CN115417694B - Catalytic honeycomb ceramic material and preparation method and application thereof - Google Patents
Catalytic honeycomb ceramic material and preparation method and application thereof Download PDFInfo
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- CN115417694B CN115417694B CN202211060757.0A CN202211060757A CN115417694B CN 115417694 B CN115417694 B CN 115417694B CN 202211060757 A CN202211060757 A CN 202211060757A CN 115417694 B CN115417694 B CN 115417694B
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- 229910010293 ceramic material Inorganic materials 0.000 title claims abstract description 65
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 54
- 238000002360 preparation method Methods 0.000 title claims abstract description 28
- 239000000919 ceramic Substances 0.000 claims abstract description 80
- 239000000758 substrate Substances 0.000 claims abstract description 72
- 239000011248 coating agent Substances 0.000 claims abstract description 65
- 238000000576 coating method Methods 0.000 claims abstract description 65
- 239000007788 liquid Substances 0.000 claims abstract description 44
- 238000010438 heat treatment Methods 0.000 claims abstract description 25
- 238000002156 mixing Methods 0.000 claims abstract description 19
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims abstract description 13
- 239000012298 atmosphere Substances 0.000 claims abstract description 13
- 229910017604 nitric acid Inorganic materials 0.000 claims abstract description 13
- 239000003344 environmental pollutant Substances 0.000 claims abstract description 12
- 231100000719 pollutant Toxicity 0.000 claims abstract description 12
- 238000009835 boiling Methods 0.000 claims abstract description 10
- 238000010926 purge Methods 0.000 claims abstract description 9
- 230000000087 stabilizing effect Effects 0.000 claims abstract description 9
- 238000005406 washing Methods 0.000 claims abstract description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 9
- 229910052751 metal Inorganic materials 0.000 claims abstract description 8
- 239000002184 metal Substances 0.000 claims abstract description 8
- 150000003839 salts Chemical class 0.000 claims abstract description 8
- 239000003795 chemical substances by application Substances 0.000 claims abstract description 7
- 239000000853 adhesive Substances 0.000 claims abstract description 6
- 230000001070 adhesive effect Effects 0.000 claims abstract description 6
- 238000002791 soaking Methods 0.000 claims abstract description 6
- 239000012752 auxiliary agent Substances 0.000 claims abstract description 5
- 238000000034 method Methods 0.000 claims description 14
- UIIMBOGNXHQVGW-UHFFFAOYSA-M Sodium bicarbonate Chemical compound [Na+].OC([O-])=O UIIMBOGNXHQVGW-UHFFFAOYSA-M 0.000 claims description 12
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 10
- 239000004202 carbamide Substances 0.000 claims description 10
- KCXVZYZYPLLWCC-UHFFFAOYSA-N EDTA Chemical compound OC(=O)CN(CC(O)=O)CCN(CC(O)=O)CC(O)=O KCXVZYZYPLLWCC-UHFFFAOYSA-N 0.000 claims description 8
- DHMQDGOQFOQNFH-UHFFFAOYSA-N Glycine Chemical compound NCC(O)=O DHMQDGOQFOQNFH-UHFFFAOYSA-N 0.000 claims description 8
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 claims description 8
- ORTQZVOHEJQUHG-UHFFFAOYSA-L copper(II) chloride Chemical compound Cl[Cu]Cl ORTQZVOHEJQUHG-UHFFFAOYSA-L 0.000 claims description 8
- ONDPHDOFVYQSGI-UHFFFAOYSA-N zinc nitrate Chemical compound [Zn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ONDPHDOFVYQSGI-UHFFFAOYSA-N 0.000 claims description 8
- 229910000030 sodium bicarbonate Inorganic materials 0.000 claims description 6
- 235000017557 sodium bicarbonate Nutrition 0.000 claims description 6
- 238000000746 purification Methods 0.000 claims description 5
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 claims description 4
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical compound NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 claims description 4
- 239000004471 Glycine Substances 0.000 claims description 4
- 239000000654 additive Substances 0.000 claims description 4
- 230000000996 additive effect Effects 0.000 claims description 4
- 239000001110 calcium chloride Substances 0.000 claims description 4
- 229910001628 calcium chloride Inorganic materials 0.000 claims description 4
- 229910001629 magnesium chloride Inorganic materials 0.000 claims description 4
- 238000001179 sorption measurement Methods 0.000 abstract description 22
- 238000007654 immersion Methods 0.000 abstract description 8
- 230000000694 effects Effects 0.000 abstract description 6
- 238000003756 stirring Methods 0.000 description 16
- 230000000052 comparative effect Effects 0.000 description 14
- 229910021645 metal ion Inorganic materials 0.000 description 11
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 10
- GETQZCLCWQTVFV-UHFFFAOYSA-N trimethylamine Chemical compound CN(C)C GETQZCLCWQTVFV-UHFFFAOYSA-N 0.000 description 10
- 239000003054 catalyst Substances 0.000 description 8
- 239000006185 dispersion Substances 0.000 description 8
- 238000001132 ultrasonic dispersion Methods 0.000 description 8
- 229920006395 saturated elastomer Polymers 0.000 description 7
- 238000010586 diagram Methods 0.000 description 6
- 229910052782 aluminium Inorganic materials 0.000 description 5
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 5
- 229910021529 ammonia Inorganic materials 0.000 description 5
- 239000000463 material Substances 0.000 description 5
- 230000007935 neutral effect Effects 0.000 description 5
- 241000282414 Homo sapiens Species 0.000 description 4
