CN111495411A - Catalyst for decomposing ozone and preparation method thereof - Google Patents

Catalyst for decomposing ozone and preparation method thereof Download PDF

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CN111495411A
CN111495411A CN202010360934.1A CN202010360934A CN111495411A CN 111495411 A CN111495411 A CN 111495411A CN 202010360934 A CN202010360934 A CN 202010360934A CN 111495411 A CN111495411 A CN 111495411A
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catalyst
ozone
mno
mnac
melamine
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CN111495411B (en
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罗孟飞
方晨涛
陈建
李丹丹
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Zhejiang Normal University CJNU
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Zhejiang Normal University CJNU
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    • 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
    • B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
    • B01J27/24—Nitrogen compounds
    • 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
    • B01D53/8671—Removing components of defined structure not provided for in B01D53/8603 - B01D53/8668
    • B01D53/8675—Ozone
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08—Heat treatment
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08—Heat treatment
    • B01J37/082—Decomposition and pyrolysis
    • 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
    • B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/08—Heat treatment
    • B01J37/082—Decomposition and pyrolysis
    • B01J37/084—Decomposition of carbon-containing compounds into carbon
    • 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 provides a catalyst for decomposing ozone, which consists of MnO and Mn2N0.86And C. The invention also provides a method for preparing the catalyst, MnAc2·4H2Adding O into ethanol, stirring to dissolve completely, adding melamine, mixing, stirring, evaporating, and calcining to obtain MnO-Mn2N0.86-a catalyst C. The invention has the advantages that the catalyst still has high activity and stability even under the condition that the relative humidity is 90 percent, the raw materials and conditions for preparing the catalyst are easy to obtain, the preparation cost is low, and the large-scale production and popularization are easy.

