CN109096567B - TPO (thermoplastic polyolefin) automotive interior material of graphene reinforced ethylene propylene diene monomer, and preparation method and application thereof - Google Patents
TPO (thermoplastic polyolefin) automotive interior material of graphene reinforced ethylene propylene diene monomer, and preparation method and application thereof Download PDFInfo
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- CN109096567B CN109096567B CN201810790632.0A CN201810790632A CN109096567B CN 109096567 B CN109096567 B CN 109096567B CN 201810790632 A CN201810790632 A CN 201810790632A CN 109096567 B CN109096567 B CN 109096567B
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- 239000000463 material Substances 0.000 title claims abstract description 70
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 59
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 59
- 229920002943 EPDM rubber Polymers 0.000 title claims abstract description 47
- 238000002360 preparation method Methods 0.000 title claims abstract description 18
- 229920002397 thermoplastic olefin Polymers 0.000 title abstract description 60
- 239000010410 layer Substances 0.000 claims abstract description 58
- 238000005187 foaming Methods 0.000 claims abstract description 28
- 238000000034 method Methods 0.000 claims abstract description 16
- -1 polypropylene Polymers 0.000 claims abstract description 13
- 239000004743 Polypropylene Substances 0.000 claims abstract description 12
- 239000011248 coating agent Substances 0.000 claims abstract description 12
- 238000000576 coating method Methods 0.000 claims abstract description 12
- 238000001125 extrusion Methods 0.000 claims abstract description 12
- 229920001155 polypropylene Polymers 0.000 claims abstract description 12
- 238000004519 manufacturing process Methods 0.000 claims abstract description 8
- 238000002156 mixing Methods 0.000 claims abstract description 7
- 239000000049 pigment Substances 0.000 claims abstract description 7
- 229920006124 polyolefin elastomer Polymers 0.000 claims abstract description 7
- 238000013329 compounding Methods 0.000 claims description 11
- 239000004594 Masterbatch (MB) Substances 0.000 claims description 10
- 229920000098 polyolefin Polymers 0.000 claims description 7
- 239000011247 coating layer Substances 0.000 claims description 6
- 238000001816 cooling Methods 0.000 claims description 6
- 238000005303 weighing Methods 0.000 claims description 6
- 239000003795 chemical substances by application Substances 0.000 claims description 5
- 238000005469 granulation Methods 0.000 claims description 5
- 230000003179 granulation Effects 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- 229920002635 polyurethane Polymers 0.000 claims description 5
- 239000004814 polyurethane Substances 0.000 claims description 5
- 238000005266 casting Methods 0.000 claims description 3
- 238000001035 drying Methods 0.000 claims description 3
- 238000004049 embossing Methods 0.000 claims description 3
- 238000005498 polishing Methods 0.000 claims description 3
- 238000004146 energy storage Methods 0.000 claims description 2
- 229910002804 graphite Inorganic materials 0.000 claims 1
- 239000010439 graphite Substances 0.000 claims 1
- 230000003014 reinforcing effect Effects 0.000 claims 1
- 230000032683 aging Effects 0.000 abstract description 8
- 239000004611 light stabiliser Substances 0.000 abstract description 8
- 239000010985 leather Substances 0.000 abstract description 3
- 230000003068 static effect Effects 0.000 abstract 1
- 239000002344 surface layer Substances 0.000 abstract 1
- 239000002904 solvent Substances 0.000 description 4
- 230000000694 effects Effects 0.000 description 3
- 206010051246 Photodermatosis Diseases 0.000 description 2
- 239000012752 auxiliary agent Substances 0.000 description 2
- 238000003912 environmental pollution Methods 0.000 description 2
- 231100000053 low toxicity Toxicity 0.000 description 2
- 230000008845 photoaging Effects 0.000 description 2
- 229920003023 plastic Polymers 0.000 description 2
- 239000004033 plastic Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 230000035882 stress Effects 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- 238000005452 bending Methods 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000005034 decoration Methods 0.000 description 1
- 229920001971 elastomer Polymers 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 230000004807 localization Effects 0.000 description 1
- 230000001050 lubricating effect Effects 0.000 description 1
- 239000005060 rubber Substances 0.000 description 1
- 238000010998 test method Methods 0.000 description 1
- 229920001169 thermoplastic Polymers 0.000 description 1
- 229920002725 thermoplastic elastomer Polymers 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L23/00—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers
- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
- C08L2205/035—Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2207/00—Properties characterising the ingredient of the composition
- C08L2207/04—Thermoplastic elastomer
Abstract
The invention provides a TPO (thermoplastic polyolefin) automotive interior material of graphene reinforced ethylene propylene diene monomer, and a preparation method and application thereof. The TPO automobile interior material sequentially comprises a TPO surface layer, a foaming layer and a back coating from bottom to top; the preparation method comprises the steps of firstly preparing ethylene propylene diene monomer master batches containing graphene in a double-screw extrusion mode, and then mixing a TPO component, a graphene reinforced ethylene propylene diene monomer component, a polyolefin elastomer component, a polypropylene component and a pigment component through a metering device to prepare the TPO skin material; the preparation method is simple and controllable, has good repeatability and low production cost; the TPO automotive interior material prepared by the method does not need to add a light stabilizer, has the characteristics of light aging resistance, heat resistance, static resistance and the like, and can improve the quality and the comprehensive performance of finished leather when being used for automotive leather; the soft TPO material prepared by the method has the advantages of comfortable use, low odor and low VOC, can be recycled, and is green and environment-friendly.
