Embed Size (px)
Citation preview
EDGEWOOD CHEMICAL BIOLOGICAL CENTER
U.S. ARMY RESEARCH. DEVELOPMENT AND ENGINEERING COMMAND
ECBC-TR-777
EVAPORATION RATES OF CHEMICAL WARFARE AGENTS USING 5 CM WIND TUNNELS
IV. VX FROM GLASS
Carol A. S. Brevett Christopher V. Giannaras
John J. Pence Joseph P. Myers Robert G. Nickol
SCIENCE APPLICATIONS INTERNATIONAL CORPORATION
Gunpowder, MD 21010-0068
Bruce E. King Kenneth B. Sumpter
Seok H. Hong H. Dupont Durst
RESEARCH AND TECHNOLOGY DIRECTORATE
June 2010
Approved for public release; distribution is unlimited.
20100923366 ABERDEEN PROVING GROUND, MD 21010-5424
Disclaimer
The findings in this report are not to be construed as an official Department of the Army position unless so designated by other authorizing documents.
REPORT DOCUMENTATION PAGE Form Approved
OMB No. 0704-0188 Public reporting burden for this collection of information is estimated to average 1 hour per response, including the time for reviewing instructions, searching existing data sources, gathenng and maintaining the data needed, and completing and reviewing this collection of information Send comments regarding this burden estimate or any other aspect of this collection of information, including suggestions for reducing this burden to Department of Defense. Washington Headquarters Services. Directorate for Information Operations and Reports (0704-0188). 1215 Jefferson Davis Highway, Suite 1204. Arlington. VA 22202-4302 Respondents should be aware that notwithstanding any other provision of law. no person shall be subject to any penalty for failing to comply with a collection of information if it does not display a currently valid OMB control number PLEASE DO NOT RETURN YOUR FORM TO THE ABOVE ADDRESS
1. REPORT DATE (DD-MM-YYYY)
XX-06-2010 2. REPORT TYPE
Final 3. DATES COVERED (From - To)
Aug 2006 - Sep 2009
4. TITLE AND SUBTITLE
Evaporation Rates of Chemical Warfare Agents Using 5 cm Wind Tunnels IV. VX from Glass
5a. CONTRACT NUMBER
DAAD13-03-D-0017 5b. GRANT NUMBER
5c. PROGRAM ELEMENT NUMBER
6. AUTHOR(S)
Brcvctt, Carol A. S.; Giannaras, Christopher V.; Pence. John J.; Myers. Joseph P.; Nickol, Robert G. (SAIC); King, Bruce E.; Sumpter, Kenneth B.; Hong, Seok H.; and Durst. H. Dupont (ECBC)
5d. PROJECT NUMBER
BA07TAS041
5e TASK NUMBER
5f. WORK UNIT NUMBER
7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES)
SAIC. P.O. Box 68, Gunpowder, MD 21010-0068 D1R, ECBC, ATTN: RDCB-DRC-M, APG. MD 21010-5424
8. PERFORMING ORGANIZATION REPORT NUMBER
ECBC-TR-777
9. SPONSORING / MONITORING AGENCY NAME(S) AND ADDRESS(ES)
Defense Threat Reduction Agency, 8725 John J Kingman Road, Fort Belvoir, VA 22060-6201
10. SPONSOR/MONITORS ACRONYM(S)
DTRA
11. SPONSOR/MONITOR'S REPORT NUMBER(S)
12. DISTRIBUTION / AVAILABILITY STATEMENT
Approved for public release; distribution is unlimited.
13. SUPPLEMENTARY NOTES
14. ABSTRACT The evaporation of VX from glass was studied as a function of temperature, drop size, and air How rate, using the same instrumentation as prior studies of sulfur mustard evaporation from glass, concrete, and sand. The evaporation rate increased with higher temperature and drop size; wind speed was not a significant factor. An empirical equation was determined that would allow for the calculation of the evaporation rate given the atmospheric conditions. The data collected provide input for the validation of empirical and physics-based models on the evaporation of agent designed by other authors, and are input for the VLSTRACK model, which predicts agent vapor concentrations as a function of environmental conditions.
15. SUBJECT TERMS
VX Glass Evaporation rate Wind tunnc
16. SECURITY CLASSIFICATION OF:
a. REPORT
u b. ABSTRACT
U c. THIS PAGE
U
17. LIMITATION OF ABSTRACT
UL
18. NUMBER OF PAGES
68
19a. NAME OF RESPONSIBLE PERSON
Sandra J. Johnson 19b. TELEPHONE NUMBER (include area code)
(410)436-2914 Standard Form 298 (Rev. 8-98) Prescribed by ANSI Std. Z39.18
Blank
PREFACE
The work described in this report was authorized under Contract No. DAAD13- 03-D-0017. The work began in August 2006 and was completed in September 2009.
The use of either trade or manufacturers' names in this report does not constitute an official endorsement of any commercial products. This report may not be cited for purposes of advertisement.
This report has been approved for public release. Registered users should request additional copies from the Defense Technical Information Center; unregistered users should direct such requests to the National Technical Information Service.
Acknowledgments
The authors thank Drs. James Savage and Terrence D'Onofrio (U.S. Army Edgewood Chemical Biological Center) for program guidance and Christine Franklin (Science Applications International Corporation) for administrative support. Funding from the Defense Threat Reduction Agency is gratefully acknowledged.
Blank
CONTENTS
1. INTRODUCTION 9
2. EXPERIMENTAL PROCEDURES 9
2.1 Wind Tunnel 9 2.2 Detection ofVX in the Wind Tunnel Effluent 10 2.3 Analysis of Neat Ton Container VX 11 2.4 Experimental Design and Data Analysis 12
3. RESULTS 12
3.1 Time to Plateau 12 3.2 Percentage Recovery 12 3.3 Evaporation Rates 13 3.4 Combined Effects 13
4. DISCUSSION 24
5. CONCLUSIONS 25
LITERATURE CITED 27
APPENDIX: WIND TUNNEL DATA 29
FIGURES
1. Retention Times of Ethyl Methylphosphonofluoridate, 1 min. Internal Standard Bromofiuorobenzene, 2.1 min, and Hydroxymandelic Acid, Ethyl Ether, 3.4 min 11
2. Mass Spectrum of the 1.1 min Ethyl Methylphosphonofluoridate Peak 11
3. Vapor Concentrations for 1 uL Droplets of VX Evaporating from Glass at 35 °C. 18 SLPM, and 50 °C, 405 SLPM 14
4. Average Time to Reach a Plateau in the Evaporation Rate of VX from Glass 14
5. Actual vs. Predicted Plots for the Time Taken to Reach a Plateau for the Evaporation of VX from Glass 15
6. Scatterplot of Temperature, Drop Mass, Air Flow, %Recovery, and Raw Evaporation Rate 18
7. Cube Plot of %VX Recovered for Evaporation from Glass 18
8. Least Squares Regression Analysis of %VX Recovered Data as a Function of Temperature, Air Flow, Drop Size, Tunnel Identity, and Time to Plateau 19
9. Calculation of the Evaporation Rate for a 6 uL Droplet of VX Evaporating from Glass at 35 °C and 181 SLPM 19
10. Cumulative VX Vapor Recovered for 1 uL Droplets of VX Evaporating from Glass at 35 °C, 18 SLPM, and 50 °C, 405 SLPM 20
11. Cube Plot of the Raw Evaporation Rates for VX Evaporating from Glass 20
12. Actual vs. Predicted Plots for the Raw Evaporation Rates for VX on Glass 21
13. Relative Contributions of Degradation and Evaporation for the Loss ofVX from Glass 22
TABLES
Parameter Estimates for Major Effects for the Time to Plateau during the Evaporation of VX from Glass 15
Conditions and Experimental Evaporation Rates for the Evaporation of VX from Glass 16
Parameter Estimates for the Major Effects Contributing to the Raw Evaporation Rate for the Evaporation of VX from Glass 21
Comparison of Predicted and Measured Raw Evaporation Rates for the Evaporation of VX from Glass 23
SCHEMES
V-to-G Conversion on Silver Fluoride Pads 10
Degradation Pathways for VX 25
Blank
EVAPORATION RATES OF CHEMICAL WARFARE AGENTS USING 5 CM WIND TUNNELS
IV. VX FROM GLASS
1. INTRODUCTION
The evaporation rates of the chemical warfare agent sulfur mustard from glass, concrete, and sand as a function of temperature, drop size, and air flow rate have been previously reported.1 "J Select evaporation and degradation rates of ton container VX on sand and glass have also been reported in the literature.4 In this work, additional evaporation data for VX on the same glass, as used previously, as a function of temperature, drop size, and air flow rate measured in 5 cm wind tunnels are presented. This report describes the data analysis and demonstrates the robustness of the set of data that will be passed to the modelers for eventual incorporation into field models such as VLSTRACK, which predicts vapor concentration as a function of environmental conditions.
2. EXPERIMENTAL PROCEDURES
2.1 Wind Tunnel
The 5 cm wind tunnels that were used in the present investigations have been previously described and were the same as those used for similar earlier studies on glass/ The design of the 5 cm laboratory-sized wind tunnels6 and the wind tunnel characteristics compared to other wind tunnels and outdoors measurements have been published. In order to expose the agent to the wind flow, the piston was removed and the test substrate (a 1.5 in. diameter circle) with the droplet of agent on it was placed onto the piston and inserted into the wind tunnel. The humidified, temperature-controlled air from a Miller-Nelson Environmental Control Unit (ECU) (tunnel a) or an Aalborg MFC (tunnels c, d, k, 1) was then passed over the sample and the vapors were collected on Markes TenaxR thermal desorption tubes (Agilent Technologies, Santa Clara. CA) at the vapor sampling inlet. The amount of agent on each tube was measured based upon a standard in the Gas chromatography/Mass Spectrometry (GC/MS). The sample volume and tunnel air flow rate were known; thus, the agent concentration (mg/nr) and evaporation rate (ug/min) could be calculated. The rates were not calculated for the initial 5 min of the experiment (before the instrumentation reached equilibrium) nor at the end of the experiment (when concentration of mustard was nearing a plateau due to sample exhaustion). Hence, the data in the middle of each experimental run were used to calculate the evaporation rates.
Air flows were 18, 181, and 405 standard liters per minute (SLPM), which corresponded to velocity values at a I cm height of 0.22, 1.7, and 3.6 m/s. The flow volume per thermal desorption tube was typically 2 to 10 L volume, and the tubes were automatically switched using a proprietary Versatile Tube Sampler. The rate at which the tubes were switched was adjusted based upon the evaporation rate of the agent. The air and substrate temperatures investigated in this work were 35, 42, and 50 °C, and the droplet sizes were 1, 6, and 9 uL, corresponding to droplet diameters of 1.24, 2.25, and 2.58 mm and contamination densities of
approximately 1.3, 7, and 11 g/m". The droplets masses used in the calculations and tables were based upon the pipette setting; the samples were not weighed.
In general, the evaporation of the VX was measured until no further decrease in the concentration of vapor was detected at which time the experiment was terminated. Summation of the concentrations over time yielded the cumulative amount of VX that had evaporated. The data collected are shown in the Appendix.
2.2 Detection of VX in the Wind Tunnel Effluent
For the analysis of VX, a silver fluoride pad (CAMSCO, Houston, TX) was inserted onto the end of Tenax TA thermal desorption tubes (Markes International, Llantrisant, UK) to convert any VX in the stream to its G-analog, ethyl methylphosphonofluoridate (EMPF, EA-1207) which is more volatile and therefore easier to analyze by thermal desorption GC. The chemical equation for the reaction is shown in Scheme 1.
O C3H7 O C3H7
H3C—P—S—CH2CH2N + AgF • H3C—P—F + AgSCH2CH2N
OC2H5 C3H7 OC2H5 C3H7
Scheme 1. V-to-G Conversion on Silver Fluoride Pads.
The ethyl methylphosphonofluoridate was desorbcd from the thermal desorption tubes using a Markes UNITY/ULTRA Desorption system (Markes International, Llantrisant, UK), and analyzed on an Agilent 6890/5973 Gas Chromatography/Mass Spectrometry Detector (GC/MSD [Agilent Technologies, Santa Clara, CA]) using a HP-5MS capillary column (30 m long, 0.25 mm id, 0.25 um film thickness, (5%-phenyl)-methylpolysiloxane stationary phase).4
Oven parameters were 60 (1.5 min) to 250 °C at 50 °C/min. Thermal desorber parameters were a tube desorption temperature of 250 °C for 2.5 min and a 10 mL/min split flow. The tube purge/sweep flow was 50 mL/min, the trap desorption temperature was 300 "C for 2.0 min. The sample was carried into a split/splitless injection port at 250 °C. The split vent was turned on at 0.5 min with a purge flow of 50 mL/min of helium. Retention times were I min for ethyl methylphosphonofluoridate, 2.1 min for the internal standard bromofluorobenzene, and 3.4 min for 3-hydroxymandelic acid, ethyl ether (impurity, not from VX) (Figure 1). The mass spectrometer was operated in Electron Ionization (El) mode and scanned from 35-300 amu in 2.78 s. The molecular ion for ethyl methylphosphonofluoridate (m/z = 126) was not typically observed, but the characteristic fragment ion at m/z = 99 was observed (Figure 2).
