CN112125298A - Substrate rapid screening method for graphene with vertical structure - Google Patents
Substrate rapid screening method for graphene with vertical structure Download PDFInfo
- Publication number
- CN112125298A CN112125298A CN202010843466.3A CN202010843466A CN112125298A CN 112125298 A CN112125298 A CN 112125298A CN 202010843466 A CN202010843466 A CN 202010843466A CN 112125298 A CN112125298 A CN 112125298A
- Authority
- CN
- China
- Prior art keywords
- substrate
- vertical structure
- graphene
- plasma
- rapidly screening
- 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
Links
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/184—Preparation
- C01B32/186—Preparation by chemical vapour deposition [CVD]
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/194—After-treatment
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Nanotechnology (AREA)
- Inorganic Chemistry (AREA)
- Carbon And Carbon Compounds (AREA)
Abstract
The invention discloses a method for quickly screening a substrate of graphene with a vertical structure, which comprises the following steps: 1) dividing regions on the surface of the substrate and respectively adopting different materials for deposition pretreatment on different regions; 2) placing the pretreated substrate on a sample table in a reaction chamber of the jet plasma; 3) pumping the reaction chamber to vacuum, introducing Ar gas, adjusting the pressure of the reaction chamber to 200-1500 Pa, exciting plasma, and introducing H2And a carbon-containing reaction gas; the method can grow the vertical structure graphene under the same plasma environment on the substrate area pretreated by various materials at one time, and can also grow the vertical structure graphene under different plasma conditions in a micro-area multi-point mode.
Description
Technical Field
The invention relates to the technical field of preparation of vertical structure graphene, in particular to a method for rapidly screening a substrate of vertical structure graphene.
Background
Vertical-structure graphene (vertical-oriented graphene) is a member of a family of carbon materials, also called carbon nanosheets (carbon nanofilakes), and is a 3D material with rich edges formed by vertically growing graphene nanosheets consisting of several layers of graphene on a substrate, wherein the width and height of a single nanosheet can reach 0.1 to tens of micrometers, but the thickness of the single nanosheet is generally only a few nanometers or less than 1 nm. As a layered material with atomic thickness, the graphene with a vertical structure has the advantages of large specific surface area, rich sharp edges, high electron mobility, high sensitivity to electron disturbance and the like, and is widely applied to the fields of electrocatalysis, energy storage, sensors and the like.
At present, a plasma-enhanced chemical vapor deposition (plasma-enhanced chemical vapor deposition) technology is mainly adopted in a synthesis method of graphene with a vertical structure, a substance (generally, carbon-containing gas) providing a carbon source is decomposed in a plasma environment, and the graphene with the vertical structure is gradually grown on the surface of a substrate under the combined action of stress and an electric field, and the whole growth process generally comprises three stages of nucleation, growth and termination. PECVD has many advantages in the growth of nanostructures: relatively low substrate temperature, high free growth selectivity and good nanostructure mode control. These advantages make PECVD the most suitable method for growing vertical graphene, which can be classified into: planar inductively coupled plasma chemical vapor deposition (ICP-PECVD), radio frequency plasma enhanced chemical vapor deposition (RF-PECVD), microwave plasma enhanced chemical vapor deposition (MW-PECVD), electron beam excited plasma enhanced chemical vapor deposition (EBE-PECVD), capacitively coupled plasma enhanced chemical vapor deposition (CCPE-PECVD), and helicon wave plasma chemical vapor deposition. Hot filament chemical vapor deposition (HF-CVD) and some self-built devices such as the one disclosed in patent No. CN202465870U have also been used.
Although the growth of the vertical structure graphene is not as harsh as the growth of the common two-dimensional graphene and requires a catalytic substance, due to the lattice mismatch degree between the substrate material and the vertical graphene, the type of the substrate material can greatly affect the actual growth process of the vertical structure graphene, further affect the prepared morphological structure, and relate to the initial nucleation and growth process. In the traditional preparation process of the graphene with the vertical structure, only one process condition of one substrate can be explored through one experiment, and the process exploration time under various substrate conditions is high in cost and low in efficiency, so that a method capable of rapidly and efficiently screening the substrate needs to be developed.
