CN114700083A - Composite catalyst for low-concentration VOC and preparation method thereof - Google Patents

Composite catalyst for low-concentration VOC and preparation method thereof Download PDF

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CN114700083A
CN114700083A CN202210461307.6A CN202210461307A CN114700083A CN 114700083 A CN114700083 A CN 114700083A CN 202210461307 A CN202210461307 A CN 202210461307A CN 114700083 A CN114700083 A CN 114700083A
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alumina
composite catalyst
nitrate solution
carrier
coating
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张鹏
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Hunan Litai Environmental Engineering Co ltd
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Hunan Litai Environmental Engineering Co ltd
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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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/889—Manganese, technetium or rhenium
    • B01J23/8892—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
    • B01D53/8678—Removing components of undefined structure
    • B01D53/8687—Organic components
    • 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
    • B01J23/002—Mixed oxides other than spinels, e.g. perovskite
    • 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
    • B01J35/61—Surface area
    • B01J35/615—100-500 m2/g
    • 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
    • B01J37/02—Impregnation, coating or precipitation
    • B01J37/0215—Coating
    • 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
    • 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
    • B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
    • 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 provides a composite catalyst for low-concentration VOC, which comprises a carrier and a coating, wherein the coating is arranged on the carrier, and the loading amount is 100-250 g/L; the coating comprises the following raw material components of an active component and a modifier, wherein the mass ratio of the active component to the modifier is 1:1-4: 1; the active components comprise copper oxide and manganese oxide; the modifier is modified gamma-alumina. The invention also provides a preparation method of the composite catalyst, which comprises the steps of S1, preparing modified gamma-alumina; step S2, preparing coating slurry; and step S3, preparing the composite catalyst. The composite catalyst prepared by the invention has low cost, is not easy to be poisoned and inactivated and has low catalysis temperature.

Description

Composite catalyst for low-concentration VOC and preparation method thereof
Technical Field
The invention relates to the technical field of volatile organic gas purification, in particular to a composite catalyst for low-concentration VOC and a preparation method thereof.
Background
The concentration of low-concentration volatile organic gases (VOC for short) in the atmosphere is generally not more than 2000mg/Nm3. Most of the existing catalysts for treating VOC are noble metal catalysts, the active ingredients of the catalysts mainly comprise platinum/palladium, and the content of the active ingredients is highUp to 500-2000 mg/L. Although the noble metal catalyst can treat high-concentration and low-concentration VOC, the active component of the noble metal catalyst, namely platinum/palladium, belongs to scarce noble metals and is expensive, so that the use cost of a client is high. In addition, VOC contains impurities such as P and silicone, which easily causes poisoning of the active ingredient platinum/palladium and loss of catalytic activity.
Disclosure of Invention
The invention aims to provide a composite catalyst for low-concentration VOC and a preparation method thereof, which are used for solving the problems of high cost and easy poisoning and inactivation of a noble metal catalyst. The specific technical scheme is as follows:
a composite catalyst for low-concentration VOC comprises a carrier and a coating, wherein the coating is arranged on the carrier and has an uploading amount of 100-250 g/L; the coating comprises the following raw material components of an active component and a modifier, wherein the mass ratio of the active component to the modifier is 1:1-4: 1; the active components comprise copper oxide and manganese oxide; the modifier is modified gamma-alumina.
In some embodiments, the mass ratio of copper oxide to manganese oxide is from 1:3 to 3: 1.
In some embodiments, the raw material components adopted by the modified gamma-alumina in the modification comprise strontium nitrate solution, yttrium nitrate solution and gamma-alumina; the mass ratio of the strontium nitrate solution to the yttrium nitrate solution to the gamma-alumina is 0.5:0.5:150-2:5: 150.
In some embodiments, the strontium nitrate solution is 30% to 60% by weight; the mass fraction of the yttrium nitrate solution is 40-65%.
In some embodiments, the support is a ceramic support or an iron-chromium-aluminum alloy support; the porosity of the ceramic carrier or the iron-chromium-aluminum alloy carrier is 200-400 meshes.
The preparation method of the composite catalyst for low-concentration VOC comprises the following steps:
step S1, preparing modified gamma-alumina
Firstly, weighing gamma-alumina with required mass, adding strontium nitrate solution and yttrium nitrate solution with required mass, and stirring for 2-4 h; secondly, adding a thickening agent, and continuously stirring for 20-25 h; then, dropwise adding a pH regulator until the pH value is 10-11 to obtain a pre-preparation; finally, drying and roasting the pre-preparation to obtain modified gamma-alumina;
step S2, preparing coating slurry
Weighing modified gamma-alumina and active components with required mass, adding the modified gamma-alumina and the active components into water, stirring for 1-3h, and then ball-milling until D90 is 20-25 mu m to obtain coating slurry;
step S3, preparing composite catalyst
Coating the coating slurry with the required loading amount on a carrier, and drying and roasting to obtain the composite catalyst.
