CN101962492B - Novel multi-layer coating angularly heterochrome interference color pearlescent pigment - Google Patents
Novel multi-layer coating angularly heterochrome interference color pearlescent pigment Download PDFInfo
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- CN101962492B CN101962492B CN200910161502.1A CN200910161502A CN101962492B CN 101962492 B CN101962492 B CN 101962492B CN 200910161502 A CN200910161502 A CN 200910161502A CN 101962492 B CN101962492 B CN 101962492B
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Abstract
The invention discloses a novel multi-layer coating angularly heterochrome interference color pearlescent pigment, which takes a transparent or a semitransparent sheet as a substrate. High refractive index coating and low refractive index coating are repeatedly coated on the outer surface of the substrate in sequence in an alternating manner, wherein, the number of the coating is at least three layers; the low refractive index coating is arranged between two high refractive index coatings; intermediate transitional coatings with gradually changed refractive indexes are arranged between the high refractive index coating and the low refractive index coating, and between the low refractive index coating and the high refractive index coating; the intermediate transitional coating is composed of metallic silicate, metallic aluminate and mixture composed of the metallic silicate, the metallic aluminate, high refractive index metallic oxide and low refractive index compound. Because of the existence of the intermediate transition coating, the pigment provided by the invention enables the color-changing transition region color variability to be more clear and obvious, and the color saturation to be higher. The pigment can be used in automobile paint, cosmetic formula, paint, printing ink, plastics and glass industries.
Description
Technical field
The present invention relates to a kind of pearly pigment, relate in particular to the interference color pearly pigment that a kind of novel multi-layer applies.
background technology
When high refractive index metal oxide and low refractive index compound alternately are coated on slim substrate, the material applied by change, thickness and structure, can present many different optical effects.And can be by suitable structure design and the thickness of selecting coat, as the color change of visibility function, also can become strongly, with the viewing angle difference, can present the variation that two or more interfere colors, formation effect interference look pearly pigment.
In recent years, many patents (JP2000517374, US6656259, US6284034, CN1470569, CN1563210 etc.) have proposed the employing liquid-phase chemistry deposition technique, rely on high and low refractive index material alternate multiple coating processes to prepare the method for effect interference look pearly pigment.Pigment prepared by this method has the changeable colors along with angle effect, but color changes the variation that is great-jump-forward with visual angle, and the zone of transition colour of two kinds of color change is very not obvious.This is because in pigment structure, the refractive index of adjacent high and low refractive index coating differs greatly, the sudden change that in the high refractive index coating, to low refractive index coating transit time, can produce refractive index, thereby make that the zone of transition color change is not obvious, colorimetric purity is also low, this pigment is greatly affected in the application in each field.
summary of the invention
The objective of the invention is the defect for above-mentioned prior art, a kind of transition zone in colour-change is provided, and not only colorimetric purity is high, and changeable colors along with angle changes obviously the effect interference look pearly pigment that novel multi-layer applies clearly.
The effect interference look pearly pigment of multiple coating of the present invention, take transparent or semitransparent inorganic sheet as substrate, alternately apply successively the high refractive index coating of metal oxides of refractive index>1.8 and the low refractive index compound coat of refractive index<1.8 at the substrate outside surface, be coated with at least three layers of the numbers of plies, wherein, the low refractive index compound coat must be to be placed between two high refractive index coating of metal oxides, between high refractive index coating of metal oxides and low refractive index compound coat, between low refractive index compound coat and high refractive index metal oxide, the middle transition coating that all there is a refractive index gradual change.
Being applicable to transparent or semitransparent inorganic sheet of the present invention is natural mica, synthetic mica, glass, silicon-dioxide, aluminum oxide etc.
The high refractive index metal oxide that the present invention adopts is TiO
2, Fe
2o
3, Fe
3o
4, SnO
2, ZrO
2, Cr
2o
3, CoO, Co
2o
3and/or their mixture or mixture, preferably TiO
2, Fe
2o
3and/or their mixture or mixture.
The low refractive index metal oxide that the present invention adopts is silicon-dioxide, hydrated SiO 2, aluminum oxide, hydrated aluminum oxide and/or their mixture or mixture, preferably silicon-dioxide, hydrated SiO 2 and/or their mixture or mixture.
