Europaisches Patentamt | | | | | 1 1| | | | | || ||| || || || | | | | | | |

(19) J European Patent Office

Office europeen des brevets (11) EP 0 905 226 A1

(12) E U R O P E A N PATENT A P P L I C A T I O N

(43) Date of publication:

ation: (5-|) |nt. CI.6: C1 1 D 3/395, C1 1 D 3 / 3 6
31.03.1999 Bulletin 1999/13

(21) Application number: 97870141.5

(22) Date of filing : 19.09.1 997

(84) Designated Contracting States: • Briatore, Andrea

AT BE CH DE DK ES Fl FR GB GR IE IT LI LU MC 17040 Savona (IT)
NLPTSE • Di Capua, Gloria
Designated Extension States: 00040 Ardea (IT)
AL LT LV RO SI
(74) Representative:
(71) Applicant: Engisch, Gautier et al
THE PROCTER & GAMBLE COMPANY BVBA Procter & Gamble Europe SPRL,
Cincinnati, Ohio 45202 (US) Temselaan 100
1853 Strombeek-Bever (BE)
(72) Inventors:
• Scialla, Stefano
00128 Rome (IT)

(54) The use of phosphonate compounds in hypochlorite bleaching compositions for treating
textiles, for fabric whiteness and safety

(57) The present invention relates to the bleaching

of textiles with hypochlorite bleaching compositions
which comprise a phosphonate ingredient, for improved
fabric whiteness and improved fabric safety.

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 EP 0 905 226 A1

Description

Field of the invention

5 [0001 ] The present invention relates to the bleaching of textiles with hypochlorite bleaching compositions.

Background of the invention

[0002] Bleaching compositions are well-known in the art. Amongst the different bleaching compositions available,
10 those relying on bleaching by hypohalite bleaches such as hypochlorite are often preferred, mainly for performance rea-
sons, especially at lower temperature.
[0003] However, a problem encountered with the use of hypochlorite based-compositions is the resulting damage
and/or yellowing of the fabrics being bleached.
[0004] It is therefore an object of the invention to provide a hypohalite-containing composition, suitable for use in laun-
15 dry applications, which provides improved fabric whiteness to fabrics treated therewith.
[0005] It is another object of the invention to provide a hypohalite-containing composition, suitable for use in laundry
applications, which provides improved fabric safety to fabrics treated therewith.
[0006] The Applicant has thus now surprisingly found that this problem is solved by the provision, in a hypohalite
bleaching composition, of a phosphonate ingredient. Indeed, it has been found that improved fabric whiteness and/or
20 safety were obtained with those composition, compared to hypohalite compositions without said phosphonate ingredi-
ent. The benefits are particularly noticeable in hypohalite bleaching compositions which further comprise a pH buffering
component.
[0007] Another advantage of the compositions in the invention is that they are chemically stable. By "chemically sta-
ble", it is meant that the hypohalite bleaching compositions of the present invention should not undergo more than 15%
25 loss of available chlorine after 5 days of storage at 50°C ± 0.5°C. The % loss of available chlorine may be measured
using the method described, for instance, in "Analyses des Eaux et Extraits de Javel" by "La chambre syndicale nation-
ale de L'eau de Javel et des produits connexes", pages 9-10 (1984). Said method consists in measuring the available
chlorine in the fresh compositions, i.e. just after they are made, and in the same compositions after 5 days at 50°C.
[0008] A further advantage of the compositions in the invention is that they are suitable for the bleaching of different
30 types of fabrics including natural fabrics (e.g., fabrics made of cotton, viscose, linen, silk and wool), synthetic fabrics
such as those made of polymeric fibers of synthetic origin as well as those made of both natural and synthetic fibers.
Indeed, the compositions in the present invention may be used on synthetic fibers despite a standing prejudice against
the use of hypohalite beaches, especially hypochlorite beaches, on synthetic fibers, as evidenced by warning on labels
of commercially available hypochlorite beaches and clothes.
35 [0009] EP 0 743 250 discloses a process producing bleaching compositions comprising phosphonates. J07-1 09, 107
discloses compositions comprising hypochlorite and a phosphonate ingredient. None of these prior art documents dis-
closes the fabric whiteness and safety benefits obtained from the provision of a phosphonate ingredient in a hypochlo-
rite composition.

40 Summary of the invention

[0010] The present invention encompasses the use, in a hypohalite bleaching composition, of a phosphonate ingre-
dient, for providing improved fabric whiteness and/or safety to the fabrics treated therewith.

