US3761262A - Photographic color developing process - Google Patents
Photographic color developing process Download PDFInfo
- Publication number
- US3761262A US3761262A US00172891A US3761262DA US3761262A US 3761262 A US3761262 A US 3761262A US 00172891 A US00172891 A US 00172891A US 3761262D A US3761262D A US 3761262DA US 3761262 A US3761262 A US 3761262A
- Authority
- US
- United States
- Prior art keywords
- color
- bleach
- bleaching
- bath
- fixing
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime
Links
- 238000000034 method Methods 0.000 title description 12
- 238000004061 bleaching Methods 0.000 abstract description 24
- 230000015572 biosynthetic process Effects 0.000 abstract description 7
- 230000003647 oxidation Effects 0.000 abstract description 6
- 238000007254 oxidation reaction Methods 0.000 abstract description 6
- DHCDFWKWKRSZHF-UHFFFAOYSA-N sulfurothioic S-acid Chemical compound OS(O)(=O)=S DHCDFWKWKRSZHF-UHFFFAOYSA-N 0.000 abstract description 3
- 239000000463 material Substances 0.000 description 16
- 229910052709 silver Inorganic materials 0.000 description 12
- 239000004332 silver Substances 0.000 description 12
- 239000000126 substance Substances 0.000 description 10
- 239000007844 bleaching agent Substances 0.000 description 8
- -1 silver halide Chemical class 0.000 description 8
- 239000000839 emulsion Substances 0.000 description 7
- XYXNTHIYBIDHGM-UHFFFAOYSA-N ammonium thiosulfate Chemical compound [NH4+].[NH4+].[O-]S([O-])(=O)=S XYXNTHIYBIDHGM-UHFFFAOYSA-N 0.000 description 6
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 5
- 150000001875 compounds Chemical class 0.000 description 5
- 239000007800 oxidant agent Substances 0.000 description 5
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 4
- 229910052708 sodium Inorganic materials 0.000 description 4
- 239000011734 sodium Substances 0.000 description 4
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- 229960001484 edetic acid Drugs 0.000 description 3
- GGCZERPQGJTIQP-UHFFFAOYSA-N sodium;9,10-dioxoanthracene-2-sulfonic acid Chemical compound [Na+].C1=CC=C2C(=O)C3=CC(S(=O)(=O)O)=CC=C3C(=O)C2=C1 GGCZERPQGJTIQP-UHFFFAOYSA-N 0.000 description 3
- 229940101006 anhydrous sodium sulfite Drugs 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 2
- IOLCXVTUBQKXJR-UHFFFAOYSA-M potassium bromide Chemical compound [K+].[Br-] IOLCXVTUBQKXJR-UHFFFAOYSA-M 0.000 description 2
- BWHMMNNQKKPAPP-UHFFFAOYSA-L potassium carbonate Chemical compound [K+].[K+].[O-]C([O-])=O BWHMMNNQKKPAPP-UHFFFAOYSA-L 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- GEHJYWRUCIMESM-UHFFFAOYSA-L sodium sulfite Chemical compound [Na+].[Na+].[O-]S([O-])=O GEHJYWRUCIMESM-UHFFFAOYSA-L 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- CBCKQZAAMUWICA-UHFFFAOYSA-N 1,4-phenylenediamine Chemical compound NC1=CC=C(N)C=C1 CBCKQZAAMUWICA-UHFFFAOYSA-N 0.000 description 1
- CDAWCLOXVUBKRW-UHFFFAOYSA-N 2-aminophenol Chemical class NC1=CC=CC=C1O CDAWCLOXVUBKRW-UHFFFAOYSA-N 0.000 description 1
- OURXRFYZEOUCRM-UHFFFAOYSA-N 4-hydroxymorpholine Chemical compound ON1CCOCC1 OURXRFYZEOUCRM-UHFFFAOYSA-N 0.000 description 1
- QXNVGIXVLWOKEQ-UHFFFAOYSA-N Disodium Chemical class [Na][Na] QXNVGIXVLWOKEQ-UHFFFAOYSA-N 0.000 description 1
- WTDHULULXKLSOZ-UHFFFAOYSA-N Hydroxylamine hydrochloride Chemical compound Cl.ON WTDHULULXKLSOZ-UHFFFAOYSA-N 0.000 description 1
- 229910021578 Iron(III) chloride Inorganic materials 0.000 description 1
- 125000003545 alkoxy group Chemical group 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 150000001491 aromatic compounds Chemical class 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 125000004432 carbon atom Chemical group C* 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 150000002367 halogens Chemical group 0.000 description 1
- RBTARNINKXHZNM-UHFFFAOYSA-K iron trichloride Chemical compound Cl[Fe](Cl)Cl RBTARNINKXHZNM-UHFFFAOYSA-K 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- MKQLBNJQQZRQJU-UHFFFAOYSA-N morpholin-4-amine Chemical compound NN1CCOCC1 MKQLBNJQQZRQJU-UHFFFAOYSA-N 0.000 description 1
- 125000000449 nitro group Chemical group [O-][N+](*)=O 0.000 description 1
