CN108404911A - A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst - Google Patents
A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst Download PDFInfo
- Publication number
- CN108404911A CN108404911A CN201810328276.0A CN201810328276A CN108404911A CN 108404911 A CN108404911 A CN 108404911A CN 201810328276 A CN201810328276 A CN 201810328276A CN 108404911 A CN108404911 A CN 108404911A
- Authority
- CN
- China
- Prior art keywords
- ceo
- preparation
- catalyst
- carrier
- added
- 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
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
- B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/66—Silver or gold
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/702—Hydrocarbons
- B01D2257/7027—Aromatic hydrocarbons
Abstract
The invention discloses a kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst, includes the following steps:(1) cerium salt is dissolved in deionized water, and citric acid is added;(2) BSA solution is added;(3) dry at 50~200 DEG C, then in 300~800 DEG C of roastings, obtain carrier;(4) after mixing golden precursor solution with deionized water, above-mentioned carrier is added, stirs at room temperature;(5) by the material obtained by step (4) in 50~100 DEG C of stirrings;(6) it by after the material filtering washing obtained by step (5), in 50~100 DEG C of dryings, is then roasted to get the catalyst in 200~800 DEG C.CeO in the present invention2Carrier is to make CeO with BSA templated synthesis2Possess graded porous structure, improve its specific surface area, Kong Rong and aperture, and the sintering for slowing down crystal grain becomes larger, and grain dispersion is made to improve.
Description
Technical field
The invention belongs to technical field of nanometer material preparation, and in particular to a kind of Au/CeO for benzene catalysis oxidation2It urges
The preparation method of agent.
Background technology
Volatile organic gases (VOCs) from industrial waste gas is the main component of atmosphere pollution, and catalysis oxidation is at present
One of most effective technologies of VOCs are thoroughly eliminated, thermal oxide is different from, the temperature that it is needed is relatively low, non-secondary pollution.Catalysis
The catalyst of VOCs oxidations is broadly divided into loaded noble metal catalyst and transition metal oxide and its composite oxides.Your gold
Metal catalyst possesses higher catalytic activity, can be with low-temperature catalytic oxidation VOCs, such as Au, Pt, Pd, Ru.In your many gold
In metal catalyst, Au/CeO2Au particles and CeO in catalyst2There is synergistic effect between carrier, the oxygen of cerium ion can be promoted
Change reduction, improves CeO2Surface oxygen species activity and mobility are advantageous to improving its catalytic oxidation performance.Au nano particle rulers
Very little and Au particles and CeO2The power of interaction between carrier is to influence Au/CeO2The key factor of catalyst activity, and CeO2
Carrier structure and golden carrying method have large effect to Au particle sedimentation states again.Therefore suitable CeO is selected2It is prepared by carrier
Method and golden carrying method are necessary.
Currently, CeO2Preparation method mainly have thermal decomposition method, sol-gal process, the precipitation method, hydro-thermal method, chemical template method
Deng, however all have the shortcomings that respective, such as the product easy-sintering of thermal decomposition method and sol-gal process, structure is single;The precipitation method need
Strictly to control the generating rate of precipitating reagent;The equipment of hydro-thermal method is expensive;The process of chemical template method is complicated, difficult etc..
Invention content
It is an object of the invention to overcome prior art defect, a kind of Au/CeO for benzene catalysis oxidation is provided2Catalysis
The preparation method of agent.
Technical scheme is as follows:
A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst, includes the following steps:
(1) cerium salt is dissolved in deionized water, and citric acid is added, 1~50h is stirred at 50~100 DEG C;
(2) BSA solution is added in the material obtained by step (1), continues 1~60min of stirring;
(3) material obtained by step (2) is dried to 10~100h at 50~200 DEG C, is subsequently placed in Muffle furnace in 300
~800 DEG C of 1~10h of roasting, obtain CeO2Carrier;
(4) after mixing golden precursor solution with deionized water, pH to 7~14 is adjusted, above-mentioned CeO is then added2Carrier,
It then continues to adjust pH to 7~14, stirs 1~5h at room temperature;
(5) material obtained by step (4) is stirred into 1~5h in 50~100 DEG C;
(6) by after the material filtering washing obtained by step (5), in 50~100 DEG C of dry 1~50h, it is subsequently placed at Muffle furnace
In in 200~800 DEG C roast 1~10h to get the Au/CeO2Catalyst.
In a preferred embodiment of the invention, the cerium salt is cerous nitrate.
