1412 J. A. IBERS, W. C. HAMILTON, AND D. R. MACKENZIE more negative values would apply to the less shielded cores. The presumed minor importance of the 6s orbitals in the bonding would also be worthy of quantitative investigation. Such refinements would, of course, substantially increase the size of the problem, and they would be expected to result in only relatively small changes in the energies so that the essence of the present conclusions regarding the structure would remain unaltered. The Bigs+ species is evidently the first example of a homopolyatomic cation of a metallic element that is sufficiently stable to exist in a pure state, excepting, of course, the diatomic HgzZ+and CdzZ+. It is interesting to note that this grouping may not be without analogy, however, since it is isoelectronic with Pbg4- and Sng4-, two (of many) species of the post-transition metals for which Zintl and co-workerslg found evidence in liquid ammonia. This relationship has also been noted by Britton.*O On the other hand, no evidence for a bis(19) Summarized by H. J. Emelkus and J. S. Anderson in “Modern Aspects of Inorganic Chemistry,” 3rd Ed., D. Van Yostrand Co., New York, iV.P., 1960, p. 512.
Inorganic Chemistry
muth analog of P ~ T the ~ - other , lead anion suggested by Zintl’s work, has been I’ound in the BiCla-Bi system. In addition there is no evidence for any comparable, polynuclear cation of antimony in the SbX3-Sb system,z1g22 perhaps due to its reluctance to form cations in the presence of halide. Compositions corresponding to the many species suggested by Zintl are generally not found in the binary alloy systems although a few isolated examples of other homopolyatornic ioiis with “closed-shell” 110’s may occur in the latter.2J Coiitinued investigations may well disclose other examples ol such ions for the post-transition elements that are commonly thought of as metallic in character. Acknowledgments.- J. D. C. is particularly indebted t o J. \V. Richardson for the overlap computations and to D. S. Martin, Jr., for helpful discussions. (20) 1).Britton, I J Z O Chem., V ~ .3, 305 (1964). (21) J. D . Corbett, S. yon Winbush, and F. C. Albei-s, J . A W LL‘hem. . SCC., 79, 3020 (1957). ( 2 2 ) J. D. Corbett and F. C. Aibers, ibid., 82, 5 3 3 (1960). (23) J. D. Corbett, to be published.
COSTRIBUTIOX FROM
CHEMISTRY AXD NUCLEAR ENGINEERISG DEPARTMENTS, YORK BROOKHAVES XATIONAL LABORATORY, UPTON,SEW
THE
The Crystal Structure of Sodium Perxenate Octahydratel BY JAMES A. IBERS, WALTER C. HAMILTOX,
AND
D. R. MAcKESZIE
Received M u y 25, 1964 Sodium perxenate octahydrate, Ka&eO6.8HzO, is orthorhombic with cell constants a = 11.86, b = 10.36, c = 10.43 k , space group Pbcn, Z = 4. A three-dimensional X-ray diffraction investigation has resulted in a complete structure deterThe mination. The perxenate ion is approximately a regular octahedron with a mean Xe-O distance of 1.864 + 0.012 0.8”. The two crystallographically independent sodium greatest deviation of an 0-Xe-0 angle from the ideal 90” is 2.6 atoms are surrounded by very distorted octahedra composed of water molecules and perxenate oxygen atoms. A complex array of hydrogen bonds completes the structure.
a.
+
Introduction The reaction of XeF6 with sodium hydroxide was shown by Malm, et a1.,3to produce compounds which contain octavalent xenon and which, on the basis of chemical analyses, were thought to contain the perxenate ion, XeOo-4. In a previous communication3 we sketched the evidence from a n X-ray study that one of the compounds that forms is sodium perxenate octahydrate. Subsequent to that study Zalkin, et u Z . , ~ have shown that another product is sodium perxenate hexahydrate. In this paper we present in detail the results of our crystallographic study of sodium perxenate octahydrate and also discuss the geometry of the per(1) Research carried out under the auspices of the U. S. Atomic Energy Commission. ( 2 ) J. G . Malm, B. D. Holt, and K. W. Bane, “Noble Gas Compounds,” H. H. Hyman, Ed., University of Chicago Press, Chicago, Ill., 1963, p. 187. (3) W. C. Hamilton, J . A. Tbers, and n. K. hIacKenzir, S & J L G ~ , 141,532 (1963). (4) A . Zalkin, J, L). Forrester, D . H . Templeton, S. M. Williamson, and C. W. Koch, i b i d . , 142, 501 (1063); A. Zalkin, J. n.For-rester, and D . H. Templeton, Iiiovg. Chem., 3, 1417 (1964).
