CN113797925B - Formaldehyde removal catalyst and preparation method and application thereof - Google Patents
Formaldehyde removal catalyst and preparation method and application thereof Download PDFInfo
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- CN113797925B CN113797925B CN202111162197.5A CN202111162197A CN113797925B CN 113797925 B CN113797925 B CN 113797925B CN 202111162197 A CN202111162197 A CN 202111162197A CN 113797925 B CN113797925 B CN 113797925B
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- WSFSSNUMVMOOMR-UHFFFAOYSA-N Formaldehyde Chemical compound O=C WSFSSNUMVMOOMR-UHFFFAOYSA-N 0.000 title claims abstract description 249
- 239000003054 catalyst Substances 0.000 title claims abstract description 149
- 238000002360 preparation method Methods 0.000 title claims abstract description 19
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 claims abstract description 64
- 239000011148 porous material Substances 0.000 claims abstract description 28
- 239000003638 chemical reducing agent Substances 0.000 claims description 39
- 238000000034 method Methods 0.000 claims description 34
- 239000006185 dispersion Substances 0.000 claims description 23
- 238000001035 drying Methods 0.000 claims description 21
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 20
- 150000002696 manganese Chemical class 0.000 claims description 18
- 238000000227 grinding Methods 0.000 claims description 17
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- 238000006722 reduction reaction Methods 0.000 claims description 10
- 238000001914 filtration Methods 0.000 claims description 9
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 8
- 239000011572 manganese Substances 0.000 claims description 8
- OQVYMXCRDHDTTH-UHFFFAOYSA-N 4-(diethoxyphosphorylmethyl)-2-[4-(diethoxyphosphorylmethyl)pyridin-2-yl]pyridine Chemical compound CCOP(=O)(OCC)CC1=CC=NC(C=2N=CC=C(CP(=O)(OCC)OCC)C=2)=C1 OQVYMXCRDHDTTH-UHFFFAOYSA-N 0.000 claims description 7
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 claims description 6
- 238000000498 ball milling Methods 0.000 claims description 6
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- PWHULOQIROXLJO-UHFFFAOYSA-N Manganese Chemical compound [Mn] PWHULOQIROXLJO-UHFFFAOYSA-N 0.000 claims description 5
- 229910052748 manganese Inorganic materials 0.000 claims description 5
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 4
- WQZGKKKJIJFFOK-VFUOTHLCSA-N beta-D-glucose Chemical compound OC[C@H]1O[C@@H](O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-VFUOTHLCSA-N 0.000 claims description 4
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- NJVOHKFLBKQLIZ-UHFFFAOYSA-N (2-ethenylphenyl) prop-2-enoate Chemical compound C=CC(=O)OC1=CC=CC=C1C=C NJVOHKFLBKQLIZ-UHFFFAOYSA-N 0.000 claims description 3
- 238000004026 adhesive bonding Methods 0.000 claims description 3
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
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- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 2
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- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 description 2
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- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 description 2
- 239000012855 volatile organic compound Substances 0.000 description 2
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- CETPSERCERDGAM-UHFFFAOYSA-N ceric oxide Chemical compound O=[Ce]=O CETPSERCERDGAM-UHFFFAOYSA-N 0.000 description 1
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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
- B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/32—Manganese, technetium or rhenium
- B01J23/34—Manganese
-
- 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
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/40—Catalysts, in general, characterised by their form or physical properties characterised by dimensions, e.g. grain size
-
- 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
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/60—Catalysts, in general, characterised by their form or physical properties characterised by their surface properties or porosity
- B01J35/64—Pore diameter
- B01J35/647—2-50 nm
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2255/00—Catalysts
- B01D2255/20—Metals or compounds thereof
- B01D2255/207—Transition metals
- B01D2255/2073—Manganese
-
- 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
- B01D2257/708—Volatile organic compounds V.O.C.'s
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Environmental & Geological Engineering (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Catalysts (AREA)
Abstract
The invention provides a formaldehyde removal catalyst, a preparation method and application thereof, wherein the formaldehyde removal catalyst comprises the following components: and the aperture of the manganese dioxide is d 1, wherein d 1 is satisfied, and d 1 is more than or equal to 5nm and less than or equal to 50nm. The formaldehyde removal catalyst according to the specific embodiment of the invention comprises a manganese dioxide catalyst which is nano-sized particles, wherein the aperture of the manganese dioxide is d1, and d1 is more than or equal to 5nm and less than or equal to 50nm; the catalyst can be used for catalyzing and oxidizing formaldehyde at room temperature, the pore structure in the catalyst increases the specific surface area of the catalyst, is favorable for adsorption and anchoring of formaldehyde molecules in the catalyst pores, and improves the oxidative decomposition performance of formaldehyde.