In a preferred embodiment of the invention, the molar ratio of the citric acid and cerium salt is 1~5: 1.
In a preferred embodiment of the invention, a concentration of 1~500mg/mL of the BSA solution.
In a preferred embodiment of the invention, the chlorauric acid solution that the golden precursor solution is 48~50mM.
In a preferred embodiment of the invention, in the step (4) pH is adjusted with NaOH aqueous solutions.
It is further preferred that in the step (1) to (3), the ratio of the cerium salt, deionized water and BSA solution is 1~
10g: 10~100mL: 10~100mL;In the step (4), the gold precursor solution, deionized water and CeO2The ratio of carrier
Example is 0.1~2mL: 5~50mL: 0.1~10g.
The beneficial effects of the invention are as follows:
1, the CeO in the present invention2Carrier is to make CeO with BSA templated synthesis2Possess graded porous structure, improves it
Specific surface area, Kong Rong and aperture, and the sintering for slowing down crystal grain becomes larger, and grain dispersion is made to improve.Compared to chemical template,
The biological template is relatively inexpensive, is easy to get, is environmentally protective;
2, catalyst of the invention is with the classifying porous CeO of BSA templated synthesis2For carrier, the size of gold particle is reduced
With the actual negative carrying capacity for improving gold, more absorption points and activation point can be provided for the catalysis oxidation of benzene;
3, preparation method of the invention is simple to operation, and reaction condition is mild, and BSA templates used have not only acted as structure
The effect of template, it may have stablize the effect with dispersed crystallites, there is larger application value;
4, by the Au/CeO of the present invention2Catalyst is used for the catalysis oxidation of benzene, shows good catalytic activity and stabilization
Property.Its T90%It is 210 DEG C, and can keeps activity stabilized in the continuous operation of 140h, tool has significant practical applications.
Description of the drawings
Fig. 1 is CeO in the embodiment of the present invention 12Scanning electron microscope (SEM) photograph.
Fig. 2 is CeO in the embodiment of the present invention 12Pore-size distribution.
Fig. 3 is Au/CeO in the embodiment of the present invention 12Transmission electron microscope picture.
Specific implementation mode
Technical scheme of the present invention is further detailed and is described below by way of specific implementation mode combination attached drawing.
Embodiment 1
(1) by 2.5g Ce (NO3)3·6H2O is dissolved in 20mL deionized waters, while 4.0g citric acids are added, and then will
The mixed solution is stirred overnight under the conditions of being placed in 70 DEG C;
(2) 10mL 70mg/mL BSA solution is added into the mixed solution of step (1), continues to stir 10min, then exist
Fully dry under the conditions of 100 DEG C, obtained yellow solid powder roasts 3h in Muffle furnace at 600 DEG C, obtains CeO2Carrier;
(3) it takes 520 μ L48.6mM aqueous solution of chloraurate to be mixed with 10mL deionized waters, pH is adjusted with 0.1M NaOH solutions
Value is 9, and 2.5g CeO are then added2Carrier, then it is 9 to adjust pH value, and 1h is stirred at room temperature;
(4) by the mixed solution in step (3) with 80 DEG C of heating stirring 1h, filtration washing, dry 12h at 50 DEG C, finally
With 300 DEG C of roasting 6h of Muffle furnace, Au/CeO is obtained2Catalyst.
The CeO of the present embodiment2Scanning electron microscope (SEM) photograph, graph of pore diameter distribution and the Au/CeO of carrier2The projection electron microscope of catalyst
Respectively successively as shown in Figure 1, Figure 2 and Figure 3.
Embodiment 2
(1) by 3.0g Ce (NO3)3·6H2O is dissolved in 20mL deionized waters, while 6.0g citric acids are added, and then will
The mixed solution is stirred overnight under the conditions of being placed in 80 DEG C;
(2) 10mL 300mg/mL BSA solution is added into the mixed solution of step (1), continues to stir 60min, then
Fully dry under the conditions of 110 DEG C, obtained yellow solid powder roasts 3h in Muffle furnace at 350 DEG C, obtains CeO2Carrier;
(3) it takes 700 μ L48.6mM aqueous solution of chloraurate to be mixed with 10mL deionized waters, pH is adjusted with 0.1M NaOH solutions
Value is 10, and 2.5g CeO are then added2Carrier, then it is 9 to adjust pH value, and 1h is stirred at room temperature;
(4) by the mixed solution in step (3) with 90 DEG C of heating stirring 1h, filtration washing, dry 12h at 50 DEG C, finally
With 300 DEG C of roasting 6h of Muffle furnace, Au/CeO is obtained2Catalyst.