Description
Technical Field
The invention relates to the technical field of automotive interior, in particular to a graphene reinforced ethylene propylene diene monomer (TPO) automotive interior material and a preparation method and application thereof.
Background
TPO (polyolefin thermoplastic elastomer) is a high-performance polyolefin product which can be processed like thermoplastic plastics at high temperature, has rubber elasticity at normal temperature, small density, high bending elastic modulus, good low-temperature impact resistance, good fluidity, easy processing and repeated use, and has the characteristics of great feasibility in the fields of automobile interior and exterior decoration. According to the relevant data, the use of TPO can reduce the weight of the automobile by 20% to 25%, and is considered to be an ideal material for reducing the weight of the automobile.
With the promotion of automobile localization and the progress of science and technology, the society puts forward higher and higher requirements on clean production and saving production, and the improvement of the quality of automobile interior leather and the environmental protection are more and more concerned by the public. The traditional method for adding the light stabilizer does not meet the requirements of ecological environment-friendly automotive interior materials. According to the invention, the light aging resistance of the TPO automobile interior material can be effectively improved by utilizing the lubricating property of graphene, enhancing the ethylene propylene diene monomer by the graphene and adding no light stabilizer.
Disclosure of Invention
The invention aims to provide a TPO (thermoplastic polyolefin) automotive interior material of graphene reinforced ethylene propylene diene monomer, which consists of a back coating, a foaming layer and a TPO skin material layer; simultaneously, the preparation method of the TPO automotive interior material is also provided; the method is characterized in that firstly, the ethylene propylene diene monomer is enhanced by utilizing the characteristics of stable structure and good lubricity of graphene, and the light aging resistance of the TPO automobile interior material can be effectively improved without adding a light stabilizer; secondly, the method is simple and controllable, has good repeatability, can obtain the automotive interior material with excellent performance, has the advantages of comfortable use, low odor and low VOC, can be recycled, and is green and environment-friendly.
In order to achieve the purpose, the technical scheme of the invention is as follows:
the invention provides a graphene reinforced ethylene propylene diene monomer (TPO) automotive interior material which sequentially comprises a back coating layer, a foaming layer and a TPO skin material layer from bottom to top, wherein the TPO skin material layer comprises the following components in parts by weight: TPO: 20-60 parts; the graphene reinforced ethylene propylene diene monomer master batch: 10-40 parts; polyolefin elastomer: 5-20 parts of a solvent; modified polypropylene: 5-15 parts of a solvent; pigment: 4-8 parts. The light stabilizer is not needed, the graphene reinforced ethylene propylene diene monomer is used instead, and the characteristics of stable structure and good lubricity of the graphene are utilized, so that the light aging resistance of the TPO automotive interior material can be effectively improved, the addition of the auxiliary agent is reduced, the environmental pollution and the production cost are reduced, and the pollution problem of the light stabilizer is reduced.
Preferably, the back coating layer is a polyurethane or polyolefin finishing agent layer. The water-based, benzene-free, low-toxicity and environment-friendly polyurethane or polyolefin finishing agent layer is adopted, and a good bonding effect can be achieved only by a small amount.
Preferably, the foamed layer is a polypropylene foamed layer. Because the TPO skin material layer and the polypropylene foaming layer have better compatibility.
Preferably, the graphene reinforced ethylene propylene diene monomer master batch comprises the following components in parts by weight: 100 parts of ethylene propylene diene monomer and 0.5-1 part of graphene.
Preferably, the graphene is at least one of conductive graphene, heat-conductive graphene, energy-storage graphene, enhanced graphene and graphene oxide.
