kHz). The POWERTRAN 2000 SHF-1-XA is capable of 0 to :t 40 volts, 0 to :t 120 Amps with
a maximum continuous power output of 2000 watts AND AN AMPLIFICATION FACTOR OF 25;
a B&K Precision model 3011 B function generator capable of generating square, triangle, and sine
waves at frequencies up to 2 MHz with duty cycles ranges from 1 to 99 percent, with output
amplitude up to 5 volts; a Rapid Power Technologies Inc., DC power supply, model
TRSAA100012, with output 0 to +12 vDC, 0 to 100 Amps and continuous power available of 1000
watts. The electrolyzer was connected to the power supply by two one-foot long #4 AWG bare
copper wires.
The pressure, temperature, and flow (in ccm) of the generated hydrogen and oxygen were
measured using Ashcroft pressure sensors, a J-type thermocouple, and a Teledyne HastingsRaydist flowmeters, model HFM-200, of 0 to 500 seem range. The electric current was measured
using a F.WBell hall-effect current sensor, modeiiHA-100, capable of measuring DC and pulsed
current up to 50 kHz. Both current and voltage were displayed using a TEKTRONIX 2232 100
MHz oscilloscope then plotted using a TEKTRONIX HC-100 plotter. The plots were digitized
using Summa Sketch II Professional digitizer. The current was measured in volts, 50 millivolts
being equal to 1 amp. Voltage measurements were taken at the cell and at power supply output.
This allowed the measurement of line losses.
B.
Four sets of tests were planned. The four test series consisted of: (1) A nonpulsed DC
power test set to determine the cell's baseline performance; (2) A pulsed DC power test set to
determine the cell performance as a function of the pulsed energy parameters; (3) Anode
depolarization under nonpulsed DC power test set to determine the cell baseline performance
efficiency using sulfur dioxide as anode depolarizer; and (4) Anode depolarization under pulsed
DC power test set. Due to cuts in 6.1 findings, only the first three were partially accomplished.
The work accomplished is given in the following paragraphs.
1.
This test series established the performance baseline for the laboratory setup.
First, the deactivation of the cell was studied by recording the change in current at fixed voltage
as a function of time. As shown in Figure 5, the cell reached steady-state conditions 5 minutes
after potential was applied on the cell. Using this cell property throughout the experiment, data
was collected at least 10 minutes after each test started. The cell's hydrogen yield as a function
of cell potential and current was measured (Figures 6 and 7) to determine the cell's baseline
performance. The cell's baseline performance was used for comparison with cell performance
under pulsed DC and anode depolarization.
2.
Pulsed DC Power.
For comparison purposes, the hydrogen yield was kept at 100 cubic centimeter per
minute (ccm) for all pulsed DC runs. This selection was based on the baseline nonpulsed DC
current density results. At 100 ccm of hydrogen (Figure 7), the measured current density was
11
around 320 mA/cm2 which is in the current densities range of 100-500 mAJcm 2 for economical
hydrogen production. The test runs were carried out using square pulse for seven frequencies
and four duty cycles. The duty cycle is the ratio of the pulse on-time to the pulse period. The
seven frequencies are 10 Hz, 500 Hz, 1 kHz, 5 kHz, 10 kHz, 25 kHz, and 40 kHz. The duty
cycles are 10 percent, 25 percent, 50 percent, and 80 percent. The test was divided into four test
runs, one for each duty cycle. Each test run started by measuring the nonpulsed DC current and
voltage for a 100 ccm of hydrogen yield. Then, a duty cycle was selected and the test run pulse
frequency was changed. The cell potential was then changed to maintain the 100 ccm hydrogen
yield. Data collection started after a period of fifteen minutes to allow for steady state condition.
The applied potential was measured at the power amplifier output terminals and
at the cell electrodes. The voltage drop across the one-foot long #4 AWG bare copper wire was
also recorded for some cases. The rate of electrical energy consumption (power) can be
calculated using the relationship:
P=- Ji( t) e( t)
T
at
(15)
where T is the pulse period, i(l) is the current wave form, and e(t) is the voltage wave form.
13,-------,-------,-------,------,-------,-------,-------,
12.5
....
gs
t::
11
9.5
........__J'--~--':-~--:'
L--~--~-.....c--'---'---"---'----'--
10
12
14
Time (min)
Figure 5 :
----------------------------
500
~400
~300
'-'
::-
-~
Q 200
::l
---
...
100
oe-----~----~~-------~~~----~-----J-------~----~
0
Figure 6:
250 ,-----
._,
"0 150
;><
Cl
1to100
so
0~----~----~----~~&B~~~~-----L----~----~
0
Figure 7 :
Hydrogen Yield vs. Cell Potential for 10 Percent by Weight Sulfuric Acid.
13
3.
In this test series, sulfur dioxide was used to depolarize the cell anode. Used in
its gaseous state, it was bubbled through the anolyte prior to and during the cell's nonpulsed DC
operation. The test started by setting the DC power supply output to zero. Then, the potential
was incremented by 0.05 of a volt until a 5 ccm of hydrogen yield was recorded. The applied
potential was then incremented by 0.2 of a volt thereafter. For each voltage increment, the cell
potential, current, and hydrogen flow were measured after steady state was reached.
14
SECTION IV
RESULTS AND DISCUSSION
PULSED DC POWER
During the preliminary test runs, conducted to examine the experiment setup, the current
reversed polarity during the off-period of the pulse (Figure 8). The polarity reversal is attributed
to a reversible reaction in the electrolyzer cell during the off-period. The effect of the current
polarity reversal was seen in the catholyte when its color changed to a light blue. To examine
and quantify the various metals in the catholyte, the atomic absorption spectrometry was used.
The observations were made with a Perkin-Elmer 6500 flame atomic absorption spectrometer,
using a laminar flame burner and equipped with hollow-cathode emission lamps for the different
metals sought. Metals sought were based on the stainless steel alloy content of the cathode.
The catholyte was found to give no absorbance signal for Molybdenum and Titanium, and only
a weak absorbance for copper. Low absorbencies were obtained for Chromium and Zinc, but a
large signal was given for Nickel and Iron. These analyses showed that the cathode had lost
some of its content to the catholyte. This was confirmed by weighing the cathode which showed
2 grams loss. To separate the power amplifier from the cell during the off-time, a Motorola
schottky diode, model MBR8045, was installed. The diode's maximum ratings are 45 volts and
80 Amps. Use of the diode stopped the current polarity reversal, but allowed the cell to maintain
about a 2.3 volts instead of zero volt during the off-period.
I Voltage ~l;l!!~J!t
I
-- 1'
4 .----- - - - - - - - - - - - - - - - - - - - - - - - -
10
'
0
,.....,
~
!-c:
"....
_, u....:::1
10
Time ( millisec)
Figure 8 :
15
10
The digitized waveforms of the current, power amplifier output voltage (source V), and the
cell voltage (cell V) are given in Figures 9-31. The digitized data is given in Appendix A These
figures represent the experiment setup responses in generating the 100 ccm of hydrogen and
cover the test matrix. A careful examination of these figures reveals the current is lagging behind
the voltage, an indication of an inductive circuit. However, the delay in the current is also due
to the cell voltage. With the diode installed, the cell has maintained a DC level of about 2.3 volts.
