CN1279125C - Nano-grade inorganic colour paste for ink-jet printing ink - Google Patents
Nano-grade inorganic colour paste for ink-jet printing ink Download PDFInfo
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- CN1279125C CN1279125C CN 200410000322 CN200410000322A CN1279125C CN 1279125 C CN1279125 C CN 1279125C CN 200410000322 CN200410000322 CN 200410000322 CN 200410000322 A CN200410000322 A CN 200410000322A CN 1279125 C CN1279125 C CN 1279125C
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Abstract
The present invention belongs to the field of ink for ink jet printers, and particularly to nanometer-grade inorganic pigment color paste for the ink for ink jet printers. The nanometer-grade inorganic pigment paste is obtained by the following steps: adding inorganic pigment to water and stirring to form a turbid liquid; removing impurities from the turbid liquid by 30 micrometer type filtration; adding a raw material for the coating layers of a wrapping agent and a surface active agent to the processed raw materials; carrying out the shock wave or ultrasonic wave type cyclic processing with superspeed turbulent flows under the pressure of 80 to 150MPa; after the cyclic processing, regulating the pressure to 100 to 130MPa for sunsequent processing to obtain the nanometer-grade inorganic pigment paste. The nanometer-grade inorganic pigment paste has the core wrapping particle size of 30 to 90 nanometers and has the surface at least partially forming a coating layer of the wrapping agent, and the coating layer of the wrapping agent has the surface at least partially bonding with a coating layer of the surface active agent. The nanometer-grade inorganic pigment paste of the present invention can improve the light resistance and the weather resistance of the ink and has vivid colors, and can effectively avoid the clogging of a printing nozzle.
Description
Technical field
The invention belongs to the jetted ink field, particularly a kind of nano grade inorganic dispersible pigment color paste that is used for ink-jet printing ink.
Background technology
At present, domestic widely used ink-jet print cartridge is a dye-type.Dye ink has the weakness that is difficult to overcome: one, and very fastidious to print media, good printing effect often needs special print media support to realize, and especially print on common copy paper, effect is barely satisfactory; Its two, the color resisting power is not enough, the oxygenizement of illumination and air all can make the print image original beautiful color that fades away.For ink-jet printer, two weakness of this of dye ink also are to limit the technology barrier of ink-jet technology development for a long time.
In order to address these problems, once attempted to use pigment to replace dyestuff.Disclosed Japanese patent application (KOKAI) 11-131001 (1999) wherein be described to " ... there are some problems in dyestuff because of its inherent characteristic, and is relatively poor as its print image water tolerance and photostabilization.For addressing these problems, once attempted to use pigment to replace dyestuff to develop ink.Yet "; this ink for ink-jet print is to stick on the fine granular of silica or barium sulfate with pigment; its bounding force is very faint; so in being dispersed in the ink-jet print water mixture time; fine granular is easily from the surface of pigments desorption, and this grain pattern design and preparation method are difficult to the waterproof photostabilization ink jet ink for printing that acquisition has remarkable dispersion stabilization and anti-blocking performance.
The preparation method that other is relevant, as disclosed Chinese patent application CN 1310748A, preferred ball mill, wet type circulation mill; Disc type that disclosed Chinese patent application CN 1214473A is then preferred mill and test omnipotent mill; Other similar approach has ball mill, sand mill, Artlighter, roll formula grinds device, colloidal mill, ultrasonic wave homogenizer, ultra-high voltage homogenizer etc.All there are the following problems in various degree for above method: size-grade distribution is inhomogeneous, energy consumption is too high, mix foreign matter easily, can not handle, be easy to generate acidifying phenomenon etc. continuously.
In addition, because the ink major part that extensively applies in the common spray ink Printing is made up of water, as dispersion and stable be difficult to of insoluble granules of pigments in aqueous environments, and because big or small and the inhomogeneous and particle agglomeration phenomenon of its possible granularity causes easily such as being easy to blocking problem at the ink-jet printer inkjet mouth.
Summary of the invention
One of purpose of the present invention provides a kind of fast light weathering resistance that can improve ink, and simultaneously because of its particle exquisiteness, the color expressive force is outstanding, can effectively avoid stopping up the nano grade inorganic dispersible pigment color paste that is used for ink-jet printing ink that the printing nozzle phenomenon occurs.