Embodiment 3
(1) by 2.5g Ce (NO3)3·6H2O is dissolved in 20mL deionized waters, while 5.0g citric acids are added, and then will
The mixed solution is stirred overnight under the conditions of being placed in 90 DEG C;
(2) 20mL 300mg/mL BSA solution is added into the mixed solution of step (1), continues to stir 60min, then
Fully dry under the conditions of 120 DEG C, obtained yellow solid powder roasts 3h in Muffle furnace at 600 DEG C, obtains CeO2Carrier;
(3) it takes 200 μ L48.6mM aqueous solution of chloraurate to be mixed with 10mL deionized waters, pH is adjusted with 0.1M NaOH solutions
Value is 7, and 2.5g CeO are then added2Carrier, then it is 9 to adjust pH value, and Ih is stirred at room temperature;
(4) by the mixed solution in step (3) with 70 DEG C of heating stirring 1h, filtration washing, dry 12h at 50 DEG C, finally
With 400 DEG C of roasting 6h of Muffle furnace, Au/CeO is obtained2Catalyst.
Embodiment 4
Au/CeO prepared by the embodiment of the present invention 12Catalyst is used it for the catalysis oxidation of benzene, is urged by experimental evaluation
The activity and stability of agent, specific experiment process are as follows:
Experiment 1
By the Au/CeO2Catalyst is used for the oxidation of 1000ppm benzene, and benzene conversion ratio temperature required when reaching 90% is
210℃.Evaluation condition is:Gas group becomes benzene, oxygen and nitrogen, and the wherein molar ratio of benzene and oxygen is 1: 400, gas flow rate
For 16.7mL/min, catalyst quality 50mg, air speed is 20000mL/ (gcat·h);
Experiment 2
By the Au/CeO2Catalyst carries out stability test, investigates the catalyst in the oxidation process for being catalyzed 1000ppm benzene
In active variation, by the continuous operation of 140h, the activity of the catalyst keeps stablizing during the reaction.Test condition
For:Gas group become benzene, oxygen and nitrogen, wherein the molar ratio of benzene and oxygen be 1: 400, gas flow rate 16.7mL/min,
Catalyst quality is 50mg, and air speed is 20000mL/ (gcatH), reaction temperature is 210 DEG C.
Those of ordinary skill in the art remain able to it is found that when technical scheme of the present invention changes in following ranges
To same as the previously described embodiments or similar technique effect, protection scope of the present invention is still fallen within:
A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst, includes the following steps:
(1) cerium salt is dissolved in deionized water, and citric acid is added, 1~50h is stirred at 50~100 DEG C;
(2) BSA solution is added in the material obtained by step (1), continues 1~60min of stirring;
(3) material obtained by step (2) is dried to 10~100h at 50~200 DEG C, is subsequently placed in Muffle furnace in 300
~800 DEG C of 1~10h of roasting, obtain CeO2Carrier;
(4) after mixing golden precursor solution with deionized water, pH to 7~14 is adjusted, above-mentioned CeO is then added2Carrier,
It then continues to adjust pH to 7~14, stirs 1~5h at room temperature;
(5) material obtained by step (4) is stirred into 1~5h in 50~100 DEG C;
(6) by after the material filtering washing obtained by step (5), in 50~100 DEG C of dry 1~50h, it is subsequently placed at Muffle furnace
In in 200~800 DEG C roast 1~10h to get the Au/CeO2Catalyst.
The molar ratio of the citric acid and cerium salt is 1~5: 1.A concentration of 1~500mg/mL of the BSA solution.It is described
Golden precursor solution is the chlorauric acid solution of 48~50mM.In the step (1) to (3), the cerium salt, deionized water and BSA
The ratio of solution is 1~10g: 10~100mL: 10~100mL;In the step (4), the gold precursor solution, deionization
Water and CeO2The ratio of carrier is 0.1~2mL: 5~50mL: 0.1~10g.
The foregoing is only a preferred embodiment of the present invention, therefore cannot limit the scope of implementation of the present invention according to this, i.e.,
According to equivalent changes and modifications made by the scope of the claims of the present invention and description, all should still belong in the range of the present invention covers.