The ability of the Tenax TA tubes to collect the VX vapor was verified by injecting a known amount of VX vapor into a 20 ft copper tube that had flowing air and showed that the VX was quantitatively recovered.
10
1.8E7
g 1 4E7 i S 1 0E7 i /
0.6E7 I |
1.00 2.00 3 00 4.00 5 00 3 00 4 00
Time An in
6 00
Figure I. Retention Times of Ethyl Methylphosphonofluoridate (MEPF), 1 min. Internal Standard Bromofluorobenzene (BFB), 2.1 min, and Hydroxymandelic Acid. Ethyl Ether. 3.4 min.
39
2E6
IE6
81
47 67 125 UL4-
Scan12(1 152 min) 10240001 D
111
r+- 10 160 180 266' 220' 240' 260' '280 300
Figure 2. Mass Spectrum of the 1.1 min Ethyl Methylphosphonofluoridate Peak.
2.3 Analysis of Neat Ton Container VX
Two samples were prepared for analyses by GC/MSD. The first sample was prepared by adding 2 uL VX to 200 uL of acetonitrile. From this dilute mixture, a 10 uL aliquot was further diluted into 0.6 mL of methylene chloride, which was analyzed by GC7MS, of which
1 pL was injected onto the GC/MS. The compounds of interest detected were 2- (diisopropylamino)ethanol, 12.1 min; diethyl dimethylpyrophosphonate, 16.2 min; VX. 20.0 min; and bis(diisopropylaminoethyl) disulfide, 23.5 min.
The second sample was prepared by adding 2 uL BSTFA and 2 uL VX to 200 uL acetonitrile. The mixture was then heated at 60 "C for 20 min. After the heating period. 10 pL of the derivatized mixture were added to 0.6 mL of methylene chloride and the resulting solution (1 pL) was analyzed by GC/MS. Compounds of interest detected were trimethylsilyl (TMS)- derivatized-ethyl methylphosphonic (EMPA)acid, 1 1.5 min; 2-(diisopropylamino)ethanol. 12.1 min; TMS-derivatized-ethyl mcthylphosphonothioic (EMPT) acid, 12.4 min;
I 1
S-trimethylsilyl-2-(diisopropylamino)ethanol, 16.0 min; diethyl dimethylpyrophosphonate, 16.2 min; VX, 20.0 min and bis(diisopropylaminoethyl) disulfide 23.5 min.
2.4 Experimental Design and Data Analysis
The data were analyzed using JMP" Statistical Discovery Software. The three variables were temperature, drop size, and air flow rate at three levels each. Measuring all combinations of these levels would yield 27 conditions (3 x 3 x 3); the cubic composite design chosen required nine conditions, which can be described as the vertices of a cube and the cube's center. This collection of data allowed for the determination of the major contributing variables and interactions among variables, although in this particular study, not all of the data points in the experimental design were collected due to the length of time of each experiment. The substrate temperature (°C), droplet mass (mg), air flow (SLPM), total percent VX recovered, and tunnel identity (four similar 5 cm tunnels, named a, c, k and 1, were available) were treated as variables that may affect the raw evaporation rate. Effect interactions among droplet mass, air flow, and temperature were included in the numerical analysis.
3. RESULTS
3.1 Time to Plateau
The VX vapor was collected until the concentration of agent reached a plateau, often ~1 x 10" mg/m . The lowest detected vapor concentration was 2 x 10"1 mg/m (Figure 3). Only the 50 °C, 0.92 uL, 405 SLPM samples consistently gave vapor values of zero. The trend in the time taken to reach a plateau is shown in the cube plot in Figure 4. For many samples, the concentration at this time was near the short-term exposure limit (STEL required by the Occupational Safety and Health Administration [OSHA]) of 1 x 10 mg/m . A least squares regression (r = 0.94, radf = 0.91 )a showed that the significant factors were temperature, drop size (in mg), air flow, %VX recovered, tunnel 'a', and mass * air flow (Figure 5, Table 1). The equation generated was
Time to plateau = 6315 - 107*T + 145 * drop mass - 2.2 * air flow -7.2 * %VX recovered - 914 * tunnel[a] - 0.42 * {(drop mass - 4.3) * (air flow - 223)} (1)
3.2 Percentage Recovery
Scatterplots of the variables substrate temperature (°C), droplet mass (mg), and air flow (SLPM), and the results %VX recovered and raw evaporation rate showed that the %VX recovered and raw evaporation rate were loosely correlated with each other (r = 0.64,h Figure 6). None of the other parameters were correlated. In fact, the data showed that the %VX recovered and raw evaporation rate data were distributed throughout their respective ranges as a function of
a r estimates the proportion of the variation that can be attributed to the model rather than to random error: r,^ adjusts for models that have different numbers of parameters. A perfect fit is r = 1.0. JMP Statistics and Graphics Guide, Version 5, by SAS Institute, Cary, NC. 2002, pi86. r is the Pearson Product-Moment correlation; a perfect fit is r = 1.0. JMP Statistics and Graphics Guide, Version 5. by SAS Institute. Cary. NC, 2002, p376.
12
temperature, drop mass, and air flow. A cube plot also shows the ranges in %recovery (Figure 7). The percentage of agent recovered was largely random; the least squares regression had a low correlation coefficient (r = 0.58, ra<if = 0.37, Figure 8).
3.3 Evaporation Rates
The evaporation rate was calculated by summing the %VX vapor recovered, plotting the cumulative %VX loss versus time, and taking the slope of the line, which was the evaporation rate (Figure 9). Examples of replicate collections of evaporation data at two different conditions demonstrate the degree of variability observed (Figure 10).
Given the large degree of variability in the raw evaporation rate (Table 2), the raw evaporation rates were divided by the %VX recovered to yield an adjusted evaporation rate. Organizing the data by condition and taking the averages showed that the adjusted evaporation rates covered a much smaller range than the raw evaporation rates, and major trends began to emerge, as shown in a cube plot (Figure 11, Table 2).
Numerical analysis of the data was performed - namely, using a least squares fit for the raw evaporation rates (mg/min) as a function of substrate temperature (°C), droplet mass (mg). air flow (SLPM), %VX recovered, tunnel identity and the interacting factors, temperature * mass, temperature * air flow and mass * air flow(Figure 12, Table 3). The r was 0.90; racy was 0.87, and the statistically significant factors were temperature, droplet mass (in mg), % agent recovered, temperature * air flow and drop mass * air flow; 40 datapoints were used. Tunnels 'a' and 'c' were significantly different from tunnels 'k' and T; and an equation was derived to represent the relationship (eq 2). A regression that included the %VX recovered yielded a lower r of 0.89. The least squares equation generated was then used to predict the evaporation rate for each sample (Table 4).
Raw evaporation rate = -8.08 x 10'*+ 1.41 x 10"4 * T + 4.05 x 10 4 * Drop mass +5.52 x 10" * %VX vapor recovered + 1.30 x 10"fl* (drop mass-4.4)* (air flow-207) +7.33 x 10"7* (T-42.6) * (air flow-207) +1.08 x 103 * tunnel[a] - 9.83 x 10"4 * tunnel[c] (2)
3.4 Combined Effects
The simultaneous effect of both degradation and evaporation was calculated. Degradation rates for VX on washed glass were calculated from the air-dried sand (ADS) values at 22. 30, 40, and 50 °C and the washed glass (WG) degradation rates at 22 °C for 97% or purer VX.4 At 22 °C, the ratio AWA'ADS = 0.0059/0.0181 = 0.325. The rate constants at 50 °C for ADS (0.0912 hr1) and the interpolated k at 35 °C (0.057 hr"1) were multiplied by 0.325 to give an estimate for the degradation rate on washed glass. Thus, the percentage of VX that had evaporated, degraded, and remained was plotted as a function of time for 35 and 50 °C (Fiyure 13).
13
0.020
0.015 * x
CO 0.010 E ••D<>D ° *
0.000 %HWWi x
g 0.005
500 1000 1500 2000 2500
Time /mins
Figure 3. Vapor Concentrations for 1 uL Droplets of VX Evaporating from Glass at 35 °C, 18 SLPM (A,D,0,0), and 50 °C, 405 SLPM (x ,+,*,-)•
2800
3030
Drop size (1, 6, 9 uL)
2340
720
1850
2430
1380
344
900
Temperature 35,42, 50 °C
Wind speed 0.22,1.5 and 3.3 m/s
Figure 4. Average Time to Reach a Plateau in the Evaporation Rate of VX from Glass.
14
3500-
3000-
§2500-
<2000-
£1500-
^1000-
500-
o-
800-
600-
.1
400-
o-
V 0 1000 2000 3000
Plateau Predicted P<0001 RSq=0.94 RMSE=312.35
(a)
4000
CO Z> •a CO I 200- 3 CO CD
5-200-
-400-
-600-
. 1
1000 2000 3000 4000
Plateau Predicted
(b)
Figure 5. Actual vs. Predicted Plots for the Time Taken to Reach a Plateau for the Evaporation of VX from Glass, (a) Least Squares Regression Fit (b) Residuals.
Table 1. Parameter Estimates for Major Effects for the Time to Plateau during the Evaporation of VX from Glass.c
Term Estimate Std Error Prob>jt| Intercept 6315 452 <0001 Temperature, T/°C -107 11 <0001 Drop mass /mg 145 31 0.0001 Air Flow rate/SLPM -2.2 0.7 0.0056 %VX recovered -7.2 2.9 0.0229 tunnel[a] -914 285 0.0044 tunnelfc] 324 198 0.118 tunnel[k] 215 141 0.144 (T-43.8)*(mg-4.3) -6.4 4.4 0.156
(T-43.X)*(SLPM-223) -0.02 0.10 0.833 (mg-4.3)*(SLPM-223) -0.42 0.12 0.0025
Values of Prob>|t| less than 0.05 are eonsidered significant.
15
y.
5 E o
X >
c o
u O a
ed o2 c
o
> _
•i—i
=
u 5.
— - -r. e o
o U
3 !-
VX
pu
rity
/ %
re re re 00 00
re iri
(N re
(N
in d re re re .re re re re oc OO
Ave
rage
pl
atea
u tim
e/
min
oc
IN
o p
o
Stan
dard
D
evia
tion
raw
ev
apor
atio
n ra
te/u
g m
in"1
CN
d © — fN
d <N
Ave
rage
raw
ev
apor
atio
n ra
te/u
g m
in"
d IN
d <N r>
Stan
dard
D
evia
tion
%V
X
reco
vere
d
i**, oc T r
Ave
rage
%
VX
re
cove
red
— <N
^c r~-
Tim
e to
re
ach
a Pl
atea
u/
min
o in
o o oc ^C
© C
re o o in IN
o o fN
C o © »n
o o c IN in
o o
o o o
o c s a- (N
O o
re re —
Raw
ev
apor
atio
n ra
te/
ug m
in '
©
o m
© d
rsi
d d
O © 2 o fN
O
IN
O
<N
O
<N rn d d q
00 in
d
© o <N
O o ri
-a
Si -? °
o E
<N oc
vC rs CN
oc
CM
»» r-°
oc
in
oc oo in
r-i t-- oc
rl -T
OC oc ri
Air
Fl
ow/
SLPM
oc oc
r*1
OC
r--
oc
oc
00 oc oc in O o
in •n in »n o
oc oc
r>
oc OC OC OC oc oc oc
Dro
p M
ass/
m
g o o
r4 ON
d
CM fN O d
O d
IN
d d
IN IN
d d
r i
d
<N r 1
d
<N a* d
(N (N in,
in
1/1 m. m
»n
m,
in
in
<n
in
in
7i £ C< o ° (-
«n in in
in rn in
in
in "2 >n
oc
in
oc
ON d in
d in
d »n
in,
d in in
d in
in oc
<*> ri in, rn
00
5 oc
-r
u O U
IT,
re r*1
in
u
O ©
r-
O i
r**4
O fN O
O i
O •
m
<^1 en
h q in
<N q T
O i
r- c •
(N O i
o 1
(N q o 1
IT)
oc in,
oc fN q q
i
T3 o 3 C
o U
_£3
5
> 0 c 0
0
>
CO
- u c
>
u
— C
V".
c 0
0 U
r i
71, f-
OC oc
C1 oc oo
OC OC
O OC
OC c"i
00 a d C3
-T A
vera
ge
plat
eau
tim
e'
min
OC
o
rj
r--
r-
Stan
dard
D
evia
tion
raw
ev
apor
atio
n ra
teug
min '
rj - ri r*"i
Ave
rage
raw
e\
apo
ratio
n ra
te/u
g m
in'1
^ r) fN vC
Stan
dard
D
evia
tion
%V
X
reeo
vere
d
rj -T
rt rj
Ave
rage
"o
VX
re
cove
red
v* r-
Tim
e to
re
aeh
a Pl
atea
u m
in
c
ri
=
8
o ©
r*"> r i O rj
rj r)
o o o vC
O o oc P
Raw
ev
apor
atio
n ra
te
ug m
in'1
ri
o r— -* On
ri ©
© ri ri
o rsi d 'r,
© © -T
ON OC
e O - •-> u
1-
oc r-
©
rj
r-'
rj X
rn
ri
ri p
Air
Fl
ow
SLPM
OC oc
r~
X ©
C -3-
r- oc 00 oc
OC
oc oc
r~- oc
1^1
Dro
p M
ass
mg IT)
r— ri oc
r~ r| oc
r~ r4 oc
(N oc
r-
oc rj oc
r i
oc
r~ ri
OC
r-
oc od oc 00
r i
oc
C E U u ° H
ri r) ri
ri ri
r-
-r r*1
</~i r*1
r-
0"! O d
i?i >r> d
o
OC
O i
c 1
r- rj
oc
o 1
m i
r">
c
vC
O •
C i
J-iL
— rj ri rt
17
50-
45-
40-
35- 9f 1-
5r 3=
1- 450=
350=
250=
15th; 50-
100-
60-
20- 0.009z
0.006^
0.003^
0=
I I-
temp
f . i*--*-- . «.*Pv»
\ •**'>,
drop mass
SLPM
5 i
» • •. i
i • % recovery 1.
