CN115672311A - Preparation method and application of shape-adjustable integral ozone decomposition catalyst - Google Patents
Preparation method and application of shape-adjustable integral ozone decomposition catalyst Download PDFInfo
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- CN115672311A CN115672311A CN202211278734.7A CN202211278734A CN115672311A CN 115672311 A CN115672311 A CN 115672311A CN 202211278734 A CN202211278734 A CN 202211278734A CN 115672311 A CN115672311 A CN 115672311A
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- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 title claims abstract description 46
- 239000003054 catalyst Substances 0.000 title claims abstract description 44
- 238000000354 decomposition reaction Methods 0.000 title claims abstract description 21
- 238000002360 preparation method Methods 0.000 title claims abstract description 10
- 238000005949 ozonolysis reaction Methods 0.000 claims abstract description 19
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 15
- 238000000034 method Methods 0.000 claims abstract description 12
- 238000004108 freeze drying Methods 0.000 claims abstract description 8
- 229910021389 graphene Inorganic materials 0.000 claims abstract description 7
- 229940071125 manganese acetate Drugs 0.000 claims abstract description 7
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 claims abstract description 7
- 239000012286 potassium permanganate Substances 0.000 claims abstract description 7
- 238000004659 sterilization and disinfection Methods 0.000 claims abstract description 5
- 238000009423 ventilation Methods 0.000 claims abstract description 3
- 238000002156 mixing Methods 0.000 claims description 23
- 239000000243 solution Substances 0.000 claims description 22
- 239000002904 solvent Substances 0.000 claims description 15
- 238000001354 calcination Methods 0.000 claims description 12
- 239000000725 suspension Substances 0.000 claims description 12
- 239000003570 air Substances 0.000 claims description 9
- 239000000463 material Substances 0.000 claims description 8
- 238000003756 stirring Methods 0.000 claims description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 6
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 claims description 6
- 239000011259 mixed solution Substances 0.000 claims description 6
- 239000007789 gas Substances 0.000 claims description 5
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- 238000001035 drying Methods 0.000 claims description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 3
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- PUPZLCDOIYMWBV-UHFFFAOYSA-N (+/-)-1,3-Butanediol Chemical compound CC(O)CCO PUPZLCDOIYMWBV-UHFFFAOYSA-N 0.000 claims 1
- 239000002243 precursor Substances 0.000 abstract description 2
- 230000001105 regulatory effect Effects 0.000 abstract 1
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 8
- 230000000694 effects Effects 0.000 description 7
- 238000005516 engineering process Methods 0.000 description 5
- 230000008901 benefit Effects 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 230000005855 radiation Effects 0.000 description 4
- 230000008569 process Effects 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- IKHGUXGNUITLKF-UHFFFAOYSA-N Acetaldehyde Chemical compound CC=O IKHGUXGNUITLKF-UHFFFAOYSA-N 0.000 description 2
- RAHZWNYVWXNFOC-UHFFFAOYSA-N Sulphur dioxide Chemical compound O=S=O RAHZWNYVWXNFOC-UHFFFAOYSA-N 0.000 description 2
- 238000010521 absorption reaction Methods 0.000 description 2
- 230000009471 action Effects 0.000 description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 238000003421 catalytic decomposition reaction Methods 0.000 description 2
- 238000005265 energy consumption Methods 0.000 description 2
- 239000003344 environmental pollutant Substances 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- 239000007800 oxidant agent Substances 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 231100000719 pollutant Toxicity 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 238000005979 thermal decomposition reaction Methods 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-N Sulfurous acid Chemical compound OS(O)=O LSNNMFCWUKXFEE-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- CDQSJQSWAWPGKG-UHFFFAOYSA-N butane-1,1-diol Chemical compound CCCC(O)O CDQSJQSWAWPGKG-UHFFFAOYSA-N 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000012824 chemical production Methods 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000000295 complement effect Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000003814 drug Substances 0.000 description 1
- 239000000428 dust Substances 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- WSFSSNUMVMOOMR-NJFSPNSNSA-N methanone Chemical compound O=[14CH2] WSFSSNUMVMOOMR-NJFSPNSNSA-N 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 150000002894 organic compounds Chemical class 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 239000002957 persistent organic pollutant Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000011012 sanitization Methods 0.000 description 1
- 239000004071 soot Substances 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000012855 volatile organic compound Substances 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
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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
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Abstract
The invention relates to a preparation method and application of an integral ozone decomposition catalyst with an adjustable shape. According to the invention, manganese acetate, potassium permanganate and graphene oxide are used as precursors, and the shape of the integral ozonolysis catalyst is regulated and controlled by changing the shape of a mould by adopting a freeze drying method. The preparation method of the monolithic catalyst can customize the catalyst according to the requirements of specific application scenes on the shape and the size of the ozone decomposition module, and meets the special requirements of disinfection cabinets, printers, air purifiers, fresh air systems, ventilation fans and the like on the shape and the size of the ozone decomposition module.