Description

Catalyst for decomposing ozone and preparation method thereof
Technical Field
The invention belongs to the technical field of chemical catalysts, and particularly relates to a catalyst for decomposing ozone and a preparation method thereof.
Background
It is well known that ozone acts as a double-edged sword for the human environment on which it lives. In the stratosphere, the ozone can resist ultraviolet rays to directly irradiate the earth, and is a natural protective barrier for the nature; tropospheric ozone is a greenhouse gas that causes global warming and air quality degradation. High concentrations of tropospheric ozone can also have deleterious effects on ecosystems, such as reduced yield in food, reduced productivity in forests and grasslands, directly threatening biodiversity. In addition, as a strong oxidant, ozone is widely applied to industries of food, sewage treatment, medical treatment and health care and the like. The residual ozone causes the discharged tail gas to contain a certain concentration of ozone, and the tail gas can be discharged after the ozone is removed. With the popularization of modern office equipment, the use of machines such as laser printers and copiers, ozone disinfection equipment and the like in large quantities, ozone is generated through high-voltage discharge, corona discharge or ultraviolet radiation, and the concentration of ozone is greatly improved in a short time in a closed environment. It has been reported that a person exposed to a high concentration of ozone for a short period of time may cause damage to the respiratory system including the onset of coughing, difficulty breathing and decreased lung function. Long-term exposure to ozone can have a variety of deleterious effects, including neurological disorders, decreased lung function and airway inflammation, hypertension, accelerated aging, and the like. Therefore, the research on ozonolysis has important significance on environmental protection and human health.
At present, methods for removing ozone include a chemical adsorption method, an electromagnetic wave radiation method, a thermal decomposition method, a catalytic decomposition method, and the like. The catalytic decomposition method has the characteristics of low energy consumption, simple operation, high conversion efficiency and the like, and is widely researched and applied. The catalyst for catalytically decomposing ozone mainly comprises noble metals and transition metal oxides.
The reaction of Pd-Mn catalyst for decomposing ozone has been reported (Journal of Hazardous Materials, 2009, 172, 631-634), and the space velocity (GHSV) is 635000h-1The ozone conversion rate after 80 hours of reaction was 90% at a reaction temperature of 40 ℃, showing excellent ozonolysis performance. However, the production cost of such a catalyst using noble metal Pd is considerably high. Chinese patents CN102513106A, CN101402047A, and CN101757933A disclose composite catalysts using transition metal oxides such as manganese oxide, iron oxide, etc. as active components, and the synthesis process generally requires high temperature and high pressure, the production process is complex, the energy consumption is high, and the catalytic performance of part of the catalysts is greatly interfered by humidity. Therefore, a method for preparing the compound is found,There is a need for a low cost ozonolysis catalyst that is highly stable in humid environments.
Disclosure of Invention
In order to solve the problem of poor stability of the catalyst in the prior art in a humid environment, the invention provides a catalyst for decomposing ozone and a preparation method thereof, which achieve the aims that the preparation method and conditions are easy to obtain and operate, and the prepared catalyst has high activity and stability even under the condition that the relative humidity is 90 percent.
In order to achieve the purpose, the technical scheme disclosed by the invention is as follows: the invention provides a catalyst for decomposing ozone, which consists of MnO and Mn2N0.86And C, the mass percentage of each component in the catalyst is respectively as follows: MnO 38%, Mn2N0.8660% and 2% of C.
The invention also provides a method for preparing the catalyst, which comprises the following steps:
according to manganese acetate MnAc2·4H2The mass ratio of O to melamine is 2:1, and the mass of ethanol is MnAc2·4H 210 times of the total mass of O and melamine, MnAc2·4H2Adding O into ethanol, stirring to dissolve completely, adding melamine, mixing uniformly, stirring in 90 deg.C water bath, evaporating, heating to 850 deg.C under nitrogen atmosphere at a heating rate of 5 deg.C/min, and calcining for 1 hr to obtain MnO-Mn2N0.86-a catalyst C.
The invention has the beneficial effects that: tests show that the catalyst prepared by the invention has high relative humidity of 90 percent at normal temperature and 20 ℃, the ozone concentration before reaction is 22 +/-1 ppm, and the airspeed is 120000h-1Under the condition, the conversion rate of the ozone reaction is 100 percent, the catalyst still has high activity and stability even under the condition that the relative humidity is 90 percent, the raw materials and the conditions for preparing the catalyst are easy to obtain, the preparation cost is low, and the large-scale production and popularization are easy.
Drawings
FIG. 1 shows MnO-Mn in example 12N0.86Catalysis of CXRD pattern of the agent.
FIG. 2 is a graph showing the stability of example 1 and comparative example 1 to ozonolysis reaction.
Detailed Description
The present invention is described in further detail below with reference to specific examples.
The first embodiment is as follows: (1) MnO-Mn2N0.86Preparation of-C
According to manganese acetate (MnAc)2·4H2O) and melamine in a mass ratio of 2:1, and the mass of the ethanol is MnAc2·4H 210 times of the total mass of O and melamine. MnAc2·4H2Adding O into ethanol, stirring to dissolve completely, adding melamine, mixing uniformly, stirring in 90 deg.C water bath, evaporating, heating to 850 deg.C under nitrogen atmosphere at a heating rate of 5 deg.C/min, and calcining for 1 hr to obtain MnO-Mn2N0.86-a catalyst C.
The test shows that the catalyst consists of MnO and Mn2N0.86And C, MnO, Mn2N0.86And C is 38 percent, 60 percent and 2 percent by mass respectively.
The XRD pattern of the catalyst is shown in figure 1
(2) Testing of catalyst Performance
The catalyst was pressed and sieved (40 mesh) before use, the catalyst was used in an amount of 0.6m L each time, the fixed bed containing the catalyst was maintained at 20 ℃, 185nm ultraviolet lamp (power 6W) was used to excite air to generate ozone, which was carried into the reactor through the air, and the measured concentration of ozone before the reaction was 22 ± 1ppm, the flow rate was 1.2L/min, and the space velocity was 120000h-1The reaction gas was bubbled through 18.5 ℃ water to saturate the water content in the reaction gas at 18.5 ℃ and then passed through a 20 ℃ catalyst at a gas relative humidity of 90%. ozone detector (model 106-L, 2 bttechnologies, USA) was used to analyze the inlet and outlet ozone concentrations in the fixed bed reactor and calculate the ozone decomposition rate, using the following formula:
O3conversion rate ═ Cin-Cout)/Cinx100％
In the formula CinIs the ozone concentration (ppm) and C before reactionoutIs the ozone concentration (ppm) after the reaction. The ozone decomposition efficiency of the catalyst as a function of reaction time is shown in FIG. 2.
Comparative example 1:
(1)Mn2O3-Mn3O4preparation of
According to manganese acetate (MnAc)2·4H2O) and melamine in a mass ratio of 2:1, and the mass of the ethanol is MnAc2·4H 210 times of the total mass of O and melamine. MnAc2·4H2Adding O into ethanol, stirring to dissolve completely, adding melamine, mixing uniformly, stirring in 90 deg.C water bath, evaporating, heating to 850 deg.C at 5 deg.C/min in air atmosphere, and calcining for 1 hr to obtain Mn2O3-Mn3O4Catalyst, XRD analysis of the catalyst phase from Mn2O3And Mn3O4Composition of
(2) The catalyst performance test was the same as in example 1, and the catalytic reaction performance is shown in FIG. 2.
As can be seen from FIG. 2, the catalyst of example 1 has a decomposition rate of 100% for ozone and is very stable, which shows that the catalyst of example 1 (MnO-Mn) is prepared by calcining manganese acetate, melamine and ethanol as raw materials in a nitrogen atmosphere2N0.86the-C) performance is obviously superior to that of the catalyst (Mn) of the comparison column 1 prepared by air atmosphere roasting2O3-Mn3O4). As described above, MnO-Mn2N0.86the-C catalyst has high activity and stability for catalytic decomposition of ozone, and the catalyst has simple preparation process and good reproducibility.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (2)

