CN114618572A - High-efficiency decomposition of N2Bimetallic catalyst of O, preparation method and decomposition method thereof - Google Patents
High-efficiency decomposition of N2Bimetallic catalyst of O, preparation method and decomposition method thereof Download PDFInfo
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- 239000003054 catalyst Substances 0.000 title claims abstract description 53
- 238000000354 decomposition reaction Methods 0.000 title claims abstract description 27
- 238000000034 method Methods 0.000 title claims abstract description 15
- 238000002360 preparation method Methods 0.000 title claims abstract description 15
- 238000006243 chemical reaction Methods 0.000 claims abstract description 24
- 239000002808 molecular sieve Substances 0.000 claims abstract description 22
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 22
- 230000003197 catalytic effect Effects 0.000 claims abstract description 14
- 229910052707 ruthenium Inorganic materials 0.000 claims abstract description 10
- 229910052703 rhodium Inorganic materials 0.000 claims abstract description 9
- 229910052742 iron Inorganic materials 0.000 claims abstract description 6
- 229910052751 metal Inorganic materials 0.000 claims description 14
- 239000002184 metal Substances 0.000 claims description 14
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 9
- 238000001035 drying Methods 0.000 claims description 9
- 239000000843 powder Substances 0.000 claims description 9
- 239000000243 solution Substances 0.000 claims description 9
- 150000003839 salts Chemical class 0.000 claims description 6
- 238000003756 stirring Methods 0.000 claims description 6
- 238000003421 catalytic decomposition reaction Methods 0.000 claims description 4
- 239000012266 salt solution Substances 0.000 claims description 4
- BNGXYYYYKUGPPF-UHFFFAOYSA-M (3-methylphenyl)methyl-triphenylphosphanium;chloride Chemical compound [Cl-].CC1=CC=CC(C[P+](C=2C=CC=CC=2)(C=2C=CC=CC=2)C=2C=CC=CC=2)=C1 BNGXYYYYKUGPPF-UHFFFAOYSA-M 0.000 claims description 3
- PAWQVTBBRAZDMG-UHFFFAOYSA-N 2-(3-bromo-2-fluorophenyl)acetic acid Chemical compound OC(=O)CC1=CC=CC(Br)=C1F PAWQVTBBRAZDMG-UHFFFAOYSA-N 0.000 claims description 3
- KKCBUQHMOMHUOY-UHFFFAOYSA-N Na2O Inorganic materials [O-2].[Na+].[Na+] KKCBUQHMOMHUOY-UHFFFAOYSA-N 0.000 claims description 3
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 3
- ZSIQJIWKELUFRJ-UHFFFAOYSA-N azepane Chemical compound C1CCCNCC1 ZSIQJIWKELUFRJ-UHFFFAOYSA-N 0.000 claims description 3
- 230000015572 biosynthetic process Effects 0.000 claims description 3
- 239000003795 chemical substances by application Substances 0.000 claims description 3
- 229910052593 corundum Inorganic materials 0.000 claims description 3
- -1 halide salt Chemical class 0.000 claims description 3
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 3
- 238000002156 mixing Methods 0.000 claims description 3
- 238000007789 sealing Methods 0.000 claims description 3
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 claims description 3
- 229910001220 stainless steel Inorganic materials 0.000 claims description 3
- 239000010935 stainless steel Substances 0.000 claims description 3
- 238000003786 synthesis reaction Methods 0.000 claims description 3
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims 1
- 229910002651 NO3 Inorganic materials 0.000 claims 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 claims 1
- 150000001875 compounds Chemical class 0.000 claims 1
- 230000002194 synthesizing effect Effects 0.000 claims 1
- 238000011068 loading method Methods 0.000 abstract description 14
- 229910000510 noble metal Inorganic materials 0.000 abstract description 4
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 22
- 239000010948 rhodium Substances 0.000 description 12
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 11
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 9
- 230000000694 effects Effects 0.000 description 7
- 239000008367 deionised water Substances 0.000 description 6
- 229910021641 deionized water Inorganic materials 0.000 description 6
- 239000012065 filter cake Substances 0.000 description 6
- 238000001914 filtration Methods 0.000 description 6
- 238000010992 reflux Methods 0.000 description 6
- 238000005406 washing Methods 0.000 description 6
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 4
- VCJMYUPGQJHHFU-UHFFFAOYSA-N iron(3+);trinitrate Chemical compound [Fe+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VCJMYUPGQJHHFU-UHFFFAOYSA-N 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 4
