CN114196976A - Long-life coating and preparation method thereof - Google Patents

Long-life coating and preparation method thereof Download PDF

Info

Publication number
CN114196976A
CN114196976A CN202111620606.1A CN202111620606A CN114196976A CN 114196976 A CN114196976 A CN 114196976A CN 202111620606 A CN202111620606 A CN 202111620606A CN 114196976 A CN114196976 A CN 114196976A
Authority
CN
China
Prior art keywords
coating
parts
plating
iridium
ruthenium
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
CN202111620606.1A
Other languages
Chinese (zh)
Inventor
潘洪明
唐正飞
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.)
Suzhou Fenggang Titanium Products And Equipment Manufacturing Co ltd
Original Assignee
Suzhou Fenggang Titanium Products And Equipment Manufacturing 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 Suzhou Fenggang Titanium Products And Equipment Manufacturing Co ltd filed Critical Suzhou Fenggang Titanium Products And Equipment Manufacturing Co ltd
Priority to CN202111620606.1A priority Critical patent/CN114196976A/en
Publication of CN114196976A publication Critical patent/CN114196976A/en
Pending legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25BELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Chemically Coating (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
  • Other Surface Treatments For Metallic Materials (AREA)

Abstract

The invention discloses a long-life coating and a preparation method thereof, wherein the long-life coating is prepared from the following components: according to the weight portion, the ruthenium coating is 75-95 parts, the iridium coating is 2-3 parts, the platinum coating is 5-6 parts, the palladium coating is 1-3 parts, the tantalum coating is 2-3 parts, the gold coating is 1-2 parts, the tin coating is 2-3 parts, the aluminum oxide coating is 1-2 parts, the ceramic coating is 2-4 parts, and the titanium coating is 1-3 parts, the novel long-life coating and the preparation method thereof, the ruthenium coating can improve the electrolytic efficiency and prolong the service life of the electrode, the iridium coating and the platinum coating enable the electrode to have better catalytic activity in an oxygen evolution type environment, the palladium coating, the tantalum coating, the gold coating and the tin coating can carry out anti-oxidation protection on the electrode, the aluminum oxide coating and the ceramic coating can form a compact isolation protective layer on the surface of the electrode, the electrode is protected against corrosion first, the titanium coating can prolong the service life of the electrode and improve the electrolytic efficiency, the addition of ruthenium, iridium, platinum, palladium, tantalum, gold and tin coating materials reduces the cost of the insoluble anode and prolongs the service life of the electrolytic cell.

