CN105542464A - Nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material - Google Patents

Nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material Download PDF

Info

Publication number
CN105542464A
CN105542464A CN201610009195.5A CN201610009195A CN105542464A CN 105542464 A CN105542464 A CN 105542464A CN 201610009195 A CN201610009195 A CN 201610009195A CN 105542464 A CN105542464 A CN 105542464A
Authority
CN
China
Prior art keywords
nano
nanometer
polyphenylene sulfide
heat dissipation
led
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
CN201610009195.5A
Other languages
Chinese (zh)
Inventor
肖宪书
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Bengbu Gaohua Resolution Technology Co Ltd
Original Assignee
Bengbu Gaohua Resolution Technology Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Bengbu Gaohua Resolution Technology Co Ltd filed Critical Bengbu Gaohua Resolution Technology Co Ltd
Priority to CN201610009195.5A priority Critical patent/CN105542464A/en
Publication of CN105542464A publication Critical patent/CN105542464A/en
Pending legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K13/00Use of mixtures of ingredients not covered by one single of the preceding main groups, each of these compounds being essential
    • C08K13/06Pretreated ingredients and ingredients covered by the main groups C08K3/00 - C08K7/00
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/18Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20Oxides; Hydroxides
    • C08K3/22Oxides; Hydroxides of metals
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/32Phosphorus-containing compounds
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/34Silicon-containing compounds
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/34Silicon-containing compounds
    • C08K3/346Clay
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K9/00Use of pretreated ingredients
    • C08K9/02Ingredients treated with inorganic substances
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K9/00Use of pretreated ingredients
    • C08K9/04Ingredients treated with organic substances
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K9/00Use of pretreated ingredients
    • C08K9/04Ingredients treated with organic substances
    • C08K9/06Ingredients treated with organic substances with silicon-containing compounds
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/18Oxygen-containing compounds, e.g. metal carbonyls
    • C08K3/20Oxides; Hydroxides
    • C08K3/22Oxides; Hydroxides of metals
    • C08K2003/221Oxides; Hydroxides of metals of rare earth metal
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00Use of inorganic substances as compounding ingredients
    • C08K3/32Phosphorus-containing compounds
    • C08K2003/321Phosphates
    • C08K2003/328Phosphates of heavy metals
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08KUse of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K2201/00Specific properties of additives
    • C08K2201/011Nanostructured additives
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08LCOMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L2203/00Applications
    • C08L2203/20Applications use in electrical or conductive gadgets
    • C08L2203/206Applications use in electrical or conductive gadgets use in coating or encapsulating of electronic parts

Landscapes

  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Dispersion Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Inorganic Insulating Materials (AREA)
  • Processes Of Treating Macromolecular Substances (AREA)

Abstract

The invention discloses a nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for an LED. According to the compound plastic, nanometer kaolin generated after high-temperature modification with nanometer lanthanum oxide serves as toughening and reinforcing filler, the surface of the nanometer kaolin is doped and mixed with stearic acid, the modified filler and polyphenylene sulfide have good compatibility, the agglomeration phenomenon among nanometer particles is effectively lowered, scattered associativity is better in the mixed melting process with the polyphenylene sulfide, the machining property and mechanical property of the polyphenylene sulfide are effectively improved, and adsorption and combination of modified masterbatch with nanometer lithium iron phosphate, nanometer silicon nitride and other high-thermal-conductivity filler are better, so that the composite material which is better in both mechanical property and thermal conductivity property is prepared, and the nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material has wide application space on the aspect of LED packaging.

