CN111054360B - Catalyst for catalytic combustion treatment of PTA tail gas - Google Patents
Catalyst for catalytic combustion treatment of PTA tail gas Download PDFInfo
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- CN111054360B CN111054360B CN201811201393.7A CN201811201393A CN111054360B CN 111054360 B CN111054360 B CN 111054360B CN 201811201393 A CN201811201393 A CN 201811201393A CN 111054360 B CN111054360 B CN 111054360B
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- 239000003054 catalyst Substances 0.000 title claims abstract description 57
- 238000007084 catalytic combustion reaction Methods 0.000 title claims abstract description 18
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims abstract description 54
- 238000000034 method Methods 0.000 claims abstract description 17
- 238000002360 preparation method Methods 0.000 claims abstract description 11
- 229910000428 cobalt oxide Inorganic materials 0.000 claims abstract description 5
- IVMYJDGYRUAWML-UHFFFAOYSA-N cobalt(ii) oxide Chemical compound [Co]=O IVMYJDGYRUAWML-UHFFFAOYSA-N 0.000 claims abstract description 5
- 238000005470 impregnation Methods 0.000 claims abstract description 5
- 239000012752 auxiliary agent Substances 0.000 claims description 13
- 238000001125 extrusion Methods 0.000 claims description 4
- 238000000151 deposition Methods 0.000 claims description 3
- 229910052787 antimony Inorganic materials 0.000 claims description 2
- 229910052797 bismuth Inorganic materials 0.000 claims description 2
- 229910052733 gallium Inorganic materials 0.000 claims description 2
- 239000007789 gas Substances 0.000 abstract description 30
- 238000007254 oxidation reaction Methods 0.000 abstract description 9
- 230000003647 oxidation Effects 0.000 abstract description 8
- 230000003197 catalytic effect Effects 0.000 abstract description 5
- 239000002440 industrial waste Substances 0.000 abstract 1
- 239000000243 solution Substances 0.000 description 153
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 114
- 238000003756 stirring Methods 0.000 description 77
- 238000001035 drying Methods 0.000 description 75
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 75
- 239000008367 deionised water Substances 0.000 description 74
- 229910021641 deionized water Inorganic materials 0.000 description 74
- 238000002390 rotary evaporation Methods 0.000 description 46
- 230000032683 aging Effects 0.000 description 40
- UFMZWBIQTDUYBN-UHFFFAOYSA-N cobalt dinitrate Chemical compound [Co+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O UFMZWBIQTDUYBN-UHFFFAOYSA-N 0.000 description 38
- 229910001981 cobalt nitrate Inorganic materials 0.000 description 38
- 238000002791 soaking Methods 0.000 description 38
- KGBXLFKZBHKPEV-UHFFFAOYSA-N boric acid Chemical compound OB(O)O KGBXLFKZBHKPEV-UHFFFAOYSA-N 0.000 description 31
- 239000004327 boric acid Substances 0.000 description 31
- RXPAJWPEYBDXOG-UHFFFAOYSA-N hydron;methyl 4-methoxypyridine-2-carboxylate;chloride Chemical compound Cl.COC(=O)C1=CC(OC)=CC=N1 RXPAJWPEYBDXOG-UHFFFAOYSA-N 0.000 description 27
- CHPZKNULDCNCBW-UHFFFAOYSA-N gallium nitrate Chemical compound [Ga+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O CHPZKNULDCNCBW-UHFFFAOYSA-N 0.000 description 26
- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 21
- 230000000052 comparative effect Effects 0.000 description 18
- DAMJCWMGELCIMI-UHFFFAOYSA-N benzyl n-(2-oxopyrrolidin-3-yl)carbamate Chemical compound C=1C=CC=CC=1COC(=O)NC1CCNC1=O DAMJCWMGELCIMI-UHFFFAOYSA-N 0.000 description 17
- URLKBWYHVLBVBO-UHFFFAOYSA-N Para-Xylene Chemical group CC1=CC=C(C)C=C1 URLKBWYHVLBVBO-UHFFFAOYSA-N 0.000 description 16
- 238000006243 chemical reaction Methods 0.000 description 14
- 238000001704 evaporation Methods 0.000 description 13
- 230000008020 evaporation Effects 0.000 description 13
- 229940044658 gallium nitrate Drugs 0.000 description 13
- 238000007598 dipping method Methods 0.000 description 9
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 8
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 8
- 238000004519 manufacturing process Methods 0.000 description 8
- 239000004417 polycarbonate Substances 0.000 description 8
- 229920000515 polycarbonate Polymers 0.000 description 8
- 238000009987 spinning Methods 0.000 description 8
- 239000012855 volatile organic compound Substances 0.000 description 8
- FJBFPHVGVWTDIP-UHFFFAOYSA-N dibromomethane Chemical compound BrCBr FJBFPHVGVWTDIP-UHFFFAOYSA-N 0.000 description 7
- 239000002912 waste gas Substances 0.000 description 7
- 230000000694 effects Effects 0.000 description 6
- 238000006555 catalytic reaction Methods 0.000 description 5
- 229910000510 noble metal Inorganic materials 0.000 description 5
- 238000000746 purification Methods 0.000 description 5
- 230000008030 elimination Effects 0.000 description 4
- 238000003379 elimination reaction Methods 0.000 description 4
- 239000003344 environmental pollutant Substances 0.000 description 4
- 238000011156 evaluation Methods 0.000 description 4
- 239000010815 organic waste Substances 0.000 description 4
- 231100000719 pollutant Toxicity 0.000 description 4
- 230000008569 process Effects 0.000 description 4
- 229910017052 cobalt Inorganic materials 0.000 description 3
- 239000010941 cobalt Substances 0.000 description 3