Description

Long-life coating and preparation method thereof
Technical Field
The invention relates to the field of electrolysis, in particular to a long-life coating and a preparation method thereof.
Background
The electrochemical cell can generate an electrolysis process called electrolysis when a direct current voltage is applied, the electrolysis is widely applied to the fields of hydrogen production, fuel cell production and the like, and the coating is one of effective structures for protecting an electrolytic cell, however, the coating on the market has the following defects: at present, most of coatings are simple iridium-tantalum and ruthenium-iridium coatings, a high-temperature sintering mode is adopted, the protection effect on an electrolytic cell is low, workers are easily accidentally injured by high-temperature sintering, and unnecessary economic loss is caused.
The technical scheme of the invention mainly aims at the problems that the coating structure is simple, the protection effect on the electrolytic cell is low, and ruthenium, iridium, platinum, palladium, tantalum, gold and tin coating materials are added, so that the cost of an insoluble anode is reduced, the service life of the electrolytic cell is prolonged, and the electrolysis efficiency of the electrolytic cell is improved.
Disclosure of Invention
The invention aims to provide a long-life coating and a preparation method thereof, and aims to solve the problems that most of the conventional coatings proposed in the background art are simple iridium-tantalum and ruthenium-iridium coatings, the protection effect on an electrolytic cell is low due to a high-temperature sintering mode, and workers are easily accidentally injured due to the high-temperature sintering, so that unnecessary economic loss is caused.
In order to achieve the purpose, the invention provides the following technical scheme: a long-life coating and a preparation method thereof are disclosed, which comprises the following components: the composition is prepared from the following components: the coating comprises, by weight, 75-95 parts of a ruthenium coating, 2-3 parts of an iridium coating, 5-6 parts of a platinum coating, 1-3 parts of a palladium coating, 2-3 parts of a tantalum coating, 1-2 parts of a gold coating, 2-3 parts of a tin coating, 1-2 parts of an aluminum oxide coating, 2-4 parts of a ceramic coating and 1-3 parts of a titanium coating.
The preferable technical scheme of the invention comprises the following components of, by weight, 80 parts of a ruthenium coating, 2 parts of an iridium coating, 5 parts of a platinum coating, 2 parts of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 2 parts of an aluminum oxide coating, 2 parts of a pure ceramic coating and 2 parts of a titanium coating.
The preferable technical scheme of the invention comprises the following components of, by weight, 83 parts of a ruthenium coating, 2 parts of an iridium coating, 5 parts of a platinum coating, 1 part of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 1 part of an aluminum oxide coating, 2 parts of a ceramic coating and 1 part of a titanium coating.
The preferable technical scheme of the invention comprises the following components of, by weight, 82 parts of a ruthenium coating, 2 parts of an iridium coating, 6 parts of a platinum coating, 1 part of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 1 part of an aluminum oxide coating, 2 parts of a ceramic coating and 1 part of a titanium coating.
A preparation method of a long-life coating comprises the following steps:
step one, selecting an original film: selecting a proper film as a coating basement membrane;
step two, ruthenium treatment: plating ruthenium on one side of the film to form a ruthenium coating on the surface of the film;
step three, iridium treatment: plating iridium on one side of the ruthenium coating in and out, and forming an iridium coating on the surface of the ruthenium coating;
step four, platinum treatment: plating platinum on one side of the iridium coating to form a platinum coating on the surface of the iridium coating;
step five, palladium treatment: plating palladium on one side of the platinum coating to form a palladium coating on the surface of the platinum coating;
step six, tantalum treatment: tantalum is plated on one side of the palladium coating, and a tantalum coating is formed on the surface of the palladium coating;
step seven, gold treatment: gold plating is carried out on one side of the tantalum coating, and a gold coating is formed on the surface of the tantalum coating;
step eight, tin treatment: tin plating is carried out on one side of the gold coating, and a tin coating is formed on the surface of the gold coating;
step nine, aluminum oxide treatment: aluminizing one side of the tin coating to form an aluminum oxide coating on the surface of the tin coating;
step ten, ceramic coating treatment: uniformly coating a ceramic coating on one side of the alumina coating;
step eleven, titanium treatment: plating titanium on one side of the ceramic coating to form a titanium coating on the surface of the ceramic coating
Step twelve, cleaning: and cleaning and disinfecting the obtained coating.
As a preferable technical scheme of the invention, the ruthenium plating in the step two, the iridium plating in the step three, the platinum plating in the step four, the palladium plating in the step five, the tantalum plating in the step six, the gold plating in the step seven and the tin plating in the step eight adopt chemical plating.
As a preferable technical scheme of the invention, the aluminizing in the ninth step and the titanizing in the eleventh step are both performed by plasma thermal spraying.
In a preferred embodiment of the present invention, the cleaning in the twelfth step is to clean the coating layer by placing the coating layer in an ultrasonic cleaner filled with ultrapure water.
Compared with the prior art, the invention has the beneficial effects that: the ruthenium coating can improve the electrolytic efficiency and prolong the service life of the electrode, the iridium coating and the platinum coating enable the electrode to have better catalytic activity when used in an oxygen evolution type environment, the palladium coating, the tantalum coating, the gold coating and the tin coating can perform anti-oxidation protection on the electrode, the aluminum oxide coating and the ceramic coating can form a compact isolation protective layer on the surface of the electrode, the electrode is protected from corrosion firstly, and the titanium coating can prolong the service life of the electrode and improve the electrolytic efficiency.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments 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 making any creative effort, shall fall within the protection scope of the present invention.
Example 1
The invention provides a long-life coating, which comprises, by weight, 80 parts of a ruthenium coating, 2 parts of an iridium coating, 5 parts of a platinum coating, 2 parts of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 2 parts of an aluminum oxide coating, 2 parts of a ceramic coating and 2 parts of a titanium coating.
The preparation method of the long-life coating comprises the following steps:
firstly, selecting a proper film to be placed on a laser cutter for cutting, and making a coating basement membrane;
secondly, plating ruthenium on one side of the film to form a ruthenium coating on the surface of the film;
thirdly, plating iridium on one side of the ruthenium coating far away from the film in an in-and-out mode, and forming an iridium coating on the surface of the ruthenium coating;
plating platinum on one side of the iridium coating layer, which is far away from the ruthenium coating layer, and forming a platinum coating layer on the surface of the iridium coating layer;
