CN110026185A - A kind of modified perovskite type catalyst and preparation method thereof - Google Patents
A kind of modified perovskite type catalyst and preparation method thereof Download PDFInfo
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- CN110026185A CN110026185A CN201811408216.6A CN201811408216A CN110026185A CN 110026185 A CN110026185 A CN 110026185A CN 201811408216 A CN201811408216 A CN 201811408216A CN 110026185 A CN110026185 A CN 110026185A
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- 239000003054 catalyst Substances 0.000 title claims abstract description 83
- 238000002360 preparation method Methods 0.000 title claims abstract description 33
- 239000000463 material Substances 0.000 claims abstract description 41
- 230000003197 catalytic effect Effects 0.000 claims abstract description 22
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 18
- 239000008367 deionised water Substances 0.000 claims abstract description 14
- 229910021641 deionized water Inorganic materials 0.000 claims abstract description 14
- 239000012153 distilled water Substances 0.000 claims abstract description 9
- 229910052751 metal Inorganic materials 0.000 claims abstract description 8
- 239000002184 metal Substances 0.000 claims abstract description 8
- 230000007935 neutral effect Effects 0.000 claims abstract description 8
- 150000003839 salts Chemical class 0.000 claims abstract description 8
- 229910052748 manganese Inorganic materials 0.000 claims abstract description 6
- 229910052712 strontium Inorganic materials 0.000 claims abstract description 5
- 239000003929 acidic solution Substances 0.000 claims abstract description 4
- 229910052804 chromium Inorganic materials 0.000 claims abstract description 4
- 238000007598 dipping method Methods 0.000 claims abstract description 4
- 229910052742 iron Inorganic materials 0.000 claims abstract description 4
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 4
- 229910052791 calcium Inorganic materials 0.000 claims abstract description 3
- 239000000243 solution Substances 0.000 claims description 12
- 238000001035 drying Methods 0.000 claims description 11
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 9
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims description 8
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 claims description 6
- 229910017604 nitric acid Inorganic materials 0.000 claims description 6
- 239000002253 acid Substances 0.000 claims description 5
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 4
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 4
- 229960000583 acetic acid Drugs 0.000 claims description 4
- 239000012362 glacial acetic acid Substances 0.000 claims description 4
- JVTAAEKCZFNVCJ-UHFFFAOYSA-N lactic acid Chemical compound CC(O)C(O)=O JVTAAEKCZFNVCJ-UHFFFAOYSA-N 0.000 claims description 4
- BDAGIHXWWSANSR-UHFFFAOYSA-N methanoic acid Natural products OC=O BDAGIHXWWSANSR-UHFFFAOYSA-N 0.000 claims description 4
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 claims description 2
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 claims description 2
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 claims description 2
- XTEGARKTQYYJKE-UHFFFAOYSA-N chloric acid Chemical compound OCl(=O)=O XTEGARKTQYYJKE-UHFFFAOYSA-N 0.000 claims description 2
- 229940005991 chloric acid Drugs 0.000 claims description 2
- GDVKFRBCXAPAQJ-UHFFFAOYSA-A dialuminum;hexamagnesium;carbonate;hexadecahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Mg+2].[Al+3].[Al+3].[O-]C([O-])=O GDVKFRBCXAPAQJ-UHFFFAOYSA-A 0.000 claims description 2
- 235000019253 formic acid Nutrition 0.000 claims description 2
- 229910001701 hydrotalcite Inorganic materials 0.000 claims description 2
- 229960001545 hydrotalcite Drugs 0.000 claims description 2
- 239000004310 lactic acid Substances 0.000 claims description 2
- 235000014655 lactic acid Nutrition 0.000 claims description 2
- 239000002808 molecular sieve Substances 0.000 claims description 2
- 235000006408 oxalic acid Nutrition 0.000 claims description 2
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 2
- XBDQKXXYIPTUBI-UHFFFAOYSA-N dimethylselenoniopropionate Natural products CCC(O)=O XBDQKXXYIPTUBI-UHFFFAOYSA-N 0.000 claims 2
- 239000002131 composite material Substances 0.000 claims 1
- 229910044991 metal oxide Inorganic materials 0.000 claims 1