- 239000012535 impurity Substances 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- 229910001868 water Inorganic materials 0.000 description 3
- WNLRTRBMVRJNCN-UHFFFAOYSA-N adipic acid Chemical compound OC(=O)CCCCC(O)=O WNLRTRBMVRJNCN-UHFFFAOYSA-N 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- VXNYVYJABGOSBX-UHFFFAOYSA-N rhodium(3+);trinitrate Chemical compound [Rh+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O VXNYVYJABGOSBX-UHFFFAOYSA-N 0.000 description 2
- YBCAZPLXEGKKFM-UHFFFAOYSA-K ruthenium(iii) chloride Chemical compound [Cl-].[Cl-].[Cl-].[Ru+3] YBCAZPLXEGKKFM-UHFFFAOYSA-K 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 159000000021 acetate salts Chemical class 0.000 description 1
- 239000001361 adipic acid Substances 0.000 description 1
- 235000011037 adipic acid Nutrition 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 238000004817 gas chromatography Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 150000002823 nitrates Chemical class 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 235000013842 nitrous oxide Nutrition 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
-
- 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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/72—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing iron group metals, noble metals or copper
- B01J29/76—Iron group metals or copper
- B01J29/7676—MWW-type, e.g. MCM-22, ERB-1, ITQ-1, PSH-3 or SSZ-25
-
- 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
- B01D53/8621—Removing nitrogen compounds
- B01D53/8625—Nitrogen oxides
- B01D53/8628—Processes characterised by a specific catalyst
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/40—Nitrogen compounds
- B01D2257/402—Dinitrogen oxide
-
- 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
- B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
- B01J2229/10—After treatment, characterised by the effect to be obtained
- B01J2229/18—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself
- B01J2229/186—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself not in framework positions
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Analytical Chemistry (AREA)
- Biomedical Technology (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Health & Medical Sciences (AREA)
- Crystallography & Structural Chemistry (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Catalysts (AREA)
Abstract
The invention belongs to N2The technical field of O treatment, in particular to a method for efficiently decomposing N2Bimetallic catalyst of O, its preparation method and decomposition method. The efficient decomposition of N2The bimetallic catalyst of O comprises a carrier and catalytic elements, wherein the carrier is an MCM-22 molecular sieve, the Si/Al value of the molecular sieve is 50-100, the catalytic elements are any two of Fe, Ru or Rh, the mass ratio of Fe to the MCM-22 molecular sieve is 0.1-5%, the mass ratio of Ru to the MCM-22 molecular sieve is 0.1-3%, and the mass ratio of Rh to the MCM-22 molecular sieve is 0.1-3%. The catalyst provided by the invention can realize N at relatively low temperature under the condition of relatively low noble metal loading2And (4) high-efficiency conversion of O.
Description
Technical Field
The invention belongs to N2The technical field of O treatment, in particular to a method for efficiently decomposing N2Bimetallic catalyst of O, its preparation method and decomposition method.
Background
N2O is commonly called laughing gas and is an important atmospheric pollutant, and the greenhouse effect of O is about CO2310 times of that of CH421 times (IPCC). At present N2The O emission mainly comes from industrial production processes, such as adipic acid and nitric acid production and combustion processes of various chemical fuels. With the continuous expansion of production scale, N2The concentration of O in the atmosphere continues to increase at a rate of 0.2-0.3% per year.
In order to eliminate N in industrial tail gas2O, direct catalytic decomposition of N2O is N2And O2Is an effective method. Many studies at home and abroad report that Fe/ZSM-5 catalyst is used for N2The O decomposition has good activity (such as CN 101786011B, CN 102091531A, Kiwi-minsker, L.J.Catal.2003,2019,273-285.), and the catalyst has good activity on impurities in the tail gas such as small amount of H2O、NO、O2Or SO2Has better tolerance, but N is required2Complete conversion of O generally requires higher temperatures, above about 500 degrees.