In some embodiments, in step S1, the thickener is hydroxymethyl cellulose used in an amount of 0.08 to 0.12 times that of γ -alumina; the pH regulator is sodium hydroxide solution; the drying temperature is 110-120 ℃; the roasting temperature is 550-650 ℃, and the roasting time is 4.5-5.5 h.
In some embodiments, in step S3, the drying temperature is 140-160 ℃; the roasting temperature is 500-600 ℃, and the roasting time is 3.5-4.5 h.
The technical scheme of the invention at least has the following beneficial effects:
(1) the composite catalyst for low-concentration VOC has high specific surface area reaching 150m by adopting active components of copper oxide and manganese oxide2More than g, is beneficial to the adsorption, reaction and desorption of low-concentration VOC; the active component accounts for a higher proportion, so that the active sites of the composite catalyst are increased, and the opportunity of contacting the low-concentration VOC with the active sites is improved; in addition, the cost of the active component is far lower than that of the noble metal platinum/palladium, the cost of the composite catalyst is greatly reduced, and the active components of copper oxide and manganese oxide have tolerance to impurities such as P, organic silicon and the like contained in VOC, so that the possibility of poisoning and inactivation is greatly reduced. The modified gamma-alumina is adopted, so that the high-temperature resistance stability and the oxidation performance of the composite catalyst can be greatly improved, the catalytic oxidation performance of the composite catalyst is further improved, the conversion rate of organic waste gas is conveniently improved, and the purification effect is realized. The invention is coatedThe arrangement of the layer loading amount enhances the adsorption of low-concentration VOC on the composite catalyst coating, and improves the mass transfer efficiency. The composite catalyst prepared by the invention is suitable for treating low-concentration VOC, can reduce the catalysis temperature and saves energy.
(2) The preparation method of the composite catalyst for low-concentration VOC has the advantages of simple steps, convenient operation, easily controlled parameters and convenient popularization.
Detailed Description
The technical solutions in the present invention will be described clearly and completely with reference to the following embodiments of the present invention, and it should be understood that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments that can be derived by one of ordinary skill in the art from the embodiments given herein are intended to be within the scope of the present invention.
Example 1:
a composite catalyst for low-concentration VOC comprises a carrier and a coating, wherein the coating is arranged on the carrier and has an uploading amount of 100-250 g/L; the coating comprises the following raw material components of an active component and a modifier, wherein the mass ratio of the active component to the modifier is 3: 1; the active components comprise copper oxide and manganese oxide; the modifier is modified gamma-alumina.
The mass ratio of the copper oxide to the manganese oxide is 1: 3.
Raw material components adopted by the modified gamma-alumina during modification comprise strontium nitrate solution, yttrium nitrate solution and gamma-alumina; the mass ratio of the strontium nitrate solution to the yttrium nitrate solution to the gamma-alumina is 1.2:3.5: 150.
The mass fraction of the strontium nitrate solution is 45 percent; the mass fraction of the yttrium nitrate solution is 50%.
The carrier is a ceramic carrier (the size is 150mm multiplied by 50mm), and the porosity of the carrier is 400 meshes.
The preparation method of the composite catalyst for low-concentration VOC comprises the following steps:
step S1, preparing modified gamma-alumina
Firstly, weighing 150g of gamma-alumina, adding 1.2g of strontium nitrate solution and 3.5g of yttrium nitrate solution, and stirring for 3 h; secondly, 18g of thickening agent (specifically hydroxymethyl cellulose) is added, and stirring is continued for 24 hours; then, dropwise adding a pH regulator (specifically a sodium hydroxide solution, the mass fraction is 30%) until the pH is 11 to obtain a pre-preparation; finally, drying the pre-preparation at 120 ℃ and roasting at 600 ℃ for 5h to prepare modified gamma-alumina;
step S2, preparing coating slurry
Weighing 100g of modified gamma-alumina and 300g of active component, adding into 1250g of water, stirring for 2h, and ball-milling until D90 is 25 mu m to obtain coating slurry;
step S3, preparing composite catalyst
And uniformly coating 225g of coating slurry on a carrier, and drying at 150 ℃ and roasting at 550 ℃ for 4 hours to obtain the composite catalyst.
Example 2:
unlike example 1, in step S1, the strontium nitrate solution was used in an amount of 4g, the yttrium nitrate solution was used in an amount of 8g, and the thickener was used in an amount of 15 g.