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 3
- 238000011068 loading method Methods 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- CPELXLSAUQHCOX-UHFFFAOYSA-N Hydrogen bromide Chemical compound Br CPELXLSAUQHCOX-UHFFFAOYSA-N 0.000 description 2
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 2
- 239000007864 aqueous solution Substances 0.000 description 2
- -1 aromatics Chemical class 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 239000007795 chemical reaction product Substances 0.000 description 2
- 238000011161 development Methods 0.000 description 2
- 230000018109 developmental process Effects 0.000 description 2
- 238000005265 energy consumption Methods 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 229930195733 hydrocarbon Natural products 0.000 description 2
- 150000002430 hydrocarbons Chemical class 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 229910052707 ruthenium Inorganic materials 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 1
- CPELXLSAUQHCOX-UHFFFAOYSA-M Bromide Chemical compound [Br-] CPELXLSAUQHCOX-UHFFFAOYSA-M 0.000 description 1
- 239000004215 Carbon black (E152) Substances 0.000 description 1
- 241000282414 Homo sapiens Species 0.000 description 1
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 1
- 244000275012 Sesbania cannabina Species 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 239000004480 active ingredient Substances 0.000 description 1
- 150000001299 aldehydes Chemical class 0.000 description 1
- 150000001335 aliphatic alkanes Chemical class 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000010953 base metal Substances 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000000969 carrier Substances 0.000 description 1
- 239000013064 chemical raw material Substances 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 150000001868 cobalt Chemical class 0.000 description 1
- 238000009841 combustion method Methods 0.000 description 1
- 239000008139 complexing agent Substances 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000012467 final product Substances 0.000 description 1
- 150000008282 halocarbons Chemical class 0.000 description 1
- 230000036541 health Effects 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 150000002576 ketones Chemical class 0.000 description 1
- 238000004898 kneading Methods 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 239000011159 matrix material Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229920000609 methyl cellulose Polymers 0.000 description 1
- 239000001923 methylcellulose Substances 0.000 description 1
- 235000010981 methylcellulose Nutrition 0.000 description 1
- 239000010812 mixed waste Substances 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Substances [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 1
- 229910052573 porcelain Inorganic materials 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 1
- 150000002910 rare earth metals Chemical class 0.000 description 1
- 239000012266 salt solution Substances 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 238000001179 sorption measurement Methods 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- 239000000725 suspension Substances 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N titanium dioxide Inorganic materials O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 239000002699 waste material Substances 0.000 description 1
Classifications
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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
- B01J23/843—Arsenic, antimony or bismuth
-
- 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
- B01J23/70—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
- B01J23/843—Arsenic, antimony or bismuth
- B01J23/8435—Antimony
-
- 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
- B01J23/843—Arsenic, antimony or bismuth
- B01J23/8437—Bismuth
-
- B01J35/60—
-
- B01J35/61—
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G7/00—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals
- F23G7/06—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases
- F23G7/07—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases in which combustion takes place in the presence of catalytic material
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G2209/00—Specific waste
- F23G2209/14—Gaseous waste or fumes
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
Abstract
The invention relates to a catalyst for catalytic combustion treatment of PTA tail gas and application thereof, and mainly solves the problems of high cost and complex preparation process of the existing catalyst. The catalyst is prepared by taking formed alumina as a carrier, taking cobalt oxide as an active component, taking IIIA group element and VA group element oxides as auxiliaries and adopting a step-by-step impregnation method, and then is used for treating the oxidized tail gas of the PTA device. The catalyst has the advantages of low cost, simple preparation process, good catalytic activity and no secondary pollution, can be used for catalytic oxidation treatment of industrial waste gases such as PTA oxidized tail gas and the like under the condition of a wide range of tail gas concentration, and can be used for catalytic oxidation treatment of PTA oxidized tail gas and the like.
