CN107413350A - Mischmetal denitrating catalyst and preparation method thereof - Google Patents

Mischmetal denitrating catalyst and preparation method thereof Download PDF

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Publication number
CN107413350A
CN107413350A CN201710372492.0A CN201710372492A CN107413350A CN 107413350 A CN107413350 A CN 107413350A CN 201710372492 A CN201710372492 A CN 201710372492A CN 107413350 A CN107413350 A CN 107413350A
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mischmetal
denitrating catalyst
earth oxide
crystal
catalyst
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CN201710372492.0A
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Inventor
龚志军
武文斐
李保卫
张凯
金光
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Inner Mongolia University of Science and Technology
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Inner Mongolia University of Science and Technology
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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
    • B01J23/83—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 rare earths or actinides
    • 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
    • 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
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/16—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
    • B01J23/32—Manganese, technetium or rhenium
    • B01J23/34—Manganese
    • 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
    • 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 present invention relates to a kind of mischmetal denitrating catalyst and preparation method thereof, the denitrating catalyst active component is to form double active ingredients by mixed rare-earth oxide and transition metal oxide.Due to the synergy between mixed rare-earth oxide and between rare earth oxide and transition metal oxide so that catalyst has the advantages that high catalytic efficiency, reaction temperature window is wide.Preparation technology is made using infusion process, and simple with technique, raw material sources are extensive, low cost and other advantages.In terms of mixed rare-earth oxide catalyst provided by the invention is mainly used in the purification of industrial waste gas, especially in terms of denitrating flue gas.The middle low-temperature denitration of flue gas of coal-burning power plant is can be not only used for, can be used for the low-temperature denitration of flue gas field of industrial source.