- 229910000027 potassium carbonate Inorganic materials 0.000 description 1
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 description 1
- NDGRWYRVNANFNB-UHFFFAOYSA-N pyrazolidin-3-one Chemical class O=C1CCNN1 NDGRWYRVNANFNB-UHFFFAOYSA-N 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 150000003378 silver Chemical class 0.000 description 1
- AKHNMLFCWUSKQB-UHFFFAOYSA-L sodium thiosulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=S AKHNMLFCWUSKQB-UHFFFAOYSA-L 0.000 description 1
- 235000019345 sodium thiosulphate Nutrition 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 230000003019 stabilising effect Effects 0.000 description 1
Classifications
-
- G—PHYSICS
- G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
- G03C—PHOTOSENSITIVE MATERIALS FOR PHOTOGRAPHIC PURPOSES; PHOTOGRAPHIC PROCESSES, e.g. CINE, X-RAY, COLOUR, STEREO-PHOTOGRAPHIC PROCESSES; AUXILIARY PROCESSES IN PHOTOGRAPHY
- G03C7/00—Multicolour photographic processes or agents therefor; Regeneration of such processing agents; Photosensitive materials for multicolour processes
- G03C7/30—Colour processes using colour-coupling substances; Materials therefor; Preparing or processing such materials
- G03C7/42—Bleach-fixing or agents therefor ; Desilvering processes
- G03C7/421—Additives other than bleaching or fixing agents
Definitions
- This invention relates to a photographic color developing process, more particularly a rapid-processing technique, using aromatic sulfhydrazides as agents to prevent the formation of fog upon bleaching.
- the compounds used according to the invention can of course also be used in the conventional processing of color photographic materials, in which case intermediate rinsing is usually carried out between the developer bath, the bleaching bath and fixing bath, or the bleach-fixing bath.
- intermediate rinsing is usually carried out between the developer bath, the bleaching bath and fixing bath, or the bleach-fixing bath.
- rapid-processing which is preferably carried out at slightly elevated temperatures and in which intermediate rinsing should if possible be avoided.
- a strong bleach fog is usually formed.
- the substances used according to the inven tion however, it is effectively suppressed.
- the sulfhydrazides can be used with particular advantage in processing machines of low bath volume, for example table-top machines.
- the bleaching baths normally used in color-photography can be used as bleaching or bleach-fixing baths.
- the bleaching substances are generally oxidizing agents which are able to oxidize any metallic silver present in the developed photographic material into the silver salt.
- Preferred bleaching agents include ferric compounds, for example ferric chloride, potassium ferricyanide or the ferric salt of ethylene diamine tetraacetic acid.
- Photographic bleach-fixing baths are baths in which bleaching oxidizing agents are combined with a solvent for silver salts, such as sodium thiosulfate or ammonium thiosulfate. Other complex-forming agents can also be present. Treatment with a bleaching and fixing bath not only oxidizes the metallic silver into the silver salt, it also subsequently dissolves the resulting silver salt from the layer as well. Bleaching and bleach-fixing baths are adequately known in photography. Reference is made for example to H. Berger, Agfacolor, 6th edition, pages 260 and 262; and E. Mutter, Dietician und Angewandte Photographie, vol. IV (1967), pages 348, 352, 353 and 362.
- the bleach fixing baths according to the invention preferably contain from 100 to 200 g. per litre of sodium or ammonium thiosulfate.
- White couplers are substances that are able to react with color-forming developer oxidation products without forming a dye.
- White couplers are known per se, for example from German patent specification No. 1,155,675. Reference is also made to the publication by W. Piischel in Mitteilungen aus den Anlagenslaboratorien der Agfa- Gevaert AG, vol. IV, page 352 (1964).
- bleachfixing baths which, in addition to the sulfhydrazides and an increased thiosulfate content, contain from 1 to g. of a white coupler substance per litre.