The invention also aims to disclose a preparation method of the TPO automobile interior material of the graphene reinforced ethylene propylene diene monomer, which comprises the following steps:
(1) preparing the graphene reinforced ethylene propylene diene monomer master batch: weighing ethylene propylene diene monomer and graphene, adding the weighed ethylene propylene diene monomer and graphene into a double-screw extruder, uniformly mixing, and performing melt extrusion granulation to obtain graphene reinforced ethylene propylene diene monomer master batches;
(2) preparation of TPO skin material layer: accurately weighing TPO, graphene reinforced ethylene propylene diene monomer master batches, polyolefin elastomers, modified polypropylene and pigments according to the formula amount by a metering device, adding the materials into a double-screw extruder, uniformly mixing, carrying out melt extrusion, carrying out press polishing, and cooling to prepare a TPO skin material layer;
(3) preparation of TPO automotive interior material: compounding a back coating layer, a foaming layer and a TPO skin material layer together according to a compounding mode from bottom to top to prepare the TPO automobile interior material; firstly, compounding, embossing and cooling the TPO skin material layer prepared in the step (2) and a foaming layer; and then coating a back coating on the back surface of the foaming layer and drying to obtain the TPO automotive interior material.
The graphene and the ethylene propylene diene monomer are directly subjected to melt extrusion granulation through a double-screw extruder, and other solvents or auxiliaries are not required to be added, so that the process and raw material cost are reduced.
Preferably, the method for compounding the TPO skin material layer and the foamed layer in the step (3) is at least one of an extrusion casting method and supercritical foaming. The plastic product prepared by the supercritical foaming method has high specific strength and high cost performance, the size precision of the product is greatly improved, the residual stress and the warping deformation of the product are greatly reduced, and the product quality is reduced.
The invention also aims to provide application of the graphene reinforced ethylene propylene diene monomer TPO automotive interior material in the manufacturing fields of the aviation industry, the traffic field, the massage equipment, the home furnishing and the like.
The invention has the beneficial effects that:
(1) the characteristics of stable structure and good lubricity of graphene are utilized to reinforce the ethylene propylene diene monomer, and the light aging resistance of the TPO automobile interior material can be effectively improved without adding a light stabilizer, meanwhile, the addition of an auxiliary agent is reduced, the environmental pollution and the production cost are reduced, and the pollution problem of the light stabilizer is reduced;
(2) the method is simple and controllable, has good repeatability, can obtain the automotive interior material with excellent performance, has the advantages of comfortable use, low odor and low VOC, can be recycled, and is green and environment-friendly;
(3) the addition amount of the graphene is 0.5-1 part, the addition amount is small, negative effects on other performances are avoided, and the automobile interior material can be endowed with better light aging resistance.
Drawings
FIG. 1 is a schematic structural view of a TPO automotive interior material of the present invention.
Wherein, 1-TPO skin material layer, 2-foaming layer and 3-back coating.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without any inventive step, are within the scope of the present invention.
In the description of the present invention, it is to be understood that the terms "upper", "lower", "front", "rear", "left", "right", "top", "bottom", "inner", "outer", and the like, indicate orientations or positional relationships based on the orientations or positional relationships shown in the drawings, are merely for convenience in describing the present invention and simplifying the description, and do not indicate or imply that the device or element being referred to must have a particular orientation, be constructed and operated in a particular orientation, and thus, should not be construed as limiting the present invention.
In the present invention, unless otherwise expressly specified or limited, the terms "mounted," "connected," "fixed," and the like are to be construed broadly and can include, for example, fixed connections, detachable connections, or integral connections; they may be connected directly or indirectly through intervening media, or they may be interconnected between two elements. The specific meanings of the above terms in the present invention can be understood by those skilled in the art according to specific situations.
Unless defined otherwise, technical or scientific terms used herein shall have the ordinary meaning as understood by one of ordinary skill in the art to which this invention belongs. The use of the words "a" or "an" and the like in the description and claims of the present patent application do not denote a limitation of quantity, but rather denote the presence of at least one.
As shown in fig. 1, the graphene reinforced ethylene propylene diene monomer TPO automotive interior material of the present invention sequentially comprises a back coating layer 3, a foaming layer 2 and a TPO skin material layer 1 from bottom to top; the back coating 3 is a polyurethane or polyolefin finishing agent layer. The water-based, benzene-free, low-toxicity and environment-friendly polyurethane or polyolefin finishing agent layer is adopted, and a good bonding effect can be achieved only by a small amount; the foaming layer 2 is a polypropylene foaming layer. Because the TPO skin material layer and the polypropylene foaming layer have better compatibility.
