SU562220A3 - Electroregistering material - Google Patents

Description

54) ELECTRIC RECORDING MATERIAL

I

BACKGROUND OF THE INVENTION The invention relates to electrical recording materials that can be used by information recording equipment B, such as facsimiles, direct-printing devices, analog recorders, etc.

An electrical registration material is known that includes a substrate, a conductive layer, containing copper iodide and a binder, and a color-forming layer containing a binder and heat sensitive color-forming component I. A disadvantage of the known electroregulating material is its high resolution and image stability.

In order to create an increased-resolution electrical recording material, the proposed electrical recording material additionally contains iodine in the a1 wire, em layer; whether hydrogen peroxide, or hydroxy acid salt, or peroxyacid, or permanganate in an amount sufficient to form free iodine from copper iodide in the layer from 0.05 to 0.2 weight. % In Dai electrofiling material, carbon or carbon-impregnated paper, or metal deposited paper, or polymer film, or glass can be used as a substrate, and a leuco-base triphenylmethane dye mixture, or a base-fluorescent fluorescent dye, and organic acid or phenol, as well as leucobase redox dye.

Co-motivation of the conductive layer of electrical registration material should be less than a few kilo. As a result, by reducing the surface resistance, a high detection rate is reached, about 3.5 m / s, when a voltage of 200-300 V is applied. In order to reduce the surface resistance of the recording material to less than a few knots, as mentioned above, copper iodide, which liMeeT resistance

10 ohm-cm and which is obtained by the reaction of potassium iodide and copper sulfate, and an amount of g / m

As a substance that reduces resistance, compounds that can themselves create iodine components, such as iodine or iodine compounds, such as iodoform, tetraiodomethane, and oxidizing elements that oxidize copper iodide to release iodine from it, can be used. potassium permanganate.

It is known that in an ionic crystal having a composition that deviates from the stoichiometric one, p-type semiconductor properties are observed, when there are not enough metal ions (or anions in excess). It is known that the conductivity of Cu20 is in close connection with the oxygen content, and the conductivity increases when the oxygen content becomes higher. Chemical analysis shows that in copper iodide CuJ, the content of iodine J is excessive compared with exactly the stoichiometric composition calculated on the formula of the molecule, i.e. one atom of iodine per copper atom. There is a close relationship between the conductivity of copper iodide and the pressure of iodine, the conductivity increases with increasing pressure of iodine. This is due to the fact that iodine is absorbed in copper iodide, forming Cu + vacancies in the lattice, acting as a p-type semiconductor, which in turn increases conductivity. Consequently, the resistance value of copper iodide depends on the amount of free iodine.

It becomes possible to increase the amount of free iodine by adding a lower, its resistance to the usual copper iodide, thus lowering the resistance of copper iodide.

After a series of experiments, it was found that a significant result is achieved when the amount of excess iodine in copper iodide is in the range of 0.05-0.2 weight. % and copper iodide are used as the conductive layer for the electrical recording material. When a large amount of iodine is added to the layer, its transparency deteriorates after application, and excess iodine can discolour during storage, which is not practical for practical use.

Compounds that reduce material resistance are iodine, iodoform, tetraiodomethane and potassium permanganate. For iodoform and tetraiodomethane, it is understood that iodine atoms are released and absorbed in copper iodide so that the resistance value decreases. Potassium permanganate acts as an oxidizing agent for copper iodide. It removes copper ions from copper iodide, forming vacancies in the Cu + lattice in order to enhance p-type conductivity. In any case, a suitable conductive material for electrical registration material is obtained when the amount of excess iodine in copper iodide is in a diaozone of 0.05-0.2 wt. The% Iodist copper with the indicated lowering agent shows no change after testing at 60 ° C and reduced pressure (100 mm Hg) for 8 hours.

FIG. 1 shows the design of the recording material; in fig. 2 shows the scheme for implementing the registration method; in fig. 3-8 - forms of construction of recording materials.

The recording material contains a substrate 1 made of paper, cardboard, glass, plastic material or the like, onto which a conductive layer 2 is deposited containing copper iodide with an agent lowering resistance, and

covering the color-forming layer 3, including the color-forming comonent, which, in response to an electrical signal, forms a color when warm energy is applied to it. Registration proceeds with the passage of electric current from a source of direct or alternating current 4 by closing switch 5 through the pin of the recording electrode 6 and the splint or flat electrode 7, through the color-forming layer 3 and conducting

layer 2, so that the short trace 8 can be formed on the conductive layer 2 adjacent to the pickup of the recording electrode 6.

