CN112588314B - Catalyst for producing propane by converting light hydrocarbon and preparation method and application thereof - Google Patents
Catalyst for producing propane by converting light hydrocarbon and preparation method and application thereof Download PDFInfo
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- CN112588314B CN112588314B CN202011476119.8A CN202011476119A CN112588314B CN 112588314 B CN112588314 B CN 112588314B CN 202011476119 A CN202011476119 A CN 202011476119A CN 112588314 B CN112588314 B CN 112588314B
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- molecular sieve
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- propane
- light hydrocarbon
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- ATUOYWHBWRKTHZ-UHFFFAOYSA-N Propane Chemical compound CCC ATUOYWHBWRKTHZ-UHFFFAOYSA-N 0.000 title claims abstract description 90
- 239000003054 catalyst Substances 0.000 title claims abstract description 87
- 239000001294 propane Substances 0.000 title claims abstract description 45
- 229930195733 hydrocarbon Natural products 0.000 title claims abstract description 24
- 150000002430 hydrocarbons Chemical class 0.000 title claims abstract description 24
- 239000004215 Carbon black (E152) Substances 0.000 title claims abstract description 22
- 238000002360 preparation method Methods 0.000 title description 5
- 239000002808 molecular sieve Substances 0.000 claims abstract description 94
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims abstract description 94
- 238000001035 drying Methods 0.000 claims abstract description 22
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 19
- 230000032683 aging Effects 0.000 claims abstract description 13
- 238000012986 modification Methods 0.000 claims abstract description 10
- 230000004048 modification Effects 0.000 claims abstract description 10
- 229910052725 zinc Inorganic materials 0.000 claims abstract description 9
- 239000011230 binding agent Substances 0.000 claims abstract description 8
- 229910052680 mordenite Inorganic materials 0.000 claims abstract description 8
- 229910052802 copper Inorganic materials 0.000 claims abstract description 7
- 229910052733 gallium Inorganic materials 0.000 claims abstract description 7
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 7
- 229910052698 phosphorus Inorganic materials 0.000 claims abstract description 7
- 238000006243 chemical reaction Methods 0.000 claims description 25
- 239000000843 powder Substances 0.000 claims description 20
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 12
- 238000002156 mixing Methods 0.000 claims description 10
- 229910052761 rare earth metal Inorganic materials 0.000 claims description 10
- VXAUWWUXCIMFIM-UHFFFAOYSA-M aluminum;oxygen(2-);hydroxide Chemical compound [OH-].[O-2].[Al+3] VXAUWWUXCIMFIM-UHFFFAOYSA-M 0.000 claims description 9
- 238000011068 loading method Methods 0.000 claims description 9
- 150000002910 rare earth metals Chemical class 0.000 claims description 8
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical group O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 7
- 238000003756 stirring Methods 0.000 claims description 7
- 238000000034 method Methods 0.000 claims description 6
- 229910052593 corundum Inorganic materials 0.000 claims description 4
- 150000002909 rare earth metal compounds Chemical class 0.000 claims description 4
- 229910001845 yogo sapphire Inorganic materials 0.000 claims description 4
- 229910052684 Cerium Inorganic materials 0.000 claims description 3
- 229910052681 coesite Inorganic materials 0.000 claims description 3
- 229910052906 cristobalite Inorganic materials 0.000 claims description 3
- 229910052746 lanthanum Inorganic materials 0.000 claims description 3
- 239000000377 silicon dioxide Substances 0.000 claims description 3
- 229910052682 stishovite Inorganic materials 0.000 claims description 3
- 229910052905 tridymite Inorganic materials 0.000 claims description 3
- 229910052779 Neodymium Inorganic materials 0.000 claims description 2
- 229910052777 Praseodymium Inorganic materials 0.000 claims description 2
- 238000005470 impregnation Methods 0.000 claims description 2
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical compound O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 claims description 2
- 238000000967 suction filtration Methods 0.000 claims description 2
- 239000002131 composite material Substances 0.000 abstract description 7
- 238000004898 kneading Methods 0.000 abstract description 7
- 229910052751 metal Inorganic materials 0.000 abstract description 6
- 239000002184 metal Substances 0.000 abstract description 6
- 239000002253 acid Substances 0.000 abstract description 4
- 230000000694 effects Effects 0.000 abstract description 3
- 239000000969 carrier Substances 0.000 abstract description 2
- 238000004939 coking Methods 0.000 abstract description 2
- 239000000203 mixture Substances 0.000 description 16
- 239000008367 deionised water Substances 0.000 description 13
- 229910021641 deionized water Inorganic materials 0.000 description 13
- 238000005303 weighing Methods 0.000 description 13
- IJDNQMDRQITEOD-UHFFFAOYSA-N n-butane Chemical compound CCCC IJDNQMDRQITEOD-UHFFFAOYSA-N 0.000 description 11
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 10
- 239000001273 butane Substances 0.000 description 9
- 239000002994 raw material Substances 0.000 description 8
- 238000002791 soaking Methods 0.000 description 7
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 description 6