Disclosure of Invention
The technical problem to be solved by the invention is to overcome the defects of the prior art: a method for rapidly screening a substrate of graphene with a vertical structure is provided.
The technical solution of the invention is as follows: a method for rapidly screening a substrate of graphene with a vertical structure comprises the following steps:
1) dividing regions on the surface of the substrate and respectively adopting different materials for deposition pretreatment on different regions;
2) placing the pretreated substrate on a sample table in a reaction chamber of the jet plasma;
3) pumping the reaction chamber to vacuum, introducing Ar gas, adjusting the pressure of the reaction chamber to 200-1500 Pa, exciting a plasma torch, and then introducing H2And a carbon-containing reaction gas;
4) and depositing the vertical structure graphene in the substrate area subjected to deposition pretreatment by adopting different materials through a plasma torch of the jet plasma, so that the substrate material meeting the requirement can be rapidly screened according to the growth characteristics of the vertical structure graphene in different areas.
The jet plasma is an inductively coupled jet plasma generated by a spiral coil method or a jet plasma generated by a direct current arc.
In the step 1), the method for deposition pretreatment on the surface of the substrate is one of vacuum film deposition equipment such as thermal evaporation, E-beam or magnetron sputtering and the like.
In the step 1), the material for deposition pretreatment on the surface of the substrate is metal or metal oxide.
Polishing and cleaning the substrate in the step 1) before the substrate is placed on a sample table.
The substrate cleaning mode is to perform ultrasonic cleaning in acetone, ethanol and deionized water for 5-15 minutes respectively.
The distance between the sample table and the injection outlet of the plasma torch in the step 3) is 20-60 mm.
The flow rates of the gas introduced in the step 2) are respectively Ar: 10-25 slm, H2: 0-0.9 slm, carbon-containing reactant gas: 10-200 sccm.
The carbon-containing reaction gas is CH4 、C2H2、C2H4Ethanol, CO2One or more of them.
The vertical structure graphene deposited in different areas in the step 4) can be deposited under the same growth condition plasma, or can be deposited under different growth conditions plasma in a micro-area multi-point mode.
The invention has the beneficial effects that: the invention firstly carries out deposition pretreatment of a plurality of materials in different areas of a substrate, and then adopts plasma jet deposition to realize deposition of the same or different growth conditions in different areas. The pretreatment of the substrate can be realized by adopting vacuum film deposition methods such as electron beam evaporation, magnetron sputtering, thermal evaporation and the like.
The method can grow the vertical structure graphene under the same plasma environment on the substrate area pretreated by various materials at one time, and can also grow the vertical structure graphene under different plasma conditions in a micro-area multi-point mode.
The research on a plurality of process combination conditions can be realized through one experiment, the rapid screening of the substrate with the crystal growth catalysis effect is realized, the experiment efficiency is greatly accelerated, and the development and research of new materials and processes are accelerated.
The utilization rate of the substrate material is improved, and the material cost and the time cost are saved.
Drawings
FIG. 1 is a schematic view of a substrate surface process assembly of example 1.
FIG. 2 is a schematic view of a substrate surface processing assembly of example 2.
FIG. 3 is a scanning electron micrograph of the growth region 1 of example 2.
FIG. 4 is a Raman spectrum of the sample of example 2.
FIG. 5 is a scanning electron micrograph of a sample of example 2.
FIG. 6 is a scanning electron micrograph of a sample of example 2.
FIG. 7 is a scanning electron micrograph of growth region 2 of example 2.
FIG. 8 is a scanning electron micrograph of growth region 2 of example 2.
Fig. 9 is a raman spectrum of the growth region 2 of example 2.
FIG. 10 is a scanning electron micrograph of growth region 2 of example 2.
