WO2008025247A1 - Procédé de récupération de chaleur régénérée pendant la production d'oléfines inférieures à partir de méthanol - Google Patents

Procédé de récupération de chaleur régénérée pendant la production d'oléfines inférieures à partir de méthanol Download PDF

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Publication number
WO2008025247A1
WO2008025247A1 PCT/CN2007/002537 CN2007002537W WO2008025247A1 WO 2008025247 A1 WO2008025247 A1 WO 2008025247A1 CN 2007002537 W CN2007002537 W CN 2007002537W WO 2008025247 A1 WO2008025247 A1 WO 2008025247A1
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WIPO (PCT)
Prior art keywords
reaction
catalyst
methanol
temperature
endothermic
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PCT/CN2007/002537
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English (en)
Chinese (zh)
Inventor
Zhongmin Liu
Yue Qi
Zhihui Lv
Changqing He
Lei Xu
Jinling Zhang
Xiangao Wang
Original Assignee
Dalian Institute Of Chemical Physics, Chinese Academy Of Sciences
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Application filed by Dalian Institute Of Chemical Physics, Chinese Academy Of Sciences filed Critical Dalian Institute Of Chemical Physics, Chinese Academy Of Sciences
Priority to JP2009524885A priority Critical patent/JP2010501495A/ja
Priority to AU2007291786A priority patent/AU2007291786A1/en
Priority to BRPI0715687-1A2A priority patent/BRPI0715687A2/pt
Publication of WO2008025247A1 publication Critical patent/WO2008025247A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C1/00—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon
    • C07C1/20—Preparation of hydrocarbons from one or more compounds, none of them being a hydrocarbon starting from organic compounds containing only oxygen atoms as heteroatoms
    • 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
    • C10G11/14—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts
    • C10G11/18—Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid catalysts according to the "fluidised-bed" technique
    • 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
    • C10G51/00—Treatment of hydrocarbon oils, in the absence of hydrogen, by two or more cracking processes only
    • C10G51/02—Treatment of hydrocarbon oils, in the absence of hydrogen, by two or more cracking processes only plural serial stages only
    • C10G51/04—Treatment of hydrocarbon oils, in the absence of hydrogen, by two or more cracking processes only plural serial stages only including only thermal and catalytic cracking steps
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry
    • Y02P30/20—Technologies relating to oil refining and petrochemical industry using bio-feedstock
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P30/00—Technologies relating to oil refining and petrochemical industry
    • Y02P30/40—Ethylene production