A further object of the present invention provides a kind of employing ultra-high speed shockwave or ultrasonic machining mode, can carry out pulverizing, emulsification, dispersion, the coating of raw material simultaneously, can shorten working hours significantly and cut down the consumption of energy, reduce production cost, simultaneously owing in the course of processing, do not mix impurity, the diameter of processing back particle can on average be stabilized between 30～90 nanometers, can realize high purity processing, and suitable preparation is used for the method for the nano grade inorganic dispersible pigment color paste of ink-jet printing ink.
The present invention be directed to the existing replacement technology that is applied to the weakness of ink-jet printing ink technology and develops.The principal element that influences the printed product preservation is the oxidation of ultraviolet irradiation and air; by the extremely strong inorganic pigment granules of preferred preparation stability; and employing has the resin glue of waterproof, antiultraviolet provide protection as coating material; make inorganic pigment granules avoid extraneous and corrode, improve the dispersive ability of inorganic pigment granules in aqueous environments and sticking power on different print media.In order to realize above target, the invention provides a kind of new preparation method, utilize wet type LINEAR CONTINUOUS device that the circular treatment function is provided, produce ultra-high voltage, cause moment ultra high rate shockwave to reach 1,000kgf/cm by reciprocating-piston simultaneously
2Above processing pressure can give enough energy dispersions and pulverize raw material to reach the particle diameter distribution below the 100nm, and produced simultaneously turbulent flow and ultrasonic wave effect can help encapsulation agents coating adhering on the coated core particle surface.
The nano grade inorganic dispersible pigment color paste that is used for ink-jet printing ink of the present invention obtains by following noodle producing method.In weight part, 4.2～15.6 parts mineral dyes are joined in 64.2～84.2 parts the water, stir its muddy liquid of back and selected 30 microns screening and removing impurities, the encapsulation agents that in the raw material of handling well, adds 3.5～18.3 parts again, 2.3～7.5 parts tensio-active agent coating material, (be preferably 100～130MPa) ultra-high speed turbulent flows under ultra-high voltage and producing shockwave or ultrasonic wave circular treatment under 80～150MPa pressure, after through 1～30 circulation, pressure is adjusted in 100～130MPa to be continued to handle, the lasting treatment time is 5 minutes～2 hours, is preferably 10 minutes～1 hour; Make nano grade inorganic pigment reach the effect of emulsification highly, dispersion, fragmentation, coating.
The mineral dye coated core particle size distribution that the present invention obtains is 30～90 nanometers, and the part surface at least of described coated core particle forms the encapsulation agents coating; And the bonding of part surface at least in described encapsulation agents coating has the tensio-active agent coating.
Described shockwave or hyperacoustic instantaneous reach 1,000kgf/cm
2More than.
The particle diameter of selected nano grade inorganic granules of pigments raw material is 30～200 nanometers among the present invention, add what of encapsulation agents by control, and the time of ultra-high speed shockwave or ultrasonication, form the encapsulation agents coating and form the tensio-active agent coating at the part surface at least of each coated core particle at the part surface at least of encapsulation agents coating.
Used bag nuclear inorganic pigment granules is the uniform red iron oxide of grain size number, iron oxide yellow, group's indigo plant or carbon black among the present invention, and the crystalline particle particle diameter is 30～200 nanometers, preferably 30～100 nanometers, more preferably 30～90 nanometers.The BET specific surface area value 20m that bag nuclear inorganic pigment granules has
2/ g～1000m
2/ g can control to a certain extent by the pressure and the treatment time of shock treatment, but main still by raw-material selection, was reunited by crystalline particle particle diameter 100 nanometers such as the starting material particle, and the specific surface value is about 50m after then handling
2/ g if the crystalline particle of 30 nanometers is reunited, then handles back specific surface value and is about 200m
2/ g is because also will consider the influence of coating, so the specific surface value is less than normal conditions.The specific surface area value preferably is not less than 20m
2/ g more preferably is not less than 50m
2/ g.Consider on bag nuclear matter surface to form even packing coating, the upper limit of the BET specific surface area of bag nuclear inorganic pigment granules is 1000m preferably
2/ g.
