CN111921524A - ABO3Perovskite catalyst, preparation method and application in plasma concerted catalysis of VOCs - Google Patents

ABO3Perovskite catalyst, preparation method and application in plasma concerted catalysis of VOCs Download PDF

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CN111921524A
CN111921524A CN202010828651.5A CN202010828651A CN111921524A CN 111921524 A CN111921524 A CN 111921524A CN 202010828651 A CN202010828651 A CN 202010828651A CN 111921524 A CN111921524 A CN 111921524A
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toluene
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CN111921524B (en
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李海龙
刘凯
刘峥
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Central South University
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Abstract

The invention discloses an ABO3A perovskite catalyst, a preparation method and application thereof in plasma concerted catalysis of VOCs. ABO3In the perovskite catalyst, A is one or more lanthanide metal elements, B is one or more selected from Ti, V, Cr, Mn, Fe, Co, Ni or Cu, and ABO3The perovskite catalyst is prepared by a high-temperature self-melting method, and the method comprises the following specific steps: (1) respectively taking nitrates of A and B and directly mixing the nitrates with citric acid; (2) placing the mixture obtained in the step (1) in a muffle furnace for calcining and crystallizing to obtainTo ABO3A perovskite-type catalyst. The invention has the beneficial effects that: the perovskite catalyst prepared by the high-temperature self-melting method saves the preparation time cost of the catalyst, saves the production cost due to no noble metal elements, and overcomes the defect of independent use of a single technology by cooperatively catalyzing VOCs by the prepared catalyst and plasma.

Description

ABO3Perovskite catalyst, preparation method and application in plasma concerted catalysis of VOCs
Technical Field
The invention belongs to the technical field of environmental pollution prevention and purification, and particularly relates to ABO3A perovskite catalyst, a preparation method and application in plasma concerted catalysis of VOCs.
Background
In recent years, environmental issues have received global attention. Volatile Organic Compounds (VOCs) are one of the important pollutants, and include hydrocarbons (alkanes, alkenes, alkynes, cyclic hydrocarbons), aromatics, ketones, esters, alcohols, ethers, aldehydes, amines, nitriles, and other organic compounds. At present, the industries such as electronics, chemical industry, petrochemical industry, coating, printing, coating, furniture, leather and the like become the VOC heavy emission source in China. Because VOCs can generate great harm to the environment and human bodies, the volatility is strong, the related industries are wide, the characteristics of unorganized discharge and low-efficiency decontamination are very obvious, and the strengthening of the comprehensive treatment of the VOCs in key industries is particularly important.
The existing VOCs treatment technologies mainly comprise an absorption method, an adsorption method, a condensation method, a membrane separation method, a combustion method, a biological method, a catalytic oxidation method, a photocatalytic method and the like. However, the above treatment methods have many limitations in technical and economical aspects. Although the low-temperature plasma technology has the advantages of mild reaction conditions, rapid reaction and the like, the low-temperature plasma technology has the problems of low energy efficiency, secondary pollution and the like when being used alone, and the defects can be effectively overcome by combining the low-temperature plasma technology with a catalytic oxidation method.
The active components of the general catalyst mostly use noble metals, and the production cost of the catalyst is high. The perovskite oxide has excellent catalytic performance and stable structure, but the preparation method of the general perovskite catalyst has longer period and large time cost.
Disclosure of Invention
The invention mainly aims to provide an ABO3The perovskite catalyst, the preparation method and the application in the plasma concerted catalysis of VOCs; the invention adopts the high-temperature self-melting method to prepare the ABO3The perovskite oxide is used as a catalyst for plasma to cooperatively catalyze VOCs (volatile organic compounds) so as to solve the problems of low temperature and the like in the prior artThe problems of low energy efficiency, secondary pollution, overhigh catalyst production cost and the like when the plasma is used independently.
In order to achieve the above object, the following technical solutions are adopted.
ABO3Process for preparing perovskite-type catalyst, ABO3In the perovskite catalyst, A is one or more lanthanide metal elements, B is one or more selected from Ti, V, Cr, Mn, Fe, Co, Ni or Cu, and ABO3The perovskite catalyst is prepared by a high-temperature self-melting method, and the method comprises the following specific steps:
(1) respectively taking nitrates of A and B and directly mixing the nitrates with citric acid;
(2) placing the mixture obtained in the step (1) in a muffle furnace for calcining and crystallizing to obtain ABO3A perovskite-type catalyst.