Li et al (y.j.li, j.n.armor, appl.catal.b 1(1992) L21) system compared the activity of different metals supported on ZSM-5 catalyst, giving the following sequence: rh, Ru>Pd>Cu>Fe>Pt>Ni>Mn.F.Kapteijn et al (F.Kapteijn, J.Ro driguez-Mirasol, J.A.Moulijn, appl.Catal.B: Environ.9(1996)25-64), G.E.Marnellos et al (G.E.Marnellos, E.A.Efthimiadis, I.A.Vasalos, appl.Catal.B: Environ.46(20036)523-539) also investigated the activity of Rh, Ru metals in different carriers and preparation conditions, respectively, and Rh and Ru can be reacted at relatively low temperatures compared to other metals<400 ℃ C.) to realize N2Complete conversion of O. They are sensitive to impurities and single metal catalysts exhibit good activity at high loading levels, which results in a significant increase in catalyst cost.
Disclosure of Invention
In order to solve the defects of the prior art, the invention provides a method for efficiently decomposing N2Bimetallic catalyst of O, its preparation process and decomposition process. The catalyst provided by the invention can realize N at relatively low temperature under the condition of relatively low noble metal loading2And (4) high-efficiency conversion of O.
The technical scheme provided by the invention is as follows:
high-efficiency decomposition of N2The bimetallic catalyst of O comprises a carrier and catalytic elements, wherein the carrier is an MCM-22 molecular sieve, the Si/Al value of the molecular sieve is 50-100, the catalytic elements are any two of Fe, Ru or Rh, the mass ratio of Fe to the MCM-22 molecular sieve is 0.1-5%, the mass ratio of Ru to the MCM-22 molecular sieve is 0.1-3%, and the mass ratio of Rh to the MCM-22 molecular sieve is 0.1-3%.
In the above technical scheme:
the molecular sieve with high Si/Al value can effectively improve the thermal stability of the catalyst, improve the dispersion of active components and reduce the consumption of noble metals;
each catalytic element is loaded on MCM-22, and the formed two-component catalytic system has good catalytic synergistic effect, and effectively improves the catalytic performance of a single component at low temperature while keeping better impurity tolerance.
Specifically, the mass ratio of the two catalytic elements loaded on the carrier is 1: 1 to 1: 10.
the invention also provides the efficient decomposition of N2A method for preparing a bimetallic catalyst of O, comprising the steps of:
1) preparing MCM-22 catalyst;
2) preparing a water-soluble metal salt solution of a catalytic element;
3) impregnating the MCM-22 catalyst obtained in the step 1) with metal salt in the water-soluble metal salt solution obtained in the step 2), and then roasting to obtain the high-efficiency decomposition N2A bimetallic catalyst of O.
Specifically, in the step 1), a dynamic hydrothermal method is adopted to synthesize the MCM-22 catalyst.
The technical proposal adopts a dynamic hydrothermal method to synthesize the MCM-22 molecular sieve with relatively high Si/Al ratio (in the range of 50-100). When the catalyst is used as a catalyst carrier, the thermal stability of the catalyst can be effectively improved, the dispersion of active components is improved, and the consumption of noble metals is reduced. Meanwhile, the invention further improves the catalyst content in N by utilizing the synergistic effect of bimetal2And O directly catalyzes the low-temperature reaction activity in the decomposition reaction.
More particularly, under stirring conditionsRespectively adding aluminum nitrate, hexamethyleneimine, silica sol and sodium hydroxide into a beaker, uniformly mixing, sealing in a stainless steel reaction kettle, dynamically crystallizing at 130 ℃, and adjusting the molar ratio n (SiO) of materials in the synthesis process2)：n(Al2O3)：n(HMI)：n(Na2O)：n(H2O) controlling the Si/Al value to obtain MCM-22 raw powder, then removing the template agent from the MCM-22 raw powder, exchanging for 3 times at 85 ℃ by using 2mol/L ammonium nitrate solution, drying, and roasting for 4 hours at 600 ℃ to obtain MCM-22.
Specifically, in the step 2), the water-soluble metal salt is a halide salt, a nitrate salt or an acetate salt.
Specifically, in step 3), two metal salts are sequentially impregnated.
The invention also provides the above N2The high-efficiency decomposition method of O adopts the bimetallic catalyst provided by the invention to catalyze and decompose N2Decomposed gas of O, wherein: n in the decomposed gas2The volume fraction of O is less than or equal to 5%; the space velocity of the decomposed gas is 3000-50000h-1Airspeed; the catalytic decomposition temperature is 250-450 ℃.