- 235000019260 propionic acid Nutrition 0.000 claims 1
- IUVKMZGDUIUOCP-BTNSXGMBSA-N quinbolone Chemical compound O([C@H]1CC[C@H]2[C@H]3[C@@H]([C@]4(C=CC(=O)C=C4CC3)C)CC[C@@]21C)C1=CCCC1 IUVKMZGDUIUOCP-BTNSXGMBSA-N 0.000 claims 1
- 238000003980 solgel method Methods 0.000 claims 1
- 239000004575 stone Substances 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 16
- 230000008569 process Effects 0.000 abstract description 8
- 239000000203 mixture Substances 0.000 abstract 1
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 27
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 18
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 15
- 238000006243 chemical reaction Methods 0.000 description 13
- 230000000694 effects Effects 0.000 description 10
- 230000004048 modification Effects 0.000 description 10
- 238000012986 modification Methods 0.000 description 10
- URLKBWYHVLBVBO-UHFFFAOYSA-N Para-Xylene Chemical group CC1=CC=C(C)C=C1 URLKBWYHVLBVBO-UHFFFAOYSA-N 0.000 description 8
- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 description 8
- 239000012855 volatile organic compound Substances 0.000 description 8
- 229910017563 LaCrO Inorganic materials 0.000 description 5
- 229910002328 LaMnO3 Inorganic materials 0.000 description 5
- 238000009835 boiling Methods 0.000 description 4
- 238000006555 catalytic reaction Methods 0.000 description 4
- 150000001768 cations Chemical class 0.000 description 4
- 229910000473 manganese(VI) oxide Inorganic materials 0.000 description 4
- 229910003367 La0.5Sr0.5MnO3 Inorganic materials 0.000 description 3
- 229910017530 LaCo0.5Mn0.5O3 Inorganic materials 0.000 description 3
- 229910052878 cordierite Inorganic materials 0.000 description 3
- 230000000593 degrading effect Effects 0.000 description 3
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 3
- 238000010183 spectrum analysis Methods 0.000 description 3
- 229910002254 LaCoO3 Inorganic materials 0.000 description 2
- 229910002262 LaCrO3 Inorganic materials 0.000 description 2
- JTCFNJXQEFODHE-UHFFFAOYSA-N [Ca].[Ti] Chemical compound [Ca].[Ti] JTCFNJXQEFODHE-UHFFFAOYSA-N 0.000 description 2
- 230000015556 catabolic process Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 238000006731 degradation reaction Methods 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000003292 glue Substances 0.000 description 2
- 230000006872 improvement Effects 0.000 description 2
- 229910000510 noble metal Inorganic materials 0.000 description 2
- 238000007254 oxidation reaction Methods 0.000 description 2
- 206010013786 Dry skin Diseases 0.000 description 1
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 1
- 208000031320 Teratogenesis Diseases 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- GNHQSAUHXKRQMC-UHFFFAOYSA-N benzene;chlorine Chemical compound [Cl].C1=CC=CC=C1 GNHQSAUHXKRQMC-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- QGUAJWGNOXCYJF-UHFFFAOYSA-N cobalt dinitrate hexahydrate Chemical compound O.O.O.O.O.O.[Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O QGUAJWGNOXCYJF-UHFFFAOYSA-N 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000010985 leather Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 238000002703 mutagenesis Methods 0.000 description 1
- 231100000350 mutagenesis Toxicity 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 230000033116 oxidation-reduction process Effects 0.000 description 1
- 239000003973 paint Substances 0.000 description 1
- 230000000149 penetrating effect Effects 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 239000011941 photocatalyst Substances 0.000 description 1
- 230000008635 plant growth Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 238000007639 printing Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical class 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
Classifications
-
- 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
- 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
- B01J23/24—Chromium, molybdenum or tungsten
- B01J23/26—Chromium
-
- 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
- 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
- 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
- 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
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- Health & Medical Sciences (AREA)