- 229910017604 nitric acid Inorganic materials 0.000 description 6
- 239000003921 oil Substances 0.000 description 6
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 239000003502 gasoline Substances 0.000 description 5
- 229910021536 Zeolite Inorganic materials 0.000 description 4
- 239000007795 chemical reaction product Substances 0.000 description 4
- 238000004587 chromatography analysis Methods 0.000 description 4
- 238000005336 cracking Methods 0.000 description 4
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 4
- 239000000047 product Substances 0.000 description 4
- 239000010457 zeolite Substances 0.000 description 4
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- 150000001335 aliphatic alkanes Chemical class 0.000 description 3
- CSDREXVUYHZDNP-UHFFFAOYSA-N alumanylidynesilicon Chemical compound [Al].[Si] CSDREXVUYHZDNP-UHFFFAOYSA-N 0.000 description 3
- 229910052782 aluminium Inorganic materials 0.000 description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 3
- 230000008901 benefit Effects 0.000 description 3
- 238000006356 dehydrogenation reaction Methods 0.000 description 3
- 238000011161 development Methods 0.000 description 3
- 230000018109 developmental process Effects 0.000 description 3
- AFABGHUZZDYHJO-UHFFFAOYSA-N dimethyl butane Natural products CCCC(C)C AFABGHUZZDYHJO-UHFFFAOYSA-N 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- -1 liquefied gas Chemical class 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- TWRXJAOTZQYOKJ-UHFFFAOYSA-L Magnesium chloride Chemical compound [Mg+2].[Cl-].[Cl-] TWRXJAOTZQYOKJ-UHFFFAOYSA-L 0.000 description 2
- 238000005899 aromatization reaction Methods 0.000 description 2
- 239000006227 byproduct Substances 0.000 description 2
- 229910000420 cerium oxide Inorganic materials 0.000 description 2
- 238000009826 distribution Methods 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- NNPPMTNAJDCUHE-UHFFFAOYSA-N isobutane Chemical compound CC(C)C NNPPMTNAJDCUHE-UHFFFAOYSA-N 0.000 description 2
- 238000006317 isomerization reaction Methods 0.000 description 2
- QWTDNUCVQCZILF-UHFFFAOYSA-N isopentane Chemical compound CCC(C)C QWTDNUCVQCZILF-UHFFFAOYSA-N 0.000 description 2
- TVMXDCGIABBOFY-UHFFFAOYSA-N octane Chemical compound CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 2
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 2
- 239000012188 paraffin wax Substances 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 239000010703 silicon Substances 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 229910000323 aluminium silicate Inorganic materials 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 238000003889 chemical engineering Methods 0.000 description 1
- 238000003776 cleavage reaction Methods 0.000 description 1
- 239000013065 commercial product Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 239000012084 conversion product Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000000446 fuel Substances 0.000 description 1
- 239000002737 fuel gas Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- VLKZOEOYAKHREP-UHFFFAOYSA-N hexane Substances CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 239000001282 iso-butane Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000000643 oven drying Methods 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 230000007017 scission Effects 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/005—Mixtures of molecular sieves comprising at least one molecular sieve which is not an aluminosilicate zeolite, e.g. from groups B01J29/03 - B01J29/049 or B01J29/82 - B01J29/89
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/80—Mixtures of different zeolites
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/82—Phosphates
- B01J29/84—Aluminophosphates containing other elements, e.g. metals, boron
- B01J29/85—Silicoaluminophosphates [SAPO compounds]
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/02—Impregnation, coating or precipitation
- B01J37/0201—Impregnation
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/10—Heat treatment in the presence of water, e.g. steam
-
- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G11/00—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
- C10G11/02—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils characterised by the catalyst used
- C10G11/04—Oxides
- C10G11/05—Crystalline alumino-silicates, e.g. molecular sieves
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
- B01J2229/10—After treatment, characterised by the effect to be obtained
- B01J2229/18—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself
- B01J2229/186—After treatment, characterised by the effect to be obtained to introduce other elements into or onto the molecular sieve itself not in framework positions
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/08—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y
- B01J29/085—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the faujasite type, e.g. type X or Y containing rare earth elements, titanium, zirconium, hafnium, zinc, cadmium, mercury, gallium, indium, thallium, tin or lead
- B01J29/088—Y-type faujasite
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/18—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the mordenite type
- B01J29/185—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the mordenite type containing rare earth elements, titanium, zirconium, hafnium, zinc, cadmium, mercury, gallium, indium, thallium, tin or lead