Until the power supply voltage overcame the cell potential and the losses in the circuit, no current
flowed. As shown in Figure 24 (50 percent duty cycle and 25 kHz), the applied potential is higher
than the electrolyzer's potential by about 25 to 40 percent, and the voltage rise and fall times are
less than 4 micro-seconds with a high current rate of change which is attributed to the low
impedance of the circuit The high voltage drop is due to the large reactive losses mainly
produced by the inductive reactance caused by the high current rate of change. This can be
seen by examining the voltage drop of the negative lead connecting the cell to the power amplifier
and the current waveforms (Figure 24). The relation between the lead voltage drop and the
current is given as:
(16)
where L is the wire inductance. For a one-foot long #4 AWG copper wire, the inductance is in
the range of micro farads; however, the time rate of change of the current is about 2 million amps
per second causing, the high voltage drop.
Figures 9-31 also reveal the interesting shape of the source voltage waveform. Although
the function generator produced a clean voltage square wave, the resulting source voltage
waveform was far from being a clean one. For example, in Figure 24 the source voltage
waveform has a step and a ringing at its trailing side instead of tuming off at the 20th
microsecond from pulse initiation. The shape of the source voltage waveform during the off-time
period of the pulse is the result of the induced voltage in the #4 AWG wires and the cell
maintained voltage of 2.3 volts. The induced voltage in the #4 AWG wires connecting the cell
to the power amplifier is induced by the discharge of current generated by the collapse of
magnetic flux around these wires.
Using Equation (15), the electrical power delivered to the setup circuit and electrolyzer
were calculated. For the setup circuit, the source voltage and current waveforms were used,
while for the electrolyzer the cell potential and current were used to calculate the power
consumption. The results are summarized in Figure 32 for the setup circuit and in Figure 33 for
the electrolyzer. From Figures 32, 33 and 34 the nonpulsed DC (100 percent duty cycle) requires
the least electrical power. The effects of pulse frequency and duty cycle on the electrical power
needed are noticeable. The demand for electrical power increases with the decrease of duty
cycle and pulse frequency. At 10 percent duty cycle the electrolyzer power demand for 10 Hz
is slightly more than twice that of nonpulsed DC, while for 25 kHz it is only 27 percent higher.
It is clear that during this effort one of the two phenomena reported by Bockris et al [ 14, 15] was
not seen, namely, the high but short-lived current spike. Furthermore, the conclusion that
nonpulsed DC requires the least electrical power conflicts with those of Ghoroghchian and Bockris
[23] and Tseung and Vassie [24]. The difference between these results should be investigated
in details so that the use of pulsed DC issue can be settled.
t6
Sou~tage
Current
Ce~ ~9.~!':~tial
10 ~------------------------------------~----------------,
'' ~ ~.:.:..-~.
..__~.__
Figure 9:
'''.
..
_,__ _..__
"'
............ , ............... .. .
ro
Time ( millisec )
'
_L_ _~--L---~__J
100
Experiment Setup Response For 10 Percent Duty Cycle and 10 Hz Pulse at 100
cern Hydrogen Yield.
Br------------~-----------------------------------~
__j
2,000
Experiment Setup Response For 10 Percent Duty Cycle and 500Hz Pulse at 100
cern Hydrogen Yield.
17
.. - - - - - - - - - - - - - - - - - - - - - - - - - - - - - - - l
!Or-------------------------~----------------------------------~
'
.........
... ""''''"'''''"'''"""
-----....
~--
-~-
0~--~~~~==----~~--~--~~---~----~--~---~
0
~
~
~
~
~
Time ( micro sec )
Figure 11 :
Experiment Setup Response For 10 Percent Duty Cycle and 1 kHz Pulse at 100
ccm Hydrogen Yield.
lOr-------------------
8
'"'
~
--'"'
~
i\
"l
I >',i
. \i
r_
' .
-~'\
. _: ---'-- ...
''
' " " ' " ' " " ' " ,,,,
............... .................. ..
,
\---
OIJ
.-l.-----~----'
,~----~~---~~~========--~~----------200
0
so
100
150
Time ( micro sec )
Figure 12:
Experiment Setup Response For 10 Percent Duty Cycle and 5kHz Pulse at 100
ccm Hydrogen Yield.
18
Figure 13 :
Experiment Setup Response For 10 Percent Duty Cycle and 10kHz Pulse at 100
ccm Hydrogen Yield.
16r-----------------------------------------------------------.
14
-'"'"'""'"""-'
.... ., ..
''"""
Figure 14 :
Experiment Setup Response For 10 Percent Duty Cycle and 25kHz Pulse at 100
ccm Hydrogen Yield.
19
------~-~-
_______ _ _____________________________________________j
....
... ,..........
0~----~----~~;~----~----~~----~----~~=-----~----~
0
-~
~
~
Time (micro sec)
Figure 15:
Experiment Setup Response For 25 Percent Duty Cycle and 500Hz Pulse at 100
ccm Hydrogen Yield,
6~--------------------~---------5
400
600
BOO
1,000
Experiment Setup Response For 25 Percent Duty Cycle and 1 kHz Pulse at 100
ccm Hydrogen Yield.
20
6r----~========----~
s
,,
lOll
200
Experiment Setup Response For 25 Percent Duty Cycle and 5 kHz Pulse at 100
cern Hydrogen Yield.
Figure 18:
Experiment Setup Response For 25 Percent Duty Cycle and 10kHz Pulse at 100
cern Hydrogen Yield.
21
8;---------------------------------------------6
'
.........
.......-------
.
.....
-........
Figure 19 :
Experiment Setup Response For 25 Percent Duty Cycle and 25 kHz Pulse at 100
cern Hydrogen Yield.
4~---------------------------------------------------~
,.r-------~---------1
.
I
I
.
I
i
ii
i.
'
0 "---~~----'--
--~ - - - - L I,i. l - - - - ' - - - - - J . _ I_ _ .~'----_J
0
SOO
1,000
I;SOO
2,000
Experiment Setup Response For 50 Percent Duty Cycle and 500 Hz Pulse at 100
cern Hydrogen Yield.
22
4~~~~--~=ooo..~~-----
1---- --
i I./
._,
.g 2 f--~
/ .....--------,------------
-r
0~'----~---=~--~--~=---~~~==~~--~--~~--~--~
0
@
~
Experiment Setup Response For 50 Percent Duty Cycle and 1 kHz Pulse at 100
ccm Hydrogen Yield.
--- .. ---
~3
1- -
Figure 22 :
Experiment Setup Response For 50 Percent Duty Cycle and 5 kHz Pulse at 100
ccm Hydrogen Yield.
23
!~~==========~--~
4 - - ; --_ __ . ; : ; : ; . . . ; . . . . - " ' " - - - - - ,
I
~~~";<""
T -. -
.. -
--.
. --.....
.~
/'
_,.~
~~
.----...--
----~-- \ .
'~I'"'-\.-~
'
-~\
.