The used encapsulation agents of the present invention can be the tackiness agent of any kind of, as long as can make parents' surface active molecules can be relatively easy to be bonded in the surface of inorganic pigment granules.Preferred encapsulation agents includes organic silicon compound, coupler, resene or their any mixture etc.Described silicoorganic compound comprise organoalkoxysilane, fluorine-containing alkyl silane or their any mixture.
Described coupler comprises silylation coupler, metatitanic acid alkali coupler, aluminate-base coupler or their any mixture.
Described resene comprises high transparent heterocycle or cycloaliphatic epoxy resin, and its molecular weight is preferably between 300～2000.
The used tensio-active agent of the present invention is selected from aniorfic surfactant, nonionic surface active agent, high molecular polymer dispersion agent or their any mixture.
Described aniorfic surfactant comprises sodium alkyl benzene sulfonate, aliphatic alcohol sulfate or their any mixture.
Described nonionic surface active agent comprises poly-butylated resin, polyxyethylated alkylphenol formaldehyde condensation products or their any mixture.
Described high molecular polymer dispersion agent comprises derivatived cellulose, styrene-maleic anhydride copolymer, vinylbenzene-Sipacril 2739OF or their any mixture.
Can obtain the inorganic pigment color paste of size distribution continuously and stably by the inventive method, and form the encapsulation agents coating at the part surface at least of described coated core particle at the coated core particle of 30～90 nanometers; With the bonding of part surface at least the tensio-active agent coating is arranged in described encapsulation agents coating.
Characteristics of the present invention are: the raw material configuration is easy, and technology is reasonable, can design the diameter of particle as required, can cut down the consumption of energy save energy significantly; Compare with working method in the past, the ratio that mixes foreign matter is few, does not need media, realizes high purity processing, and mass production is suitable for the preparation of the nano grade inorganic dispersible pigment color paste of ink-jet printing ink very much.Prepared nano grade inorganic dispersible pigment color paste is applied to ink-jet printing ink, can improve the fast light weathering resistance of ink greatly, the outstanding appearance of also effectively having avoided stopping up the printing nozzle phenomenon of color expressive force simultaneously.The toxicity organic composition that adds can promote safer Products Development with to compare usage quantity few in the past; Owing to adopted the LINEAR CONTINUOUS processing, in the course of processing, suppressed the generation of acidifying phenomenon to greatest extent.
Be described further below in conjunction with embodiment, but not as a limitation of the invention.
Embodiment
Embodiment.
At first the described interior nuclear raw material of table one is crossed 30 microns screening and removing impurities, according to carrying out proportioning raw materials shown in the table two and various materials being mixed, obtain embodiment 1～24 and comparative example 1～4 then; Embodiment 1～24 loaded on the NANOMIZER handler according to the embodiment of table three ultra-high speed shockwave circular treatment (is preferably 100～130MPa) again under 80～150MPa pressure, after through 1～30 circulation, pressure is adjusted in lasting the processing 5 minutes～2 hours about 130MPa; Comparative example and embodiment product performance detected result are as shown in Table 4.
Performance evaluation comprises: 1) the product average particle size is measured; 2) measurement of contact angle; 3) cryopreservation stability is measured; 4) thermal stability determination; 5) photostabilization is measured.
Wherein, the mensuration of average particle size has adopted the Zeta particle size analyzer as detector, injects 100 milliliters in sample in sample pool, measures size-grade distribution under middling speed stirs; Measurement of contact angle adopts the contact angle instrument, is measuring with reference to surface (the special-purpose photo papers of EPSON) with the sample drop of 0.4 microlitre; It is to preserve 3 hours under subzero 10 degrees centigrade situation that low-temperature stability is measured, and observes whether precipitation or other variations are arranged; Thermal stability determination then is 80 degrees centigrade of heating in water bath 3 hours, observes whether precipitation or other variations are arranged; It is with the flat common printer paper surface that is coated in of sample that photostabilization is measured, and under 500 watts ultra violet lamp 12 hours then, observes whether coloured variation.Above low-temperature stability, thermostability and photostabilization evaluation are divided into Three Estate: A represents best in quality, and B represents that quality is general, and C represents second-rate.