In the invention, A is selected from any one or more of La, Ce, Sm or Gd; b is selected from any one or more of Fe, Co, Ti, V and Mn.
In the present invention, ABO3In the perovskite catalyst, partial metal element C is selected to replace A or B by isomorphism replacement, and C is preferably selected from any one or more of Ga and Sr.
In the invention, in the step (1), the molar ratio of the element A in the nitrate of the element A to the element B in the nitrate of the element B is 1: 1; the mole number of the citric acid ions is 1.3-1.8 times of that of the metal cations (namely A + B).
In the invention, in the step (2), the calcining temperature in the muffle furnace is between 200 and 900 ℃, and the calcining time is between 2 and 10 hours.
The invention also provides ABO prepared by the preparation method3A perovskite-type catalyst.
The invention further provides the ABO3The application method of the perovskite catalyst in the plasma concerted catalysis of VOCs comprises the following steps: ABO (ethylene-propylene-oxide copolymer)3After being ground, the perovskite catalyst is independently placed in a discharge area in plasma, or is simultaneously placed in the discharge area and the discharge area for concerted catalysis. Preferably, ABO is3Perovskite catalyst in air atmospherePretreating the plasma in the enclosure for 0.5-5 hours, and then independently placing the plasma in a discharge area in the plasma, or placing the plasma in the discharge area and the discharge area simultaneously for carrying out concerted catalysis.
In the invention, the concentration of VOCs introduced into the plasma is between 100 and 1500ppm, the total flow rate of gas is between 250 and 1000ml/min, and the VOCs comprise any one or more of hydrocarbons, aromatics, ketones, esters, alcohols, ethers, aldehydes, amines or nitriles.
Compared with the prior art, the invention has the following advantages:
the perovskite catalyst prepared by the high-temperature self-melting method not only saves the preparation time cost of the catalyst, but also saves the production cost because no noble metal element exists;
the prepared catalyst and the plasma cooperatively catalyze the VOCs, so that the defect of independent use of a single technology is overcome, and the VOCs removing efficiency is high, and the environment is protected.
Drawings
FIG. 1 shows LaMnO3And CeMnO3The effect of single catalytic toluene removal is shown.
FIG. 2 shows LaMnO at various locations in conjunction with plasma3The effect of catalytic removal of toluene.
FIG. 3 is a plasma with a single CeMnO section3The effect of catalytic removal of toluene.
FIG. 4 shows plasma pretreated and untreated LaMnO3And (3) a synergistic effect graph of removing toluene by plasma.
FIG. 5 is a graph of plasma pretreated and untreated CeMnO3And (3) a synergistic effect graph of removing toluene by plasma.
FIG. 6 is a plasma synergistic one-segment LaMnO3And the effect of catalytic removal of toluene by LaOx and MnOx.
FIG. 7 is LaCoO3、LaFeO3And SrMnO3The effect of single catalytic toluene removal is shown.
FIG. 8 shows plasma cooperating one-stage LaCoO3The effect of catalytic removal of toluene.
FIG. 9 shows a plasma cooperating with a one-stage LaFeO3The effect of catalytic removal of toluene.
FIG. 10 is a plasma synergistic one-segment SrMnO3The effect of catalytic removal of toluene.
FIG. 11 shows plasma synergy for a one-segment LaMnO3The effect of catalytic acetone removal is shown.
Detailed Description
The technical solution of the present invention is further described by the following specific examples. The examples are not intended to limit the scope of protection.
Example 1
Adopts a high-temperature self-melting method to prepare LaMnO3A catalyst of the type (I) is provided. Respectively weighing 0.5mmol of lanthanum nitrate and manganese nitrate, directly mixing with citric acid to ensure that the mole number of the citric acid ions is 1.5 times of that of the metal cations, placing the obtained mixture in a muffle furnace, heating to 800 ℃, calcining for 2 hours to obtain LaMnO3A perovskite-type catalyst.