Detailed Description
The present invention will be described in further detail with reference to the following examples, but the present invention is not limited to the following examples.
Example 1
The jet plasma device may be specifically an inductively coupled plasma torch and a plasma device disclosed in patent CN104867801A or a device disclosed in the literature [ Carbon Volume 147, June 2019, Pages 341 and 347 ].
High density jet plasma production using inductively coupled generation, the plasma jet outlet was about 30mm from the sample stage. Cleaning a silicon wafer substrate in acetone, ethanol and deionized water for 10-20min in sequence, then carrying out evaporation pretreatment on different metals on the surface of the silicon wafer substrate through a mask plate by using an electron Beam E-Beam device, as shown in figure 1, dividing the substrate into 4 areas, wherein the number 1 is an electron Beam nickel (Ni) plating area, the number 2 is an aluminum (Al) plating area, the number 3 is a palladium (Pd) plating area, and the number 4 is an Au plating area, then placing the pretreated substrate on a sample table in a reaction chamber, introducing a plasma gas source into the reaction chamber, and exciting the reaction chamber to generate plasma. The gas flow rates are respectively argon gas 21slm, H2 0.9slm，CH4And (3) 50sccm, adjusting the pressure of the reaction chamber to 800 (+ -5) Pa, adding 18kw of radio frequency power supply, and performing vertical structure graphene deposition under the same growth condition on the substrate.
Example 2
The high density jet plasma preparation was produced using a dc arc with the plasma jet outlet approximately 40mm from the sample stage. The present embodiment is substantially the same as embodiment 1, except that the substrate material is divided into 25 regions, as shown in fig. 2, different regions are subjected to evaporation pretreatment of different materials by thermal evaporation, and a single deposition test can explore the effect of different surface processing treatments on nucleation and growth of graphene with a vertical structure. And (3) depositing different growth conditions on different areas in a micro-area multi-point mode: the gas flow rates used in the 1-5 regions are respectively argon 21slm, H2 0.9slm，CH4The gas flow for the 50sccm, 6-10 region was 20slm, H for argon respectively2 0.6slm，CH4The gas flow rates for the 60sccm, 11-15 regions were 21slm, H for argon, respectively2 0.3slm，CH4The gas flow for the 50sccm, 16-20 region was 20slm, H for argon respectively2 0.3slm，CH4The gas flow rate for the 90sccm, 21-25 region is argon 21slm, H2 0.9slm，CH4 30sccm。
For example 1, taking the regions numbered 1 and 2 as examples, the growth parameters are set consistently: argon gas 21slm, hydrogen gas 0.9slm, methane gas 50sccm, the distance between the sample stage and the plasma cavity opening is about 30mm, and the power of the radio frequency power supply is 18 kw.
For the growth region 1 (the surface of the substrate is not subjected to evaporation pretreatment), when the deposition time is 5s, the mixed buffer layer of amorphous graphite and α -C is already formed, and at this time, some nucleation sites and nano islands exist on the buffer layer, and a scanning electron microscope picture is shown in fig. 3.
When the deposition time is 7s, a complete graphene layer with a vertical structure is formed on the surface of the substrate through the Raman spectrum and the scanning electron microscope image analysis of the sample, as shown in FIGS. 4 and 5.
With the further increase of the deposition time, the density of the vertical graphene nanoplatelets growing on the substrate becomes higher, and the surface micro-topography is similar, as shown in fig. 6.
For growth region 2 (substrate surface plated with nickel about 100 nm), a mixed buffer layer of amorphous graphite and α -C has been formed at a deposition time of 3s, and a large number of nucleation sites and grown nano-islands have been observed on the buffer layer at this time, and scanning electron micrographs are shown in fig. 7 and 8.
When the deposition time is 5s, a complete graphene layer with a vertical structure is formed on the surface of the substrate through the Raman spectrum and the scanning electron microscope image analysis of the sample, as shown in FIGS. 9 and 10.