The invention also aims to disclose a preparation method of the TPO automobile interior material of the graphene reinforced ethylene propylene diene monomer, which comprises the following steps:
(1) preparing the graphene reinforced ethylene propylene diene monomer master batch: weighing ethylene propylene diene monomer and graphene, adding the weighed ethylene propylene diene monomer and graphene into a double-screw extruder, uniformly mixing, and performing melt extrusion granulation to obtain graphene reinforced ethylene propylene diene monomer master batches;
(2) preparation of TPO skin material layer: accurately weighing TPO, graphene reinforced ethylene propylene diene monomer master batches, polyolefin elastomers, modified polypropylene and pigments according to the formula amount by a metering device, adding the materials into a double-screw extruder, uniformly mixing, carrying out melt extrusion, carrying out press polishing, and cooling to prepare a TPO skin material layer;
(3) preparation of TPO automotive interior material: compounding a back coating layer, a foaming layer and a TPO skin material layer together according to a compounding mode from bottom to top to prepare the TPO automobile interior material; firstly, compounding, embossing and cooling the TPO skin material layer prepared in the step (2) and a foaming layer; and then coating a back coating on the back surface of the foaming layer and drying to obtain the TPO automotive interior material.
The graphene and the ethylene propylene diene monomer are directly subjected to melt extrusion granulation through a double-screw extruder, and other solvents or auxiliaries are not required to be added, so that the process and raw material cost are reduced.
The method for compounding the TPO skin material layer and the foaming layer in the step (3) is at least one of an extrusion casting method and supercritical foaming. The plastic product prepared by the supercritical foaming method has high specific strength and high cost performance, the size precision of the product is greatly improved, the residual stress and the warping deformation of the product are greatly reduced, and the product quality is reduced.
The invention also aims to provide application of the graphene reinforced ethylene propylene diene monomer TPO automotive interior material in the manufacturing fields of the aviation industry, the traffic field, the massage equipment, the home furnishing and the like.
Table 1 shows the composition of the TPO skin material layer according to the examples of the present invention. Table 2 shows the components of the graphene-reinforced epdm rubber masterbatch according to the embodiment of the present invention. Table 3 shows the light aging resistance test results of the TPO automotive interior material prepared by the preparation method of the embodiment of the invention, and the light aging resistance parameters are tested by adopting the PV1303 test method.
TABLE 1 composition of the TPO skin material layer (unit: parts) described in the examples
| TPO | Graphene reinforced ethylene propylene diene monomer master batch | Polyolefin elastomer | Modified polypropylene | Pigment (I) | |
| Example 1 | 0 | 10 | 5 | 5 | 4 |
| Example 2 | 0 | 40 | 20 | 15 | 8 |
| Example 3 | 5 | 10 | 12 | 8 | 4 |
| Example 4 | 5 | 28 | 12 | 8 | 4 |
| Example 5 | 5 | 40 | 12 | 8 | 4 |
TABLE 2 composition of graphene-reinforced EPDM rubber Master batch of examples (unit: part)
| Ethylene propylene diene monomer | Graphene | |
| Example 1 | 100 | 0.5 |
| Example 2 | 100 | 1 |
| Example 3 | 100 | 1 |
| Example 4 | 100 | 1 |
| Example 5 | 100 | 1 |
TABLE 3 photo aging resistance of TPO automotive interior material prepared by the preparation method of example
| Detecting items | Example 1 | Example 2 | Example 3 | Example 4 | Example 5 |
| Resistance to photoaging (kJ/m)2) | 550 | 1050 | 600 | 1240 | 1000 |
Finally, it should be noted that the above embodiments are only used for illustrating the technical solutions of the present invention and are not limited. Although the present invention has been described in detail with reference to the above embodiments, it will be understood by those skilled in the art that various changes may be made and equivalents may be substituted without departing from the scope of the present invention.
Claims (2)
1. The utility model provides a TPO automotive interior material of graphite alkene reinforcing ethylene propylene diene monomer, its characterized in that: the TPO skin material layer comprises a back coating (1), a foaming layer (2) and a TPO skin material layer (3) from bottom to top in sequence, wherein the TPO skin material layer (3) consists of the following components in parts by weight: TPO: 45 parts of (1); the graphene reinforced ethylene propylene diene monomer master batch: 28 parts of (1); polyolefin elastomer: 12 parts of (1); modified polypropylene: 8 parts of a mixture; pigment: 4 parts of a mixture;
the back coating (1) is a polyurethane or polyolefin finishing agent layer;
the foaming layer (2) is a polypropylene foaming layer;
the graphene reinforced ethylene propylene diene monomer master batch comprises the following components in parts by weight: 100 parts of ethylene propylene diene monomer and 1 part of graphene;
the graphene is at least one of conductive graphene, heat-conducting graphene, energy-storage graphene, enhanced graphene and graphene oxide;
the TPO automotive interior material of the graphene reinforced ethylene propylene diene monomer is applied to the fields of aviation industry, traffic, massage equipment and home manufacturing.