\
60
40
20
"'"""'"""'""'"""""
80
100
Experiment Setup Response For 50 Percent Duty Cycle and 10kHz Pulse at 100
ccm Hydrogen Yield.
s,-------------------------~----------4
~3
"5"'
. --
""
. .. ... ........
~2
"'"
.g
~1
e
<
~"''''"...""~~
"
. ,. .
Q,.
--
0~~~-~-~------------------------~~/
I
~--
.....-
.... - - - _ , _
____________~--~~
''-----------------
-1
-2 L....--~----L----~---'1:---~-- --:1:---~---l
10
20
30
40
Experiment Setup Response For 50 Percent Duty Cycle and 25kHz Pulse at 100
ccm Hydrogen Yield.
24
________________________
...
''"
............ ........
10
_-..
13
Experiment Setup Response For 50 Percent Duty Cycle and 40kHz Pulse at100
cern Hydrogen Yield.
4~------------------
',,
0~-~-~--._--~,
ro
80
100
Time ( millisec )
Figure 26:
Experiment Setup Response For 80 Percent Duty Cycle and 10Hz Pulse at100
cern Hydrogen Yield.
25
-_..
3 --
--~.-..
>
"
'./
2.5 ; .. -
... -
....
. ......... ..........
.... .
...... " ..........
......................................
. ........~
..... -- .. .
- -----
.,.
....... -----
-: --
....... ,
'-"
2,-
" ..
:E
!1.S
..... . .....
.. ... -
....;;"-- ....
1 - -;-~---'--==""""''""'-''"''""'"'"==-..;=~;;;;;;;;;:=:,;.;~--=~-"=
o.s
1'!
o~----~-----7.~------------~~----._----~~~--~----~
0
500
1.000
1,500
2.000
Experiment Setup Response For 80 Percent Duty Cycle and 500Hz Pulse at 100
ccm Hydrogen Yield.
------------------,
----
. _______
___ ,
-0.5
---
""
;.
.,.-~--------------------..---------- .
,-
0~~~--.~~--~----~--------~----._--~~--~--~
0
200
400
600
800
1,000
Experiment Setup Response For BO Percent Duty Cycle and 1 kHz Pulse at 100
ccm Hydrogen Yield.
26
I Source Voltage
Current
.-------------~--------------------------------------~
lO
100
:200
Experiment Setup Response For 80 Percent Duty Cycle and 5kHz Pulse at 100
ccm Hydrogen Yield,
.---------------------------------------~----
Figure 30 :
Experiment Setup Response For 80 Percent Duty Cycle and 10kHz Pulse at 100
ccm Hydrogen Yield.
27
I Source Voltage
Current
Ce~-~~~-~.~;Itial
-----
-----------::----------. . . . . .:::-.-,---.!
..
-=--...:.:_
0 L - -...
Figure 31 :
10
'
lD
30
' -.. .
40
Experiment Setup Response For 80 Percent Duty Cycle and 25kHz Pulse at100
ccm Hydrogen Yield.
...
100;-----------------------------------------------------------~
90
.-. 80
~...
'-' 70
60
I
50
40
i
I
Nonpulocd
DC
---~---~----~---J-~-----L----~~~----~--~
0
20
40
60
80
100
26
w~-----------------------------------------~--------~
0
.
-
I
*
40
i
II--
Non-pulsed
DG-
30~--~~--~~---~----~--~----~-----~-----~----------'
0
40
00
00
~
Duty Cycle (%)
Figure 33 :
10%
0
00
- -
0
0
0
6
40
30~----~----~-----------~----~--~~----------=----~----~
0
10
1'
20
25
29
B.
The results of anode depolarization and the baseline nonpulsed DC. test series are given
in Figures 35 and 36 for comparison. Using anode depolarization with 10 percent by weight
sulfuric acid at 30 c with the anolyte fully saturated with S02 , a current of 100 mAmps was
recorded at cell potential of 0.635 volts instead of the 1.8 volts required for nondepolarized
operation. The cell potential fell 1.3 volts below that of the nondepolarized cell potential at a
current density of 30 mA/cm2 At this current density, as seen in Figure 36, the depolarized-cell's
hydrogen yield was three times that of the nondepolarized cell for the same 1. 71 watts of
electrical power delivered.
During test runs the catholyte gradually changed to an opaque bluish color. The test run
was terminated when the current dropped suddenly. Examining the catholyte, revealed a rotten
egg odor confirming the generation of hydrogen sulfide which dissolved in the catholyte, changing
its color. The electrolyzer was dismantled, and sulfur powder was found on the cathode side of
the membrane. This explained the sudden drop in current. The sulfur powder had covered all the
membrane area preventing the ion exchange from taking place. The generation of hydrogen
sulfide and the sulfur covering of the membrane had affected the slope of the anode
depolarization curve given in Figure 36. At the beginning of the first change of slope, hydrogen
yield had tripled when sulfur dioxide was used as a depolarizer. Overcoming these obstacles is
technically feasible which makes anode depolarization a viable avenue to decrease hydrogen
production costs.
DC
Anode Depolarization
DC
Anode Depolarization
Hydro~n Yield
Hydt:c:>~I_I.Yield
Curr:_n~=nsity
Curr~!!i,J?~nslty
~Or-------------~~~------
- - - - - - - - - - - - - - - - , 500
. /L.
400
200
.I
I
~ 150
.i
e' 100
:;
,-
..
/!:
fli
~/
,.
il'
-_, .'... -
.,
i
. 12!..
50
..
..:r:~.
r.
''
'
/'
oL-~--~~~~-~--L-~~~~-~L-~--~~~~~~o
0
M
1
U
2
U
3
~
4
Potentlal ( volts )
Figure 35 :
30
70~-----------------------------------------------~
60
e~ so
. - i'
.
. A'
.:::;-<-~-
. ----
----_7t---- -----
..
--~
--
,______ --
- --;;..."'---'---------"'---- - ; "--~
----
---
..
''
0 . .~~--~----~----L--~----~--_.----~--~----J
0
s
10
lS
20
2S
Figure 36 :
31
SECTION VI
CONCLUSIONS AND RECOMMENDATIONS
A.
CONCLUSIONS
This effort experimentally studied the effects of pulsed DC and anode depolarization on
the performance of the water electrolysis process for hydrogen generation. The selection of the
these two concepts was based on works published in the fifties, sixties, and seventies. Juda and
Moulton (8] found that using 6 percent by weight sulfurous acid ( sulfur dioxide dissolved in water
) to depolarize the cell anode reduces the cell potential by 0.8 volts below that of nondepolarized
cell potential. Bockris et al [14, 15, and 22] and Tseung and Vassie [23] concluded that pulsed
DC may be used to improve the electrolysis process for hydrogen generation for up to twice the
performance of the nonpulsed DC electrolysis.
The work accomplished during this effort showed the potential of the anode depolarization
method in reducing the cost of electrolysis for hydrogen production. A three-to-one improvement
in electrolysis performance is feasible.
