Note: Descriptions are shown in the official language in which they were submitted.
- c ~
~458~3
The present invention relates to fat blends con-
taining palm-based fats, which fat blends are suitable
for the preparation of food spreads, particularly marga-
rine and which can also be applied in the production of
shortenings.
The invention especially relates to margarine fats
from which margarines of such a consistency can be made
that they are suitable for packing in tubs.
The invention provides a fat blend suitable for
the preparation of emulsions, particularly margarine,
having dilatation values at 10C of at most 1000, at
20C of at least 200 and at 35C of no more than 75,
which comprises a co-randomized and a non-randomized
part, the co-randomized part comprising a palm-based
` 15 fat, a lauric fat and a trans-containing fat, the non-
randomized part containing additional fats such that the
fat blend comprises 18-50% H fatty acids,3-25% T fatty
acids 3-30% M fatty acids, while the balance can be made
up to L fatty acids. The dilatation values as described
in this specification were measured as described in
H.A. Boekenoogen "Analysis and Characterization of Oils,
~ats and ~at Products", Vol. I 1964, Interscience Pu-
blishers London, pp. 143 et seq.
The term "fat" is used herein to include fatty
acid triglycerides which are solid at 20C and are com-
- monly described as "fats" as well as triglycerides which -~
are liquid at that temperature and which are commonly
described as "oils". The term "liquid oil", which is
also used in this specification refers to triglycerides -~
, . '
:
:
5~9;~
which are liquid at 5C, preferably at 0C. A "fatty
phase" is a fat or fat blend which can include liquid
oils and which is suitable as the sole fat blend in the
emulsions of the invention. Similarly a "margarine fat"
is a fat blend which can also contain liquid oils and
which is suitable as the fatty phase in margarine. Un-
less stated otherwise, the terms "emulsion", "margarine",
"food spread" etc. refer to water-in-fat emulsions con-
taining the fat blends of the invention and also suitable
amounts of fat-soluble emulsifiers, e.g. partial fatty
acid glycerides like monoglycerides, phosphatides, and
fractions thereof, etc. and/or water-soluble emulsifiers,
e.g. partial glycerides, phosphatides, egg yolk, protein
etc.
In this specification by
H fatty acids are understood saturated fatty acids with
- 16-24 carbon atoms ~-
T fatty acids: mono-trans unsaturated fatty acids with
- 16-24 carbon atoms
M fatty acids: saturated fatty acids with 12-14 carbon
atoms
L fatty acids: the remainder, being 100 - (H + T + M)%.
The term "randomizing" refers to the interchange
of the fatty acid radicals of the glycerides on the glyc-
eryl radicals in random fashion. This interchange, when
applied to at least two different fat sources is called
"co-randomizing" and can e.g. be effected under the in-
fluence of an interesterification catalyst at tempera-
tures of about 25-175C, preferably 80-140C. Suitable -~
interesterification catalysts are alkali metals, their
'
1~58~3
alloys, their hydroxides, their alkoxides, e.g. in pro-
portions of 0.01% to 0.3 or 0.5~o by weight of the fat
blend to be interesterified.
The fat blend according to the invention is partic-
ularly of importance in emulsions containing from 40 or
50 up to 85% of a fatty phase, the balance of the emul-
sion being an aqueous phase, which can be water, milk or
skim milk adjusted to the required pH value e.g. of about
4 or 4.5 to 6 or 7 and which can contain, apart from suit-
able water-soluble emulsifiers, various minor ingredients
e.g. salt, acid, protein, flavours, preservatives, etc.
In this specification all percentages, proportions ~ -
and parts are by weight unless otherwise specified. The
amount of fat in the emulsion is based on the weight of
the emulsion, the amount of fat in the fat blend is based
on the weight of the fat blend and the amount of fatty
acids in a fat is based on the total amount of fatty
acids in said fat, unless stated otherwise.
The use of a palm-based fat, which term includes ;~
both hydrogenated and unhydrogenated palm oil as well as
solid and liquid fractions thereof, preferably as a dom-
; inating constituent in margarine fats, is of great im-
portance, for reasons of availability and consistency of
such fats and also because of economic considerations.
The presence of substantial amounts of palm-based
fats in fat blends to be used in food spreads, e.g. mar-
garines, often results in inadequate products, mainly
because palm oilisaslowly crystallizing fat of a very
specific glyceride distribution. The slow crystalliza-
tion properties of palm oil can e.g. result in crystal
,:
- 4 -
.. - - ~ .- ... .
