US3708299A - Photographic developing method - Google Patents
Photographic developing method Download PDFInfo
- Publication number
- US3708299A US3708299A US00079335A US3708299DA US3708299A US 3708299 A US3708299 A US 3708299A US 00079335 A US00079335 A US 00079335A US 3708299D A US3708299D A US 3708299DA US 3708299 A US3708299 A US 3708299A
- Authority
- US
- United States
- Prior art keywords
- developing solution
- developing
- silver halide
- silver
- imidazole
- 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 abstract description 18
- RAXXELZNTBOGNW-UHFFFAOYSA-N imidazole Natural products C1=CNC=N1 RAXXELZNTBOGNW-UHFFFAOYSA-N 0.000 abstract description 56
- 229910052709 silver Inorganic materials 0.000 abstract description 37
- 239000004332 silver Substances 0.000 abstract description 37
- 239000000463 material Substances 0.000 abstract description 31
- -1 SILVER HALIDE Chemical class 0.000 abstract description 26
- QIGBRXMKCJKVMJ-UHFFFAOYSA-N Hydroquinone Chemical compound OC1=CC=C(O)C=C1 QIGBRXMKCJKVMJ-UHFFFAOYSA-N 0.000 abstract description 20
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 abstract description 14
- 239000000203 mixture Substances 0.000 abstract description 5
- 238000012545 processing Methods 0.000 abstract description 5
- 239000003795 chemical substances by application Substances 0.000 abstract description 4
- RAXXELZNTBOGNW-UHFFFAOYSA-O Imidazolium Chemical compound C1=C[NH+]=CN1 RAXXELZNTBOGNW-UHFFFAOYSA-O 0.000 abstract 1
- 238000011161 development Methods 0.000 description 13
- CDBYLPFSWZWCQE-UHFFFAOYSA-L sodium carbonate Substances [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 11
- IOLCXVTUBQKXJR-UHFFFAOYSA-M potassium bromide Chemical compound [K+].[Br-] IOLCXVTUBQKXJR-UHFFFAOYSA-M 0.000 description 10
- GEHJYWRUCIMESM-UHFFFAOYSA-L sodium sulfite Chemical compound [Na+].[Na+].[O-]S([O-])=O GEHJYWRUCIMESM-UHFFFAOYSA-L 0.000 description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 10
- 239000002245 particle Substances 0.000 description 8
- 230000006866 deterioration Effects 0.000 description 7
- 239000000839 emulsion Substances 0.000 description 7
- 230000035945 sensitivity Effects 0.000 description 6
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 5
- 229940001593 sodium carbonate Drugs 0.000 description 5
- 229910000029 sodium carbonate Inorganic materials 0.000 description 5
- 235000010265 sodium sulphite Nutrition 0.000 description 5
- WVDDGKGOMKODPV-UHFFFAOYSA-N Benzyl alcohol Chemical compound OCC1=CC=CC=C1 WVDDGKGOMKODPV-UHFFFAOYSA-N 0.000 description 3
- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 description 3
- SJOOOZPMQAWAOP-UHFFFAOYSA-N [Ag].BrCl Chemical compound [Ag].BrCl SJOOOZPMQAWAOP-UHFFFAOYSA-N 0.000 description 3
- 239000003112 inhibitor Substances 0.000 description 3
- NLKNQRATVPKPDG-UHFFFAOYSA-M potassium iodide Chemical compound [K+].[I-] NLKNQRATVPKPDG-UHFFFAOYSA-M 0.000 description 3
- 230000002441 reversible effect Effects 0.000 description 3
- 239000011734 sodium Substances 0.000 description 3
- JKFYKCYQEWQPTM-UHFFFAOYSA-N 2-azaniumyl-2-(4-fluorophenyl)acetate Chemical compound OC(=O)C(N)C1=CC=C(F)C=C1 JKFYKCYQEWQPTM-UHFFFAOYSA-N 0.000 description 2