1. A catalyst for decomposing ozone is characterized in that the catalyst consists of MnO and Mn2N0.86And C, the mass percentage of each component in the catalyst is respectively as follows: MnO 38%, Mn2N0.8660% and 2% of C.
2. A process for preparing the catalyst of claim 1, comprising the steps of:
according to manganese acetate MnAc2·4H2The mass ratio of O to melamine is 2:1, and the mass of ethanol is MnAc2·4H210 times of the total mass of O and melamine, MnAc2·4H2Adding O into ethanol, stirring to dissolve completely, adding melamine, mixing uniformly, stirring in 90 deg.C water bath, evaporating, heating to 850 deg.C under nitrogen atmosphere at a heating rate of 5 deg.C/min, and calcining for 1 hr to obtain MnO-Mn2N0.86-a catalyst C.
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Cited By (1)

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Publication number Priority date Publication date Assignee Title
CN113559848A (en) * 2021-08-06 2021-10-29 四川大学 High-activity ozonolysis manganese-based catalyst and preparation method thereof

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CN105810959A (en) * 2016-05-16 2016-07-27 中南大学 High-performance oxygen reduction catalyst MnOx/Mn2N-N-C composite catalyst and preparation method and application thereof
CN106430146A (en) * 2016-11-22 2017-02-22 重庆文理学院 Nitrogen-manganese co-doped hierarchical porous carbon material preparation method
US20170232424A1 (en) * 2016-02-17 2017-08-17 Toyota Jidosha Kabushiki Kaisha Exhaust gas purification catalyst and production method thereof
JP2017192429A (en) * 2016-04-18 2017-10-26 株式会社キャタラー Catalyst filter, deodorization device and air cleaning device
CN109678146A (en) * 2019-01-22 2019-04-26 中国科学院福建物质结构研究所 A kind of porous class graphitic carbon nano piece of N doping and its preparation and electro-catalysis application

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US20170232424A1 (en) * 2016-02-17 2017-08-17 Toyota Jidosha Kabushiki Kaisha Exhaust gas purification catalyst and production method thereof
JP2017192429A (en) * 2016-04-18 2017-10-26 株式会社キャタラー Catalyst filter, deodorization device and air cleaning device
CN105810959A (en) * 2016-05-16 2016-07-27 中南大学 High-performance oxygen reduction catalyst MnOx/Mn2N-N-C composite catalyst and preparation method and application thereof
CN106430146A (en) * 2016-11-22 2017-02-22 重庆文理学院 Nitrogen-manganese co-doped hierarchical porous carbon material preparation method
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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113559848A (en) * 2021-08-06 2021-10-29 四川大学 High-activity ozonolysis manganese-based catalyst and preparation method thereof
CN113559848B (en) * 2021-08-06 2023-10-20 四川大学 High-activity ozone decomposition manganese-based catalyst and preparation method thereof

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