Definitions

  • the present invention relates to a method for recovering heat of regeneration, and more particularly to a method for recovering heat carried by a high-temperature catalyst after regeneration of a methanol to produce a low-carbon olefin.
  • Low-carbon olefins such as ethylene and propylene are the basic raw materials for the chemical industry.
  • the sources of ethylene and propylene have been mainly steam cracking of hydrocarbons.
  • the raw materials used are naphtha, light diesel oil and hydrocracked tail oil.
  • the traditional method for the production of ethylene and propylene mainly uses high-temperature tube furnace cracking process, and the energy consumption is relatively high.
  • the basic principle of the fluidized bed process is that the raw material methanol and the catalyst are mixed in a reactor to be fluidized, and converted to a mixture containing products such as ethylene and propylene at a certain temperature, and the catalyst is partially or completely produced by carbonation after the reaction. Inactivated.
  • the gaseous reaction product flows from the reactor into the separation unit, and the deactivated catalyst continuously flows out of the reactor into the regenerator for regeneration, i.e., combustion in an oxygen-containing atmosphere to remove carbon deposits, and then returned to the reactor for contact with the reaction feed.
  • the surface area carbon of the deactivated catalyst is removed by high temperature combustion.
  • the combustion reaction temperature is higher than 600 ⁇ and up to 700 ° C or higher.
  • the heat generated by the combustion of carbon deposits is transferred out of the regenerator in two ways: The discharged high temperature regenerated flue gas carries away some of the heat, while the other part of the heat is carried away by the regenerated high temperature catalyst.
  • the heat from the high-temperature regenerated flue gas is usually recovered by means of steam production or power generation.
  • US Patent No. 2,050,238, 543 A1 discloses a method for recovering heat from regenerated flue gas, including regenerating flue gas. The heat is cooled by multiple heat exchanges, and the heat taken out is used to generate steam or the like.
  • the heat from the regenerated high-temperature catalyst is often used for reaction heating.
  • fluidized The bed reaction process is generally applied to an endothermic reaction such as catalytic cracking of a hydrocarbon, and a part of the heat of reaction is provided by regenerating a high-temperature catalyst which is regenerated after being regenerated. That is, the deactivated catalyst is combusted in an oxygen-containing atmosphere in the regenerator to remove carbon deposits, regenerated and heated, and then returned to the reactor while transferring heat from the former to the latter to provide at least a portion of the heat of reaction.
  • One object of the present invention is to provide a method for recovering heat of a high temperature catalyst after regeneration in the process of preparing a low carbon olefin from methanol.
  • the present inventors have completed the present invention through intensive research.
  • a method for recovering heat from a regenerated high temperature catalyst in the process of preparing a low carbon olefin from methanol comprising the steps of: first entering a regenerated high temperature catalyst into a cracking reaction endothermic zone And then enter the methanol conversion reactor, where
  • the temperature of the regenerated high temperature catalyst is from 500 to 800 °C.
  • the catalyst having a microporous pore size of 0. 3- 0. 6nm.
  • the matrix material of the catalyst is one or more of silica, alumina or clay.
  • the temperature of the endothermic zone of the cracking reaction is from 400 to 700 °C.
  • the temperature difference between the inlet and the outlet of the catalyst in the endothermic zone of the cracking reaction is from 50 to 300 Torr.
  • a hydrocarbon cracking reaction zone forming the olefin introduced into the endothermic reaction of the above C 4 product is methanol, and / or other C 4 -C 2.
  • the hydrocarbons introduced in the endothermic zone of the cracking reaction are naphtha, gasoline, condensate, light diesel oil, hydrogenated tail oil or/and kerosene.
  • the product produced by the hydrocarbon in the endothermic zone of the cracking reaction is combined into the product obtained from the methanol to the lower olefin.
  • the endothermic zone of the cracking reaction is a separate reaction zone in the methanol conversion zone.
  • the cleavage reaction endothermic zone is a literate section of a methanol conversion reactor.
  • the method for recovering heat of regeneration in the process of preparing low-carbon olefin from methanol is provided by flowing the regenerated high-temperature catalyst into a cracking reaction endothermic zone, and the hydrocarbon catalytic cracking reaction is carried out in the endothermic zone.
  • the heat carried by the catalyst is absorbed, and the temperature of the catalyst is lowered to enter the methanol conversion reactor.
  • the catalyst is a silica-alumina or / and phosphosilicate molecular sieve catalyst, and their elemental modified product, having a micropore diameter of 0. 3-0. 6nm.
  • the matrix material of the catalyst is one or more of silica, alumina or clay.