Description

Mischmetal denitrating catalyst and preparation method thereof
Technical field
The present invention relates to exhaust-gas treatment field of purification, more particularly to a kind of mischmetal denitrating catalyst and its preparation side Method.
Background technology
Rare earth element is due to the feature such as the 4f tracks of underfill electronics and lanthanide contract, showing uniqueness chemically Can, as catalyst, it is used widely in many important chemical processes, as petrochemical industry, fossil fuel are urged Change purification of burning, the chemical industry of carbon one, environmental catalysis, motor vehicle tail-gas purifying and toxic and harmful gas etc..From the 1960s Mid-term starts, and the related properties of rare earth compound are conducted extensive research both at home and abroad, including research rare earth alternate resources phase To the noble metal of shortage；The new catalytic material that performance is more preferable, more environmentally friendly is improved or prepares using rare earth；Research rare earth exists Mechanism of action, catalytic active site in catalysis etc..RE treatment steel is broadly divided into according to its composition：Rare earth combined oxidation Thing, rare earth-noble metal, rare earth containing zeolite etc..
Although rare earth oxide shows certain catalytic activity to some chemical reactions, and can be prepared and subtracted by nanosizing Its small particle size, increase specific surface area or modulation surface crystal face composition etc. improve its catalytic activity, but far below reaction Required perfect condition, and the heat endurance of rare earth oxide can not be satisfactory, easily sinters at high temperature, so as to lead Cause the decline of catalytic activity.
The content of the invention
In view of this, the present invention provides a kind of mischmetal denitrating catalyst and preparation method thereof.
The present invention provides a kind of mischmetal denitrating catalyst, and the denitrating catalyst active component is aoxidized by mischmetal Thing and transition metal oxide composition double active ingredients.
Further, the carrier of the mischmetal denitrating catalyst is γ-A12O3Or activated carbon.
Further, the mischmetal denitrating catalyst forms as follows by weight percentage：Mixed rare-earth oxide For 5%-15%, transition metal oxide 1%-3%, remaining is γ-A12O3Or absorbent charcoal carrier.
Further, the mixed rare-earth oxide includes by weight percentage：60%-70% CeO2, 30%- 40% La2O3。
Further, denitrating catalyst active component forms as follows by weight percentage：CeO2For 60%, La2O3For 30%, Fe2O3Or MnO2For 10%.
The present invention also provides a kind of preparation method of the mischmetal denitrating catalyst described in above-mentioned any one, further Ground, comprise the following steps：
By Ce (NO3)3·6H2O crystal, La (NO3)3·6H2O crystal, Fe (NO3)3·9H2O crystal or Mn (NO3)2· 4H2O crystal, which is dissolved in pure water, prepares catalyst precursor, then by γ-A12O3Or activated carbon is added preceding as carrier Drive in liquid solution and impregnate 24h, then the sample impregnated is put into drying box in 120-150 DEG C of dry 4-8h, it is dried Sample is in 500-700 DEG C of roasting 3-4h of inert atmosphere so that nitrate is decomposed into oxide, forms mixed rare-earth oxide and urges Agent, obtain final catalyst prod.
Above-mentioned mischmetal denitrating catalyst active component provided by the invention is by mixed rare-earth oxide and transition metal Oxide forms double active ingredients, due to cooperateing between mixed rare-earth oxide and between rare earth oxide and transition metal oxide Effect so that catalyst has the advantages that high catalytic efficiency, reaction temperature window is wide.Preparation technology is made using infusion process, tool There is technique simple, raw material sources are extensive, low cost and other advantages.Mixed rare-earth oxide catalyst provided by the invention is mainly applied In terms of the purification of industrial waste gas, especially in terms of denitrating flue gas.The middle low-temperature denitration of flue gas of coal-burning power plant is can be not only used for, also may be used For the low-temperature denitration of flue gas field of industrial source.
Embodiment
The invention discloses a kind of mischmetal denitrating catalyst and preparation method thereof.Those skilled in the art can use for reference Present disclosure, it is suitably modified technological parameter realization.In particular, all similar replacements and change are to this area skill It is it will be apparent that they are considered as being included in the present invention for art personnel.The present invention method and application by compared with Good embodiment is described, related personnel substantially can not depart from present invention, in spirit and scope to as described herein Methods and applications are modified or suitably changed with combining, to realize and using the technology of the present invention.
The present invention provides a kind of mischmetal denitrating catalyst preparation method, can apply to the NH3- selections of coal-fired flue-gas The catalytic-reduction denitrified field of property, have the advantages that catalytic efficiency is higher, good economy performance, whole technical matters is simple, small investment, energy Consume low, excellent catalytic effect.
The present invention provides a kind of mischmetal denitrating catalyst, and the denitrating catalyst activearm is to divide by mischmetal oxygen Compound and transition metal oxide composition double active ingredients.Due between mixed rare-earth oxide and rare earth oxide and transition metal Synergy between oxide so that catalyst has the advantages that high catalytic efficiency, reaction temperature window is wide.