Description
Technical Field
The invention belongs to the technical field of ozonolysis, and particularly relates to a preparation method and application of an integral ozonolysis catalyst with an adjustable shape.
Background
With the rapid development of urbanization and the severe consumption of traditional fossil energy, the environmental pollution problem is becoming more and more serious. Although the action plan for preventing and treating the Chinese atmospheric pollution implemented in 2013 has obviously reduced the main pollutants including sulfur dioxide, particulate Matters (PM) and Nitrogen Oxides (NO) in China x ：NO+NO 2 ) Is artificially discharged. However, it is not limited toThe concentration of surface ozone has been high all the time, and the trend of increasing surface ozone concentration has been shown in environmental bulletin issued by national institutes in the last 5 years. The sources of surface ozone are mainly divided into two types, indirect emission and direct emission: the indirect emission means that under illumination, carbon monoxide, volatile organic compounds and nitrogen oxides in the air generate ozone through photochemical action, and various human activity places such as chemical production, automobile exhaust emission, thermal power generation and the like are sources for emitting ozone precursors; the direct discharge is because ozone is widely used as an oxidizing agent in industry in water treatment plants, hospitals, food sanitization, and the like, but ozone cannot be stored or transported in containers, and thus ozone is generated on site by an ozone generator. Ozone leaks occur from the failure of ozone generator components such as pipes, gaskets, joint seals and valves, which exposes a large number of workers and occupants to the risk of exposure to high concentrations of ozone. And the indoor electrostatic equipment such as a disinfection cabinet, a fresh air system, a printer, a refrigerator and the like can also discharge redundant ozone gas, and the ozone gas is an important source of indoor ozone pollution.
Since the onset of photochemical smog events in the united states at the end of the 20 th century, the hazards presented by surface ozone have been recognized and valued, and the harnessing of ozone has also opened the preface. The types of ozone treatment technologies developed to date are numerous and mainly include activated carbon adsorption, liquid medicine absorption, thermal decomposition, radiation decomposition, and catalytic decomposition. The activated carbon adsorption technology uses an activated carbon material as a treating agent, and converts ozone into oxygen through an adsorption decomposition mechanism, but the ozone reacts with organic compounds such as dust and soot deposited on a filter, and the like, and harmful secondary organic pollutants such as formaldehyde, acetaldehyde and the like may be generated. In addition, activated carbon is flammable, and ozone is a strong oxidant with exothermic decomposition reactions, which has potential safety hazards. In the chemical solution absorption technique, ozone is consumed by using a reducing solvent such as sulfite, but an excessive waste liquid is generated, which increases the difficulty of operation and the cost. Thermal decomposition and radiation decomposition techniques reduce the time for ozone decomposition by heating the temperature, respectively, with light radiation, but high temperature, ultraviolet radiation requires a large amount of energy consumption and is impractical for certain applications (e.g., respirator filters) and does not meet the requirements of practical applications. The catalytic decomposition technology utilizes a catalyst to accelerate the reaction process of decomposing ozone into oxygen at normal temperature, does not produce a large amount of byproducts, has low energy consumption and simple operation, can complement short plates of other four treatment technologies, and can realize effective ozone removal effect in a complex environment, thereby being an ozone treatment technology with great development prospect at present. However, in practical application environments, due to the limitation of the size and shape of the ozone exhaust gas treatment device or the module, the traditional powder catalyst is difficult to be directly applied to such scenes, and the development of the shape-adjustable monolithic ozone decomposition catalyst is required.
Disclosure of Invention
In order to solve the problems, the invention aims to develop the shape-adjustable ozone decomposition catalyst, so that the ozone decomposition efficiency is more than 99% under the humidity of more than 60%, and the stabilization time is more than 5000h.
In order to solve the technical problems, the invention adopts the following scheme:
a preparation method of a shape-adjustable monolithic ozonolysis catalyst is characterized by comprising the following steps:
(1) Mixing manganese acetate, graphene oxide and a solvent according to the weight ratio of 9g:1g: mixing the materials in a dosage ratio of 20mL to obtain a suspension A;
(2) Mixing potassium permanganate with a solvent according to the weight ratio of 4.5g: mixing the solution A and the solution B according to the dosage ratio of 20mL to obtain a solution B;
(3) Quickly dripping the solution B into the suspension A under the stirring state;
(4) And pouring the mixed solution into a mold, and carrying out freeze drying and calcination to obtain the monolithic catalyst.
Further, the solvent is one or more of water, methanol, ethanol, ethylene glycol, propylene glycol and butanediol.
Furthermore, the stirring speed is 50-1000r/min, and the dropping speed is 10-200 drops/min.