In the case of pulsed DC, one of the phenomena recorded by Bockris in 1953 was not
duplicated by this effort, namely the high but short-lived current spike. The second phenomenon,
significant current continue to flow for a short time, was observed. Bockris explained the cause
of this phenomenon as the discharge of the ions in the double-layer facing the electrode in the
absence of the externally applied electric field. However, the current flow during the off-period
of the pulse is largely due to the discharge of the current generated by the collapse of the
magnetic flux around the leads connecting the cell to the power amplifier. Since the results of
this effort contradict those of Backris et al (14, 15 and 22] and Tseung and Vassie [23] more
effort is needed to settle the pulsed DC issue.
B.
RECOMMENDATIONS
Due to the lack in 6.1 funds this effort was terminated before its conclusion. To achieve
the objectives, a basic research program, which consists of an aggressive experimental and
theoretical investigation of the water electrolysis behavior under pulsed DC and anode
depolarization loadings, is proposed. A new cell design is also proposed. The new design is
based on a dispersion of ultramicroelectrodes to maximize surface area per unit volume under
high mass transport conditions.
The overall philosophy is to explicitly account for the
characteristics of the double-layer and the nature of the oxidation process in describing the
electrolytic process behavior under varied loading conditions. Observations of charging,
discharging, and the thickness of the double-layer and electrode oxidation process are proposed,
backed up by theoretical modeling. The following describes the proposed research.
C.
The long-term objective of this research is the development of an efficient electrolytic cell
using pulsed DC power and anode depolarization concepts. Because few, if any, researchers
have ever studied the electrolyzer behavior using the dispersive ultramicroelectrodes under pulsed
32
D.
1.
2.
Study the anodic oxidation process under both nonpulsed and pulsed DC.
Task 1.
Laboratory Experiment
charging times, so that transient measurements are simplified (the time constants are proportional
to the radius of the electrodes). This system will be used for all the depolarization processes
discussed above. The use of ultramicroelectrodes is a powerful new methodology for hydrogen
production. The number of particles that can be put into the suspension may be as large as 109
Ultramicroelectrodes per cubic centimeter of solution. This will increase the contact time with the
depolarizer materials such as S0 2 or biomass, which in tum translate to large hydrogen
generation. The space time yield (amount of product produced per time of electrolysis and per
cell volume) is expected to be 1-2 order of magnitude greater than 2-D systems.
Different electrode material, metallic powders, such as pt, Ru, Pb, PbO,
metal supported materials as well as carbon, graphite and semiconductors will be used and their
performance from a catalytic point of view will be studied. The preparation of ultramicroelectrode
dispersion will be undertaken by various methods, depending on the conducting substrates and
their physical form. Metal powders, carbon, and some supported metal powders are available
from a variety of commercial sources. Other materials will be prepared in-house by grinding and
crushing techniques followed by appropriate sieving and cleaning methods. Reactions will be
studied as function of microelectrode size and concentration (due to difference in mass transfer
rates as size is changed and thus possibility of changing reaction pathway, also microelectrode
concentration will affect reaction pathways by changing the intermediate concentration of chemical
product(s)).
Among the oxides that will be studied are oxides of lead, tin, and cobalt. Chemical reduction of
the oxides at medium temperature (e.g. by carbon monoxide) will also be considered. Following
established favorable equilibrium behavior, the kinetics of the anodic process are of great
importance. After a favorable kinetic behavior is demonstrated, the investigation will tum to other
features relevant to the chosen process. These include oxide coherence (minimize degradation
of substrate weight ratio), oxide layer conductivity, and thermal reduction parameters.
(b)
Sulfur dioxide as an anode depolarizer will also be considered
Although this has been well documented, the process will be examined from the point of view of
a new cell design (dispersion of ultramicroelectrodes) and the use of pulsed DC power as
discussed below.
(c)
34
Task 2.
Theoretical Modeling
35
36
REFERENCES
[1]
[10]
[11]
[12]
[13]
[14]
[15]
[16]
[17]
[18]
[19]
[20]
[21]
[22]
[23]
[24]
[25]
[26]
[27]
[28]
[29]
[30]
[31]
[32]
[33]
[34]
[35]
[36]
[37]
[38]
[39]
[40]
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November 1970.
Bockris, J. O'M. and Kita, Hideaki, " The Dependence of Charge Transfer and Surface
Diffusion Rates on the Structure and Stability of an Electrode Surface: Copper," Journal
of the Electrochemical Society, pp 928-g39, October 1962.
Wagner,O.C., and Williams, D.O., Abstract 49, p120, The Electrochemical Society
Extended Abstract, Fall Meeting, New York, New York, Oct. 13-17, 1974.
Bedrossian, AA, and Cheh, H.Y., Abstract 58, p. 136, The Electrochemical Society
Extended Abstract, Fall Meeting, Las Vegas, Nevada, Oct. 17-22, 1976.
Savage, D. and Thornton, J.D., Symposium On Electrochemical Engineering, (Edited by
:J.D . Thornton), Vol. 2, pp. 2.13, 1973.
Appleby, A.J., and Pichon 8., J. Electroanal. Chern, Vol. 95, pp. 59, 1979.
Popov, K.l., Keca,D.N., Vidojkovic, S.l., Lazarevic, B.J., and Milojkovic, V.B., J. Appl.
Electrochem, Vol. 6, pp. 365, 1976.
Fleischmann, M., Ghoroghchian, J , and Pons, S.; J. Phys. Chern. Vol 89, pp 5530, 1985
Fleischman, M., Ghoroghchian, J., Rolison, D. and Pons, S.; J.Phys.Chem. Vol 90, pp
6392, 1986.
Rolison, D., Nowak, R., Pon, S., Ghoroghchian, J., and Fleischmann, M.; pp401, Molecular
Electronic Devices. Carter F. ed., Elsevier, 1988.
Ghoroghchian, J.:., Pons, S. and Fleischmann, M.; J. Electroannal. Chern. Vol. 317, pp 101,
1991.
38
BIBLIOGRAPHY
Engstrom, S.,"Producing Hydrogen Gas Directly from Water," TEKNISK TIDSKRIFT, 1973.
8.
Evangelista, J., Phillips, B., and Gordon, L., "Electrolytic Hydrogen Production," NASA
Technical Memorandum, NASA TM X-71856, 1975.
9.
10.
Gregory, D.P., and Pangborn, J.B., Hydrogen Energy, Institute of Gas Technology, 1976.
11.
Goltsova, L.F., Garkusheva, V.A., Alimova, R.F., and Goltsov, V.A., "Scientometric Studies
of the Problem of "Hydrogen Energy and Technology" on the World," International Joumal
Hydrogen Energy, Vol. 15, No. 9, 1990.
12
Hammerli, M., "When will Electrolytic Hydrogen Become Competitive", International Joumal
Hydrogen Energy, Vol. 9, No. 1/2, 1984.
13.
Knoche, KF, Hasberq, W., and Roth, M., "Possibilities of Improving the Efficiency of
Power Generation with Regard to Electrolytic Water Splitting," International Joumal Hydrogen
Energy, Vol. 9, No. 8, 1984.
39
14,
Lewis, FA, Johnston, R.C., Witherspoon, M.C., and Obermann, A., "Palladium and
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15.