In the effect interference look pearly pigment of multiple coating of the present invention, the middle transition coating of described refractive index gradual change is comprised of the mixture of metal silicate, metal aluminate and they and high refractive index metal oxide and low refractive index compound, the composition of this coating is the even variation state, nearly high refractive index coating interface zone, metal content is high, and refractive index is also higher, nearly low refractive index coating interface zone, the content of silicon or aluminium is high, and refractive index is also lower.
In pigment of the present invention, the thickness of described low refractive index compound coat is 10～900nm, preferably 20～800nm.
In pigment of the present invention, the thickness of described high refractive index coating of metal oxides is 10～180nm, preferably 20～150nm.
In pigment of the present invention, the thickness of the middle transition coating of described refractive index gradual change is 5～120nm, preferably 20～100nm.
The effect interference look pearly pigment of multiple coating of the present invention, can also further carry out rear coating and aftertreatment while needing.Rear coating is painted for the multilayer interference pearly pigment is carried out, and rear coating tinting material used can be mineral dye or pigment dyestuff, and wherein mineral dye comprises ferric oxide, iron orchid, cobalt aluminate, chromium hydroxide etc. at a low price; Pigment dyestuff comprises that some phthalocyanine pigments, azo pigment, quinoline a word used for translation sting ketone pigment etc.Aftertreatment is for the multilayer interference pearly pigment is carried out to surface modification, to improve the stability of pigment to light, water and weather; Improve pigment consistency, dispersiveness and dispersion stabilization in use, aftertreatment can be at oxide compound, the hydrous oxide of surface of pigments metallizing element or non-metallic element, these elements, as aluminium, zirconium, cerium, silicon, chromium etc., can also apply organo-silicon coupling agent etc.
The effect interference look pearly pigment of multiple coating of the present invention, compare with the disclosed various effect interference look pearly pigments of previous patent, and outstanding characteristics are in the structure of pigment of the present invention, have the middle transition coating of refractive index gradual change.Due to the shock absorption that the middle transition coating is arranged, by the high refractive index coating, to low refractive index coating transit time, refractive index can not undergone mutation, but gradually evenly reduce; Equally by the low refractive index coating to high refractive index coating transit time, refractive index can not undergone mutation yet, and is gradually evenly to raise yet.The effect interference look pearly pigment that such pigment structure obtains, the color of the zone of transition of two kinds of colour-change changes can be more obvious, and the level of even variation can be very clear gradually for color.
The effect interference look pearly pigment of multiple coating of the present invention, can be used for the industries such as painting dressing automobiles paint, cosmetic formulations and coating, printing-ink, plastics, pottery and glass.
Specific embodiment
Following examples are for further describing the present invention, but non-limiting the present invention.
Embodiment 1
The natural muscovite sheet 15g that to get particle diameter be 10～60mum, be suspended in the 500ml deionized water, stirs and be heated to 80 ℃.Hydrochloric acid with 15% is adjusted to 4.0 by the pH value of suspension, the FeCl3 solution that to be metered into 285ml concentration be 10%, and keep the pH value of suspension constant by dripping 15% NaOH solution, after dropwising, continue to stir 20 minutes.
By adding 30%NaOH solution that the pH value of suspension is adjusted to 8.5, and constant temperature stirs a quarter.(water glass is containing SiO for the sodium silicate solution that to be metered into 650ml concentration be 10% weight
2be 20.5%), and keep the pH value of suspension constant by the hydrochloric acid of dropping 15%.After dropwising, continue constant temperature and stir 40 minutes.
By adding 15% hydrochloric acid soln that the pH value of suspension is adjusted to 4.0, and constant temperature stirs 20 minutes.Be metered into the FeCl that 71ml concentration is 10%
3solution, and keep the pH value of suspension constant by the NaOH solution of dropping 15%, after dropwising, continue to stir 20 minutes.
After filtration solid is separated and dry under washing and 150 ℃, then calcined 1 hour through 800 ℃ of temperature programmed controls, sieve finally by 100 orders.
