CN111822009A - Low-temperature desulfurization and denitrification catalyst and preparation method thereof - Google Patents
Low-temperature desulfurization and denitrification catalyst and preparation method thereof Download PDFInfo
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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
- B01J27/02—Sulfur, selenium or tellurium; Compounds thereof
- B01J27/053—Sulfates
- B01J27/055—Sulfates with alkali metals, copper, gold or silver
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- 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
- B01D53/8637—Simultaneously removing sulfur oxides and nitrogen oxides
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- 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
- B01D53/8643—Removing mixtures of carbon monoxide or hydrocarbons and nitrogen oxides
- B01D53/8646—Simultaneous elimination of the components
- B01D53/865—Simultaneous elimination of the components characterised by a specific catalyst
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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
- B01J23/002—Mixed oxides other than spinels, e.g. perovskite
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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
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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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0201—Impregnation
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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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
- B01J37/088—Decomposition of a metal salt
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/502—Carbon monoxide
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
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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
- B01J2523/00—Constitutive chemical elements of heterogeneous catalysts
Abstract
The invention discloses a low-temperature desulfurization and denitrification catalyst and a preparation method thereof. The low-temperature desulfurization and denitrification catalyst takes low-cost clay and fly ash as catalyst carriers, the active ingredients of the low-temperature catalyst are firstly dissolved by hydrochloric acid through nitric acid pre-oxidation (acidification), and then the metal oxides are attached to the carriers of the low-temperature desulfurization and denitrification catalyst by an equivalent impregnation method to form the low-temperature desulfurization and denitrification catalyst. The low-temperature desulfurization and denitrification catalyst disclosed by the invention is simple in preparation process and low in cost, can realize the technical effect of desulfurization and denitrification, is simple and convenient to use, reduces the treatment cost and treatment difficulty of enterprises, and has a huge industrial application value.
Description
Technical Field
The invention relates to the field of catalysts and preparation thereof, in particular to a catalyst containing manganese cerium iron copper oxide.
Background
At present, the air pollution condition in China is increasingly serious, wherein the smoke emission of a boiler (kiln) is huge, and the air quality in China is seriously influenced. The flue gas of the boiler (kiln) contains a large amount of sulfur dioxide (SO)2) And Nitrogen Oxides (NO)x) And both are also the main components of haze and the main pollution source of atmospheric pollution. Therefore, sulfur dioxide (SO) in flue gas of boiler (kiln)2) And Nitrogen Oxides (NO)x) Becomes one of the key pollutants for prevention and treatment in China. Since the 70 s of the 20 th century, the nation has successively made strict restrictions on the emission of nitric oxide from coal-fired industrial boilers (kilns), and as scientific and technical and economic construction progresses, the restrictions on the emission have become more and more strict.
During the combustion process of coal, most of combustible substances in the coal can be burnt out in a kiln, and the rest of non-combustible substances are mainly ash, and the non-combustible ash and gas are combined together to form a large amount of waste flue gas containing a large amount of SO2、NO、CO、CO2And hydrocarbons, which are major sources of atmospheric environmental pollution.
At present, in the aspect of preparing the boiler (kiln) flue gas desulfurization and denitration catalysts at home and abroad, NO is removed by independently preparingxCatalyst and SO removal2The catalyst is the main catalyst. The environmental protection design unit is in the process of treating the flue gas of the boiler (kiln) to remove NOxSO removal2In the technical design aspect, the SO in the waste flue gas also needs to be determined2And NOxContent of (A) and SO in the local environmental protection sector2And NOxRespectively designed and manufactured to remove NOxAnd SO removal2Two different reaction devices are used, and then the two devices are arranged in a front-to-back order. In the practical application process, there are several important problems in such an approach: firstly, the design process is complex; secondly, the occupied area is large; thirdly, the manufacturing cost and the energy consumption are high; fourthly for environmental management enterprisesTreatment costs and treatment difficulties are increased. These problems are NOxAnd SO2The treatment of (a) presents significant difficulties and challenges.
At present, the prior art does not have any reference to the capability of removing SO2While removing NOxThe preparation of the catalyst and the related application technology. Therefore, the method can be prepared under the low-temperature (160-250 ℃) environment without using a reducing agent and can remove SO in flue gas of an industrial boiler (kiln)2Can remove NO at the same timexThe catalysts of (a) have great industrial application requirements.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provide a low-temperature desulfurization and denitrification catalyst and a preparation method thereof.
In order to solve the technical problems, the invention adopts the following technical scheme:
the low-temperature desulfurization and denitrification catalyst comprises a catalyst carrier, wherein a catalyst active component is loaded on the catalyst carrier.