Description
Technical Field
The invention relates to the field of air purification, in particular to a formaldehyde removal catalyst and a preparation method and application thereof.
Background
With the rapid development of the economic society, the global air pollution problem is increasingly prominent, and the global air pollution problem is highly valued by governments around the world. The problem of indoor air pollution closely related to human health, life and home is one of the key problems to be solved. Formaldehyde is a typical contaminant of indoor and outdoor air, and is mainly derived from furniture, building materials and household products. In addition, formaldehyde protectants are also included in cosmetics, photolithography chemicals, preservatives, textiles, and paint coatings. Formaldehyde is a class of carcinogens that was published by the world health organization international cancer research institute at 10, 27, 2017. They can chemically react with hydroxyl radicals, nitric acid radicals, ozone to produce aldehydes, ketones, and carboxylic acids. Formaldehyde is also a toxic and harmful water pollutant, is easily dissolved in water, is easily absorbed in the respiratory tract and intestines and stomach of a human body, can obviously reduce the immunity of the human body, causes various respiratory system and digestive tract diseases (such as pneumonia, pulmonary edema, abdominal pain, convulsion and the like), and especially seriously damages the physical and mental health of pregnant women and children. Even a small amount (0.5 ppm) of formaldehyde can affect human health. Research shows that most of the time of people spends in the indoor environment, the indoor ventilation rate is low, and meanwhile, a strong formaldehyde release source exists, so that the formaldehyde content in the indoor environment is widely focused by people.
Aiming at the current problem, there are mainly two techniques for reducing the concentration of formaldehyde in air: physical adsorption and catalytic oxidation. Physical adsorption is mainly to anchor formaldehyde molecules in pore channels of a material by using activated carbon or oxide with a high specific surface and developed micropore structure, so that the concentration of formaldehyde in the air is reduced. However, due to the weak interaction force between formaldehyde molecules and the adsorbent, adsorbed formaldehyde molecules have the risk of being desorbed again from the pore channels. In addition, in order to restore the adsorption performance of the material, the desorption and regeneration treatment of the material is required at regular time. Unlike physical adsorption, catalytic oxidation is the direct conversion of formaldehyde molecules adsorbed on a surface into harmless water and carbon dioxide using a catalyst. In general, oxide or activated carbon supported noble metal catalysts are capable of decomposing formaldehyde into carbon dioxide and water at room temperature, such as Pt/TiO 2,Pt/MnO2-CeO2,Au/CeO2,Pd/TiO2, and the like. However, noble metal catalysts are expensive to produce, limiting their wide range of applications. Among various non-noble metal catalysts, manganese dioxide is favored by researchers because of its high catalytic activity and simple and easy popularization of the preparation method.
In the prior art, some formaldehyde removal catalysts have complex preparation methods and low catalytic efficiency or require high-temperature roasting treatment, for example, CN109201044B discloses a preparation method of a potassium-doped manganese dioxide catalyst and application of the catalyst in purifying Volatile Organic Compounds (VOCs). The method is characterized in that the method comprises the following steps: the first step is to obtain gamma-MnO 2 by adopting a precipitation method, and the second step is to prepare the K+ doped gamma-MnO 2 catalyst by adopting an isovolumetric impregnation method. The operation process is complex and complicated, and the catalyst needs to be activated at a higher temperature, so that the manufacturing cost of the catalyst can be increased, and the wide production of the catalyst is not facilitated. CN110523267a discloses a formaldehyde decomposition catalyst, formaldehyde catalytic decomposition felt and manufacturing method, the formaldehyde decomposition catalyst is mainly composed of submicron-micron petal-shaped particles formed by delta crystal form MnO 2. The particle size is too large, and the adsorption and reaction opportunities of formaldehyde molecules on the surface of the catalyst are reduced. CN111437874a discloses a formaldehyde-removing catalyst, its preparation method and application. The formaldehyde removal catalyst is loaded on a porous carrier (one or more of ZSM-5 molecular sieve, MCM-41 molecular sieve and silicon dioxide) and can be used for catalyzing and oxidizing formaldehyde at room temperature. The catalyst material is loaded on the porous carrier, the specific surface area of the catalyst material is enhanced, the catalytic oxidation of formaldehyde is facilitated, in addition, the formaldehyde stays in the porous material for a long time, and the complete catalytic decomposition of formaldehyde is facilitated. However, the preparation requires the provision of an additional porous material and the synthesis at a certain temperature, and the resulting catalyst precursor also requires the calcination treatment at a certain temperature, which certainly increases the manufacturing cost.