45 Detailed description of the invention

[001 1] According to the invention, there is provided the use, in a hypohalite bleaching composition, of a phosphonate
ingredient for providing improved whiteness and/or safety to the fabrics treated therewith. By "improved whiteness
and/or safety", it is meant that hypohalite bleaching compositions, with the phosphonate ingredient, provide better
so whiteness, i.e. less yellowing, and/or fabric safety compared to hypohalite bleaching compositions which do not com-
prise said phosphonate ingredient. The presence of a pH buffering component in the bleaching composition is not com-
pulsory, but is highly preferred.

Hypohalite bleach
55
[001 2] An essential component of the invention is a hypohalite bleach. Hypohalite beaches may be provided by a vari-
ety of sources, including bleaches that are oxidative beaches and subsequently lead to the formation of positive halide
ions as well as bleaches that are organic based sources of halides such as chloroisocyanurates.

2
 EP 0 905 226 A1

[0013] Suitable hypohalite bleaches for use herein include the alkali metal and alkaline earth metal hypochlorites,
hypobromites, hypoiodites, chlorinated trisodium phosphate dodecahydrates, potassium and sodium dichloroisocyanu-
rates, potassium and sodium trichlorocyanurates, N-chloroimides, N-chloroamides, N-chloroamines and chlorohydan-
toins.
5 [0014] For liquid compositions, the preferred hypohalite bleaches among the above described are the alkali metal
and/or alkaline earth metal hypochlorites selected from the group consisting of sodium, potassium, magnesium, lithium
and calcium hypochlorites, and mixtures thereof, more preferably the alkali metal sodium hypochlorite.
[0015] For solid compositions, the preferred hypohalite bleaches among the above described are the alkali metal
and/or alkaline earth metal hypochlorites selected from the group consisting of lithium hypochlorites, calcium hypochlo-
10 rites, chlorinated trisodium phosphate dodecahydrates, potassium dichloroisocyanurates, sodium dichloroisocyanu-
rates, potassium trichlorocyanurates, sodium trichlorocyanurates, and mixtures thereof, more preferably sodium
dichloroisocyanurates and/or calcium hypochlorite.
[001 6] Preferably, the liquid compositions in the present invention comprise said hypohalite bleach such that the con-
tent of active halide in the composition is of from 0.1% to 20% by weight, more preferably from 2% to 8% by weight,
15 most preferably from 3% to 6% by weight of the composition.
[0017] Preferably, the solid compositions in the present invention comprise said hypohalite bleach such that the con-
tent of active halide in the composition is of from 20% to 95% by weight, more preferably from 25% to 60% by weight of
the composition.

20 Phosphonate ingredient

[0018] Suitable phosphonates for use herein are according to the formula :

Ri OM
25

R2 C P = 0

30
R3 OM

35
where M is H or an alkali metal,
where R-|, R2 and R3 independently are:

-P03M2; or
40 - -H;or
- -OH; or
a hydrocarbon chain or cycle, optionally saturated, optionally substituted with one or several amino, oxy, amin-
eoxy, phosphonic, sulphonic or alkoxy group, or mixtures thereof, said chain having of from 1 to 20 carbon
atoms; or
45 - -NR4R5, where R4 and R5 independently are :
-P03M2; or
- -H;or
- -OH; or
a hydrocarbon chain or cycle, optionally saturated, optionally substituted with one or several amino, oxy, amin-
50 eoxy, phosphonic, sulphonic or alkoxy group, or mixtures thereof, said chain having of from 1 to 20 carbon
atoms.

[0019] Such phosphonates may include ethydronic acid, hydroxy-ethane diphosphonic acid (HEDP) as well as ami-
nophosphonate compounds, including amino alkylene poly (alkylene phosphonate), alkali metal ethane 1-hydroxy
55 diphosphonates, nitrilo trimethylene phosphonates, ethylene diamine tetra methylene phosphonates, diethylene tri-
amine penta methylene phosphonates and ethylenedinitrilotetrakis (methylenephosphonic acid) N,N-oxide. The phos-
phonate compounds may be present either in their acid form or as salts of different cations on some or all of their acid
functionalities.