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/40—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively
- B01J29/405—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of the pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11, as exemplified by patent documents US3702886, GB1334243 and US3709979, respectively containing rare earth elements, titanium, zirconium, hafnium, zinc, cadmium, mercury, gallium, indium, thallium, tin or lead
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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
- B01J29/00—Catalysts comprising molecular sieves
- B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
- B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
- B01J29/70—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65
- B01J29/7049—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof of types characterised by their specific structure not provided for in groups B01J29/08 - B01J29/65 containing rare earth elements, titanium, zirconium, hafnium, zinc, cadmium, mercury, gallium, indium, thallium, tin or lead
- B01J29/7057—Zeolite Beta
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/20—Characteristics of the feedstock or the products
- C10G2300/30—Physical properties of feedstocks or products
- C10G2300/305—Octane number, e.g. motor octane number [MON], research octane number [RON]
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2300/00—Aspects relating to hydrocarbon processing covered by groups C10G1/00 - C10G99/00
- C10G2300/70—Catalyst aspects
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G2400/00—Products obtained by processes covered by groups C10G9/00 - C10G69/14
- C10G2400/28—Propane and butane
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Materials Engineering (AREA)
- Crystallography & Structural Chemistry (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- General Chemical & Material Sciences (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Catalysts (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
A catalyst for producing propane by converting light hydrocarbon is prepared by adding binder into active component of molecular sieve, kneading, extruding, drying and roasting; then, one or more of Zn, Ga, Ni, Ag, Mo, Cu and P are used as modification elements to modify the elements, and then the elements are dried and roasted; finally, carrying out aging treatment by using water vapor to obtain the catalyst for producing propane by converting light hydrocarbon. The invention mixes HZSM-5 molecular sieve, modified Y-type molecular sieve and at least one of beta molecular sieve, mordenite and SAPO-34 molecular sieve to prepare a composite carrier, and reasonably utilizes the active sites of the three carriers; the activity and the selectivity of the catalyst are further effectively improved through metal modification treatment, and the yield of the target product propane is improved; through high-temperature hydrothermal aging treatment, the optimal acid amount and acid strength on the composite carrier are obtained, the anti-coking capability and stability of the catalyst can be effectively improved, and the propane selectivity of the catalyst is further improved.
Description
Technical Field
The invention relates to a catalyst, in particular to a catalyst for producing propane by converting light hydrocarbon, and a preparation method and application thereof.
Background
In recent years, domestic propane dehydrogenation projects start a round of investment and a round of investment, with the arrival of a large number of propane dehydrogenation projects, the source of raw material propane becomes an important topic of interest of dehydrogenation enterprises, coastal cities can rely on imported propane, but the newly built domestic PDH projects are mainly considered to be the source of propane, the domestic propane is mainly derived from refinery liquefied gas or oil field associated gas, the content of propane is low, the storage is dispersed, the sulfur content is high, and most of refinery liquefied gas mainly comprising butane is mainly used as fuel gas. In addition, only a part of refinery byproducts such as C5C6 light hydrocarbon and light naphtha are used as fuel, thereby causing great resource waste. Therefore, the development of a catalyst for producing propane by converting light hydrocarbon components (such as butane liquefied gas, C5C6 alkane, light naphtha and the like) is extremely important for solving the current situation of insufficient supply of propane raw materials in China.
The invention patent with the application number of CN201110143584.4 discloses a catalyst for producing propane and high-octane gasoline from butane, in particular to hydrogen type silicon-aluminum mesoporous zeolite, and in the embodiment 13, the conversion rate of the butane is only 72.6 percent at most, and the yield of the propane is only 55.25 percent at most.
The invention patent with publication number CN110947417A discloses a catalyst for producing propane and gasoline from paraffin, which comprises a composite carrier and rare earth oxide with the content of 0.1-2.0 mass percent calculated by taking the carrier as a reference, wherein the composite carrier comprises 5-85 mass percent of ZSM-5 zeolite, 5-85 mass percent of MCM-41 zeolite and 5-40 mass percent of alumina. The catalyst is used for converting alkane under non-hydrogenation condition, has high propane yield and produces gasoline blending component with high octane number as side product.