Comparing the area with the number 1 (the surface of the substrate is not subjected to metal evaporation pretreatment) and the area with the number 2 (the surface of the substrate is subjected to electron beam nickel plating about 100 nm), the nucleation time of the vertical structure graphene is shortened from about 5s to about 3s after the nickel plating pretreatment is carried out on the surface of the substrate, the nucleation of the vertical structure graphene on the surface of the substrate is obviously accelerated, and the preparation efficiency of the vertical structure graphene is improved.
For example 2
The set growth conditions are different for 25 micro-areas pretreated by different materials, and the vertical structure graphene deposition under different conditions can be carried out in different areas of the substrate through multi-point deposition, namely, the exploration of the influence of various materials on the growth of the vertical structure graphene is completed through a single deposition experiment, so that the rapid screening of the substrate is realized.
The above are merely characteristic embodiments of the present invention, and do not limit the scope of the present invention in any way. All technical solutions formed by equivalent exchanges or equivalent substitutions fall within the protection scope of the present invention.
Claims (10)
1. A method for rapidly screening a substrate of graphene with a vertical structure is characterized by comprising the following steps:
1) dividing regions on the surface of the substrate and respectively adopting different materials for deposition pretreatment on different regions;
2) placing the pretreated substrate on a sample table in a reaction chamber of the jet plasma;
3) pumping the reaction chamber to vacuum, introducing Ar gas, adjusting the pressure of the reaction chamber to 200-1500 Pa, exciting plasma, and introducing H2And a carbon-containing reaction gas;
4) the vertical-structure graphene is deposited in the substrate area after deposition pretreatment of different materials through the jet plasma, and the substrate material meeting the requirements can be rapidly screened according to the growth characteristics of the vertical-structure graphene in different areas.
2. The method for rapidly screening the substrate with the vertical structure graphene according to claim 1, wherein the jet plasma is an inductively coupled jet plasma generated by a spiral coil method or a jet plasma generated by a direct current arc.
3. The method for rapidly screening the substrate with the vertical structure graphene according to claim 1, wherein in the step 1), the method for deposition pretreatment on the surface of the substrate is one of thermal evaporation, E-beam or magnetron sputtering vacuum thin film deposition.
4. The method for rapidly screening the substrate with the vertical structure graphene according to claim 1, wherein in the step 1), the material deposited and pretreated on the surface of the substrate is an elemental metal or an alloy.
5. The method for rapidly screening the substrate of the vertical structure graphene according to claim 1, wherein the substrate in the step 1) is cleaned before being placed on a sample stage.
6. The method for rapidly screening the substrate of the graphene with the vertical structure according to claim 5, wherein the substrate is cleaned by ultrasonic cleaning in acetone, ethanol and deionized water for 5-15 minutes.
7. The method for rapidly screening the substrate of the vertical structure graphene according to claim 1, wherein the distance between the sample stage and the plasma torch jet outlet in the step 3) is 20-60 mm.
8. The method for rapidly screening the substrate of the graphene with the vertical structure according to claim 1, wherein the flow rates of the gas introduced in the step 3) are Ar: 10-25 slm, H2: 0-0.9 slm, carbon-containing reactant gas: 10-200 sccm.
9. The method for rapidly screening the substrate of the graphene with the vertical structure according to claim 1 or 8, wherein the carbon-containing reaction gas is CH4 、C2H2、C2H4Ethanol, CO2One or more of them.