'. ' :' ~ ~ , '- : ~
cL ~
1~)4S8~3
defects, e.g. caused by "post-hardening", which means
that on storage of the prepared product crystal growth
proceeds, which e.g. can result in an unacceptable in-
crease in hardness of the product and/or in the formation
of large, grain-like crystal aggregates, which in turn
are responsible for undesirable organoleptic properties
of the finished product.
~he fat blend of the present invention can contain
substantial proportions of palm-based fat, e.g. from 20,
30, 40 or 50 to about 80% by weight. ~he fat blends thus
obtained are - as compared with the prior art products of
the same palm-based fat content - more rapidly crystal-
lizing, probably as a result of interaction of the various
types of triglycerides which are formed as a result of -
co-randomizing part, especially the major proportion, of
the fat blend, and they can be used in margarines of out-
standing consistency and organoleptic properties. A
particular advantage of the fat blends of the invention
is that fractionating is an entirely optional process
step. If suitable fat fractions are available, they can
be incorporated in the fat blend, but if not, it is not
necessary and certainly not preferred to carry out a
complicated fractionation process, which always has the
drawback that substantial proportions of fractions remain
for which other outlets have to be found.
A further advantage is that in the fat blends of
the invention liquid oils should not be subjected to a
co-randomizing treatment, which process when applied to
liquid oils may sometimes affect the organoleptic quality
~0 of the blend.
... ..
-- 5 --
- ~ :
1~)458~3
Preferably the fat blends of the invention contain
a total of ~ and M fatty acids of 10-45% by weight, par-
ticularly 12-40%~ the total of H and ~ fatty acids being
preferably at most 60%. ~he co-randomized part of the
fat blend may constitute from 10 or 20 to 80 or 95%,pre-
ferably from 35 to 85% by weight of the total blend.
Preferably a co-randomized part is used containing
from 5 to 35% by weight of lauric fats, 10 to 50%, es-
pecially 15-45% by weight of palm-based fat and 10 to 50%
by weight of trans-containing fats based on the total
weight of the fat blend to provide from 10 to 40% H, 4
to 25% ~ and 5 to 25% M fatty acids in the co-randomized
part. In a particularly preferred embodiment of the in-
vention the palm-based fats are the dominating fats in
the co-randomized part. By "lauric fats" are understood
fats containing substantial proportions of glycerides of
~ lauric acid (M acid), particularly coconut oil, palm
f kernel oil, and babasu oil, which fats may have been sub-
' jected to hydrogenation.
The non-randomized part of the fat blend of the in-
; vention should be at least 5 or 7% by weight and prefer-
ably contains 0 to 25% of lauric fats, 0 to 50% liquid
oils, 0 to 25% palm-based fats and 0 to 35% of trans-
containing fats. ~specially proportions of at least 10
or 20% liquid oils in the non-randomized part provide
- suitable refrigeration type margarines.
Both in the randomized and the non-randomized part
of the fat blend of the invention the palm-based fats
can consist of or contain substantial proportions of
hydrog nated palm oil, particularly hydrogenated palm
.
.
.. . .
.
lV4SE~93
oil of a melting point of 40 to 48C, as well as frac-
tions, particularly the liquid fractions, of hydrogenated
or unhydrogenated palm oil obtained by dry fractionating
or fractionating in the presence of organic solvents or
detergent solutions. Unhydrogenated palm oil is general-
ly preferred since thereby a complicating hydrogenating
step can be avoided, without detrimentally affecting the
ultimate quality of the fat blend of the invention.
The trans-containing fats can be present in both
the randomized and the non-randomized part of the fat
blend and hydrogenated oils of a melting point of 25-55C,
particularly hydrogenated llquid oils of a melting point
between 30 and 45C are preferred.
Suitably the high trans-containing fats are pre-
pared by hydrogenating liquid oils in a conventional iso-
promoting way to semi-solid fats having a melting point
e.g. between 30 and 45C and generally having steep tem-
perature/dilatation curves. Such fats generally have
relatively few saturated fatty acids, particularly at
most 35% and have a trans-fatty acid content of at least
20%, preferably at least 30 or 40%. The preferred range
of the trans-fatty acid content of such hydrogenated oils
is 50 to 70% and that of the saturated fatty acid content
about 15 to 35%. Preferably an iso-promoting sulphur-
poisoned hydrogenation catalyst is used in the hydrogena-
tion of such oils, for example 1.5% of a sulphur-poisoned
nickel catalyst precipitated on kieselguhr and the hydro-
genation can be effected at temperatures varying from
about 140C to 180C. In this way it is possible to ob-
tain hydrogenated high trans-containing fats containing
-- 7 --
.