Further, the carrier of the mischmetal denitrating catalyst is γ-A12O3Or activated carbon.The carrier have than Surface area is big, the advantages that pore structure prosperity, low-temperature SCR catalytic denitration field in being adapted to.The preparation technology of this catalyst uses Infusion process makes, and simple with technique, raw material sources are extensive, low cost and other advantages.
Preferably, above-mentioned mischmetal denitrating catalyst its form by weight percentage it is as follows：Mixed rare-earth oxide For 5%-15%, transition metal oxide 1%-3%, remaining is γ-A12O3Or absorbent charcoal carrier.
Further, the mixed rare-earth oxide includes by weight percentage：60%-70% CeO2, 30%- 40% La2O3。
Further, the denitrating catalyst active component forms as follows by weight percentage：CeO2For 60%, La2O3 For 30%, Fe2O3Or MnO2For 10%.
The present invention also provides a kind of preparation method of above-mentioned mischmetal denitrating catalyst, comprises the following steps：
By Ce (NO3)3·6H2O crystal, La (NO3)3·6H2O crystal, Fe (NO3)3·9H2O crystal or Mn (NO3)2· 4H2The addition that O crystal is converted according to aforementioned proportion, which is dissolved in pure water, prepares catalyst precursor, then by γ-A12O3Or Person's activated carbon as carrier add 24h is impregnated in precursor solution, then by the sample impregnated be put into drying box in 120-150 DEG C of dry 4-8h, dried sample are calcined 3-4h in inert atmosphere at 500-700 DEG C so that nitrate resolves into For oxide, mixed rare-earth oxide catalyst is formed, obtains final catalyst prod.
Above-mentioned mischmetal denitrating catalyst denitrating catalyst active component provided by the invention is by mixed rare-earth oxide Double active ingredients are formed with transition metal oxide, due between mixed rare-earth oxide and rare earth oxide and transiting metal oxidation Synergy between thing so that catalyst has the advantages that high catalytic efficiency, reaction temperature window is wide.Preparation technology is using dipping Method makes, and simple with technique, raw material sources are extensive, low cost and other advantages.Mixed rare-earth oxide catalysis provided by the invention In terms of agent is mainly used in the purification of industrial waste gas, especially in terms of denitrating flue gas.It can be not only used for the middle low temperature cigarette of coal-burning power plant Qi exhaustion nitre, it can be used for the low-temperature denitration of flue gas field of industrial source.
With reference to embodiment, the present invention is expanded on further：
Embodiment 1
Precise 0.6g Ce (NO3)3·6H2La (the NO of O crystal, 0.16g3)3·6H2The Fe of O crystal, 0.06g (NO3)3·9H2O crystal, it is dissolved in 40ml pure water, is stirred continuously to being completely dissolved.Precise 4g γ-A12O3Particle, Add in the mischmetal aqueous solution of above-mentioned preparation, stand 1 day at normal temperatures, dry 3h in 150 DEG C, dried sample is in argon The lower 500 DEG C of roastings 3h of gas atmosphere, obtains mischmetal denitrating catalyst.Mischmetal denitrating catalyst activity made from this method Temperature window is 300-400 DEG C, is mainly used in the SCR denitrating flue gas of coal-burning power plant.
Embodiment 2
Precise 0.6g Ce (NO3)3·6H2La (the NO of O crystal, 0.16g3)3·6H2The Mn of O crystal, 0.06g (NO3)2·4H2O crystal, it is dissolved in 40ml pure water, is stirred continuously to being completely dissolved.Precise 4g γ-A12O3Particle, Add in the mischmetal aqueous solution of above-mentioned preparation, stand 1 day at normal temperatures, dry 3h in 150 DEG C, dried sample is in argon The lower 500 DEG C of roastings 3h of gas atmosphere, obtains mischmetal denitrating catalyst.Mischmetal denitrating catalyst activity made from this method Temperature window is 200-300 DEG C, is mainly used in the low-temperature SCR denitrating flue gas of industrial source.
Embodiment 3
Precise 0.3g Ce (NO3)3·6H2La (the NO of O crystal, 0.08g3)3·6H2The Fe of O crystal, 0.03g (NO3)3·9H2O crystal, it is dissolved in 40ml pure water, is stirred continuously to being completely dissolved.Precise 2g activated carbon granules or work Property Carbon fibe, add in the mischmetal aqueous solution of above-mentioned preparation, at normal temperatures stand 1 day, in 120 DEG C dry 4h, it is dried Sample under an argon atmosphere 600 DEG C roasting 3h, obtain mischmetal denitrating catalyst.Mischmetal denitration made from this method Catalyst activity temperature window is 300-400 DEG C, is mainly used in the SCR denitrating flue gas of coal-burning power plant.
Embodiment 4
Precise 0.3g Ce (NO3)3·6H2La (the NO of O crystal, 0.08g3)3·6H2The Mn of O crystal, 0.03g (NO3)2·4H2O crystal, it is dissolved in 40ml pure water, is stirred continuously to being completely dissolved.Precise 2g activated carbon granules or work Property Carbon fibe, add in the mischmetal aqueous solution of above-mentioned preparation, at normal temperatures stand 1 day, in 120 DEG C dry 4h, it is dried Sample under an argon atmosphere 600 DEG C roasting 3h, obtain mischmetal denitrating catalyst.Mischmetal denitration made from this method Catalyst activity temperature window is 200-300 DEG C, is mainly used in the low-temperature SCR denitrating flue gas of industrial source.
Described above is only the preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art For member, under the premise without departing from the principles of the invention, some improvements and modifications can also be made, these improvements and modifications also should It is considered as protection scope of the present invention.