- CIWBSHSKHKDKBQ-JLAZNSOCSA-N Ascorbic acid Chemical compound OC[C@H](O)[C@H]1OC(=O)C(O)=C1O CIWBSHSKHKDKBQ-JLAZNSOCSA-N 0.000 description 2
- 108010010803 Gelatin Proteins 0.000 description 2
- 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 2
- YNAVUWVOSKDBBP-UHFFFAOYSA-N Morpholine Chemical compound C1COCCN1 YNAVUWVOSKDBBP-UHFFFAOYSA-N 0.000 description 2
- NQRYJNQNLNOLGT-UHFFFAOYSA-N Piperidine Chemical compound C1CCNCC1 NQRYJNQNLNOLGT-UHFFFAOYSA-N 0.000 description 2
- ZLMJMSJWJFRBEC-UHFFFAOYSA-N Potassium Chemical compound [K] ZLMJMSJWJFRBEC-UHFFFAOYSA-N 0.000 description 2
- 229910021612 Silver iodide Inorganic materials 0.000 description 2
- 150000008064 anhydrides Chemical class 0.000 description 2
- QRUDEWIWKLJBPS-UHFFFAOYSA-N benzotriazole Chemical compound C1=CC=C2N[N][N]C2=C1 QRUDEWIWKLJBPS-UHFFFAOYSA-N 0.000 description 2
- 239000012964 benzotriazole Substances 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 229920000159 gelatin Polymers 0.000 description 2
- 239000008273 gelatin Substances 0.000 description 2
- 235000019322 gelatine Nutrition 0.000 description 2
- 235000011852 gelatine desserts Nutrition 0.000 description 2
- 229910052700 potassium Inorganic materials 0.000 description 2
- 239000011591 potassium Substances 0.000 description 2
- ZUNKMNLKJXRCDM-UHFFFAOYSA-N silver bromoiodide Chemical compound [Ag].IBr ZUNKMNLKJXRCDM-UHFFFAOYSA-N 0.000 description 2
- 229940045105 silver iodide Drugs 0.000 description 2
- 229910052708 sodium Inorganic materials 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 150000005208 1,4-dihydroxybenzenes Chemical class 0.000 description 1
- HDGMAACKJSBLMW-UHFFFAOYSA-N 4-amino-2-methylphenol Chemical compound CC1=CC(N)=CC=C1O HDGMAACKJSBLMW-UHFFFAOYSA-N 0.000 description 1
- ZFIQGRISGKSVAG-UHFFFAOYSA-N 4-methylaminophenol Chemical compound CNC1=CC=C(O)C=C1 ZFIQGRISGKSVAG-UHFFFAOYSA-N 0.000 description 1
- ZVNPWFOVUDMGRP-UHFFFAOYSA-N 4-methylaminophenol sulfate Chemical compound OS(O)(=O)=O.CNC1=CC=C(O)C=C1.CNC1=CC=C(O)C=C1 ZVNPWFOVUDMGRP-UHFFFAOYSA-N 0.000 description 1
- XPAZGLFMMUODDK-UHFFFAOYSA-N 6-nitro-1h-benzimidazole Chemical compound [O-][N+](=O)C1=CC=C2N=CNC2=C1 XPAZGLFMMUODDK-UHFFFAOYSA-N 0.000 description 1
- CPELXLSAUQHCOX-UHFFFAOYSA-M Bromide Chemical compound [Br-] CPELXLSAUQHCOX-UHFFFAOYSA-M 0.000 description 1
- SXRSQZLOMIGNAQ-UHFFFAOYSA-N Glutaraldehyde Chemical compound O=CCCCC=O SXRSQZLOMIGNAQ-UHFFFAOYSA-N 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 description 1
- 235000010724 Wisteria floribunda Nutrition 0.000 description 1
- QMJDEXCUIQJLGO-UHFFFAOYSA-N [4-(methylamino)phenyl] hydrogen sulfate Chemical compound CNC1=CC=C(OS(O)(=O)=O)C=C1 QMJDEXCUIQJLGO-UHFFFAOYSA-N 0.000 description 1
- 230000001133 acceleration Effects 0.000 description 1
- 150000001299 aldehydes Chemical class 0.000 description 1
- 150000003973 alkyl amines Chemical class 0.000 description 1
- 230000004075 alteration Effects 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 150000003974 aralkylamines Chemical class 0.000 description 1
- 235000010323 ascorbic acid Nutrition 0.000 description 1
- 229960005070 ascorbic acid Drugs 0.000 description 1
- 239000011668 ascorbic acid Substances 0.000 description 1