  • the temperature of the endothermic zone of the cleavage reaction is from 400 to 700 °C.
  • the temperature difference between the inlet and the outlet of the catalyst in the endothermic zone of the cracking reaction is 50-300. C.
  • the hydrocarbons introduced into the endothermic zone of the cracking reaction are methanol to form a product of C4 or higher in the olefin reaction, or / and other C4-C20 hydrocarbons.
  • the hydrocarbons introduced into the endothermic zone of the cracking reaction are naphtha, gasoline, condensate, light diesel oil, hydrogenated tail oil or/and kerosene.
  • part of the heat of regeneration in the process of recovering methanol to produce low carbon olefins can be recovered by an endothermic hydrocarbon cracking reaction.
  • the invention is characterized in that, for the process of preparing a low-carbon olefin from methanol in a reaction-regeneration fluidized bed process with continuous reaction characteristics, the regenerated high-temperature catalyst enters a cracking reaction endothermic zone before contacting with methanol, in which the endothermic C 4 -C 2 is introduced in the area .
  • Hydrocarbons are contacted with a high temperature catalyst after regeneration, utilizing hydrocarbon cracking reaction absorption catalysis
  • the heat carried by the agent after the temperature of the catalyst drops to the temperature required for methanol conversion, enters the methanol conversion reactor.
  • the low carbon olefin produced by the cracking reaction can be added to the methanol-derived olefin product.
  • the present invention provides the following method for recovering partially recovered heat in the process of recovering methanol to produce low carbon olefins: In the process of preparing low carbon olefins by using a fluidized bed process methanol, the methanol raw materials and the catalyst are mixed in a reactor to be fluidized.
  • the catalyst is partially or completely deactivated by carbon deposition after reaction; the gaseous reaction product flows out of the reactor into the separation device, and the deactivated catalyst continuously
  • the reactor flows out into the regenerator for regeneration; the deactivated catalyst is passed through a stripper before entering the regenerator, and the residual hydrocarbons on the catalyst are removed by an inert gas such as water vapor, and then burned in an oxygen-containing atmosphere in the regenerator.
  • the separate dense phase reaction section can also be used to transport the catalyst to the upgrading section of the methanol conversion reactor. In the endothermic region of the reaction, the hydrocarbon feedstock is contacted with the regenerated catalyst, and the heat carried by the crack absorption catalyst occurs.
  • the temperature of the endothermic zone of the reaction is 400-70 (TC, after the catalyst flows out of the reaction endothermic zone, the temperature is lowered by 50-300 ° C than the inlet of the endothermic zone to achieve the conversion of methanol to an olefin reactor. The temperature is then passed to a reactor for the conversion of methanol to olefins.
  • the products comprising ethylene and propylene formed in the endothermic zone of the above cracking reaction can be combined into the methanol converted product.
  • the above catalyst comprises a silica-alumina or/and a phosphosilicate molecular sieve catalyst having a pore diameter of 0.3 to 0.6-nm, such as ZSM-5, ZSM 11, SAP0-34, SAP0-11, etc., and their elemental modifications. Sex product.
  • the above catalyst further comprises a matrix material which is one or more of silica, alumina or clay.
  • the hydrocarbons used in the above reaction endothermic zone have a carbon number of 4-20, which may be a product of C 4 or more in the methylene formation reaction, or may be other C 4 _C 2 . Hydrocarbons, including naphtha, gasoline, condensate, light diesel, hydrogenated tail oil and kerosene. Specific embodiment
  • SAP0—34 (Dalian Institute of Chemical Physics, silicon-aluminum ratio 0.2) mixed with clay, aluminum sol and silica sol (both purchased from Zhejiang Yuda Chemical Co., Ltd.) and dispersed into water slurry After spray molding, the microspheres have a particle size distribution of 20 to 100 microns. The above microspheres were calcined at 600 Torr for 4 hours, which is the catalyst used in this example. The content of SAP0-34 in the catalyst is 30 weight%.
  • the reaction was carried out in a fluidized bed microreactor having an inner diameter of 20 mm.
  • the reaction conditions are as follows: The catalyst loading is 10g, butene-2 (Fushun Petrochemical Company, purity 98%, cis, anti-butene-2 ratio is 1), the feed mass space velocity is
  • reaction pressure was 0. lMPa.
  • the reaction product was analyzed by Varian CP-3800 gas chromatography, Pona column and hydrogen flame detector, and the sampling time was 2 minutes.
  • the heat of reaction is calculated from the thermodynamic constants of the starting materials and products.
  • the thermodynamic data of C5 is the average of 10 isomers, olefins, diolefins and cycloalkane isomers.
  • C6 is 12 kinds of terpenes, olefins, diolefins and rings. The average of the alkane isomers. Each substance is assumed to be an ideal gas under the reaction conditions.
  • c 6 + represents a product of ⁇ and above.
  • Example 2 The procedure described in Example 1 was repeated except that the reaction temperature was 550 ° C.