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- Oil, Petroleum & Natural Gas (AREA)
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Abstract
It is ABO the invention discloses a kind of modified perovskite type catalyst3Structure, wherein A is La1‑xMx, x=0 or 0.5, one of M Sr, Ce, Ba, Ca, the B one or two for Mn, Co, Cr, Fe, Ni.The preparation method of the catalyst, comprising the following steps: one, according to the ratio that A and B molar ratio is 1:0.8~1:1.2 the metal salt of A mix with the metal salt of M, it is supported on carrier according to sol-gal process, it is dry, roast, prepare ABO3Perovskite-type material；Two, in an acidic solution by the Perovskite Catalytic material dipping of step 1 preparation；Three, the material obtained in step 2 is washed with distilled water or deionized water, when PH is neutral, is placed in baking oven and is being dried, obtained material is modified perovskite catalyst.The catalytic activity of the modified perovskite type catalyst of preparation is dramatically increased compared to former perovskite type catalyst, while also remaining the excellent high temperature resistance of perovskite material.
Description
Technical field
The present invention relates to a kind of modified perovskite type catalyst and preparation method thereof, belong to catalyst technical field.
Background technique
Currently, volatile organic compounds (volatile organic compounds, abbreviation VOCs) has become sky
One of the main source of pollutant in gas.Its source is very extensive, and PETROLEUM PROCESSING, leather synthesis, electronics, printing, is baked coating
There are during the industry productions such as paint, pharmacy, vehicle exhaust a large amount of VOCs to generate, and there is penetrating odor mostly, have teratogenesis,
Carcinogenic, mutagenesis, it is huge to atmospheric environment, animal and plant growth and human health damage.Therefore the control of VOCs is administered
It is one of the emphasis of modern environment work.Catalysis burning is a kind of effective low temperature VOCs purification techniques, and in entire catalysis combustion
In burning technology system, catalyst occupies core status, and the superiority and inferiority of catalyst performance directly affects catalytic effect.
Noble metal catalyst catalytic activity with higher usually compared with transition metal, but at high cost and thermal stability
It is low.And perovskite catalyst forms the features such as flexible, oxidation-reduction quality is good, thermal stability is good due to it, it has also become urged in multiphase
The mixed oxidization objects system of current most study in change field.However it is still compared with noble metal in the catalytic treatment of VOCs
There is a problem of that low-temperature catalytic activity is lower.Therefore, perovskite type catalyst is restricted in industrial application.
Numerous results of study show that the catalytic oxidation of VOCs generally carries out on the surface of catalyst, and perovskite knot
The grown surface of structure then preferentially occupies by A bit element, and A ions mainly play the skeleton and rock-steady structure of photocatalyst crystals
It acts on and does not have catalytic activity.It therefore, if can be from ABO3In be selectively removed part A cation, expose height
Active B bit element, then the catalytic activity of resulting materials can be dramatically increased compared to former perovskite catalyst.
Summary of the invention
The technical problem to be solved by the present invention is to overcome the deficiencies of existing technologies, a kind of modified perovskite type catalysis is provided
Agent and preparation method thereof, from ABO3In part A cation is selectively removed, high activity B bit element is exposed, so that preparation
The catalytic activity of modified perovskite type catalyst dramatically increased compared to former perovskite type catalyst, while also remaining calcium titanium
The excellent high temperature resistance of pit wood material.
In order to solve the above technical problems, the present invention provides a kind of modified perovskite type catalyst, the modified perovskite type
Catalyst is ABO3Structure, wherein A is La1-xMx, x=0 or 0.5, one of M Sr, Ce, Ba, Ca, B for Mn, Co, Cr,
The one or two of Fe, Ni.