2. The preparation method of the TPO automobile interior material of graphene reinforced ethylene propylene diene monomer according to claim 1, is characterized in that: the method comprises the following steps:
(1) preparing the graphene reinforced ethylene propylene diene monomer master batch: weighing ethylene propylene diene monomer and graphene, adding the weighed ethylene propylene diene monomer and graphene into a double-screw extruder, uniformly mixing, and performing melt extrusion granulation to obtain graphene reinforced ethylene propylene diene monomer master batches;
(2) preparation of TPO skin material layer: accurately weighing TPO, graphene reinforced ethylene propylene diene monomer master batches, polyolefin elastomers, modified polypropylene and pigments according to the formula amount by a metering device, adding the materials into a double-screw extruder, uniformly mixing, carrying out melt extrusion, carrying out press polishing, and cooling to prepare a TPO skin material layer;
(3) preparation of TPO automotive interior material: compounding a back coating layer, a foaming layer and a TPO skin material layer together according to a compounding mode from bottom to top to prepare the TPO automobile interior material; firstly, compounding, embossing and cooling the TPO skin material layer prepared in the step (2) and a foaming layer; then coating a back coating on the back surface of the foaming layer and drying to obtain the TPO automotive interior material;
the TPO skin material layer and the foaming layer are compounded by at least one of an extrusion casting method and supercritical foaming.
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| CN201810790632.0A CN109096567B (en) | 2018-07-18 | 2018-07-18 | TPO (thermoplastic polyolefin) automotive interior material of graphene reinforced ethylene propylene diene monomer, and preparation method and application thereof |
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| CN110643117A (en) * | 2019-10-14 | 2020-01-03 | 中国科学院长春应用化学研究所 | Low-processing-viscosity matte TPO skin material, and preparation method and application thereof |
| CN113121858B (en) * | 2019-12-31 | 2023-01-31 | 苏州瑞高新材料有限公司 | Novel transparent superconducting automotive interior material and preparation method thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH10217821A (en) * | 1997-02-06 | 1998-08-18 | Yamato Kagaku Kogyo Kk | Backing member composition for automobile floor mat |
| CN103965800A (en) * | 2014-05-09 | 2014-08-06 | 天津市大林新材料科技有限公司 | Environment-friendly thermoplastic polyolefin (TPO) auto interior material and preparation method thereof |
| CN104589748A (en) * | 2015-02-04 | 2015-05-06 | 上海铱塑科技有限公司 | Enhanced TPO (thermoplastic polyolefin) automobile instrument skin material and manufacturing method thereof |
| CN106117935A (en) * | 2016-07-01 | 2016-11-16 | 宁波硫华聚合物有限公司 | Pre-dispersed masterbatch particles of Graphene and its preparation method and application |
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Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH10217821A (en) * | 1997-02-06 | 1998-08-18 | Yamato Kagaku Kogyo Kk | Backing member composition for automobile floor mat |
| CN103965800A (en) * | 2014-05-09 | 2014-08-06 | 天津市大林新材料科技有限公司 | Environment-friendly thermoplastic polyolefin (TPO) auto interior material and preparation method thereof |
| CN104589748A (en) * | 2015-02-04 | 2015-05-06 | 上海铱塑科技有限公司 | Enhanced TPO (thermoplastic polyolefin) automobile instrument skin material and manufacturing method thereof |
| CN106117935A (en) * | 2016-07-01 | 2016-11-16 | 宁波硫华聚合物有限公司 | Pre-dispersed masterbatch particles of Graphene and its preparation method and application |
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Address after: 215400 No.5 Youyi Road, Huangjing Industrial Park, Taicang City, Suzhou City, Jiangsu Province Patentee after: Suzhou Rui High Tech Materials Co.,Ltd. Guo jiahuodiqu after: Zhong Guo Address before: 215400 No.5 Youyi Road, Huangjing Industrial Park, Taicang City, Suzhou City, Jiangsu Province Patentee before: SUZHOU GREENTECH Co.,Ltd. Guo jiahuodiqu before: Zhong Guo |