<• •
. raw evap rate
35 40 45 50 12345678950150 300 45020 60 100 0 .003.007
Figure 6. Scattcrplot of Temperature, Drop Mass, Air Flow (SLPM), %Recovery, and Raw Evaporation Rate.
43-75
13-50
Drop size (1, 6, 9 uL)
25-70
40-75
21-37
45-87
6-42
7-27
Temperature 33-114 35, 42, 50 X
Wind speed 0.22, 1.5 and 3.3 m/s
Figure 7. Cube Plot of %VX Recovered for Evaporation from Glass.
is
120-
100-
"I 80- o < 60- o
£ 40-
20-
0-
,..._><
V 0 20 40 60 80 100 120
%rec Predicted P=0.0268 RSq=0.58 RMSE=20.931
Figure 8. Least Squares Regression Analysis of %VX Recovered Data as a Function of Temperature, Air Flow, Drop Size, Tunnel Identity, and Time to Plateau.
6.0
•S 5.0 g O) 4.0 c 'c
E 0)
c 0)
<
30
2.0
1.0
0.0
• •
y = -0.0011x + 5.5194
R2 = 0.9962
•••••• »
500 1000 1500 2000 2500 3000 3500 4000
Time (min.)
4500 5000 • Md-Time D Linear Linear (Linear)
Figure 9. Calculation of the Evaporation Rate for a 6 uL Droplet of VX Evaporating from Glass at 35 °C and 181 SLPM. The squares show the data that were used to generate the regression line of slope 0.0011 mg/min.
19
100%
?W£!*I*'M § *Ao«
a a
500 1000 1500
Time/mins
2000 2500
Figure 10. Cumulative VX Vapor Recovered for 1 uL Droplets of VX Evaporating from Glass at 35 °C, 18 SLPM (A,D,0,0), and 50 °C, 405 SLPM ( x,+,*,-). The solid line represents the degradation rate of VX at 50 °C and the dashed line represents the degradation rate of VX at 35 °C.
2 + 1
0.9 ± 0.2
Drop size (1, 6, 9 uL)
6+3
4±2
0.1 ±0.1
0.6 ± 0.2
2±2
0.2 ±0.2
Temperature
3±1 35,42, 50 °C
Wind speed 0.22, 1.5 and 3.3 m/s
Figure 11. Cube Plot of the Raw Evaporation Rates (ug/min) for VX Evaporating from Glass.
20
0.009-
0.007-
•S 0.005-
m o < & TO
<z
ro 0.003- > UJ
I 0.001-
-0.001- .->
-0.002 .002 .004 .006 .008 .010 Raw Evap Rate Predicted P<.0001 RSq=0.90 RMSE=0.0007
0.002-
0.0015-
0.001-
0.0005-
o-
cc ZJ
"D </> cr 0) 03 cc CL
& -0.0005-
I -0.001-
.-• •
-0.0015- -0.002 .002 .004 .006 .008 .010
Raw Evap Rate Predicted
Figure 12. Actual vs. Predicted Plots for the Raw Evaporation Rates for VX on Glass, (a) Least squares regression fit (b) residuals.
Table 3. Parameter Estimates for the Major Effects Contributing to the Raw Evaporation Rate for the Evaporation of VX from Glass.d
Term Estimate Std Error Prob>|t| Intercept -8.1 x 10"' 9.4 x 10"4 <0001 Temperature, T /°C 1.4x10"4 2.3 x 10s <.0001 Drop mass /mg 4.0 x 10"4 5.3 x 10*5 <.0001 Air flow /SLPM -1.0 x 10"(' 1.0x10"6 0.3004 %VX vapor recovered 5.5 x 10- 6.0 x lO" <.000l (T-42.6)*(drop mass-4.4) -8x 10"7 7.0 x 10"6 0.9106 (drop mass-4.4)*(air flow-207) 1.3 x 10"(1 2.6 x 10"7 <0001 (T-42.6)*(air flow-207) 7.3 x 10"7 1.5 x 10'' <.0001 tunnel[a] l.lxl 0-' 4.5 x 10"4 0.0219 tunnel[c] -9.8 x 10"4 4.3 x 10 4 0.0316 tunnehk 1.9 x 10 4 2.6 x 10"4 0.4716
' Values of Prot»|t| less than 0.05 are considered significant.
21
100
80
60
40
20
0 I il 100
80
60
40
20
0 o o o o o o o o r- <N CO T*
o o CO o t CO
o o o o o r- O O O O
T- c\j n M-
Time /mins Time /mins
• 50C degraded • 50C evaporated K 50C remaining D35C degraded • 35C evaporated B35C remaining
(a) (b) Figure 13. Relative Contributions of Degradation and Evaporation for the Loss of VX from Glass, (a) 50 °C (b) 35 °C.
22
Table 4. Comparison of Predicted and Measured Raw Evaporation Rates for the Evaporation of VX from Glass.
Code Temperature/ °C
Drop mass/ mg
Air Flow/ SLPM
Raw Evaporation/ Rate
ug min '
Predicted Raw Evaporation Rate/
ug min ' 3k-016 34.5 0.92 181.7 0.33 0.23 3a-115 34.9 0.92 181.9 0.7| 0.76 3c-157 35.2 0.92 181.3 0.60 1.0 31-039 35.3 0.92 18.7 0.15 0.22 3k-037 35.3 0.92 18.7 0.11 0.57 3k-()29 35.5 0.92 18.8 0.12 0.45 31-030 35.5 0.92 18.8 0.01 -1.2 31-036 35.8 0.92 18.7 0.19 0.8 3k-023 49.6 0.92 405.6 4.3 5.3 3k-035 49.8 0.92 406.2 I.I 0.94 31-033 50.1 0.92 405.4 3.2 4.0 31-034 50.1 0.92 405.7 2.1 1.7 3k-025 50.2 0.92 405.6 2.1 1.9 3k-034 50.3 0.92 405.6 2.9 2.5 3k-027 50.5 0.92 405.6 3.1 2.7 3k-024 50.4 0.92 18.7 0.07 -0.29 3k-026 50.6 0.92 18.7 0.36 0.81 3k-022 34.5 5.51 181.7 1.03 1.5 3a-l16 34.6 5.51 181.9 0.75 0.70 31-020 34.8 5.51 181.6 0.58 0.0 3c-158 35.2 5.51 181.3 I.I 0.70 3k-028 41.4 5.51 181.7 7.2 6.2 3k-033 41.8 5.51 181.6 3.7 3.4 31-032 41.8 5.51 181.6 2.4 1.8 3k-038 42 5.51 181.6 2.6 3.2 31-037 42.2 5.51 181.5 3.2 3.7 3k-031 42.2 5.51 181.7 3.7 -i 2
31-027 34.7 8.27 405.4 3.9 3.3 31-031 34.7 8.27 405.4 1.4 2.1 31-038 34.9 8.27 405 2.5 2.2 3k-039 35.6 8.27 404.1 1.5 2.3 31-029 :o.5 8.27 18.7 0.39 1.0 31-035 50.7 8.27 18.7 2.0 2.3 3k-036 49.6 8.27 18.7 2.7 2.6 3k-032 50.1 8.27 18.8 1.7 2.1 31-022 50.5 8.27 18.7 0.26 0.37 31-026 50.6 8.27 18.7 4.7 4.4 31-021 50.1 8.27 405.4 5.0 5.4 31-023 50.7 8.27 405.4 4.0 5.1 31-025 50.6 8.27 405.5 8.9 7.5
23
4. DISCUSSION
The precise reasons for the large, vexing variation in %VX recovered and raw evaporation rate remains unknown. The raw evaporation rate was derived from the cumulative %VX recovered. Thus, the loose correlation between %VX recovered and raw evaporation rate was not surprising. The least squares analysis used both %VX recovered and raw evaporation rate to generate the predictive empirical equation that had r = 0.90.
Since the drops were not individually weighed, the exact mass for each drop was not known, which would also add variability to the data. In addition, small changes in the amount of adventitious water present in the VX would affect the VX degradation rate, which would in turn affect the %VX recovered. Independent studies4 showed that the VX degraded with a half-life of 16 hr (960 min) at 30 °C, and 8 hr (480 min) at 40 and 50 °C. Thus, agent degradation was competing with agent evaporation in these experiments. Comparisons of the measured evaporation rates with the calculated degradation rates indicated that both processes occurred on a similar timescale. For the 50 °C samples, there was great variation in the cumulative %VX values (Figure 10), although evaporation for all samples had ceased at 400 min, indicating that all the VX had been exhausted. A mid-range sample was chosen for the comparison of the two processes. The calculated comparisons of evaporation and degradation at 50 °C in the bar graph indicated that VX would still be present at 600 min, but the vapor recovery in all cases indicated that the evaporation of the VX had ceased. This difference may indicate that the actual degradation rate was faster than the rate used in the calculations, possibly due to water in the air or EMPA in the VX. In addition, as the VX evaporated, the concentration of EMPA increased, thus increasing the degradation rate further in the autocatalytic cycle. As seen in Scheme 2, EMPA is both product and reactant for the degradation of VX. Thus, degradation rates in an open system may be faster than in a closed system at the same temperature. At 35 °C, the calculations indicated that VX would be present at 2400 min, as observed. The degradation rate was faster than the evaporation rate at 35 °C, whereas the evaporation rate was faster at 50 °C. The rate constants for degradation did not consider air flow or drop size effects, and thus only the temperature component is reflected in the bar graphs. In other words, with a different air flow or drop size, the evaporation/degradation balance will shift.
The EMPA formed is non-volatile; thus a mass-only method (such as balances or TGA) for following the evaporation of VX would be difficult, because the mass loss would be due to both VX and diisopropylaminoethyl thiol (DESH). As much as 3% EMPT product was detected in the NMR studies; the wind tunnel studies were not designed to detect the expected concomitant bis(2-diisopropylaminoethyl) sulfide product.
24
o , II / o-p-s Me
n EM PA t-2
VX
66
O
Me-P=0
Me-P=0 i
•pyro'
© /
DIAZ+
O II 0
Me
EMPT
^3
H20
O 2. \ n O-P-OH
^8
DES- 0&
^7
f H20
O O-P-OH + HS"
Me
EMPA
Me
EMPA
HS DESH
Mo DESH [O]
.N.
S i
s.
H'
(DES)2
disulfide
sulfide
Scheme 2. Degradation Pathways for VX.4
5. CONCLUSIONS
During the first 1500 min, the VX vapors emanating from the glass substrate were above the Immediately Dangerous to Life and Health (IDLH) limit of 3 x 10" tng/m (IDLH is the Occupational Safety and Health Admininstration [OSHA] limit and the short-term exposure limit [STEL] of 1 x 10* mg/m ). Both degradation and evaporation were equally important contributors to the concentration decrease of VX vapors in these experiments. The exact point at which no further agent evaporated depended on the temperature, drop size, humidity of the air. and initial purity of the VX.