3
 EP 0 905 226 A1

[0020] Many of the suitable phosphonates suitable for use herein are aminophosphonates, while the amino group is
somewhat unstable in a hypochlorite matrix. Accordingly stablized aminophosphonates are preferably used where the
amino group is transformed into an N-oxide group, which in turn is stable to hypochlorite.
[0021] Preferred phosphonates for use herein are those produced by Monsanto under the tradename - Dequest® -
5 and by Bozzetto under the tradename - Sequion® - and, among them, preferred are HEDP (hydroxy-ethane diphospho-
nate) and ATMP (amino trimethylenephosphonate) including their N-oxidyzed version, and most preferred is ATMP N-
oxide by Bozzetto (Sequion®CLR).
[0022] The phosphonate ingredients herein are present in amounts of from 0.001% to 20%, preferably 0.005% to 5%,
most preferably 0.005% to 1% by weight of the total composition. Of course, mixtures of different phosphonate ingredi-
10 ents can be used.
[0023] The whitening effect, i.e. the yellowing-prevention effect, and /use of safety effect of the present invention can
be evaluated by comparing the composition according to the present invention to the use of the same composition with-
out the phosphonate ingredient.
[0024] The degree of yellowing can be determined by both visual and instumental grading. Visually, the difference in
15 yellowing between items treated with different compositions can be determined by a team of expert panelists. Instru-
mentally, the assessment can be determined with the help of Colorimeters such as Ganz Griesser® instruments (e.g.,
Datacolor® Spectraflash® SF 500, Machbet White-eye® 500) or a ZEISS ELREPHO® or others which are available
for instance from Hunterlab® or Gardner®.
[0025] Fabric safety may be evaluated by different test methods including the degree of polymerisation test method
20 according to UNI (Ente Nazionale Italiano di Unificazione) official method UNI 8282-Determinazione del la viscosita
intrinseca in soluzione di cuprietilendiammina (CED).
[0026] The compositions in the present invention are either in liquid or solid form. Solid forms include forms such as
powders, tablets and granules. Preferably, the compositions of the invention are in liquid aqueous form. More preferably,
they comprise water in an amount of from 60% to 98% by weight, more preferably of from 80% to 97% and most pref-
25 erably of from 85% to 97% by weight of the total aqueous liquid bleaching composition.

pH buffering component

[0027] A pH buffering component is an optional but highly preferred component for the compositions in the invention.
30 The pH buffering component ensures that the pH of the composition is buffered to a pH value ranging from 7.5 to 13,
preferably from 8 to 12, more preferably from 8.5 to 11.5 after the composition has been diluted into 1 to 500 times its
weight of water.
[0028] Suitable pH buffering components for use herein are selected from the group consisting of alkali metal salts of
carbonates, polycarbonates, sesquicarbonates, silicates, polysilicates, borates, metaborates, phosphates, stannates,
35 alluminates and mixtures thereof, and preferably are selected from the group consisting of sodium carbonate, sodium
silicate, sodium borate, and mixtures thereof.
[0029] The raw materials involved in the preparation of hypohalite bleaches usually contain by-products, e.g calcium
carbonate resulting in an amount of up to 0.4% by weight of by-product within the hypohalite composition. However, at
such amount, the by-product will not have the buffering action defined above.
40 [0030] Liquid bleaching compositions herein will contain an amount of pH buffering component of from 0.5% to 9%
by weight, preferably from 0.5% to 5% by weight, and more preferably in an amount of from 0.6% to 3% by weight of
the composition.
[0031] Solid bleaching compositions herein will preferably contain an amount of pH buffering component of from 3%
to 30% by weight, more preferably from 5% to 25% by weight, and most preferably in an amount of from 10% to 20%
45 by weight of the composition.

pH

[0032] The pH of the liquid compositions in the present invention, as is, is typically from 12 to 14 measured at 25°C.
so Solid compositions or liquid compositions of the invention have a pH of from 7.5 to 13, preferably from 8 to 12, more
preferably from 8.5 to 11.5, when diluted into 1 to 500 times its weight of water. It is in this alkaline range that the opti-
mum stability and performance of the hypohalite as well as fabric whiteness and/or safety are obtained. The pH range
is suitably provided by the pH buffering component and the hypohalite bleach mentioned hereinbefore, which are alka-
lis. However, in addition to these components, a strong source of alkalinity may also optionally be used.
55 [0033] Suitable sources of alkalinity are the caustic alkalis such as sodium hydroxide, potassium hydroxide and/or
lithium hydroxide, and/or the alkali metal oxides such as sodium and/or potassium oxide. A preferred strong source of
alkalinity is a caustic alkali, more preferably sodium hydroxide and/or potassium hydroxide. Typical levels of such caus-
tic alkalis, when present, are of from 0.1% to 1.5% by weight, preferably from 0.5% to 1.5% by weight of the composi-

4
 EP 0 905 226 A1

tion.