step five, plating palladium on one side of the platinum coating, which is far away from the iridium coating, and forming a palladium coating on the surface of the platinum coating;
step six, tantalum plating is carried out on one side, away from the platinum coating, of the palladium coating, and a tantalum coating is formed on the surface of the palladium coating;
step seven, gold plating is carried out on one side of the tantalum coating layer, which is far away from the palladium coating layer, and a gold coating layer is formed on the surface of the tantalum coating layer;
step eight, tin plating is carried out on one side of the gold coating layer, which is far away from the tantalum coating layer, and a tin coating layer is formed on the surface of the gold coating layer;
step nine, aluminizing the side, away from the gold coating, of the tin coating, and forming an aluminum oxide coating on the surface of the tin coating;
step ten, uniformly coating a ceramic coating on one side of the aluminum oxide coating, which is far away from the tin coating;
step eleven, performing titanium plating on one side of the ceramic coating far away from the alumina coating to form a titanium coating on the surface of the ceramic coating
And step twelve, placing the prepared coating in an ultrasonic cleaner filled with ultrapure water for cleaning and disinfection to obtain a coating finished product.
Example 2
The invention provides a long-life coating, which comprises, by weight, 83 parts of a ruthenium coating, 2 parts of an iridium coating, 5 parts of a platinum coating, 1 part of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 1 part of an aluminum oxide coating, 2 parts of a ceramic coating and 1 part of a titanium coating.
The preparation method of the long-life coating comprises the following steps:
firstly, selecting a proper film to be placed on a laser cutter for cutting, and making a coating basement membrane;
secondly, plating ruthenium on one side of the film to form a ruthenium coating on the surface of the film;
thirdly, plating iridium on one side of the ruthenium coating far away from the film in an in-and-out mode, and forming an iridium coating on the surface of the ruthenium coating;
plating platinum on one side of the iridium coating layer, which is far away from the ruthenium coating layer, and forming a platinum coating layer on the surface of the iridium coating layer;
step five, plating palladium on one side of the platinum coating, which is far away from the iridium coating, and forming a palladium coating on the surface of the platinum coating;
step six, tantalum plating is carried out on one side, away from the platinum coating, of the palladium coating, and a tantalum coating is formed on the surface of the palladium coating;
step seven, gold plating is carried out on one side of the tantalum coating layer, which is far away from the palladium coating layer, and a gold coating layer is formed on the surface of the tantalum coating layer;
step eight, tin plating is carried out on one side of the gold coating layer, which is far away from the tantalum coating layer, and a tin coating layer is formed on the surface of the gold coating layer;
step nine, aluminizing the side, away from the gold coating, of the tin coating, and forming an aluminum oxide coating on the surface of the tin coating;
step ten, uniformly coating a ceramic coating on one side of the aluminum oxide coating, which is far away from the tin coating;
step eleven, performing titanium plating on one side of the ceramic coating far away from the alumina coating to form a titanium coating on the surface of the ceramic coating
And step twelve, placing the prepared coating in an ultrasonic cleaner filled with ultrapure water for cleaning and disinfection to obtain a coating finished product.
Example 3
The invention provides a long-life coating, which comprises 82 parts by weight of a ruthenium coating, 2 parts by weight of an iridium coating, 6 parts by weight of a platinum coating, 1 part by weight of a palladium coating, 2 parts by weight of a tantalum coating, 1 part by weight of a gold coating, 2 parts by weight of a tin coating, 1 part by weight of an aluminum oxide coating, 2 parts by weight of a ceramic coating and 1 part by weight of a titanium coating.
The preparation method of the long-life coating comprises the following steps:
firstly, selecting a proper film to be placed on a laser cutter for cutting, and making a coating basement membrane;
secondly, plating ruthenium on one side of the film to form a ruthenium coating on the surface of the film;
thirdly, plating iridium on one side of the ruthenium coating far away from the film in an in-and-out mode, and forming an iridium coating on the surface of the ruthenium coating;
plating platinum on one side of the iridium coating layer, which is far away from the ruthenium coating layer, and forming a platinum coating layer on the surface of the iridium coating layer;
step five, plating palladium on one side of the platinum coating, which is far away from the iridium coating, and forming a palladium coating on the surface of the platinum coating;
step six, tantalum plating is carried out on one side, away from the platinum coating, of the palladium coating, and a tantalum coating is formed on the surface of the palladium coating;
step seven, gold plating is carried out on one side of the tantalum coating layer, which is far away from the palladium coating layer, and a gold coating layer is formed on the surface of the tantalum coating layer;
step eight, tin plating is carried out on one side of the gold coating layer, which is far away from the tantalum coating layer, and a tin coating layer is formed on the surface of the gold coating layer;
step nine, aluminizing the side, away from the gold coating, of the tin coating, and forming an aluminum oxide coating on the surface of the tin coating;
step ten, uniformly coating a ceramic coating on one side of the aluminum oxide coating, which is far away from the tin coating;
step eleven, performing titanium plating on one side of the ceramic coating far away from the alumina coating to form a titanium coating on the surface of the ceramic coating
And step twelve, placing the prepared coating in an ultrasonic cleaner filled with ultrapure water for cleaning and disinfection to obtain a coating finished product.
According to the above description, the ruthenium coating, the iridium coating, the platinum coating, the palladium coating, the tantalum coating, the gold coating, the tin coating, the aluminum oxide coating, the ceramic coating and the titanium coating are added on the surface of the film, ruthenium has stable chemical properties at a medium temperature, the ruthenium coating can improve the electrolytic efficiency and prolong the service life of the electrode, the iridium coating and the platinum coating enable the catalytic activity of the electrode to be better when the electrode is used in an oxygen evolution type environment, the palladium coating, the tantalum coating, the gold coating and the tin coating are inactive in chemical properties and can perform anti-oxidation protection on the electrode, the aluminum oxide coating and the ceramic coating can form a compact isolation protective layer on the surface of the electrode, the electrode is protected from corrosion firstly, and the titanium coating can prolong the service life of the electrode and improve the electrolytic efficiency.
Although the present invention has been described in detail with reference to the foregoing embodiments, it will be apparent to those skilled in the art that various changes in the embodiments and/or modifications of the invention can be made, and equivalents and modifications of some features of the invention can be made without departing from the spirit and scope of the invention.