Table one inner core particles material and performance
| The inner core particles kind | Inner nuclear material | Shape | Average particulate diameter (nm) |
| Inner core particles 1 | Red iron oxide | Spherical | 200 |
| Inner core particles 2 | Red iron oxide | Spherical | 150 |
| Inner core particles 3 | Red iron oxide | Spherical | 100 |
| Inner core particles 4 | Iron oxide yellow | Granular | 80 |
| Inner core particles 5 | The group is blue | Spherical | 100 |
| Inner core particles 6 | Carbon black | Spherical | 50 |
Table two product is mainly filled a prescription
| Embodiment | Inner nuclear material and parts by weight | Coating material and parts by weight | Tensio-active agent coated material and parts by weight |
| Embodiment 1 | Inner core particles 1 (4.2) | Organoalkoxysilane (8.2) | Vinylbenzene-methacrylic acid (5.2) |
| Embodiment 2 | Inner core particles 2 (15.6) | Organoalkoxysilane (8.2) | Vinylbenzene-methacrylic acid (5.2) |
| Embodiment 3 | Inner core particles 3 (10.3) | Organoalkoxysilane (8.2) | Vinylbenzene-methacrylic acid (5.2) |
| Embodiment 4 | Inner core particles 3 (10.0) | Organoalkoxysilane (18.3) | Vinylbenzene-methacrylic acid (7.5) |
| Embodiment 5 | Inner core particles 3 (10.0) | Organoalkoxysilane (3.5) | Vinylbenzene-methacrylic acid (2.3) |
| Embodiment 6 | Inner core particles 3 (10.0) | Organoalkoxysilane (8.0) | Sodium dodecylbenzene sulfonate (2.3) |
| Embodiment 7 | Inner core particles 3 (10.0) | Organoalkoxysilane (8.0) | Poly-butylated resin (2.3) |
| Embodiment 8 | Inner core particles 3 (10.0) | Organoalkoxysilane (8.0) | Derivatived cellulose etc. (2.3) |
| Embodiment 9 | Inner core particles 3 (10.0) | Silylation coupler (10.0) | Vinylbenzene-methacrylic acid (7.5) |
| Embodiment 10 | Inner core particles 3 (10.0) | Silylation coupler (10.0) | Sodium dodecylbenzene sulfonate (7.5) |
| Embodiment 11 | Inner core particles 3 (10.0) | Silylation coupler (10.0) | Poly-butylated resin (7.5) |
| Embodiment 12 | Inner core particles 3 (10.0) | Silylation coupler (10.0) | Derivatived cellulose etc. (7.5) |
| Embodiment 13 | Inner core particles 3 (10.0) | Aluminate-base coupler (8.0) | Vinylbenzene-methacrylic acid (3.2) |
| Embodiment 14 | Inner core particles 3 (10.0) | Aluminate-base coupler (8.0) | Sodium dodecylbenzene sulfonate (3.2) |
| Embodiment 15 | Inner core particles 3 (10.0) | Aluminate-base coupler (8.0) | Poly-butylated resin (3.2) |
| Embodiment 16 | Inner core particles 3 (10.0) | Aluminate-base coupler (8.0) | Derivatived cellulose etc. (3.2) |
| Embodiment 17 | Inner core particles 3 (10.0) | Metatitanic acid alkali coupler (8.0) | Vinylbenzene-methacrylic acid (3.2) |
| Embodiment 18 | Inner core particles 3 (10.0) | Metatitanic acid alkali coupler (8.0) | Sodium dodecylbenzene sulfonate (3.2) |
| Embodiment 19 | Inner core particles 3 (10.0) | Metatitanic acid alkali coupler (8.0) | Poly-butylated resin (3.2) |
| Embodiment 20 | Inner core particles 3 (10.0) | Metatitanic acid alkali coupler (8.0) | Derivatived cellulose etc. (3.2) |
| Embodiment 21 | Inner core particles 3 (10.0) | Resins, epoxy coupler (8.0) | Vinylbenzene-methacrylic acid (3.2) |
| Embodiment 22 | Inner core particles 4 (10.0) | Resins, epoxy coupler (8.0) | Vinylbenzene-methacrylic acid (3.2) |
| Embodiment 23 | Inner core particles 5 (10.0) | Organoalkoxysilane (8.0) | Vinylbenzene-methacrylic acid (3.2) |
| Embodiment 24 | Inner core particles 6 (10.0) | Metatitanic acid alkali coupler (8.0) | Vinylbenzene-methacrylic acid (3.2) |