  • Reaction Endotherm (KJ/Kg) 7. 04*10 2 C e + means (: 6 and ( 6 or more products.
  • C e + means ( 3 and (: 6 or more products).
  • the cleavage of kerosene on the ZSM-5 molecular sieve catalyst, the preparation procedure and the reaction operation of the catalyst are the same as those in the first embodiment except that the SAP0-34 molecular sieve is replaced by ZSM-5 (Nankai University molecular sieve plant, the ratio of silicon to aluminum is 50), and the raw material is replaced by kerosene. (No. 3 aviation kerosene, Qilu Petrochemical).
  • the heat of reaction calculation was the same as in Example 1.
  • the combustion of kerosene was -7513 kJ.
  • the conversion reaction results and heat of reaction of Kg-kerosene on the molecular sieve catalyst are shown in Table 4.
  • the reaction temperature is 550 ° C.
  • thermodynamic functions of kerosene are in the order of twelve iridium. From the data in the table, the selectivity of ethylene and propylene in the reaction product was 28.91% under this condition, and the reaction endotherm of the cracking reaction was 2238 KJ/Kg under the distribution condition of the product.
  • Table 4 Pyrolysis of kerosene in Example 4 Reaction product and heat of reaction (550 ⁇ )
  • Example 4 The procedure described in Example 4 was repeated except that the reaction temperature was 600 ° C.
  • the conversion reaction results and reaction heat of kerosene on a molecular sieve catalyst are shown in Table 5.
  • the combustion of kerosene is -7513 kj. Kg" 1 , and other thermodynamic functions of kerosene are measured by n-dodecane. From the data in the table, it is known that The selectivity of ethylene and propylene in the product was 36.97%. Under the distribution condition of the product, the reaction endotherm of the cracking reaction was 2821 KJ/Kg.
  • C 5 + means (: 5 and (: 5 or more products).
  • the methanol-to-olefin conversion unit with a methanol conversion scale of 600,000 tons/year is operated at an average of 300 days per year, and the daily methanol treatment capacity is 2,000 tons.
  • the conversion device adopts a reaction-regeneration fluidized bed process, mainly comprising a methanol conversion reactor and a catalyst regenerator, and a cracking endothermic reactor is arranged on the catalyst transport route from the regenerator to the methanol conversion reactor, the reactor adopts Fluidized bed mode.
  • the regenerated high temperature catalyst first passes through the above-mentioned cracking reaction endothermic zone and then enters the methanol conversion reactor.
  • the SAP0-34 fluidized catalyst was used (the preparation procedure of the catalyst was the same as in Example 1), and the catalyst circulation amount was 2,000 tons/day.
  • the temperature of the regenerated catalyst (after stripping) was 650 ⁇ and the temperature was required to drop to 430 ° C before the catalyst entered the methanol conversion reactor.
  • the heat carried by the regenerated catalyst was absorbed by the catalytic cracking of butene-2 (sourced as in Example 1) and allowed to cool to 550 Torr.
  • the catalyst heat capacity is 840 J / (Kg, K), and the heat released by the catalyst during the cooling process is 1.68X103 ⁇ 4J/day.
  • the catalyst flows out of the above-mentioned endothermic reactor, and is cooled by the heat of the pipeline to 43 (TC, the heat loss of heat dissipation is 0.02 ⁇ 10 8 KJ/day before entering the methanol conversion reactor.
  • TC the heat loss of heat dissipation
  • the butene-2 in the cracking reactor was preheated to a feed of 20 CTC at a reaction temperature of 550 °C.
  • the heat of the butene-2 catalytic cracking reaction was 704 KJ/Kg.
  • the heat absorption per ton of butene-2 from feed to complete reaction is 12. 14X103 ⁇ 4J/Kg, the conversion of butene-2 is 75%, and the feed of butene-2 is 184 tons/day.
  • the catalyst temperature was lowered from 650 Torr to 550 °C.
  • the amount of heat that can be recovered by the catalytic cracking of the butene-2 is 4.45%, and the heat recovered is used for the catalytic cracking of butene-2, which can increase the yield of ethylene. , propylene 76. 0 tons / day.
  • Comparative example 1 Comparative example 1 :
  • the methanol-to-olefin conversion unit with a methanol conversion scale of 600,000 tons/year is treated with an average of 300 days per year and a daily methanol treatment capacity of 2,000 tons.
  • the conversion apparatus adopts a reaction-regeneration fluidized bed process similar to that of Embodiment 8, which mainly comprises a methanol conversion reactor and a catalyst regenerator, but does not provide a cleavage reaction endothermic zone, and the catalyst flows directly from the regenerator to the methanol conversion reaction through a transport route. Device.
  • the SAP0-34 fluidized catalyst was used (the preparation procedure of the catalyst was the same as in Example 1), and the catalyst circulation amount was 2000 tons/day.
  • the temperature of the regenerated catalyst (after stripping) is 650 ⁇ , and the catalyst is required before entering the methanol conversion reactor.
  • the temperature drop was 430 °C.
  • the catalyst is completely cooled by the transfer line to 430 ° C, and the catalyst heat capacity is 840 J / (Kg - K), then the heat loss during heat dissipation is 3.70X10 8 KJ / day.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
  • Catalysts (AREA)