- 238000004458 analytical method Methods 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 239000011148 porous material Substances 0.000 description 4
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 3
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 3
- 239000011593 sulfur Substances 0.000 description 3
- 229910052717 sulfur Inorganic materials 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 description 2
- LSDPWZHWYPCBBB-UHFFFAOYSA-N Methanethiol Chemical compound SC LSDPWZHWYPCBBB-UHFFFAOYSA-N 0.000 description 2
- 125000003277 amino group Chemical group 0.000 description 2
- 229910001431 copper ion Inorganic materials 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 2
- 239000013110 organic ligand Substances 0.000 description 2
- 230000003068 static effect Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 125000003396 thiol group Chemical group [H]S* 0.000 description 2
- 238000012876 topography Methods 0.000 description 2
- QMMFVYPAHWMCMS-UHFFFAOYSA-N Dimethyl sulfide Chemical compound CSC QMMFVYPAHWMCMS-UHFFFAOYSA-N 0.000 description 1
- 206010019233 Headaches Diseases 0.000 description 1
- 206010028813 Nausea Diseases 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 238000004887 air purification Methods 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006065 biodegradation reaction Methods 0.000 description 1
- 238000004364 calculation method Methods 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000002131 composite material Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 239000000356 contaminant Substances 0.000 description 1
- 238000010411 cooking Methods 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- 238000003795 desorption Methods 0.000 description 1
- 201000010099 disease Diseases 0.000 description 1
- 208000037265 diseases, disorders, signs and symptoms Diseases 0.000 description 1
- 230000002526 effect on cardiovascular system Effects 0.000 description 1
- 238000000921 elemental analysis Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 239000000383 hazardous chemical Substances 0.000 description 1
- 231100000869 headache Toxicity 0.000 description 1
- 238000005470 impregnation Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 230000008693 nausea Effects 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 238000006479 redox reaction Methods 0.000 description 1
- 239000000523 sample Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
Classifications
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/45—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
- C04B41/50—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials
- C04B41/5076—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials with masses bonded by inorganic cements
-
- 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
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
- B01J21/10—Magnesium; Oxides or hydroxides thereof
-
- 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
- B01J23/02—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the alkali- or alkaline earth metals or beryllium
-
- 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
- B01J23/06—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of zinc, cadmium or mercury
-
- 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
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/72—Copper
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- B01J35/56—
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- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/009—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone characterised by the material treated
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/45—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements
- C04B41/50—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials
- C04B41/5076—Coating or impregnating, e.g. injection in masonry, partial coating of green or fired ceramics, organic coating compositions for adhering together two concrete elements with inorganic materials with masses bonded by inorganic cements
- C04B41/5089—Silica sols, alkyl, ammonium or alkali metal silicate cements
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B41/00—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone
- C04B41/80—After-treatment of mortars, concrete, artificial stone or ceramics; Treatment of natural stone of only ceramics
- C04B41/81—Coating or impregnation
- C04B41/85—Coating or impregnation with inorganic materials
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Abstract
The invention discloses a catalytic honeycomb ceramic material and a preparation method and application thereof, wherein the preparation method comprises the following steps: s1, pretreatment of a honeycomb ceramic substrate: soaking the honeycomb ceramic substrate into boiled nitric acid solution for boiling, then taking out and washing with water, and performing first heat treatment in an aerobic atmosphere to obtain a pretreated honeycomb ceramic substrate; s2, preparing a coating liquid: mixing soluble metal salt, pore-forming agent and stabilizing auxiliary agent with water-soluble adhesive to obtain coating liquid; s3, coating the surface of the honeycomb ceramic substrate: and (2) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2), taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing secondary heat treatment in an aerobic atmosphere until the weight is constant, thus obtaining the catalytic honeycomb ceramic material. The catalytic honeycomb ceramic material prepared by the preparation method has excellent adsorption effect on peculiar smell pollutants.