Claims (7)
1. a kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst, it is characterised in that:Include the following steps:
(1) cerium salt is dissolved in deionized water, and citric acid is added, 1~50h is stirred at 50~100 DEG C;
(2) BSA solution is added in the material obtained by step (1), continues 1~60min of stirring;
(3) by the material obtained by step (2) at 50~200 DEG C dry 10~100h, be subsequently placed in Muffle furnace in 300~
800 DEG C of 1~10h of roasting, obtain CeO2Carrier;
(4) after mixing golden precursor solution with deionized water, pH to 7~14 is adjusted, above-mentioned CeO is then added2Carrier, then
Continue to adjust pH to 7~14, stirs 1~5h at room temperature;
(5) material obtained by step (4) is stirred into 1~5h in 50~100 DEG C;
(6) by obtained by step (5) material filtering washing after, in 50~100 DEG C of dry 1~50h, be subsequently placed in Muffle furnace in
200~800 DEG C of 1~10h of roasting are to get the Au/CeO2Catalyst.
2. preparation method as described in claim 1, it is characterised in that:The cerium salt is cerous nitrate.
3. preparation method as described in claim 1, it is characterised in that:The molar ratio of the citric acid and cerium salt is 1~5: 1.
4. preparation method as described in claim 1, it is characterised in that:A concentration of 1~500mg/mL of the BSA solution.
5. preparation method as described in claim 1, it is characterised in that:The gold chloride that the gold precursor solution is 48~50mM
Solution.
6. preparation method as described in claim 1, it is characterised in that:In the step (4) pH is adjusted with NaOH aqueous solutions.
7. the preparation method as described in any claim in claim 1 to 6, it is characterised in that:The step (1) to (3)
In, the ratio of the cerium salt, deionized water and BSA solution is 1~10g: 10~100mL: 10~100mL;The step (4)
In, the gold precursor solution, deionized water and CeO2The ratio of carrier is 0.1~2mL: 5~50mL: 0.1~10g.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CN201810328276.0A CN108404911A (en) | 2018-04-12 | 2018-04-12 | A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CN201810328276.0A CN108404911A (en) | 2018-04-12 | 2018-04-12 | A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst |
Publications (1)
Publication Number | Publication Date |
---|---|
CN108404911A true CN108404911A (en) | 2018-08-17 |
Family
ID=63135316
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
CN201810328276.0A Pending CN108404911A (en) | 2018-04-12 | 2018-04-12 | A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst |
Country Status (1)
Country | Link |
---|---|
CN (1) | CN108404911A (en) |
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN109317141A (en) * | 2018-11-14 | 2019-02-12 | 泉州师范学院 | A kind of preparation method of the Pt base catalyst for benzene catalysis oxidation |
CN111167450A (en) * | 2020-03-16 | 2020-05-19 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation method of niobium modified cerium oxide supported gold catalyst, product and application thereof |
Citations (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN102951940A (en) * | 2012-11-05 | 2013-03-06 | 昆明理工大学 | Mesoporous cerium dioxide material preparation method |
CN103920492A (en) * | 2014-03-10 | 2014-07-16 | 苏州科技学院相城研究院 | Mesoporous mesomorphic cerium oxide loaded noble metal catalyst and preparation method and application |
CN105536777A (en) * | 2015-12-17 | 2016-05-04 | 杭州电子科技大学 | Catalytic combustion active ingredient highly-dispersed catalyst and preparation method thereof |
CN105693922A (en) * | 2016-02-02 | 2016-06-22 | 扬州大学 | Amphiprotic protein ice gel imprinted polymer, and preparation method and application thereof |
CN107597109A (en) * | 2017-08-09 | 2018-01-19 | 华东师范大学 | Load type gold catalyst of nano-metal-oxide doping and preparation method and application |
CN107857307A (en) * | 2017-11-20 | 2018-03-30 | 青岛农业大学 | A kind of new strategy for realizing one kettle way grape grape color developing detection |
-
2018
- 2018-04-12 CN CN201810328276.0A patent/CN108404911A/en active Pending
Patent Citations (6)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN102951940A (en) * | 2012-11-05 | 2013-03-06 | 昆明理工大学 | Mesoporous cerium dioxide material preparation method |
CN103920492A (en) * | 2014-03-10 | 2014-07-16 | 苏州科技学院相城研究院 | Mesoporous mesomorphic cerium oxide loaded noble metal catalyst and preparation method and application |