Abstract

L'invention concerne un procédé de récupération de chaleur régénérée pendant la production d'oléfines inférieures à partir de méthanol par utilisation d'un lit fluidisé. Le procédé est caractérisé en ce que, avant la mise en contact avec le méthanol, les catalyseurs régénérés à température élevée entrent dans une zone de réaction par craquage à absorption thermique dans laquelle les catalyseurs entrent en contact avec les hydrocarbures. La réaction de craquage de ces hydrocarbures absorbe une partie de la chaleur portée par les catalyseurs régénérés afin d'en réduire la température pour satisfaire aux exigences de température de la conversion de méthanol.
PCT/CN2007/002537 2006-08-23 2007-08-22 Procédé de récupération de chaleur régénérée pendant la production d'oléfines inférieures à partir de méthanol WO2008025247A1 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
JP2009524885A JP2010501495A (ja) 2006-08-23 2007-08-22 メタノールからの低級オレフィンの製造過程における再生熱の回収方法
AU2007291786A AU2007291786A1 (en) 2006-08-23 2007-08-22 A process for recovering regenerated heat during the production of lower olefins from methanol
BRPI0715687-1A2A BRPI0715687A2 (pt) 2006-08-23 2007-08-22 Método para recuperação do calor de regeneração em um processo preparação das olefinas inferiores a partir do metanol.

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CN200610112557.X 2006-08-23
CN200610112557XA CN101130469B (zh) 2006-08-23 2006-08-23 一种甲醇制取低碳烯烃过程中再生热量的回收方法

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WO2008025247A1 true WO2008025247A1 (fr) 2008-03-06

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JP (1) JP2010501495A (fr)
KR (1) KR20090057027A (fr)
CN (1) CN101130469B (fr)
AU (1) AU2007291786A1 (fr)
BR (1) BRPI0715687A2 (fr)
WO (1) WO2008025247A1 (fr)
ZA (1) ZA200901045B (fr)

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CN101844087A (zh) * 2010-06-22 2010-09-29 西南化工研究设计院 一种甲醇转化制丙烯催化剂的制备方法

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US8704028B2 (en) * 2010-03-30 2014-04-22 Uop Llc Conversion of acyclic symmetrical olefins to higher and lower carbon number olefin products
US20120041243A1 (en) * 2010-08-10 2012-02-16 Uop Llc Integration of a methanol-to-olefin reaction system with a hydrocarbon pyrolysis system
CN102464522B (zh) * 2010-11-17 2015-02-11 中国石油化工股份有限公司 低碳烯烃的生产方法
CN102875295B (zh) * 2011-07-12 2015-01-07 中国石油化工股份有限公司 低碳烯烃的生产方法
CN102875297B (zh) * 2011-07-12 2015-09-09 中国石油化工股份有限公司 用甲醇和石脑油制备低碳烯烃的方法
CN102875288B (zh) * 2011-07-12 2015-06-10 中国石油化工股份有限公司 生产低碳烯烃的方法
CN102875299A (zh) * 2011-07-12 2013-01-16 中国石油化工股份有限公司 用甲醇和石脑油生产低碳烯烃的方法
KR101803406B1 (ko) 2014-08-01 2017-12-01 한국화학연구원 나프타와 메탄올 혼합 접촉분해 반응공정
WO2016018097A1 (fr) * 2014-08-01 2016-02-04 한국화학연구원 Processus réactionnel de craquage catalytique mixte du pétrole et du méthanol
KR20240010329A (ko) * 2022-07-15 2024-01-23 한국화학연구원 디젤과 메탄올 혼합원료의 접촉분해용 촉매 및 이의 제조방법

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GB2171718A (en) * 1985-02-15 1986-09-03 Inst Francais Du Petrole Olefin preparation
CN1382198A (zh) * 1999-09-29 2002-11-27 埃克森化学专利公司 由氧合物生产烯烃的方法

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ZA200901045B (en) 2010-05-26
AU2007291786A1 (en) 2008-03-06
CN101130469A (zh) 2008-02-27
KR20090057027A (ko) 2009-06-03
CN101130469B (zh) 2011-04-13
BRPI0715687A2 (pt) 2014-12-23
JP2010501495A (ja) 2010-01-21

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