Description
Technical Field
The invention belongs to the technical field of air purification, and particularly relates to a catalytic honeycomb ceramic material, and a preparation method and application thereof.
Background
The peculiar smell pollutant which is one of the seven environmental hazards mainly consists of nitrogen-containing and sulfur-containing compounds such as ammonia, amine, methyl mercaptan, methyl sulfide and the like, and amino groups, mercapto groups and the like in the molecular structures are easy to spread to a human body through air to directly stimulate the smell, so that headache, nausea and even cardiovascular related diseases of the human body are caused, and the production and the life of the human are greatly influenced. Meanwhile, the direct emission of peculiar smell pollutants can cause serious environmental pollution, and seriously threaten the living environment of human beings.
The current methods for purifying the peculiar smell pollutants mainly comprise an adsorption method, a condensation method, a catalytic oxidation method and a biodegradation method. Because the adsorption method has the advantages of simple operation, low energy consumption and the like, the current commercial peculiar smell air purifier usually utilizes adsorption materials to filter and remove the gas pollution, thereby achieving the purpose of removing the peculiar smell. However, the common adsorption material has the defects of low selectivity, poor adsorptivity, easy desorption after reaching adsorption saturation, secondary pollution and the like. Aiming at the problems, the finding of the integral peculiar smell removal material which has obvious effect and no secondary pollution has important practical significance.
Disclosure of Invention
The present invention aims to solve at least one of the technical problems existing in the prior art. Therefore, the invention provides a catalytic honeycomb ceramic material, a preparation method and application thereof, and the catalytic honeycomb ceramic material has an excellent adsorption effect on peculiar smell pollutants.
The technical aim of the invention is realized by the following technical scheme:
a preparation method of a catalytic honeycomb ceramic material comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: soaking the honeycomb ceramic substrate into boiled nitric acid solution for boiling, then taking out and washing with water, and performing first heat treatment in an aerobic atmosphere to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: mixing soluble metal salt, pore-forming agent and stabilizing auxiliary agent with water-soluble adhesive to obtain coating liquid;
s3, coating the surface of the honeycomb ceramic substrate: and (2) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2), taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing secondary heat treatment in an aerobic atmosphere until the weight is constant, thus obtaining the catalytic honeycomb ceramic material.
Preferably, in step S1, the volume concentration of the nitric acid solution is 8-15%.
Further preferably, in step S1, the volume concentration of the nitric acid solution is 10%.
Preferably, in step S1, the washing is to wash the honeycomb ceramic substrate with water to neutrality.
Preferably, in step S1, the cooking time is 5-20min.
Preferably, in step S1, the temperature of the first heat treatment is 250-350 ℃ and the treatment time is 2-4h.
Further preferably, in step S1, the temperature of the first heat treatment is 300 ℃ and the treatment time is 3 hours.
Preferably, in step S2, the soluble metal salt is at least one of copper chloride, zinc nitrate, magnesium chloride and calcium chloride.
Preferably, in step S2, the pore-forming agent is at least one of urea and sodium bicarbonate.
Preferably, in step S2, the stabilizing additive is at least one of ethylenediamine tetraacetic acid, ethylenediamine and glycine.
Preferably, in step S2, the water-soluble adhesive is one of an aluminum sol and a silica sol, and the mass percentage of the water-soluble adhesive is 20-40%.
Preferably, in step S2, the mixing means that the dispersion mixing is performed by ultrasonic waves in a stirring state, the ultrasonic dispersion time is 5-15min, and the stirring time is 25-35min.
Further preferably, in step S2, the mixing means that the dispersion mixing is performed by ultrasonic waves in a stirring state, the ultrasonic dispersion time is 10min, and the stirring time is 30min.