Optional polymers

5 [0034] An optional component of the compositions herein is a polymer. That polymer, has surprisingly been found to
also reduce the yellowing of the fabrics treated therewith, i.e. improve whiteness, as well as improve fabric safety. Nat-
urally, for the purpose of the invention, the polymer has to be stable to the hypohalite bleach.
[0035] Suitable polymers for use are polymers comprising monomeric units selected from the group consisting of
unsaturated carboxylic acids, polycarboxylic acids, sulphonic acids, phosphonic acids and mixtures thereof. Co-polym-
10 erisation of the above monomeric units among them or with other co-monomers such as styrenesulfonic acid is also
suitable.
[0036] Preferred examples of such polymers are the polymers and co-polymers of monomeric units selected from the
group consisting of acrylic acid, maleic acid, vinylsulphonic acid and mixtures thereof. Also suitable for use herein are
the above mentioned polymers and co-polymers which are modified in order to contain other functional groups such as
15 aminophosphonic and/or phosphonic units. More preferred polymers are selected from the group consisting of polyacr-
ylate polymers, co-polymers of acrylic and maleic acid, co-polymers of styrene sulphonic acid and maleic acid, and mix-
tures thereof, preferably modified with aminophosphonic and/or phosphonic groups.
[0037] The molecular weight for these polymers and co-polymers is preferably below 100,000, most preferably
between 500 and 50,000. Most suitable polymers and co-polymers for use herein will be soluble in an amount up to
20 0.1% by weight, in an aqueous composition comprising 5% by weight of sodium hypochlorite with its pH adjusted to 13
with sodium hydroxide.
[0038] Commercially available such polymers, suitable for use herein, are the polyacrylate polymers sold under the
tradename Good-Rite® from BF Goodrich, Acrysol® from Rohm & Haas, Sokalan® from BASF, Norasol® from Norso
Haas. Also suitable for use herein are the co-polymers of styrene sulphonic acid and maleic acid, commercially availa-
25 ble under the tradename Versaf lex® from National Starch such as Versaf lex 157, as well as Acumer® terpolymers from
Rohm and Haas, in particular Acumer® 3100. Preferred commercially available polymers are the polyacrylate poly-
mers, especially the Norasol® polyacrylate polymers and more preferred are the polyacrylate polymer Norasol® 41 ON
(MW 10,000) and the polyacrylate polymer modified with phosphonic groups Norasol® 440N (MW 4000) and its corre-
sponding acid form Norasol® QR 784 (MW 4000).
30 [0039] A preferred polymer for use herein is a polyacrylate polymer modified with phosphonic groups commercially
available under the tradename Norasol® 440N (MW 4000) and its corresponding acid form Norasol® QR 784 (MW
4000) from Norso- Haas.
[0040] Mixtures of polymers as herein described may also be used in the present invention.
[0041] Polymers herein are preferably present in low amounts, i.e. in amounts of up to 0.5% by weight, more prefer-
35 ably from 0.001% to 0.3% by weight, most preferably from 0.005% to 0.2% by weight of the liquid composition.

Optional phosphates

[0042] An optional component of the compositions herein is a phosphate. That phosphate has surprisingly been found
40 to also reduce the yellowing of the fabrics treated therewith, i.e. improve whiteness, as well as improve fabric safety.
Suitable phoshates for use herein are :

linear or branched polyphosphates of structure

45 0 O

II II
MO - P 0 p OM

50 n
MO OR

55
when R is M or

5
 EP 0 905 226 A1

o
II
-.0 _P ■OM
I m
OR

10

when M is a counterion, preferably alkali metal;

when O <, n+m < 500 (if n+m = 0 then the compound is phosphonic acid)

15 cyclic polyphosphates (also referred to as metaphosphates), of structure

0 0
II II
20
P - 0 P - 0
I
OM OR
25

where R is M or
30
o
.,

0 - P OM
35
I m
OR

40 o
II
if R is - O - P OM,
45 m
OR

the phosphate compound contains both cycles and branched chain, and can be referred to as an ultraphos-
50 phate.)
where M is a counterion, preferably an alkali metal
where O <, n+m < 500

[0043] All such phosphate ingredients are suitable for use herein, and preferred are linear phosphate ingredients (i.e.
55 R is M) where n is 1 (pyrophosphate) and n is 2 (tripolyphosphate), most preferably where n is 2. The most commonly
available form of these phosphate is where M is Sodium.
[0044] The phosphate ingredients herein can be present herein in amounts of from 0.001% to 20%, preferably 0.005%
to 5%, most preferably 0.005% to 1% by weight of the total composition. Of course, mixtures of different phosphate

6
 EP 0 905 226 A1

ingredients can be used.

