WO2004065005A1 - Catalyseur pour le craquage catalytique d'hydrocarbures et procede de production d'olefines legeres au moyen de ce catalyseur - Google Patents

Catalyseur pour le craquage catalytique d'hydrocarbures et procede de production d'olefines legeres au moyen de ce catalyseur Download PDF

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Publication number
WO2004065005A1
WO2004065005A1 PCT/JP2004/000428 JP2004000428W WO2004065005A1 WO 2004065005 A1 WO2004065005 A1 WO 2004065005A1 JP 2004000428 W JP2004000428 W JP 2004000428W WO 2004065005 A1 WO2004065005 A1 WO 2004065005A1
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Prior art keywords
catalyst
zeolite
mass
catalytic cracking
type
Prior art date
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PCT/JP2004/000428
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English (en)
Japanese (ja)
Inventor
Kenichi Wakui
Kinsho Furusawa
Fumitaka Honjo
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Idemitsu Kosan Co., Ltd.
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Application filed by Idemitsu Kosan Co., Ltd. filed Critical Idemitsu Kosan Co., Ltd.
Publication of WO2004065005A1 publication Critical patent/WO2004065005A1/fr

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J29/00—Catalysts comprising molecular sieves
    • B01J29/04—Catalysts comprising molecular sieves having base-exchange properties, e.g. crystalline zeolites
    • B01J29/06—Crystalline aluminosilicate zeolites; Isomorphous compounds thereof
    • B01J29/80—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
    • B01J2229/00—Aspects of molecular sieve catalysts not covered by B01J29/00
    • B01J2229/30—After treatment, characterised by the means used
    • B01J2229/42—Addition of matrix or binder particles
    • 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
    • B01J29/084—Y-type faujasite
    • 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
    • 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
    • C10G2400/20—C2-C4 olefins