- An exposed color-photographic multi-layer material including a blue sensitive silver halide emulsion layer having a yellow color coupler, a green sensitive silver halide emulsion layer containing a magenta color coupler and a red sensitive silver halide emulsion layer with a cyan color coupler was developed for 50 seconds at 40 C. in a developer of the following composition:
- the material was then squeezed and treated for 60 seconds at 40 C. with the following bleach-fixing bath:
- the material was then washed, treated with a conventional stabilising bath and dried.
- the processed material showed extremely low dye-fog values which were comparable with the fog values obtainable in conventional processing, whilst a material processed in the manner described above, but using a conventional bleach-fixing bath from which the sulfhydrazide was absent, instead of the aforementioned bleach-fixing bath, showed excessively high fogging.
- R represents hydrogen, nitro or carboxyl and R represents hydrogen, halogen, or alkyl or alkoxy having up to three carbon atoms, the amount of sulfhydrazide being such that it reduces the formation of color fog during the bleaching.
Landscapes
- Physics & Mathematics (AREA)
- General Physics & Mathematics (AREA)
- Silver Salt Photography Or Processing Solution Therefor (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
THE FORMATION OF COLOR FOG DURING THE BLEACHING STEP OF COLOR PROCESSING, PARTICULARLY RAPID COLOR PROCESSING, IS SUSPRESSED BY INCLUDING CERTAIN SULFHYDRAZIDES IN THE BLEACH, BATH, AND PREFERABLY FURTHER ADDING A LARGE QUANTITY OF THIOSULFATE AS WELL AS A COLOR COUPLER THAT COUPLES WITH DEVELOPER OXIDATION PRODUCTS WITHOUT FORMING A DYE.
Description
United States Patent Office PHOTOGRAPHIC COLOR DEVELOPING PROCESS Karl-Wilhelm Schranz, Opladen, and Erwin Schiin and Wolfgang Hiinicke, Leverkusen, Germany, assignors to Agfa-Gevaert Aktiengesellschaft, Leverkusen, Germany No Drawing. Filed Aug. 18, 1971, Ser. No. 172,891 Claims priority, application Germany, Aug. 20, 1970,
P 20 41 325.6 Int. Cl. G03c 5/00, 5/38, 5/44 US. C]. 96-22 6 Claims ABSTRACT OF THE DISCLOSURE The formation of color fog during the bleaching step of color processing, particularly rapid color processing, is suppressed by including certain sulfhydrazides in the bleach bath, and preferably further adding a large quantity of thiosulfate as well as a color coupler that couples with developer oxidation products without forming a dye.
This invention relates to a photographic color developing process, more particularly a rapid-processing technique, using aromatic sulfhydrazides as agents to prevent the formation of fog upon bleaching.
It is known to produce color-photographic images by color-forming development of exposed silver halide emulsion layers in the presence of suitable color couplers capable of reaction with the oxidation product of the color-forming developer substance, to form a dye image. Aromatic compounds containing primary amino groups, especially those of the p-phenylene diamine type, are normally used as color-forming developers. After color development, the photographic material has to be treated with a bleaching bath and a fixing bath, or with a bleachfixing bath, in order to remove image silver and any silver halide still present after development. The bleaching substances used are oxidizing agents which not only oxidize the image silver but also some residual color developers that are still present in the photographic emulsion after the development operation. This oxidation, in the presence of color couplers, leads to undesired formation of a dyefog of azomethine or indoquinone dye, referred to below as bleach fog.
To avoid this defect in processing, it is known to rinse the developed material rising rinsing times that are long in relation to the total processing time after development, or alternatively the material has to be pretreated with a stopping, or stopping and fixing bath, before the bleaching or bleach-fixing operation. Both these measures are obstacles to quick processing in the true sense and involve additional costs. Another method is to carry out the bleaching or bleach-fixing operation in the presence of special substances which inhibit formation of bleach fog. Examples of compounds that have been recommended for this purpose include N-hydroxymorpholine, N-amino morpholine, certain 3-pyrazolidone derivatives and certain amino-phenol derivatives; unfortunately, these compounds are relatively unstable in the bleaching or bleachfixing bath, or if they are sufficiently stable, they are not sufficiently active.
It is among the objects of the present invention to provide improved anti-foggants for the bleaching bath to prevent formation of the bleach fog.