| Comparative example 1 | Inner core particles 3 (10.0) | ||
| Comparative example 2 | Inner core particles 4 (10.0) | ||
| Comparative example 3 | Inner core particles 5 (10.0) | ||
| Comparative example 4 | Inner core particles 6 (10.0) |
Table two product is mainly filled a prescription (continuing)
| Embodiment | The umber that adds entry |
| Embodiment 1 | 82.4 |
| Embodiment 2 | 71.0 |
| Embodiment 3 | 76.3 |
| Embodiment 4 | 64.2 |
| Embodiment 5 | 84.2 |
| Embodiment 6 | 79.7 |
| Embodiment 7 | 79.7 |
| Embodiment 8 | 79.7 |
| Embodiment 9 | 72.5 |
| Embodiment 10 | 72.5 |
| Embodiment 11 | 72.5 |
| Embodiment 12 | 72.5 |
| Embodiment 13 | 78.8 |
| Embodiment 14 | 78.8 |
| Embodiment 15 | 78.8 |
| Embodiment 16 | 78.8 |
| Embodiment 17 | 78.8 |
| Embodiment 18 | 78.8 |
| Embodiment 19 | 78.8 |
| Embodiment 20 | 78.8 |
| Embodiment 21 | 78.8 |
| Embodiment 22 | 78.8 |
| Embodiment 23 | 78.8 |
| Embodiment 24 | 78.8 |
| Comparative example 1 | 90.0 |
| Comparative example 2 | 90.0 |
| Comparative example 3 | 90.0 |
| Comparative example 4 | 90.0 |
Table three implementation method
| Embodiment | Cycle index | Processing pressure (MPa) | Continue the treatment time (minute) |
| Embodiment 1 | 2 | 130 | 5 |
| Embodiment 2 | 3 | 130 | 8 |
| Embodiment 3 | 4 | 130 | 10 |
| Embodiment 4 | 5 | 100 | 12 |
| Embodiment 5 | 8 | 150 | 15 |
| Embodiment 6 | 12 | 130 | 30 |
| Embodiment 7 | 20 | 150 | 60 |
| Embodiment 8 | 30 | 150 | 120 |
| Embodiment 9 | 10 | 150 | 30 |
| Embodiment 10 | 10 | 150 | 30 |
| Embodiment 11 | 10 | 130 | 30 |
| Embodiment 12 | 10 | 130 | 30 |
| Embodiment 13 | 10 | 100 | 30 |
| Embodiment 14 | 10 | 100 | 30 |
| Embodiment 15 | 10 | 150 | 30 |
| Embodiment 16 | 10 | 150 | 30 |
| Embodiment 17 | 10 | 150 | 30 |
| Embodiment 18 | 10 | 150 | 30 |
| Embodiment 19 | 10 | 150 | 30 |
| Embodiment 20 | 10 | 130 | 30 |
| Embodiment 21 | 10 | 130 | 30 |
| Embodiment 22 | 10 | 100 | 30 |
| Embodiment 23 | 10 | 100 | 30 |
| Embodiment 24 | 10 | 150 | 30 |
Table four-product Performance Detection
| Embodiment | Average particulate diameter (nm) | Contact angle | Cold storage stability | Thermostability | Photostabilization |
| Embodiment 1 | 150 | 43 | B | A | A |
| Embodiment 2 | 100 | 41 | B | A | A |
| Embodiment 3 | 83 | 42 | A | A | A |
| Embodiment 4 | 80 | 45 | A | A | A |
| Embodiment 5 | 75 | 42 | A | A | A |
| Embodiment 6 | 82 | 48 | A | A | A |
| Embodiment 7 | 73 | 51 | A | A | A |
| Embodiment 8 | 70 | 36 | A | A | A |
| Embodiment 9 | 76 | 39 | A | A | A |
| Embodiment 10 | 78 | 48 | A | A | A |
| Embodiment 11 | 74 | 47 | A | A | A |
| Embodiment 12 | 80 | 41 | A | A | A |
| Embodiment 13 | 85 | 43 | A | A | A |
| Embodiment 14 | 86 | 31 | A | A | A |
| Embodiment 15 | 79 | 62 | A | A | A |
| Embodiment 16 | 75 | 47 | A | A | A |
| Embodiment 17 | 74 | 45 | A | A | A |
| Embodiment 18 | 78 | 46 | A | A | A |
| Embodiment 19 | 78 | 44 | A | A | A |
| Embodiment 20 | 80 | 44 | A | A | A |
| Embodiment 21 | 81 | 49 | A | A | A |
| Embodiment 22 | 50 | 65 | A | A | A |
| Embodiment 23 | 65 | 42 | A | A | A |
| Embodiment 24 | 50 | 50 | A | A | A |
| Comparative example 1 | 100 | 18 | C | C | A |
| Comparative example 2 | 80 | 21 | C | C | A |
| Comparative example 3 | 100 | 15 | C | C | A |
| Comparative example 4 | 50 | 19 | C | C | A |
Claims (5)