Preferably, in step S2, the concentration of each component in the coating solution is as follows: the concentration of the soluble metal salt is 0.1-1.2mol/L, the concentration of the pore-forming agent is 0.1-1.2mol/L, and the concentration of the stabilizing auxiliary agent is 0.8-9.6mol/L.
Preferably, in step S3, the time of the impregnation is 2 to 15 hours.
Preferably, in step S3, the temperature of the second heat treatment is 100-200 ℃ and the treatment time is 5-12h.
A catalytic honeycomb ceramic material is prepared by the preparation method.
The use of a catalytic honeycomb ceramic material as described above in the purification of contaminants.
The mechanism of the invention is as follows:
(1) After the honeycomb ceramic substrate is pretreated by the step S1, the surface of the honeycomb ceramic substrate can be corroded to form a richer pore structure, so that more attachment sites are provided for the subsequent deposition of metal ion active components;
(2) The method comprises the steps of dispersing soluble metal salt into a water-soluble adhesive and coating the soluble metal salt on the inner surface of a through pore canal of a honeycomb ceramic substrate, so that metal ion active components are firmly supported on the surface of the honeycomb ceramic substrate to form a catalyst coating; according to the theory of the hard and soft acid bases, metal ions in the catalyst coating can have strong chemical action with nitrogen-containing and sulfur-containing groups of peculiar smell molecules, so that the chemical bonds of amino groups, sulfhydryl groups and other groups are weakened or even broken, and the metal ions are converted into molecules without peculiar smell, thereby achieving the aim of removing the peculiar smell;
(3) The added stabilizing auxiliary agent is mainly a water-soluble organic ligand, and the organic ligand is introduced to carry out coordination bonding with metal ions, so that on one hand, the stability of the metal ions in the catalyst coating can be improved, and on the other hand, the oxidation potential of the metal ions can be improved, so that the metal ions can be more easily subjected to strong oxidation-reduction reaction with peculiar smell pollutants containing nitrogen and sulfur;
(4) The added pore-forming agent is heated and decomposed in the heat treatment process of the step S3, so that the catalyst coating becomes more porous, the contact probability and contact time of the metal ion active components in the catalyst coating and the peculiar smell pollutant gas molecules are improved, and the purification effect of the product is improved.
The beneficial effects of the invention are as follows:
(1) The honeycomb ceramic substrate material has the advantages of high mechanical strength, good thermal stability, easy industrial application and the like, so the prepared catalytic honeycomb ceramic material has good applicability and application popularization value.
(2) The preparation method is simple, and the catalyst coating with firm, thin and uniform load can be directly coated on the inner surface of the through hole of the honeycomb ceramic substrate, so that the wind resistance is not additionally increased.
(3) Compared with commercial honeycomb ceramics, the saturated adsorption capacity of the catalytic honeycomb ceramic product prepared by the preparation method for odor pollutants such as trimethylamine, ammonia and the like is greatly improved, and the purification effect is excellent.
Drawings
FIG. 1 is a physical view showing the appearance of a catalytic honeycomb ceramic material prepared in example 1 of the present invention;
FIG. 2 is an external physical view of the honeycomb ceramic material of comparative example 1 of the present invention;
FIG. 3 is a microscopic surface topography of the catalytic honeycomb ceramic material prepared in example 1 of the present invention under a scanning electron microscope;
FIG. 4 is a microscopic surface topography of the honeycomb ceramic material of comparative example 1 of the present invention under a scanning electron microscope;
FIG. 5 is a graph of the results of surface elemental analysis of the catalytic honeycomb ceramic material of example 1 as measured by a spectrometer;
fig. 6 is a graph showing the results of surface element analysis of the honeycomb ceramic material of comparative example 1 measured by an energy spectrometer.
Detailed Description
The invention will be further illustrated with reference to specific examples.
Example 1:
a preparation method of a catalytic honeycomb ceramic material comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: immersing a commercial honeycomb ceramic substrate with the specification of 50 x 20 x 10mm into a boiled nitric acid solution with the volume concentration of 10% for boiling for 10min, taking out, washing with water to be neutral, and carrying out heat treatment for 3h at the temperature of 300 ℃ in air atmosphere to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: adding copper chloride, urea and ethylenediamine tetraacetic acid into aluminum sol with the mass percentage of 20%, performing dispersion mixing by ultrasonic waves in a stirring state, wherein the ultrasonic dispersion time is 10min, the stirring time is 30min, and uniformly mixing to obtain a coating liquid, wherein the concentration of the copper chloride in the coating liquid is 0.8mol/L, the concentration of the urea is 0.5mol/L and the concentration of the ethylenediamine tetraacetic acid is 6.4mol/L;
s3, coating the surface of the honeycomb ceramic substrate: and (3) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2) for 10 hours, taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing heat treatment at 180 ℃ for 12 hours until the weight is constant, thus obtaining the catalytic honeycomb ceramic material.