McMillien, OF, and Golden, D.M., "Hydrocarbon Bond Dissociation Energies," Annual
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16.
Scott, D.S., and Hafele, W., ''The Coming Hydrogen Age: Preventing World Climatic
Disruption," International Journal Hydrogen Enemy. Vol. 15, No. 10, 1990.
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Stuart, A.K., A Perspective on Electrolysis, Proceedings Publication for 1st Annual meeting
of the National Hydrogen Association, 1990.
18.
Veziroglu, T. N., Fueki, K., and Ohta, T., "Hydrogen Energy Progress," Proceedings of the
3rd World Hydrogen Energy Conference, 1980.
19.
White, R.E., Bcokris, J., and Conway, B. E., Modem Aspects of Electrochemistry, Plenum
Press, New York, 1983..
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~-------------------
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APPENDIX A
0.0000
0.0862
0.1725
0.2587
0.3018
0.4743
0.7330
1 . 4661
3.2340
4.2688
5.9505
6.51854
9.516851
51 .. 51606
Source V
0.00000
0.30387
1.98101
2. 71147
3.73411
0.0000
0.21!52
0.5595
0.518519
1.3772
4.514960
7 .33516&
2.3671
4.8204
7.75457
7.31045
7.512998
7.251291
7.898517
5.51J51
6.1QI'16
7.30460
7. 8SSI7!5
10.21$13
7 .. 17604
10. 4'781
10.8661
10.99!15
114.0000
4.04383
1.03433
0.00000
0.00000
CUrrant
0,.00000
0.12837
4.33552
7.22392
7.223512
7.465100
7.16557
0.0000
L1343
3.29SJ8
7.5277
11 .. 5494
22.3769
28,9765
59 .. 1905
80.3300
101 '9660
128,.8~92
155.2978
196,5455
199.4328
200.7734
203.6607
205.5165a
206.8574
210.9822
231.3998
232.9466
216.2542
30L0054
Source V
o.ooooo
J,.JB52B
5.93567
5.93846
5.82702
6.25590
6.32452
6.B33U
7 ,0621SIJ
7.18227
7.26233
7. 34239
7 .. 40529
2,65332
2.3155114
2.46462
2 .. 25304
2.29878
2.29307
1.6468!ll
o. 71480
0.245851
0<12005a
Coll
o.oooo
4.13913
0.0434
0.34'76
o. 6082
1.5206
2.,606'7
4.5183
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7.51'751
10.32513
10.1167
7.10722
51.'7318
9,8621
10.2531
8.4356
11.2332
114.0000
3.115517
o.ooooo
o.ooooo
0.0000
1.0333
2.1700
13.1232
26.1431.
43.70!l6
54.5595
69.0261
85.3526
105.502!5
141.0488
174.5285
196.050
197.8817
ua.nso
209.0416
221.3382
231.15.f7
296,6675
320.0000
2000,0000
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0.00000
o.ooooo
0-21761
2.920!4
.sun
5.90.f08
6.33357
6.61417
6. 75161
6.~0623
6.92341
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7.03194
6.99185
6.90623
... 02577
1.47173
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0 .. 05727
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o.ooooo
1.927.54
7.44565
7 -38'731
7 .. 06054
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.....
7.42512
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51.1235
10.426!ll
11,03!51
11- !ISJ9!a
12.9033
U,3804
16.20.51
19.4201J
20.29!liO
22.BSJ!I7
25.3287
27.9!ll20
31.4110
34.8432
37.5368
42.5765
47.4858
51.00U
56 .. 2618
50.9981
65.2116
70 .. 2078
74.8130
79,9830
85.5440
114.0000
6.22029
6.28116
6.22608
6.73333
6.20870
6.64058
6.26661
6.551110
6.44348
6.29275
5.96812
4.04051
2.428!ll!ll
2.373U
2.31014
2.26377
2.2289!ll
2-19420
2.17391
2.15362
2.12464
2.0D855
2-09406
2.06097
2-04928
2.04639
2.04638
2.03188
2 .. 014U
1.95t130
1,SJ8261
1. 973il
1 .. 96522
1.95942
1.95U4
1.94203
1.92754
Coll
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1.1385
2 .. 690i
4" 5538
6.1063
8 .. 3832
10.1426
12.8335
15.420g
18 .. 3188
21,6306
25 .. 4600
30.4278
36.2236
40.9844
.cs. 9522
52.9899
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61.9969
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2.10000
2.255151
2 .. .f21B8
2.60293
2. 75813
2.96505
3.16335
3.3673!ll
3 .. 56857
3.77836
3.95367
4.14909
4.37038
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4.80147
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5.10898
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.5 .. 45672
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s. 67.513
88.7994
,5,83320
81.3477
47
L___ _ _ _ _ _ _ _ _ _ _ _ _ - - - - - - - """
5.77860
339.1.596
2000,0000
93 "76'73
100.7015
107 .. 5322
113.7420
118.9157
123.7811
130.3013
0,00000
0 .. 00000
137.1320
152.8634
161.4535
173.0451
180,8073
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194.2617
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199'.022!5
200,4115
201"51204
204 .. 1973
206.6812
211.8560
215.4784
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222.8266
226.2419
226.24UI
228.9328
234.93.56
251.287i
260.SI131
276.U74
29.5.6871
325.0805
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2000.0000
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24.2986
29.6525
47.3616
66"9241
85.04SO
97 .. 9151
99,0476
100.3861
102,1364
105.8430
107.7992
110.1673
113.8739
117,5804
123.9610
129,0090
132.7156
137 .. 3488
143 .. 1145
152,7928
162.4710
188.5199
213.024:1
245 .. 353!il
273.6680
317 .. 0142
1000.0000
Source V
0.00000
0.04644
0.22061
2.41509
4.83019
6.56604
5 .. 60668
6.50798
6,75181
7.03628
7,05370
1.40203
7,.70!il12
7.,87808
7. 88970
5.3S268
2.945120
2.18868
1.85U6
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1. 77068
1 .. 68360
1 .. 60813
1.48621
1.39332
0.59797
0,5166!il
0 .. 41800
0.31350
0 .. 24383
0 .. 19158
0.14514
0.10450
0.00000
0.00000
0.0000
2.9891
4 .5361
5.3608
15 .. 7010
!ii.0722
10.4124
12.5773
15.1S4S
18.2414
22.6804
28.2474
32.160
36.5979
to. 7216
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54.1237
61.2371
61' 9381
73.1959
79.58715
86 .. 1856
!it .. 2371
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100.0000
102.7835
104.3299:
106.59751
108.3505
110 .. 4124
112.3711
114.6392
117 .. 0103
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124 .. 1237
127.9381
131,.6-495
133.6082
137 .. 4227
141.9588
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0.00000
0.00000
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0.48766
0 .. 96952
1.50363
1. 95S46
2.42671
3.01308
3.S4136
4.27866
4.95210
5.49202
5 .. 86938
6.20610
6 .. 54282
6. 76343
6.89115
6.96662
7 .. 04790
7.08273
7.11176
7 .. 18723
7.18723
7 .. 16401
15.86081
6.4!il057
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2 .. 31060
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0,01161
0 .. 00000
0.00000
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5.962.52
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6.04299
6 .. 07461
6.09185
6.12059
6.15220
6.18381
6.22692
6.22692
6.25854
6.26428
6.26716
5.86481
5 .. 51994
.5.26704
4. 97103
4 .. 654510
4.34452
3. 72376
3.415112
3.10587
2 .. 85584
2.63742
2.63167
2.4U12
2 .. 43625
2.41901
2.39314
2.37871
2.37302
2.352511
2.29543
2.10000
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0. 0000
0,4132
2.7S!il3
4.8554
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6,7U9
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11.1570
13.7397
15,7025