Recording material depicted

in fig. 1 is a typical example of such

designs. Can be constructed

various modifications of this design.

Examples of them are shown in FIG. 3-8.

Recording material depicted

in fig. 3, contains a single layer 9 consisting of a heat sensitive color-forming component and copper iodide and formed on the surface of the substrate 1. The recording material shown in FIG. 4, includes

conductive layer 10: an aluminum layer deposited from the ion phase, formed on the substrate 1 in a manner similar to that shown in FIG. 1, a conductive copper iodide layer 2 and a color forming layer 3 successively applied thereto. The recording material shown in FIG. 5 comprises a conductive carbon layer 11 on the surface of the substrate 1 and a coating layer 9 comprising a heat sensitive color-forming component and copper iodide. The recording material depicted in FIG. 6 consists of carbon-impregnated paper 12 placed on substrate 1 shown in FIG. 3. The recording material shown in FIG. 7,

contains paper 13 impregnated with copper iodide as a substrate, and a color-forming layer 3 deposited on it. The recording material shown in FIG. 8, formed from paper impregnated with copper iodide

and a heat-colorizing component.

Examples 1 and 2 below relate to the structure shown in FIG. 1, and the irimers 3-7 to the structures shown in FIG. 3-7, respectively.

The color-forming component of the compounds used is the triphenylmethane tiaa dye of general formula I or the dye in the leucoase-based fluorane type

formulas P

with about

III

where RX, Ry, Rz are hydrogen or halogen atoms, or hydroxyl, alkyl, nitro, amio-, dialkylamino, monoalkylamino- or aryl-butypes;

Z is an atom required to form a heterocyclic ring, O or S.

Compounds of formula I:

3,3-bis- (l-dimethylaminophenyl) -phthalide;

3,3-bis- (p-dimethylaminophenyl) -6-dimethylaminophthalide (crystal violet lactane);

3,3-bis- (l-dimethylaminophenyl) -6-aminophthalide;

3,3-bis - (l-dimethylaminophenyl) -6-nitrophthalide;

3,3-bis- (l-dibutylaminophenyl) -phthalide;

3,3-bis- (l - dimethylaminophenyl) -4,5,6,7-tetrachlorophthalide. Compounds of formula II:

3-dimethylamino-6-methoxyfluorane;

7-acetamino-3-dimethylaminofluorane;

3-dimethylamino-5,7-dimethylfluorane;

3-diethylamino-5,7-dimethylfluorane;

3,6-bis-p-methoxyethoxyethoxyfluorane;

3,6-bis-p-cyanoethoxyfluorane; Other lactam compounds:

9-l - nitroanilino-3,6-bis- (diethylamino) -9 xanthinyl-o-lactam of benzoic acid (rhodamine B lactam);

9-l-nitroanilino-3,6-bis- (dnmethylamino) -9thioxanthynyl-o-lactam benzoic acid.

These dyes are poorly soluble in water and can be pulverized to the smallest particles less than 10 microns in size.

Color forming, comonent.

The phenolic compound or organic acid is most preferred as a color-forming agent capable of forming a dye through a chemical reaction with a color-forming dye. It is desirable that the specified compound or acid be in solid form at room temperature and can be transferred to the liquid phase or evaporated at a temperature above 70 ° C.

Examples of phenol compounds are:

3,5-xylene, timol 4-tertiary butylphenol, 4-hydroxyphenoxide, methyl 4-hydroxybenzoate, 4-hydroxyacetophenone, catechin, hydroquinone, resorcin, 4-tuset-octylcatechol, 4.4-8Gr.-butylidenediphenol, 2,2 -oxiphenyl, 2,2-methylenebis- (4-methyl6-treg-butylphenol), 2,2-bis- (4-xyphenyl) -propane, 4,4 - isopropylidenebis - (2-greg-butylphenol), 4,4 - dry-butylenediphenol, pyrogalol and 4,4-iso-cronylenediphenol.

Examples of organic acids are

the following, not: stearinova, Galiyev, benzoin,

salicylic acid, amber, 1-hydroxy-2-naphthoic, 2-hydroxy-l-toluicyl, oxybenzoic, l-hydroxybenzoic and 4-hydroxyphthalic acid.