(one) LaMnO alone3Effect of removing toluene under action of catalyst
The experimental procedure was as follows: 1000ppm of toluene were introduced into the air at a total gas flow rate of 1000ml/min, and 0.1g of this catalyst was taken and its catalytic action on toluene was examined when it was used alone. The toluene removal rate is shown in FIG. 1. As can be seen from the figure, LaMnO3When the catalyst is used alone, the catalytic efficiency of the p-toluene is not high and does not reach 80%.
Effect of (II) plasma on removing toluene
The experimental procedure was as follows: the removal of toluene only under the action of plasma was examined by introducing 1000ppm of toluene into the air at a total gas flow rate of 1000ml/min and an input power of 43W-53W at normal temperature and pressure. The toluene removal rate is shown in FIG. 2. As can be seen from the figure, the removal efficiency of toluene is 74% only when the plasma is applied.
Application of plasma concerted catalysis in toluene removal
The experimental procedure was as follows: introducing 1000ppm toluene into air, the total flow rate of the gas is 1000ml/min, the input power is in the range of 43W-53W at normal temperature and normal pressure, taking 0.1g of catalyst and plasma without adoptingThe same position relation is used for carrying out the concerted catalysis. The toluene removal rate is shown in FIG. 2. As can be seen from the figure, the plasma is compared to LaMnO either with the plasma alone to treat toluene or with the catalyst alone to catalyze toluene3When the catalyst is used in combination, the removal efficiency of the toluene is obviously improved no matter the catalyst is in a one-stage (IPC) or two-stage (PPC).
Example 2
Adopts a high-temperature self-melting method to prepare CeMnO3A catalyst of the type (I) is provided. Respectively weighing 0.5mmol of cerium nitrate and manganese nitrate, directly mixing with citric acid to ensure that the mole number of citric acid ions is 1.5 times of that of metal cations, placing the obtained mixture in a muffle furnace, heating to 850 ℃, calcining for 2 hours to obtain CeMnO3A perovskite-type catalyst.
(one) Single CeMnO3Effect of removing toluene under action of catalyst
The experimental procedure was as follows: 1000ppm of toluene were introduced into the air at a total gas flow rate of 1000ml/min, and 0.1g of this catalyst was taken and its catalytic action on toluene was examined when it was used alone. The toluene removal rate is shown in FIG. 1. As can be seen from the figure, CeMnO3The catalytic efficiency of p-toluene when the catalyst is used alone is only 68%.
Application of (II) plasma in removal of toluene through concerted catalysis
The experimental procedure was as follows: 1000ppm toluene is introduced into the air, the total flow rate of the gas is 1000ml/min, the input power is in the range of 43W-53W at normal temperature and normal pressure, 0.1g of catalyst and plasma are taken to carry out one-stage (IPC) concerted catalysis. The toluene removal rate is shown in FIG. 3. As can be seen from the figure, the plasma is compared to CeMnO either alone for treating toluene or alone for catalyzing toluene3When the catalyst is used in combination, the toluene removal efficiency is obviously improved.
Example 3
LaMnO prepared in example 13Catalyst and CeMnO prepared in example 23The catalyst and the catalyst are respectively pretreated by plasma in the air atmosphere for 1 hour and then are co-processed with the plasmaAnd (4) processing toluene. 1000ppm toluene is introduced into the air, the total gas flow rate is 1000ml/min, and when the input power of the plasma is 51W at normal temperature and normal pressure, 0.1g of catalyst and the plasma are taken to perform one-stage (IPC) concerted catalysis for 120 minutes. The results are shown in FIGS. 4 and 5. As can be seen from the figure, LaMnO after plasma pretreatment3And CeMnO3The removal efficiency of the toluene is as high as 97%. LaMnO after plasma pretreatment3And CeMnO3The removal efficiency of p-toluene is significantly higher than that of the catalyst without plasma pretreatment.
Example 4
In the embodiment, LaMnO is prepared by adopting a high-temperature self-melting method3LaOx and MnOx, and adopts one-stage cooperative LaMnO for plasma3Experiments for catalytically removing toluene by using LaOx and MnOx and experiments for catalytically removing toluene by using a single catalyst. 1000ppm toluene is introduced into the air, the total gas flow rate is 1000ml/min, and when the input power of the plasma is 51W at normal temperature and normal pressure, 0.1g of catalyst and (or not) the plasma are adopted to perform one-stage (IPC) concerted catalysis for 120 minutes. The results are shown in FIG. 6. As can be seen from the figure, the plasma cooperates with LaMnO3The removal efficiency of p-toluene is higher than that of plasma-co-LaOx and MnOx and that of toluene catalyzed by each catalyst alone, due to the co-action between lanthanum and manganese.