- 229960004217 benzyl alcohol Drugs 0.000 description 1
- 235000019445 benzyl alcohol Nutrition 0.000 description 1
- 229910021538 borax Inorganic materials 0.000 description 1
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 description 1
- 239000004327 boric acid Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 125000000118 dimethyl group Chemical group [H]C([H])([H])* 0.000 description 1
- DHHNSJJTDFVVSG-UHFFFAOYSA-L disodium;benzene-1,4-diol;sulfite Chemical compound [Na+].[Na+].[O-]S([O-])=O.OC1=CC=C(O)C=C1 DHHNSJJTDFVVSG-UHFFFAOYSA-L 0.000 description 1
- 230000001747 exhibiting effect Effects 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 239000006174 pH buffer Substances 0.000 description 1
- CMCWWLVWPDLCRM-UHFFFAOYSA-N phenidone Chemical compound N1C(=O)CCN1C1=CC=CC=C1 CMCWWLVWPDLCRM-UHFFFAOYSA-N 0.000 description 1
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
- 231100000614 poison Toxicity 0.000 description 1
- 230000007096 poisonous effect Effects 0.000 description 1
- ZNNZYHKDIALBAK-UHFFFAOYSA-M potassium thiocyanate Chemical compound [K+].[S-]C#N ZNNZYHKDIALBAK-UHFFFAOYSA-M 0.000 description 1
- 229940116357 potassium thiocyanate Drugs 0.000 description 1
- 238000004904 shortening Methods 0.000 description 1
- 229940076133 sodium carbonate monohydrate Drugs 0.000 description 1
- 239000001488 sodium phosphate Substances 0.000 description 1
- 229910000162 sodium phosphate Inorganic materials 0.000 description 1
- 239000004328 sodium tetraborate Substances 0.000 description 1
- 235000010339 sodium tetraborate Nutrition 0.000 description 1
- 125000003944 tolyl group Chemical group 0.000 description 1
- RYFMWSXOAZQYPI-UHFFFAOYSA-K trisodium phosphate Chemical compound [Na+].[Na+].[Na+].[O-]P([O-])([O-])=O RYFMWSXOAZQYPI-UHFFFAOYSA-K 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
- G03C5/00—Photographic processes or agents therefor; Regeneration of such processing agents
- G03C5/26—Processes using silver-salt-containing photosensitive materials or agents therefor
- G03C5/29—Development processes or agents therefor
- G03C5/305—Additives other than developers
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10S430/00—Radiation imagery chemistry: process, composition, or product thereof
- Y10S430/135—Cine film
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10S430/00—Radiation imagery chemistry: process, composition, or product thereof
- Y10S430/162—Protective or antiabrasion layer
Definitions
- This invention relates to the processing of silver halide photographic materials and more particularly to developing solution for fine grained photographic materials.
- the well known development accelerators are amine compounds, such as alkylamines (U.S. Pat. No. 2,196,037), aralkylamines (U.S. Pat. No. 2,496,903; 2,515,147; 2,541,889), phenoxyalkylamines (U.S. Patent No. 2,482,546), heterocyclic alkylamines (U.S. Pat. 2,605,183), morpholine and piperidine (U.S. Pat. No. 1,086,681).
- alkylamines U.S. Pat. No. 2,196,037
- aralkylamines U.S. Pat. No. 2,496,903; 2,515,147; 2,541,889
- phenoxyalkylamines U.S. Patent No. 2,482,546
- heterocyclic alkylamines U.S. Pat. 2,605,183
- morpholine and piperidine U.S. Pat. No. 1,086,681.