Furthermore, the calcination temperature is 100-700 ℃, the calcination time is 0.5-10h, and the calcination atmosphere is one of air, argon and nitrogen.
Further, the drying process is freeze drying, the temperature is-85 ℃, and the drying time is 24 hours.
Furthermore, the shape and the size of the monolithic catalyst are consistent with those of a mold, and the shape and the size of the monolithic catalyst can be adjusted according to the requirements of application scenes.
The monolithic catalyst is used for the ozone decomposition reaction with the humidity of more than 60 percent, and the time of the ozone decomposition efficiency of more than 99 percent exceeds 5000h.
The integral catalyst is used in application scenes with special requirements on the volume and the shape of an ozone tail gas treatment system, and comprises but is not limited to a disinfection cabinet, a printer, an air purifier, a fresh air system and a ventilation fan.
The invention has the beneficial effects that: ozone pollutants can be generated in the using process of a disinfection cabinet, a printer, an air purifier and the like, and an ozone decomposition module needs to be additionally arranged. Due to the limitation of the volume, the ozone decomposition module needs to be small in volume and adjustable in shape, so that the requirements of different application scenes on the shape and the size of the ozone decomposition module are met. The traditional ozone decomposition catalyst mainly takes honeycomb and short rod shapes as main materials, has the problems of large volume, fixed shape and the like in the using process, and is difficult to be applied to the scenes. Aiming at the problems, the monolithic catalyst has the advantage of adjustable shape, and the shape and the size of the catalyst can be adjusted according to the requirements of practical application scenes, so that the practical application requirements are met. Meanwhile, the monolithic catalyst has the advantage of good stability under high humidity, and has great application potential.
Drawings
FIG. 1 is a pictorial view of an integral ozonolysis catalyst according to the invention;
FIG. 2 is a graph showing the ozonolysis activity of the ozonolysis catalyst of the invention at 60% humidity;
Detailed Description
The technical solutions of the present invention will be described in detail below in order to clearly understand the technical features, objects, and advantages of the present invention, but the present invention is not limited to the practical scope of the present invention.
The embodiment provides a preparation method of a monolithic ozone decomposition catalyst with an adjustable shape.
Example 1: mixing manganese acetate, graphene oxide and a solvent according to a ratio of 9g:1g: mixing the materials in a dosage ratio of 20mL to obtain a suspension A; mixing potassium permanganate with a solvent according to the weight ratio of 4.5g: mixing the solution A with the dosage of 20mL to obtain a solution B; quickly dropping the solution B into the suspension A at a stirring speed of 200r/min, wherein the dropping speed is 100 drops/min; and pouring the mixed solution into a cylindrical mold, freeze-drying at-85 ℃ for 24h, and calcining at 450 ℃ for 4h to obtain the cylindrical monolithic catalyst.
FIG. 1 is a schematic diagram of the monolithic ozonolysis catalyst obtained in example 1. As can be seen from the figure, the monolithic catalyst has a cylindrical shape, the same as the mold.
FIG. 2 is a graph showing the activity of the ozonolysis catalyst obtained in example 1 at 60% humidity. As can be seen from the figure, the catalyst can achieve an ozonolysis efficiency of greater than 99% for 5000h.
Example 2: mixing manganese acetate, graphene oxide and a solvent according to a ratio of 9g:1g: mixing the materials in a dosage ratio of 20mL to obtain a suspension A; mixing potassium permanganate with a solvent according to the weight ratio of 4.5g: mixing the solution A with the dosage of 20mL to obtain a solution B; quickly dripping the solution B into the suspension A at a stirring speed of 150r/min, wherein the dripping speed is 50 drops/min; and pouring the mixed solution into a five-pointed star mold, freeze-drying at-85 ℃ for 24h, and calcining at 550 ℃ for 5h to obtain the cylindrical monolithic catalyst.
Example 3: mixing manganese acetate, graphene oxide and a solvent according to a ratio of 9g:1g: mixing the materials in a dosage ratio of 20mL to obtain a suspension A; mixing potassium permanganate with a solvent according to the weight ratio of 4.5g: mixing the solution A with the dosage of 20mL to obtain a solution B; rapidly dripping the solution B into the suspension A at a stirring speed of 500r/min, wherein the dripping speed is 150 drops/min; and pouring the mixed solution into an S-shaped mold, freeze-drying at-85 ℃ for 24h, and calcining at 400 ℃ for 3h to obtain the cylindrical monolithic catalyst.
Comparative example 1: mixing manganese acetate, graphene oxide and a solvent according to a ratio of 9g:1g: mixing the materials in a dosage ratio of 20mL to obtain a suspension A; mixing potassium permanganate with a solvent according to the weight ratio of 4.5g: mixing the solution A with the dosage of 20mL to obtain a solution B; rapidly dripping the solution B into the suspension A at a stirring speed of 200r/min, wherein the dripping speed is 100 drops/min; and drying the mixed solution at 70 ℃ for 24h, and calcining at 450 ℃ for 4h to obtain the catalyst.