Disclosure of Invention
The present invention aims to solve at least one of the technical problems existing in the prior art. Therefore, an object of the present invention is to provide a formaldehyde removal catalyst capable of efficiently removing formaldehyde at room temperature.
Another object of the invention is to propose a method for preparing the formaldehyde-removing catalyst.
A third object of the present invention is to propose the use of a formaldehyde removal catalyst.
In one aspect of the present invention, the present invention provides a formaldehyde removal catalyst comprising: and the aperture of the manganese dioxide is d 1, wherein d 1 is satisfied, and d 1 is more than or equal to 5nm and less than or equal to 50nm.
The formaldehyde removal catalyst according to the specific embodiment of the invention comprises a manganese dioxide catalyst which is nano-sized particles, wherein the aperture of the manganese dioxide is d1, and d1 is more than or equal to 5nm and less than or equal to 50nm; the catalyst can be used for catalyzing and oxidizing formaldehyde at room temperature, the pore structure in the catalyst increases the specific surface area of the catalyst, is favorable for adsorption and anchoring of formaldehyde molecules in the catalyst pores, and improves the oxidative decomposition performance of formaldehyde.
According to some embodiments of the invention, the catalyst comprises manganese dioxide, the manganese dioxide comprising w as a percentage of the total mass of the catalyst, wherein w satisfies that w > 95%.
According to an embodiment of another aspect of the present invention, the present invention provides a method for preparing a formaldehyde removal catalyst, comprising the steps of:
step one, reduction reaction: dropwise adding a reducing agent into the manganese salt-containing solution, and reacting for a period of time;
Step two, grinding and dispersing: grinding the reaction liquid obtained in the step one to obtain a dispersion liquid containing the catalyst, and drying the dispersion liquid to obtain the formaldehyde-removing catalyst.
According to an embodiment of the third aspect of the present invention, the present invention proposes the use of the formaldehyde removal catalyst.
According to some embodiments of the present invention, a formaldehyde-removing semi-finished component is provided, comprising a microporous medium having the catalyst attached to the surface or inside the pores.
According to some embodiments of the invention, the microporous medium is one or more of foam sponge, PET, carbon cloth.
According to some embodiments of the invention, the microporous medium has a pore size d 2, wherein d 2 is satisfied and d 2 > 60 μm.
According to some embodiments of the present invention, the present invention provides a method for manufacturing a formaldehyde-removing semi-finished product assembly, comprising the steps of:
step one, reduction reaction: dropwise adding a reducing agent into the manganese salt-containing solution, and reacting for a period of time;
step two, grinding and dispersing: grinding the reaction liquid obtained in the step one to obtain a dispersion liquid containing the catalyst;
step three, gluing load: and (3) adding an adhesive into the dispersion liquid obtained in the step (II), then adding a microporous carrier, and drying to obtain the formaldehyde-removing semi-finished product component.
According to some embodiments of the invention, in step three, comprising immersing the catalyst-containing dispersion on a microporous support.
According to some embodiments of the invention, in the third step, the adhesive is further added into the dispersion liquid obtained in the second step to obtain the cement, then the micropore medium is immersed in the cement, and after extrusion, the cement is dried to obtain the formaldehyde-removing semi-finished product component.
According to some embodiments of the invention, in step three, the adhesive comprises one or more of polyurethane, styrene-acrylate, polyacrylate, and polyesteramide.
According to some embodiments of the invention, the molar ratio of manganese-containing salt to reducing agent in step one is: 0.5:1-10:1; preferably, it is: 2.2:1.
According to some embodiments of the invention, the manganese salt-containing solution in step one includes potassium permanganate and/or potassium manganate.
According to some embodiments of the invention, the manganese salt-containing solution in the first step is obtained by adding potassium permanganate and/or potassium manganate to water at room temperature or 20-55 ℃ for dissolution.
According to some embodiments of the invention, the reducing agent in step one is an organic reducing agent, preferably the organic reducing agent comprises one or more of glucose, absolute ethanol and glycerol.
According to some embodiments of the invention, the reduction reaction in step one is stirring the manganese salt-containing solution at 25-45 ℃ for 20-50 minutes; adding the organic reducing agent, heating to 50-80 ℃, and reacting for 1-4 hours to obtain brown or black suspension.