Definitions

  • the present invention relates to a catalytic cracking catalyst for hydrocarbons, and a method for producing light olefins using the catalyst.
  • the present invention relates to a catalyst capable of producing light olefins such as ethylene and propylene in a high yield by catalytically cracking hydrocarbons, and to catalytically crack hydrocarbons using the catalyst. And a method for producing light olefins such as ethylene and propylene in a high yield.
  • Light olefins such as ethylene and propylene are extremely important compounds as basic raw materials for various chemical products.
  • gaseous hydrocarbons such as ethane, propane, and butane
  • liquid hydrocarbons such as naphtha
  • the reaction temperature is relatively low at about 500 to 700 ° C. Since a high ethylene and propylene yield (each about 10 to 30 mass./. Relative to the raw material hydrocarbons) can be obtained, many techniques using the catalyst have been proposed.
  • a catalytic cracking method using a ZSM-5 type catalyst having a specific acid amount and acid strength see, for example, Japanese Patent Application Laid-Open No. 3-5047337, Japanese Patent Application Laid-Open No. 6-346062), ⁇ , Catalytic cracking method using ZSM-5 type catalyst containing transition metal such as cobalt (see, for example, JP-A-2-1113 and JP-A-2-184638), rare earth elements
  • Catalytic cracking method using ZSM-5 type catalyst containing (RE) for example, US Pat. No. 5,232,675, US Pat. No. 5,380,6.90, European Patent No. 727, 40'4, Japanese Patent Application Laid-Open No. 11-180902, and Japanese Patent Application Laid-Open No. 11-253807) are disclosed.
  • pentasil-type zeolites such as ZSM-5 have relatively small pore diameters of about 0.5 to 0.6 nm, so raw materials with a large molecular weight or with many branches cannot enter the pores. Therefore, heavy raw materials have the disadvantage of being difficult to decompose.
  • zeolite having a relatively large pore diameter (pore diameter of about 0.7 nm or more) represented by Y-type zeolite (FAU-type zeolite) has the above-mentioned raw materials having a large molecular weight, Because it can crack even highly branched feeds, it has been widely used as a catalyst in fluidized bed catalytic cracking reactors, mainly for gasoline production.
  • a hydrocarbon material with a nitrogen content of 100 mass ppm or less and an initial boiling point of 230 ° C or more is converted to a zeolite catalyst containing both Y-type and ZSM-5 type components.
  • a method of catalytic decomposition is disclosed (for example, see Japanese Patent Application Laid-Open No. 6-220466).
  • a catalytic cracking method using zeolite and a catalyst in which 75 to 100% by mass is a pentasil-type phosphorus-containing zeolite is disclosed (for example, Japanese Patent Application Laid-Open No. H11-191924). Gazette).
  • Zeolite catalysts promote permanent deterioration due to dealumination at high temperatures, and such high temperatures cause catalyst deterioration. Therefore, catalysts that exhibit high activity at lower temperatures are required.
  • the present invention provides a catalyst capable of catalytically decomposing hydrocarbons at a relatively low temperature under such circumstances to produce light olefins in a high yield, and a method for contacting hydrocarbons using the catalyst. It is an object of the present invention to provide a method for decomposing and producing light-olefins. Disclosure of the invention
  • the present inventors have conducted intensive studies to achieve the above object, and as a result, contain zeolite and a clay mineral and / or inorganic oxide other than zeolite at a specific ratio, and as the zeolite component It has been found that a catalyst using a pentasil-type zeolite carrying a rare earth element as an oxide at a specific ratio and a Y-type zeolite in a predetermined ratio can achieve the object. did.
  • the present invention has been completed based on such findings.
  • a catalyst comprising 5 to 90% by mass of zeolite and 10 to 95% by mass of a clay mineral and / or inorganic oxide other than zeolite, wherein 30 to 90% by mass of the zeolite component 9 5 mass% in the pentasil type Zeorai bets carrying as oxides of rare earth elements, 5-7 0 weight 0 /. Is a Y-type zeolite (FAU type), and the amount of the rare earth element carried in the pentasil-type zeolite is in the range of 0.4 to 20 in terms of atomic ratio to aluminum in the pentasil-type zeolite.
  • a catalyst for catalytic cracking of hydrocarbons
  • the catalyst for catalytic cracking of hydrocarbons of the present invention is a catalyst comprising (A) zeolite and (B) a clay mineral and / or inorganic oxide other than zeolite.
  • the hydrocarbons to which this catalyst is applied include paraffins having 2 or more carbon atoms, preferably 2 to 30 carbon atoms, more preferably 2 to 20 carbon atoms, or paraffins thereof. Examples of carbon carbides containing fin as a main component (about 10% by mass or more) can be given.
  • hydrocarbons for example, paraffins such as ethane, propane, butane, pentane and hexane, and light hydrocarbon fractions such as naphtha and gas oil are used.
  • the catalyst of the present invention has a characteristic of exhibiting a high activity even for hydrocarbons having a relatively high boiling point and a high molecular weight, and the hydrocarbons used as a raw material to which the catalyst is applied are saturated. It is not limited to a hydrocarbon compound, and a compound containing a hydrocarbon compound having an unsaturated bond can also be used.
  • the zeolite of the component (A) in the catalyst of the present invention comprises (a) a pentasil type zeolite in which a rare earth element is supported as an oxide, and (b) a Y type zeolite.
  • the rare earth element in the pentasil-type zeolite of the component (a) is not particularly limited, and any of them can be used.
  • any of them can be used.
  • One of these rare earth elements may be supported alone as an oxide, or two or more may be supported in combination.
  • the method for supporting the rare earth element on the pentasil-type zeolite is not particularly limited, and may be appropriately selected from conventionally known methods. For example, using salts such as acetates, nitrates, halides, sulfates, and carbonates, or alkoxides, acetyl acetatetonate, etc., by ion exchange, impregnation, hydrothermal synthesis, or other methods, Rare earth elements are supported as oxides on pentasil-type zeolite.