[0045] The composition in the invention may also comprise further optional components such as perfumes, bleach-
stable surfactants, organic or inorganic alkalis, pigments, dyes, optical brighteners, solvents, cheating agents, radical
scavengers and mixtures thereof.
5 [0046] Preferably, the compositions in the invention are used in diluted form in laundry applications. The expression
"used in diluted form" herein includes dilution by the user, which occurs for instance in hand laundry applications, as
well as dilution by other means, such as in a washing machine. Preferably, the composition is diluted into 5 to 500 times
its weight of water for hand laundry application and 10 to 500 times its weight of water in a washing machine.
[0047] The invention is illustrated in the following non-limiting examples, in which all percentages are on a weight
10 basis unless otherwise stated.

Examples

[0048]

Composition (weight %) 1 2 3 4 5
Sodium hypochlorite 5.0 5.0 3.5 3.5 5
Sodium hydroxide 1 1.5 1 1.5 0.8
Sodium carbonate 1 2 2 1.5 2
Sodium silicate - - 0.5 0.5 0.5
Sodium metaborate 1 . . . .
Sequion® CLR (N-oxydized aminotrimethylenephoshonate 0.1 0.1 0.1 0.1 0.1
HEDP (Hydroxyethane diphosphonic acid) . . . . .
STTP . . . . .
Norasol 440N . . . . .
Water and minors up to 100%

Composition (weight %) 6 7 8 9 10
Sodium hypochlorite 5.0 5.0 3.5 3.5 5
Sodium hydroxide 1 1.5 1 1.5 0.8
Sodium carbonate 1 2 2 1.5 2
Sodium silicate - - 0.5 0.5 0.5
Sodium metaborate 1 . . . .
Sequion® CLR (N-oxydized aminotrimethylenephosphonate) 0.05 0.1 0.05 0.1 0.1
HEDP (Hydroxyethane diphosphonic acid) 0.05 0.02
STTP 0.05 -0 0.05 - 0.02
Norasol 440N 0.05 - - 0.05 0.02
Water and minors up to 100%

Claims

55 1. The use, in a hypohalite bleaching composition, of a phosphonate ingredient, for providing improved whiteness
and/or safety to the fabrics treated therewith.

2. The use according to claim 1 wherein said composition further comprises a pH buffering component.

7
 EP 0 905 226 A1

3. The use according to claim 2, wherein said pH buffering component is selected from the group consisting of alkali
metal salts of carbonates, polycarbonates, sesquicarbonates, silicates, polysilicates, borates, metaborates, phos-
phates, stannates, alluminates, and mixtures thereof.

4. The use according to claim 3, wherein said pH buffering component is selected from the group consisting of sodium
carbonate, sodium silicates, sodium borate, and mixtures thereof.

5. The use according to claims 2-4, wherein said pH buffering component is in an amount of from 0.5% to 9% by
weight, preferably 0.5% to 5% by weight of the liquid composition or in an amount of from 3% to 30% by weight,
preferably from 5% to 25% by weight of the solid composition.

6. The use according to any one of claims 1-5, wherein said hypohalite bleach is, for liquid bleaching compositions,
an alkali metal sodium hypochlorite or, for solid compositions, sodium dichloroisocyanurate and/or calcium
hypochlorite.

7. The use according to any one of claims 1-6, wherein said hypohalite, based on active halide, is present in an
amount of from 0.1% to 20% by weight, preferably from 2% to 8% by weight of the liquid composition or in an
amount of from 20% to 95% by weight, preferably from 25% to 60% by weight of the solid composition.

8. The use according to any one of claims 1-7, wherein said composition further comprises a strong source of alka-
linity.