Due to the excitation of heat, between hydrous iron oxide coating and aqua oxidation silicon coating, mutual migration and the infiltration of ion can occur in calcination process, iron ion is to the migration of aqua oxidation silicon coating, infiltration and joint; Silicate ion, to the migration of hydrous iron oxide coating, infiltration and joint, finally, between ferric oxide coating and silica dioxide coating, forms the middle transition coating of refractive index gradual change.This tie coat is by the compositions of mixtures of the silicate of iron and ferric oxide, silicon-dioxide, and the silicate content of central section iron is higher; Higher near the nearlyer ferric oxide ratio of ferric oxide coating interface, refractive index is also higher; Higher near the nearlyer silica ratios in silica dioxide coating interface, refractive index is also lower.The structure that the final like this pigment obtained has is: sheet mica/Fe
2o
3layer/Fe
2o
3silicate+the SiO of+iron
2mixolimnion/SiO
2layer/SiO
2silicate+the Fe of+iron
2o
3mixolimnion/Fe
2o
3layer.
The pigment and the water white transparency printing ink medium PU tackiness agent that obtain are mixed in proportion, then on black and white base stock card, scrape sample.The color saturation that colour atla shows is high, the color change from the vertical angle of view to the horizontal view angle be red-purple to scarlet to orange, more obviously change continuously clearly to yellowish green to orange-yellow.
Embodiment 2
Get 15g glass flake (particle diameter is 30～70mum) and be suspended in the 350ml deionized water, stir and be heated to 75 ℃.Hydrochloric acid with 15% is adjusted to 2.2 by the pH value of suspension, is metered into the TiCl that 24ml concentration is 400g/L
4solution, and keep the pH value of suspension constant by the NaOH solution of dropping 32%, after dropwising, continue constant temperature and stir 30 minutes.
By adding 32%NaOH solution that the pH value of suspension is adjusted to 8.5, and constant temperature stirs a quarter.(water glass is containing SiO for the sodium silicate solution that to be metered into 590ml concentration be 10% weight
2be 20.5%), and keep the pH value of suspension constant by the hydrochloric acid of dropping 15%.After dropwising, continue constant temperature and stir 40 minutes.
By adding 15% hydrochloric acid soln that the pH value of suspension is adjusted to 2.2, and constant temperature stirs 20 minutes.Be metered into the TiCl that 35ml concentration is 400g/L
4solution, and keep the pH value of suspension constant by the NaOH solution of dropping 32%, after dropwising, continue to stir 20 minutes.
After filtration solid is separated and dry under washing and 140 ℃, then calcined 1 hour through 700 ℃ of temperature programmed controls, sieve finally by 100 orders.
Due to the excitation of heat, between hydrous titanium oxide coating and aqua oxidation silicon coating, mutual migration and the infiltration of ion can occur in calcination process, titanium ion is to the migration of aqua oxidation silicon coating, infiltration and joint; Silicate ion to
The migration of hydrous titanium oxide coating, infiltration and joint, finally, between coating of titanium dioxide and silica dioxide coating, form the middle transition coating of refractive index gradual change.This tie coat is by the compositions of mixtures of the silicate of titanium and titanium dioxide, silicon-dioxide, and the silicate content of central section titanium is higher; Higher near the nearlyer titanium dioxide ratio in coating of titanium dioxide interface, refractive index is also higher; Higher near the nearlyer silica ratios in silica dioxide coating interface, refractive index is also lower.The structure that the final like this pigment obtained has is: glass unicorn sheet/TiO
2layer/TiO
2silicate+the SiO of+titanium
2mixolimnion/SiO
2layer/SiO
2silicate+the TiO of+titanium
2mixolimnion/TiO
2layer.
The pigment and the water white transparency printing ink medium PU tackiness agent that obtain are mixed in proportion, then on black and white base stock card, scrape sample.The color saturation that colour atla shows is high, and the colour-change from the vertical angle of view to the horizontal view angle is that beautiful yellow-green colour is green to orchid to green, then obviously changing continuously clearly to blue purple to intense violet color
Embodiment 3
Get 15g natural mica sheet (particle diameter is 10～60mum) and be suspended in the 400ml deionized water, stir and be heated to 75 ℃.Hydrochloric acid with 15% is adjusted to 2.0 by the pH value of suspension, is metered into the TiCl that 59ml concentration is 400g/L
4solution, and keep the pH value of suspension constant by the NaOH solution of dropping 32%, after dropwising, continue constant temperature and stir 30 minutes.
By adding 32%NaOH solution that the pH value of suspension is adjusted to 8.5, and constant temperature stirs a quarter.(water glass is containing SiO for the sodium silicate solution that to be metered into 680ml concentration be 10% weight
2be 20.5%), and keep the pH value of suspension constant by the hydrochloric acid of dropping 15%.After dropwising, continue constant temperature and stir 40 minutes.