xenate ion and the complex hydrogen bonding scheme in the octahydrate. Experimental The material studied here was prepared by adding about 1 ml. of 1 M NaOH to several mg. of XeF6 at 77’K. The XeFs was almost certainly contaminated with XeF?. A yellow color appeared in the frozen mixture and disappeared as the mixture melted. Colorless, well-developed crystals with dimensions of up to several tenths of a mm. formed within several minutes in the reaction vessel. Several of these crystals were selected for X-ray photography and were sealed in thin-walled glass capillaries to reduce dehydration or possible decomposition. All photographs were taken with ,No KC^ X-rays from plate-like crystals with approximate dimensions 0.2 X 0.2 X 0.05 mrn. Data suitable for structure analysis were collected at room temperature by multiple-film Weissenberg photography. In order to minimize the time required to collect a complete data set, three crystals were photographed simultaneously on differed cameras to obtain data from the reciprocal nets Okl, l k l , . . . 1 3 k l . All independent intensities strong enough to be observed and accessible within the scattering angle B>fo _L 26” were estimated vis-
CRYSTAL STRUCTURE OF SODIUM PERXENATE OCTAHYDRATE1413
Vol. 3, No. 10, October, 1964
ually. The 716 observed intensities were corrected for Lorentz and polarization effects, but not for absorption. The linear absorption coefficient calculated for the formula NarXeOs. 8Ht0 is 29 cm.-', so that absorption errors should not seriously affect the intensity measurements. Although a number of the strong reflections seem to suffer from extinction, no corrections were made. A final set of photographs of the Okl net was taken a t the end of the experiment. The identity of these photographs with the initial photographs provides good evidence for the stability of the material during the photography. The crystals investigated are orthorhombic with c ~ l constants l a = 11.864, b = 10.358, c = 10.426, each 4~0.005Asg The obk odd; h01,Z odd; Okl, k odd) indiserved extinctions (hkO, h cate that the space group is probably D ~ h ' ~ - P b c n .The ~ density, as measured by flotation in mixtures of methylene dibromide and carbon tetrachloride, is 2.33 =!= 0.05 g. cm.-3. Siegel' ascribes to a compound of formula Na4XeOe. 5H20 an orthorhombic cell with constants a = 10.36, b = 10.45, c = 11.87 A. It is clear on the basis of the agreement between that cell and the one found here (after redefinition of axes) that the two compounds are identical. Analytical results a t Argonne2 indicate a Na:Xe ratio of and an oxidation number of eight for Xe. The density observed here is in poor agreement with four formula weights of the . it pentahydrate in the units cell ( p o = 2.10 g. ~ m . - ~ ) However, is in excellent agreement with the formula Na4XeOe.8H20 ( p o = 2.38 g. ~ m . - ~ which ) was deduced here from the structure determination.
+
Solution of the Structure The multiplicity of the general positions in Pbcn is 8 and the four Xe atoms must therefore lie in special positions. It was clear from examination of the intensities of several reflections and from the threedimensional Patterson function that the Xe atoms are in positions (k),=!=((I, y, l/4), y, l/J, with y approximately 0.20. From the Patterson function the positions of six atoms bonded to the Xe were readily found. Two of these were placed in two sets OF special positions (4c) along the twofold axis, and four were placed in two sets of general positions =!=(x,y , z ) ,
+
+
+
( l / 2 - x, '/z - Y, '/z z), ( l / z x, '/z - Y, 3, (3, y, - z ) . Successive least-squares and difference electron-density syntheses led t o the placement of six more atoms in general positions in the asymmetric unit. From their coordination and peak heights in the electron density maps, two of the atoms were identified as sodium, and the four remaining were assigned as oxygen, presumably as water molecules. In a final series of least-squares refinements the Xe was allowed to vibrate anisotropically, while the other atoms were constrained to vibrate isotropically. In these refinements, which were carried out on F, unit weights were assigned for F < 50 electrons, and weights were taken as ( 5 0 / F ) 2 for F 3 50 electrons. The atomic scattering [actors used were those of Watson and Freeman8 lor Xe, Berghuis, et U Z . , ~ for Na, and Hoerni and Ibers for 0.'" Proper account was taken
( 5 ) These are the cell constants quoted in ref. 4 (X Mo K a i = 0.70926 they are in satisfactory agreement with our less precise values quoted in ref. 3, where an accidental transposition of b and c was made. (6) "International Tables for X - R a y Crystallography," Vol. 1, T h e Kynoch Press, Birmingham, 1952. (7) S. Siege1 and E. Gebert, ref. 2, p. 193. (8) R . E. Watson and A . G. Freeman, private communication, 1963. (9) J. Berghuis, I. M. Haanappel. M. Potters, B. 0. Loopstra, C . H. MacGillavry, and A . L. Veenendaal, A d a Cvyst., 8, 478 (1955). (10) J. A. Hoerni and J. A . Ibers, i b i d . , 7 , 744 (1954).