Description
Technical Field
The invention relates to a catalyst for treating PTA tail gas by catalytic combustion, belonging to the technical field of environmental protection.
Background
Volatile Organic Compounds (VOCs) are common exhaust pollutants in the petrochemical industry. The kinds of VOCs are various and are mainly classified into eight categories according to their chemical structures: alkanes, aromatics, alkenes, halogenated hydrocarbons, esters, aldehydes, ketones, and others. The direct discharge of VOCs not only causes serious pollution to the environment, but also has serious influence on the indoor air quality, and greatly harms the health of human beings.
Due to the limitation of the technical development level, various VOCs pollutants are inevitably discharged into the atmosphere in many industries related to the national civilization at present. The traditional VOCs treatment method comprises an absorption method, an adsorption method, a condensation method and a direct combustion method, and the methods have the defects of easy generation of secondary pollution, high energy consumption, easy limitation of concentration and temperature of organic waste gas and the like. The catalytic combustion treatment method has the characteristics of high treatment efficiency, low operation temperature, low energy consumption and no secondary pollutant, and can effectively treat pollutants with lower concentration.
Purified Terephthalic Acid (PTA) is an important organic chemical raw material and has wide application in the aspects of chemical fibers, light industry, electronics, buildings and the like. At present, the industrial production of PTA mainly adopts a high-temperature liquid-phase oxidation method, wherein the oxidation waste gas discharged by an oxidation reactor is the organic waste gas with the maximum discharge amount of a PTA device, and the total mass concentration of organic matters exceeds 1000mg/m 3 And include various VOCs such as methyl acetate, p-xylene, brominated hydrocarbons, and the like. Wherein the mass concentration of bromide is about 100mg/m 3 The mass concentration of CO is about 5000mg/m 3 All of them are seriously over the national emission standard.
At present, the catalytic combustion method is a more concerned PTA tail gas emission control technology, and the catalyst for catalytic combustion of PTA waste gas applied in industry mainly focuses on a noble metal catalyst, and noble metals such as Pt and Pd are used as active components, and the catalyst is expensive in price and poor in toxicity resistance to brominated hydrocarbon components in PTA tail gas.
CN 105126834 discloses an integral ruthenium catalyst for purifying PTA oxidized tail gas, the active component is ruthenium simple substance and/or oxide, the first carrier is rutile phase TiO 2 The second carrier being ZrO 2 ，Al 2 O 3 ，SiO 2 Or ZnO, and honeycomb ceramics is adopted as a framework. The catalyst has longer preparation steps, and the noble metal is used as an active component, so the cost is higher. CN 105026041 discloses a base metal catalyst and its use in PTA waste stream treatment, the catalyst uses rare earth metal as carrier, and the cost is also high. CN 102481549 discloses a catalyst deposited on a substrate for destroying CO and volatile organic compounds in an exhaust stream, using platinum group metals as active components and rare earth metal oxides as carriers, which is complicated in preparation process and relatively expensive. CN 103252242 discloses a non-noble metal catalyst for catalytic combustion of PTA tail gas, which takes honeycomb ceramics as a matrix and CeO 2 As coating, non-noble metals CuO, mnO 2 Is an active component, and the preparation process is complex. Therefore, the catalyst which has the advantages of low development cost, simple preparation process and good elimination effect has good industrial application prospect.
Disclosure of Invention
The invention aims to provide a catalyst for treating PTA tail gas by catalytic combustion, aiming at the problem of high cost of the precious metal catalyst for treating PTA tail gas at present, transition metal with lower price is used as an active component, and a preparation process with shorter steps is adopted to achieve a better elimination effect.
The second technical problem solved by the invention is a preparation method of the catalyst corresponding to the first problem.
The third technical problem solved by the invention is the application of the catalyst corresponding to the first problem.
In order to solve the technical problem one, the technical scheme adopted by the invention is as follows: the catalyst for treating PTA tail gas by catalytic combustion comprises the following components in parts by weight:
a) Taking the formed alumina as a carrier, wherein the carrier is 56-82 parts of the weight of the catalyst;
b) Taking cobalt oxide as an active component, wherein the active component is 15-35 parts of the catalyst by weight;
c) The IIIA group element oxide is used as an auxiliary agent, and the auxiliary agent is 2-5 parts of the catalyst by weight.
d) The V A group element oxide is used as an auxiliary agent, and the auxiliary agent accounts for 1-4 parts of the weight of the catalyst.