- the principal object of this invention is to provide an improved accelerator for the developing solution, which is easily handled, capable of increasing the rate of development and increasing the effective speed of the photographic material without undesirable increase in fog and the deterioration in the granularity of the developed silver.
- Still another object of this invention is to provide a process for accelerating the developing of the fine grained photographic materials without deterioration in the granularity of the developed silver.
- the developing solution of this invention is applied to the black-and-white photographic materials, especially to low sensitivity silver halide photographic materials which require fine granularity and is generally used for the oflice works, documentary works, industrial works, or reprographic works.
- the present invention can be applied to telephotographic materials; lithographic materials (used for producing dots), phototypesetting materials, microfilms, microplates, materials for facsimile, materials for prints of scanned dots, materials for production of integral circuit master and photographic materials for astronomical study; these photographic materials are composed of extremely fine grained silver halide and contain very small amounts of silver halide.
- the granularity of the developed silver image should be adequately low throughout the development in the development of, e.g., fine grain silver halide emulsions as in the developing acceleration of this invention.
- the present invention provides a method of treating a photographic material which comprise developing the materials with the developer containing imidazole and hydroquinone (substituted or unsubstituted) thus increasing the rate of development or shortening the developing time, inhibiting the fog formation, increasing the effective sensitivity and making fine the developed silver particles.
- the increase in speed of the black-and-white photographic material to which this invention is applied by the imidazole is much greater than that of the reversible color film described in the U.S. lPat. 3,126,282.
- the reversible color film of this is considered to be composed of an emulsion of coarse silver iodobromide particles, while the emulsion of the Black and White photographic materials used in this invention contains finely divided silver halide particles.
- the process for developing the photographic material containing fine grain silver halides according to this invention has been made on a discovery that the increase in speed by an imidazole depends on the size of the silver halide grain.
- fine grained denotes a particle size of from 0.1 to 0.3 micron.
- the developing solution exhibiting the aforesaid advantageous effects with the addition of the imidizole contains at least 120 parts/liter hydroquinone as the main developing agent and, in addition, a conventional developer such as 1-phenyl-3-pyrazolidone or N-methyl-paminophenol.
- an oxidation inhibitor such as Na sulfite or ascorbic acid
- a suitable pH buffer such as boric acid, sodium hydroxide, sodium carbonate or sodium phosphate
- a developing inhibitor such as potassium iodide or potassium bromide
- an organic fog inhibitor such as 6-nitro-benzimidazole or benzotriazole
- an aldehyde such as formaldehyde or glutaraldehyde
- the pH of this developing solution may be adjusted in a range between 8.5 and 12.0 and preferably 10 to 11.
- the amounts of the imidazole to be added to the developing solution vary with the type of the photographic material employed and the pH of the developing solution, but favorably in the range of between 0.5 part/liter and parts/liter.
- the finely divided silver halide is present in a concentration of from 10-70 mg./100 cm. and preferably 20-50 mg./crn.
- the process of this invention was not effective for the Benzylalcohol VOL)" films (I)-(IV), but the test results were shown to be Sodium sulfite 30 compared with those of the films (V)(VII).
- the mean Sodium carbonate 4L0 diameter of the silver halide grains in each of the photo- Sodium hydroxide L0 graphlc films were as follows: 4-amino 3 methyl-N-ethyl-N-methane sulfon- Mean diameter of the amidethylaniline sulfate 5.0 Photographic film: silver particle, microns Potassium bromide 0.5
- EXAMPLE 2 Commercial fine grain positive film for the cinematography composed of grained silver bromochloride-gelatinemulsion was subjected to development with solution having following composition at 27 C.
- Developing solution C Parts Water (by vol.) 800 l-phenyl-B-pyrazolidone 0.5 Sodium sulfite 50 Hydroquinone 12 Sodium carbonate (NaCO H O) 60 Potassium bromide 2.0 Benzotriazole 0.2 Water to make 1 liter.