Example 3:
unlike example 1, in step S2, the modified gamma-alumina was used in an amount of 300g, and the active component was used in an amount of 100 g.
Example 4:
unlike example 1, in step S1, the strontium nitrate solution was used in an amount of 4g, the yttrium nitrate solution was used in an amount of 8g, and the thickener was used in an amount of 15 g; in step S2, the modified gamma-alumina was used in an amount of 300g, and the active component was used in an amount of 100 g.
Example 5:
unlike example 1, in step S1, the strontium nitrate solution was used in an amount of 3g, and the yttrium nitrate solution was used in an amount of 6 g; in step S2, the modified gamma-alumina was used in an amount of 200g, and the active component was used in an amount of 200 g.
Comparative example 1:
adding 400g of unmodified gamma-alumina into 1250g of water, stirring for 2 hours, and then ball-milling until D90 is 25 mu m to obtain coating slurry; adding a platinum nitrate solution, and stirring the mixture until the mixture is uniform, wherein the mass of the platinum nitrate is 659mg relative to the dosage of 1L of finished noble metal catalyst prepared finally; uniformly coating a coating layer with the net content of 112.5g on a carrier (specifically a ceramic carrier (the size is 150mm multiplied by 50mm), the porosity of which is 400 meshes) by adopting a quantitative coating technology, drying at 150 ℃, and then roasting at 550 ℃ for 4 hours to obtain the finished product of the noble metal catalyst.
Comparative example 2:
adding 350g of unmodified gamma-alumina and 50g of copper oxide into 1250g of water, stirring for 2 hours, and then ball-milling until D90 is 25 micrometers to obtain coating slurry; adding a platinum nitrate solution, and stirring the mixture until the mixture is uniform, wherein the mass of the platinum nitrate is 659mg relative to the dosage of 1L of finished noble metal catalyst prepared finally; uniformly coating a coating layer with the net content of 112.5g on a carrier (specifically a ceramic carrier (the size is 150mm multiplied by 50mm), the porosity of which is 400 meshes) by adopting a quantitative coating technology, drying at 150 ℃, and then roasting at 550 ℃ for 4 hours to obtain the finished product of the noble metal catalyst.
Comparative example 3:
adding 350g of unmodified gamma-alumina, 25g of copper oxide and 25g of manganese oxide into 1250g of water, stirring for 2 hours, and then ball-milling until D90 is 25 micrometers to obtain coating slurry; adding a platinum nitrate solution, and stirring the mixture until the mixture is uniform, wherein the mass of the platinum nitrate is 659mg relative to the dosage of 1L of finished noble metal catalyst prepared finally; uniformly coating a coating layer with the net content of 112.5g on a carrier (specifically a ceramic carrier (the size is 150mm multiplied by 50mm), the porosity of which is 400 meshes) by adopting a quantitative coating technology, drying at 150 ℃, and then roasting at 550 ℃ for 4 hours to obtain the finished product of the noble metal catalyst.
Comparative example 4:
adding 400g of strontium nitrate (the mass is 3.2g) modified gamma-alumina into 1250g of water, stirring for 2h, and then ball-milling until the D90 is 25 mu m to obtain coating slurry; adding a platinum nitrate solution, and stirring the mixture until the mixture is uniform, wherein the mass of the platinum nitrate is 659mg relative to the dosage of 1L of finished noble metal catalyst prepared finally; uniformly coating a coating layer with the net content of 112.5g on a carrier (specifically a ceramic carrier (the size is 150mm multiplied by 50mm), the porosity of which is 400 meshes) by adopting a quantitative coating technology, drying at 150 ℃, and then roasting at 550 ℃ for 4 hours to obtain the finished product of the noble metal catalyst.
Comparative example 5:
adding 350g of strontium nitrate (the mass is 2.8g) modified gamma-alumina, 25g of copper oxide and 25g of manganese oxide into 1250g of water, stirring for 2 hours, and then ball-milling until the D90 is 25 mu m to obtain coating slurry; adding a platinum nitrate solution, and stirring the mixture until the mixture is uniform, wherein the mass of the platinum nitrate is 659mg relative to the dosage of 1L of finished noble metal catalyst prepared finally; uniformly coating a coating layer with the net content of 112.5g on a carrier (specifically a ceramic carrier (the size is 150mm multiplied by 50mm), the porosity of which is 400 meshes) by adopting a quantitative coating technology, drying at 150 ℃, and then roasting at 550 ℃ for 4 hours to obtain the finished product of the noble metal catalyst.