. .
~04S~9 3
40, 45 or 50 to 65, 70 or even 75% of trans-acids and
no more than 10 or 15 to 25 or 30% of saturated fatty
acids.
The hydrogenation treatment can also be carried out
with non-poisoned nickel catalyst precipitated on kiesel-
guhr. ~hese catalysts are especially used with oils,
e.g. certain types of soya bean oil which do not remain
stable as regards flavour after a treatment with an iso-
promoting catalyst. Such oils therefore are preferably
hydrogenated with a fresh nickel catalyst in two or more
stages, or in the first stage with a fresh and the second
stage with a sulphur-poisoned catalyst, first at about
90 to 120C and subsequently at about 170-190C. With
these catalysts also high trans-fatty acid contents can
be obtained, e.g. of 30, 35 or 40% up to 55 to 65% by
weight and also low saturated fatty acid contents, e.g.
no more than 15, 20 or 25 to 30 or 35% by weight based
on the total amount of fatty acids in the hydrogenated
fats.
Fractions of hydrogenated oils can also be used to
; provide a suitable trans-containing fat for the fat blend
of the invention. The fractionation treatment can be
carried out by removing part of the tri-saturated glycer-
ides and thus increasing the proportion of trans-acids,
until a fraction of a high trans-acid content is obtained.
With a given trans-content of the trans-containing
fats the total proportion of trans-containing fat in the -
fat blend of the invention is preferably adjusted to
provide a fat blend of a trans-fatty acid content of 3
to 25%, particularly 3 to 25% in the co-randomized part,
.. . .
-.. : . .. - . ~ , . . ~. . , - -: .
cL 532
.
1045~393
calculated on the total blend.
Fractionation of the hydrogenated fat and/or the
palm-based fat to be used in the fat blend of the inven-
tion, is preferably carried out by heating the fat to a
temperature of about 50 or 60C, cooling the liquid fat
obtained to 40C, followed by a gradual cooling in about
4 hours to about 32 to 38C in the case of hydrogenated
fats or 15 to 35C in the case of a palm-based fat. ~he
mass obtained is subsequently kept at this temperature
for a period of about 1.5 to 3 hours, after which the
solid fraction is separated, e.g. by filtration.
Oils which are suitable for the preparation of
trans-containing fats are for instance groundnut, rape-
seerl, sunflower, safflower, soyabean, fish and cotton-
seed oil.
~he melting point referred to above is the "slip
melting point" as defined in Bailey "Melting and Solid-
` ification of Fats", Interscience Publishers Incorporated,
New York, 1950, p. 110.
~he liquid oil component to be used in the fat
blend of the invention is preferably one containing at
t least 40% by weight of poly-unsaturated fatty acids, for
example sunflower, safflower, cottonseed, wheat germ,
soyabean, grapeseed, poppyseed, tobaccoseed, rye, walnut
or corn oil.
According to a specific embodiment of the inven-
tion, margarine fats are provided which are suitable for
, ~ refrigerator-type margarines, i.e. those which are pre-
ferably packed in tubs, having dilatation values at 10C
; 30 of no more than 700 and at 35C of no more than 50, said
,; ~',~. .
_ g _ --
. ' .
104589~ ~
margarine fats comprising about 45 to 7G% by weight of -~
co-randomized constituen-ts, the remainder being non-ran-
domized constituents, the co-randomized part comprising
20-45% unhydrogenated palm oil, 5 to 30% of lauric fats,
the balance being hydrogenated trans-containing fats.
The margarines can be prepared by emulsifying the
suitable aqueous phase in a suitable proportion in the
fat blend of the invention and chilling and working the
mass in a conventional manner. The aqueous phase can con-
tain additives which are customary for margarine, for
example emulsifying agents, salt and flavours. Oil-
soluble additives e.g. flavouring compounds, vitamins etc.
can be included in the fatty phase. Generally the pro-
portion of fatty phase in a margarine varies from about
75 to 85% of the emulsion depending on local statutory
requirements for margarine. Alternatively higher propor-
tions of the aqueous phase can be adopted in the produc-
tion of so-called low-fat spreads, which can contain as
little as 35~ 40 or 50 up to 60% by weight of fat.