A,);
Fig. 1.-Perxenate ion with surrounding water molecules. A twofold axis coincides with the line 01-Xe-02. The dashed lines are hydrogen bonds. The sodium ions coordinated to the perxenateoion and the water molecules are not shown. Distances are in A. TABLEI PARAMETERS IN SODIUM PERXENATE OCTAHYDRATE~ Atom
Position
X
Y
2
Xe
4c
0
0.20199(14)
'/4
B , b.2 Anisotropic 01 4c 0 0.3836 (23) '/4 2.0(4) 0 2 4c 0 0.0233 (22) '/4 2.0(4) 03 8d 0.1079(18) 0.2041(20) 0.3766(22) 2 . 2 ( 4 ) 0 4 8d 0.1190(14) 0.2051(15) 0.1301(17) 0 . 8 ( 3 ) Nal 8d 0.1188(9) 0.4299(10) 0.4368(10) 1 . 8 ( 2 ) Nat 8d 0.2811 (15) 0.2139 (10) 0.2644(12) 1 . 9 (3) Wi 8d 0.3153(17) 0.4159(17) 0.4090(17) 2 . 2 ( 3 ) Wz 8d 0.4364(18) 0.1456(17) 0.4255(17) 2 . 0 ( 3 ) 8d 0.3259(16) 0.0174(17) 0.1558(17) 2 . 0 ( 3 ) Wa W4 8d 0.3823(17) 0.3486(17) 0.1245(18) 2 O(3) a The numbers in parentheses are estimated standard deviations. W indicates the oxygen atom in a water molecule.
TABLE IA ANISOTROPIC THERMAL PARAMETERS FOR XENOK pi1 = 0.00117 (45) Pzz = 0.00181 (17) p 3 3 = 0.00182 (17) ( Y I ~ ) ' / ' = 0.087 i 0 015" (~2~)'/'= 0,099 f 0.005 plz = 0 by symmetry ( ~ 3 ~ ) ' / ' = 0.104 f 0.007 018 = 0.00023 (17) p 2 3 = 0 by symmetry a Root mean square amplitudes of vibration. The deviations from isotropy are so insignificant that the derived directions of the principal axes of the motion are meaningless.
of the effects of anomalous dispersion by applying corrections to FC.I1 The final parameters derived from these refinements are given in Table I. The conventional R factor 211 Fo( - \Fel//21F,j is 0.105. In Table I1 the final values of observed and calculated structure amplitudes are given. A final difference Fourier, based on the data OF Table 11, shows one peak of height 6.6 e/A.3 a t the Xe site; the next peak is of height 2.7 e/&3, approximately 25% of the height of an oxygen peak in this structure and about 15% of the height of a sodium atom. The residual density a t the Xe site presumably arises from improper treatment of the Xe scattering or vibrations, but is only about 49.', of the Xe peak height of 178 e/A.3. Since the Xe lies (11) J. A. Ibers and W . C. Hamilton, ibid., 17,781 (1964)
1414 J. A. IBERS, W.
C.HAMILTON, AND I>. R. MACKENZIE
Inorganic Chemistry
TABLE I1 OBSERVED AND CALCULATED STRUCTURE AMPLITUDES (IN ELECTROSS) FOR Na4Xe06.8H10 K
L a e s c4t
K
L BAS C ~ L
6
I 2
t 6 6 6
7 7
....