In the above technical solution, the carrier is preferably cylindrical alumina formed by extrusion molding, and the diameter of the cylindrical alumina is preferably 1 to 6mm, and more preferably 2 to 3mm.
In the above technical scheme, the carrier is spherical alumina.
In the technical scheme, the content of the active component cobalt oxide is preferably 20-30 parts by weight of the catalyst.
In the above technical solution, the IIIA group auxiliary agent is selected from at least one of B and Ga, and the VA group auxiliary agent is selected from at least one of Sb and Bi. The IIIA group promoter is preferably 3-4 parts of catalyst by weight, and the VA group promoter is preferably 2-3 parts of catalyst by weight.
The preparation method of the catalyst for treating PTA tail gas by catalytic combustion comprises the steps of firstly loading IIIA family auxiliary agent components by an equivalent impregnation method, drying and roasting a carrier, and then loading active components and VA family auxiliary agent by a sol-gel deposition method in one step. The method specifically comprises the following steps:
1) Extruding and molding an alumina carrier: kneading the alumina powder and the extrusion assistant into a ball and then extruding the ball into strips. Wherein the alumina is gamma-alumina, and the extrusion assistant comprises nitric acid, water, sesbania powder and methyl cellulose.
The spherical alumina is commercially available spherical alumina.
2) Modification of the carrier: loading the salt solution of IIIA group elements onto the formed carrier by equivalent impregnation at 20-60 deg.c for 4-8 hr, drying at 90-150 deg.c for 8-12 hr at 350-450 deg.c for 2-6 hr, and obtaining the assistant modified carrier.
3) Impregnation of active ingredients: uniformly mixing an aqueous solution of cobalt salt, an aqueous solution of VA group element salt and a complexing agent by adopting a sol-gel deposition method to generate a sol-gel solution, adding an auxiliary agent modified carrier into the sol-gel solution, wherein the dipping temperature is 60-80 ℃, and aging for 2-4 hours after the stirring is stopped for 4-8 hours of dipping time. And (3) removing the carrier after aging, drying and roasting at the drying temperature of 90-150 ℃ for 8-12 hours at the roasting temperature of 400-550 ℃ for 4-6 hours to obtain the supported cobalt catalyst.
The application of the supported cobalt catalyst in the treatment of the oxidized tail gas of the PTA device can adopt the following process conditions: 1) Pretreatment of a catalyst: treating the catalyst in air at 400-550 deg.c for 1-3 hr; 2) Catalytic oxidation: after the organic waste gas and air are uniformly mixed, catalytic oxidation reaction is carried out in a reactor, the reaction temperature is 150-400 ℃, the reaction pressure is 0.05-0.10 MPa, the concentration of the organic waste gas is 500-25000ppm, and the amount of the waste gas treated by the catalyst per gram is 5-50L per hour.
Compared with the prior art, the invention adopts the transition metal cobalt as the active component, adopts the preparation process with shorter steps, achieves better elimination effect, and has high activity and stability as well as lower price and cost. The formed alumina carrier has larger specific surface area and proper pore distribution, the mechanical strength can reach more than 100N/cm, and the formed alumina carrier has certain surface acidity, so that active components can be highly dispersed on the surface of the carrier.
The treatment of the oxidation off-gas of the PTA unit can be carried out in a fixed bed continuous flow reactor, the process of which is briefly described as follows: the required amount of catalyst is put into the constant temperature area of the reactor, and the upper and lower parts of the catalyst are filled with porcelain rings. The main components of the oxidation tail gas of the PTA device are methyl acetate, paraxylene and dibromomethane. Under the set temperature and pressure, the waste gas is fed to a preheater by a flowmeter, mixed and gasified with oxygen and nitrogen, then enters the upper end of a reactor, flows through a catalyst bed layer for catalytic reaction, a reaction product is directly injected by a valve and enters a gas chromatograph, and the conversion rate of the waste gas and the selectivity of the product are analyzed on line.
The catalyst prepared by the method is used for PTA tail gas treatment reaction, the purification rate of mixed waste gas is more than 99% at the reaction temperature of 275-350 ℃, and the reaction product is CO 2 ，H 2 O, HBr and Br 2 The selectivity of the final product carbon dioxide is more than 99 percent. Wherein HBr and Br 2 Can be completely absorbed by the alkali solution, has good elimination effect, keeps the performance of the catalyst stable, and obtains better technical effect.
The invention is further illustrated by the following examples.
Detailed Description
[ example 1 ]
Firstly, adding 1.77g of boric acid into 200ml of deionized water to prepare a solution 1, then adding 81g of cylindrical alumina carrier with the diameter of 1mm into the solution 1, dipping for 4 hours at 40 ℃, then spin-drying the dipped sample, and then putting the sample into an oven to dry for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 5.60g of citric acid, 18.13g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 1, wherein the content of each component in the example 1 is shown in table 1.