10. The method for rapidly screening the substrate of the vertical structure graphene according to claim 1, wherein the vertical structure graphene deposited in different areas in the step 4) can be deposited under the same growth condition plasma, or can be deposited under different growth conditions plasma by a micro-area multi-point mode.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010843466.3A CN112125298A (en) | 2020-08-20 | 2020-08-20 | Substrate rapid screening method for graphene with vertical structure |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN202010843466.3A CN112125298A (en) | 2020-08-20 | 2020-08-20 | Substrate rapid screening method for graphene with vertical structure |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN112125298A true CN112125298A (en) | 2020-12-25 |
Family
ID=73850368
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN202010843466.3A Pending CN112125298A (en) | 2020-08-20 | 2020-08-20 | Substrate rapid screening method for graphene with vertical structure |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN112125298A (en) |
Citations (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CA2331278A1 (en) * | 2000-02-25 | 2001-08-25 | Wei Zhu | Process for controlled growth of carbon nanotubes |
| JP2001288625A (en) * | 2000-02-04 | 2001-10-19 | Ulvac Japan Ltd | Graphite nanofiber, electron emitting source and method for producing the same, display element having the electron emitting source, and lithium ion secondary battery |
| CN1512545A (en) * | 2002-12-26 | 2004-07-14 | ��ʽ���綫֥ | Templet mask for charging-proof and its producing method |
| CN1992190A (en) * | 2005-12-29 | 2007-07-04 | 三星电子株式会社 | Semiconductor process evaluation methods including variable ion implanting conditions |
| CN102021526A (en) * | 2009-09-23 | 2011-04-20 | 中芯国际集成电路制造(上海)有限公司 | Target and method for setting element ratio of target |
| CN103553029A (en) * | 2013-10-31 | 2014-02-05 | 中国科学院上海微系统与信息技术研究所 | Method for preparing vertical graphene-based thermal material |
| CN104805419A (en) * | 2014-01-23 | 2015-07-29 | 中国科学院上海微系统与信息技术研究所 | Preferable selection method of CVD graphene film region |
| CN205335089U (en) * | 2015-12-30 | 2016-06-22 | 广州墨储新材料科技有限公司 | Plasma chemical vapor deposition's graphite alkene nanometer wall based on electromagnetic field is reinforceed |
| KR20160084351A (en) * | 2016-07-04 | 2016-07-13 | 이윤택 | Manufacturing method of substrate graphene growth and substrate graphene growth |
| CN106024828A (en) * | 2015-03-30 | 2016-10-12 | 三星显示有限公司 | Display apparatus and apparatus and method of manufacturing display apparatus |
| CN106957051A (en) * | 2017-01-20 | 2017-07-18 | 中国科学院物理研究所 | A kind of overlength SWCN horizontal array, preparation method and reaction unit |
| CN110838346A (en) * | 2019-10-10 | 2020-02-25 | 中国建筑材料科学研究总院有限公司 | Screening method and device for substrate material in low-emissivity glass |
-
2020
- 2020-08-20 CN CN202010843466.3A patent/CN112125298A/en active Pending
Patent Citations (12)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001288625A (en) * | 2000-02-04 | 2001-10-19 | Ulvac Japan Ltd | Graphite nanofiber, electron emitting source and method for producing the same, display element having the electron emitting source, and lithium ion secondary battery |
| CA2331278A1 (en) * | 2000-02-25 | 2001-08-25 | Wei Zhu | Process for controlled growth of carbon nanotubes |
| CN1512545A (en) * | 2002-12-26 | 2004-07-14 | ��ʽ���綫֥ | Templet mask for charging-proof and its producing method |
| CN1992190A (en) * | 2005-12-29 | 2007-07-04 | 三星电子株式会社 | Semiconductor process evaluation methods including variable ion implanting conditions |
| CN102021526A (en) * | 2009-09-23 | 2011-04-20 | 中芯国际集成电路制造(上海)有限公司 | Target and method for setting element ratio of target |
| CN103553029A (en) * | 2013-10-31 | 2014-02-05 | 中国科学院上海微系统与信息技术研究所 | Method for preparing vertical graphene-based thermal material |
| CN104805419A (en) * | 2014-01-23 | 2015-07-29 | 中国科学院上海微系统与信息技术研究所 | Preferable selection method of CVD graphene film region |