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20.1446
22.3140
25.5165
28.5124
31.6116
35.0207
38,7397
42.871!il
47.9339
52.2727
57,.3347
61.1769
65.599'2
69,8050
71.15942
75.1033
77.6860
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85.9504
90.2893
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517.5207
98.,5537
100.92!il1
101,.9629
103.6157
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105.5795
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6.44820
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15.46843
6.35865
6.10731
5.76641
5.67107
5.489015
5.29261
108.7810
5.00327
110 .. 2273
4.87082
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2.19274
2.19274
2.20718
2.27363
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3.31077
3.52167
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3.98102
4 .2236!il
4.40858
4.55881
4.72926
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113.6364
115.7025
117.11752
120.6612
122.5207
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130.0620
132.5413
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34.9989
37.111361
40.8134
43.8934
46.3342
53.7907
64.1646
81.4158
111.2020
142.9740
167.5063
190.0000
200 .. 0000
49
2.30000
2.57930
2. 512710
3o23292
3 .. 44599
3. 78576
4 .. 07092
4 .. 35300
4.5S743
4. 758~9
5.00374
5.1~11153
5 .. 357~0
5 .. 46732
5 .. 18226
4.91370
4.6171110
4.32420
4.07370
3.17136
3.50934
3.24156
3 .. 00545
2.75206
2.,52747
2 .. 41230
2 .. 37174
2.37774
2.36911
2.3481115
2 .. 32016
2.33161
2.30576
2.30000
Nov~
.imo
o.oooo
0,2694
0.3304
0.5575
1.0943
1. 75!50
2.4157
2.93U
3.4607
4.02152
5 .. 38851
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8.2175
9,9931
10.1376
10.2822
10.91510
11,4178
11.9546
12.28U
12 .. 7392
13.2347
13,3999'
14,2051
u. 7213
15.7330
17.,2915
17.9628
19 .. 7385
20.3164
22.2161
23.103~
23 .. 3310
24.1982
24. 9209'
26.5520
27 .. 9'972
29'.0502
29.6490
3t.1n5
32.7254
32.9319
33.1590
33.,3655
33.5719'
33.9642
34.1707
34.3152
34 .. 7075
34 9346
35 .. 1411.
35.2650
35 .. 5127
36.3386
36.8135
38.0936
40.5506
44.8658
45.7123
46.0427
46.6621
47.0544
47.5912
48.2312
48.9332
49.3462
89.5960
100.0000
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0,00000
0.02900
0.13340
1.333~9
3.02214
6.3na;
8.579015
9.45964
10.12663
10.43403
10.43403
10,38183
10.35863
10.35283
10.32383
10.23103
8.31126
5.608.51
3.68874
3.04495
t .. 942n
1.328111
1.25278
0.9'7438
1.05558
1.37458
1.36878
1.,24698
1.26438
1.33398
1v32238
1.25278
1 .. 18318
1.17738
1.53697
1.44418
1.37458
1.23538
1.09038
1.13098
1 .. 14258
0 .. 4059'9'
0.829'3~
0,49719'
0.67859
0.,07540
0.7249~
0.31319
0 .. 37699
0 .. 22620
0 .. 35959
0 .. 21460
0.26680
0.15660
0.22620
0 .. 26680
0.25520
0.20300
0.16240
0.02320
0.13340
0,01160
0.06960
0.00000
0.05220
0.02320
0.00000
0.00000
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1.B36i7
2.414G
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5.489tS
8.1312
10.2715
11.2474
11.!5983
11.94511
12.2380
12.6~20
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14.6732
15.0860
115.1385
20.348.5
22.9488
2.5.15'83
25.9000
26.4572
26.8700
27.3240
28.~~56
29.7386
30.2959
30.8737
32.0500
33.0612
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100.0000
0.00000
0.00000
0.081587
0.11954
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2.05019
3 .50~65
4.54054
4.9.57.53
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4.516911
5.00386
4.515174
4.514595
4.30888
4.29730
3.94556
2.49614
1.88224
1.33205
1.14672
1.14093
0.9'9'614
0.99456
0.153127
0" 5849'4
0.34749
0 .. 31274
0,18533
0.,04633
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0.,00000
Call
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0.0000
0.8073
1.6352
2.3597
2.6909
3.1877
3. 6224
4.1398
4.2019
4 .. 3882
4.7401
5.1334
5.5267
5. 6923
5.9200
6.2305
6.6237
6.97.56
7.1826
7.5138
7.9071
9.5281
8.8179
9.376'7
2.30218
2.30218
2.30791
2.29G44
2.35092
2.47706
2.594151
2. 75516
2.746!56
2.83830
2.~2144
3. 0504fi
3.19094
3.18234
3.3256i
3.34576
3.47477
3.56651
3.155926
3.71846
3. 75860
3.90195
3.98508
4.12844
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4.202~8
10 .. 2461
10.5566
11.0534
4 .. 30~06
4.35780
4.46101
4.5UBi
4 .. 6&143
4. 71~04
4.73624
4.65023
4.65023
4. SGSISIS
4.51835
4.44667
4.35206
4.2689'2
4.17431
4,10937
4.01376
3.9:3349
3.96181
3.75573
3.69553
3.59805
3.51U1
3.43463
3.36009
3,29268
3 .. 21674
3 .. 18234
3.13073
3.04186
2.98452
2.89'278
2.91823
2.17523
2.67175
2.61468
2.55161
2.49'713
2.44839
2.40539
2.36238
2.350U
2 .. 39245
2.36812
2.39'679
2,36812
2.3824.5
2.359'52
2.36525
2.36239
2.327i8
2.32225
2 .. 32511
2.32511
2.31651
2,32225
11.425~
11.~227
12,0676
12.8956
13,5373
13 .. 7443
13.9305
14.4066
14.6757
15 .. 069'0
15.7521
16.1247
16.6421
17.4908
17.9048
19,5051
19.4365
19.8919'
20.9441
21.4029
21. ~204
22.1688
22.8312
23.3487
23 .. 7213
24.4664
25.2323
25.7705
26.7225
27.3229
27.9025
29.730.5
29'. 7240
30.5313
31 .. 1109
32 .. 0009'
32.8496
33,5534
33. 9'673
34 .. 1950
34.6504
3.5.4163
36.1201
39.2107
42.0814
45.9'250
51 .. 1270
54" 9770
59.3031
63.5979
67" 9726
73.0681
76.2351
50
79,46fo1
82.8174
86.3983
510.0621
91.862i
93.7466
100.0000
25 kBs, 101 Duty cyel
Nov~ 13, U91 ( ~ ia. lllicro-a.condlt
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0,0718
0.1144
0.2462
0.5848
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1.7543
2.3904
2.8520
3.2316
3.6112
4.0010
4.1139
4-2780
4.4832
4.,8320
5.1500
5.7040
6,5453
7.0172
7.3865
7.6019
7.7866
8 .14!57
8 .5560
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9 .. 07513
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51,7358
10.5360
12.1467
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13.34.70
13.4906
13.6753
13.8081
13.,9215
14.1370
14.3421
14.5576
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15.00510
15.4604
17 .. 0095
17.1121
18.9392
20.t668
20.5694
20.6412
20 .. 1438
20.87'71
20.51284
21.0310
21 .. 1234
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21.tl06
21.5850
21.7081
21.8825
22.0467
22 .. 2006
22.3032
22.4878
22.55104
22.7853
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0.04636
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0,28D74
2.25993
4.68191
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8.85430
11.46172
12.59768
13.21192
13.72185
13 .. 81831
13.87252
13,70447
13.04387
11.13742
8.651U
5.42964
2. 70613
1 .. 51821
0.5103517
0.86341
0.74172
0,67219
0"62.583
0.70695
0.70U5
0.89818
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1.1589'4
1.17053
1.39652
1.305160
1.251222
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1.4U70
1.30381
1.U503
1. 42550
1.485124
1.41391
1.44868
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1.35017
1.27483
1.12417
0 .. 00000
0.69536
0.651536
0.00000
1,08361