The catalytic honeycomb ceramic material is prepared by the preparation method, a physical diagram of the catalytic honeycomb ceramic material is shown in fig. 1, a microscopic surface morphology diagram of the catalytic honeycomb ceramic material under a scanning electron microscope is shown in fig. 3, and an analysis result diagram obtained by analyzing surface elements of the catalytic honeycomb ceramic material by an energy spectrometer is shown in fig. 5.
Example 2:
a preparation method of a catalytic honeycomb ceramic material comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: immersing a commercial honeycomb ceramic substrate with the specification of 50 mm by 20 mm by 10mm into a boiled nitric acid solution with the volume concentration of 10% for boiling for 5min, taking out, washing with water to be neutral, and carrying out heat treatment for 3h at the temperature of 300 ℃ in air atmosphere to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: adding zinc nitrate, sodium bicarbonate and glycine into silica sol with the mass percentage of 40%, carrying out dispersion mixing by ultrasonic waves in a stirring state, wherein the ultrasonic dispersion time is 10min, the stirring time is 30min, and uniformly mixing to obtain a coating liquid, wherein the concentration of zinc nitrate in the coating liquid is 1.2mol/L, the concentration of sodium bicarbonate is 1.2mol/L, and the concentration of glycine is 9.6mol/L;
s3, coating the surface of the honeycomb ceramic substrate: and (3) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2) for 2 hours, taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing heat treatment at 120 ℃ for 12 hours until the weight is constant, thus obtaining the catalytic honeycomb ceramic material.
A catalytic honeycomb ceramic material is prepared by the preparation method.
Example 3:
a preparation method of a catalytic honeycomb ceramic material comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: immersing a commercial honeycomb ceramic substrate with the specification of 50 x 20 x 10mm into a boiled nitric acid solution with the volume concentration of 10% for boiling for 20min, taking out, washing with water to be neutral, and carrying out heat treatment for 3h at the temperature of 300 ℃ in air atmosphere to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: adding calcium chloride, sodium bicarbonate and ethylenediamine into aluminum sol with the mass percentage of 20%, performing dispersion mixing by ultrasonic waves in a stirring state, wherein the ultrasonic dispersion time is 10min, the stirring time is 30min, and uniformly mixing to obtain a coating liquid, wherein the concentration of the calcium chloride in the coating liquid is 0.9mol/L, the concentration of the sodium bicarbonate is 1.2mol/L and the concentration of the ethylenediamine is 8.1mol/L;
s3, coating the surface of the honeycomb ceramic substrate: and (3) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2) for 10 hours, taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing heat treatment at 120 ℃ for 12 hours until the weight is constant, thus obtaining the catalytic honeycomb ceramic material.
A catalytic honeycomb ceramic material is prepared by the preparation method.
Example 4:
a preparation method of a catalytic honeycomb ceramic material comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: immersing a commercial honeycomb ceramic substrate with the specification of 50 mm by 20 mm by 10mm into a boiled nitric acid solution with the volume concentration of 10% for boiling for 15min, taking out, washing with water to be neutral, and carrying out heat treatment for 3h at the temperature of 300 ℃ in air atmosphere to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: adding magnesium chloride, urea and ethylenediamine tetraacetic acid into silica sol with the mass percentage of 40%, performing dispersion mixing by ultrasonic waves in a stirring state, wherein the ultrasonic dispersion time is 10min, the stirring time is 30min, and uniformly mixing to obtain a coating liquid, wherein the concentration of the magnesium chloride in the coating liquid is 1.0mol/L, the concentration of the urea is 0.3mol/L and the concentration of the ethylenediamine tetraacetic acid is 9.6mol/L;
s3, coating the surface of the honeycomb ceramic substrate: and (3) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2) for 2 hours, taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing heat treatment at 200 ℃ for 5 hours until the weight is constant, thus obtaining the catalytic honeycomb ceramic material.