The emulsions, particularly the margarine, can be
manufactured in a conventional closed tubular surface-
scraped exchanger as described in "Margarine" by A.J.C.
Andersen and P.N Williams, Pergamon Press 1965 ~ pp. 246
et seq. Votator arrangements described in British patent
specification 639~743~ British patent specification
650~481 and British patent specification 765~870 are
particularly suitable. Alternatively, emulsions can be
prepared by means of a phase inversion process as de-
scribed in British patent specification 1, 215 ~ 868 or on
3G conventional cooling drums as described in the same book
e. ~Q~
- 10 -
. . - .. . - , ~ ., ~ , ~ .. ... . .
1~458~3
by Andersen and Williams"
~he invention will be illustrated by the following
examples:
EXA~PLES I -XXI I
Fat blends were prepared containing non-randomized
and co-randomized constituents.
~he fat blends of Examples I-XIX were used for the
preparation of margarine, the blend of Example XX for a
low calorie spread and the blends of Examples XXI and XXII
were used as shortenings.
Margarines were prepared as follows: -
~he margarine fat blend was melted and emulsified
with an aqueous phase prepared from soured milk contain-
ing 0.1% monodiglycerides to give an emulsion containing
80% of fat.
~he emulsion was crystallized and worked in a closed
tubular surface-scraped heat exchanger (Votator A-unit),
which was left at a temperature of 15C. The cooling
temperatures in the A-unit were from -6 to -10C and
40% of the treatment emulsion was recirculated. There-
after the crystallized emulsion was passed through a
resting tube (Votator B-unit), where it crystallized
further for 160 sec. and was then liquid-filled into tubs.
~he low calorie spread was prepared as follows:
~or the preparation of a low calorie spread with
good spreadab,ility at refrigerator temperature and a
very satisfactory melting behaviour, 4t of the fat blend
of Example XVIII were mixed with 4 kg of a high-mel-ting
distilled monoglyceride and 12.5 kg of a distilled sun-
flower oil monoglyceride. ~his fat phase was mixed and
- 11 -
.
-
,~ cL 532
.
lal~S~93
`, . :
emulsified in a normal votator arrangement using less
cooling, with 6t of a water phase containing 1% of salt
and sufficient citric acid to maintain a pH in the emul-
sion of 4.2.
The votated product was tub-filled and possessed
; the described properties in the fresh state and also
after 6 weeks' storage at 15C.
The shortenings were prepared as follows:
A specially refined, rather white fat composition
was continuously fed in the molten state into a tubular
heat exchanger, in which the mass quickly crystallized
while sufficient nitrogen (about 20 Vol%) was dosed into
the solidifying fat stream, most of the gas being dis-
solved under the pressure in the equipment. After heavy
but short mechanical working in a high speed crystallizer -
under almost normal pressure, the shortening mass was
- ready for pack-filling. The final stiffening period was
less than 1 minute.
~he co-randomization was carried out as follows:
The fats to be co-randomized were dried to a water
content of about 0~01% by weight and subsequently co-
randomized at 110C in a stirred vessel which was kept
under a vacuum of 2 cm mercury, in the presence of 0.1%
by weight of sodium methoxide as a catalyst. After 20
minutes the mixture was cooled and the vacuum released.
The catalyst was destroyed by washing the co-randomized
mixture with water and dried as before.
Preparation of hardened fats:
:
Palm ~, having a melting point of 38C, was heated
in a hydrogenation vessel to 120C under hydrogen gas,
.:
- 12 -
7 ~
~, `
10~5893
then 0.5% of a sulphurized Ni-on-guhr catalyst was added
and the hydrogenation started. After 90 mins. at 180C
hydrogen supply was stopped and the oil was filtered free
of catalyst. The hardened palm oil obtained had a melt-
ing point of 42C, a trans-fatty acid content of 30%,
and contained 50% H-, 1% M- and 29% L-fatty acids.
So~bean oil was treated in a similar way as de-
scribed above; however, the initial hydrogenation temper-
ature was held at 140C for 2 hours before the tempera-
ture was allowed to rise to 180C after addition of 0.2%
of fresh Ni-on-guhr catalyst for a further 1.5 hours.