The bimetallic catalyst provided by the invention can realize N at relatively low temperature under the condition of relatively low precious metal loading2And (4) high-efficiency conversion of O.
Detailed Description
The principles and features of this invention are described below in conjunction with examples which are set forth to illustrate, but are not to be construed to limit the scope of the invention.
Experimental and analytical methods used in the examples:
N2the O decomposition catalyst evaluation experiment was carried out in a fixed bed quartz tube reactor (i.d.4mm) containing N2Mixed gas of O and He (N)2The O content is 5 percent), the catalyst loading is 0.1g, (40-60 meshes), and the space velocity range is 3000-50000h-1The reaction temperature range is 250-450 ℃. The product was analyzed by gas chromatography (HP6890, TCD detector, Porapak Q column) and the catalyst was activated by heating to 600 ℃ in the reaction tube for 1h before the reaction started.
Example 1
Preparation and performance of Fe-Rh/MCM-22 catalyst
Adding aluminum nitrate, hexamethyleneimine, silica sol and sodium hydroxide into a 500mL beaker according to a certain sequence under the condition of stirring, uniformly mixing, sealing in a 500mL stainless steel reaction kettle, and dynamically crystallizing at 130 ℃ for 7 d. The molar ratio of the materials in the synthesis process is n (SiO)2)：n(Al2O3)：n(HMI)：n(Na2O)：n(H2O) ═ 1: 0.0086: 0.75: 0.13: 40. and (3) removing the template agent from the raw powder MCM-22, exchanging the raw powder with 2mol/L ammonium nitrate solution at 85 ℃ for 3 times, each time for 2 hours, drying, and roasting at 600 ℃ for 4 hours to obtain H-MCM-22.
250mL of an aqueous ferric nitrate solution containing 0.06104g of iron ions was prepared, and 3g of MCM-22 molecular sieve was added thereto, followed by stirring and refluxing at 85 ℃ for 6 hours. Filtration, washing of the filter cake with deionized water and drying at 60 ℃ for 12 h. The solid powder obtained was then added to 250mL of an aqueous rhodium nitrate solution containing 0.01531g of rhodium and stirred at reflux at 85 ℃ for 6 h. Filtration and washing of the filter cake with deionized water. Drying at 60 ℃ for 12h, and then roasting at 600 ℃ for 6h to obtain the Fe-Rh/MCM-22 catalyst, wherein the Fe loading is 2%, and the rhodium loading is 0.5%. The catalyst is used for N2O is decomposed and the gas composition is N2Under the conditions of O5 percent and He 95 percent, the space velocity is 25000h-1Reaction temperature 250 ℃ and N2The conversion rate of O is 10 percent; reaction temperature 430 ℃ and N2O can achieve 100% decomposition.
Example 2
Preparation of Fe-Ru/MCM-22 catalyst
MCM-22 molecular sieve is prepared as above
250mL of an aqueous ferric nitrate solution containing 0.06104g of iron was prepared, and 3g of MCM-22 molecular sieve was added thereto, followed by stirring and refluxing at 85 ℃ for 6 hours. Filtration, washing of the filter cake with deionized water and drying at 60 ℃ for 12 h. The solid powder obtained was then added to 250mL of an aqueous ruthenium chloride solution containing 0.01524g of ruthenium and stirred at 85 ℃ under reflux for 6 h. Filtration and washing of the filter cake with deionized water. Drying at 60 deg.C for 12h, and calcining at 600 deg.C for 6h to obtain Fe-Rh/MCM-22 catalyst with Fe loading of 2% and rhodiumThe loading was 0.5%. The catalyst is used for N2O is decomposed and the gas composition is N2Under the conditions of O5 percent and He 95 percent, the space velocity is 30000h-1Reaction temperature 250 ℃ C, N2The conversion rate of O is 15 percent; reaction temperature 450 ℃, N2O can achieve 100% decomposition.