  • the pentasil-type zeolite in which the rare earth element is supported as an oxide has an effect of suppressing a hydrogen transfer reaction that causes the generation of by-products, and The yield of quality olefins can be improved.
  • the oxide of the rare earth element needs to be supported on the pentasil-type zeolite, and the effect of the catalyst of the present invention can be obtained only by physically mixing the oxide with the pentasil-type zeolite together with the binder. I can't get it.
  • S i 0 2 / A 1 2 Rei_3 (molar ratio) is rather preferably be in the range of 2 5-8 00, more preferably 3 0-6 00, further c also preferably a 40-3 0 0, the amount of rare earth element supported on the pentasil type zeolite DOO, compared aluminum in the pentasil-type zeolite preparative, atomic ratio It is selected in the range of 0.4 to 20.
  • the atomic ratio is less than 0.4, the production of heavy coke and aromatic components as by-products increases, and if it exceeds 20, the catalytic activity decreases, and the yield of light olefins decreases. .
  • a preferable range of the atomic ratio is 0.6 to 5, and a range of 1 to 3 is particularly preferable.
  • Examples of the pentasil-type zeolite used for the component (a) include ZSM-15, ZSM_8, and ZSM-11 type.
  • the Y-type zeolite of the component (b) is not particularly limited, and any type can be used.
  • USY type, RE-USY, REY, and the like are preferable.
  • the zeolite of the component (A) includes (a) a pentasil-type zeolite that supports a rare earth element as a component as an oxide,
  • component (b) in Y-type zeolite is as follows: (a) component is 30 to 95 mass%. / 0 , the component (b) is 5 to 70% by mass.
  • the content of the component is 30% by mass. /. If it is less than 30, the amount of light olefins formed will be small, and the above-mentioned 95 mass is required. If it exceeds / 0 , the decomposition rate will decrease.
  • the preferred content of the component (a) is 40 to 85% by mass, and the content of the component (b) is 15 to 6 ° by mass. /. The more preferred content of the component (a) is 50 to 75 mass. /.
  • In the content of component (b) is a 2 5-5 0 weight 0/0.
  • a clay mineral other than zeolite may be used, only an inorganic oxide may be used, or a clay mineral and an inorganic oxide may be used in combination.
  • examples of the clay mineral include kaolin, bentonite, smectite, and the like
  • examples of the inorganic oxide include alumina, silica, and siliceous alumina.
  • the content of the component (A) zeolite is 5 to 90% by mass. It is selected in the range.
  • the content is less than the above 5% by mass, the catalytic activity is too low to lower the yield of light olefins, and if it exceeds the above 90% by mass, the fluidity of the catalyst particles deteriorates when used in a fluidized bed. .
  • the preferred content of the component (A) is 5 to 50% by mass, and particularly preferably 10 to 40% by mass.
  • the catalyst of the present invention comprises, for example, a pentasil-type zeolite and a Y-type zeolite each carrying a predetermined amount of a rare earth element as an oxide together with a clay mineral and Z or an inorganic oxide or a precursor thereof at a predetermined ratio. , And dried by spray drying or the like to form particles.
  • light olefins are produced by catalytically cracking the hydrocarbons having 2 or more carbon atoms in the presence of the catalyst thus obtained.
  • the light-olefins include ethylene and propylene.
  • the type of catalytic cracking reaction in this method For example, using a fixed bed, moving bed, fluidized bed, or other type of reactor, hydrocarbons are supplied to the catalyst bed packed with the aforementioned catalyst. As a result, a catalytic cracking reaction is performed.
  • a catalytic cracking reaction using a continuously regenerating fluidized bed or a moving bed is preferred.
  • the raw material hydrocarbons can be diluted with nitrogen, hydrogen, helium, or water vapor as necessary.
  • the reaction temperature of the catalytic cracking is usually selected in the range of 350 to 780 ° C, preferably 500 to 750 ° C, more preferably 600 to 700 ° C.
  • reaction temperature is lower than 350 ° C., sufficient catalytic activity is hardly obtained, and the yield of light olefins per pass is low, which is not practical. weight, the c-reactive pressure there is a risk that by-product amount of methane and coke is rapidly increased normal pressure, can be carried either vacuum or pressure, usually atmospheric pressure of doctor and pressure conditions are employed.
  • hydrocarbons can be efficiently decomposed at a relatively low temperature as compared with the conventional method, and light olefins such as ethylene and propylene can be obtained at a high yield. Can be manufactured at a rate.
  • the atomic ratio of La to aluminum in ZSM-5 zeolite was 1.1.
  • the catalyst A was treated with 100% steam at 800 ° C. for 6 hours to be pseudo equilibrated.
  • Aromatic compound 2% by mass
  • catalyst B Without using USY Zeorai bets, 1 0% L Azz SM- 5 to 20 weight 0/0, kaolin 5 0 wt%, the silica-alumina 5 weight 0 /.
  • a catalyst (hereinafter, referred to as catalyst B) was prepared in the same manner as in Example 1, except that the catalyst was prepared using 20% by mass of alumina sol and 5% by mass of silicic acid sol.
  • catalyst C A catalyst (hereinafter, referred to as catalyst C) was prepared in the same manner as in Example 1 except that the mass% and the silica sol were changed to 5 mass%.
  • the catalyst C was treated with 100% steam at 800 ° C. for 6 hours to simulate equilibrium.
  • catalyst D Without using a silica-alumina, 1 0% L a / Z SM- 5 to 20 weight 0/0, USY Zeorai Doo (HS Z- 3 3 0 HUA) 5 mass 0/0, kaolin 4 0 mass%, A catalyst (hereinafter, referred to as catalyst D) was prepared in the same manner as in Example 1 except that the amount of alumina sol was 30% by mass and the amount of silica sol was 5% by mass.
  • the catalyst D was treated with 800% steam at 800 ° C. for 6 hours to make it pseudo-equilibrate.
  • Table 1 shows the results.
  • Example 1 As can be seen from the comparison between Example 1 and Comparative Example 1 and between Examples 2 to 4 and Comparative Example 2, when a catalyst containing no Y-type zeolite was used, a product with a fraction of 5 or more was produced. Many, low yield of light ethylenes and propylene.
  • a catalyst capable of catalytically cracking hydrocarbons at a relatively low temperature to produce light olefins such as ethylene and propylene in a high yield, and It is possible to provide a method for producing hydrocarbons such as ethylene and propylene in high yield by catalytically cracking hydrocarbons using the above catalyst.