By adding 15% hydrochloric acid soln that the pH value of suspension is adjusted to 3.5, and constant temperature stirs 20 minutes.Be metered into the FeCl of 53ml concentration 9.5%
3solution, and keep the PH value of suspension constant by the NaOH solution of dropping 15%, after dropwising, continue to stir 20 minutes.
After filtration solid is separated and dry under washing and 150 ℃, then calcined and coolingly sieve by 100 orders in 1 hour through 800 ℃ of temperature programmed controls.
In calcination process due to the excitation of heat, between hydrous titanium oxide coating and aqua oxidation silicon coating, aqua oxidation silicon coating and hydrous iron oxide be coated with mutual migration and the infiltration that ion all can occur interlayer, titanium ion is to the migration of aqua oxidation silicon coating, infiltration and engage; Silicate ion is to the migration of hydrous titanium oxide coating, infiltration and joint; Iron ion is to the migration of aqua oxidation silicon coating, infiltration and joint; Silicate ion is to the migration of hydrous iron oxide coating, infiltration and joint.Finally between coating of titanium dioxide and silica dioxide coating, form the middle transition coating of refractive index gradual change, this tie coat is by the compositions of mixtures of the silicate of titanium and titanium dioxide, silicon-dioxide, and the silicate content of central section titanium is higher; Higher near the nearlyer titanium dioxide ratio in coating of titanium dioxide interface, refractive index is also higher; Higher near the nearlyer silica ratios in silica dioxide coating interface, refractive index is also lower; Be coated with interlayer at silica dioxide coating and ferric oxide, also form the middle transition coating of refractive index gradual change.This tie coat is by the compositions of mixtures of the silicate of iron and three oxygen two iron, silicon-dioxide, and the silicate content of central section iron is higher; Higher near the nearlyer three oxygen two iron ratios of ferric oxide coating interface, refractive index is also higher; Higher near the nearlyer silica ratios in silica dioxide coating interface, refractive index is also lower; The structure that the final like this pigment obtained has is: sheet mica/TiO
2layer/TiO
2silicate+the SiO of+titanium
2mixolimnion/SiO
2layer/SiO
2silicate+the Fe of+iron
2o
3mixolimnion/Fe
2o
3layer.
The pigment and the water white transparency printing ink medium PU tackiness agent that obtain are mixed in proportion, then on black and white base stock card, scrape sample.The color saturation that colour atla shows is high, and the colour-change from the vertical angle of view to the horizontal view angle is that beautiful red-purple is to redness to orange, then to orange-yellow to yellow clear continuous variation.
Embodiment 4
After carrying out the liquid phase chemical coating by the method for embodiment 2, after washing after filtration, obtain work in-process pigment, be suspended in the 500ml deionized water, stir and be heated to 75 ℃.And by dripping 30% NaOH solution, the pH value of suspension is adjusted to 8.5, and constant temperature stirs 15 minutes.(water glass is containing SiO for the sodium silicate solution that to be metered into 630ml concentration be 10% weight
2be 20.5%), and keep the pH value of suspension constant by the hydrochloric acid of dropping 15%.After dropwising, continue constant temperature and stir 40 minutes.
By adding 15% hydrochloric acid soln that the pH value of suspension is adjusted to 2.2, and constant temperature stirs 20 minutes.Be metered into the TiCl that 20ml concentration is 400g/L
4solution, and keep the pH value of suspension constant by the NaOH solution of dropping 32%, after dropwising, continue to stir 20 minutes.
After filtration solid is separated, dry under washing and 150 ℃, then calcine 1 hour through 700 ℃ of temperature programmed controls, coolingly by 100 orders, sieve.
Due to the excitation of heat, mutual migration and the infiltration of ion can occur between hydrous titanium oxide coating and aqua oxidation silicon coating in calcination process, titanium ion is to the migration of aqua oxidation silicon coating, infiltration and joint; Silicate ion, to the migration of hydrous titanium oxide coating, infiltration and joint, finally, between coating of titanium dioxide and silica dioxide coating, forms the middle transition coating of refractive index gradual change.This tie coat is by the compositions of mixtures of the silicate of titanium and titanium dioxide, silicon-dioxide, and the silicate content of central section titanium is higher; Higher near the nearlyer titanium dioxide ratio in coating of titanium dioxide interface, refractive index is also higher; Higher near the nearlyer silica ratios in silica dioxide coating interface, refractive index is also lower.The structure that the final like this pigment obtained has is: glass unicorn sheet/TiO
2layer/TiO
2silicate+the SiO of+titanium
2mixolimnion/SiO
2layer/SiO
2silicate+the TiO of+titanium
2mixolimnion/TiO
2layer/TiO
2silicate+the SiO of+titanium
2mixolimnion/SiO
2layer/SiO
2silicate+the TiO of+titanium
2mixolimnion/TiO
2layer.