Meanwhile the present invention also provides a kind of preparation methods of modified perovskite type catalyst, comprising the following steps:
(1) metal salt of A is mixed with the metal salt of M according to the ratio that A and B molar ratio is 1:0.8~1:1.2, according to
Sol-gal process is supported on carrier, and ABO is prepared in dry, roasting3Perovskite-type material；
(2) in an acidic solution by the Perovskite Catalytic material dipping of step (1) preparation；
(3) material obtained in step (2) is washed with distilled water or deionized water, when PH is neutral, is placed in
It is being dried in baking oven, obtained material is modified perovskite catalyst.
Preferably, drying temperature is 105~120 DEG C in the step (1), and drying time is 6~10h, and maturing temperature is
500~700 DEG C, calcining time is 4~6h.
Preferably, step (2) acid solution is nitric acid, glacial acetic acid, oxalic acid, hydrochloric acid, chloric acid, formic acid, lactic acid, third
One of acid, acrylic acid solution.
Preferably, step (2) the acid solution concentration is 1~3mol/L.
Preferably, the dip time of the step (2) is 20~120min.
Preferably, drying temperature is 60~200 DEG C in the step (3), and drying time is 2~5h.
Preferably, the carrier is one of cordierite, aluminium oxide, molecular sieve or hydrotalcite.
Advantageous effects of the invention:
(1) a kind of modified perovskite type catalyst and preparation method thereof of the invention, from ABO3In portion is selectively removed
Points of A cations expose high activity B bit element so that the catalytic activity of the modified perovskite type catalyst prepared compared to
Former perovskite type catalyst dramatically increases, while also remaining the excellent high temperature resistance of perovskite material.
(2) modified perovskite type catalyst prepared by the present invention is reaching being compared to common perovskite type catalyst
Temperature needed for same catalytic activity reduces, and saves energy.
(3) modified technique of the invention is simple, and operating cost is low, is easy to industrial applications, marketing with higher
Prospect.
Detailed description of the invention
Fig. 1 is the LaMnO of the embodiment of the present invention 13Perovskite catalyst before modified after EDS energy spectrum analysis figure；
Wherein, (a) is LaMnO before modified3The EDS energy spectrum analysis figure of perovskite catalyst is (b) modified
LaMnO3The EDS energy spectrum analysis figure of perovskite catalyst.
Specific embodiment
The invention will be further described below in conjunction with the accompanying drawings.Following embodiment is only used for clearly illustrating the present invention
Technical solution, and not intended to limit the protection scope of the present invention.
As shown in Figure 1, a kind of modified perovskite type catalyst, modified perovskite type catalyst is ABO3Structure, wherein A be
La1-xMx, x=0~0.8, one of M Sr, Ce, Ba, Ca, the B one or two for Mn, Co, Cr, Fe, Ni.
A kind of preparation method of modified perovskite type catalyst, which comprises the following steps:
(1) metal salt of A is mixed with the metal salt of M according to the ratio that A and B molar ratio is 1:0.8~1:1.2, according to
Sol-gal process is supported on carrier, and ABO is prepared in dry, roasting3Perovskite-type material；
(2) in an acidic solution by the Perovskite Catalytic material dipping of step (1) preparation；
(3) material obtained in step (2) is washed with distilled water or deionized water, when PH is neutral, is placed in
It is being dried in baking oven, obtained material is modified perovskite catalyst.
Embodiment 1
A kind of modified perovskite type catalyst, modified perovskite type catalyst are ABO3Structure, wherein A is La1-xMx, x=
0, B is Mn.