Example 5
In the embodiment, a high-temperature self-melting method is adopted to prepare LaCoO3A catalyst of the type (I) is provided. Respectively weighing 0.5mmol of lanthanum nitrate and cobalt nitrate, directly mixing with citric acid to ensure that the mole number of citric acid ions is 1.5 times of that of metal cations, placing the obtained mixture in a muffle furnace, heating to 850 ℃, calcining for 3 hours to obtain LaCoO3A perovskite-type catalyst.
(one) LaCoO alone3Effect of removing toluene under action of catalyst
The experimental procedure was as follows: 1000ppm of toluene were introduced into the air at a total gas flow rate of 1000ml/min, and 0.1g of this catalyst was taken and its catalytic action on toluene was examined when it was used alone. The toluene removal rate is shown in FIG. 7. From the figureAs can be seen, LaCoO3When the catalyst is used alone, the catalytic efficiency of the p-toluene is not high and does not reach 60%.
Application of (II) plasma in removal of toluene through concerted catalysis
The experimental procedure was as follows: 1000ppm toluene is introduced into the air, the total flow rate of the gas is 1000ml/min, the input power is in the range of 43W-53W at normal temperature and normal pressure, 0.1g of catalyst and plasma are taken to carry out one-stage (IPC) concerted catalysis. The toluene removal rate is shown in fig. 8. As can be seen from the figure, the plasma is compared to LaCoO compared to either treating toluene with plasma alone or catalyzing toluene with the catalyst alone3When the catalyst is used in combination, the toluene removal efficiency is obviously improved.
Example 6
In this example, a LaFeO was prepared by a high temperature self-melting method3A catalyst of the type (I) is provided. Respectively weighing 0.5mmol of lanthanum nitrate and ferric nitrate, directly mixing with citric acid to ensure that the mole number of citric acid ions is 1.5 times of that of metal cations, placing the obtained mixture in a muffle furnace, heating to 750 ℃, calcining for 5 hours to obtain LaFeO3A perovskite-type catalyst.
(one) LaFeO alone3Effect of removing toluene under action of catalyst
The experimental procedure was as follows: 1000ppm of toluene were introduced into the air at a total gas flow rate of 1000ml/min, and 0.1g of this catalyst was taken and its catalytic action on toluene was examined when it was used alone. The toluene removal rate is shown in FIG. 7. As can be seen from the figure, LaFeO3When the catalyst is used alone, the catalytic efficiency of the p-toluene is not high and does not reach 55%.
Application of (II) in removal of toluene by plasma concerted catalysis
The experimental procedure was as follows: 1000ppm toluene is introduced into the air, the total flow rate of the gas is 1000ml/min, the input power is in the range of 43W-53W at normal temperature and normal pressure, 0.1g of catalyst and plasma are taken to carry out one-stage (IPC) concerted catalysis. The toluene removal rate is shown in fig. 9. As can be seen from the figure, the catalyst catalyzes the toluene phase as compared to the plasma treatment of toluene alone or as compared to the use of the catalyst aloneRatio of plasma to LaFeO3When the catalyst is used in combination, the toluene removal efficiency is obviously improved.
Example 7
In the embodiment, SrMnO is prepared by adopting a high-temperature self-melting method3A catalyst. Respectively weighing 0.5mmol of strontium nitrate and manganese nitrate, directly mixing with citric acid to ensure that the mole number of citric acid ions is 1.5 times of that of metal cations, placing the obtained mixture in a muffle furnace, heating to 800 ℃, calcining for 2 hours to obtain SrMnO3A perovskite-type catalyst.
(one) SrMnO alone3Effect of removing toluene under action of catalyst
The experimental procedure was as follows: 1000ppm of toluene were introduced into the air at a total gas flow rate of 1000ml/min, and 0.1g of this catalyst was taken and its catalytic action on toluene was examined when it was used alone. The toluene removal rate is shown in FIG. 7. As can be seen from the figure, SrMnO3When the catalyst is used alone, the catalytic efficiency of the p-toluene is not high and does not reach 62%.