25
Blank
26
LITERATURE CITED
1. Brevett, C.A.S.; Giannaras, C.V.; Maloney, E.L.; Myers, J.P.; Nickol, R.G.; Pence, J.J.; King, B.E.; Sumpter, K.B.; Hong, S.H.; Durst, H.D. Evaporation Rates of Chemical Warfare Agents Using 5-cm Wind Tunnels. II. Munitions Grade Sulfur Mustard (H) from Sand: ECBC-TR-699; U.S. Army Edgewood Chemical Biological Center: Aberdeen Proving Ground, MD, 2009; UNCLASSIFIED Report (AD-A508 851).
2. Brevett, C.A.S.; Pence, J.; Nickol, R.G.; Myers, J.P.; Maloney, E.; Giannaras. C.V.; Flowers, A.; Sumpter, K.B.; Durst, H.D.; King, B.E. Evaporation Rates of Chemical Warfare Agents Using 5-cm Wind Tunnels. I. CASARM Sulfur Mustard (HD) from Glass; ECBC-TR-647; U.S. Army Chemical Biological Center: Aberdeen Proving Ground, MD. 2008: UNCLASSIFIED Report (AD-A493 238).
3. Brevett C.A.S.; Pence, J.J.; Nickol, R.G.; Myers, J.P.; Maloney, E.L.; Giannaras, C.V.; King, B.E.; Sumpter, K.B.; Hong, S.H.; Durst, H.D. Evaporation Rates of Chemical Warfare Agents Using 5-cm Wind Tunnels. III. CASARM Sulfur Mustard (H) from Concrete; ECBC-TR-745; U.S. Army Edgewood Chemical Biological Center: Aberdeen Proving Ground, MD. 2009; UNCLASSIFIED Report (AD-A516 459).
4. Brevett, C.A.S.; Sumpter. K.B.; Pence. J.; Nickol. R.G.; King. B.E.; Giannaras, C.V.; Durst, H.D. Evaporation and Degradation of VX on Silica Sand. ./. Phys. Chem. C. 2009, 113 (16), pp 6622-6663.
5. Weber. D.J.; Scudder. M.K.; Moury, C.S.; Donnelly, T.; Park, K.; D'Onofrio, T.G.; Molnar, J.W.; Shuely, W.J.; Nickol, R.G.; King, B.: Danberg. J.; Miller. M.C. Micro Wind Tunnel for Hazardous Chemical Fate Studies. In Proceedings of the 45th A/AA Conference. January. 2007; AIAA-2007-0960.
6. Weber. D.J.; Scudder, M.K.; Moury. C.S.; Shuely, W.J.; Molnar, J.W.; Miller, M.C. Development of the 5-cm Agent Fate Wind Tunnel; ECBC-TR-327, U.S. Army Edgewood Chemical Biological Center: Aberdeen Proving Ground, MD, 2006; UNCLASSIFIED Report (AD-A462 884).
7. Danberg, J. Evaluation of 5-cm Agent Fate Wind Tunnel Velocity Profiles; ECBC-CR-091; U.S. Army Edgewood Chemical Biological Center: Aberdeen Proving Ground. MD. 2007; UNCLASSIFIED Report (AD-A472 909).
8. Weber. D.; Scudder, M.K.; Moury, C; Shuely, W.; Molnar, J.; Danberg, J.F.; Miller, M. Velocity Profile Characterization for 5-cm Agent Fate Wind Tunnel; ECBC- TR-567; U.S. Army Edgewood Chemical Biological Center: Aberdeen Proving Ground, MD, 2007: UNCLASSIFIED Report (AD-A476 518).
9. Smith. J.E. Jr.; Boyd. W.D.; Mason, D.W. Depot Area Air Monitoring System and VX Study', Contract DAAK11-77-C-0087; Southern Research Institute: Birmingham, AL, 1982.
27
10. Committee on Review and Assessment of the Army Non-Stockpile Chemical Materiel Demilitarization Program: Workplace Monitoring, National Research Council, Impact of Revised Airborne Exposure Limits on Non-Stockpile Chemical Materiel Program Activities; National Academy of Science: Washington, DC, 2005, p 37.
2S
a en n Q.
3 E CD CM
$ cni^fvh-h-Nr^f^-h' * •* ^r ^r 'tf
5 1 LU LU LU LU 111 O tO i- 0\ -*t in o ^r oo co
38838S88888S8888888S8888888 X. Z. ^. ,;,,• J, ******************** *
'"lUllJU)U-IUJUJ>.ULLllI[LijmiLJlul_L!LiJLUlllU)LiJIUUIUilUlu
S3S888888888888888888888 ooooooooooooooooooooo
M CO Ol N 00 0> Oi Sin ui
in CO
<N N « £ Si o o r r • s s « £ g S a O N *
N <M r- CM r-. CM co co -q- v
N W N N
<C IO (D <C <C <U at o »- CM co 3 W IJ) N 9) >- cO UJ r* CMCMCMCMCOCOCOrO
m o *n
CO CO co to CO
CM N CM N CM r-- O O y- i- CM CM c\i cy CM CM CM csi
(%) Bjjuiciuoy iua6v
C3
>
CO o a; o o 5
•D TO o c
"53 •a o
ro eg to in to o St-' in
co co
8 Q :0
C a) o c o o o TO >
•«
•« •« •« •« •«
•*
4
•*
•*
-*
•*
•*
•*
•*
•4
•*
Oo
p
Giu/6ui u| JUBEV
29
° E § i o E
I!
omcor-cocotnmtocoir) tnOlr-inCMlOCOCOCOCOi-
CT) Ul O) Oi CJ> CD CM <J> ID Tj
O) CD CD CD N K N.
S3 CO CD 3 P » a
2 s a in 8 S IT) •*
IT) 1?)
„s gS ^ s
^P * jjS 6n
s 5 § < CD
in 0 n
Ifl tn if) in 10 in Ul •/>
88888S888888888888888S33S3S3SS UJ UJ UJ UJ UJ UJ UJ LLJ LJ UJ I1J LU UJ UJ 01 LU UJ UJ LU IJJ LU UJ UJ UJ tU L±J U UJ UJ L i 1
co cn CD m o> 't u
CM cb m ^ V K) cd iri o*JOJcof^LOcooom*-r*-o>ioec>cn,'*cpi-irtcp(o lOcoco^OTrKr^K^^^ncDTrfOtococococN
ed cd oi **' oi c\i cj
$ a » - g g B 3 OJ o
C\J o> in r- eg o 8o in o in o u?
CO CO O) OJ o o in E co CO U] (\iccu)N0imu)in
tO CV O h-
NWWNWWNCO CO rt CO CO CO O N ifl 15
O I x >
3 s s c (£ C S N P3
0)
o
o
8 I E E O 99 o ID *- o m h
CO to in ft 00
in
£* J* CO CO oS oi
8 a
8 •5 CJ
|
(%) BUIUIEUISH jusBv s? sS s!
"5 ;"
ay jo
e
9, E
8 s « P £• i
ill £ Q K h- 2 Z S U < < 5 I
W 4>
EUi/Buj ui )uo6v
APPENDIX 30
CD
s 0-
£ £
^ -5. 3 t
II
co^oNT-oco^a>wwu5«eoo}roNwoo(D<DKrti-rtf^wco
5 N 8 S 81 S to h- to m Tt ^t co
88888888 88?SS888??8 8S8 8S???3c!? LU LU UJ ID o co 10 * w *- co
LU UJ
in co
UJ U LU LU UJ UJ LU UJ LU UJ r-cooor-N-ior^mroin n w on y w q oo q
CM co
UJ Ul LU LU s s ILJ UJ LU LU UJ UJ in co o co CM o rt o i?) OJ m h-
CO CM OJ CM o> m en CM y-
88?
x
X >
CD O CO O CO
8 c
& O CM
o e
1
C3 c o TS a
HI
2 Q
E E
SSi o gj
«; l
5 - < <
*~ O 0) CM co m U} r^ UJ CO CD CO
•t *-. jf> tn rri .V "£ <D" CD CO CO
(%) BUIUJUUIOH luo6v -j> ~p ^p x y as o o o <o tb •<#
i s I
g I V. m tn
sf t fl & I
OJ CP
CD •
I §
M U O 10
I fe s - 5 O <
I g 5. (5 E E
••! I 0) 0 5
S S o < < u
sj 0> J
5^2
! 1— 1- —1— —1—
+ •
«• «• «•
• « • «
• «• • < • <• fl
? • •« v> c
C ^ 4 o m • « E c 1 ^ 4
o r
^ 4
o o o 1
3
• ^
4 4
a ^ 4
> I ^ 4 1-
• • < • «
• « • «
• <
•
< • < •
•* 1 •*!
•
cSq>
P
o ID
8 i © u> o m o 5 co CM CM »- T-
§88888 3 o o o d o
CUJ/6UJ U| iua6y
APPENDIX 31
a.) a CO
s? # aS O O) CM
0? S5 S? cn o) co CO <7>
GO <0
DO GO
... CM <£> CJ w o>
<* K «* (O CO N N N N N N
££££££££
8888?SS88S8S8S88888^ ''JWWUJLijWlLllilUJWlJJWWlUUJliJWlijUJWW
)c00)CSinQ'i--*-r--cnc0T-5r00OC3»-NC0'^'C0T-OoOOOOO jrt^cy>-ocvjoooi^coc6inNu5c\Ju5^rcyco^'>-oooooo r^oicocnc^OTrocncocoKtowtotD^Trmiocon ,*'-oooodd
ffi<000'-r^lSj(D pj^oooKujpfy
a* n g§ § § E; i s 11111111111 r-mcOwocpr^tncocNjQ *-ma>cor-OTcoc\j(Do
"gcotyggcMiooi rS8 CO CM to CO
6 E f E
CO x
(3 x' > 8
CO o
CD o o C\J
5 O
{%) 6uiu ecue;j iuo6v vfl sO ^p ill
o c
8
• •
I a
1 LU
A3
TO a
i r C) E o O
• CO 5 o
g ft CM
3
If ' <
*~ 5 d
n CD
a 3
b B,
* a a
s f & t- •§ n o
3 a i a • c
E 1 3 4
o c
to c S 13 s ft n
O ai g i n
g n E 9 o I p CJ ^ p >
H r- ^ ^ -> Q < *i •a u
-t-
< •4
•4
•4
« •
8
c o'E Ocp
p
• • •
•4
1:
• •
8 8 g o o c eui/Bui ui iue6v
o o
APPENDIX 32
a a Q.
APPFNDIX 33
I a
< I
3l
II
$ 8!
co eg
ro 3? m
CO a CO ro co
•f s C
If)
5?
s 0
8 CO 1 Ol ID
* CO oj
in 3 ro 5i g en CO
CO cu cu CO
IO CO
in ID an 3 CD
m CD CO CO a> s a
r- 3J CO
888388838888888888388883388888 UJliJUJLUliJUJLUUJLULUlLlLuJlilJLULUUJlililUUUUJ g>'?-cocyi~h-i-'-if>'-NO)VT-T-tt)Qmiooc,ycoocy<pP3 0jr^mo iri Lfi (D © (fl s
i- ^ If) r S Ol v
SNiDtduiiovuiirin m in _
U") 1- ic! n ri pj
(T) <t «C 'f t t N CM
.--.inomoinOinQiooinQlnS
22ifirs5S^cj)Nir)Qr(nS*: ""•-NNnvinifitDsaJoift?:
iO O iO O in o *n tp r- h- oo co 0> O) ? !? 8
3 x >
a
8 s o o CM
O
>~ a.
•D TO o
Q) •D O
T5
a E E
CO § 5 E a 8 «5
Q.
9 Bj i5
<M iO m B J o a a: <
m »- o m a> ? s
•& ^ ^
I (%) 6uiu|EiU9U |uo6v
CM
I
CJ
£ 9
i E S
8 C o
1 £
1 1
jjj i 1 id
"5 > a. 1 en
Vi
1 •n
5: 0 £ f
Cfl o a 01 a ft, s
19 w 1 3
L- n s o a 0) fee
z z i o < < <r 0
-U si ?. F cT E « s 5? 6 1
W a> r
„': •9 if) p
2 £ 5
8 U) CM
• •
••"l — „': cr r
in c
c r. 0 E
ra tr
c 0) < 0 c •«
0 0 • »- r' 0 3 ^ 1-
ro K
> t- cu jr h-
• 1
•
• • •
oE 1041 "E
/
• ^
; V O O Q O
8 8 8 o 8 o
etu/6uj u| )un6v
APPENDIX 34
0)
CL
*4
^p *p »p fc R 6 O) CO CO Q) CD Q>
N <q <o in oi oi oi oi o> oi o> Ol o> en O Ol
tf; 9* <C ov P" «r- p^ ov o* tf*- ofeQ^cot-sngeo
<7>aiaioio><J)cococococococbco OlC4C'lCnftCft(7>OiO)00)0)a)dl)
"WO)CbiSlCOCOO)tCOJQOON N «S ifi «5 © JS m
UJ til UJ W UJ LU UJ UJ til UJ ULJ til UJ Ul UJ LU LU LU wcof^o'*±inrucQottf-><oo>Kcpio*i'C\jo r^ocotn^'h-Nuii-OJCoooioiniONcnr-
rio^nmwm'tnnrt'jojtMNN N W r N N N N
s s & s s ???S UJ LU in UJ UJ UJ UJ UJ UJ CO C7> (Si CO s a a S q 8 8
*- »- - O N
r^ OJ in to
8 8 !S£F:8&8iS>8!&£fcRi«88. P) 03 W N CM N N ^r v in in to <o r- OOOOOOO»-*-I-*-Y- m r* F- ' «- CNJ CU n ^ s •"T-^-^T-^T-T-^I-r-^T-WOJrt
R
LL
>
1 E
V
i I CO > -: •v
?