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  • Chemical & Material Sciences (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Catalysts (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)

Abstract

L'invention concerne un catalyseur pour le craquage catalytique d'hydrocarbures, lequel comprend de 5 à 90 % en poids de zéolites et de 10 à 95 % en poids de minéraux argileux autres que des zéolites et/ou de l'oxyde inorganique, 30 à 95 % en poids de l'ingrédient zéolite étant un zéolite pentasil possédant un élément de terre rare déposé sous forme d'oxyde, alors que 5 à 70 % en poids de cet ingrédient zéolite est un zéolite Y (de type FAU), la quantité d'élément de terre rare déposé dans le zéolite pentasil étant comprise entre 0,4 et 20 en terme de rapport atomique entre ce zéolite et de l'aluminium contenu dans le zéolite pentasil. L'invention concerne également un procédé de production d'oléfines légères, qui consiste au craquage catalytique de C2 ou d'hydrocarbures plus élevés en présence du catalyseur. A cause de ce catalyseur, des hydrocarbures peuvent être soumis au craquage catalytique à une température relativement basse pour produire des oléfines légères avec un grand rendement.
PCT/JP2004/000428 2003-01-24 2004-01-20 Catalyseur pour le craquage catalytique d'hydrocarbures et procede de production d'olefines legeres au moyen de ce catalyseur WO2004065005A1 (fr)