[ example 2 ]
Firstly, adding 1.77g of boric acid into 200ml of deionized water to prepare a solution 1, then adding 81g of cylindrical alumina carrier with the diameter of 6mm into the solution 1, dipping for 4 hours at 40 ℃, then spin-drying the dipped sample, and then putting the sample into an oven to dry for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 5.60g of citric acid, 18.13g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 2, wherein the content of each component in the example 2 is shown in table 1.
[ example 3 ] A method for producing a polycarbonate
Firstly, 1.77g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 81g of cylindrical alumina carrier with the diameter of 2mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 5.60g of citric acid, 18.13g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 3, wherein the content of each component in the example 3 is shown in table 1.
[ example 4 ] A method for producing a polycarbonate
Firstly, 1.77g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 81g of cylindrical alumina carrier with the diameter of 2mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 5.60g of citric acid, 18.13g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 4, wherein the content of each component in the example 4 is shown in table 1.
[ example 5 ] A method for producing a polycarbonate
Firstly, adding 1.77g of boric acid into 200ml of deionized water to prepare a solution 1, then adding 61g of cylindrical alumina carrier with the diameter of 3mm into the solution 1, dipping for 4 hours at 40 ℃, then spin-drying the dipped sample, and then putting the sample into an oven to dry for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 12.57g of citric acid, 42.30g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 5, wherein the content of each component in the example 5 is shown in table 1.
[ example 6 ]
Firstly, adding 1.77g of boric acid into 200ml of deionized water to prepare a solution 1, then adding 76g of cylindrical alumina carrier with the diameter of 3mm into the solution 1, dipping for 4 hours at 40 ℃, then spin-drying the dipped sample, and then putting the sample into an oven to dry for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 7.34g of citric acid, 24.17g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 6, wherein the content of each component in the example 6 is shown in table 1.
[ example 7 ] A method for producing a polycarbonate
Firstly, adding 1.77g of boric acid into 200ml of deionized water to prepare a solution 1, then adding 71g of cylindrical alumina carrier with the diameter of 3mm into the solution 1, dipping for 4 hours at 40 ℃, then spin-drying the dipped sample, and then putting the sample into an oven to dry for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.08g of citric acid, 30.21g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 7, wherein the content of each component in the example 7 is shown in table 1.
[ example 8 ]
Firstly, adding 1.77g of boric acid into 200ml of deionized water to prepare a solution 1, then adding 66g of cylindrical alumina carrier with the diameter of 3mm into the solution 1, dipping for 4 hours at 40 ℃, then spin-drying the dipped sample, and then putting the sample into an oven to dry for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 10.83g of citric acid, 36.25g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 8, wherein the content of each component in the example 8 is shown in table 1.
[ example 9 ]
Firstly, 4.44g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 68g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.08g of citric acid, 30.21g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 9, wherein the content of each component in the example 9 is shown in table 1.
[ example 10 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 70g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at the temperature of 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at the temperature of 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 9.08g of citric acid, 30.21g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 10, wherein the content of each component in the example 10 is shown in table 1.
[ example 11 ]
Firstly, 3.55g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.08g of citric acid, 30.21g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 11, wherein the content of each component in the example 11 is shown in table 1.
[ example 12 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 71g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 8.91g of citric acid, 30.21g of cobalt nitrate and 1.04g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 12, wherein the content of each component in the example 12 is shown in table 1.
[ example 13 ] to prepare a suspension
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 9.27g of citric acid, 30.21g of cobalt nitrate and 3.12g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 13, wherein the content of each component in the example 13 is shown in table 1.
[ example 14 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, 68g of a cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.45g of citric acid, 30.21g of cobalt nitrate and 4.16g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 14, wherein the content of each component in the example 14 is shown in table 1.
[ example 15 ] A method for producing a polycarbonate
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 71g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.02g of citric acid, 30.21g of cobalt nitrate and 0.78g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 15, wherein the content of each component in the example 15 is shown in table 1.
[ example 16 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 70g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at the temperature of 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at the temperature of 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.30g of citric acid, 30.21g of cobalt nitrate and 1.56g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 16, wherein the content of each component in the example 16 is shown in Table 1.
[ example 17 ] to provide
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 9.59g of citric acid, 30.21g of cobalt nitrate and 2.35g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 17, wherein the content of each component in the example 17 is shown in Table 1.
[ example 18 ] A method for producing a polycarbonate
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, 68g of a cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 9.88g of citric acid, 30.21g of cobalt nitrate and 3.13g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 18, wherein the content of each component in the example 18 is shown in table 1.