E E u J O * J° * ,_ g CD T K OJ z f> '" o m
CO OJ a
s 1- *- -r- •r- O)
C ^P -wP vP g 5. 4;
c 0) o c o o 1- o a m >
4
« •
oE 8V
• • •
• •
• •
^t CM
s o
8 8 8
£UJ/6UJ ui lueSy
APPENDIX 35
rd £
s« a* # 8? 6* 8 3
Ol(OSO*W'-0)N 00 O i/) <\J »- o
3? a? j5 d £ * fi SC s? s?
s s CO 00 ^ StSRRKf 8 tD Irt « 6 « «
»§ ooopooooo WWUJfjJUJUJLULJJlJJ i-0)rtNO)NNT-(p OT-ojooNOOcym «^ 1-^ T» 0 V « '
9 9 9. LU UJ LU Ul * QI & 9 oi m <o o)
co co co co o o o o
LU UJ UJ O Q> Tt r- o> CVJ
888S88SSS8 i UJ UJ 8 81
UJ UJ UJ HI ID CO O) W i/l Tf (D If)
i-OiNCOOTr-tOCOr-NtOCONUJlDCOCO
C S fe S 8 8 8 ? ? S 8 § S S ?« fe^ ^ R ^ g^ 8 P § 8 8 g it) lO ID N a s a § s1 a
in o io o O T~ T- CM W C\i <N C\3 8 § Si 3 CM CM CM CU
x
X >
<£> g O
o a £ o o N
o >1 a
{%) Buiuieujstj |usBv
I E
ai
TO
c
o 3
s o o s
2 a 3 CD < o
E E £> _1 35 O
5 C\J s 8 en
ssa
c a> o c o O k_ o a, >
" 8
• • •
5 E
1 iS 3 I
e •8 e <r
£ I a E E S z z S
8 I 6 s
i I I 6 «
E S '5 £ at co -s
co e K 0)
* s 1 n O B to « (8 w o <D co i^ > > > O < < < U
8 6s
« • « •
X •
« •
oE
i/JCO ^E
p
• «
• <
• «
:•• ,1 •
5 o o
CUJ/Bui ui iua6v
APPENDIX 36
0)
H 0.
c Si
!
3 I
.< j! )S j! S! j! j! ,-8 Jf i! ^. j gt j! ^ >! SS ^ !« i« S* !! # J« S* S' i? i! i? i5
8S88S§888SS88888SS383SSS333g38 tM iLlXJLUUJLULULUUJUJlilUJLlJlUlLlUlJJLULUlLlUJli oooi-^-ooor^ayT-uiT-ojOi-tDr^Nh-WKODropjincNjoarioj
« s n » s s $ n ^s n ^ s s n E ' (O ID (O CO ii 7 <C » " N W W W n n S s s oj w a eg
<0 Oi e»5 gu ^ V « ul
0)
C
>
Q 65 2 O
X 5
E pi E O
o 09 o '-D
n o> u> z ^
| E o c o
UJ
1 &
§1.1 fe e off?
E i &S| V> w J?
I s s 2 O <
a. cB
8 E
S> to
•s •§ |
HJ « w
3 3 8 s g
sr o
(%) 6u{Ujeuiau (uaBy
Cai/6ui u| lueBy
APPFNDIX 37
01 en S
c i, II 1 I
II
s s
S 9 5s p- o*~ o~- &* CO « p t-~ Q O co N cy eg
N? »! iP ^ •>? »•" s? S- S^ 3^ d^ a~- os <r 8 o o o o o o
8?SS88S8888888S UJ UJ IU UJ
CT> O) in IU III HI III liJ Ul HI UJ ill fflfflNSOlfflrPJi-Q ocoTj-cDr^ojcocoNco
^^cvJcvJ*j'cjrjesioJcjc\ic>JrycJ
"' UJ UJ UJ UJ yj UJ UJ
** 5 o o o o o
_UlUJUJUJUJuJli| O) CO CO CJ CO O —
- 10 r- in CD <n m i- C\l W OJ Pi N « t-
8g5S8i58S°"SKg iri CD CO CD CD *- OJ m •* LO
p tf> o *n W PJ CO 03
o in o
D O O O O O
o in o m o *- y- C\J CM O
i-rfllMNWOnt in to co en
TJ TO V-
a C
ffl •o o 2
o •D
E a c o a 3
CO > III
•1 Ol E E
2 a- 9
o
T- T- *- cv <D tn o o en r*. cy o
& I
» P c 0.- E c
I UJ ^ Mi
a JQ
5 |
go? * •
8. E
• g T5 ti w 5>
w 3 'flj £ g> A. ft. ft. 3 *° ro (U (U « IB
t_> < < <
I
8. •«
1 I 8 |
Is
•=. E
£ s
{%) BuiuicaKiy iua6y
S? 5? ^ o o Q * o ft
s E
3*f
^ ?
(/> C c Q o fe (TI cc i- f 0) 2 o c 4 o o o 1 a- >- HI > t &>
|S •
Kg
8
3 S Q 9 8 8 S 8 d o d d
£UJ/6UJ Ul )U9&V
APPENDIX 38
Q)
a
it
If
P £.
PJ P- M CM O) 0)
^ -sP vg vO
rt oo S O K N co co m vP ^S -5 »£ -? --* 5*- 3* «r> «? o"- ©v
ID in n ft a oi (O <D -
"'• LU UJ UJ Ul UJ til '" •e 5 to h- o <p in N in * W 3>
HI lil m in _ CO OJ y- CO lO <* n in N (o •" — l-vOidifOlDcd
UJUJliJUJUiUJUJUJUJUJUlLiJUJLilllJliJtiJliJ
uDTtinmmmoj^tcnT-oj'- S 8 8 S
odd
ao en en a CO CD Oi Ol
<l v Q ID fl o
(%) Bujuieujau jue6v
i - H
APPENDIX 39
in a
S. d < I
8 1
F I
aS sR #
v> u o o> o> o
g? as s? s? o s m ID <p co oi co
od in co
>P „0 ^p ,n ^O 0s- o- cc «*• «? OJ O O f O) co co rt i- co 8 3
3? a? S* # £ S I £ 3s 5s' ^ ^ CM CM OJ OJ to r-» r^ OJ
00 O) <o n CO f 0 CM CM CM <M OJ a CO ID O O) S S
r0T-CQtD^t-e0inOJO00tD(O<DCDCDtp<ptt)
8888SSSS8S88888S888^ LUUJLULUL^lLliJLJLlJlijLJJlUUJLIJtjjuJlillJJUJLJJlij eM<Dsgojwin»-incocM<Otf)OJ«^scowo»-«r-nooQooo o^djo^^^rcMKpcQcnN^OTOiO^mioocMrtK^Sooooo
£*8838"3K8S££ 10 T-OJC0'JU>(DNCOOi^r:?j^
ID <v ta a> *t o> ir> r^ co
SCOCOCOCpCOeOCiCDCOCO OOlOOi-rWWnO
! K f^-" r^ I--• K r^ i^ • tD OJ CO S o> c O
OJ CM CM
(%) 6uiu!etuou juo6v ^P ^P -j rT- d* cr
tfl x
CD x' >
i
o o c\j
o >. c o O
O •o re O D) c "5 o 2
g
Q CO
§ i 5
8 a E E ^> 03 O
i- CM O O)
K O (D
ra n T- O d M9 a.
TO 3 TO >
UJ t 8 TO s c S >-
r
a 3 c
111 i II if? * wi
2 S
•A «)
& 8,
S 5 o a I- z -z. 5 o < < <o_5_£
s.1 -O 1 E
£ J*
1 9 e 1 (fa a - 0J u o ft? <-• g
o 0 8 a f
5 S
1 B 1 ra
! a
1 1 £ £tii/6ui U{ iue6v
APPENDIX 40
CD cn CO a.
o- s? s? IONO>«JNaifflO)S<DfiO)tt oi^*'T
;SNOi(lJ^'(\i(' pimNOcsjcomr-oooooooo
«5<ocoinmmirtininioininioioioinu)
Sn n rt c*> p o o o IU LU LiJ LU UJ W C\J N Q> r- «•• ID m co o
S888S8888§88888?388888888 lilliiLJlijiijlijlJlLlijLLJlijliJlJJLillLlJlijljJuJUJiiJUJLJUJUJ
"fNCiririNNNNNNN^Nrdi o o o o o o o
(D Q o P © Q 3 t - oo co O) cn o o CO CO CO
rt co rt n t ^ Oi Oi oj OJ
CD I
x >
CD
+
: CM
oo S s CM
C
>. a. 8 cc
0) •a co
O ai c QJ
T3 O
o c o
'IS a
LU TO
•»—
CO
Q
i
(%) Buiuieiuoy tuoSv
in 5
i O) CT1 i E £
0.
Poi" 5! g | 2 .- t- i- « r- w rv
OJ CO CM
3 $ 3 < 10 m o m
p 8 <
1 > '-
I 1 9
III
If .5 JS
a s 1 -5 5 a 's 2 « S
2 8. E
Q> -r- C C & ^ I I 1-1-2 2
o c
11 * 6 £ s
_. o; CT * fl> (0 (8 fll W C O 4) <5 > O > > > O o < < < u 1?
1 1 1 • ••
4
H 1—
•
4 •
•* •
4 •
t 4 T
</> C c a o L 4 m S k- c c 4 <D < O c < o 4 o o H 4 a. re >
4
4 • •
• < • 4 • 4 •
4 • 4 4 X 4 •
« • « •
« • 4 •
4 • 4 • -
+ • • 4 * •
4 4 < •
•—c-4-,—,—r , • -*-.
E P
8 8 8 8 8 8 d d d ci d c
eu»/6w ui iuo6v
CM i-
8 8 d d
APPENDIX 41
a
u £ o 6>
5? 59 $ 5? IQ 00 0> CO CO CO (0 US
81/i « 0 uj N a> CT> 00 00 00
fa S- 01 o> Hs
OJOlDCOQ'^-'tQ SNlOffliJlfliOi?)