According to some embodiments of the invention, step one further comprises suction filtering the brown or black suspension, washing with water for 2-5 times, and drying to obtain brown or black sediment.
According to some embodiments of the invention, the grinding in the second step is to mix the brown or black sediment and water in a weight ratio of 1:2-1:1, and ball mill for 5-8 hours to obtain a dispersion of the catalyst containing manganese dioxide.
According to some embodiments of the invention, the speed of dropping the reducing agent in the first step is 10g/min to 80g/min; preferably 30g/min to 70g/min.
According to some embodiments of the invention, the milling in step two is water-added ball milling.
According to some embodiments of the invention, the drying comprises: drying at 90-120 deg.c for 8-16 hr; preferably 12 hours.
According to some embodiments of the present invention, a screen assembly is provided, including the formaldehyde-scavenging semi-finished product assembly.
According to some embodiments of the present invention, an air purifier is provided, including the filter assembly.
According to some embodiments of the present invention, an air conditioner is provided, including the air purifier.
According to some embodiments of the invention, a new wind system is provided, including the air purifier.
Additional aspects and advantages of the invention will be set forth in part in the description which follows, and in part will be obvious from the description, or may be learned by practice of the invention.
Drawings
The foregoing and/or additional aspects and advantages of the invention will become apparent and may be better understood from the following description of embodiments taken in conjunction with the accompanying drawings in which:
FIG. 1 is an XRD pattern of a formaldehyde removal catalyst of example 4 of the present invention;
FIG. 2 is a graph showing pore size distribution of formaldehyde removal catalyst of example 4 of the present invention;
FIG. 3 is an XPS spectrum of Mn 4+ of the formaldehyde removal catalyst of example 4 of the present invention;
FIG. 4 is an SEM image of a formaldehyde-removing catalyst of example 4 of the invention.
Detailed Description
Embodiments of the present invention will be described in detail below, by way of example with reference to the accompanying drawings.
The formaldehyde removal catalyst of the present invention, and the preparation method and application thereof are described below according to specific examples of the present invention. In one aspect of the present invention, the present invention provides a formaldehyde removal catalyst comprising: manganese dioxide, wherein the aperture of the manganese dioxide is d 1, and d 1 is satisfied, and d 1 is more than or equal to 5nm and less than or equal to 50nm.
The formaldehyde removal catalyst according to the specific embodiment of the invention comprises a manganese dioxide catalyst which is nano-sized particles, wherein the aperture of manganese dioxide is d1, d1 is satisfied, and d1 is more than or equal to 5nm and less than or equal to 50nm; the catalyst can be used for catalyzing and oxidizing formaldehyde at room temperature, the pore structure in the catalyst increases the specific surface area of the catalyst, is favorable for adsorption and anchoring of formaldehyde molecules in the catalyst pores, and improves the oxidative decomposition performance of formaldehyde.
According to some embodiments of the invention, the catalyst comprises manganese dioxide, the manganese dioxide comprising w, wherein w is satisfied, w > 95% of the total mass of the catalyst.
According to the formaldehyde removal catalyst provided by the embodiment of the invention, formaldehyde can be rapidly decomposed into nontoxic carbon dioxide and water at room temperature, the initial FCADR is 53.36m 3/h, the formaldehyde removal catalyst can be applied to an air filtration system, and the application range of the powder catalyst is greatly widened.
According to an embodiment of another aspect of the present invention, the present invention provides a method for preparing a formaldehyde removal catalyst, comprising the steps of:
step one, reduction reaction: dropwise adding a reducing agent into the manganese salt-containing solution, and reacting for a period of time;
Step two, grinding and dispersing: grinding the reaction liquid obtained in the step one to obtain a dispersion liquid containing the catalyst, and drying the dispersion liquid to obtain the formaldehyde-removing catalyst.
According to the preparation method of the formaldehyde-removing catalyst, disclosed by the embodiment of the invention, the preparation method is simple and convenient to operate, the requirement on synthesis equipment is low, the used raw materials are low and are easy to obtain, the obtained catalyst does not need to be subjected to a high-temperature activation process, the problem of high cost of noble metal catalyst synthesis is effectively avoided, the requirement on equipment is reduced, and the preparation method can be widely applied to industrial production.
According to an embodiment of the third aspect of the present invention, the present invention proposes an application of a formaldehyde removal catalyst to an air filtration system.
According to some embodiments of the present invention, a formaldehyde-removing semi-finished component is provided that includes a microporous medium having a catalyst attached to a surface or inside a channel.
According to some embodiments of the invention, the microporous medium is one or more of foam sponge, PET, carbon cloth.