By organic reagent, referred to herein, is meant a compound capable of staining or repainting as a result of reaction with metal ions. A large number of such compounds are currently known. The invention uses the phenomenon when one of the organic components and the metal used in combining it is melted due to thermal energy generated during the application of an electric current, and the two substances react with each other to form a color. As a consequence, it is desirable that one of them, having a lower melting point, is in a solid state at a temperature of 70 ° C and has a melting point of 20 ° C. 150 ° C or lower. In this regard, metal soap is most desirable as an organic metal salt. The following combinations of organic component and metal can be applied. Organic component: metal: diphenylthiocarbazide: Cu, Fe, Mg or Hg;

dimethylglyoxime: Cu, Fe or Ni;

benzoinxime: Sy;

8-hydroxyquinoline: Cd, Cu, Fe, Pb, Mn, Ni or Zn; dinitrophenylcarbazide: Cd;

Rodania: C or Hg;

diphenylthiocarbazone: Cu, Ba, Co, Pu, Pb, ng or Zn;

diphenylcarbazone: Co, Cu, Pb, Mg, Mn, Hg, Ni, or Zn;

amine dithiooxide: Co, Cu, Pb or Ni;

2-mercapto-4-phenylthiazole: Co or Pb;

3,5-dimethylpyrazole: Co;

ss-naphthylamindiocarbamic acid: Co or Fe;

benzidine: C, Pb or Mn;

L-dimethylaminobenzylideneradanine: Cu, Fe, Mg or Hg;

salicylaldoxime: C or Pb; Triphenyl thiophosphate: Ni;

l, l - tetramethyldiaminodiphenylmethane: Pb or Mn;

anthranilic acid: Zn;

diphenylbenzene: Zn; catechin: Fe;

Galic acid: Fe;

dehydroxynaphthalene: D;

alizarin: sy;

Quinolizarin: Sy. Organic metal salt.

As an organic metal salt, a metal soap containing metal ions is effectively used. Typical examples of combinations of organic point reagents with organic metal salts, and

7

shades of colors obtained using such combinations are given below.

Organic component: organic metal salt (color shade of the obtained dvet):

dimethylglyoxime: nickel stearate (pink);

cupron: copper myristate (yellow-green);

dithiooxamide: nickel stearate (purple);

8-hydroxyquinoline: iron oleate (black);

halic acid: iron stearate (black);

alizarin: copper oleate (bright red);

quinalizarin: copper oleate (bright red);

diphenylcarbazone: copper stearate (red);

diphenylcarbazone: cadmium stearate (red);

diphenylcarbazone: copper myristate (purple);

diphenylcarbazone: zinc palmitate (deep red);

diphenylthiocarbazide: mercury stearate (magenta);

dphenylthiocarbazide: lead myristate (deep red).

It has been found that a substance that was previously known as a redox dye forms a color near the recording pin during the passage of electric current, therefore it can be used as a color forming compound for use in electrical registration paper. The redox dye used here is a substance that is colored or repainted as a result of oxidation when exposed to heat during the application of an electric current, it is a leuco base, which is preferable from the point of view of the transparency of the substrate. Examples of redox dyes used in the invention, as well as shades of color obtained with these indicators, are given below. Redox dyes (color):

leucoethyl blue (blue);

lememetil Capril blue (blue);

leukotoluidine cyan (magenta);

leukod, ifenylamine (purple);

leico - N - methyldiphennlamine- / g-sulfonic acid (bright red);

leucophenyl anthranilic acid (red red);

Triphenyltetrazolchloride (red);

methyliologen (purple);

leucosafranin T (red);

leucoindigosulfonic acid (blue);

leucophenosafranin (red);

leukemethylene blue (blue);

leucodiphenylbenzidine (magenta);

leukoeryodultsin A (from yellowish-green to red);

leuko-p-nitrodiphenylamine (magenta);

malachite green (green);

Reducing the resistance of substances for copper iodide:

a) iodine;

eight

b) iodine compounds: iodoform, tetraiodomethane, iodide salt, periodate, iodate, hypoiodate;

c) peroxide: hydrogen peroxide, sodium peroxide, barium peroxide;

g) hydroxy acid salt: hypochlorite, chlorate, perchlorate, bromate.

e) peroxoacid: peroxodisulfate, peroxosulfuric acid, peroxophosphoric acid;

e) Permanganate: manganic acid, potassium permanganate, sodium permanganate, calcium permanganate, etc.