bil
c
0 906 a 3 8
C C
4 55 67 6 2 4 7 27C
o c
2 l a 5 244 8 183 167
C LO 130 C 12 8 3 2 0 150 2 L 124 2 2 199 2 3 I77 2 4 131 2 5 bB 2 6 I38 2 7 7b 2 8 177 2 9 70 2 LO b 8 2 11 5 3 2 1 2 41 4 0 b5
145 86
199 115 206 147 I19
58 I2h 75 lb3 76
71 4b 40
b6
4 4 4
1 2 6 0 271 2 1 7 7 141
3
58
4
4
76
4 4 4 4 4 4
5 21b 1 9 5 7 159 147
P 1
89
IC
54
51
I 1 91 27 4 12 t 0 36 t 1 235 6 2 71 t 3 200 6 5 96 L 7 181 51 6 R t 9 150 t ir 21 6 11 bb a o 123 8 1 95 8 2 5n e 3 92 8 4 66 e 5 47 88 d t e 7 103 e a 59 e 9 9? 55 8 IC I C C 12b
90
IC
IC IC IC 12 12 12 12 12
7 7
4
99 107 5 5 '54 65 67 5 b 57
99
R 9
7
58 103 62 43
e7 59 85
55 122
18 71
I I 1
I
I 1
I 1 1
2 2 2 2 2 2 3 3
3 3 3 3 3 3
3
I..... 9t
76 b5
2 125 9 7 3 196 175 'I 29 28 5 129 I22 b 25 25 7 1 3 3 127 e 79 82 9 129 I24 78 1 1 75 38 3 3 I 2 11 I 3 29 21 4 92 7 3 5 22 21 9 21 24 0 ILL 181 I 122 1 1 7 2 I60 I l b 3 4
39 19
42
8 10
IC IC
IC 12 I2 12 I2 12
76
71
29 35
151 3 68 138 5 36 6 155 7 I6 5 8 120 5 10 I l l
32
I 2 2 2
140
2
13
2 3 3
5 5 5 5 5
2 4
I46 59 118
120
99
I
7
4
7 7 7 7
5
b4 79 49
5
..a.
ai 33
17 32
1
c
3ti 59
45 52
IB 143 106 56
87 29
31 25 37 21 15 61
2 114 117
4 2b5 32b 6 1 4 3 L5b
e
112 123 88
91
12 I O > 108 2 I30 95 3 22 23 4 31 29
_ I' .
6 9
IC
9 5
9 F
I8
10
F
23 22
25 20 I1 Ill 125 53 1e5
9
11 1 3 I 139 2 157 3 51 4 191 5 11) 118 b 147 128 7 5 1 60 e 4 9 44 2 9 47 44 2 I C a 3 85 2 11 5 3 57 2 1 7 a2 7 1 3 1 22 1 4 3 3 2 1 16 3 4 57 48 3 5 3 1 29 4 0 86 74 4 1 138 117 4 2 6 6 59 4 I 211 217 4 4 7 b b9 4 5 121 115 4 b 65 6 6 4 7 112 101 4 8 31 36 4 1 89 90 4 IC 37 32 4 11 7 1 6n 5 1 31 J I 5 4 23 24 5 5 20 1 9 5 C 24 I2 5 7 3 1 34 5 8 27 3 3 t c 34 34 6 I 144 I 3 4 6 3 223 i a r 6 4 44 47 6 5 197 I 9 1 6 t 47 4 6 6 7 100 95 b 9 10 74 6 10 24 25 e o 3 2 34 8 1 63 b1 2 90 9 4 8.~ 1 83 9 2 e 4 82 a4 a 5 93 9 8 8 b 52 4 9 a 7 32 4 0 e e 6 1 61 a 9 35 3 L 9 I 24 3 1 IC 0 94 9% I O 2 9 4 95 LO 3 3 7 4 5 IC 4 93 107 I C 6 e o 91 73 12 0 7 4 12 2 6 6 7 2
e
7 8
I
5
86
61
H.;....G
10
94 22 94 30
3 3 3 30 7 37 34 0 74 b 5 1 111 I06 2 27 27 3 12b 119 4 29 32 5 1 0 3 96 6 59 57 7 105 7 P a 29 25 9 87 a8 11 5 4 b3 o n2 t i I 48 4b 7 73 77 3 32 3 3 4 57 b l 5 28 25 6 41 49 7 4 3 42 8 63 57 1 40 41 0 77 72 2 96 8'1 84 4 bd b 72 6 8
It 59
6 I74 I 3 3
9 11 11 11
11 11
C C
3 6 7
a
25
81 56 86 45