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0.135107
0 .. 84023
0 .. 011551
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0.02897
0.30132
0.11010
0.21440
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1.2511
1,3505
1. 6185
1,8241
1.8794
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2.4124
2.6082
2.8241
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3.2414
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3.6U5
3,89651
4.0309
4.2680
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4.6907
4.8144
5.1134
5.3093
5.463!i
5.5173
5.7732
5.89'69
6.1649
6.t6351
6.6598
6.8454
7.1237
7.1856
1.4021
7. 5610
7.9381
8.1649
8.4.536
8.628t
9.0412
51.4142
51,.9897
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10.6392
10.8557
11.2680
11.6289
11.8454
12.2062
12.4227
12. '7216
12.51794
13.05128
13.2577
13.46351
13.7320
13.9175
14.3711
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15.1546
15.7216
16,1856
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16.8454
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11.31516
17.5670
18,0206
19,2680
18.5561
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0.0421J2
0.04292
0.10300
0.10300
0.18312
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0.55222
0.68814
0.87268
1.0410
1.21602
1.38U7
1.54793
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1.81688
2.01717
2.13734
2,30043
2.t0628
2.58655
2.70672
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2. 91845
2.98712
3 .. 07868
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3.144451
3.18455
3.181651
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3.14163
3.07.582
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2.516137
2, 885184
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2.651242
2.52641
2.42060
2.33190
2.22604
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2.04578
1.9U89
1.99700
1.82260
1. 73104
1. 70815
1.61373
1.567515
1.527510
1.513551
1.4105t
1.351342
1.251041
1.18455
1,092t9
0.98712
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0.82403
0. 73247
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0.63233
0.5B36!iJ
0,54650
0.47210
0.40343
0.37196
2.33085
2.33085
2.29644
2.32511
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0.5805
1.0158
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1.6792
1.8658
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3.3895
3. 7834
4.1047
4.4467
4.8199
5.0790
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5.7735
6.1363
6.4368
6. 8412
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7.5460
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8.2197
8.8209
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51.6916
10.3032
10.6038
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11.82651
12.2415
12.5110
12.9360
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15,0091
15.3511
15.'7554
16.1804
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17.1340
17.5496
17.7041
17.9217
18.2639
18.8235
19.1760
151.7171
20.2741
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21.3527
21.44.60
21.6325
21.9746
22.4514
23.3221
24.2446
25.2397
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28.35108
29.0956
251.8005
30.8992
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2.33218
2.32350
2.32928
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2.44213
2.58681
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3.22627
3.41635
3.5U61
3.68345
3.81076
3.91204
3.116101
3.97280
3.97568
3.80600
3.842551
3.80208
3. 73553
3,65162
3.58507
3,51852
3.43461
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3,30ttO
3.23206
3,19155
3.14815
3.11343
3,07002
3.04688
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2.951063
2.84144
2. 79646
2.75174
2. 71123
2. 67072
2.63310
2.60417
2.56076
2.56076
2.51736
2.451421
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2.42188
2.39005
2.35532
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2.332111
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0.18312
0.163051
0.12303
0.06861
0.02575
0.02289
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99.7106
110.7947
128.5714
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163.9182
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222.9296
264.1709
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341.2724
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358.3248
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470,6844
496.4249
500.5107
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552.4004
576.5067
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2.00966
3.01299
3.32756
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3.50072
3.54690
3.59985
3. 64502
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3.6U97
3.70851
3.72006
3.72294
3.70851
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1.30880
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1.45166
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1.53924
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1.48485
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8.1716
11.8481
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17.1J775
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35.9551
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52.2983
551.2441
69.8672
82.5332
95.6078
110.7252
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210.4198
290.5005
351.3790
411.8481
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503.7794
510.3167
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518.3673
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0.23081
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0.62572
0.79191
0.91698
1.11561
1.24566
1.34971
1.40607
1.4C942
1.50000
1.53324
1.55347
1.56069
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1.54046
1.52168
1.49855
1. 451855
1.10694
0 .. 71243
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------
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39.7554
57.0846
70.3364
84.6075
102.9562
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188.5831
209.9898
293.5780
503.5678
704.3833
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3.10370
3.17041
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3.16171
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23.5390
35.3084
451.5130
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113.6364
136.7695
162.3317
189.5292
226.8669
257.7110
306.0065
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372.1591
408.6851
437.9059
465.5032
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3.07686
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5154,9513
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November 13, 1991, ( t:J...mra in miero-aeconda
......