Description

A kind of LED nano lanthanum oxide modified kaolin strengthens polyphenylene sulfide ether heat sink material and preparation method thereof
Technical field
The present invention relates to heat-conducting plastic preparing technical field, particularly relate to a kind of LED nano lanthanum oxide modified kaolin and strengthen polyphenylene sulfide ether heat sink material and preparation method thereof.
Background technology
LED is as the novel light source of a generation, there is efficient, energy-saving and environmental protection, long service life, be easy to safeguard etc. advantage, by the pre-third generation light source for incandescent light and luminescent lamp can be replaced, the working temperature of the light extraction efficiency of LED and life-span and chip has direct relation, heat dissipation problem is the subject matter that restriction packaged LED product improves power and luminous efficiency, the effective means solving LED heat dissipation problem be exactly utilize high heat conduction, high insulation, high permeability material heat is passed fast.
The heat sink material that current LED is commonly used is mainly metal aluminium or stupalith, all there are some defects in actual use in these materials, although such as aluminium base heat sink material has comparatively excellent heat-sinking capability, but its exist the moulding process cycle long, itself there is electroconductibility and the problem such as moulding is single, and although stupalith insulate, but higher than great, shaping difficulty, be unfavorable for batch production, its application is also restricted.
Polyphenylene sulfide is a kind of crystallinity, thermoplastic special engineering plastic, its over-all properties is superior, there is excellent thermotolerance, insulativity, erosion resistance, good stability of the dimension etc. advantage, its encapsulating plastics as LED lamp are particularly suitable, improving its thermal conductivity is a vital link, the method of common raising polyphenylene sulfide plastic thermal conductivity is blending high conduction powder in the plastic, but ubiquity plastic substrate intensity reduces in actual applications, mechanical property weakens, problem that heat-conducting effect is not good etc., application is restricted, along with the development on a large scale of high-power LED lamp, industry is badly in need of improving existing technique, to obtain the matrix material with the heat-conducting effect of efficient stable.
Summary of the invention
The object of the invention is exactly the defect in order to make up prior art, provides a kind of LED nano lanthanum oxide modified kaolin to strengthen polyphenylene sulfide ether heat sink material and preparation method thereof.
The present invention is achieved by the following technical solutions:
A kind of LED nano lanthanum oxide modified kaolin strengthens polyphenylene sulfide ether heat sink material, and this composite plastic is made up of the raw material of following weight part: nano lanthanum oxide 0.1-0.2, polyphenylene sulfide 50-60, nano-grade lithium iron phosphate 1-2, nano-silicon nitride 8-10, silane coupling agent 0.4-0.5, nano kaoline 3-4, calcium zinc stabilizer 1-2, stearic acid 0.5-0.6, dehydrated alcohol 8-10, deionized water are appropriate.
Described a kind of LED nano lanthanum oxide modified kaolin strengthens polyphenylene sulfide ether heat sink material and preparation method thereof, and described preparation method is:
(1) first by nano lanthanum oxide, nano kaoline, deionized water drops in high-energy mills, abundant ground and mixed 40-50min, by fully dry for mixture removing moisture after grinding terminates, subsequently gained composite granule is heated to 700-800 DEG C with the temperature rise rate of 15-20 DEG C under nitrogen atmosphere, insulation calcining 1-1.5h, room temperature is naturally cooled to after calcining terminates, obtain nano lanthanum oxide modified Nano kaolinite compound powder, last again by this powder and stearic acid, dehydrated alcohol mixes, heating in water bath is to 70-80 DEG C, after high-speed mixing stirs 1.5-2h, complete drying removes ethanol, the grinding of gained crushing material is for subsequent use,
(2) drop in high-speed mixer together with the material prepared by polyphenylene sulfide and step (1), be uniformly mixed melt blending granulation in rear input twin screw extruder, obtain modified polyphenyl thioether master batch for subsequent use;
(3) nano-grade lithium iron phosphate, nano-silicon nitride and dropping in high-speed mixer together with modified polyphenyl thioether master batch and other remaining component after silane coupling agent mixing and stirring is uniformly mixed, again drop in twin screw extruder and extrude pelletizing, obtain described matrix material.
Advantage of the present invention is: the present invention is using nano kaoline after nano lanthanum oxide is high temperature modified as toughened and reinforced filler, and at its surperficial blending stearic acid, this modified filler and polyphenylene sulfide have good consistency, agglomeration between nanoparticle is effectively reduced, with polyphenylene sulfide mixed smelting process in disperse associativity better, effectively improve processing characteristics and the mechanical property of polyphenylene sulfide, modified master batch and nano-grade lithium iron phosphate, the absorption associativity of the contour heat conductive filler of nano-silicon nitride is also better, thus prepare mechanical property and all good matrix material of heat conductivility, it has wide application space in LED.
Embodiment
The composite plastic of this embodiment is made up of the raw material of following weight part: nano lanthanum oxide 0.1, polyphenylene sulfide 50, nano-grade lithium iron phosphate 1, nano-silicon nitride 8, silane coupling agent 0.4, nano kaoline 3, calcium zinc stabilizer 1, stearic acid 0.5, dehydrated alcohol 8, deionized water are appropriate.
The preparation method of this embodiment matrix material is:
(1) first by nano lanthanum oxide, nano kaoline, deionized water drops in high-energy mills, abundant ground and mixed 40min, by fully dry for mixture removing moisture after grinding terminates, subsequently gained composite granule is heated to 700 DEG C with the temperature rise rate of 15 DEG C under nitrogen atmosphere, insulation calcining 1h, room temperature is naturally cooled to after calcining terminates, obtain nano lanthanum oxide modified Nano kaolinite compound powder, last again by this powder and stearic acid, dehydrated alcohol mixes, heating in water bath to 70 DEG C, after high-speed mixing stirs 1.5h, complete drying removes ethanol, the grinding of gained crushing material is for subsequent use,
(2) drop in high-speed mixer together with the material prepared by polyphenylene sulfide and step (1), be uniformly mixed melt blending granulation in rear input twin screw extruder, obtain modified polyphenyl thioether master batch for subsequent use;
(3) nano-grade lithium iron phosphate, nano-silicon nitride and dropping in high-speed mixer together with modified polyphenyl thioether master batch and other remaining component after silane coupling agent mixing and stirring is uniformly mixed, again drop in twin screw extruder and extrude pelletizing, obtain described matrix material.
The performance test results of the composite heat conducting material obtained by the present embodiment is:
Project Index
Tensile strength (MPa) 154
Flexural strength (MPa) 348
Thermal conductivity (w/mk) 9.6
Flame retardant rating UL94-V0
Volume specific resistance (Ω .cm) >10 13