00 CO IT) y- s oi to n If) CO OJ N
S? # # BI C" fit O) K 35
88SS88888SSS?S8S8883SSS888«SS8 lUlLJIULULUUJLLtLLJLULLjIULUUJ'*' T- ID O Ift fl COtDOlCO O?)N0)4'-n(D(p (O00SS(ONN(DTfa>NIDN(DN^nn'-O)N
LU LU UJ LU UJ W LU LU LU LU UJ LU 'JJ LU LiJ UJ SOCOCVOCD^-tDt^PcpoOJoQO _«cqrtr-i/>o^cqqNKSoooc5oo
i/l o o (>J o o o
SS O N N s o m 8 8 S n 0
r- I; iO to So
APPENDIX 42
OJ
5 I
II
<b 6 ^* j? ^p ^s <£ ir> (P- tf-
q S c^ CMOOoooooooicnOTcncncncn
O) O CO CO u^cn^minQ^f^cncDcocpscocgcococot^Nr^fih-t-i^r-
888888888888838888888888888888 ujlLwWWWWWWUIWlljlijLUWluUJWWWUIWWijLiuJUUJlJJllJ 28a8SS!sa§88SR!588888888t888888S
882 rt ^- 3
SPS888n§2? W N (\l C\) (M f) a ?> ns
CD i x
>
3
O
8 o to
c
s Ql
2 <5 PI
o
e £ o O * h|D *° r~ CM O 0) 3 IS a, S > « O o
t- o tf in o 9 ID U
8 (%) 6uiui8Uieu juafiy
O CO
—I—
I
:
•4
•* •*
•«
•* •*
•*
•4
• V
^i
•4
o o EUi/fiui u; »uat>y
APPENDIX 43
0) en n
CL
! E
ST CM en a;
£ 8 0~"
CO 0>
CM OJ
CO 9 If) OJ CO g O
b o
5s- 3s 5" 5"*
8 S 3 8 CO o
CM O o d i jfj
en O!
a N t- CO <I) CO p CO CO ri ro CO CM ft A 0) a^ u; <J> O) Of CD U) CO n CO 01 CO CJj CO en CO CO (J) a> c. 7) a> CD CO
i E ft
en o 8 co CO o 8 8 co
o o CO o o
CO o CO o CO o CO
o o 4 o 8 S 3 9
O o in
a a O CO o
/I 8 8 8 in in HI 11! III 111 Hi 111 111 111 III Ml 111 III III lit III 111 111 111 111 HI HI in III III II Ul 111
o a T *t •f LO n s 8 SO in in co (M f- c-j CO * 1> co iU
M F \n iV O) CD CO r-- o o co CM CO CM ^ O O CM <£' m Cvl U> CM Ol OJ iri CO OJ OJ CO CD *Q CM CO CM N *" o
o co d
CM h- CM On En
CM ED • n
OJ IS C-J g o OJ N. CM
OJ CM CM CO CO
CM OJ in IS >1
CD K ts i co
O a H
o CD CM §
o OJ
O CD
o CD If)
o s in o
in en 1^-
m CD no Si 8 CD 0) 5 N CO
CM CO 3 8 <D
3 p 5 CO
O CM cv
1 CM
X
X >
o
ill
00 5 CO
o >. a o U in
a) •D
o en c
"8
(%) Sujumiuay juaBv
5! O
S " - S i < o
^ E I" P _j
B5 O
o Si 3 M- CO
•• o o CO CD z •£
ore •• - *- r1
| |£ 1 I I rB % c ii E g 5- o u
c I 6 E o
a 0 Eh E 1 a n1' «
EH' m
2 14 > n I < < u ^ 1- .^ H U
o ro t- +-• c <u o c o O o Q ro >
•« O
6 8 o o d
£UJ/6UJ ui lueBy
APPENDIX 44
a.
s*
UJ _
CO CO
QrtcotocDfyootncMOKy-cNC'ar) cOC\jincOCMC>J»-»-»-»-OOOOCB
'•'' lii in UJ iu ui UJ UJ m UJ UJ U'J ULI iii U'J i:/ in uJ ui lD*-^t3ph-OOCDCOt-h-CDO>'»<DO'T9> iflV«rtNONrrqa)«(Dr-lft5*N
APPENDIX 45
a.
NflT-vmii-OlDibi/ltWCO'JNfflOOCIlCDh rlOOit.-OlCOlO
oioioii}ieDCDa)SsSN<DU}(OiD<cininiommi/)U)mini/)inmmm
S?8S8§8888888888?SS3?S88SS8nS UJUJIlJUlliJUJlUllllillUliJUlULlJUUJLUlLlUiiJUILJlillijUJU
cioi'triDicci'jircoy vrioorir^r^r irioi^oioiT-'iriiooir-'ri
APPENDIX 46
Bi as
t 1
F S
* c-°
QO)*0)U)01ID(QCOro()5COID(Oa)(t)IJ)(Dffl(DCDCDK)
PtR
UJUJUJLUlillJJ^lLILIJlULULUWlllLlJLillilliJlJJUIliJW 0»-OI)iOWONI»NWU)(a(V*W(MT-WNU)NWiflNO»5ir(MW05
o c\i co tn N
c\j v tn r--
co o CM co SS CO Q m CM o
8 <M CJ co m 8 8 S
W CO ID S N CO — in CM
cO a> CO CM CO CO CO
CD in CM in i- r-.
(N CM CM
inC\JO<PCMC7)tOCPl0CD
ojcMcococorotoco-^ •*
X
d X >
o o
8
o CM
CD •D CO W
(9 en c
Q)
£ a c o
3
§ LU
(%) Buiuieuioa tuoSv
*- «- O)
_i g1 g> 0 _i a. E E V u>
81
Rj
* T z
5 w " >
I i 1 ©
5. 5 e-
S i
111* & 3 1 °
s? 'B i? JJ
% **! Q I- I- Z
f I m "5
«- ? F • v> — c> O •g r r c ID id m '^
5
l a o « z 5
tj O) Cft U> ii E 2 g ^ o> <D m o > > > u < < < 5 £ 2
c CD o c o o o Q.
>
-I-
c^ °° o
4 •
«•
oE
• •
• •
s ) Q ID Q tO O j CO CM CM <- T-
18 8 8 8 8 ) o o o d d
EUJ/Bui Uj )U86v
APPENDIX 47
05 a
It
II
8 en 3i
5*
Cvj 0) Si
o9
m in
s N CO
a
i cu
i So
s N CO
^ N
*
Q CO to « rt eg « CO n CO CO CO
*~ i- o> u>
fc fc to m in m in m t^ N. s i-- K r^
o^ 5s 3< 3^ S* &•• &-• •- y B a s ® w in ^ co co co CM CM
in iri m uj S N h- r^
N W N N iri u> iri iri S S N N
concococococococococococococo^giv^ininin cpooc^oooooooooooo^ooooo lit III UJ UJ LU LU UJ lij li'l UJ UJ UI IU UJ UJ LU Lil UJ UJ LU UJ LU §o>cvi'*p(Din'-QOcoa)OKc\io>NOT-co>-ai
tocowwcMomotneoh-Tto^fcoco^cDcocDcD aiNUJNNPJriniNOiNVT-'r^cipi^T^O)^©
m m m m to m co o o o o o o o UJ UJ UJ UJ UJ UJ UJ
to in K oo O CM CO
S u> w o " r- co m
s ? 9 fe S CD CO
CM CM CM
8 ssnsp: t\i o N w to c5 (O 00 O) E 89 ffl
CM PJ CM <\l CO CO CO s
s <7> o s s & ID
1^ SI CO IO * <M ^r n *~ •*
CO 8 8 CD B O •1
CVJ
C0 CO o
iT)
CM | 4
• 0
CO
4
in 8 in
CVJ in IM in
(5 X >
o o
o CM O
| CVJ
c >. Q. O o in
Q) •a to k_
O
c a
•D O
ai
1 a
m
03 Q
(%) SuiujEiuay iuo6v
8
a §
I* 1
to ^
< 9
o E
a E Cp
8 in s CO m Ifj
^ n; ai ifl •^ ^ ^ 5
CM CM ^
If 8 &
I §
& s
| 2 8 6 to t o <g o Z S O
ro « « > > w < < o
11
9 I IB £ I o
c <D O c o o w o a ro >
I
4
8 CNJ
^ •
4
.<-
• •
O O Q Q O O O h- go in 5 to cvj i- S 8 8 8 8 8 8 d d d d d o d
EUi/bui U| luoby
APPENDIX 4S
Dl rO
It
3 I
II
o> a> a> co 3 co r- NNS(ci5(t(Dinininii)i/iiriifl
?J $• $ a8 g> *j- s m ft -- CD N
88^8888888888888888883SS3?cS33S '''lUliJUJLilUJUJUJIilLlJUJUJLUmUJUJiLlUtiJIJJIiJtUlU
o>oJrtF-ipcoooin»-NO)inooa)5<Dv-ina>(or^ (Oooco--o^'N-h'f^^*^'»-i*gOTtrttDU)coco<NJo)
njuimiiiujujiuiuiu OD m to v in o> M- cJcdiri^Winctivi^ nsn©N>*wwnirj'-oi(ON'fNin
3 -rcoiflwcdifiwcpiriNqjiniriioiotb o in s ft?
CM v m r^-
oo in w n in .SPSS..
IN w OJ w w co en co ro to CO
5 X >
c o
o >1 c c O
I E
•D TO o 5 2
s
< u
a. E
D E p 0.
05
8 in N S CD (O in s
;* #
> s o
5 3 1 ra u i * a
F a E
en ra j= p v, a & * 1 B 0 I
E CO > <
V) > O o s 1
&• ro
s I I 3
(%) SujUjeiuou tuoBv •-s •* -5 £ p £ O Q Q CO (0 ^T
1 (•- - 4—
S ? (/> C
c o P m rx •- c c s c
< 4
o o l-
o 1 a. ro ro > £
Q>
t •
4
• «
« •
« • « •
« • •
•
•
eo o o o o 3 PS CM •- & Q O O O p o o o o 5
d d d d d d EUI/SUJ U| luaBv
APPENDIX -W
X CT> a a
3 |
en en
* £ h° rf tf r- o" n° n^ ^ r? :<i =5 „- Si co s 5 % ?> ft o
u-j S3 E s <*> a 8 r •
•X) CO f: S s 18 <£) s <3 in 5f
5s i8 <? ? »! *l 8? i« S; ^ p? ^
UJUJLUUJUIUJUJlJJlilLlLlUUJLLJlililiuJtijliuJlULULUli
COCOlMtMcJCJCMOJ
R b !0 0 S S in oi p) s ^ "! o » ^ w S Ul »- io co o> • !£
8<M O CO S if) o •»• S l- IO
(O * I N W S CM cu CM co co co
nss S !S R f:
(0
6
o o o bo o
o a> o <r> o o CM
o >, o.
c "53 •D O 2
E E
5 a, P TA P
E a
TO w 3 o i
*^ % <s cd iri *- .- cj ^" •- *-
£ a
(%) Buiuieaioti )uoBv
o« 3? 3°- i« O Q O O DO w *r cy
C 0) o c o o o TO >
5? ^ CO GO CO CO
•
• •
• : • <
•4
• « • « • «
• + • «
«• « •
« • « •
• « •
" — -I—
8 8 o o d d
o in c\j *- o o d d
CUi/Bui ui )U06v
APPENDIX 50
I CO
Q.
5 I
II
to eg CM r- ^ S? 5? 3S o> co *- co N m a) 01
SSMUJCOQh-OCDON •^eootBocoNOTi-io
iOrs»(MQO)ON({)i ^ co CM ssss
UJWUJUJUJULJlilLJLlJlil cOS-CMi-Q<pincMl--^ O>IOOCOOOJCONCOCO
CM CM CM CM CM o o o o o s NWNNWNNWOINWNNrtPl o o o o o o o o UJUJUJIlJLlJLUUJUUUJUJLJJIlillJliJIiJLUUJLlJIU
m r^ »- m CM -- <p to 10 n W oi 45 oo oi s a O CM CM r*- r^
CM CM CM CM CM CM
M 8 S S K " S S 5 S
m o m p m 8 8 § 2 CM r-
to to
i". r» en o CM
CM CM co m co JTI o> to co o r- "?
5 in O) m oi "
o x >
o c co
O I
M o o CD a o CM
0) •a is k-
a o> c Q)
•a o
1 O c o
3
5 UJ
TO Q
1 E ?s> Si 2 - 8 6 8
.- r\i ^~
o
I c 0J o c o o
5
(%) 6ujU!oujoa )ua6v ^p .J> >fl a* d* p O Q O CO CD 5t
1 1 1 —1-
•• t:
V / • •
if P
• <
• « * • <n
8 8
Eui/6ui U| )U96v
APPENDIX 51
0)
03 0.
!£
i I 3 t
11
S? 3? ^ S* ^ $S Ol lO © T- s * O) lO i- *- i- •* oi oo <b co d K 0)0)01010)00
£ K § o> m m
OB M r TJ ^j- CM to r*
a? g? 55 a? ID 5 oo n * (O W N
CM O O) CO P- xO vO sO
S fc & 5« * * P ° s
00000000000000000
UJUJlUlUUJLUlijlJL^llJL^LlJUJUJi^UlUILUlUl^UJUJUJUJlULUUJUJUJ^ ocpw^r^tDincDONCo^rineoNfoor^(DtDcy5P<o>(DN(Oc\ico oooou)to^NNtqr^coincM(0*r^CMOocDOcMCoo^uiGocoino>
ujoiioiot'vciwoii-1
COCOCOCQCOCQCOCO s N n rt 't 5 in in
cocoNiom^TcocM
v*5 co m f». 00 o CM
* r « ID n Pi «i to 03 6 g to <£> tt cr>
co in r*- 00 o CM sn? i-oiWif)©wmi»
m to co o> o ST- h* •* Q K < «
-* -* in to «> t-- 06 CMCMCMCMCMOJCMCM
co 3 CM raQN CM CO CD
X
3 >
+
CM CO o
CO CM O) o CO o o CM
I E
i- 0 0
3K
CM
SD
/28
/06
tf) 13
CO
c £> S
E
• •
! CJ5
c .2
LU
CD
n Q
-1 E E O 0 "-S * „» 8 0 g
CM K T z r- Rl S < at IT, 5T
a U
s * E
c o E
! 11
§ f111 1 £ * ft I
JL i 1 1 8
£ a.