9. The use according to any one of claims 1-8, wherein said phosphonate ingredient is of structure :

Pm OM
I I
R2 — C — P = 0
I I
R3 OM

where M is H or an alkali metal;

where R-|, R2 and R3 independently are :
-P03M2; or
- -H;or
- -OH; or
a hydrogen chain or cycle, optionally saturated, optionally substituted with one or several amino, oxy, amineoxy,
phosphonic, sulphonic or alkoxy group, or mixtures thereof, said chain having from 1 to 20 carbon atoms; or
-NR4R5, where R4 and R5 independently are :
-P03M2; or
- -H;or
- -OH; or
a hydrocarbon chain or cycle, optionally saturated, optionally substituted with one or several amino, oxy, amin-
eoxy, phosphonic, sulphonic or alkoxy group, or mixtures thereof, said chain having of from 1 to 20 carbon
atoms.

10. The use according to any of the preceding claims, wherein said composition comprises from 0.001% to 20%, pref-
erably from 0.005% to 5%, most preferably from 0.01% to 1% of said phosphonate ingredient.

11. The use according to any of the preceding claims, wherein said composition further comprises a polymer.

12. The use according to any of the preceding claims wherein said composition further comprises a phosphate.

8
 EP 0 905 226 A1

European Patent Application Number

EUROPEAN SEARCH REPORT
Office EP 97 87 0141

DOCUMENTS CONSIDERED TO BE RELEVANT

Category Citation of document with indication, where appropriate, Relevant CLASSIFICATION OFTHE
of relevant passages to claim APPLICATION (lnt.CI.6)
EP 0 743 280 A (THE PROCTER & GAMBLE CO. ) 1-10,12 C11D3/395
20 November 1996 C11D3/36
* the whole document *

US 3 297 578 A (CRUTCHFIELD M.M. ET AL. ) 1-10,12

10 January 1967
* the whole document *

US 3 629 124 A (KING THOMAS M. ) 1-10,12

21 December 1971
* the whole document *

EP 0 743 279 A (THE PROCTER & GAMBLE CO. ) 1-8

20 November 1996
* claims 1,6-9 *

EP 0 668 345 A (THE PROCTER & GAMBLE CO. ) -8

23 August 1995

US 3 740 187 A (K0WALSKI X. ) ,6,9,12

19 June 1973 TECHNICAL FIELDS
* column 2, line 21 - line 57 * SEARCHED (lnt.CI.6)
CUD
US 3 391 083 A (IRANI RIYAD R. ET AL. ) 1-6,8,9
2 July 1968
* column 7, line 3 - 1 i ne 55 *

D,A DATABASE WPI 1,6,9

Section Ch, Week 9525
Derwent Publications Ltd., London, GB;
Class A14, AN 95-190679
XP002055523
& JP 07 109 107 A (NIPPON PEROXIDE CO LTD)
, 25 April 1995
* abstract *

-/--

The present search report has been drawn up for all claims
Place ofsearch Dateofcompletionofthe search Examiner
THE HAGUE 17 February 1998 Serbetsoglou, A
CATEGORY OFCITED DOCUMENTS T: theory or principle underlying the invention
E: earlier patent document, but published on, or
X: particularly relevant if taken alone after the filing date
Y: particularly relevant if combined with another D: document cited in the application
document of the same category L: document cited for other reasons
A: technological background
O: non-written disclosure &: member of the same patent family, corresponding
P : intermediate document document

9
 EP 0 905 226 A1

J European Patent Application Number

EUROPEAN SEARCH REPORT
Office EP 97 87 0141

DOCUMENTS CONSIDERED TO BE RELEVANT

Category Citation of document with indication, where appropriate, Relevant CLASSIFICATION OFTHE
of relevant passages to claim APPLICATION (lnt.CI.6)
EP 0 509 382 A (W. R. GRACE & CO.) 21 1,6,9
October 1992
* page 2, line 21 - page 4, line 49 *

TECHNICAL FIELDS
SEARCHED (lnt.CI.6)

The present search report has been drawn up for all claims
Place ofsearch Dateofcompletionofthe search Examiner
THE HAGUE 17 February 1998 Serbetsoglou, A
CATEGORYOFCITED DOCUMENTS T: theory or principle underlying the invention
E: earlier patent document, but published on, or
X: particularly relsvant iftaken alone after the filing date
Y: particularly relevant if combined with another D: document cited in the application
document of the same category L: document cited for other reasons
A: technological background
0 : non-written disclosure &: member of the same patent family, corresponding
P : intermediate document document

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