According to some embodiments of the invention, the microporous medium has a pore size d 2, wherein d 2 is satisfied and d 2 > 60 μm.
The formaldehyde-removing catalyst comprises manganese dioxide, wherein the aperture of the manganese dioxide is d 1, d 1 is more than or equal to 5nm and less than or equal to 1 and less than or equal to 50nm; the manganese dioxide catalyst and the micropore medium are manufactured into a filter screen component through ball milling, dipping, extrusion and other processes, and can be applied to an air purifier, an air conditioner and a fresh air system. The catalyst is loaded in the pore canal of the microporous carrier, the pore diameter of the microporous carrier medium is d 2, wherein d 2 is satisfied, and d 2 is more than 60 mu m.
The formaldehyde removal catalyst according to the specific embodiment of the invention comprises a manganese dioxide catalyst which is nano-sized particles, can be used for catalyzing and oxidizing formaldehyde at room temperature, has an internal pore structure which increases the specific surface area of the catalyst, is beneficial to adsorption and anchoring of formaldehyde molecules in the catalyst pores, and improves the oxidative decomposition performance of formaldehyde. The microporous medium contains one or more of foam sponge, PET, carbon-sandwiched cloth and active carbon, which is favorable for supporting the catalyst and facilitating the application of the catalyst.
According to some embodiments of the present invention, the present invention provides a method for manufacturing a formaldehyde-removing semi-finished product assembly, comprising the steps of:
step one, reduction reaction: dropwise adding a reducing agent into the manganese salt-containing solution, and reacting for a period of time;
step two, grinding and dispersing: grinding the reaction liquid obtained in the step one to obtain a dispersion liquid containing the catalyst;
step three, gluing load: and (3) adding an adhesive into the dispersion liquid obtained in the step (II), then adding a microporous carrier, and drying to obtain the formaldehyde-removing semi-finished product component.
According to the preparation method of the formaldehyde-removing catalyst, disclosed by the embodiment of the invention, the formaldehyde-removing catalyst is attached to the surface and the inside of the pores of the porous material by adopting an impregnation and extrusion process, so that the dispersibility of the catalyst can be improved, and the agglomeration problem of catalyst particles can be effectively inhibited. The porous materials such as sponge or PET with low wind resistance and good toughness are adopted, so that the porous materials are beneficial to being assembled into a filtering system; and simultaneously, the capability of removing formaldehyde is improved.
According to some embodiments of the invention, in step three, comprising immersing the dispersion comprising the catalyst on a microporous support.
According to some embodiments of the invention, in the third step, the adhesive is further added into the dispersion liquid obtained in the second step to obtain the cement, then the micropore medium is immersed in the cement, and after extrusion, the cement is dried to obtain the formaldehyde-removing semi-finished product component.
According to some embodiments of the invention, in step three, the adhesive comprises one or more of polyurethane, styrene-acrylate, polyacrylate, and polyesteramide.
According to some embodiments of the invention, the molar ratio of manganese salt to reducing agent in step one is: 0.5:1-10:1; preferably, it is: 2.2:1.
According to some embodiments of the invention, the manganese salt-containing solution in step one includes potassium permanganate and/or potassium manganate.
According to some embodiments of the invention, the manganese salt-containing solution of step one is obtained by adding potassium permanganate and/or potassium manganate to water at room temperature or 20-55 ℃ for dissolution.
According to some embodiments of the invention, the reducing agent in step one is an organic reducing agent, preferably the organic reducing agent comprises one or more of glucose, absolute ethanol and glycerol.
According to the preparation method of the formaldehyde-removing catalyst, the catalyst containing 10-50 nm holes is obtained in situ by adopting the organic reducing agent as the pore-forming agent, no additional pore-forming agent is needed, the operation process is simpler, and the cost is reduced. Meanwhile, the anchoring effect of the catalyst holes is beneficial to the reaction of formaldehyde molecules on the surface of the catalyst and in the pore channels, so that the contact opportunity of the formaldehyde molecules and the catalyst is greatly improved, and the formaldehyde removal performance of the catalyst is improved.
According to some embodiments of the invention, in the first step, the reduction reaction is that the manganese salt-containing solution is stirred for 20 to 50 minutes at 25 to 45 ℃; adding organic reducer, heating to 50-80 deg.C, reacting for 1-4 hours to obtain brown or black suspension.
According to some embodiments of the invention, step one further comprises suction filtering the brown or black suspension, washing with water for 2-5 times, and drying to obtain brown or black sediment.