A catalytic honeycomb ceramic material is prepared by the preparation method.
Comparative example 1: (compared with example 1, only the commercial honeycomb ceramics were heat-treated)
A preparation method of a honeycomb ceramic material comprises the following steps: and (3) carrying out heat treatment on the commercial honeycomb ceramics with the specification of 50-10 mm in an air atmosphere at 300 ℃ for 3 hours to obtain the honeycomb ceramics.
A honeycomb ceramic material is prepared by the preparation method. The physical diagram of the honeycomb ceramic material is shown in fig. 2, the microscopic surface morphology diagram of the honeycomb ceramic material under a scanning electron microscope is shown in fig. 4, and the analysis result diagram obtained by analyzing the surface elements of the honeycomb ceramic material by an energy spectrometer is shown in fig. 6.
Comparative example 2: (compared with example 1, the commercial honeycomb ceramics were not immersed in a boiled nitric acid solution and were boiled in the same manner as in the other steps)
A preparation method of a catalytic honeycomb ceramic material comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: carrying out heat treatment on a commercial honeycomb ceramic substrate with the specification of 50-10 mm at the temperature of 300 ℃ in an air atmosphere for 3 hours to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: adding copper chloride, urea and ethylenediamine tetraacetic acid into aluminum sol with the mass percentage of 20%, performing dispersion mixing by ultrasonic waves in a stirring state, wherein the ultrasonic dispersion time is 10min, the stirring time is 30min, and uniformly mixing to obtain a coating liquid, wherein the concentration of the copper chloride in the coating liquid is 0.8mol/L, the concentration of the urea is 0.5mol/L and the concentration of the ethylenediamine tetraacetic acid is 6.4mol/L;
s3, coating the surface of the honeycomb ceramic substrate: and (3) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2) for 10 hours, taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing heat treatment at 180 ℃ for 12 hours until the weight is constant, thus obtaining the catalytic honeycomb ceramic material.
A catalytic honeycomb ceramic material is prepared by the preparation method.
Comparative example 3: (As compared with example 1, the same procedure was carried out except that no stabilizing additive was added to the coating liquid)
A preparation method of a catalytic honeycomb ceramic material comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: immersing a commercial honeycomb ceramic substrate with the specification of 50 x 20 x 10mm into a boiled nitric acid solution with the volume concentration of 10% for boiling for 10min, taking out, washing with water to be neutral, and carrying out heat treatment for 3h at the temperature of 300 ℃ in air atmosphere to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: adding copper chloride and urea into aluminum sol with the mass percent of 20%, carrying out dispersion mixing by ultrasonic waves in a stirring state, wherein the ultrasonic dispersion time is 10min, the stirring time is 30min, and uniformly mixing to obtain a coating liquid, wherein the concentration of the copper chloride in the coating liquid is 0.8mol/L, and the concentration of the urea is 0.5mol/L;
s3, coating the surface of the honeycomb ceramic substrate: and (3) immersing the honeycomb ceramic substrate obtained in the step (S1) in the coating liquid obtained in the step (S2) for 10 hours, taking out the honeycomb ceramic substrate after immersion, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing heat treatment at 180 ℃ for 12 hours until the weight is constant, thus obtaining the catalytic honeycomb ceramic material.
A catalytic honeycomb ceramic material is prepared by the preparation method.
Test example:
the catalytic honeycomb ceramic materials prepared in examples 1 to 4 and the honeycomb ceramic materials prepared in comparative examples 1 to 3 were respectively subjected to static saturation adsorption test of odor pollutants at room temperature and normal pressure, and Trimethylamine (TMA) and ammonia were used as probe molecules, and the results are shown in table 1.
The calculation formula of the saturated adsorption capacity is as follows: saturated adsorption capacity= (product mass after adsorption saturation-product mass before adsorption)/product volume
Table 1: results of static saturation adsorption test for odor pollutants
As can be seen from Table 1, under the conditions of room temperature and normal pressure, the saturated adsorption capacity of the catalytic honeycomb ceramic material prepared by the preparation method is 70.2-82.1g/L for trimethylamine, the saturated adsorption capacity for ammonia is 72.3-81.7g/L, the saturated adsorption capacity of the honeycomb ceramic material of comparative example 1 for trimethylamine is only 3.3g/L, the saturated adsorption capacity for ammonia is only 6.5g/L, and the catalytic honeycomb ceramic material of the invention is greatly superior to the adsorption effect of the honeycomb ceramic material of comparative example 1, and has excellent peculiar smell pollutant purifying and removing capacity; meanwhile, as can be seen from comparative examples 1 and 2, when commercial honeycomb ceramics are not soaked in boiled nitric acid solution for boiling, the adsorption performance of the finally prepared honeycomb ceramics material is obviously reduced; as is clear from comparative examples 1 and 3, when no stabilizing additive is added to the coating liquid, the adsorption performance of the finally produced honeycomb ceramic material is significantly lowered.