The catalyst carrier consists of the following components:
the catalyst active ingredients comprise the following components by weight of the catalyst carrier:
further, the molar ratio of the element Mn to the element Ce in the low-temperature desulfurization and denitrification catalyst is 4: 1.
further, the content of Mn oxide in the low-temperature desulfurization and denitrification catalyst is 5-25 wt% based on 100% of metal oxide by mass; the content of the oxide of Ce is 1-4 wt%.
Further, the clay material is one or more of kaolinite clay, sericite clay and montmorillonite clay.
The invention also provides a preparation method of the low-temperature desulfurization and denitrification catalyst, which comprises the following steps:
(1) mixing 35 parts of montmorillonite clay, 25 parts of zeolite, 1.5 parts of ignition loss agent, 30 parts of diatomite, 2.5 parts of ferric oxide and 1 part of copper oxide according to a proportion, adding proper water, uniformly stirring into a mud shape, and naturally aging in a cool and dry place;
(2) the aged blank mud is subjected to compression molding or extrusion molding to obtain a required catalyst blank;
(3) naturally drying the green body in the shade for 24 hours, then placing the green body in a hot air drying furnace at the temperature of 200 ℃ for drying for 2 hours, and placing the dried catalyst green body in a muffle furnace at the temperature of 950 ℃ for 8 hours to obtain a multi-gap foam ceramic-based catalyst carrier;
(4) soaking the porous foam ceramic-based catalyst carrier in 35% nitric acid for acidification, wherein the soaking time is 2 hours;
(5) the active components of the catalyst are attached to the surface of the catalyst carrier by an equivalent impregnation method;
(6) calculating the weight of the required solution and the weight of various catalyst active components according to the water absorption of the catalyst carrier, wherein the weight of manganese acetate, cerium nitrate, copper sulfate and ferrous sulfate is 9 wt%, 3 wt%, 2 wt% and 1 wt%, respectively, and dissolving the components in a proper amount of water to prepare an aqueous solution containing the catalyst carrier active components;
(7) soaking a catalyst carrier into an aqueous solution containing active ingredients of the catalyst carrier for 2 hours, taking out the catalyst carrier, and drying the catalyst carrier at 200 ℃ for 10 hours;
(8) and (3) placing the dried catalyst in a muffle furnace at 950 ℃ for 8h to obtain the catalyst capable of removing CO, SO2 and NOx simultaneously. Further, the shape of the catalyst body in the step (2) is one or more of honeycomb shape, spherical shape and plate shape.
Further, the volume of the hydrochloric acid solution in the step (4) is equal to the water absorption capacity of the catalyst carrier.
Further, the drying method in the step (5) is one of hot air drying, infrared drying, microwave drying and natural drying.
Further, the heating temperature in the step (6) is 220-240 ℃.
Further, the heating temperature in the step (6) is 230 ℃.
Compared with the prior art, the invention has the beneficial technical effects that:
the low-temperature desulfurization and denitrification catalyst is prepared by using cheap clay and fly ash as catalyst carriers, carrying out nitric acid pre-oxidation (acidification), dissolving active ingredients of the low-temperature catalyst by hydrochloric acid, and then adhering metal oxides to the carrier of the low-temperature desulfurization and denitrification catalyst by an equivalent impregnation method. By controlling the heating temperature, the excellent lattice density of the active ingredients of the catalyst is ensured, the phase change which is not beneficial to catalytic reaction and is formed by metal oxides in the active ingredients is avoided, and the nitrogen oxide can be reduced without any additional reducing agent.
The low-temperature desulfurization and denitrification catalyst disclosed by the invention is simple in preparation process and low in cost, can realize the technical effect of desulfurization and denitrification, reduces the treatment cost and treatment difficulty of enterprises, and has a huge industrial application value.
Detailed Description
The invention will be further described with reference to the following examples of 4 ton gas boiler waste flue gas treatment by the Changyuan brewing Co., Ltd, Chengde, Hebei province, but it should be understood that these examples are for illustrative purposes only and should not be construed as limiting the practice of the invention.
Example 1
(1) Adding part of water into 36 parts of montmorillonite clay, 25 parts of fly ash, 1.5 parts of ignition loss agent, 37 parts of diatomite and 0.5 part of engine oil to ensure that the water content is 28 percent, mixing, ageing, compression molding, shaping, drying, and roasting at 950 ℃ to obtain a carrier of the multi-gap foam ceramic-based catalyst;
(2) soaking the porous foam ceramic-based catalyst carrier in 35% nitric acid for acidification, wherein the soaking time is 2 hours;
(3) respectively weighing MnO accounting for 4.2 percent of the weight of the catalyst carrier23.3% of CeO2And 2.5% CuO. These weighed medicines of the catalyst active ingredient were slowly poured into a hydrochloric acid tank filled with a concentration of 20% a plurality of times (ten million cares were paid not to quickly pour the medicines into the hydrochloric acid tank once) to obtain a hydrochloric acid solution containing the catalyst active ingredient.