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JP2003016379A JP2004261628A (ja) 2003-01-24 2003-01-24 炭化水素類の接触分解触媒及びそれを用いた軽質オレフィン類の製造方法
JP2003-16379 2003-01-24

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9701914B2 (en) 2006-11-07 2017-07-11 Saudi Arabian Oil Company Advanced control of severe fluid catalytic cracking process for maximizing propylene production from petroleum feedstock
US9764314B2 (en) 2006-11-07 2017-09-19 Saudi Arabian Oil Company Control of fluid catalytic cracking process for minimizing additive usage in the desulfurization of petroleum feedstocks

Families Citing this family (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
AR052122A1 (es) * 2004-11-05 2007-03-07 Grace W R & Co Catalizadores para olefinas livianas y glp gas licuado de petroleo en unidades de craqueo catalitico fluidizado
JP4714589B2 (ja) * 2006-01-20 2011-06-29 石油コンビナート高度統合運営技術研究組合 重質油の接触分解触媒及びオレフィンと燃料油の製造方法
KR101503069B1 (ko) 2008-10-17 2015-03-17 에스케이이노베이션 주식회사 유동층 접촉 분해 공정의 경질 사이클 오일로부터 고부가 방향족 및 올레핀을 제조하는 방법
RU2473385C1 (ru) * 2011-08-25 2013-01-27 Окрытое акционерное общество "Газпромнефть-Омский НПЗ" Микросферический катализатор для крекинга нефтяных фракций и способ его приготовления
JP6074559B2 (ja) * 2012-05-25 2017-02-08 サウジ アラビアン オイル カンパニー 流動接触分解においてプロピレンを増強させるための触媒
JP5904922B2 (ja) * 2012-10-10 2016-04-20 コスモ石油株式会社 炭化水素油の接触分解触媒及び炭化水素油の接触分解方法
JP6329436B2 (ja) * 2014-05-30 2018-05-23 Ｊｘｔｇエネルギー株式会社 重質油の流動接触分解法

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3748251A (en) * 1971-04-20 1973-07-24 Mobil Oil Corp Dual riser fluid catalytic cracking with zsm-5 zeolite
US3758403A (en) * 1970-10-06 1973-09-11 Mobil Oil Olites catalytic cracking of hydrocarbons with mixture of zsm-5 and other ze
EP0727404A1 (fr) * 1993-11-05 1996-08-21 China Petro-Chemical Corporation Procede a rendement eleve de production d'olefines inferieures par conversion catalytique
EP0909582A1 (fr) * 1997-10-15 1999-04-21 China Petro-Chemical Corporation Catalyseur pour le craquage catalytique pour la production d'oléfines légers et sa préparation
JPH11180902A (ja) * 1997-12-16 1999-07-06 Agency Of Ind Science & Technol 低級オレフィンの製造方法

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3758403A (en) * 1970-10-06 1973-09-11 Mobil Oil Olites catalytic cracking of hydrocarbons with mixture of zsm-5 and other ze
US3748251A (en) * 1971-04-20 1973-07-24 Mobil Oil Corp Dual riser fluid catalytic cracking with zsm-5 zeolite
EP0727404A1 (fr) * 1993-11-05 1996-08-21 China Petro-Chemical Corporation Procede a rendement eleve de production d'olefines inferieures par conversion catalytique
EP0909582A1 (fr) * 1997-10-15 1999-04-21 China Petro-Chemical Corporation Catalyseur pour le craquage catalytique pour la production d'oléfines légers et sa préparation
JPH11180902A (ja) * 1997-12-16 1999-07-06 Agency Of Ind Science & Technol 低級オレフィンの製造方法

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9701914B2 (en) 2006-11-07 2017-07-11 Saudi Arabian Oil Company Advanced control of severe fluid catalytic cracking process for maximizing propylene production from petroleum feedstock
US9764314B2 (en) 2006-11-07 2017-09-19 Saudi Arabian Oil Company Control of fluid catalytic cracking process for minimizing additive usage in the desulfurization of petroleum feedstocks

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