Claims (6)

1. a kind of mischmetal denitrating catalyst, it is characterised in that the denitrating catalyst active component is aoxidized by mischmetal Thing and transition metal oxide composition double active ingredients.
2. mischmetal denitrating catalyst according to claim 1, it is characterised in that the mischmetal denitrating catalyst Carrier be γ-Al2O3Or activated carbon.
3. mischmetal denitrating catalyst according to claim 1, it is characterised in that it is formed such as by weight percentage Under：Mixed rare-earth oxide is 5%-15%, transition metal oxide 1%-3%, and remaining is γ-Al2O3Or carried by active carbon Body.
4. mischmetal denitrating catalyst according to claim 3, it is characterised in that the mixed rare-earth oxide is with weight Amount percentages include：60%-70% CeO2, 30%-40% La2O3。
5. mischmetal denitrating catalyst according to claim 1, it is characterised in that denitrating catalyst active component is by weight It is as follows to measure percentages composition：CeO2For 60%, La2O3For 30%, Fe2O3Or MnO2For 10%.
6. the preparation method of the mischmetal denitrating catalyst described in claim 1 to 5 any one, it is characterised in that including Following steps：
By Ce (NO3)3·6H2O crystal, La (NO3)3·6H2O crystal, Fe (NO3)3·9H2O crystal or Mn (NO3)2·4H2O Crystal, which is dissolved in pure water, prepares catalyst precursor, then by γ-A12O3Or activated carbon is added in presoma as carrier 24h is impregnated in solution, then the sample impregnated is put into drying box in 120-150 DEG C of dry 4-8h, dried sample In 500-700 DEG C of roasting 3-4h of inert atmosphere so that nitrate is decomposed into oxide, forms mixed rare-earth oxide catalysis Agent, obtain final catalyst prod.
CN201710372492.0A 2017-05-24 2017-05-24 Mischmetal denitrating catalyst and preparation method thereof Pending CN107413350A (en)

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Cited By (5)

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CN107930637A (en) * 2017-12-05 2018-04-20 内蒙古科技大学 A kind of high entropy solid solution catalyst of rare-earth-based iron content and preparation method thereof
CN107961794A (en) * 2017-12-05 2018-04-27 内蒙古科技大学 A kind of high entropy solid solution catalyst of rare-earth-based and preparation method thereof
CN109261163A (en) * 2018-09-25 2019-01-25 山东国铭球墨铸管科技有限公司 A kind of purification process of flue gas during smelting denitrifying oxide
CN110898843A (en) * 2018-09-17 2020-03-24 内蒙古智萃科技信息咨询有限公司 Mixed rare earth catalytic natural gas combustion catalyst and preparation method thereof
CN113813960A (en) * 2021-08-19 2021-12-21 南京工业大学 Dual-functional powder and preparation method and application thereof

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Cited By (6)

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Publication number Priority date Publication date Assignee Title
CN107930637A (en) * 2017-12-05 2018-04-20 内蒙古科技大学 A kind of high entropy solid solution catalyst of rare-earth-based iron content and preparation method thereof
CN107961794A (en) * 2017-12-05 2018-04-27 内蒙古科技大学 A kind of high entropy solid solution catalyst of rare-earth-based and preparation method thereof
CN110898843A (en) * 2018-09-17 2020-03-24 内蒙古智萃科技信息咨询有限公司 Mixed rare earth catalytic natural gas combustion catalyst and preparation method thereof
CN109261163A (en) * 2018-09-25 2019-01-25 山东国铭球墨铸管科技有限公司 A kind of purification process of flue gas during smelting denitrifying oxide
CN113813960A (en) * 2021-08-19 2021-12-21 南京工业大学 Dual-functional powder and preparation method and application thereof
CN113813960B (en) * 2021-08-19 2023-09-26 南京工业大学 Dual-function powder and preparation method and application thereof

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