The invention patent with publication number CN111229299A discloses a catalyst for high-efficiency isomerization and aromatization of straight-chain paraffin and a preparation method thereof. The catalyst is metal-loaded and highly porous aluminosilicate (ZSM-5), and can efficiently perform isomerization or aromatization conversion on a straight-chain C3-C12 alkane raw material so as to produce high-octane isoparaffin and high-quality gasoline components.
The catalyst for producing propane only adopts hydrogen type silicon-aluminum zeolite or selects a rare earth metal modified composite molecular sieve catalyst, so that the single-pass conversion rate of raw materials and the propane selectivity are low, the device circulation volume is large, the investment is increased, the economic benefit is low, and the optimal benefit cannot be created for enterprises; in addition, the research on the catalyst for simultaneously converting C4-C12 light hydrocarbon into high-yield propane under milder conditions has not been reported.
Disclosure of Invention
Aiming at the technical defects of the existing propane catalyst production technology, the first purpose of the invention is to provide a catalyst for producing propane, the catalyst takes one or more of HZSM-5 molecular sieve, HY type molecular sieve, beta molecular sieve, mordenite and SAPO-34 molecular sieve as active components, and takes one or more of rare earth metal, Zn, Ga, Ni, Ag, Mo, Cu, P and the like as modification elements, so that the activity and selectivity of the catalyst for producing propane are improved, and meanwhile, the selectivity and thermal stability of the catalyst are further improved through high-temperature steam treatment, the service life of the catalyst is prolonged, and the economy of the device is improved.
In order to achieve the above purpose of the invention, the following technical scheme is adopted:
a catalyst for producing propane by converting light hydrocarbon is prepared by adding binder into active component of molecular sieve, kneading, extruding, drying and roasting; then, one or more of Zn, Ga, Ni, Ag, Mo, Cu and P are used as modification elements to modify the elements, and then the elements are dried and roasted; finally, carrying out aging treatment by using water vapor to obtain the catalyst for producing propane by converting light hydrocarbon.
The catalyst comprises the following components: HZSM-5 molecular sieve, SiO thereof2/Al2O3The molar ratio is 10-300, and the mass percentage content is 45-75%; modified Y-type molecular sieve made of SiO2/Al2O3The HY molecular sieve with the molar ratio of 2-10 is obtained by modifying with rare earth metal, the mass percentage content of the HY molecular sieve is 0.01-30%, and the rare earth content of the HY molecular sieve is 0.01-20%; at least one of beta molecular sieve, mordenite and SAPO-34 molecular sieve, the mass percentage of which is 0.01-5%, preferably beta molecular sieve; 0.01-10% of modified metal by mass; the balance of the binder.
The rare earth metal is at least one of La, Ce, Pr and Nd, preferably La and Ce.
The modified metal is at least one of Zn, Ga, Ni, Ag, Mo, Cu and P, and Zn is preferred.
The binder is at least one of aluminum sol, silica sol, SB powder and pseudo-boehmite, preferably pseudo-boehmite and SB powder.
The invention also aims to provide a preparation method of the catalyst, which specifically comprises the following steps:
(1) adding a certain amount of HY molecular sieve into a pressure-resistant container which has a stirring function and is filled with a rare earth metal compound solution, controlling the pressure in the container to be 0.01-2.0 MPa and the temperature to be 40-100 ℃, carrying out pressure relief and suction filtration after 2-5 h of treatment, drying at 100-120 ℃ for 2h, and roasting at 400-600 ℃ for 4h to obtain a modified Y molecular sieve;
(2) uniformly mixing a certain amount of HZSM-5 molecular sieve with at least one of modified Y-type molecular sieve and beta molecular sieve, mordenite and SAPO-34 molecular sieve, adding a binder and water, fully and uniformly stirring, and extruding to form strips;
(3) drying the wet strips prepared in the step (2) at 110-120 ℃ for 2-10 h, and then roasting at 500-750 ℃ for 2-12 h;
(4) performing impregnation modification on the catalyst prepared in the step (3), wherein the modified metal can be at least one of Zn, Ga, Ni, Ag, Mo, Cu and P, and Zn is preferred;
(5) drying the wet strips dipped in the step (4) at 110-120 ℃ for 2-8 h, and then roasting at 500-750 ℃ for 2-12 h to obtain a modified catalyst;
(6) and (3) loading the modified catalyst obtained in the step (5) into a reactor, and carrying out hydrothermal aging treatment for 0.1-20 h under the conditions of normal pressure, 400-800 ℃ and 100% of steam to obtain the catalyst for producing propane by converting light hydrocarbon.