Example 3
Preparation of Rh-Ru/MCM-22 catalyst
MCM-22 molecular sieve is prepared as above
250mL of aqueous rhodium nitrate solution containing 0.01531g of rhodium was prepared, and 3g of MCM-22 molecular sieve was added thereto, followed by stirring and refluxing at 85 ℃ for 6 hours. Filtering, washing the filter cake by deionized water, and drying for 12h at 60 ℃. The solid powder obtained was then added to 250mL of an aqueous ruthenium chloride solution containing 0.01524g of ruthenium and stirred at 85 ℃ under reflux for 6 h. Filtration and washing of the filter cake with deionized water. Drying at 60 ℃ for 12h, and then roasting at 600 ℃ for 6h to obtain the Fe-Rh/MCM-22 catalyst, wherein the loading of ruthenium is 0.5%, and the loading of rhodium is 0.5%. The catalyst is used for N2O is decomposed and the gas composition is N2O5% and He 95%, and the space velocity is 20000h-1Reaction temperature 250 ℃ C, N2The O conversion rate is 19 percent; reaction temperature 400 ℃, N2O can achieve 100% decomposition.
Comparative example 1
Preparation of Fe-Ru// ZSM-5 catalyst
Using commercially available ZSM-5 and the same loading method as in example 3, Fe-Ru// ZSM-5 catalyst was prepared with an iron loading of 2% and a ruthenium loading of 0.5%. The catalyst is used for N2O is decomposed and the gas composition is N2Under the conditions of O5 percent and He 95 percent, the space velocity is 20000h-1Reaction temperature 350 ℃ and N2The conversion rate of O is 11 percent; reaction temperature 490 ℃ N2O can achieve 100% decomposition.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents, improvements and the like that fall within the spirit and principle of the present invention are intended to be included therein.
Claims (8)
1. High-efficiency decomposition of N2The bimetallic catalyst of O is characterized by comprising a carrier and catalytic elements, wherein the carrier is an MCM-22 molecular sieve, the Si/Al value of the molecular sieve is 50-100, the catalytic elements are any two of Fe, Ru or Rh, the mass ratio of Fe to the MCM-22 molecular sieve is 0.1-5%, the mass ratio of Ru to the MCM-22 molecular sieve is 0.1-3%, and the mass ratio of Rh to the MCM-22 molecular sieve is 0.1-3%.
2. Efficient decomposition of N according to claim 12A bimetallic catalyst of O, characterized by: the mass ratio of the two catalytic elements loaded on the carrier is 1: 1 to 1: 10.
3. a high efficiency decomposition of N according to claim 1 or 22The preparation method of the bimetallic catalyst of O is characterized by comprising the following steps:
1) preparing MCM-22 catalyst;
2) preparing a water-soluble metal salt solution of a catalytic element;
3) impregnating the MCM-22 catalyst obtained in the step 1) with metal salt in the water-soluble metal salt solution obtained in the step 2), and then roasting to obtain the high-efficiency decomposition N2A bimetallic catalyst of O.
4. Efficient decomposition of N according to claim 32The preparation method of the bimetallic catalyst of O is characterized by comprising the following steps: in the step 1), synthesizing the MCM-22 catalyst by adopting a dynamic hydrothermal method.
5. Efficient decomposition of N according to claim 42The preparation method of the bimetallic catalyst of O is characterized in that: respectively adding aluminum nitrate, hexamethyleneimine, silica sol and sodium hydroxide into a beaker under the condition of stirring, uniformly mixing, sealing in a stainless steel reaction kettle, dynamically crystallizing at 130 ℃, and adjusting the molar ratio n of materials (SiO) in the synthesis process2)：n(Al2O3)：n(HMI)：n(Na2O)：n(H2O) control of Si/Al valueObtaining MCM-22 raw powder, then removing the template agent from the MCM-22 raw powder, then exchanging for 3 times at 85 ℃ by using 2mol/L ammonium nitrate solution, baking for 4 hours at 600 ℃ after drying, and obtaining the MCM-22.
6. Efficient decomposition of N according to claim 32The preparation method of the bimetallic catalyst of O is characterized by comprising the following steps: in the step 2), the water-soluble metal salt is halide salt, nitrate or acetate.
7. Efficient decomposition of N according to any one of claims 3 to 62The preparation method of the bimetallic catalyst of O is characterized in that in the step 3), two metal salts are sequentially impregnated.
8. N2The method for efficiently decomposing O is characterized by comprising the following steps of: catalytic decomposition of N-containing compounds using a bimetallic catalyst as claimed in claim 1 or 22Decomposed gas of O, wherein: n in the decomposed gas2The volume fraction of O is less than or equal to 5%; the space velocity of the decomposed gas is 3000-50000h-1Airspeed; the catalytic decomposition temperature is 250-450 ℃.
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