(4) The porous foamed ceramic-based catalyst carrier acidified by nitric acid is equivalently immersed in hydrochloric acid solution containing catalyst active ingredients for 2.5h and then taken out, and then the taken-out porous foamed ceramic-based catalyst carrier is dried for 10 h.
(5) And (3) putting the dried catalyst into a muffle furnace, and heating for 10 hours at the temperature of 200 ℃ to prepare the low-temperature desulfurization and denitrification catalyst.
The low-temperature desulfurization and denitrification catalyst prepared by the embodiment is applied to the practical application of 4-ton gas boiler waste flue gas treatment of Changyuan brewing Co Ltd in Chengde city, Hebei province, and SO in flue gas before and after treatment by the catalyst is respectively measured2And NOxThe case (1).
TABLE 1 actual detection situation for flue gas treatment of gas-fired boiler
As can be seen from Table 1, the SO in the boiler flue gas after the treatment with the catalyst described herein2And NOxThe content is obviously reduced, and the removal rates of the two reach 85.7 percent and 77.8 percent respectively. After treatment, SO in the flue gas2And NOxThe content is far lower than the emission standard, and the removal effect is good.
The above-described embodiments are merely illustrative of the preferred embodiments of the present invention, and do not limit the scope of the present invention, and various modifications and improvements of the technical solutions of the present invention can be made by those skilled in the art without departing from the spirit of the present invention, and the technical solutions of the present invention are within the scope of the present invention defined by the claims.
Claims (10)
1. The low-temperature desulfurization and denitrification catalyst is characterized by comprising a catalyst carrier, wherein a catalyst active component is loaded on the catalyst carrier;
wherein the catalyst support comprises the following components:
the catalyst active ingredients comprise the following components by weight of the catalyst carrier:
2. the low-temperature desulfurization and denitrification catalyst according to claim 1, wherein the molar ratio of the element Mn to the element Ce in the catalyst is 4: 1.
3. The low-temperature desulfurization and denitrification catalyst according to claim 1, wherein the content of the oxide of Mn is 5-25 wt% based on 100% by mass of the metal oxide; the content of the oxide of Ce is 1-4 wt%.
4. The low-temperature desulfurization and denitrification catalyst according to claim 1, wherein the clay material is one or more of kaolinite clay, sericite clay and montmorillonite clay.
5. The low-temperature desulfurization and denitrification catalyst according to claim 1, wherein the ignition loss agent is flour.
6. The preparation method of the low-temperature desulfurization and denitrification catalyst according to claims 1-5, characterized by comprising the following steps:
(1) mixing the raw materials of the catalyst carrier in proportion, adding a proper amount of water, uniformly stirring into a mud shape, and placing the mud in a cool and dry place for aging;
(2) molding or extruding the aged mud-like substance by a molding press or an extruder to obtain a catalyst green body;
(3) placing the green body in a shade drying place for naturally drying in the shade for 24h, then drying for 2-4h by hot air at 200 ℃, placing the dried catalyst green body in a muffle furnace, and roasting for 8h at 950 ℃ to obtain a multi-gap foam ceramic-based catalyst green body;
(4) immersing the porous foam ceramic-based catalyst blank into a nitric acid solution with the concentration of 35%, soaking for 2h, and naturally drying in the shade to obtain a catalyst carrier;
(5) weighing the catalyst active ingredients according to a proportion, slowly adding the weighed catalyst active ingredients into a 25% hydrochloric acid solution for multiple times, and fully stirring to prepare a hydrochloric acid solution containing the catalyst active ingredients;
(6) soaking a catalyst carrier in a hydrochloric acid solution containing a catalyst active component for 2-4h, taking out, and drying by hot air at 200 ℃ for 10-24 h;
(7) and (3) placing the dried catalyst carrier in a muffle furnace, and heating for 8-15h at the temperature of 200-250 ℃ to obtain a finished product of the low-temperature desulfurization and denitrification catalyst.
7. The method for preparing a catalyst for low-temperature desulfurization and denitrification according to claim 6, wherein the volume of the hydrochloric acid solution in the step (4) is calculated from the water absorption of the catalyst carrier. The water absorption of the catalyst carrier is determined by experimental data obtained from practical experiments, and the water absorption of a general catalyst carrier is 38% -50%.
8. The method for preparing the catalyst for low-temperature desulfurization and denitration according to claim 6, wherein the drying method in the step (5) is one of hot air drying, infrared drying, microwave drying and natural drying.
9. The method for preparing a low-temperature desulfurization and denitrification catalyst according to claim 3, wherein the heating temperature in the step (6) is 220 ℃ to 240 ℃.
10. The method for preparing a low-temperature desulfurization and denitrification catalyst according to claim 3, wherein the heating temperature in step (6) is 230 ℃.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114452811A (en) * | 2021-12-27 | 2022-05-10 | 深圳华明环保科技有限公司 | Desulfurization and denitrification agent and preparation method thereof |
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