[ example 19 ]
Firstly, 4.09g of gallium nitrate is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at the temperature of 40 ℃, and then the soaked sample is dried by evaporation in a rotary manner and then is placed into an oven to be dried for 12 hours at the temperature of 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 9.26g of citric acid, 30.21g of cobalt nitrate and 3.12g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 19, wherein the content of each component in the example 19 is shown in table 1.
[ example 20 ]
Firstly, 4.09g of gallium nitrate is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at the temperature of 40 ℃, and then the soaked sample is dried by evaporation in a rotary manner and then is placed into an oven to be dried for 12 hours at the temperature of 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.59g of citric acid, 30.21g of cobalt nitrate and 2.35g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 20, wherein the content of each component in the example 20 is shown in table 1.
[ example 21 ]
Firstly, 1.77g of boric acid and 1.36g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, then 69g of a cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by spinning to dryness and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.26g of citric acid, 30.21g of cobalt nitrate and 3.12g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 21, wherein the content of each component in the example 21 is shown in table 1.
[ example 22 ]
Firstly, 1.33g of boric acid and 2.04g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried in an oven by spinning to dryness and then is dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.26g of citric acid, 30.21g of cobalt nitrate and 3.12g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 22, wherein the content of each component in the example 22 is shown in table 1.
[ example 23 ]
Firstly, 0.89g of boric acid and 2.73g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, then 69g of a cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by spinning to dryness and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 9.26g of citric acid, 30.21g of cobalt nitrate and 3.12g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 23, wherein the content of each component in the example 23 is shown in table 1.
[ example 24 ] A method for producing a polycarbonate
Firstly, 1.77g of boric acid and 1.36g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried in an oven by spinning to dryness and then is dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.59g of citric acid, 30.21g of cobalt nitrate and 2.35g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 24, wherein the content of each component in the example 24 is shown in Table 1.
[ example 25 ]
Firstly, 1.33g of boric acid and 2.04g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried in an oven by spinning to dryness and then is dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.59g of citric acid, 30.21g of cobalt nitrate and 2.35g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 25, wherein the content of each component in the example 25 is shown in Table 1.
[ example 26 ]
Firstly, 0.89g of boric acid and 2.73g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried in an oven by spinning to dryness and then is dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.59g of citric acid, 30.21g of cobalt nitrate and 2.35g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven for drying at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain example 26, wherein the content of each component in the example 26 is shown in Table 1.
[ example 27 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then calcined in a muffle furnace at 400 ℃ for 3 hours. Adding 9.38g of citric acid, 30.21g of cobalt nitrate, 2.08g of bismuth nitrate and 0.78g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, stopping stirring, aging for 2 hours, drying by rotary evaporation, putting into an oven at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 27, wherein the content of each component in the example 27 is shown in Table 1.
[ example 28 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.43g of citric acid, 30.21g of cobalt nitrate, 1.56g of bismuth nitrate and 1.17g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, stopping stirring, aging for 2 hours, drying by rotary evaporation, putting into an oven at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 28, wherein the content of each component in the example 28 is shown in Table 1.
[ example 29 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried by rotary evaporation and then is put into an oven to be dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.48g of citric acid, 30.21g of cobalt nitrate, 1.04g of bismuth nitrate and 1.57g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, stopping stirring, aging for 2 hours, drying by rotary evaporation, putting into an oven at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 29, wherein the content of each component in the example 29 is shown in Table 1.
[ example 30 ]
Firstly, 4.09g of gallium nitrate is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at the temperature of 40 ℃, and then the soaked sample is dried by evaporation in a rotary manner and then is placed into an oven to be dried for 12 hours at the temperature of 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.38g of citric acid, 30.21g of cobalt nitrate, 2.08g of bismuth nitrate and 0.78g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 30, wherein the content of each component in the example 30 is shown in Table 1.
[ example 31 ]
Firstly, 4.09g of gallium nitrate is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at the temperature of 40 ℃, and then the soaked sample is dried by evaporation in a rotary manner and then is placed into an oven to be dried for 12 hours at the temperature of 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.43g of citric acid, 30.21g of cobalt nitrate, 1.56g of bismuth nitrate and 1.17g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, stopping stirring, aging for 2 hours, drying by rotary evaporation, putting into an oven at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 31, wherein the content of each component in the example 31 is shown in Table 1.
[ example 32 ] A method for producing a polycarbonate
Firstly, 4.09g of gallium nitrate is added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at the temperature of 40 ℃, and then the soaked sample is dried by evaporation in a rotary manner and then is placed into an oven to be dried for 12 hours at the temperature of 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.48g of citric acid, 30.21g of cobalt nitrate, 1.04g of bismuth nitrate and 1.57g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 32, wherein the content of each component in the example 32 is shown in Table 1.