33 3~ 3 3 30 2 21 21 I 59 4 4 2 26 27 3 110 112 4 27 29 5 60 6 3 37 44 7 e 27 24 0 20 30 1 6 3 61 2 23 I1 3 6 7 79 4 I2 15
95 i o 4 87
1Ob
c IC
ai
90
1
37
3*
2 2 2 2 2 2 2 ~
2 2 2 3 3 3 4 4
4 4 4 4
4 4 4
6 6
t b
t
t t
4
2 a4 17 3 105 92 4 130 123 5 4 e 48 6 8 5 85 7 3 3 37 e ~. 58 57 9 49 5 7 1 0 47 57 11 2 5 4 0 I 1 7 67 53 4 4 5 t 4 1 75 C 57 62 I 98 8 9 2 39 3 6 ~
3 139 I 1 6 4 3 3 25 5 I20 102 7 91 9 1 9 65 b e 52 0 0 11 0 24 25 I 140 119
2 5 3 44 3 129 I 1 0 50 3 1 4 5 I30 1 1 3 7
91
81
6 7
9
72
2
a
C I 2 3
E
4
73 57 50 29 62 52 65
e
5
63
8
6 7
62 54
8
44 a7
e 8
a
a IC IC IC IO
b
42
4
o 2 4 6
a2 73 73
74 7 31 8 101
3
2 4 b
c I
2
2 2 2 2 2 2 2 2 3 3 3
70
4 4
49
1 2
96
9) 53 91
41
'16
3
63 39
77 45
4 4 4 4 4 4
66 40
5 5
4
5 6
bl 38
t t b
6 6 b
7 111 139 1 1 4 114
C C C C
I23 120 I28 124 104 99 26 27 1 7 2b 8 1 129 51 52 115 1 1 3 97 a 8
C
I 1
2 2 2 2 2 2 2 2 2 2 2
56
41
32 62
30 57 b4
63 1 0 5 103
52
52 58 47 47 I 1 3 125 29 2 7 b6
4 4
4
91
4 4 4
a4
3b '12 5 3 53 77 75 3 6 26 103 e7 125 1 3 3 3 7 39 1 0 2 91 99 8 2 125 107
31 LO8
4 4 4
4 6 t
6 6
6 b
e
8 8
a
e
8
a
IC
46 a9 89
44
53 22
49 24
46
46
29
30
60
63
58 61
74
e5
97 e4
7 7
e
a 8 P
8
e5
H;
9.....
24 20 6 9 120 53 43 3e 46 90 a 5
56 34
6
1
I 2
32
L
bo 56 68
i
65 66 37 47 ?L 77
I
e
46
I
9
80
a5 47 71
1 10
25 30
23 20
I
I
2 3
3 3
3 3
I
3 5 7 IOI
2
C 107 LO6 34 1 29 7 CO 4 0 3 6 5 57 4 33 27 7 1 b4 8
2 3
)a
4
37
5
34
.....
6b
51
47 til 57 42
b 7
B
19
11
32
23
45 13a 114 '13 3 4 6b
9n
18
35 92 37
36
94
35
3
I1
4
41
a6 35 84
2e 2C 26
1 130 11'1 32 3 7 98 89 4 1 6 20 5 108 8 4 7 109 92 2 11 1 9 4 20 24 t i a 15 c 7 3 75 I 67 62 7 4 7 50 1 45 45 4 39 4 5 ? 3
Piill.....
1
1 76 I19 2 I5 20 3 1 0 4 120 G 25 3 5 5 IC9 1 0 4 50 b 59 I 7 107 91 2 2 I3 21 ~. 2 3 IY i b 2 4 I3 15 2 7 1 7 18 3 c 72 a7 3 I 70 7 7 3 2 a3 el 3 1 47 4 9 3 4 79 70 3 5 77 b5 1 b 77 6 2 3 7 68 53 4 2 1 3 16 5 0 108 92 5 2 I44 1 1 5 5 3 29 27 5 4 I26 115 5 6 112 V O b 4 24 2 1 7 0 104 9 8 7 1 38 4 c 7 7 a 5 77 7 3 41 37
I
I
1 1 1
4
ti3
68
.... C
c
2 4
IO4 9 4 I02 68
bb
C 6 76 I 3 2 9 2 0 30 2 I 40 2 2 40 2 3 27 2 G 91 2 5 59 2 6 92 7 'r3 4 0 31
i 4
I
12 24 32 57
18
83
5
85 2a 5b
95
I
Id 88 3b
I
8 9 1 5 7 2 3
IO
2
6 7
4
65
71
lb 35
0
95 12'I 99 99 129 115 8 138 ioe 2 33 47 3 I b 12 4 26 11 97 0 b9 52 1 46 2 86 I 7 3 73 i n 4 76 IC 5 35 3e
0
69
,.....