According to some embodiments of the invention, grinding in the second step is to obtain a dispersion of the catalyst containing manganese dioxide after mixing and ball milling for 5-8 hours, wherein the weight ratio of the brown or black sediment to water is 1:2-1:1.
According to some embodiments of the invention, the speed of dropping the reducing agent in the first step is 10g/min to 80g/min; preferably 30g/min to 70g/min.
According to some embodiments of the invention, the grinding in step two is water ball grinding.
According to some embodiments of the invention, the drying comprises: drying at 90-120 deg.c for 8-16 hr; preferably 12 hours.
According to the preparation method of the formaldehyde-removing catalyst, one or more or mixed catalysts of amorphous manganese dioxide or crystalline manganese dioxide are obtained under mild conditions, so that the high-temperature activation process of the catalyst is avoided, and the requirements on equipment and the manufacturing cost are reduced.
According to some embodiments of the present invention, a screen assembly is provided, including the formaldehyde-removing semi-finished product assembly described above.
According to some embodiments of the present invention, an air purifier is provided, including the above-described filter assembly.
According to some embodiments of the present invention, an air conditioner is provided, including the air purifier.
According to some embodiments of the invention, a new wind system is provided, including the air purifier.
According to the application of the formaldehyde-removing catalyst provided by the invention, the catalyst can be attached to a medium to be applied to an air filtering system, so that the application range of the powder catalyst is greatly widened.
The following detailed description of embodiments of the invention is provided for the purpose of illustration only and is not to be construed as limiting the invention. In addition, all reagents employed in the examples below are commercially available or may be synthesized according to methods herein or known, and are readily available to those skilled in the art for reaction conditions not listed, if not explicitly stated.
Example 1
A preparation method of a formaldehyde removal catalyst comprises the following steps:
220.5g of potassium permanganate was added to 2L of water at room temperature and stirred for 30min to form a homogeneous solution. 31.89g of glucose powder was dissolved in 0.5L of water and stirred for several minutes to give a clear solution. The reducing agent solution was then added dropwise to the above manganese solution at a rate of 10.0 g/min. Stirring for 30min after the dripping is finished to obtain suspension, filtering to obtain brown or black sediment, drying at 110 ℃ for 12h to obtain brown or black powder, and adding a certain amount of water in a weight ratio: catalyst=1:1, ball milling to obtain dispersion containing manganese dioxide catalyst, adding a certain adhesive, and the adhesive is prepared by the following weight ratio: catalyst=1:1.8, to obtain catalyst cement, then immersing the micropore medium in the cement, extruding, and drying to obtain the formaldehyde-removing filter screen semi-finished product component with the load of 700g/m 2.
The formaldehyde-removing catalyst prepared in this example was numbered 1, and the performance test results are shown in Table 1.
Example 2
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 1. The difference is that the dropping speed of the reducing agent solution is 18.8g/min.
The formaldehyde-removing catalyst prepared in this example was numbered 2, and the performance test results are shown in table 1.
Example 3
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 1. The difference is that the dropping speed of the reducing agent solution is 39.7g/min.
The formaldehyde-removing catalyst prepared in this example was numbered 3, and the performance test results are shown in Table 1.
Example 4
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 1. The difference is that the dropping speed of the reducing agent solution was 49.1g/min.
The formaldehyde-removing catalyst prepared in this example was numbered 4, and the performance test results are shown in Table 1.
Further tests were carried out according to the invention on the performance of the catalyst obtained in example 4: FIG. 1 is an XRD pattern of a formaldehyde removal catalyst according to example 4 of the present invention, from which it can be seen that the diffraction peaks are dispersed, illustrating the catalyst being one or more mixtures of amorphous or crystalline manganese dioxide; FIG. 2 is a graph showing pore diameter distribution of formaldehyde removal catalyst of example 4 of the present invention, which has an average pore diameter of 8nm; FIG. 3 is an XPS spectrum of Mn 4+ for a formaldehyde removal catalyst of example 4 of the present invention, wherein the binding energies are the peaks at 641.8eV and 643.5eV, corresponding to the characteristic peaks at 2P 3/2 and 2P 1/2 for Mn 4+ in manganese dioxide; FIG. 4 is an SEM image of formaldehyde-removing catalyst of example 4 of the present invention, the catalyst having an average particle size of 40nm and being uniformly dispersed in the pores of a microporous support.
Example 5
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 1. The difference is that the dropping speed of the reducing agent solution is 66.3g/min.
The formaldehyde-removing catalyst prepared in this example was numbered 5, and the performance test results are shown in Table 1.