In the steps (3) and (5), the drying method is preferably an oven, and the baking method is preferably a muffle furnace.
The invention also aims to use the catalyst prepared by the method in the process for producing propane by converting light hydrocarbon (such as liquefied gas, C5C6 alkane and light naphtha) to obtainTo a higher propane yield. The specific process steps are as follows: putting a certain amount of the catalyst prepared in the step (6) into a fixed bed reactor, and reacting at the temperature of 320-450 ℃, the reaction pressure of 0.1-3.0 MPa and the space velocity of 0.1-2.0 h-1Under the condition of (1), light hydrocarbon is introduced for reaction, so that a better propane yield can be obtained.
Compared with the prior art, the invention has the following beneficial effects:
(1) the HZSM-5 molecular sieve and the modified Y-type molecular sieve are mixed with at least one of the beta molecular sieve, the mordenite and the SAPO-34 molecular sieve to prepare the composite carrier, the active sites of the three carriers are reasonably utilized, and the modified Y-type molecular sieve improves the cracking performance and the water-resistant heat treatment capability of light hydrocarbon, thereby improving the high conversion rate and the stability of the catalyst; the HZSM-5 molecular sieve fully utilizes the advantages of the pore channels, and improves the secondary cracking of the primary cracking product and the polymeric hydrocarbon, thereby further effectively improving the one-way conversion rate and the propane selectivity of the raw materials; the doped small amount of beta molecular sieve, mordenite and SAPO-34 molecular sieve can effectively promote the cracking of light hydrocarbon, and the single-pass conversion rate and the octane number of gasoline are improved;
(2) the activity and the selectivity of the catalyst are further effectively improved through metal modification treatment, and the yield of the target product propane is improved;
(3) through high-temperature hydrothermal aging treatment, the optimal acid amount and acid strength on the composite carrier are obtained, the anti-coking capability and stability of the catalyst can be effectively improved, and the propane selectivity of the catalyst is further improved.
The foregoing is a summary of the present invention, and the following detailed description is of preferred embodiments in order to provide a clear understanding of the technical means of the present invention.
Detailed Description
The technical scheme of the invention is further explained by combining specific examples.
Example 1
1000g of HY molecular sieve with the molar ratio of silicon to aluminum of 4.2 is taken and added into a pressure-resistant container with a stirring function and a rare earth metal compound solution, and the modified solution is a solution containing 100g of mixed rare earth halides (containing 20 percent of lanthanum oxide and 13 percent of cerium oxide). Stirring continuously at the temperature of 60 ℃ under the pressure of 0.5MPa, treating for 4 hours, then releasing pressure, filtering, drying and roasting to obtain the modified Y-type molecular sieve A. The HY type molecular sieve raw powder is obtained from a product of ZiBo Qi Chun chemical technology development company Limited (the same is applied to other embodiments) sold in the market.
Example 2
Weighing 60g of modified Y-type molecular sieve A, 240g of HZSM-5 molecular sieve raw powder with the silica-alumina molar ratio of 60 and 12g of beta molecular sieve, uniformly mixing the three, adding 100g of nitric acid acidified pseudo-boehmite and a proper amount of deionized water, uniformly kneading, extruding into strips, drying at 120 ℃ for 3h, and roasting at 550 ℃ for 5h to prepare the unmodified catalyst B1. 4.55g Zn (NO) are weighed out3)2*6H2O, adding deionized water to prepare a solution, weighing 100g B1, and uniformly soaking Zn (NO)3)2Standing the solution for 2h, drying the solution at 120 ℃ for 4h, roasting the solution at 600 ℃ for 6h to obtain a modified catalyst B2, loading the modified catalyst B2 into a reactor, and carrying out high-temperature steam aging treatment for 2h under the conditions of normal pressure, 500 ℃ and 100% of steam to obtain a catalyst B, wherein the composition of the catalyst B is shown in Table 1. The HZSM-5 molecular sieve and the beta molecular sieve are both obtained from a commercial product of Ziboziqi chemical engineering and technology development company Limited (the same is carried out in other examples).