In addition, as can be seen from fig. 1 and 2, the catalytic honeycomb ceramic material obtained in example 1 has no significant change in overall appearance, but changes in color from pale yellow to pale green, compared with the honeycomb ceramic material of comparative example 1, indicating that the introduced metal ion active components (copper ions) are uniformly distributed on the surface of the honeycomb ceramic substrate, and the formed catalyst coating is very thin, without causing additional windage in use; further, as can be seen from the surface micro-morphology graphs of fig. 3 and 4, the catalytic honeycomb ceramic material obtained in example 1 has a relatively coarse surface and a relatively rich pore structure, and the nano particles of the metal ion active component are uniformly distributed in the porous coating structure, so that adsorption enrichment and catalytic oxidation purification of the odor molecules in the catalytic coating are facilitated, while the surface of the honeycomb ceramic material of comparative example 1 is very smooth and has a small number of pores; meanwhile, as can be seen from the surface element analysis results of FIGS. 5 and 6, the honeycomb ceramic material of comparative example 1 is composed mainly of MgO, al 2 O 3 And SiO 2 Composite oxidation composition; the presence of Cu element was also observed in the catalytic honeycomb ceramic material obtained in example 1, demonstrating that the metallic copper ion active component had entered the catalyst coating on the honeycomb ceramic substrate surface. The above test was repeated for the catalytic honeycomb ceramic materials prepared in examples 2 to 4, and test results similar to those in example 1 were obtained, and will not be repeated here.
The above examples are preferred embodiments of the present invention, but the embodiments of the present invention are not limited to the above examples, and any other changes, modifications, substitutions, combinations, and simplifications that do not depart from the spirit and principle of the present invention should be made in the equivalent manner, and the embodiments are included in the protection scope of the present invention.
Claims (5)
1. A preparation method of a catalytic honeycomb ceramic material is characterized by comprising the following steps: the method comprises the following steps:
s1, pretreatment of a honeycomb ceramic substrate: soaking the honeycomb ceramic substrate into boiled nitric acid solution for boiling, then taking out and washing with water, and performing first heat treatment in an aerobic atmosphere to obtain a pretreated honeycomb ceramic substrate;
s2, preparing a coating liquid: mixing soluble metal salt, pore-forming agent and stabilizing auxiliary agent with water-soluble adhesive to obtain coating liquid;
s3, coating the surface of the honeycomb ceramic substrate: soaking the honeycomb ceramic substrate obtained in the step S1 in the coating liquid obtained in the step S2, taking out the honeycomb ceramic substrate after soaking, purging the redundant coating liquid in the through holes of the honeycomb ceramic substrate, and performing secondary heat treatment in an aerobic atmosphere until the weight is constant, thus obtaining the catalytic honeycomb ceramic material;
in the step S1, the volume concentration of the nitric acid solution is 8-15%, the boiling time is 5-20min, the temperature of the first heat treatment is 250-350 ℃, and the treatment time is 2-4h; in the step S2, the stabilizing additive is at least one of ethylenediamine tetraacetic acid, ethylenediamine and glycine, and the soluble metal salt is at least one of copper chloride, zinc nitrate, magnesium chloride and calcium chloride; in the step S3, the temperature of the second heat treatment is 100-200 ℃ and the treatment time is 5-12h.
2. The method for preparing the catalytic honeycomb ceramic material according to claim 1, wherein the method comprises the following steps: in step S2, the pore-forming agent is at least one of urea and sodium bicarbonate.
3. The method for preparing the catalytic honeycomb ceramic material according to claim 1, wherein the method comprises the following steps: in the step S3, the soaking time is 2-15h.
4. A catalytic honeycomb ceramic material, characterized by: a preparation method according to any one of claims 1 to 3.
5. The use of the catalytic honeycomb ceramic material of claim 4 for the purification of pollutants.
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