After filtration of the catalyst, the hardened bean oil
; had a melting point of 43C, and showed the followlng
fatty acid class composition: ~ = 55%, H = 30%~ M ' oO5%
and L = 14.5%.
~ ~a-~e~eed Oil was hJ-drogenated with 0.3,~ of n^r-
sulphurized active Ni-catalyst at 190C until the final
iodine value was below 1. ~he melting point then was
70C.
20 kg of peruvian fish oil, iodine value 190, was
hydrogenated at 145C in the presence of 0.5% of fresh
Ni-on-guhr catalyst, said catalyst containing 60% of
Ni on dry weight. After 90 minutes the iodine value
had dropped to 150 and the temperature was then allowed
to rise to 180-185C for a further 120 minutes. After
that period the hydrogen gas supply was stopped and the
oil filtered after cooling to 85C under an atmosphere
of carbon dioxide. ~he final iodine value of the harden-
ed fish oil was 70, and the m.p. 41C. ~he fatty acid
oomposltion of the oil was ~ = 40%, H = 40.5% and M r 8%~ -
' '
- - 13 -
, ' ' '
,
c~
l. ~
~i 1045~93
Neutralized and bleached so~bean oil, I.V. 132.8,
was subjected to a first hydrogenation step at 10~C
using 0.1% Ni based on oil as a fresh, nonsulphurized
on-guhr catalyst. After reaching of an iodine value
of 95 and a m.p. of 28.5C, the catalyst was filtered off.
The fatty acid composition of the oil was H = 21%~ ~ =
r 22%, M = 0%.
j Part of this hydrogenated soybean oil was further
! hydrogenated at 1800C after addition of 0 4% of a sulphur-
ized Ni-catalyst up to a m.p. of ~6C. After filtration
the oil had a fatty acid composition of H = 22%, ~ = 56%,
M = 0.
~he composition of the fat blends, expressed in
proportions of fats and fatty acids, as well as t~e di-
~; 15 latometric characteristics are compiled in the accompany-
ing table.
. : .
~:
~".
,: . ' . ' "
'~
'
',
- 14 - ~
. . , ~, . ,
.:
- .. _
1~4~ 3
_ , _
H O I I I I I I I 1~ l l I .
~C d~ o
_ ,,
U~
O I I O I I O I U~ I I o
~ CO
._
~C O I I I
H ~ ~ O ~:)
. __
ID
10 1 1 1 10 1 1 1 1 1 1 1
C~l O ~
_ ... .. _._
~ ~ U~
~ X I I I r- I I I I u~
. ~ o I I I u~ I I I I I 'Q I ~ o ~ ,
_ . __ ' '
U~ O I I ~ I I I
,_1 ~ C~
___ _ : -
IQ I I I I I O I I ~ I I :,
H C\~ .--I O ~1 0
Ii~ . .
~ ~ - '
1~ U~ D I O I I I I I
_~ CO
_ -- . _~
':
I I U~ ~ I I I I I O O
1-1 C~
_ . _ _ . ._
C~ O
_~ O O I I ~ I O O I II I
~ O ~ ~
_ .__ - ___ .
~Q C~
O ~ ~ E~
O O O S~
OD C3 ~ t~ -
1~ ~ ~ 0~ .
~1 C~ S
. ~
O ~ ~ o .
C~ _~ ~1 o rl C'
~ . . ~ O ~ . .
= .
~1 t~ ~ O ~ I
O ~ ., . ~
~1 0 0 td - t~ ~
~d ~ ,~ . ,
~ ~ ~ o ~l ~
O
~ o--l o ~ ~ o ~
O rl ~.rl ~ ~ ~~ O ~ ~ O . . .
~; S~ O ~ C~ O ~ 1 ~ . '.
~ . .
o ~ o bD ~ DO
~ ~ i~ o ~ o o o o h
q~ 0
C ~ o ~ c~
~ O ~ o o ~ td P, hh c
c,~ l X ¢I'~
, , , .. _ ,_, 1 :
- 15 -
.
- . . ~ . . .
-
c L
1~)458~3
_~ . .
H
I ~0~ 1 1 1 1 ~ I I I I ~ O O
U~ U~
l O
...~
~ ~0 1 1 1 1 1 1 1 1 1 1 1 ~ O O
_
.' ~ LOu~IIIIIIIIII c~d~o ..
_ .. .. _ _
H
~ I ~ I I I I I I I I II
~ ~ ~ O O :'
_ : '
~ ~ ~ :'' -.