A kind of preparation method of modified perovskite type catalyst, comprising the following steps:
(1) LaMnO using sol-gal process preparation load on cordierite3Perovskite.Take La (NO3)2.6H2O
11.5g, the Mn (NO that weight fraction is 50%3)2Deionized water 7g is added in 9.5g, citric acid 1.7g.It is steamed in 60 DEG C of water-baths
It boils, is allowed to that sol form is presented, then cordierite carrier is placed in colloidal sol, after taking-up is dried, 105 DEG C of dry 6h, then 700 DEG C
Roast 4h.Then prepare LaMnO3Perovskite material.
(2) LaMnO for preparing step (1)3Perovskite is soaked in the HNO of 3M3In solution, Shi Changwei 20min.
(3) the modified material distilled water or deionized water that obtain in step (2) are rinsed, when PH is neutral, then
Place the material in 4h is dried in baking oven at 130 DEG C, obtained material is modified LaMnO3Perovskite catalyst.
As shown in Figure 1, it can be seen that LaMnO3Perovskite passes through HNO3Element La/Mn ratio declines after processing, this can return
Cause is in La in HNO3In slight dissolution, then expose B activity position (Mn element).
To sample carry out catalytic activity test, method are as follows: toluene concentration be 1000ppm, air speed 15000h-1Item
Under part, 500mg is taken, the modification LaMnO that granularity is 40~60 mesh3Perovskite catalyst.Test result is as follows: at 265 DEG C to first
Benzene conversion ratio is 50%, is 95% to toluene conversion at 280 DEG C.And common LaMnO395% conversion ratio of the catalyst to toluene
Generally at 350 DEG C or so.So the modification LaMnO of the embodiment of the present invention 13Perovskite catalyst shows degradation of toluene activity
It writes and improves.
Embodiment 2
A kind of modified perovskite type catalyst, modified perovskite type catalyst are ABO3Structure, wherein A is La1-xMx, x=
0, B is Co.
A kind of preparation method of modified perovskite type catalyst, comprising the following steps:
(1) LaCoO using sol-gal process preparation load on alumina3Perovskite.Take La (NO3)2.6H2O
11.5g, Co (NO3)2.6H2Deionized water 7g is added in O 7.7g, citric acid 1.7g.The boiling in 60 DEG C of water-baths, is allowed to present molten
Then alumina support is placed in colloidal sol by glue, take out after drying, 120 DEG C of dry 10h, then 500 DEG C of roasting 6h.Then make
Standby LaCoO out3Perovskite material.
(2) LaCoO for preparing step (1)3Perovskite is soaked in the glacial acetic acid solution of 3M, Shi Changwei 80min.
(3) the modified material distilled water or deionized water that obtain in step (2) are rinsed, when PH is neutral, then
Place the material in 5h is dried in baking oven at 60 DEG C, obtained material is modified LaCoO3Perovskite catalyst.
To sample carry out catalytic activity test, method are as follows: benzene concentration be 1000ppm, air speed 15000h-1Condition
Under, take 500mg, the modification LaCoO that granularity is 40~60 mesh3Perovskite catalyst.Test result is as follows: turning at 271 DEG C to benzene
Rate is 50%, is 95% to benzene conversion ratio at 285 DEG C.And common LaCoO3Catalyst generally exists to 95% conversion ratio of benzene
325~400 DEG C.So the modification LaCoO of the embodiment of the present invention 23Perovskite catalyst is significantly improved to benzene degrading activity.
Embodiment 3
A kind of modified perovskite type catalyst, modified perovskite type catalyst are ABO3Structure, wherein A is La1-xMx, x=
0.5, M Sr, B are Mn.
A kind of preparation method of modified perovskite type catalyst, comprising the following steps:
(1) La using sol-gal process preparation load on cordierite0.5Sr0.5MnO3Perovskite.Take La (NO3)2.6H2O 5.6g, Sr (NO3)22.8g, the Mn (NO that weight fraction is 50%3)2Deionized water is added in 9.5g, citric acid 1.7g
7g.The boiling in 70 DEG C of water-baths is allowed to that sol form is presented, then cordierite carrier is placed in colloidal sol, after taking-up is dried, 110
DEG C dry 8h, then 600 DEG C of roasting 5h.Then prepare La0.5Sr0.5MnO3Perovskite material.