The pigment and the water white transparency printing ink medium PU tackiness agent that obtain are mixed in proportion, then on black and white base stock card, scrape sample.The color saturation that colour atla shows is higher, and the color change transition is also softer.Color change from the vertical angle of view to the horizontal view angle is that beautiful green blue look changes to orange-yellow obviously continuous flow clearly.
Embodiment 5
The finished product pigment suspension that obtains in embodiment 1, in the 500ml deionized water, is stirred and is heated to 75 ℃, and the hydrochloric acid with 15% is adjusted to 5.0 by the pH value of suspension, is metered into the AlCl that 10ml concentration is 5% weight
3.6H
2o solution, and keep the pH value of suspension constant by the NaOH solution of dropping 6%, after dropwising, continue to stir 20 minutes.By adding 32%NaOH solution that the pH value of suspension is adjusted to 8.5, and constant temperature stirs a quarter.(water glass is containing SiO for the sodium silicate solution that to be metered into 15ml concentration be 5% weight
2be 20.5%), and keep the pH value of suspension constant by the hydrochloric acid of dropping 10%.After dropwising, continue constant temperature and stir 20 minutes.
After filtration solid is separated, drying under washing and 120 ℃, coolingly sieve by 100 orders.
The structure that the pigment finally obtained has is: sheet mica/Fe
2o
3layer/Fe
2o
3silicate+the SiO of+iron
2mixolimnion/SiO
2layer/SiO
2silicate+the Fe of+iron
2o
3mixolimnion/Fe
2o
3layer/Al
2o
3.H
2o+SiO
2.H
2the O external protection.This pigment good hydrophilic property, dispersed good in aqueous solution.
The pigment and the water white transparency printing ink medium PU tackiness agent that obtain are mixed in proportion, then on black and white base stock card, scrape sample.The color saturation that colour atla shows is high, the color change from the vertical angle of view to the horizontal view angle be red-purple to scarlet to orange, more obviously change continuously clearly to yellowish green to orange-yellow.
Can draw thus, the external protection coating is thin, refractive index is low, little to the influence of color of pigment self.
Above-described embodiment, just the specific embodiment of the invention is a kind of, and the common variation that those skilled in the art carries out in the technical solution of the present invention scope and replacement all should be included in protection scope of the present invention.
Claims (7)
1. the effect interference look pearly pigment of a multiple coating, it is characterized in that: this pigment be take transparent or semitransparent inorganic sheet as substrate, alternately apply successively the high refractive index coating of metal oxides of refractive index>1.8 at the substrate outside surface, the low refractive index compound coat of refractive index<1.8, be coated with at least three layers of the numbers of plies, and the low refractive index compound coat is placed between two high refractive index coating of metal oxides, between high refractive index coating of metal oxides and low refractive index compound coat, between low refractive index compound coat and high refractive index coating of metal oxides, the middle transition coating that all there is the refractive index gradual change,
The thickness of described high refractive index coating of metal oxides is 10～180nm; The thickness of described low refractive index compound coat is 10～900nm; The thickness of the middle transition coating of described refractive index gradual change is 5～120nm;
The middle transition coating of described refractive index gradual change is comprised of the mixture of metal silicate, high refractive index metal oxide and low refractive index compound; Or the middle transition coating of described refractive index gradual change is comprised of the mixture of metal aluminate, high refractive index metal oxide and low refractive index compound;
The composition of this coating is the even variation state, nearly high refractive index coating interface zone, and metal content is high, and refractive index is also higher; Nearly low refractive index coating interface zone, the content of silicon or aluminium is high, and refractive index is also lower.
2. the effect interference look pearly pigment of multiple coating according to claim 1, it is characterized in that: described transparent or semitransparent inorganic sheet is natural mica, synthetic mica, glass, silicon-dioxide, aluminum oxide.