14
H*l2..*..
C
54
."SI
17
LI
52
19
2
42
35
a6 63
84
....
7
....
I
40 a3 88
66
iirlo
0
4
43
30
c c
c
45
7b 79
I...
4q
1
6 8
57
4 4
1
1 I
7
5 9
7 9 9 9
2
5
58 35 43 43
7
I
7
9 5
7 7 7
0 195 I 8 6
5 8 IO1 IO8 5 LO 8 6 Be 7 ? a8 9 0 7 1 51 51 7 2 141 I30 7 3 5 1 51 7 4 I I C 104
31
29
7
5
b7
64
230 76 I70
1
53 1 56 2 137 1 3 4 3 54 58 4 208 167 b 9s 90 B 74 e o
9
3 205 4 79 5 202 b 20 7 157 9 120 I O 55 11 90 12 31 2 34 3 za 5 43 6 23
I I I
44
99 98 32 31 74 7 6 27 37 114 9 8 I 0 1 97 I01 LOO
53 56 72
46
1
5
52 56
34
3
18
2
86 35
2b 26 39 4 3 21 1 6 10 27 25 5 0 211 227 5 I 49 4 1
5
5n 97
84 43
2b 58 103 19 103
5 5 5
41
25 25 17
7 7
43
7
e
52
71
S
31 57
16
5
31
3i
30 21
5
0
90 42
30
5 C
85 23
bl
2b 28 2 IC5 I52 3 I6 I7 4 1 6 1 135 5 72 1 4
4
44
62
40
5
4 4 4
47 72
I04
ans c4t 24
7
58
7
I 5
I
4
47 71 18 64
5 5 5
7
53
7 5
4
1
1b
4
4
L
2 27 3 LO1 4 I7 5 a2
7
15
11 1
56 1 3 11 205 I 5 3 1 1 I1 61
5
56
5 5 5
L aBs G A L
3 153 141 53 4 1
I4
4 4 4
K
3
5 208 1 6 4 41 31 7 I21 I28 B 44 4 4 9 92 96 1 0 23 23 11 1 7 88 2 37 3 1 3 37 31 c 184 163 1 LOO 03 2 IO8 95 3 142 1 1 4 4 87 15 5 58 5 1 h I09 9 8 7 11 7 3 8 71 74 1 72 7 1 IC b9 66 1 1 7 I7 2 42 4 0 3 I 8 15
4
6
't2
41
C 6 C LO
C
I?
4
62
57
7 8
95
36
95
17
4
60
50
32 20
9 10
3
26
C
4
J
43
44 57 31 81
1 2
72 17 72 56 2h 30
26 91
21 55
28 3 12 3 3 4 I 108 4 2 42 4 3 21
3 10
3 11
R
7
I1 I2 5 3 I 34 2 91 3 129 2 26 3 107 4 29 92 5
74 40 71 41 54
ie
2
24 24
98 53 27 30
4 0 1
5M 7 88 a 1 8 I 1 3 110 9 6 1 65 6
5 6
C
0
3 3
3
64
67 30 72
le
E
4?
51 23
25
8
3
3
41
2
8
3
17
2 3
34
e
37 23
15 43 86
72
I
e e
37 21
14
72 33
8
I 2 2 3 3
16
a?
t t t 6 8
L
72
ab
b b
1 1
I
65
5 5 6 t
I
IC
4 4 4 4 4 b 'I 7 4 8 4 9 4 I1
5 5
1
3
4
67
IO
90
~~
I
L
ti3 b? 111 1 3 5 44 49 116 1 1 4 36 38
8
5
b3 76 68 39 55 38
2 3
I I
6
ti6
b
7
a
1 125 205
5
3
5
3 4
8
1
4 120 106
6
21
12 2
b
C
91 I O 1
106 96
6h 124
10 11
.....
C
64
145
32 77
9
58 52 41 4 0 l b 3 159 63 63 121 117 87 8 8 95 81 75 I b 15 27 75 7 5 35 32 22 27 10 e 32 30 I 6 19 I8 15
1
5
69
7
39 35 32 21 15 27 2 3 22) 193 26 22 208 197 34
7
*...Hi
2
1
I
b
0 I
4
2
5
11 17 37
I0 9 4 91 I 4 0 39 7 22 22 0 12b 1 1 4
I61
4