| CN106024828A (en) * | 2015-03-30 | 2016-10-12 | 三星显示有限公司 | Display apparatus and apparatus and method of manufacturing display apparatus |
| CN205335089U (en) * | 2015-12-30 | 2016-06-22 | 广州墨储新材料科技有限公司 | Plasma chemical vapor deposition's graphite alkene nanometer wall based on electromagnetic field is reinforceed |
| KR20160084351A (en) * | 2016-07-04 | 2016-07-13 | 이윤택 | Manufacturing method of substrate graphene growth and substrate graphene growth |
| CN106957051A (en) * | 2017-01-20 | 2017-07-18 | 中国科学院物理研究所 | A kind of overlength SWCN horizontal array, preparation method and reaction unit |
| CN110838346A (en) * | 2019-10-10 | 2020-02-25 | 中国建筑材料科学研究总院有限公司 | Screening method and device for substrate material in low-emissivity glass |
Non-Patent Citations (4)
| Title |
|---|
| HUANZHANG ET AL: ""Efficient and controllable growth of vertically oriented graphene nanosheets by mesoplasma chemical vapor deposition"", 《CARBON》 * |
| 折伟林 等: ""长波碲镉汞薄膜外延用碲锌镉衬底筛选方法研究"", 《红外》 * |
| 芦子玉: ""基于中压等离子体技术的多晶硅薄膜快速晶化及低温生长"", 《中国优秀博硕士学位论文全文数据库(硕士)信息科技辑》 * |
| 陈玉华 主编: "《新型清洁能源技术》", 31 January 2019, 知识产权出版社 * |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| TWI299320B (en) | Production of carbon nanotubes | |
| US20090311445A1 (en) | Synthesis of Carbon Nanotubes by Selectively Heating Catalyst | |
| Zhang et al. | Efficient and controllable growth of vertically oriented graphene nanosheets by mesoplasma chemical vapor deposition | |
| US20210253430A1 (en) | Carbon nanostructured materials and methods for forming carbon nanostructured materials | |
| KR20030028296A (en) | Plasma enhanced chemical vapor deposition apparatus and method of producing a cabon nanotube using the same | |
| US7585484B2 (en) | Apparatus and method for synthesizing carbon nanotubes | |
| CN110323270B (en) | Preparation method of graphene conductive film and thin film transistor | |
| CN110106492A (en) | Quickly prepare the method for vertical graphene | |
| CN112125298A (en) | Substrate rapid screening method for graphene with vertical structure | |
| KR100669394B1 (en) | Carbon nano tube comprising magnet metal rod and method of preparing same | |
| CN107244666B (en) | Method for growing large-domain graphene by taking hexagonal boron nitride as point seed crystal | |
| CN113072063B (en) | Hydrogen-resistant coating based on inner surface of hydrogen storage and transportation equipment and preparation method thereof | |
| Jeong et al. | Effective parameters on diameter of carbon nanotubes by plasma enhanced chemical vapor deposition | |
| CN111620340B (en) | Method for in-situ growth of TiC nanotube | |
| CN102534544A (en) | Carbon nanotube composite material and its preparation method | |
| Lee et al. | Effects of post treatment on the field emission properties of CNTs grown by ECR-CVD | |
| CN111910171A (en) | Device and method for synthesizing two-dimensional material by regulating and controlling electric field and/or magnetic field | |
| CN111994899A (en) | Large-area rapid preparation method of graphene with vertical structure | |
| CN111501010A (en) | In-situ preparation method of metal fiber reinforced composite film | |
| KR20210055903A (en) | Method for forming bi-layer graphene | |
| JP4802321B2 (en) | Carbon nanotube growth method | |
| TWI494268B (en) | Method of manufacturing aligned carbon nanotubes | |
| JP2005247639A (en) | Method for producing carbon nanotube | |
| TW201122143A (en) | Method for forming smooth diamond thin film. | |
| CN112647059B (en) | Rapid growth of Ni by utilizing atomic layer deposition technologyxMethod for forming C film |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| PB01 | Publication | ||
| PB01 | Publication | ||
| SE01 | Entry into force of request for substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| RJ01 | Rejection of invention patent application after publication |
Application publication date: 20201225 |
|
| RJ01 | Rejection of invention patent application after publication |