Example 3
300g of HZSM-5 molecular sieve raw powder with the silica-alumina molar ratio of 60 and 12g of beta molecular sieve are weighed, are uniformly mixed, then 100g of pseudo-boehmite acidified by nitric acid and a proper amount of deionized water are added to be uniformly kneaded and extruded into strips, the strips are dried for 3h at the temperature of 120 ℃, and are roasted for 5h at the temperature of 550 ℃, thus preparing the unmodified catalyst C1. 4.55g Zn (NO) are weighed out3)2*6H2O, adding deionized water to prepare a solution, weighing 100g C1, and uniformly soaking Zn (NO)3)2Standing in the solution for 2h, oven drying at 120 deg.C for 4h, calcining at 600 deg.C for 6h to obtain modified catalyst C2, loading the modified catalyst C2 into a reactor, and reacting at 500 deg.C under normal pressure with 100% water vaporHigh temperature steam aging for 2 hours gave catalyst C, the composition of which is shown in Table 1.
Example 4
Weighing 300g of modified Y-type molecular sieve A and 12g of beta molecular sieve, uniformly mixing the two, adding 100g of nitric acid acidified pseudo-boehmite and a proper amount of deionized water, kneading uniformly, extruding into strips, drying at 120 ℃ for 3h, and roasting at 550 ℃ for 5h to prepare the unmodified catalyst D1. 4.55g Zn (NO) are weighed out3)2*6H2O, adding deionized water to prepare a solution, weighing 100g D1, and uniformly soaking Zn (NO)3)2Standing the solution for 2h, drying the solution at 120 ℃ for 4h, roasting the solution at 600 ℃ for 6h to obtain a modified catalyst D2, loading the modified catalyst D2 into a reactor, and carrying out high-temperature steam aging treatment for 2h under the conditions of 500 ℃, normal pressure and 100% of steam to obtain a catalyst D, wherein the composition of the catalyst D is shown in Table 1.
Example 5
Weighing 120g of modified Y-type molecular sieve A, 180g of HZSM-5 molecular sieve raw powder with the silicon-aluminum molar ratio of 60 and 8g of beta molecular sieve, uniformly mixing the modified Y-type molecular sieve A, the modified Y-type molecular sieve raw powder, the modified Y-type molecular sieve raw powder, and the modified Y-type molecular sieve beta molecular sieve raw powder, the modified Y-type molecular sieve raw powder, and the modified Y-type molecular sieve beta molecular sieve raw powder, wherein the modified Y-type molecular sieve raw powder, 120 g-type molecular sieve, and the modified Y-type molecular sieve, wherein the modified Y-type molecular sieve are uniformly mixing, 120g, 180g, 0, 180, 0, 100g, 0, 180, 0, and 0, respectively. 9.1g of Zn (NO) are weighed out3)2*6H2O, adding deionized water to prepare a solution, weighing 100g E1, and uniformly soaking Zn (NO)3)2Standing the solution for 2h, drying the solution at 120 ℃ for 4h, roasting the solution at 600 ℃ for 6h to obtain a modified catalyst E2, loading the modified catalyst E2 into a reactor, and carrying out high-temperature steam aging treatment for 2h under the conditions of 500 ℃, normal pressure and 100% of steam to obtain a catalyst E, wherein the composition of the catalyst E is shown in Table 1.
Example 6
Weighing 10g of modified Y-type molecular sieve A, 300g of HZSM-5 molecular sieve raw powder with the silica-alumina molar ratio of 60 and 4g of beta molecular sieve, uniformly mixing the modified Y-type molecular sieve A, the modified Y-type molecular sieve raw powder, the HZSM-5 molecular sieve raw powder and the beta molecular sieve, adding 90.5g of nitric acid acidified pseudo-boehmite and a proper amount of deionized water, uniformly kneading, extruding into strips, drying at 120 ℃ for 3h, roasting at 550 ℃ for 5h, and preparing the unmodified catalyst F1. 11.4g Zn (NO) are weighed out3)2*6H2O, addAdding deionized water to prepare solution, weighing 100g F1, and soaking in Zn (NO)3)2Standing the solution for 2h, drying the solution at 120 ℃ for 4h, roasting the solution at 600 ℃ for 6h to obtain a modified catalyst F2, loading the modified catalyst F2 into a reactor, and carrying out high-temperature steam aging treatment for 2h under the conditions of 500 ℃, normal pressure and 100% of steam to obtain a catalyst F, wherein the composition of the catalyst F is shown in Table 1.