0.0000
0.5111
1.1073
1.192.!5
1.5332
1.7898
2.4702
2.9813
3.7418
4.0034
4.5145
1 '7513
8.6031
10.0511
11.4140
13.6296
17,3765
18.4838
22.6576
23 .. 76411
32.5383
33.7308
31f.1823
41.2261!1
47 '7002
52.2146
67 .. 1210
69-33.56
99.5741
100.6814
101.3621f
102.555-t
103 .. 3220
104.6848
106.1329
107.3254
109 .. 2945
110.2215
110.8171
112.6917
114.5656
115 .. 4174
116.6951
118.6542
120 . .5291
121.2947
123.5094
126.,0647
127 .. 6831
128 .. 9608
131.34.58
132.1976
133.8160
136.6261f
139.6082
200.0000
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0.67825
1.1049!5
1.50749
1.98922
2 .. 60755
3.07969
3.42960
3.50150
3.52796
3.53026
3.56141
3.53505
3.52786
3.6069.!5
3.6069!5
3.64769
3,64530
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3. 69083
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3,73977
3. 71711
3.77711
3.90927
3.91067
3.84182
3,86818
3.46794
2,5811"
1.72798
1.32774
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1.207il
1,26303
1.26303
1.20312
0 .. 18214
0 .. 17735
0.1150-t
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0.08.388
0.03116
0,10785
0.07909
0.12463
0.14859
0.071il09
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0.07430
0.07430
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0.0000
5.1783
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8.,5934
11.1508
12.6854
15,1407
18 .5166
21.99U
25.8824
28.644.5
33.2481
37.2379
42.2506
47.1611
51.9693
57.5951J
63-5294
68.74158
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82.9644
88.2964
91.6624
94 .5269
98.5166
102.3018
104,5524
105,0638
106,0870
106. SIOS4
107.7238
109.2583
110.4858
111.7136
112 .. 2251
114 .. 2857
200 .. 0000
0.0000
0.1652
0 .. 3304
0.51fi3
0.681.5
0.9106
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0.15196
0.33898
0.451411
0.5751:i9
0,66774
0.84015
0,96727
1.08416
1.10352
1,28434
1.37341
1.46251f
1.54734
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1.64962
1.68117
1.72f14
1.76651
1.79866
1.91327
1.83372
1,94249
1,85272
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1. 70076
1.55026
1,32379
1.14553
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0.52162
0.27469
0.05114
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8.2770
9.961:i2
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14.1892
16.8074
20 .. 1014
23.7331
26.4359
31.0911
35.8953
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98.3108
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102.21104
103.2938
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105.9966
107.1791
108,8682
110.3041
111.4865
112.6689
115.4561
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124 .. 8311
126,3513
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138.17.57
142.9899
152.2804
155.,9966
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165 .. 2027
174.15.!54
179.1395
183.6SI93
191.0473
200.0000
2.20000
2.22943
2.27748
2. 40240
2,47688
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2.58739
2,61387
2.72192
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2.83243
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3.01261
3,06306
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3.10631
3.09670
3.11832
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3,20721
3.21201
3.22643
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3.07027
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2.39039
2.27148
2.28949
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2.27267
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2.26787
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2.25826
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2.22222
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Duty cycl
cw:rent
2.2C5355
2.23090
2.111528
2.1804-t
2.14482
2.11:i5!511
2.11:i263
2.151166
2.1418!5
2.14185
2.13909
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0"32107
0, 74431
1.11208
1 .54991
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2.743.5
6.0440
8.9319
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0.323.51
0 . .53871
0.73368
0.80878
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0.7897
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3.0341
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2.28242
2.31412
2.37464
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2.3543
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3.5108
3.6SJ66
3.9032
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5.9683
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10.6356
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14.5801
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24.5961
26.4341
28.4167
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35.8100
37.9784
39.7132
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43,1827
45.3304
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48.9032
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49.9'771
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50,36~4
50 .. 5140
50.63751
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51.0303
51.05051
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51.1955
51.2701
51.3401
51 .. 4433
51.5879
51 .. 6292
51.7118
51 .. 7738
52 .. 0216
52' 1561
52.2487
52. 2900
52.4966
52 .. 6824
52.9715
53.1987
53.3846
53.5498
53.'71.50
54.,0454
54.2313
54.7269
54 .. 9541
55 .. 2226
55.7389
55.9041
56" 1106
56.9573
57.4530
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58.2997
58.6921
58.9605
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60.3442
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2.96848
3.22825
3,42966
3.52306
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3.69235
3.73322
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3.77408
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3, 77100
3, 79451
3. 79743
3.79743
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3.89959
3.510835
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3.99299
4.00759
4.01343
4.00175
4.00175
4.01635
4.03386
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4.05721
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3.90835
3.805111
3.66900
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3.23409
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2.91302
2.77875
2. 65616
2. 55692
2.39930
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2.22125
2.08990
1.92936
1. 84764
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1.54991
1.49737
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1,19089
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1.17630
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1.19381
14.6253
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25.5168
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32.2828
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46.1439
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51.1SJ87
51,63U
52.1476
52.8283
53.5916
54.2104
54.7261
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57.2840
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60.8526
61.8221
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1.63200
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1. 76SJ21
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1.85442
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1.56268
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0.96187
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0,63403
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0.29806
0 .. 14876
0.01878
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8.084.0
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10.9934
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14.7340
16.45951
18.2668
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21.0723
22.9011
24.2934
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28 .. 6793
30.6733
31.9202
33.5827
35.6401
37.2402
38 .. 8820
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44.0150
44.4306
45.2411
46.1139
47.3192
49.5245
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51 .. 1945
52.4522
53.MS2
55,.0083
56,5046
57.7515
59.1022
60.7440
61.7207
62.6351
64.6.508
67.0615
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73.6700
76.8080
80 .. 9435
84..8088
88.6741
92.0615
95.3034
98.2128
99.9377
100.0000
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1.16170
1.15879
1.17338
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2.47262
2.49280
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3.02305
3.04035
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3.07205
3.080651
3.12680
3.141l86
3.1671.!5
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3.19885
3.22190
3.18444
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3.21902
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3.27378
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3.08646
2.94813
2.78386
2.65706
2.55620
2.41787
2.33718
2.30259
2.29683
2.28.530
2.28530
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2.28242
2.27378
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2.29683
2.25072
2.27089
2.270892.27378
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151.1703
61.3g74
61.6246
61.7485
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62.1615
62,.3681
62.7399
62.9670
63.2354
63.4419
63 .. 7517
63.U7S
64.123!1
64.3300
64.6191
65.0734
65.3213
65.7136
66.0028
66.6843
67.4897
68.1092
68.5223
69.2864
69.8027
70.3809
71.1037
71.8412
72 .. 4461
12.9624
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14.1602
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75.1927
76.2460
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77 .. 6503
79.352!5
78.8481
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79.8807
80.2111
80.5828
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81.5948
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96.4273
81.3153
88.1620
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0.26562
0.22767
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0.11384
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1.5694
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2.7569
2.9427
3.1492
3.45510
3.6759
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4.6980
6.4739
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2.06087
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2.2601
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3.1682
3.8803
4.6336
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1.05354
1.16005
1.22913
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4.7589
5.3810
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2.32425
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2.30703
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2.48207
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2.60832
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2. 69727
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0.5752
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1.6025
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2.2599
2.6502
2.9173
3.1229
3.3282
3.5336
3.9007
5.0334
5.0950
5.5265
5.7524
6.1428
6. 6769
7.0262
7.6838
9.1972
Loo4 DV
0.00000
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13 .. 443~
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17 .. 9966
20.0310
20.1342
20-.2272
20.36U
20.4853
20.85183
21.362Sf
21.6107
21.83'7Sii
22.054.7
22.2.508
22.4677
22.7672
23.1492
23.5312
23.8720
24.3263
25.4104
26.4223
27.21'13
28.0124
28.5700
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30.0465
30.3975
30.6SI70
30.7393
30.8725
31.,0274
31.2235
31 .. 3371
31"5333
31.6262
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32.1322
32,3283
32.4522
32.6000
40.0000
4.371J71
4-423151
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4.18841
3.98841
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2.51J130
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1.87825
1.67536
1.52174
1.373SJ1
1.26667
1.16812
1-13913
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