Claims (2)

1. a LED nano lanthanum oxide modified kaolin strengthens polyphenylene sulfide ether heat sink material, it is characterized in that, this composite plastic is made up of the raw material of following weight part: nano lanthanum oxide 0.1-0.2, polyphenylene sulfide 50-60, nano-grade lithium iron phosphate 1-2, nano-silicon nitride 8-10, silane coupling agent 0.4-0.5, nano kaoline 3-4, calcium zinc stabilizer 1-2, stearic acid 0.5-0.6, dehydrated alcohol 8-10, deionized water are appropriate.
2. a kind of LED nano lanthanum oxide modified kaolin as claimed in claim 1 strengthens polyphenylene sulfide ether heat sink material and preparation method thereof, and it is characterized in that, described preparation method is:
(1) first by nano lanthanum oxide, nano kaoline, deionized water drops in high-energy mills, abundant ground and mixed 40-50min, by fully dry for mixture removing moisture after grinding terminates, subsequently gained composite granule is heated to 700-800 DEG C with the temperature rise rate of 15-20 DEG C under nitrogen atmosphere, insulation calcining 1-1.5h, room temperature is naturally cooled to after calcining terminates, obtain nano lanthanum oxide modified Nano kaolinite compound powder, last again by this powder and stearic acid, dehydrated alcohol mixes, heating in water bath is to 70-80 DEG C, after high-speed mixing stirs 1.5-2h, complete drying removes ethanol, the grinding of gained crushing material is for subsequent use,
(2) drop in high-speed mixer together with the material prepared by polyphenylene sulfide and step (1), be uniformly mixed melt blending granulation in rear input twin screw extruder, obtain modified polyphenyl thioether master batch for subsequent use;
(3) nano-grade lithium iron phosphate, nano-silicon nitride and dropping in high-speed mixer together with modified polyphenyl thioether master batch and other remaining component after silane coupling agent mixing and stirring is uniformly mixed, again drop in twin screw extruder and extrude pelletizing, obtain described matrix material.
CN201610009195.5A 2016-01-07 2016-01-07 Nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material Pending CN105542464A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN201610009195.5A CN105542464A (en) 2016-01-07 2016-01-07 Nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN201610009195.5A CN105542464A (en) 2016-01-07 2016-01-07 Nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material

Publications (1)

Publication Number Publication Date
CN105542464A true CN105542464A (en) 2016-05-04

Family

ID=55822044

Family Applications (1)

Application Number Title Priority Date Filing Date
CN201610009195.5A Pending CN105542464A (en) 2016-01-07 2016-01-07 Nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material

Country Status (1)

Country Link
CN (1) CN105542464A (en)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107177203A (en) * 2017-05-19 2017-09-19 合肥市惠科精密模具有限公司 A kind of AMOLED screens composite heat dissipation material
CN116855077A (en) * 2023-06-16 2023-10-10 东莞市曼塔新材料科技有限公司 High-wear-resistance polyphenylene sulfide modified material and preparation method thereof

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101239308A (en) * 2008-03-18 2008-08-13 江苏工业学院 Method for preparing attapulgite loading with nano cerium oxide
CN104364900A (en) * 2012-04-17 2015-02-18 莫门蒂夫性能材料股份有限公司 Thermally conductive polymer compostions to reduce molding cycle time

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101239308A (en) * 2008-03-18 2008-08-13 江苏工业学院 Method for preparing attapulgite loading with nano cerium oxide
CN104364900A (en) * 2012-04-17 2015-02-18 莫门蒂夫性能材料股份有限公司 Thermally conductive polymer compostions to reduce molding cycle time

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107177203A (en) * 2017-05-19 2017-09-19 合肥市惠科精密模具有限公司 A kind of AMOLED screens composite heat dissipation material
CN116855077A (en) * 2023-06-16 2023-10-10 东莞市曼塔新材料科技有限公司 High-wear-resistance polyphenylene sulfide modified material and preparation method thereof