Example 7
Weighing 60G of modified Y-type molecular sieve A, 240G of HZSM-5 molecular sieve raw powder with the silica-alumina molar ratio of 60 and 12G of SAPO-34 molecular sieve, uniformly mixing the three, adding 100G of nitric acid acidified pseudo-boehmite and a proper amount of deionized water, uniformly kneading, extruding into strips, drying at 120 ℃ for 3h, and roasting at 550 ℃ for 5h to prepare the unmodified catalyst G1. 4.55g Zn (NO) are weighed out3)2*6H2O, adding deionized water to prepare a solution, weighing 100g of G1, and uniformly soaking Zn (NO) in the solution3)2Standing the solution for 2h, drying the solution at 120 ℃ for 4h, roasting the solution at 600 ℃ for 6h to obtain a modified catalyst G2, loading the modified catalyst G2 into a reactor, and carrying out high-temperature steam aging treatment for 2h under the conditions of 500 ℃, normal pressure and 100% of steam to obtain a catalyst G, wherein the composition of the catalyst G is shown in Table 1.
Comparative example 1
Adding 200g of a commercially available HY molecular sieve with the molar ratio of silicon to aluminum of 4.2 into a pressure-resistant container with a stirrer and a rare earth metal compound solution, wherein the modified solution is a solution containing 20g of mixed rare earth halide (containing 20% of lanthanum oxide and 13% of cerium oxide); continuously stirring under the pressure of 0.5Mpa and the temperature of 60 ℃, treating for 4 hours, then releasing pressure, filtering, drying and roasting to obtain the modified Y-type molecular sieve S1. Weighing 180g of modified Y-type molecular sieve S1, 120g of HZSM-5 molecular sieve raw powder with the silica-alumina molar ratio of 60 and 12g of beta molecular sieve, uniformly mixing the modified Y-type molecular sieve S1, the modified Y-type molecular sieve raw powder, the HZSM-5 molecular sieve raw powder with the silica-alumina molar ratio of 60 and the beta molecular sieve, adding 100g of nitric acid acidified pseudo-boehmite and a proper amount of deionized water, uniformly kneading, extruding into strips, drying at 120 ℃ for 2h, roasting at 550 ℃ for 5h, and preparing the unmodified catalyst S2. 4.55g Zn (NO) are weighed out3)2*6H2O, adding deionized water to prepare a solution, weighing 100g S2, and uniformly soaking Zn (NO)3)2Standing the solution for 2h, drying the solution at 120 ℃ for 4h, roasting the solution at 600 ℃ for 6h to obtain a modified catalyst S3, loading the modified catalyst S3 into a reactor, and carrying out high-temperature steam aging treatment for 2h under the conditions of 500 ℃, normal pressure and 100% of steam to obtain a catalyst S, wherein the composition of the catalyst S is shown in Table 1.
TABLE 1 catalyst sample composition
Example 8
The above catalyst B was charged into a laboratory 10ml adiabatic fixed bed reactor and the reaction product was analyzed by on-line chromatography. The composition of the mixed butane feed is shown in table 2. The experimental conditions and the experimental results are shown in table 3.
TABLE 2 composition of mixed butane feed
| Name of material | Mass fraction of% |
| Less than or equal to carbon four | 0.07 |
| N-butane | 52.74 |
| Isobutane | 45.21 |
| Others | 1.98 |
TABLE 3 reactivity of catalyst B prepared under different reaction conditions
Example 9
The above catalyst B, C, D, E, F, G, S was charged to a laboratory 10ml adiabatic fixed bed reactor and the reaction product was analyzed by on-line chromatography. The composition of the mixed butane feed is shown in table 2. The experimental conditions are as follows: the reaction temperature is 320 ℃, and the mass space velocity of the raw materials is 0.5h-1The reaction pressure was 0.5 MPa. The results of the butane conversion to propane are shown in Table 4.
TABLE 4 butane cleavage product composition
Example 10
The above catalyst B, C, D, E, F, G, S was charged to a laboratory 10ml adiabatic fixed bed reactor and the reaction product was analyzed by on-line chromatography. The C5C6 light oil composition is shown in table 5. The experimental conditions are as follows: the reaction temperature is 340 ℃, and the mass space velocity of the raw material is 0.5h-1The reaction pressure was 0.5 MPa. The results of the experiments on the conversion of light C5C6 oil to produce propane are shown in Table 6.