Application of (II) in removal of toluene by plasma concerted catalysis
The experimental procedure was as follows: introducing 1000ppm toluene into air, the total flow rate of the gas is 1000ml/min, the input power is in the range of 43W-53W at normal temperature and normal pressure, and 0.1g SrMnO is taken3The catalyst and the plasma adopt one-stage (IPC) for concerted catalysis. The toluene removal rate is shown in fig. 10. As can be seen from the figure, the plasma is in comparison with SrMnO either when the plasma is used alone to treat toluene or when the catalyst is used alone to catalyze toluene3When the catalyst is used in combination, the removal efficiency of toluene is obviously improved, and the removal efficiency is more than 85% after the plasma power is more than 50W.
Example 8
In the embodiment, LaMnO is prepared by adopting a high-temperature self-melting method3The catalyst (same as example 1) was used to detect the application of the catalyst in plasma-assisted catalysis of VOCs. Introducing 500ppm acetone into air, controlling the total gas flow rate at 1000ml/min and the input power at 43-53W at normal temperature and pressure, taking 0.1g catalyst and plasma, and performing one-stage catalysis (IPC)And (4) transforming. The acetone removal rate is shown in fig. 11. As can be seen from the figure, the plasma cooperates with LaMnO3The efficiency of removing the acetone is higher than that of the plasma acting alone, and the highest efficiency can reach 84%.
The above embodiments are illustrative of the present invention, and are not intended to limit the present invention, and any modifications of the present invention are within the scope of the present invention.

Claims (9)

1. ABO3A process for the preparation of a perovskite catalyst, characterized in that ABO3In the perovskite catalyst, A is one or more lanthanide metal elements, B is one or more selected from Ti, V, Cr, Mn, Fe, Co, Ni or Cu, and ABO3The perovskite catalyst is prepared by a high-temperature self-melting method, and the method comprises the following specific steps:
(1) respectively taking nitrates of A and B and directly mixing the nitrates with citric acid;
(2) placing the mixture obtained in the step (1) in a muffle furnace for calcining and crystallizing to obtain ABO3A perovskite-type catalyst.
2. The preparation method according to claim 1, wherein A is selected from any one or more of La, Ce, Sm or Gd; b is selected from any one or more of Fe, Co, Ti, V and Mn.
3. The method of claim 1, wherein ABO is3In the perovskite catalyst, partial metal elements C are selected to replace A or B by isomorphism replacement, and C is selected from one or more of Ga and Sr.
4. The production method according to claim 1, wherein in the step (1), the molar ratio of the element A in the nitrate salt of A to the element B in the nitrate salt of B is 1: 1; the mole number of the citric acid ions is 1.3-1.8 times of that of the metal cations.
5. The method according to claim 1, wherein in the step (2), the temperature of the muffle furnace is 200-900 ℃ and the time of the muffle furnace is 2-10 hours.
6. ABO prepared by the preparation method according to any one of claims 1 to 53A perovskite-type catalyst.
7. An ABO according to claim 63The application of the perovskite catalyst in the plasma concerted catalysis of VOCs is characterized in that the application method is as follows: ABO (ethylene-propylene-oxide copolymer)3After being ground, the perovskite catalyst is independently placed in a discharge area in plasma, or is simultaneously placed in the discharge area and the discharge area for concerted catalysis.
8. Use according to claim 7, characterized in that ABO is applied3After the perovskite catalyst is pretreated by plasma in the air atmosphere for 0.5-5 hours, the perovskite catalyst is independently placed in a discharge area in the plasma, or is placed in the discharge area and the discharge area simultaneously for concerted catalysis.
9. The use according to claim 7, wherein the concentration of VOCs introduced into the plasma is between 100 and 1500ppm, the total flow rate of gas is between 250 and 1000ml/min, and the VOCs comprise any one or more of hydrocarbons, aromatics, ketones, esters, alcohols, ethers, aldehydes, amines or nitriles.
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CN113385184A (en) * 2021-05-24 2021-09-14 浙江工商大学 Mn-Co-La composite catalyst for catalyzing and degrading VOCs (volatile organic compounds) by synergistic discharge plasma and preparation method and application thereof

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