)D O I I O I I O I I I I ' :-
. ~C ~ ~ ~ ~ a~ ,~ o - :-
_
U~
_~ I I I O O I I I I I I
, ~ C\l ~ O1- 0 C~
O . __ , . . .
C.:l 11~)
_ ~ O O I I O ' I I O I I I I C~ C~l o
U~ ~_1
. ____ : :'
. ` '
O I I I ~ I ~ I I I I I ~ O ~ ~,
_ .
H
H ~ 1
.' X C~l .,
. ~ . '.
~ ~ I I I I O I OI I I I o
C~ ~ ~I CD CU CC ..
.... __ ... __ .. ,
6q ~ O+~ X E-l ~
~ C`~ ~ o~.) . C~
~ CU ~ ~
3 ~ 13 N
O _I _1. o rl O
~ 'o 'o ~ O j~
t-d ~B o ~ I ~)
~o ~
~ ~ o o ~ ~ ~
r~
_I _I rl O rl _I
i~ ~ o ~ ~ ~ ~ ~
l o --l o ~ q
R ~1 ~ rl ~) ~) t~ t~ O ~ ~1 0
o ;-, o ~ c~ o
z ~ a ~
C ~ ~
~ S O ~ D o
O ~ O O O O
n ~ ~ o ~ h
:~ O t~ ~ ~ ~ o
o ~ o o.~ h P, ~
U~ X
- 16 -
' ' ' . ' , ' . ' . '
.
;' . ' . ' , . .
C
10458~3
. . .
o o~~ ~
e e e e ~
. ~ 'O~'O~ ~
.' ~ ~ 5 0
~ '~ u~ 3 U~ i-l ~ O
. ~ . ~q~
O ~1 ~1) '1 ' J ~ ~ +~ O ~ ~
~ O ~ ~.,
., ~ ~ ~C~
~ ~ D
O ~0 ~ ~ ~, ~ ~0 0 o O ~+~
H u~
H I 0 ~1 1 1 1 ~ I O 0
'~ ~ ~ C`J ~ ~ ~ C\l ~ : ~ '
~ _ ~10
V~ ~ O I U~ II I U~ I O ~ 00 ~
!~ ~ ~ r- ~1
~ u~ I o I I I u~ I r- u~ ~0 0
~' _ _
~............................................... ~ .,
,. ~ U~ 1 ~0 1 1 1 0 1 ~0 ~ ~0 0
l'.' . . . _ . : "
, ' O I O I I I O I O 3 1~ ~
~_1 C~ l ~O _l _l
,., _ _ _.
H ~1 C~:~ I II I ~1 ~ ~:
U~
~, ~ ~ l l l O l O ~ ~ O
.. ... _
I_J ~0 1 ~ 0 1 ~O . ..
.
,
' .
- 17 - :::
:
', ,'
, , : . ' ~, .~ :
Cl, 5
1C)~5~3
.~ ~ _ ~ '
.: ~ ~ ~
~ . . o o o
V o ~ o ~ ~ s~ ~
C~ ~ ~ I ~1
~ ~ n a -o ~ O
. ~ O ~ ~ ~ ~ ~ C~
rl O ~ O
o U~ ~ ~Q ~ N ~ +~
~ ~ ~ ~ ~ ~ ~
N ~ ~( ~ 1) ~ ~ ~ ~3 U~
~1 ~ ~ ~ +) ~ ~ ~ O
a O ~ ~ .,,~, ~
O ~ ~ ~0 ~0 ~0 ~0 0 ~ ~
~:1 ~ ~ c~ ~ CJ ~ CO~ O ~ t~ C~, n
,!4 0 C~D ~ bL dl bD ~ Cl~ ;~
O O O O O l ~ ^~
i~ o a ~ h . i~ . O ~ ~ ~
l C)~1 ~ ~ ~, ~ ~, 5 ~, ~ ~, ~ ~ ;~ ~
O v p~ ~ ~q a ~ a ~ a ~ a
.. .__ ___
~ X I N I I I O I O ~Q C~ 11~1
c~ d~ o~ c~ J
_.................... . ._. ._ ,
~-1
k~ c~ I c3 1 1 1 O 11~) 0 -I
X C' ) C~ 0~ C\l ~1 C\l
.. _ _ .... _.__ ,
U~
~d~ I ~ I ~ ¦ ¦ ¦ ~ ~ ~ u~
_ _ C~ ~ ~ ~
~ P~ 0 IQ
~, ~ ~ H d~ I X I I I CD ~ ~ C5
;: X_~ ~ C~ ~
V ... __
~_ H
U~ ~ U~
C~ I ~ I C~ cO~ ~
. . . _ .. _ ___ .