3. the effect interference look pearly pigment of multiple coating according to claim 1, it is characterized in that: described high refractive index metal oxide is TiO
2, Fe
2o
3, Fe
3o
4, SnO
2, ZrO
2, Cr
2o
3, CoO and/or Co
2o
3, described low refractive index compound is silicon-dioxide, hydrated SiO 2, aluminum oxide and/or hydrated aluminum oxide.
4. the effect interference look pearly pigment of multiple coating according to claim 1, it is characterized in that: described high refractive index metal oxide is TiO
2, Fe
2o
3or their mixture; Described low refractive index compound is silicon-dioxide and/or hydrated SiO 2.
5. the effect interference look pearly pigment of multiple coating according to claim 1, it is characterized in that: the thickness of described high refractive index coating of metal oxides is 20～150nm; The thickness of described low refractive index compound coat is 20～800nm; The thickness of the middle transition coating of described refractive index gradual change is 20～100nm.
6. the effect interference look pearly pigment of multiple coating according to claim 1, it is characterized in that: this pigment carries out rear coating or aftertreatment, and the organic or mineral dye of rear coating is for painted; Aftertreatment applies hydrate or the organic coupling agent of oxide compound or oxide compound, improves pigment performance.
7. the effect interference look pearly pigment of multiple coating according to claim 1, for cosmetic formulations, coating, printing-ink, plastics, pottery and glass industry.
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| CN102675931B (en) * | 2012-05-09 | 2013-12-25 | 四川省川宏精细化工有限公司 | Golden effect pigment and production technology thereof |
| CN103804963B (en) * | 2012-11-14 | 2015-09-09 | 上海纳米技术及应用国家工程研究中心有限公司 | A kind of preparation method possessing optical interference camouflage paint compared with high saturation |
| CN103421357B (en) * | 2013-07-10 | 2015-10-21 | 杭州弗沃德精细化工有限公司 | A kind of preparation technology with the Study On Mica of high durable performance |
| CN103602102A (en) * | 2013-11-15 | 2014-02-26 | 浙江凯色丽科技发展有限公司 | 3D (Three-Dimensional) color-changing shimmer pigment |
| CN103741118B (en) * | 2013-12-25 | 2016-06-15 | 上海纳米技术及应用国家工程研究中心有限公司 | The preparation method of colorful silver product |
| US9815970B2 (en) * | 2014-05-28 | 2017-11-14 | Basf Se | Effect pigments |
| CN107641339A (en) * | 2017-10-27 | 2018-01-30 | 河北欧克精细化工股份有限公司 | Changeable colors along with angle stereoscopic series feature pearlescent pigment and its preparation technology and purposes |
| CN110358327A (en) * | 2019-07-25 | 2019-10-22 | 汕头市镇发珠光颜料有限公司 | A kind of high-purity red pearl effect pigment and preparation method thereof |
| CN110437676B (en) * | 2019-09-16 | 2022-10-25 | 杭州科望特种油墨有限公司 | High-light-transmittance UV (ultraviolet) ink for solar panel |
| CN114350179B (en) * | 2021-12-31 | 2023-07-14 | 浙江凯色丽科技发展有限公司 | Preparation method of liquid-phase synthesized iron blue coloring pearlescent pigment |
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| DE19618569A1 (en) * | 1996-05-09 | 1997-11-13 | Merck Patent Gmbh | Highly transparent multilayer interference pigments for lacquers, inks, cosmetics, laser-markable plastics etc. |
| CN1092220C (en) * | 1997-05-23 | 2002-10-09 | 默克专利股份有限公司 | Multi-coated interference pigment |
| DE19803550A1 (en) * | 1998-01-30 | 1999-08-05 | Merck Patent Gmbh | Interference pigments with a blue body color |
| DE10051062A1 (en) * | 2000-10-14 | 2002-04-18 | Merck Patent Gmbh | Interference pigments for security uses have alternating high and low refractive index metal oxide layers wet deposited on a transparent carrier and give novel three-tone effects |
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Effective date of registration: 20140221 Address after: 215400 Taicang City, Jiangsu province Binhe Road loujiang Nga Court 40 Room 101 Patentee after: Lin Yizhong Address before: 325500, No. 9-2, West Village, Dongyang village, Xiao Cun, Taishun County, Zhejiang Patentee before: Lin Wenguang |