We have now found a photographic process for making color-photographic images including color development of an image-wise-exposed color photographic material comprising at least one silver halide emulsion layer, bleaching and fixing or bleach-fixing, wherein bleaching or bleach-fixing is performed in the presence of an aro- 3,761,262 Patented Sept. 25, 1973 matic sulfhydrazide corresponding to the following formula R1 4 SO2NH-NH2 R The aforementioned substances are added to the bleaching or bleach-fixing bath in quantities of preferably from 0.5 to 10 g. per litre. It is also possible to briefly treat the developed material with an aqueous solution of the compound according to the invention before bleaching. In this instance, it is advisable to employ a relatively high concentration of the sulfhydrazides in the pretreatment bath. Useful results are obtained for example with aqueous pretreatment baths containing from 5 to 50 g. per litre of the sulfhydrazides.
The compounds used according to the invention can of course also be used in the conventional processing of color photographic materials, in which case intermediate rinsing is usually carried out between the developer bath, the bleaching bath and fixing bath, or the bleach-fixing bath. However, they can be used with particular advantage in so-called rapid-processing, which is preferably carried out at slightly elevated temperatures and in which intermediate rinsing should if possible be avoided. In such a process, a strong bleach fog is usually formed. In the presence of the substances used according to the inven tion, however, it is effectively suppressed.
The sulfhydrazides can be used with particular advantage in processing machines of low bath volume, for example table-top machines.
The bleaching baths normally used in color-photography can be used as bleaching or bleach-fixing baths. The bleaching substances are generally oxidizing agents which are able to oxidize any metallic silver present in the developed photographic material into the silver salt.
Preferred bleaching agents include ferric compounds, for example ferric chloride, potassium ferricyanide or the ferric salt of ethylene diamine tetraacetic acid.
Photographic bleach-fixing baths are baths in which bleaching oxidizing agents are combined with a solvent for silver salts, such as sodium thiosulfate or ammonium thiosulfate. Other complex-forming agents can also be present. Treatment with a bleaching and fixing bath not only oxidizes the metallic silver into the silver salt, it also subsequently dissolves the resulting silver salt from the layer as well. Bleaching and bleach-fixing baths are adequately known in photography. Reference is made for example to H. Berger, Agfacolor, 6th edition, pages 260 and 262; and E. Mutter, Die Wissenschaftliche und Angewandte Photographie, vol. IV (1967), pages 348, 352, 353 and 362.
Particularly good results are obtained with bleach-fixing baths having a high content of sodium or ammonium thiosulfate. Accordingly, the bleach fixing baths according to the invention preferably contain from 100 to 200 g. per litre of sodium or ammonium thiosulfate.
A further improvement is obtained if in addition socalled white couplers are applied in the bleach-fixing baths. White couplers are substances that are able to react with color-forming developer oxidation products without forming a dye. White couplers are known per se, for example from German patent specification No. 1,155,675. Reference is also made to the publication by W. Piischel in Mitteilungen aus den Forschungslaboratorien der Agfa- Gevaert AG, vol. IV, page 352 (1964).
The most favourable results are obtained with bleachfixing baths which, in addition to the sulfhydrazides and an increased thiosulfate content, contain from 1 to g. of a white coupler substance per litre.
The invention is illustrated by the following example:
An exposed color-photographic multi-layer material including a blue sensitive silver halide emulsion layer having a yellow color coupler, a green sensitive silver halide emulsion layer containing a magenta color coupler and a red sensitive silver halide emulsion layer with a cyan color coupler was developed for 50 seconds at 40 C. in a developer of the following composition:
6 g. of N-butyl-N-w-sulfobutyl-p-phenylene diamine, 4 g. of anhydrous sodium sulfite,
2 g. of hydroxylamine HCl,
100 g. of potassium carbonate, and
1 g. of potassium bromide,
made up to 1000 ml. with water.
The material was then squeezed and treated for 60 seconds at 40 C. with the following bleach-fixing bath:
3 g. of m-nitrophenylsulfhydrazide,
6 g. of the disodium salt of ethylene diamine tetraacetic acid,
40 g. of the ferric salt of ethylene diamine tetraacetic acid,
200 g. of ammonium thiosulfate,
4 3 g. of l-(m-sulfophenyl)-3-methyl-4-isopropyl-5-pyrazozolone, and 4 g. of anhydrous sodium sulfite,
made up to 1000 ml. with water.
The material was then washed, treated with a conventional stabilising bath and dried. The processed material showed extremely low dye-fog values which were comparable with the fog values obtainable in conventional processing, whilst a material processed in the manner described above, but using a conventional bleach-fixing bath from which the sulfhydrazide was absent, instead of the aforementioned bleach-fixing bath, showed excessively high fogging.