¢ ~ O
P~ H O I O O I I I I u~ ~ C
_ _ .
U~
H C~l I CO l I I C~ 10 O C'U C~
C'' l _l _l r- C~ C~l
. .... _. 1~ - .
~ U~ I O I I IU~ I O O ~ O
X ,~ I CO C~
._ _...... .
~ ~ I O I I I ~ I O O G~ O
_ _
H U~ U~
. ~ ~C O I O I I I I
_
U~ U~
H O I ~ I I IO I ~ ~ c2
P~ _I c~ _I ~O c~
. .... _ _ ...
u~
H O I o I I IO I o c;o u~ co
PC ~ ~ _1 ~ . -1 .
~ O 1 0~ 1 o I I I O cO ~ co
_._ . . _ _ . v_
C~I CO I I C~lI I O O _l~.
c~ ~ c~ oo c~ ,~ c~l
_ . ~ ; ' ' ~
- 18 -
,.
- c ~
1~)45~,~3
...
U~
~~ C~ ~D O I O I O O
~C CU ~ o ~
= ._
o a~ ~ o I oI U~ o
__ ~
P~c~l o d~ O o ~ o u~ o
H i~1 ~J OD C~ C\l O ~ ~
00 1~ 1
_
H u')
H --I X C~l O O O O ~ 0
~ C':1 ~ oOo C`J ~
. _
H U~l
H ~ O O O l!~ O
C~ 1 O O C~
0~ l
___ .
~ U~ : .,
O ~ C~ O O O C~l O ~ ..
1~ _I O d~ 00 ~ c~
t~ I
,_ _
` ~ ~ ~ '
O O ~ C':) O O O O O O
C~ ~ ~ C`~ '. '-
~ _ . ~
~ ~ 0 1- C~ O O O O O O
P~ H e':l --I Cl~ O 00 1~:) H
S ~ 1
~ ._ _ . ~
~ O U~ O O O O O O .:
H ~H ~ 00 CC~
. __ C~ .
H ~0 ~ :
H ~1 ~) 1:~ O O O O O O
_I ~ o cC~
CO ~
_ . . _
11~
i-t ~ ~0 ~ ~ ~ ~ UO~ . '
_ . _ _ ___ , , '
E~ S ~
: ~'
_t In ~ ..
.~ ~ P :' '.:
~d tl~ o " '
CH ~ ~ C~ ~:"
_~ ~ ~t O O O O O O O
C~ ~~ O ~) O U~ O U~ O ':
~o ~) ~ -:'
_ 0~
-- 19 --
Pl.' -
- . - - . - - . . , . . .: : .
.
cL
.
1~)45~93
. ..._
H
~ ~ ~ O O O O O
C~ l C~ ~ C\l O ~
~ U~ U~
~, ~q O 'I ~1 ~ O O O O O
c~ a~
~ r~
._ .. .
U~
~q ~ 1- U~ O I OI O O
~i C~ C~ 1
X U~ U~
H dl 00 ~ O I U~ I 10 11~
:~q c~l a~ o ~:~
H _ . _. . __
H ~ 10
~ ~ O I OI O O
X C`J ~ ~
.
H U~ )
~ 0 10 CO O I U~ I ~ ~
_~ PC ~:) ~I C~ l
~ _ ~
O H 11~110
;~ c~ O I O I ~ 1
_, P~ ~ ~ c" ~ e~J
~ U~
O CD O I U~ I O U~
~1 ~ 0~ ~ O C~l
.~ C
~ ~ U~
H ~ CO ~ ) o I o I ~:) o
C\l _I O ~ O
CD 0~
_.
H
H It~ U:)
X 0~ ~ O I O I ~ U~
~1 _1 C~ ~ ~ IXI
H U~ ~.
~C ~ oo e~l o I o I o
e~l _I ~ ~ ~
~ C':1 _I
_
p ~: '
.^ ~ P ~:
l . . ~
4~1 ~
_I t~ t~l o o o o o o o
O U~ O 10 0 ~ O
td t~ ~:
O ~ _I
E~ ~rl
_
-- 20 --
. : .: .- :