TABLE 5C 5C6 light oil composition
| Name of material | Mass fraction of% |
| ≤C4 | 0.07 |
| N-pentane | 35.03 |
| Isopentane | 26.35 |
| N-hexane | 18.17 |
| Isohexane | 7.63 |
| Benzene and its derivatives | 6.74 |
| Others | 6.01 |
TABLE 6 distribution of light oil C5C6 light oil conversion products
Example 11
The above catalyst B, C, D, E, F, G, S was charged to a laboratory 10ml adiabatic fixed bed reactor and the reaction product was analyzed by on-line chromatography. The naphtha feed composition is shown in table 7. The experimental conditions are as follows: the reaction temperature is 360 ℃, and the mass space velocity of the raw material is 0.5h-1The reaction pressure was 0.5 MPa. The results of the naphtha conversion to propane are shown in Table 8.
TABLE 7 naphtha composition
| Name of material | Mass fraction of% |
| ≤C4 | 3.24 |
| C5 component | 7.63 |
| C6 component | 33.09 |
| C7 component | 27.56 |
| C8 component | 13.06 |
| ≥C9 | 15.42 |
TABLE 8 naphtha conversion distribution Table
It should be noted that the above-mentioned embodiments are only preferred embodiments of the present invention, and any person skilled in the art can make any equivalent modifications and modifications to the above-mentioned embodiments without departing from the scope of the present invention.
Claims (7)
1. A catalyst for producing propane by converting light hydrocarbon is characterized by comprising the following components: the HZSM-5 molecular sieve is 45-75% in mass percentage; the modified Y-type molecular sieve is obtained by modifying an HY-type molecular sieve by using rare earth metal, and the mass percentage content of the modified Y-type molecular sieve is 0.01-30%, and the rare earth content of the modified Y-type molecular sieve is 0.01-20%; at least one of beta molecular sieve, mordenite and SAPO-34 molecular sieve, wherein the mass percentage content is 0.01-5%; at least one of Zn, Ga, Ni, Ag, Mo, Cu and P is used as a modifying element, and the mass percentage content is 0.01-10%; the balance of the binder.
2. The catalyst for producing propane by conversion of light hydrocarbons as claimed in claim 1, wherein the HZSM-5 molecular sieve is SiO2/Al2O3The molar ratio is 10-300.
3. The catalyst for producing propane by conversion of light hydrocarbons as claimed in claim 1, wherein the molecular sieve HY type is SiO2/Al2O3The molar ratio is 2-10.
4. The catalyst for producing propane by light hydrocarbon conversion as claimed in claim 1, wherein the rare earth metal is at least one of La, Ce, Pr and Nd.
5. The catalyst for producing propane by light hydrocarbon conversion as claimed in claim 1, wherein the binder is at least one of alumina sol, silica sol, SB powder and pseudo-boehmite.
6. A method for preparing the catalyst of claim 1, comprising the steps of:
(1) adding a certain amount of HY molecular sieve into a pressure-resistant container which has a stirring function and is filled with a rare earth metal compound solution, controlling the pressure in the container to be 0.01-2.0 MPa and the temperature to be 40-100 ℃, carrying out pressure relief and suction filtration after 2-5 h of treatment, drying at 100-120 ℃ for 2h, and roasting at 400-600 ℃ for 4h to obtain a modified Y molecular sieve;
(2) uniformly mixing a certain amount of HZSM-5 molecular sieve with at least one of modified Y-type molecular sieve and beta molecular sieve, mordenite and SAPO-34 molecular sieve, adding a binder and water, fully and uniformly stirring, and extruding to form strips;
(3) drying the wet strips prepared in the step (2) at 110-120 ℃ for 2-10 h, and then roasting at 500-750 ℃ for 2-12 h;
(4) carrying out impregnation modification on the catalyst prepared in the step (3) by adopting at least one of Zn, Ga, Ni, Ag, Mo, Cu and P as a modification element;
(5) drying the wet strips dipped in the step (4) at 110-120 ℃ for 2-8 h, and then roasting at 500-750 ℃ for 2-12 h to obtain a modified catalyst;
(6) and (3) loading the modified catalyst obtained in the step (5) into a reactor, and carrying out hydrothermal aging treatment for 0.1-20 h under the conditions of normal pressure, 400-800 ℃ and 100% of steam to obtain the catalyst for producing propane by converting light hydrocarbon.
7. The application of the catalyst prepared in the claim 6 in the process of producing propane by converting light hydrocarbon is characterized by comprising the following specific steps: a certain amount of the catalyst prepared in the claim 6 is loaded into a fixed bed reactor, and the reaction temperature is 320-450 ℃, the reaction pressure is 0.1-3.0 MPa, and the space velocity is 0.1-2.0 h-1Introducing light hydrocarbon to react under the condition (1).
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