Claims (8)

1. A long life coating, comprising the following components: the coating comprises, by weight, 75-95 parts of a ruthenium coating, 2-3 parts of an iridium coating, 5-6 parts of a platinum coating, 1-3 parts of a palladium coating, 2-3 parts of a tantalum coating, 1-2 parts of a gold coating, 2-3 parts of a tin coating, 1-2 parts of an aluminum oxide coating, 2-4 parts of a ceramic coating and 1-3 parts of a titanium coating.
2. The long life coating of claim 1, comprising, in parts by weight, 80 parts of a ruthenium coating, 2 parts of an iridium coating, 5 parts of a platinum coating, 2 parts of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 2 parts of an alumina coating, 2 parts of a ceramic coating, 2 parts of a titanium coating.
3. The long life coating of claim 1, comprising, in parts by weight, 83 parts of a ruthenium coating, 2 parts of an iridium coating, 5 parts of a platinum coating, 1 part of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 1 part of an alumina coating, 2 parts of a ceramic coating, and 1 part of a titanium coating.
4. The long life coating of claim 1, comprising, in parts by weight, 82 parts of a ruthenium coating, 2 parts of an iridium coating, 6 parts of a platinum coating, 1 part of a palladium coating, 2 parts of a tantalum coating, 1 part of a gold coating, 2 parts of a tin coating, 1 part of an alumina coating, 2 parts of a ceramic coating, and 1 part of a titanium coating.
5. A method of producing a long life coating as claimed in any one of claims 1 to 4, comprising the steps of:
step one, selecting an original film: selecting a proper film as a coating basement membrane;
step two, ruthenium treatment: plating ruthenium on one side of the film to form a ruthenium coating on the surface of the film;
step three, iridium treatment: plating iridium on one side of the ruthenium coating in and out, and forming an iridium coating on the surface of the ruthenium coating;
step four, platinum treatment: plating platinum on one side of the iridium coating to form a platinum coating on the surface of the iridium coating;
step five, palladium treatment: plating palladium on one side of the platinum coating to form a palladium coating on the surface of the platinum coating;
step six, tantalum treatment: tantalum is plated on one side of the palladium coating, and a tantalum coating is formed on the surface of the palladium coating;
step seven, gold treatment: gold plating is carried out on one side of the tantalum coating, and a gold coating is formed on the surface of the tantalum coating;
step eight, tin treatment: tin plating is carried out on one side of the gold coating, and a tin coating is formed on the surface of the gold coating;
step nine, aluminum oxide treatment: aluminizing one side of the tin coating to form an aluminum oxide coating on the surface of the tin coating;
step ten, ceramic coating treatment: uniformly coating a ceramic coating on one side of the alumina coating;
step eleven, titanium treatment: plating titanium on one side of the ceramic coating to form a titanium coating on the surface of the ceramic coating
Step twelve, cleaning: and cleaning and disinfecting the obtained coating.
6. The method of claim 5, wherein the second step of plating ruthenium, the third step of plating iridium, the fourth step of plating platinum, the fifth step of plating palladium, the sixth step of plating tantalum, the seventh step of plating gold, and the eighth step of plating tin are performed by electroless plating.
7. The method of claim 5, wherein the aluminizing in step nine and the titanizing in step eleven are both performed by plasma thermal spraying.
8. The method for preparing a long-life coating according to claim 5, wherein the cleaning in the twelfth step is performed by placing the coating in an ultrasonic cleaner filled with ultrapure water.
CN202111620606.1A 2021-12-28 2021-12-28 Long-life coating and preparation method thereof Pending CN114196976A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202111620606.1A CN114196976A (en) 2021-12-28 2021-12-28 Long-life coating and preparation method thereof