(2) La for preparing step (1)0.5Sr0.5MnO3Perovskite is soaked in the nitric acid solution of 1M, Shi Changwei
120min。
(3) the modified material distilled water or deionized water that obtain in step (2) are rinsed, when PH is neutral, then
Place the material in 2h is dried in baking oven at 200 DEG C, obtained material is modified La0.5Sr0.5MnO3Perovskite catalyst.
To sample carry out catalytic activity test, method are as follows: xylene concentration be 1500ppm, air speed 15000h-1's
Under the conditions of, take 500mg, the modification La that granularity is 40~60 mesh0.5Sr0.5MnO3Perovskite catalyst.Test result is as follows:
270 DEG C of paraxylene conversions are 50%, are 95% in 282 DEG C of paraxylene conversions.And common La0.5Sr0.5MnO3Catalysis
95% conversion ratio of agent paraxylene is generally at 325~375 DEG C.So the modification La of the embodiment of the present invention 30.5Sr0.5MnO3Calcium
Titanium ore catalyst paraxylene degrading activity is significantly improved.
Embodiment 4
A kind of modified perovskite type catalyst, modified perovskite type catalyst are ABO3Structure, wherein A is La1-xMx, x=
0, B is two kinds of Mn, Co of mixing.
A kind of preparation method of modified perovskite type catalyst, comprising the following steps:
(1) LaCo using sol-gal process preparation load on alumina0.5Mn0.5O3Perovskite.Take La (NO3)2.6H2O 5.6g, Co (NO3)2.6H2O 3.8g, 50%Mn (NO3)2Deionized water 7g is added in 4.8g, citric acid 1.7g.70
Boiling in DEG C water-bath, is allowed to that sol form is presented, then alumina support is placed in colloidal sol, after taking-up is dried, 105 DEG C of dryings
6h, then 700 DEG C of roasting 6h.Then prepare LaCo0.5Mn0.5O3Perovskite material.
(2) LaCo for preparing step (1)0.5Mn0.5O3Perovskite is soaked in the nitric acid solution of 1M, Shi Changwei 80min.
(3) the modified material distilled water or deionized water that obtain in step (2) are rinsed, when PH is neutral, then
Place the material in 4h is dried in baking oven at 120 DEG C, obtained material is modified LaCo0.5Mn0.5O3Perovskite catalyst.
To sample carry out catalytic activity test, method are as follows: toluene concentration be 1000ppm, air speed 20000h-1Item
Under part, 500mg is taken, the modification LaCo that granularity is 40~60 mesh0.5Mn0.5O3Perovskite catalyst.Test result is as follows: 262
DEG C to toluene conversion be 50%, 275 DEG C to toluene conversion be 95%.And common LaCo0.5Mn0.5O3Catalyst is to toluene
95% conversion ratio generally at 325 DEG C or so.So the modification LaCo of the embodiment of the present invention 40.5Mn0.5O3Perovskite catalyst pair
Degradation of toluene activity is significantly improved.
Embodiment 5
A kind of modified perovskite type catalyst, which is characterized in that the modified perovskite type catalyst is ABO3Structure,
Middle A is La1-xMx, x=0, B are Cr.
A kind of preparation method of modified perovskite type catalyst, comprising the following steps:
(1) LaCrO using sol-gal process preparation load on alumina3Perovskite.Take La (NO3)2.6H2O
11.5g, Cr (NO3)2.6H2Deionized water 7g is added in O 6.3g, citric acid 1.7g.The boiling in 60 DEG C of water-baths, is allowed to present molten
Then alumina support is placed in colloidal sol by glue, take out after drying, 120 DEG C of dry 8h, then 700 DEG C of roasting 5h.Then prepare
LaCrO out3Perovskite material.