The composite catalysts prepared in examples 1 to 5 and the noble metal catalyst prepared in comparative example 1 were subjected to a fresh-state catalytic performance test and an aged-state catalytic performance test, respectively, and the test procedures were as follows:
1) fresh state catalytic performance test
100 parts by mass of each of the composite catalysts prepared in examples 1 to 5 and the noble metal catalyst prepared in comparative example 1 was subjected to fresh-state catalytic performance test without aging treatment. The test conditions were as follows: 200ppm of propylene, 10% (volume fraction) O25% (volume fraction) H2O, using N as balance gas2The reaction temperature is between room temperature and 300 ℃, and the space velocity is 20000h-1。
2) Aging state catalytic performance test
100 parts of a composite catalyst prepared in examples 1 to 5 and a precious metal catalyst prepared in comparative example 1, each having the same mass, were subjected to an aging-state catalytic performance test after aging treatment, wherein the aging conditions were as follows: the sample is placed in an aging test chamber for heat aging at 650 ℃ for 24 h. The test conditions were the same as 1).
T of the corresponding sample is obtained by 1) to 2) experimental tests50(indicating the temperature at which the conversion of the reactant propylene reached 50%) and sample T100(indicating the temperature at which the conversion of propylene as a reactant reached 100%), and the specific results are shown in Table 1.
TABLE 1
Figure BDA0003620532170000051
Figure BDA0003620532170000061
As is clear from the data in Table 1, the present invention performed T using the composite catalysts prepared in examples 1 to 5, as compared with comparative examples 1 to 550And T100With lower catalytic temperatures. This shows that the composite catalyst prepared by the invention has better catalytic oxidation performance.
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 (8)

1. The composite catalyst for low-concentration VOC is characterized by comprising a carrier and a coating, wherein the coating is arranged on the carrier and is loaded at the load amount of 100-250 g/L; the coating comprises the following raw material components of an active component and a modifier, wherein the mass ratio of the active component to the modifier is 1:1-4: 1; the active components comprise copper oxide and manganese oxide; the modifier is modified gamma-alumina.
2. The composite catalyst for low concentration VOC according to claim 1, wherein the mass ratio of copper oxide to manganese oxide is 1:3-3: 1.
3. The composite catalyst for low-concentration VOC according to claim 2, wherein the raw material components adopted in the modification of the modified γ -alumina include strontium nitrate solution, yttrium nitrate solution and γ -alumina; the mass ratio of the strontium nitrate solution to the yttrium nitrate solution to the gamma-alumina is 0.5:0.5:150-2:5: 150.
4. The composite catalyst for low-concentration VOC according to claim 3, wherein the mass fraction of the strontium nitrate solution is 30-60%; the mass fraction of the yttrium nitrate solution is 40-65%.
5. The composite catalyst for low concentration VOC according to claim 4, wherein said carrier is a ceramic carrier or an iron-chromium-aluminum alloy carrier; the porosity of the ceramic carrier or the iron-chromium-aluminum alloy carrier is 200-400 meshes.
6. A method for preparing the composite catalyst for low concentration VOC according to any one of claims 3-5, which comprises the following steps:
step S1, preparing modified gamma-alumina
Firstly, weighing gamma-alumina with required mass, adding strontium nitrate solution and yttrium nitrate solution with required mass, and stirring for 2-4 h; secondly, adding a thickening agent, and continuously stirring for 20-25 h; then, dropwise adding a pH regulator until the pH value is 10-11 to obtain a pre-preparation; finally, drying and roasting the pre-preparation to obtain modified gamma-alumina;
step S2, preparing coating slurry
Weighing modified gamma-alumina and active components with required mass, adding the modified gamma-alumina and the active components into water, stirring for 1-3h, and then ball-milling until D90 is 20-25 mu m to obtain coating slurry;
step S3, preparing composite catalyst
Coating the coating slurry with the required loading amount on a carrier, and drying and roasting to obtain the composite catalyst.
7. The method according to claim 6, wherein in step S1, the thickener is hydroxymethyl cellulose used in an amount of 0.08 to 0.12 times that of γ -alumina; the pH regulator is sodium hydroxide solution; the drying temperature is 110-120 ℃; the roasting temperature is 550-650 ℃, and the roasting time is 4.5-5.5 h.
8. The method as claimed in claim 6, wherein in step S3, the drying temperature is 140-160 ℃; the roasting temperature is 500-600 ℃, and the roasting time is 3.5-4.5 h.
CN202210461307.6A 2022-04-28 2022-04-28 Composite catalyst for low-concentration VOC and preparation method thereof Pending CN114700083A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115463668A (en) * 2022-09-29 2022-12-13 湖南立泰环境工程有限公司 Preparation method of catalyst and obtained catalyst
CN115463668B (en) * 2022-09-29 2023-12-08 湖南立泰环境工程有限公司 Preparation method of catalyst and catalyst obtained by preparation method

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