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202111620606.1A CN114196976A (en) 2021-12-28 2021-12-28 Long-life coating and preparation method thereof

Publications (1)

Publication Number Publication Date
CN114196976A true CN114196976A (en) 2022-03-18

Family

ID=80656874

Family Applications (1)

Application Number Title Priority Date Filing Date
CN202111620606.1A Pending CN114196976A (en) 2021-12-28 2021-12-28 Long-life coating and preparation method thereof

Country Status (1)

Country Link
CN (1) CN114196976A (en)

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20030022016A1 (en) * 2001-07-27 2003-01-30 Ramgopal Darolia Article having a protective coating and an iridium-containing oxygen barrier layer
CN1473206A (en) * 2000-11-08 2004-02-04 Plasma electroplating
CN103060862A (en) * 2012-12-26 2013-04-24 广东电网公司电力科学研究院 Titanium coating and preparation method thereof
CN104562078A (en) * 2014-12-24 2015-04-29 蓝星(北京)化工机械有限公司 Electrode for electrolysis, preparation method of electrode and electrolytic bath

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1473206A (en) * 2000-11-08 2004-02-04 Plasma electroplating
US20030022016A1 (en) * 2001-07-27 2003-01-30 Ramgopal Darolia Article having a protective coating and an iridium-containing oxygen barrier layer
CN103060862A (en) * 2012-12-26 2013-04-24 广东电网公司电力科学研究院 Titanium coating and preparation method thereof
CN104562078A (en) * 2014-12-24 2015-04-29 蓝星(北京)化工机械有限公司 Electrode for electrolysis, preparation method of electrode and electrolytic bath

Similar Documents

Publication Publication Date Title
CN101532147B (en) Nanocrystal metal oxide composite electrode and method for preparing same
EP2098616B1 (en) Cathode for hydrogen generation
CN102174704A (en) Preparation method for tantalum-contained interlayer metallic oxide electrode
CN110318068B (en) Anode coating for ion-exchange membrane electrolyzer
KR20050083767A (en) Coatings for the inhibition of undesirable oxidation in an electrochemical cell
KR20220142468A (en) Polarity reversible electrode and use thereof
EP0262369B1 (en) Lead oxide-coated electrode for use in electrolysis and process for producing the same
EP3772547B1 (en) Anode, preparation method and use thereof, ozone generating system, and dental scaler
CN113061926A (en) Titanium dioxide anode diffusion layer for PEM water electrolysis cell and preparation method and application thereof
KR20220068205A (en) Oxygen electrode comprising a dual plating catalyst, water electrolysis device, regenerative fuel cell including the same and method for preparing the oxygen electrode
JPH0488182A (en) Electrode structure for ozone production and its production
EA029324B1 (en) Electrode for oxygen evolution in industrial electrochemical processes
CN114196976A (en) Long-life coating and preparation method thereof
JPH0238669B2 (en)
CN102864465A (en) Preparation method of high-activity Ti/Pr2O3-PbO2 modified electrode
US5004626A (en) Anodes and method of making
JP3010496B2 (en) Electrode for water electrolysis and method for producing the same
CN109402654A (en) A kind of MoS with substrate protective function2/Ni3Se2Compound Electrocatalytic Activity for Hydrogen Evolution Reaction agent and preparation method thereof
Tamm et al. Cathodic hydrogen evolution on nickel in acidic environment
JPH03188291A (en) Electrolytic catalyst coating
JPS58136790A (en) Insoluble anode
JP5669894B2 (en) Method for producing corrosion-resistant conductive coating material
EP2655693B1 (en) Electrode for electrolytic cell
JPH02179891A (en) Anode for generate oxygen and production thereof
CN115537883B (en) IrO for electrolytic copper foil production 2 -Ta 2 O 5 Method for reducing oxygen evolution potential of Ti electrode

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
RJ01 Rejection of invention patent application after publication

Application publication date: 20220318