[ example 33 ]
Firstly, 1.33g of boric acid and 2.04g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, then 69g of cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be soaked for 4 hours at 40 ℃, and then the soaked sample is dried in an oven by spinning to dryness and then is dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 9.43g of citric acid, 30.21g of cobalt nitrate, 1.56g of bismuth nitrate and 1.17g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, stopping stirring, aging for 2 hours, drying by rotary evaporation, putting into an oven at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain an example 33, wherein the content of each component in the example 33 is shown in Table 1.
Comparative example 1
Firstly, adding 1.77g of boric acid into 200ml of deionized water to prepare a solution 1, then adding 81g of cylindrical alumina carrier with the diameter of 8mm into the solution 1, dipping for 4 hours at 40 ℃, then spin-drying the dipped sample, and then putting the sample into an oven to dry for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 5.60g of citric acid, 18.13g of cobalt nitrate and 2.08g of bismuth nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain a comparative example 1, wherein the content of each component in the comparative example 1 is shown in table 1.
Comparative example 2
Adding 8.73g of citric acid and 30.21g of cobalt nitrate into 300ml of deionized water to prepare a solution 1, adding 75g of a cylindrical alumina carrier with the diameter of 3mm into the solution 1, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven to dry at 110 ℃ for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain a comparative example 2, wherein the content of each component in the comparative example 2 is shown in Table 1.
[ COMPARATIVE EXAMPLE 3 ]
Firstly, 2.66g of boric acid is added into 200ml of deionized water to prepare a solution 1, then 72g of a cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by evaporation in a drying oven for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 8.73g of citric acid and 30.21g of cobalt nitrate into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, placing into an oven to dry at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain a comparative example 3, wherein the content of each component in the comparative example 3 is shown in table 1.
Comparative example 4
Adding 9.27g of citric acid, 30.21g of cobalt nitrate and 3.12g of antimony trichloride into 200ml of deionized water to prepare a solution 1, adding 72g of a cylindrical alumina carrier with the diameter of 3mm into the solution 1, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven at 110 ℃ for drying for 12 hours, and roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain a comparative example 4, wherein the content of each component in the comparative example 4 is shown in Table 1.
[ COMPARATIVE EXAMPLE 5 ]
Firstly, 1.33g of boric acid and 2.04g of gallium nitrate are added into 200ml of deionized water to prepare a solution 1, 84g of a cylindrical alumina carrier with the diameter of 3mm is added into the solution 1 to be impregnated for 4 hours at 40 ℃, and then the impregnated sample is dried by spinning to dryness and then is placed into an oven to be dried for 12 hours at 110 ℃. The dried sample was then fired in a muffle furnace at 400 ℃ for 3 hours. Adding 4.19g of citric acid, 12.08g of cobalt nitrate, 1.56g of bismuth nitrate and 1.17g of antimony trichloride into 300ml of deionized water to prepare a solution 2, adding a roasted sample into the solution 2, stirring and soaking at 60 ℃ for 4 hours, aging for 2 hours after stopping stirring, drying by rotary evaporation, putting into an oven at 110 ℃ for 12 hours, roasting the dried sample in a muffle furnace at 500 ℃ for 4 hours to obtain a comparative example 5, wherein the content of each component in the comparative example 5 is shown in Table 1.
[ example 34 ]
The performance evaluation of the catalytic reaction was carried out under the same conditions in examples 1 to 33 and comparative examples 1 to 5 on a catalytic reaction apparatus of a continuous flow fixed bed reactor. In this experiment, the single evaluation concentrations of the main components of the exhaust gas were: 20000ppm of methyl acetate, 5000ppm of p-xylene, 500ppm of dibromomethane, and the concentrations of the mixed samples are as follows: 12000ppm of methyl acetate, 2000ppm of p-xylene and 200ppm of dibromomethane. The process conditions evaluated were: the reaction pressure is 0.05MPa to 0.10MPa, the waste gas amount treated by each gram of catalyst is 25L per hour, and the temperature is programmed to be oppositeThe temperature is adjusted to 400 ℃. The results of the reactions of examples 1 to 32 and comparative examples 1 to 5 described above are shown in Table 1. Wherein T is 99 The reaction temperature at which the purification rate of the component in the exhaust gas was 99% was indicated. T of Mixed sample 99 Expressed as the reaction temperature at which the purification of all components reached 99%. Tn of the mixed sample indicates that the purifying rate of dibromomethane at 400 ℃ is n%, and the purifying rate of methyl acetate and paraxylene reaches more than 99%.