(2) LaCrO for preparing step (1)3Perovskite is soaked in the glacial acetic acid solution of 2M, Shi Changwei 100min.
(3) the modified material distilled water or deionized water that will be obtained in step (2) rinse 3 times, then place the material in
2h is dried in baking oven at 80 DEG C, obtained material is modified LaCrO3Perovskite catalyst.
To sample carry out catalytic activity test, method are as follows: chlorobenzene concentration be 1000ppm, air speed 15000h-1Item
Under part, 500mg is taken, the modification LaCrO that granularity is 40~60 mesh3Perovskite catalyst.Test result is as follows: at 275 DEG C to chlorine
Benzene conversion ratio is 50%, is 95% to chlorobenzene transformation ratio at 295 DEG C.And common LaCrO395% conversion ratio of the catalyst to chlorobenzene
Generally at 350~400 DEG C.So the modification LaCrO of the embodiment of the present invention 53Perovskite catalyst obtains chlorobenzene degrading activity
It significantly improves.
A kind of modified perovskite type catalyst of the invention and preparation method thereof, from ABO3In part A is selectively removed
Position cation exposes high activity B bit element, so that the catalytic activity of the modified perovskite type catalyst of preparation is compared to protocalcium
Titanium ore type catalyst dramatically increases, while also remaining the excellent high temperature resistance of perovskite material.It is prepared by the present invention to change
Property perovskite type catalyst be compared to common perovskite type catalyst temperature needed for reaching same catalytic activity drop
It is low, save energy.Modified technique of the invention is simple, and operating cost is low, is easy to industrial applications, marketing with higher
Prospect.
The above is only a preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art
For member, without departing from the technical principles of the invention, several improvement and deformations can also be made, these improvement and deformations
Also it should be regarded as protection scope of the present invention.
Claims (8)
1. a kind of modified perovskite type catalyst, which is characterized in that the modified perovskite type catalyst is ABO3Structure, wherein A
For La1-xMx, x=0 or 0.5, one of M Sr, Ce, Ba, Ca, the B one or two for Mn, Co, Cr, Fe, Ni.
2. a kind of preparation method of modified perovskite type catalyst according to claim 1, which is characterized in that including following
Step:
(1) metal salt of A is mixed with the metal salt of M according to the ratio that A and B molar ratio is 1:0.8~1:1.2, according to colloidal sol
Gel method is supported on carrier, and ABO is prepared in dry, roasting3Perovskite-type material；
(2) in an acidic solution by the Perovskite Catalytic material dipping of step (1) preparation；
(3) material obtained in step (2) is washed with distilled water or deionized water, when PH is neutral, is placed in baking oven
In be dried, obtained material is modified perovskite catalyst.
3. the preparation method of Ca-Ti ore type O composite metallic oxide catalyst according to claim 2, which is characterized in that institute
Stating in step (1) drying temperature is 105~120 DEG C, and drying time is 6~10h, and maturing temperature is 500~700 DEG C, when roasting
Between be 4~6h.
4. the preparation method of modified perovskite catalyst according to claim 2, which is characterized in that step (2) acid
Property solution be one of nitric acid, glacial acetic acid, oxalic acid, hydrochloric acid, chloric acid, formic acid, lactic acid, propionic acid, acrylic acid solution.
5. the preparation method of modified perovskite catalyst according to claim 4, which is characterized in that step (2) acid
Property solution concentration be 1~3mol/L.
6. the preparation method of modified perovskite catalyst according to claim 5, which is characterized in that the step (2)
Dip time is 20~120min.
7. the preparation method of modified perovskite catalyst according to claim 2, which is characterized in that in the step (3)
Drying temperature is 60~200 DEG C, and drying time is 2~5h.
8. the preparation method of modified perovskite catalyst according to claim 1, which is characterized in that the carrier is that violet is green
One of stone, aluminium oxide, molecular sieve or hydrotalcite.
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