I O HJ-_Z Z
E i £ «
b iu o S O
e s > O O
5 2 £ 8
F O
(%) 6u|LllRlU0tJ JUOfiv
8 o
—I- 8 o
<
•*
•«
•4
•*
•«
« •
• • c
Ocii
- •
• *
S 8 c odd rjiu/fiiu Uj )uc 6v
APPENDIX 52
m 01 a a.
fi
fit
3 tf^ av tf*- 6-
, CM O) *- Oi oioiJi^nNnio
M n n is ci « a a) a) N N io 8 8
ft ft K ' CO N (D i S' Q N «0 ^' 0) W r
ift ^J "tf ^ T •<* "tf
offlnnnnnwnnno
umojtLiiJiLiiiuJUjiijiLiuijJwmmiiiiiiiiiiiiiiiijuJiiJiiJiiiiiJiiJiiJiLi iAcpcZico^tnnc\J^^ajT^u5a>rocnr^coS
O) o 8S§ "v „; in m ID *D
in o in o m J u5 m
(0 CO CM CO
in o in p tp h- m f- ro a> Si o» to co
~ C cb yj CO N PI
8 SG CD tD CD CO tO i" N A i- (O in oi to r- ta w O) o
OJ M C\J CO CM CO CO
CD I
X >
o o O i o
CD O
o OJ
o >. o
o
(%) SUIUIKUJOU luofiv vO -.O ^O
cS
0) T3 ro I- a a c ai
•o o
a en 3 a C3
CT>
E C7>
E P 3 B 2 ^ CD 8 35 £ s < CO tn
T BO
3 0
£ c3
f
It
s £
g
| 1 in 1!
i > *
£ o 5* fli 1 • 8 a 1
1-
to E £ o 2
CJ O 3) CM »- t- i- •- »- Q o o o o o o o d ci c> d o o d
fjui/Bui ui )uabv
APPENDIX 53
a a re 0.
I I 31
6 f Q) 3) a ft CD CM
iff ro 9
3?
3 ,0
5 in CO in
CX> 0 CM to S o in
Q (O CO
CO n CO
ID O) i- CM
O CO CO CM
&> a to in co *- s to cp d ID W W N W W
to to io m m >o, «n tn in N W W W N « « CM CM
S8n^8888g8g8cJ88S83S88S8S8888 UJLUlljlillijliJlJJLilUJLUlijlLuiliJlLlULjJlLuJtjJllJliJlL CM*ti^cDino«)cyco(D^i^cMcyo)rOTfcoin«jiNoQ,~o5:Sooo
^CMN^^cicMT-ffl^cOTfM^cnrtOJ^SqwoPoooo CM w CM •- *- i- CO CD CO CO *- to 1^. o w CM o o o o o
m o m o co do o> a
•^ io ui uj io i/j ^- 2 TTi ',
m in ID ID COi IC'CD id (O
5 r: 95 NOW S3 $ 8
IT t a; c\J eg c\i oi m S OT
d i
X > ro
o o o S m c
CO
5 5 o o
a o O
"o E a C
"5
% E a c o is
(%) Suiujcuiay ;uoBv
O
3 tr
u
a en M
8T- CM t- O m CM m a
CM E *- " to ^j-
co m z "e CO CO
> ^
I
if *ti
£1
r
& c a> _ a w UJ "5 cl a) « I & I Q (- H
E ..
B E 9 *fi
5 5 5 5
.5 * 11 5 oi
1 1 ^^, £ c
10 c c ra 0 E
i" EC
c HI < o f- 4 o o — o
£ *!
Q »- ro C0
> 1
£ • i
« <
I T> CX *1
Z 5 O
o ti t) i oi o> n * ca co re co «) <D © r? > > > O < < < O
1) F n
o I 8 E 1 o i
E E
9 1 s > H 2 i- o
• «
• «
*v
8§
8 a 6 o o
Ciu/Sui ui IUJBV
8 S o
APPENDIX 54
nj
2 g
£ E
o U> O E
o»s«rODioONinrT-p)(ciiooi««)Ni{)i))inweD^CDna)W(o oiroroffl^r-'njiorN'^wdtsN^ffliQiQiriricijwoi^rQQoi
UUJUllUUIIIIUJLiJlJUllUUILLlUUIiUIUUJUJlillilLUUUJUJlU
^^'T-'T-'^'aJodcDNTOcbajh-'i^ioaicdodi^'r^r^isIi-s!
i- r^ r- aj N o o T- ^ r CT> C\j Ol Oi W IN CO
-SSS8SPS»SS8S ^-'•••'•W'-OWNN
w n 10 a> ' (0
8 O) o» o
l
APPENDIX ss
CX TO £
si
, eh O E
I I
iissp a> •<* «o o W r- CO (O
55 3* 5? SS 5? 5? £ m co n 01 co r- w en co to « © »- n s <^ p~- «f- o fc *b
C7) CJ> CO i t^Tl^DfOrtCOtoSlNfiOJN
'' LL111J IXJLUUJ L1J UJUJ lilLillllUJ OinNOlCOONUoilDoB
LllUiUJUJLULUUJLLIUJUJLLJliJlDUJUJUJLiJ
^ri^T^^r-' r^oioioJccicci 3 to
lOcDicuiuiinidri m n w M N d
OJ N OJ N CV
SCOtOnCNJCM^CO© (O T- a> N If) CO 1- Q) viomiONCocftO) s^t Ri a s 8
o X >
+ +
C\l o
CD O CO o o C\J
•a
2 o en c
"ai T3 o 2
1 c g 1 TO >
LU
TO +-* re Q
* 8 u i
• C7> C7>
1 E £ 1- ft o) N
3 oc
< o
c s? 3: in co o
CO cq iri iri
s afi ~P J? ©^ tf* ff-
& S
I! a* K I1- €
i» | R I b 1 3 | E |D O
E E
5 1 ^1 U
t- U K 1-
5 .? a. o
rt '<3
8 8
<4
' , . f CT <~ </> c
c | 0 > fc ro cc
c QJ 4
4 0 0 S!
I— 2 0 •s n H ro (0
> F
P •
1 1
«• oE o—
p
• « • « • « • «
• « • « •
£ 6 g
JO 2
z z 5 U < < < o
S 8
CUi/Bui ui tuoBv
APPENDIX 56
CD 3 Q_
< I & s
$ Tf (O S 0)
CTI a> v) oo
Si 3 i-ocor^m^jcvo
toSStowinmin
3S38888o8688888888888888838S8S LUUJliuJLLJlUUJUJlijUJLJJUJLLuJUJLLJliJLUUJUjIUUIL^ 0iu}0)r-NtfQi3)(DNpia)inrtNdi(Dt{»(5g)O'-iDOT-<i.-!:m 7rtOS»lfl»NOINS'-WllSNPlOiflSi!li)lrtN3(CNK(,)(5 ri o rf <«) to ^' n ^' ^ •*' ri COCOCJCOCDOJWNtOCiCMCMCNJCVJ'-
s»«0 8 8 co ao co co <o
8 $ o> ^ ;: ^
COCOODCOCOpttJCOCQCOCOCOCDtr)
iniriuiuiioirjiriifliriiriiri^cflj
j w w (M rt n *- e\j co •«• to to to N o> p 8
(%) Suiuiauisu juaBy
„5 O
I X >
I i
8 E Q O
D. c o
<D •a 0!
O
S
1 a c .2
D) CJ> ,N
E e P
38S
« •
« •
? • « Ol
</> • « l- o 1
tr • « c a> • -« U> <* c o
•4 *• o o I «• CL • > 1 • «
F •
• •: • •4
• 4
• 4
• 4
< •
«• 4 •
•« • -•-* • , • , , ,
8|
S o o S 8
Eiu/Bui ui )ua6v
APPENDIX 57
CD O) CO
Q_
8 I
1 ? i! I
&iicint1'0»^i;-<!lso)cpNnS)ci)CoNrNO)CJO(Dlbni35m w«ion(OrN(ON*a)(Dcii'-a*Nwcn(iicOf-oaiNiBnrtO(D dNirtwgn^cowfflt^^on^oicoNKNKNcoioibipwictifi CTicno)0>ooaScoNSuJcocDi/5iniOi/)*'t'*'tf^^**VTT'r'<j'Vf
8SB3S888S888888888Sc33§3333<53<5<S lUUlilllilLlllllLuillliJUlU/lUUIliJULilLilUUllJJUIlUljJ^ T-T-a>tnocnocooocn»-cM3io«-toa>QCO^ ujrtWfOJNifi^roS NOiBOiomNNN^WrtT-IDCIin5(00'-r;Sfs®^lO|''N,f <DaJ(d(fliD<Da>iri^i:^^cJcot^c\joi'J^cocJw<y'-:'-;T^\-^^:i-:T-'
N N f- N N £; co rt •* -* o d o • b 8 8 8 ,. in in ID to _
K in <*) y- o o lnr*tni-i-'-i-i-^OitMC\l(N
SS8 tO i£> OJ C*> CO (O
T>
o m CO ^* Tf *t
9 >
3 + a? 0 o
01 5
c & o O
a
&
D) £
o 5
CD c o I
Q TO u S
_i P U) 3. E b
5 <- rr <
n g a; CD
en
S5P 3 8 3 S S
I i
c E I ft. | E jS 8 8 a
II
lit I 2. « I I s 6*9
G 8 « g ig * i C d qj O _
h- £ Q t- \~
I i 11! TO OJ
•a (Q
l "S tS I? E
t c
en s
I 6 < o 8 4
•2^5
(%) Bu UICUJDH IUSBV
6? o? is? is« o o o o 00 , CD Tt OJ
1 1 1 h-
c CD o c O O k o a CO >
8 3
* 4
•*
•*
•*
•«
<
•4
•*
•4
< • « •
* •
« •
4 4 4 4 4 4 •
o g
• «•
! 4
8 o 3 S
pjj/Eui u> ju.ifiv
APPENDIX 58
a 9) ra a
? E
i t
& N 6 oo co in r- <c co N IT) (0 cb ri 3 (C ^ 3? ^ oo a> (D £ 8 •* CM O
u>wcnu3coc)NiricgQC»oQoococDooKKNh-h.N oDcor--r^h-h-(DiDto(oioini/)iOLfiininininininin
888S8888838888838333SS3S333333 LJ LU UJ LLJ UJ UJ • LU UJl^^l^UJ^I^UUJl^j^t^LiJL^l^LlllLlIllUUliJI^UI l\J O)
CO CO CO 3 CO CO
Sw o a> g> m ^ O) o>
to cocooiwwoicdco"
1/1 S to ^ co m CD CO CO
OJ CO 8 OJ 8 ifi
m OJ
CO
C\J CD
3506.87
3643.58
3780.30 s '6
8
CM
5
6j
APPENDIX 59
a a n
D_
c I o m O E
Zl
^y vy ^o ^o ^p ^o vp IJ- tf1- tf*- S- tf- tf- d^ in 10 m in w ui r o) >t in s o» op co oi O) co s <b ui ^ 0)0)0)0)0 0)0)
N.O vO »o o- 5^ o* CD S r* r^ oo o
>slsl4tf^Ji0rf)fi(^4^il4d!44 SWrngiNSOoiyinNinoifflNNt
OlfCONSNtO^oiflWOllOVNCnS NrdoicftoNSiofflin^uJV^tSrtfjriww O>O"><7iCQ<0c0G0COCOCDC0C0 COCOCOCOCQCOCOGOQO
CM CM 9 9 LU 111
CM CM CM CO o o o o LU til UJ LU
Si
CJ CM 9 9 88?
uj li UJ sssssssssssssss
UJLULDUJUJLIJUJUIliiLLILJLiJliltiJ
i- CO O CO coh-o)coomior^(^ v to CO t- CO O O O) JO
i-WWCJNWWW O) *— O) CD O) CO O N
K. w o m s s £ N v T- cq in 2 N K S O) oi • r~ <M "^t lO f-
S 8 fS a ^ t
co in N co o in s s (o
s s s Q CJ in r~- CO CJ
U*) CO o y~ -g in CM co co co
8 co n T»
m r^ CJ N -N N w s t in m ^ to s T- CO CO CO 'iO CO CO a © s (O O) n 5
*t-Mul'-a)(ODO
*» •* *r i/i m
(%) BuiuiBiua j iua6v
(3 x1
c\j o
0) o CD o 5 CM
O
>. Q O 0 CM
XJ (C i_
a a c a3 TJ O 5
4)
a c o
'•*-*
fC 3
UJ
a a ;; o g o
2 >, ffi fc
1 i "B i? k
o t- t- r z
3. E 05 E o
2 • IT <
- O) S & o> CO s
APPENDIX 60
1) en a a
5 f
II
ill 8 8 fe iT) <J> (7) CO CO
•J •? i9 -P v? \° -J 5*. $•» (p *» 5> 3~- S^ w ?? r* H E II *" rr ,f TJ (D o 1- N
S P f: pi fc £ fc t£> s m <D iri t to to (5
s?sa§
858888838888 LUUJUJUJUJLUWWUJllJlilUJ
T-cMcoi/it^r^^'S'-Nifln'-rtoamr- oj<T-owwo3imoifiiD'-iMiSNw
999009^03 UJLUlllLLJLLJUJLLJUJ 3 r; W W "D ^ '
S IO IT)
S8SS83838 111 W LU
8 8 2 W UJ LU UJ uJ
o»a>No>Niomu>ipi/>co^ •* co •<- a> c> •«*
mom B fc 8 fe « S S 8 S S R £ 2 3 g
co 00 to 00 co co co
co o CM o a> co m N m M (c en in 01
co to cri 8 8 a a a O 1- CM OJ
o X >
+
co o
5 (0 p o
I O CO
II) X!