- microfilm comprising a support with a fine grain silver chlorobromide, gelatin emulsion coated thereon, was subjected to development at 20 C. with a developing solution having following composition.
- the developing solution of E required 4 minutes to develop the microfilm, but the addition of the imidazole to the developing solution shortened the developing time as shown in Table 3. On the other hand, a development time of 4 minutes with the imidazole added to the developing solution produced a high sensitivity on the microfilm. Furthermore, the developed silver grains in the picture were favorably fine and uniform according to the process of this invention using the imidazole containing developing solution.
- a method for processing an exposed silver halide black-and-white photographic material, wherein the silver halide grains are less than 0.3 micron which comprises developing the photographic material with a developing solution comprising at least 1.0 part of hydroquinone as the main developing agent and at least 0.5 part of imidazole per one liter of the developing solution.
Landscapes
- Physics & Mathematics (AREA)
- General Physics & Mathematics (AREA)
- Silver Salt Photography Or Processing Solution Therefor (AREA)
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP44080538A JPS4828295B1 (enrdf_load_stackoverflow) | 1969-10-08 | 1969-10-08 |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| US3708299A true US3708299A (en) | 1973-01-02 |
Family
ID=13721115
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| US00079335A Expired - Lifetime US3708299A (en) | 1969-10-08 | 1970-10-08 | Photographic developing method |
Country Status (5)
| Country | Link |
|---|---|
| US (1) | US3708299A (enrdf_load_stackoverflow) |
| JP (1) | JPS4828295B1 (enrdf_load_stackoverflow) |
| DE (1) | DE2049502A1 (enrdf_load_stackoverflow) |
| FR (1) | FR2065100A5 (enrdf_load_stackoverflow) |
| GB (1) | GB1275375A (enrdf_load_stackoverflow) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3808003A (en) * | 1969-01-24 | 1974-04-30 | Fuji Photo Film Co Ltd | Photographic material development method |
| US4147543A (en) * | 1972-04-01 | 1979-04-03 | Fuji Photo Film Co., Ltd. | Developer compositions for high contrast diffusion transfer photographic materials and process therefor |
| US4810622A (en) * | 1986-07-02 | 1989-03-07 | Fuji Photo Film, Co. Ltd. | Method for processing silver halide photographic material with an alkaline black and white developer |
| US5026629A (en) * | 1990-02-07 | 1991-06-25 | Eastman Kodak Company | Fixing bath for black and white photographic elements |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5811937A (ja) * | 1981-07-15 | 1983-01-22 | Fuji Photo Film Co Ltd | 銀染料漂白処理方法 |
-
1969
- 1969-10-08 JP JP44080538A patent/JPS4828295B1/ja active Pending
-
1970
- 1970-10-07 GB GB47751/70A patent/GB1275375A/en not_active Expired
- 1970-10-07 FR FR7036141A patent/FR2065100A5/fr not_active Expired
- 1970-10-08 US US00079335A patent/US3708299A/en not_active Expired - Lifetime
- 1970-10-08 DE DE19702049502 patent/DE2049502A1/de active Pending
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US3808003A (en) * | 1969-01-24 | 1974-04-30 | Fuji Photo Film Co Ltd | Photographic material development method |
| US4147543A (en) * | 1972-04-01 | 1979-04-03 | Fuji Photo Film Co., Ltd. | Developer compositions for high contrast diffusion transfer photographic materials and process therefor |
| US4810622A (en) * | 1986-07-02 | 1989-03-07 | Fuji Photo Film, Co. Ltd. | Method for processing silver halide photographic material with an alkaline black and white developer |
| US5026629A (en) * | 1990-02-07 | 1991-06-25 | Eastman Kodak Company | Fixing bath for black and white photographic elements |
Also Published As
| Publication number | Publication date |
|---|---|
| FR2065100A5 (enrdf_load_stackoverflow) | 1971-07-23 |
| JPS4828295B1 (enrdf_load_stackoverflow) | 1973-08-31 |
| GB1275375A (en) | 1972-05-24 |
| DE2049502A1 (de) | 1971-04-15 |
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