Example 6
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 1. The difference is that the dropping speed of the reducing agent solution is 79.7g/min.
The formaldehyde-removing catalyst prepared in this example was numbered 6, and the performance test results are shown in Table 1.
Example 7
A preparation method of a formaldehyde removal catalyst comprises the following steps:
220.5g of potassium permanganate are added to 2L of water at room temperature and stirred for 30min to form a homogeneous solution. 112.8g of glucose powder was dissolved in 0.5L of water and stirred for several minutes to give a transparent solution. The reducing agent solution was then added dropwise to the above manganese solution at 38.9 g/min. Stirring for 30min after the dripping is finished to obtain suspension, filtering to obtain brown or black sediment, drying at 110 ℃ for 12h to obtain brown or black powder, and adding a certain amount of water in a weight ratio: catalyst=2:1, ball milling to obtain dispersion containing manganese dioxide catalyst, adding a certain adhesive, and the adhesive is prepared by the following weight ratio: catalyst=1:1.8, get catalyst daub, then soak the micropore medium in daub later, get except that the semi-finished product assembly of formaldehyde filter screen after squeezing, oven drying, its load is 700g/m 2 oven drying, get except that formaldehyde catalyst.
The formaldehyde-removing catalyst prepared in this example was numbered 7, and the performance test results are shown in Table 1.
Example 8
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 7. Except that the mass of the reducing agent powder was 222.4g.
The formaldehyde-removing catalyst prepared in this example was numbered 8, and the performance test results are shown in Table 1.
Example 9
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 7. The difference is that the synthesis temperature is 35 ℃.
The formaldehyde-removing catalyst prepared in this example was numbered 9, and the performance test results are shown in Table 1.
Example 10
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 7. The difference is that the synthesis temperature is 40 ℃.
The formaldehyde-removing catalyst prepared in this example was numbered 10, and the performance test results are shown in Table 1.
Example 11
A method for preparing a formaldehyde removal catalyst was substantially the same as in example 7. The difference is that the synthesis temperature is 55 ℃.
The formaldehyde-removing catalyst prepared in this example was numbered 11, and the performance test results are shown in Table 1.
Performance test:
The formaldehyde-removing semi-finished product assembly obtained in each specific example was assembled into an air purifier, and the formaldehyde-removing performance thereof was tested. The screen was tested for FCADR, and resistance, in terms of the amount of clean air provided per unit time (particles with a particle size range above 0.3um, in m 3/h) according to GB18801-2015, a parameter characterizing the purification capacity of an air purifier, and the test results are shown in table 1 below.
Table 1. Results of the screen FCADR and load air volume test.
| Sequence number | FCADR(m3/h) | Average resistance (Pa) |
| 1 | 9.54 | 31.3 |
| 2 | 10.62 | 32.1 |
| 3 | 13.86 | 33.7 |
| 4 | 16.92 | 34.5 |
| 5 | 41.04 | 40.2 |
| 6 | 36.36 | 38.2 |
| 7 | 32.44 | 36.4 |
| 8 | 41.58 | 43.2 |
| 9 | 53.36 | 45.8 |
| 10 | 34.2 | 35.7 |
| 11 | 38.2 | 37.2 |
In the description of the present specification, reference to the terms "one embodiment," "some embodiments," "illustrative embodiments," "examples," "specific examples," or "some examples," etc., means that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the invention. In this specification, schematic representations of the above terms do not necessarily refer to the same embodiments or examples.
While embodiments of the present invention have been shown and described, it will be understood by those of ordinary skill in the art that: many changes, modifications, substitutions and variations may be made to the embodiments without departing from the spirit and principles of the invention, the scope of which is defined by the claims and their equivalents.
Claims (18)
1. A formaldehyde removal catalyst comprising: manganese dioxide, wherein the aperture of the manganese dioxide is d 1, and d 1 is satisfied, and d 1 is more than or equal to 5 and less than or equal to 50nm;
The manganese dioxide accounts for w in the total mass percent of the catalyst, wherein w is satisfied, and w is more than 95%;
The preparation method of the formaldehyde removal catalyst comprises the following steps:
step one, reduction reaction: dropwise adding a reducing agent into the manganese salt-containing solution, and reacting for a period of time;
Step two, grinding and dispersing: grinding the reaction liquid obtained in the step one to obtain a dispersion liquid containing the catalyst, and drying the dispersion liquid to obtain the formaldehyde-removing catalyst;
the molar ratio of the manganese-containing salt to the reducing agent in the first step is as follows: 2.2:1-10:1;
The manganese salt-containing solution in the first step comprises potassium permanganate and/or potassium manganate;
The reduction reaction is that the manganese salt-containing solution is stirred for 20-50 minutes at the temperature of 25-45 ℃; adding the reducing agent, heating to 50-80 ℃, and reacting for 1-4 hours to obtain brown or black suspension;
The speed of dropwise adding the reducing agent in the first step is 30 g/min-70 g/min;
The reducing agent in the first step is an organic reducing agent; the organic reducing agent comprises one or more of glucose, absolute ethyl alcohol and glycerol.