2 <5 C
OJ s 2
to s 5 s o 2 a
t.
CJ) Di E E O O en r-* O CM
10 •D to
CT) 00
o> 00 O 00 <J>
O O IT:
aJ
(%) 6uiuieui3u IUSBV
o
'1 8
$ a c </> r.
c 0 P ra DC
i: C '
0) S1 0 c < 0 0 l- R 0 3
a r-
ro <T3 > i- H
•
•*
•
4
• •
• •
« •
« •
• « •
•« < •
• «
li o 8
£Ul/8ui ui IUOBv
8 8 S S
APPENDIX 61
m a m CL
3 I
I!
o £ i-WlirS(J)0)W01lDr)rrNfinO» ., 1 § $ I i I
^0»tt5)O)O3a)(0SNNS|s(OiO(fl(0<OIO«iffilDl0(O(D<O(OlD(O(fl
00900009000009099009000000000 UJ LU UJ
0 to 5 HJlUUJUJUJlJJlJJlIlllJUJUJUJlUlUliJUJUJllJLiJLlJlilUJUJ a>totONa>cooioJOcomcoa»o}u>mtOi-cxjcOioio*i er)eocvi^NOOcoo>ooo>WTi-5St-OT-»-'<f^c»io
NtJi^r^f'T-' oioi^aitfisttiioniw*
U> GO co OO
S S S £ R fc S fe S! S; P £ ¥ S S t S S S S 8 R a> 03 co ~• O CT) (D
? 2? 8 to CO to 00 CO
- CO (O l/l S CO O)
M r ri ffl Oi tO CO O N
" in in •1- N CJ CO xj-
ai IT) ol CNJ -'
R CJ to 9 co 8 r^
h 1 C7>
S CO 0
(%) Buiuiciuott juoBv
C5
+ + to
8 m us 8
01 O
T3 TO k-
CO
0J •D O 2
4 o c o
'1?
8 a
3
E F 0 _i a £ # S? 2 *- r- ,- 0
0 OJ .0 10 o> <i r- < if)
UJ OO [JO 9 0 CO
< u x >
I
s 6 1
s 0 I Q
c 1 Q
e 0*
6 7) a a
9 1 > 1)
V
H e 1
TO I 9 | 3
u «. < < U J> i-
APPENDIX 62
0)
ro
£ £ 5 I
a 10 oo to n Q o> CT) CT> £J>
m m
8 R
s! «? s£ s s a
5? # -? ^S ^? S^ 0> 6^ to ^ 00 ^ (O CM
o o o o o o
<D m Tf to «- o o> T- T- T- V* «- «- O
dddodddodd r*. rv. h- N r^ r^ r** N N S S
SSSSSSSS8SSSSg3883383SSS3333S3 UJWUJlLuililUJUJLIJUtLlJLUUJUIWUIUJWUJUJiULJj 8g?cNT-h^Smoo^-cM^ina)(^mof^<J?<POJ^p^a)tpr^cpr»jcD
ooOinto^^r^CDKtoincsitOTrr^cuoocoocNcowSOTrJina)
K 8 •- CO iri cd 3 8
8SS 2§s
IT) t^- CD 8 S 3 S fc cd d c\i
CM ** in W (V w
ssnss 8?8SS ?> <2 CM ^ m CM CO CO CO CO
3 X >
+ C\f re a
CJ) 6 CO o o CV
o O to
, D> Ui ,-. _J 1 e e 9 « S t; 00 O O CM O r- •* Z cd d to a)
S r V
n 5
|
n cji tji ^ (71 oi
CM CM
(%) buiuieiuay )us6v
83 Ofl) tNJE
o
« •
S;UJ/BU ui iuc6v
APPENDIX 63
0J
(6 Q_
i t si
II
^ S? S8 £ £ «3wc^r^oi-o>^co^-cO(O*-cJc\jwcoo«jT-oooooo>'3>0>o>a) ,tDmanSOjlOO(Ori«l(0'-0>a)NSSNNSNNN(DlI)<D«)(D
^oioio>(iii7ioiO)a)0)i))Acbo)0)0)oioio)a>ino)aicncnai'3)0)aio)
990000000000090000000000900 111 in en
LU OJ n
m r-- 0
LU LU LU CD OJ
w 8
LU r- CO
LU LU O OJ
a> LU
s? LU
CO
LU OJ ft
LU
b LU
a. UJ
0
UJ CO m
UJ
s N 8 8 IS LU S P LU CO
1:
to UJ
5 LU
5 LU CM
* *~ •" «• •" *" *• •" h* O) re •" <0 LO CO *- *• v CO «\l oJ a> »• - in O- to *• OJ -*
8 ni 3 LD rs a R 8 to -r
i-~ CD S CO s CM in in ffi r- H 1; CO 03
OJ s 0 OJ
P. ? s in i iri OJ OD
CO 0 in
ni G) CO
CO r- CO
in S OJ
u
Si a, H
OJ
t-
£ 00
f: O Cl
O ?i
in
n 8 OJ 1 ?! 0
CO
<-o
CO n CO
CO
Ml x d
>
+
ST CM O
C\J CO o ID o o CM
(%) BujuieuiOM lueBv
o •o 9 a c ai
•c o 5
C5 c o
'•s 3
> LU ro (U Q
a
5 »- O) IE < CO < u
E E O _j '71 O
S £ N •* CD CO
0 2 OB CO O CO O)
* • £
« I il 1
Iff III 3 I 5 SEE U 1
E if
e fl 1 I
» O Tj O O) F W s 2 2
E I £
APPENDIX 64
CD
a
& f
1 I
£ £ o" f ? d^
SN CO N P") *"" (Q en O) CD S N to
m b- O CM <D OJ « >* •* n w w
o>3cgcocMcocDO>cocO'fr OJOcoNcqinM;cococMCM
CMCMCMCMCMCMCMCMJJ
CO CO O N
CM CM CM CM CM CM CM
oo555555o5o5SSSS8SSS888883SSS3 LLJLXlUJU^lLJWtUlUlUWWWIJjUJlijLJUlilUiL^ r->mO'-»-rtioaitDCM(MODT-u?cotf>Q»-ipvior-- lo^nocptNr- NioniiDSiOTtnnoi'-Or-TfsiD^piinroliD^rtoooioeov
CM O CM O
s 8 g a £ ^ CM CO •* CO
8 EM 8 8 S CO r- f- m to oi
«J N $ Q N g O) CD 00 (O CO o CM O) CO Q CM 10 CO *- LO CO 5 £ t | g s a M- 3>
CM CM
15 S § CO CO 5 CM CM CM
Sin N § o Si N Oi N
T^ © If) f" (6 lO O CM lO h- W V ID CO CJ n rt rt rt Tt
3 > 05
I I
+ +
o
(». o O) o m o o CM
O
EL o On C\IC
0) i
o
O
TO > LU
a TO Q
(%) Ci.iuisuiaa lueBv
o,
^ >. w S "1
I | ~ LU O
f iI* i §
4? D E p
s- - <
- o> g Cs) In
09 CO O in
CO
Cui/6m ui |ue6v
APPKNDIX 65
10 O) CD a.
sf
yfi *Q _0 -« £ £; °" £ n n r v CO 0> CM CM
N? V? N? p fc £ O tO CO
5? 3? S? ;£ O) C7) <7) -i— cooooco'ccococo^oint-cnco
Ol CO N IC(OlOlflU7i01QlQI/)V)IOIOiOiOiO
83gSSB83£!888888333S383S838;$333 iJUUJUjmaiiJjujiitiuiiui^iijiijiLiiiiJJULuujuJujLuti
~coi/}^^QtMCOCMO)T-oroo)^ingrtgcMino>oocMr^ IQCOCOCOUII-T-QCMCOCMO) co»-,*cocScooo,SrOT-u)(D
oii-Kco<D(jDO*e\ja>K •<tifi«min,«riocMco
.? £5 t» « c£> o <s iDNini^nN^maNioof
vrotco'JOJt'P^powiOrt coco^-rfuivntotoSScocooi
if) o w 5 *- CM CM CO
is a . g 5 8 8 3 § 8 8! o o o - *- — o> O) ft ii ^ ^
CD
>
+ +
OD o 85 o c CM
o >. c c o 1*
4) XI TO o c
s
(%) BuiuiEUJOij IUOBV
s« s« #
2
1
s? a E E P _1 O
- o> K o CM O <D CM
< a
0) CO 8 8 d
u X
2 •£ S 3 >
I S 9 g
> g
1 a V h i Q>
O E * E 1 F -c
1 n
o
9
0 r. 6
1 B CT; HI 5 9 1 s •> W
< < < o -?
I e
fr ro
8 g X 8
£ 2 1= O
8
? o> c
l/> c c 2 o I m IT
c ft- <D < o c 4 o O SI 8 ra ca > §
:£ 1*
I • 4 •
• •
• •
• « •
« • « •
« •
« • « •
• <•
g 9 O O cS O O O O d d o o d c> o
s s eui/Sui u| tuaBv
APPENDIX 66
6
*i
8 1
II
r*-oe*)oOTtOh-mftMSoicooo3 «- i- maJtpvmwQojcDNiririNT-'rioitD OjC7!(JlOilJ>(J)(Jl(DCDtDlDlfl(D!OIDNS
C-" o - t * Bfi s •*r nj m rt (\j a t£ U) in in m ;« iO jt TT h- r~ h. N r*. N
iiiLJLiimujuJuiujiJiiidjLiiujLijiLmiuuiLLLumiiiuiUJUJUJiu
T- r- 01 01 00 P- N- (0 S N i- IO«tP)(0r©l0n«W
KSnPS^rSSn St5SSS£8^S Si
I- CD 8 8 3 N O lO o (D N N (D
SO lO Q Oi Oi o
if •>* *f U) h- C\J CO S SI
1 o c o
S Si o> Oi I*- Ol q w ID Oi CD O
s II _l
w o 0^ c? 8*
^t 3 3 ? OJ CM
Si 8 o in
M
(%) Buiuieiuoy iuo6\/ s? 6* a?
o
l I 1 cn 3
E °
c B E
|
~ § 2
* 5 1! E
E Ot ^
• a '£ g
6 IS Hi III'
i
I
4i <<<OSI-2HO
I
"8
•
CUi/8ui ui luoBy
APPFND1X 67
a>
m o>
o^ d*
S 5! CO Q
C) IO 00 Cl O) S
ri j* nC „? tO
CJ a <n n K to 3
^SrinrW't«PgNr(J|f)i-ftrffl K(0»-tf>OOtNJr-COOtOlD\n(MQOa>
S'wQ^iriwoiiiiwoJs^Qcicldo) tbtoinioin^^-^cotococotococON
UJllJlJJUJlUUJLUWUJUJUJLULlJWUJLUWlUlllllJW 2NNQrtOinO)N(DIO(7lOiaiC!)NO)i-N(DW(CNQNrinN
NNriNdwNW«W(\iSr^cJ<\ioirNC\ioiNWOi'r('
Wkftl^Nf-CJinOlOWNNNCJSNN g£^tminio(DNScoooo)0)OOi-T-
•»ri<oritdricdricdrtc6 ' (O Ol i- -f <o <J>
T- r- CM DJ CM CM
if) N W i-
9 8 Si g 8 * ca to CO 4 m c r* * CD CJ> 1- ^ en rt o o ^ TT
cMcocomaioOrr;
CD c8 T- Oi « N O <J r- K 03
X
o X > CO
+ +
K CM o
CO o C7- o CO
8
O O
ffl XI TO k-
o c
•u o
(%) BUIUICIUOH IUOBV
c tt) o c o o o Q
i E E
<-> § cO O if CO
5
_n; CL
<
h. CO CD CO </J CM to ^ CM « 11
:
•
« •
•
• • «
• « • * • «
• « • <
• «
*• . .
§|
I 8 CM
8 j? S 8 o d
Ciu/Sui u; juaBv
APPENDIX 68