Binder.

The binder is used to distribute, in the form of small particles, a color-forming dye, a color-forming agent, an organic reagent and an organic metal salt used in the color-forming layer, and / or copper iodide and a desensitizing agent, as well as call them. Since most of the mentioned color-forming dyes, color-forming, their agents, organic reagents and copper iodide, are water-insoluble, it is effective to use water-soluble binder and other materials. Further, the water-soluble substance has such characteristics that it is easily manufactured and processed during the preparation of the control paper.

Water soluble binder. Examples of water-soluble binders include hydroethyl cellulose, carboxymethyl cellulose, methoxy cellulose, polyvinyl alcohol, polyvinyl pyrrolidone, polyacrylamide, polyacrylic acid, gelatin, starch, and arabolic acid. Water insoluble binder.

As a binder, an organic solvent soluble binder can also be used. In the case of binary systems, including, for example, a color-forming dye and a zhzet-forming agent used as a thermal recording material for the color of the developed layer, the two components can be separately dispersed in the form of small particles in a binder. If one of the two

the components are soluble in the solvent used to dissolve the binder, the color formation reaction loses its function when the recording medium arises during the displacement of both. Therefore, the solvents for the binder listed here need to be limited in use depending on the type of color forming components.

Specific examples of water-insoluble bonding agents include natural rubber, synthetic rubber, chlorinated rubber, alkyd resins, styrene-butadiene sonolymers, polybutyl methacrylate, low molecular weight ethylene polymers, low molecular weight styrene polymers

Lightweight, polyvinyl butyrol, phenolic resins and nitrocellulose.

Example 1. 200 weight. including copper iodide mixed with 200 weight. including aqueous solution containing I weight. % polyvinyl alcohol (PVA), and then crushed and mixed in a mixer for 2 hours

During this process, 1 ml of an aqueous solution containing 2 wt. % potassium permanganate. The formed dispersion solution is further referred to as solution A. Dispersion solution A is applied onto artificial paper with the aid of a wire bar designed to form a covering layer 8 µm thick (15 g / m in the layer). The surface resistance thus obtained is 3.5-4.5 x X. ohm. When potassium permanganate is removed from solution A, the surface resistance is 2-5-10 ohms. Thus, it is clear that surface resistance is significantly reduced by adding potassium permanganate as an agent that lowers the resistance of copper iodide. With a given amount of deposition, it is possible to use a small recording voltage, since the surface resistance is low, or, with a small amount of the applied layer, it is possible to obtain the desired surface resistance, reducing the cost and obtaining a flatter paper-like plate.

Then 200 weight. including aqueous solution containing 1 wt. % polyvinyl alcohol, mixed with 35 wt. including 3,3-bis - ("- dimethylaminophenyl) -6-dimethylaminophthalide as a color-forming component, and then the mixture is crushed and stirred for 48 hours in a vessel with an internal volume of 500 ml. The dispersion solution thus obtained is hereinafter referred to as solution B. In solution B, the light-forming component dissolves only slightly, and is mainly dispersed in

KMpO4

Surface resistance after application of solution A, com

Example 2. 200 weight. including copper iodide and 0.5 wt. including iodine is added to 200 wt. the hydroxyethyl cellulose is ground and mixed in a mixer for 2 hours. The dispersion solution thus obtained is hereinafter referred to as solution E. Dispersion solution E is then applied to artificial paper by means of a wire to form a coating layer 10 µm thick and the paper is then dried. After application, surface coating. is 2-310 ohms. When iodine is not added as a drag reducing agent, the surface resistance is 2-510

the form of small particles with a size of not more than 5 microns. To solution B after 200 weight. including an aqueous solution containing 10 wt. % polyvinyl alcohol, add 35 weight. 4,4-isopropylidenediphenol as a color-forming component is ground and stirred in a ball mill for 48 hours to obtain a dispersion solution, hereinafter referred to as solution C. The color-forming component in solution C is also dispersed in the form of small particles with a size not larger than than 5 microns. Since the particles are surrounded by polyvinyl alcohol, there is no direct contact between the particles. 15 wt. including solution B and 100 wt. parts of solution C are mixed together while stirring. The resulting solution is designated as D. Then solution D is applied onto artificial paper, which was previously applied with solution A, by means of a wire bar to form a covering layer with a thickness of about 5 microns. The paper is then dried to form an electrical recording material. The surface resistance of the recording material thus formed is 4.2 lump and provides a clear registration, having a reflected optical density of 0.88 when using a recording potential of 300 volts.