What is claimed is:
1. In a process for the production of color photographic images by imagewise exposure of a light-sensitive color photographic material which contains at least one silver halide emulsion layer and a color coupler, developing in a color-forming substance in the presence of said color coupler to react the color coupler with oxidation product of the color-forming substance so as to form a dye image and then treating the material with oxidizing agents to remove image silver and in which process the developed material is subjected to fixing, the improvement wherein the treatment of the exposed and developed material with the oxidizing agent is carried out in the presence of a sulfhydrazide having the formula:
in which R represents hydrogen, nitro or carboxyl and R represents hydrogen, halogen, or alkyl or alkoxy having up to three carbon atoms, the amount of sulfhydrazide being such that it reduces the formation of color fog during the bleaching.
2. The process of claim 1 wherein the bleach-fixing bath contains from -200 grams per litre of sodium or ammonium thiosulfate.
3. The process of claim 1 wherein the bleach-fixing bath contains from 1 to 5 grams per litre of a coupler that on reaction with color-forming developers form colorless products.
4. The process of claim 1 in which the bleaching is effected in a bleach-fixing bath containing from 100 to 200 grams of sodium or ammonium thiosulfate per litre and from 1 to 5 grams of a coupler that on reaction with color-forming developers form colorless products.
5. The combination of claim 1 in which the bleaching is effected with a bleach bath containing 0.5 to 10 grams of the sulfhydrazide per litre.
6. The combination of claim 1 in which the bleaching is effected without a preliminary rinse of the image.
References Cited UNITED STATES PATENTS 2,286,662 6/1942 Weyde et al. 9656 2,384,658 9/1945 Vittum 9656 3,293,036 12/1966 Meckl et al 96-60 BF FOREIGN PATENTS 6516093 2/1966 Netherlands 9666.1
NORMAN G. TORCHIN, Primary Examiner M. F. KELLEY, Assistant Examiner US. Cl. X.R.
9660 R, 60 BF, 61 R
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE19702041325 DE2041325A1 (en) | 1970-08-20 | 1970-08-20 | Photographic color development process |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| US3761262A true US3761262A (en) | 1973-09-25 |
Family
ID=5780239
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| US00172891A Expired - Lifetime US3761262A (en) | 1970-08-20 | 1971-08-18 | Photographic color developing process |
Country Status (5)
| Country | Link |
|---|---|
| US (1) | US3761262A (en) |
| BE (1) | BE770912A (en) |
| DE (1) | DE2041325A1 (en) |
| FR (1) | FR2104620A5 (en) |
| GB (1) | GB1338714A (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4293639A (en) * | 1979-05-09 | 1981-10-06 | Fuji Photo Film Co., Ltd. | Bleaching compositions for photographic processing |
| US4590150A (en) * | 1984-07-27 | 1986-05-20 | Fuji Photo Film Co., Ltd. | Method for processing silver halide color photographic light-sensitive material |
| US4770987A (en) * | 1985-12-17 | 1988-09-13 | Fuji Photo Film Co., Ltd. | Silver halide color photographic materials containing an antisain agent and a magenta coupler in lipophilic fine particles |
-
1970
- 1970-08-20 DE DE19702041325 patent/DE2041325A1/en active Pending
-
1971
- 1971-08-04 BE BE770912A patent/BE770912A/en unknown
- 1971-08-11 GB GB3762471A patent/GB1338714A/en not_active Expired
- 1971-08-18 US US00172891A patent/US3761262A/en not_active Expired - Lifetime
- 1971-08-20 FR FR7130469A patent/FR2104620A5/fr not_active Expired
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4293639A (en) * | 1979-05-09 | 1981-10-06 | Fuji Photo Film Co., Ltd. | Bleaching compositions for photographic processing |
| US4590150A (en) * | 1984-07-27 | 1986-05-20 | Fuji Photo Film Co., Ltd. | Method for processing silver halide color photographic light-sensitive material |
| US4770987A (en) * | 1985-12-17 | 1988-09-13 | Fuji Photo Film Co., Ltd. | Silver halide color photographic materials containing an antisain agent and a magenta coupler in lipophilic fine particles |
Also Published As
| Publication number | Publication date |
|---|---|
| DE2041325A1 (en) | 1972-02-24 |
| GB1338714A (en) | 1973-11-28 |
| FR2104620A5 (en) | 1972-04-14 |
| BE770912A (en) | 1972-02-04 |
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