TABLE 1
[ example 35 ]
The performance evaluation of the catalytic reaction was carried out under the same conditions on the catalytic reaction apparatus of the continuous flow fixed bed reactor in examples 13, 19, 22, 28, 33 and comparative examples 3, 4. In this experiment, the single evaluation concentrations of the main components of the exhaust gas were: 20000ppm of methyl acetate, 5000ppm of p-xylene, 500ppm of dibromomethane, and the concentrations of mixed samples are as follows: 12000ppm of methyl acetate, 2000ppm of p-xylene and 200ppm of dibromomethane. The process conditions evaluated were: the reaction pressure is 0.05 MPa-0.10 MPa, the amount of the waste gas treated by each gram of the catalyst is 50L per hour, the temperature is programmed to the reaction temperature until 400 ℃, and the reaction results are shown in Table 2. Wherein T is 99 The reaction temperature at which the purification rate of the component in the exhaust gas was 99% was indicated. T of Mixed sample 99 Expressed as the reaction temperature at which the purification of all components reached 99%. Tn of the mixed sample indicates that the purifying rate of dibromomethane at 400 ℃ is n%, and the purifying rate of methyl acetate and paraxylene reaches more than 99%.
TABLE 2
Claims (7)
1. The catalyst for treating PTA tail gas through catalytic combustion is characterized by comprising the following components in parts by weight:
a) Taking the formed alumina as a carrier, wherein the carrier is 56-82 parts of the weight of the catalyst;
b) Taking cobalt oxide as an active component, wherein the active component is 15-35 parts of the catalyst by weight;
c) Taking IIIA group element oxide as an auxiliary agent, wherein the auxiliary agent is 2-5 parts of the catalyst by weight;
d) The V A group element oxide is taken as an auxiliary agent, and the auxiliary agent is 1-4 parts of the catalyst by weight;
the IIIA group element is selected from at least one of B and Ga;
the element of VA group is at least one selected from Sb and Bi.
2. The catalyst of claim 1, which is used for catalytic combustion treatment of PTA tail gas, wherein the formed alumina is a cylindrical alumina with a diameter of 1-6 mm formed by extrusion.
3. The catalyst for catalytic combustion processing of PTA exhaust gas according to claim 1, wherein the cobalt oxide active component is 20-30 parts by weight of the catalyst.
4. The catalyst for catalytic combustion treatment of PTA tail gas according to claim 1, wherein the group IIIA promoter is 3-4 parts by weight of the catalyst.
5. The catalyst for catalytic combustion processing of PTA tail gas according to claim 1, wherein the group va promoter is 2-3 parts by weight of the catalyst.
6. The preparation method of any one of the catalysts for catalytic combustion treatment of PTA tail gas as claimed in claims 1 to 5, wherein the group IIIA promoter component is loaded by an equivalent impregnation method, and after the carrier is dried and roasted, the active component and the group VA promoter are loaded by one step by a sol-gel deposition method.
7. Use of a catalyst for catalytic combustion treatment of PTA exhaust gas according to any of claims 1-5 wherein the treatment of exhaust gas containing 500-25000ppm per gram of catalyst is 5-50L per hour.
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| CN1314206A (en) * | 2000-03-22 | 2001-09-26 | 中国科学院大连化学物理研究所 | Metal oxide catalyst for clearing halogenated aromatic through catalytic oxidation |
| JP2005034677A (en) * | 2003-07-15 | 2005-02-10 | Mitsui Eng & Shipbuild Co Ltd | Catalyst for treating exhaust gas and method for treating exhaust gas |
| CN101443118A (en) * | 2006-05-08 | 2009-05-27 | Bp北美公司 | Process for the production of aromatic carboxylic acids in water |
| CN103894200A (en) * | 2014-04-22 | 2014-07-02 | 华东理工大学 | Method and catalyst for low-temperature catalytic combustion elimination of polychlorinated aromatic hydrocarbon |
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| CN1314206A (en) * | 2000-03-22 | 2001-09-26 | 中国科学院大连化学物理研究所 | Metal oxide catalyst for clearing halogenated aromatic through catalytic oxidation |
| JP2005034677A (en) * | 2003-07-15 | 2005-02-10 | Mitsui Eng & Shipbuild Co Ltd | Catalyst for treating exhaust gas and method for treating exhaust gas |
| CN101443118A (en) * | 2006-05-08 | 2009-05-27 | Bp北美公司 | Process for the production of aromatic carboxylic acids in water |
| CN103894200A (en) * | 2014-04-22 | 2014-07-02 | 华东理工大学 | Method and catalyst for low-temperature catalytic combustion elimination of polychlorinated aromatic hydrocarbon |
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