With such a recording material, it is further possible to make copying in transmitted light.

The relationship between the amount of potassium permanganate added when Solution A is applied and the surface resistance under the conditions listed above is shown below.

When the amount of substance I added

the solution becomes reddish

Ic

40

The conductivity decreases as the amount of copper oxide increases.

one

one

102

104

ir.s 25

10,800

100

four

10 ohm Thus, it is clear that the surface resistance is significantly reduced.

when adding iodine and achieve registration with a lower value of registration potential.

Then 20 wt. including 3,3-bis - ("- dimethylaminophenyl) - 6 - dimethylaminophthalide is added to

100 weight. including an aqueous solution containing 5 wt. % hydroxyethylcellulose as a color-forming component, crushed and mixed in a ball mill for 48 hours. The resulting solution is referred to as

solution F. In addition to 100 weight. including an aqueous solution containing 5 wt. % hydroxyethylcellulose add 35 weight. including 4,4-isopropylidenediphenol as a color-forming component. The mixture is ground and mixed in a ball mill for 48 hours. The thus prepared solution is hereinafter referred to as solution G. 15 wt. including solution F and 100 wt. of solution G is mixed and the mixture is applied onto synthetic paper, onto which solution E was previously applied, by means of a wire bar to create a covering layer with a thickness of about 5 microns. The paper is then dried to obtain an electrical recording material. The surface resistance of the electro-recording plate, thus obtained, is 3.8 lump and provides a recording having a reflection optical density of 0.91 using a recording potential of 300 volts. Example 3. 100 weight. including copper iodide and 1 wt. including iodoform added to 100 weight. including aqueous solution containing 1 wt. % polyvinyl alcohol, milled and displaced in a ball mill for 48 hours. The dispersion solution thus obtained is hereinafter referred to as solution P. Then

As can be seen from the table above, the surface resistance of the recording plate can be reduced by adding iodoform and copper iodide, as a result of which it is possible to ensure recording with sufficient optical density at a relatively low recording potential.

Example 4. 100 g of copper iodide and 0.5 g of tetraiodomethane are added to 100 cm of a toluene solution containing 10 wt. A 85: 15% styrene-butadiene copolymer with a ratio of 85: 15 is crushed and mixed in a ball mill for 48 hours. The dispersion solution obtained in this way is applied to the paper with precipitated aluminum using a wire bar to deposit the coating layer of 15 µm and then the paper is dried. The surface resistance of the coated paper is 4.3-10 ohms.

Then 35 wt. Part of the C-dimethylamino-6-methoxyfluorane as a color-forming component is added to 200 weight. including an aqueous solution containing 10 wt. % polyvinyl alcohol, crushed and shifted in a nozzle mill for 48 hours, 10 weight. h of this mixture

10 wt. including solution C, described in example 1, and 5 wt. including a dispersion solution of copper iodide, including tetraiodomethane, is mixed together and then applied to the indicated conductive layer by means of a wire bar for

making a coating layer about 10 microns thick. The structure of the recording material obtained by such a cutout is depicted in FIG. 4. On paper 1 a layer of precipitated aluminum 10 is formed, on which

the conductive layer 2 and the color forming layer 3 are applied. The surface resistance is 8.3-10 ohms, and a clear red recording trace is obtained, having a reflected optical density of 0.85 at a recording potential of 350 volts. When no tetriodomethane is added, the recording material in all other respects, obtained under the same conditions, shows surface resistance. including iron stearate and 30 wt. including halic acid, respectively, added to 100 weight. including aqueous solution containing 10 wt. % polyvinyl alcohol, stirred in a ball mill for 24 hours 50 weight. including both mixtures are mixed to obtain a solution of K100 weight. including solution H and 30 wt. Part of Solution K is mixed in a blender and applied to the paper with a thickness of around 15 microns. It is then dried to obtain a light yellow recording material. The surface resistance of the recording plate is 1.45-10 ohm, and a clear dark gray recording trace is obtained, having a reflected optical density of 0.80 at a recording potential of 300 volts. The design of the recording material is depicted in FIG. 3. Color forming current layer 10 is created on paper 1. The recording materials are made with a variable amount of iodoform added to copper iodide in solution P to determine the magnitude of the recording voltage at which the reflected optical density of the recording trace is 0.80.