CN105536777A (en) * | 2015-12-17 | 2016-05-04 | 杭州电子科技大学 | Catalytic combustion active ingredient highly-dispersed catalyst and preparation method thereof |
CN105693922A (en) * | 2016-02-02 | 2016-06-22 | 扬州大学 | Amphiprotic protein ice gel imprinted polymer, and preparation method and application thereof |
CN107597109A (en) * | 2017-08-09 | 2018-01-19 | 华东师范大学 | Load type gold catalyst of nano-metal-oxide doping and preparation method and application |
CN107857307A (en) * | 2017-11-20 | 2018-03-30 | 青岛农业大学 | A kind of new strategy for realizing one kettle way grape grape color developing detection |
Non-Patent Citations (2)
Title |
---|
FANG YING ET AL.: ""Highly active and stable mesoporous Au/CeO2 catalysts prepared from MCM-48 hard-template"", 《MICROPOROUS AND MESOPOROUS MATERIALS》 * |
何少斌 等: ""牛血清白蛋白模板法制备的金属复合纳米材料在生物检测中的应用"", 《分析科学学报》 * |
Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN109317141A (en) * | 2018-11-14 | 2019-02-12 | 泉州师范学院 | A kind of preparation method of the Pt base catalyst for benzene catalysis oxidation |
CN111167450A (en) * | 2020-03-16 | 2020-05-19 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation method of niobium modified cerium oxide supported gold catalyst, product and application thereof |
CN111167450B (en) * | 2020-03-16 | 2023-09-15 | 上海纳米技术及应用国家工程研究中心有限公司 | Preparation method of niobium modified cerium oxide supported gold catalyst, product and application thereof |
Similar Documents
Publication | Publication Date | Title |
---|---|---|
CN111905793B (en) | Preparation method of nitrogen-doped carbon-supported non-noble metal monatomic catalyst | |
US8450236B2 (en) | Supported precious metal catalysts via hydrothermal deposition | |
CN111889101B (en) | Modified composite oxide catalyst for synergistic purification of VOCs and NO and preparation method thereof | |
CN104743529B (en) | Synthesis method of tungsten nitride with high catalytic performance | |
CN109772463B (en) | Catalyst ZIF-67-Me/CuO for CO reduction and low-temperature denitrationxAnd preparation method and application thereof | |
CN105413705A (en) | Catalyst for removing VOCs through photocatalysis in cooperation with thermal catalytic oxidation and preparation method and application of catalyst | |
CN107511147A (en) | A kind of high stability catalyst for catalytic oxidation and preparation method | |
US8921259B2 (en) | Exhaust gas purification catalyst for removing CO or HC, and method for manufacturing same | |
CN106732581A (en) | A kind of Ru/CeTiO for low-temperature SCR reactionXThe preparation method of catalyst | |
CN108906044B (en) | Manganese-cerium-ruthenium composite oxide catalyst and preparation method and application thereof | |
CN107008490A (en) | A kind of oxidation catalyst of purifying tail gas of diesel vehicles and preparation method thereof | |
CN110193368B (en) | Preparation method of spinel type catalytic material | |
CN108404911A (en) | A kind of Au/CeO for benzene catalysis oxidation2The preparation method of catalyst | |
CN109772442B (en) | Supported composite transition metal oxide, preparation method and application as catalyst | |
CN113019364A (en) | Preparation method of porous ruthenium dioxide-cerium dioxide microsphere composite material | |
CN109174092B (en) | Zinc oxide/platinum composite material microsphere and preparation method and application thereof | |
CN105879869A (en) | Catalyst used for hydrogen selective reduction of nitric oxide as well as preparation method and application thereof | |
CN113663671A (en) | Ternary metal catalyst and preparation method and application thereof | |
CN113694933A (en) | High-entropy co-doped low-temperature SCR denitration catalyst and preparation method and application thereof | |
CN113772710A (en) | Preparation method and application of cerium dioxide nanowire | |
JP2012187523A (en) | Exhaust gas-purifying catalyst support, exhaust gas-purifying catalyst made using the support, and method for producing exhaust gas-purifying catalyst support | |
CN112584926B (en) | Catalyst for purifying exhaust gas | |
CN110302819B (en) | MOFs-derived bimetallic magnetic nanoporous carbon ozone catalyst and application thereof | |
Wang et al. | Evaluation of NO oxidation properties over a Mn-Ce/γ-Al 2 O 3 catalyst | |
JP4591920B2 (en) | Photocatalyst and method for producing the same |
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: 20180817 |
|
RJ01 | Rejection of invention patent application after publication |