Similar Documents

Publication Publication Date Title
CN113150541B (en) High-strength high-thermal-conductivity nylon composite material and preparation method thereof
CN104559149A (en) Carbon composite high-thermal-conductivity plastic material and preparation method thereof
CN105524447A (en) PC-PET-based LED heat dissipation material containing modified potassium hexatitanate whisker-carbon nanotubes, and a preparation method thereof
CN105524446A (en) PC-PET-based LED heat dissipation material containing modified nano hydroxyapatite-carbon nanotubes, and a preparation method thereof
CN105524445A (en) PC-PET-based LED heat dissipation material containing modified nano diatomite-carbon nanotubes, and preparation method thereof
CN105542464A (en) Nanometer-lanthanum-oxide-modified kaolin-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material
CN105985623A (en) PC-PET (polycarbonate and polyethylene terephthalate) based LED radiating material comprising modified tetrapod-like zinc oxide whiskers and preparation method thereof
CN105542465A (en) Nanometer-lanthanum-oxide modified bentonite-enhanced-and-toughened polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material
CN105331069A (en) PC-PET-based LED cooling material comprising modified mesoporous silica-carbon nano tubes and preparation method thereof
CN105542462A (en) Nanometer-lanthanum-oxide-modified mica-powder-enhanced polyphenylene-sulfide-based high-strength heat dissipation material for LED and preparation method of heat dissipation material
CN105385132A (en) PC-PET-based LED heat dissipating material containing modified boron nitride fiber-carbon nano tube powder and preparing method thereof
CN105985640A (en) Nano lanthanum oxide modified sepiolite fiber enhanced polyphenylene sulfide-based heat dissipating material for LED and preparation method of nano lanthanum oxide modified sepiolite fiber enhanced polyphenylene sulfide-based heat dissipating material
WO2019037564A1 (en) Non-metal composite nano heat dissipation material and preparation method therefor
CN104894435A (en) Diamond-doped aluminum-based composite heat radiation material and preparation method thereof
CN105985622A (en) PC-PET ((polycarbonate and polyethylene terephthalate) based LED radiating material comprising modified carbon black and carbon nanotubes and preparation method thereof
CN105542463A (en) Nanometer-lanthanum-oxide-modified kieselguhr-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material
CN105542461A (en) Nanometer-lanthanum-oxide-modified organic-bentonite-enhanced polyphenylene-sulfide-based heat dissipation material for LED and preparation method of heat dissipation material
CN105985638A (en) Nano lanthanum oxide modified montmorillonite enhanced polyphenylene sulfide high-heat-conduction composite material for LED and preparation method of nano lanthanum oxide modified montmorillonite enhanced polyphenylene sulfide high-heat-conduction composite material
CN105985639A (en) Nano lanthanum oxide modified hydrotalcite powder enhanced polyphenylene sulfide-based heat dissipating material for LED and preparation method of nano lanthanum oxide modified hydrotalcite powder enhanced polyphenylene sulfide-based heat dissipating material
CN105985641A (en) Nano lanthanum oxide modified talcum powder enhanced polyphenylene sulfide-based heat dissipating material for LED and preparation method of nano lanthanum oxide modified talcum powder enhanced polyphenylene sulfide-based heat dissipating material
CN105985642A (en) Nano lanthanum oxide modified carbonized polyacrylonitrile fiber enhanced polyphenylene sulfide-based heat dissipating material for LED and preparation method of nano lanthanum oxide modified carbonized polyacrylonitrile fiber enhanced polyphenylene sulfide-based heat dissipating material
CN105238044A (en) Graphene oxide-nanometer aluminium nitride filled modified PPS/PBT composite heat-conduction plastic for LED and preparation method thereof
CN104829988A (en) Teflon-based irradiation and aging-resistant heat radiation material used for LED light source and preparation method thereof
CN105985621A (en) PC-PET (polycarbonate and polyethylene terephthalate) based LED radiating material comprising modified mesophase pitch-based carbon fiber and carbon nanotubes and preparation method thereof
CN105331077A (en) PC-PET (Polycarbonate-Polyethylene Terephthalate)-based LED (Light Emitting Diode) heat dissipation material containing modified calcium sulfate whisker-carbon nano tube and preparation method of PC-PET-based LED heat dissipation material

Legal Events

Date Code Title Description
C06 Publication
PB01 Publication
C10 Entry into substantive examination
SE01 Entry into force of request for substantive examination
RJ01 Rejection of invention patent application after publication
RJ01 Rejection of invention patent application after publication

Application publication date: 20160504