Table 1 shows the comparison of the effects of different examples and different comparative examples, and it can be seen from the table that the monolithic ozonolysis catalyst obtained by the present invention has an adjustable shape and does not deteriorate in activity exceeding 5000 hours at 60% humidity, while the comparative example is in the form of powder, and has not only low activity but also poor stability at 60% humidity.
TABLE 1 comparison of catalytic ozonolysis Performance between different examples and different comparative examples
The present invention is not limited to the above examples, and the ozonolysis reaction in a special application scene can be realized by changing the preparation conditions and the shape of the mold and controlling the shape of the catalyst.
Processes, methods, and apparatus not described in the embodiments of the present invention are known in the art. And will not be described in detail herein.
The above embodiments, objects, technical solutions and advantages of the present invention are further described in detail, it should be understood that the above embodiments are only examples of the present invention, and are not intended to limit the scope of the present invention, and any modifications, equivalent substitutions, improvements and the like made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (8)
1. A preparation method of a shape-adjustable monolithic ozonolysis catalyst is characterized by comprising the following steps:
(1) Mixing manganese acetate, graphene oxide and a solvent according to the weight ratio of 9g:1g: mixing the materials in a dosage ratio of 20mL to obtain a suspension A;
(2) Potassium permanganate and solvent were mixed according to a ratio of 4.5g: mixing the solution A with the dosage of 20mL to obtain a solution B;
(3) Quickly dropping the solution B into the suspension A under the stirring state;
(4) And pouring the mixed solution into a mold, and carrying out freeze drying and calcination to obtain the monolithic catalyst.
2. The method of claim 1, wherein the solvent is one or more of water, methanol, ethanol, ethylene glycol, propylene glycol, and butylene glycol.
3. The method for preparing a shape-adjustable monolithic ozonolysis catalyst according to claim 1, wherein the stirring speed is 50-1000r/min and the dropping rate is 10-200 drops/min.
4. The method for preparing a shape-adjustable monolithic ozonolysis catalyst according to claim 1, wherein the calcination temperature is 100 to 700 ℃, the calcination time is 0.5 to 10 hours, and the calcination atmosphere is one of air, argon and nitrogen.
5. The method for preparing a shape-adjustable monolithic ozonolysis catalyst according to claim 1, wherein the drying process is freeze-drying at-85 ℃ for 24 hours.
6. The method for preparing a shape-adjustable monolithic ozone decomposition catalyst as claimed in claim 1, wherein the shape and size of the monolithic catalyst are consistent with those of the mold, and the shape and size of the monolithic catalyst can be adjusted according to the requirements of application scenarios.
7. Use of the monolithic catalyst obtained by the preparation method according to any one of claims 1 to 6, characterized in that it is used for ozonolysis reactions with a humidity greater than 60% or more, with an ozonolysis efficiency of 99% or more for a time greater than 5000h.
8. The use of claim 7, wherein the monolithic catalyst is used in application scenarios with special requirements on the volume and shape of the ozone exhaust gas treatment system, including but not limited to disinfection cabinets, printers, air purifiers, fresh air systems, and ventilation fans.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116351424A (en) * | 2023-03-31 | 2023-06-30 | 西南石油大学 | Preparation method and application of high-moisture-resistance LDH@graphene ozonolysis catalyst |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108339546A (en) * | 2018-02-12 | 2018-07-31 | 中国科学院城市环境研究所 | A kind of ozone decomposition catalyst and its preparation method and application |
| WO2022102810A1 (en) * | 2020-11-12 | 2022-05-19 | Purespace Inc. | Catalytic activity recovery method of manganese oxide catalyst |
| CN114700062A (en) * | 2022-04-28 | 2022-07-05 | 江苏嘉宁环境科技有限公司 | Preparation method and application of salt-tolerant ozone catalyst of porous carbon aerogel |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108339546A (en) * | 2018-02-12 | 2018-07-31 | 中国科学院城市环境研究所 | A kind of ozone decomposition catalyst and its preparation method and application |
| WO2022102810A1 (en) * | 2020-11-12 | 2022-05-19 | Purespace Inc. | Catalytic activity recovery method of manganese oxide catalyst |
| CN114700062A (en) * | 2022-04-28 | 2022-07-05 | 江苏嘉宁环境科技有限公司 | Preparation method and application of salt-tolerant ozone catalyst of porous carbon aerogel |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116351424A (en) * | 2023-03-31 | 2023-06-30 | 西南石油大学 | Preparation method and application of high-moisture-resistance LDH@graphene ozonolysis catalyst |
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