1. nano grade inorganic dispersible pigment color paste that is used for ink-jet printing ink, it is characterized in that: described dispersible pigment color paste obtains by following noodle producing method, in weight part, 4.2～15.6 parts mineral dyes are joined in 64.2～84.2 parts the water, stir its muddy liquid of back and selected 30 microns screening and removing impurities, the encapsulation agents that in the raw material of handling well, adds 3.5～18.3 parts again, 2.3～7.5 parts tensio-active agent coating material, produce shockwave or ultrasonic wave circular treatment in the ultra-high speed turbulent flow under ultra-high voltage under 80～150MPa pressure, through after the circular treatment, pressure is adjusted in 100～130MPa continues to handle, obtain the nano grade inorganic dispersible pigment color paste;
Described mineral dye is red iron oxide, iron oxide yellow, group's indigo plant or carbon black, and its grain diameter is 30～200 nanometers;
Described encapsulation agents comprises organoalkoxysilane, fluorine-containing alkyl silane, silylation coupler, metatitanic acid alkali coupler, aluminate-base coupler, high transparent heterocycle or cycloaliphatic epoxy resin or their any mixture.
2. dispersible pigment color paste as claimed in claim 1 is characterized in that: the coated core particle size distribution of described nano grade inorganic pigment is 30～90 nanometers, and the part surface at least of described coated core particle forms the encapsulation agents coating; And the bonding of part surface at least in described encapsulation agents coating has the tensio-active agent coating.
3. dispersible pigment color paste as claimed in claim 1 or 2 is characterized in that: the coated core particle of described nano grade inorganic pigment has BET specific surface area value 20m
2/ g～1000m
2/ g.
4. dispersible pigment color paste as claimed in claim 1 is characterized in that: described tensio-active agent is selected from aniorfic surfactant, nonionic surface active agent, high molecular polymer dispersion agent or their any mixture.
5. dispersible pigment color paste as claimed in claim 4 is characterized in that: described aniorfic surfactant comprises sodium alkyl benzene sulfonate, aliphatic alcohol sulfate or their any mixture;
Described nonionic surface active agent comprises poly-butylated resin, polyxyethylated alkylphenol formaldehyde condensation products or their any mixture;
Described high molecular polymer dispersion agent comprises derivatived cellulose, styrene-maleic anhydride copolymer, vinylbenzene-Sipacril 2739OF or their any mixture.
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|---|---|---|---|
| CN 200410000322 CN1279125C (en) | 2004-01-07 | 2004-01-07 | Nano-grade inorganic colour paste for ink-jet printing ink |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 200410000322 CN1279125C (en) | 2004-01-07 | 2004-01-07 | Nano-grade inorganic colour paste for ink-jet printing ink |
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| CN1279125C true CN1279125C (en) | 2006-10-11 |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| US9034430B2 (en) | 2008-10-16 | 2015-05-19 | Institute Of Chemistry, Chinese Academy Of Sciences | Manufacture method of metal plate substrate for computer-to-plate of inkjet printing |
| CN101659808B (en) * | 2009-08-25 | 2011-09-21 | 江苏格美高科技发展有限公司 | Aqueous jet ink printing pigment ink for textile and production method thereof |
| CN103183984A (en) * | 2011-12-28 | 2013-07-03 | 广东天龙油墨集团股份有限公司 | Nanometer long afterglow energy storage type ink-jet ink for ink-jet printing |
| CN113549371A (en) * | 2021-08-18 | 2021-10-26 | 朗升柯式印刷(深圳)有限公司 | Environment-friendly water-based printing ink and preparation method thereof |
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