6-10 ohms and provides a recording having a reflected optical density of about 0.35 at a recording potential of 600 volts.

Example 5. Solution / has the following composition, wt. including:

Amorphous carbon100

Low styrene polymer

molecular weight10

Toluene100

The solution / composition given is ground and shifted in a ball mill for 24 hours, and then applied to white paper to form a conductive layer 10 microns thick after drying. The surface resistance of the conductive layer is 250-500 ohms. Then 10 weight. h. Leiko Malachite Green, 100 wt. including copper iodide, 0.2 wt. including sodium peroxide, 5 wt. including sodium sulfopate and polystyrene 130 weight. parts of water are ground and mixed for 24 hours, and then the mixture is applied to the indicated conductive layer to obtain a coating layer 10 microns thick after drying. Light yellow recording material is obtained. When scanning with a recording pin with an applied DC voltage of 40 V, a green recording register is formed, next. When sodium peroxide is not added as an oxidizing agent, registration is not achieved until the applied voltage exceeds 70 volts. Pa figs. 5 shows the structure of the recording material. The carbon layer 11 and the color-forming conductive layer 9 are applied to the paper 1.

Example 6. Solution K, wt. including:

Polmint copper25

Aqueous solution containing 10% PVA100 Solution L, wt. including: Diphenylcarbazone25 Aqueous solution containing 10% PVA 100 Solution H, wt. including:

Yodist Copper1000

Pyroxosulfuric acid1

An aqueous solution containing 5% PVA1000 The above three solutions are respectively ground and mixed for

24 h, and 15 wt. including solution K, 15 wt. including solution L and 100 wt. of solution M is displaced together and applied onto conductive paper (having a surface resistance of 25 ohms) including 40% carbon fiber to form a covering layer with a thickness of 10 µm. Get electroregister plate.

When pyroxoperic acid is not added,

registration is not achieved even with a recording potential of 100 volts, but when it is added, red registration is achieved with a recording potential of 45 volts. The structure of the recording material obtained by such

The image shown in FIG. 6. A color-forming conductive layer 9 is formed of paper 12 impregnated with carbon 12.

Example 7. Bleached sulfite pulp is roughly ground in a hammer mill.

1000 weight. h. copper iodide in the form of small particles and 1 wt. iodine is added to the resulting paper based on the solution containing the size-determining agent. The paper material is then made in the form of paper by means of a cylindrical paper mill so that a paper thickness corresponding to 45 g / m-1 is obtained. In this case, since a significant amount of conductive material along with the determinant

The dimensions of the agent enter the white water during the paper making process, the white water turns black during the material preparation process, depending on the amount of addition, so that the conductive material is maintained in the range of 6.0 wt. % relative to paper weight.

Solution D is applied to the specified paper in a manner similar to that described in Example 1 to form an electrical recording material. The resulting structure is shown in FIG. 7. Color forming layer 3 is obtained on paper 13 including a conductive layer. In this register material, a blue trace of recording is obtained, having a distinct optical density of 0.4 at a recording potential of 600 volts. When iodine is not added as an agent that consumes resistance, registration is not obtained at a voltage of 600 volts.

Comparison of recording processes is given in the table. 17 F o rumula m invented 1. Electro-regenerative material, including a substrate, a conductive layer containing copper iodide and a binder, and a color-forming layer, containing a binder and the sensitive color-forming component, characterized in that the ability of the material, the conductive layer additionally contains iodine or hydrogen peroxide, or an oxo-salt, or ieroxyacid, or nermanganate in a quantity sufficient to form free iodine from copper iodide in the layer from 0.05 to 0.2%. 2. The material of Clause 1, of which it is apt, and in that it contains a mixture of leukoosnosani triphenylmethane dye or leuco-base fluorane dye and organic acid or phenol as the body-sensitive color-forming component. 3. Material io and. 1, characterized in that, as a color-sensitive component, it contains a leukoosiovai redox dye. 4. Material clause 1, characterized in that the substrate contains paper or paper impregnated with carbon, or paper with a deposited metal, or half-size film, or glass. The sources of the information, irinigated in view of the expert examination of PGteit Japan L 1331 cl. USS, 1973.