2. A formaldehyde-scavenging semi-finished component comprising a microporous medium having the catalyst of claim 1 attached to the surface or inside the pores.
3. The formaldehyde-removing semi-finished component according to claim 2, wherein the microporous medium is one or more of foam sponge, PET, carbon cloth.
4. The formaldehyde-scavenging semi-finished component of claim 3 wherein the microporous medium has a pore size d 2, wherein d 2 is satisfied and d 2 > 60 microns.
5. A method of producing a formaldehyde-scavenging semi-finished component according to any one of claims 2 to 4, comprising the steps of:
step one, reduction reaction: dropwise adding a reducing agent into the manganese salt-containing solution, and reacting for a period of time;
step two, grinding and dispersing: grinding the reaction liquid obtained in the step one to obtain a dispersion liquid containing the catalyst;
step three, gluing load: adding an adhesive into the dispersion liquid obtained in the step two, then adding a micropore medium, and drying to obtain a formaldehyde-removing semi-finished product component;
wherein, in the first step, the molar ratio of the manganese-containing salt to the reducing agent is as follows: 2.2:1-10:1;
The manganese salt-containing solution in the first step comprises potassium permanganate and/or potassium manganate;
The reduction reaction is that the manganese salt-containing solution is stirred for 20-50 minutes at the temperature of 25-45 ℃; adding the reducing agent, heating to 50-80 ℃, and reacting for 1-4 hours to obtain brown or black suspension;
The speed of dropwise adding the reducing agent in the first step is 30 g/min-70 g/min;
The reducing agent in the first step is an organic reducing agent; the organic reducing agent comprises one or more of glucose, absolute ethyl alcohol and glycerol.
6. The method of claim 5, wherein step three comprises immersing the catalyst-containing dispersion on a microporous medium.
7. The method according to claim 6, further comprising, in the third step, adding an adhesive to the dispersion obtained in the second step to obtain a cement, immersing the microporous medium in the cement, extruding, and drying to obtain the formaldehyde-removing semi-finished product assembly.
8. The method of any one of claims 5-7, wherein in step three, the adhesive comprises one or more of polyurethane, styrene-acrylate, polyacrylate, and polyesteramide.
9. The method according to claim 5, wherein the manganese salt-containing solution is obtained by adding potassium permanganate and/or potassium manganate to water at room temperature or 20-55 ℃.
10. The method according to claim 9, wherein step one further comprises suction-filtering the brown or black suspension, washing with water for 2-5 times, and drying to obtain a brown or black deposit.
11. The method according to claim 10, wherein in the second step, the brown or black deposit is milled to have a weight ratio of 1:2-1:1 with water, and the mixture is ball milled for 5-8 hours to obtain a dispersion of the catalyst containing manganese dioxide.
12. The method according to claim 5, wherein the grinding in the second step is water-adding ball milling.
13. The method of claim 5, wherein the drying comprises: drying at 90-120 ℃ for 8-16 hours.
14. The method of claim 13, wherein the drying comprises: drying for 12 hours.
15. A screen assembly comprising a formaldehyde-scavenging semi-finished assembly according to any one of claims 2-4.
16. An air purifier comprising the screen assembly of claim 15.
17. An air conditioner comprising the air cleaner according to claim 16.
18. A fresh air system comprising the air cleaner of claim 16.
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| PCT/CN2022/079481 WO2023050724A1 (en) | 2021-09-30 | 2022-03-07 | Formaldehyde removal catalyst and preparation method therefor, formaldehyde removal semi-finished assembly and preparation method therefor, and filter screen assembly |
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| CN116212853B (en) * | 2022-12-28 | 2023-10-31 | 重庆工商大学 | δ-MnO 2 Catalytic material, preparation method thereof and application of catalytic material in preparation of filter screen capable of degrading formaldehyde |
| CN116943634B (en) * | 2023-07-13 | 2024-07-12 | 浙江大学 | High-performance formaldehyde and VOC (volatile organic compound) removal honeycomb catalyst nanomaterial and preparation method thereof |
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