CN111233608A - A kind of raw material conversion method containing naphtha - Google Patents

A kind of raw material conversion method containing naphtha Download PDF

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CN111233608A
CN111233608A CN201811446192.3A CN201811446192A CN111233608A CN 111233608 A CN111233608 A CN 111233608A CN 201811446192 A CN201811446192 A CN 201811446192A CN 111233608 A CN111233608 A CN 111233608A
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catalyst
fluidized bed
bed reactor
naphtha
product gas
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赵银峰
叶茂
刘中民
唐海龙
王静
张今令
张涛
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Dalian Institute of Chemical Physics of CAS
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    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C4/00Preparation of hydrocarbons from hydrocarbons containing a larger number of carbon atoms
    • C07C4/02Preparation of hydrocarbons from hydrocarbons containing a larger number of carbon atoms by cracking a single hydrocarbon or a mixture of individually defined hydrocarbons or a normally gaseous hydrocarbon fraction
    • C07C4/06Catalytic processes
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    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10GCRACKING 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
    • C10G11/00Catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
    • YGENERAL 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
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Abstract

本申请公开了一种含有石脑油的原料的转化方法,包括以下步骤:a)含有石脑油的原料与催化剂在提升管反应器中接触反应后,通入流化床反应器,经流化床反应器扩大段分离,得到产品气I和经预积碳的催化剂;所述经预积碳的催化剂下行至所述流化床反应器的反应段;b)将含有石脑油和/或甲醇的原料从所述流化床反应器的底部输入,上行至所述流化床反应器的反应段与所述经积碳的催化剂接触,得到产品气II和待再生催化剂;所述待再生催化剂下行进入再生器再生后,得到再生催化剂;c)经所述再生催化剂返回所述提升管反应器中。该方法用于石脑油催化裂解中,具有产物种类可调变的优势。The present application discloses a method for converting a raw material containing naphtha, which includes the following steps: a) after the raw material containing naphtha and a catalyst are contacted and reacted in a riser reactor, pass into a fluidized bed reactor, and pass through a fluidized bed reactor. Separation in the enlarged section of the fluidized bed reactor to obtain a product gas I and a catalyst pre-deposited; the catalyst pre-deposited goes down to the reaction section of the fluidized bed reactor; b) will contain naphtha and/or Or the raw material of methanol is input from the bottom of the fluidized-bed reactor, and goes up to the reaction section of the fluidized-bed reactor to contact with the catalyst after carbon deposition, to obtain product gas II and the catalyst to be regenerated; After the regenerated catalyst descends into the regenerator for regeneration, a regenerated catalyst is obtained; c) returns to the riser reactor through the regenerated catalyst. The method is used in the catalytic cracking of naphtha, and has the advantage of adjustable product types.

Description

一种含有石脑油的原料转化方法A kind of raw material conversion method containing naphtha

技术领域technical field

本发明涉及一种含有石脑油的原料转化为低碳烯烃、芳烃和高品质汽油的方法,属于催化领域。The invention relates to a method for converting raw materials containing naphtha into low-carbon olefins, aromatic hydrocarbons and high-quality gasoline, and belongs to the field of catalysis.

背景技术Background technique

石脑油是生产乙烯、丙烯最主要的原料之一。石脑油高温水蒸气裂解制乙烯、丙烯等化工产品是一个巨大的石化产业。每年有数以亿吨的石脑油用于生产乙烯丙烯,其产量占乙烯丙烯生产总量50%以上。经过多年的发展,水蒸气裂解技术已经达到很高水平,它的转化率高,经过一次反应,产物的产率就可以达到较高的水平。但是缺点同样明显,选择性差,产物中有大量的甲烷生成,反应温度高,能耗高。其发展潜力已经很小。为此,采用催化剂降低裂解温度的催化裂解技术得到了大力发展。目前石脑油催化裂解技术主要通过提升管反应器进行,提高乙烯丙烯的收率。但是相对可调节范围较小。Naphtha is one of the most important raw materials for the production of ethylene and propylene. High-temperature steam cracking of naphtha to produce chemical products such as ethylene and propylene is a huge petrochemical industry. Every year, hundreds of millions of tons of naphtha are used to produce ethylene propylene, and its output accounts for more than 50% of the total ethylene propylene production. After years of development, steam cracking technology has reached a high level, and its conversion rate is high. After one reaction, the product yield can reach a high level. However, the disadvantages are also obvious, the selectivity is poor, a large amount of methane is generated in the product, the reaction temperature is high, and the energy consumption is high. Its development potential is already very small. To this end, catalytic cracking technology that uses catalysts to reduce the cracking temperature has been vigorously developed. At present, the naphtha catalytic cracking technology is mainly carried out through a riser reactor to improve the yield of ethylene and propylene. But the relatively adjustable range is small.

随着煤经甲醇制烯烃技术、丙烷脱氢制丙烯等技术的应用,乙烯、丙烯的来源日益丰富。这就要求石脑油催化裂解技术要求具有更高的可调变性,满足市场需求的变化。本申请很好的解决了该问题。With the application of technologies such as coal-to-olefin technology and propane dehydrogenation to propylene, the sources of ethylene and propylene are increasingly abundant. This requires the naphtha catalytic cracking technology to have higher adjustable variability to meet changes in market demand. This application solves this problem very well.

发明内容SUMMARY OF THE INVENTION

根据本申请的一个方面,提供了一种含有石脑油的原料转化为低碳烯烃、芳烃和高品质汽油的方法。该方法用于石脑油催化裂解中,具有产物种类可调变的优势。According to one aspect of the present application, a method for converting a naphtha-containing feedstock into light olefins, aromatics and high-quality gasoline is provided. The method is used in the catalytic cracking of naphtha, and has the advantage of adjustable product types.

为实现上述目的,本申请提供了一种含有石脑油的原料转化为低碳烯烃、芳烃和高品质汽油的方法,该方法包括以下步骤:包括石脑油的原料进入提升管反应器与催化剂接触,生成的产物和催化剂物流进入流化床反应器扩大段分离,产物进入产品气出口管线,催化剂进入流化床反应器反应段,包括石脑油或/和甲醇的原料通过流化床反应器进料口进入流化床反应器反应段与催化剂反应,生成的产物进入产品气出口管线,催化剂下行进入流化床反应器汽提段,经过汽提后,通过待生斜管、提升管,进入再生器,经过再生的催化剂通过再生器汽提段、再生斜管进入提升管反应器;产品气经过产品气出口管线进入分离系统,得到不同产物。In order to achieve the above purpose, the present application provides a method for converting a naphtha-containing feedstock into low-carbon olefins, aromatic hydrocarbons and high-quality gasoline, the method comprising the following steps: the feedstock including the naphtha enters a riser reactor and a catalyst Contact, the generated product and catalyst stream enter the expansion section of the fluidized bed reactor for separation, the product enters the product gas outlet line, and the catalyst enters the reaction section of the fluidized bed reactor, and the raw materials including naphtha or/and methanol are reacted through the fluidized bed The feed port of the reactor enters the reaction section of the fluidized bed reactor to react with the catalyst, the generated product enters the product gas outlet pipeline, and the catalyst descends into the stripping section of the fluidized bed reactor. , into the regenerator, the regenerated catalyst enters the riser reactor through the regenerator stripping section and the regeneration inclined pipe; the product gas enters the separation system through the product gas outlet pipeline to obtain different products.

上述方案中,所述提升管反应器的条件:反应温度为580~720℃,反应压力以表压计为0.01~0.3MPa,气相线速为3~10m/s;流化床反应器条件:反应温度580~720℃,反应压力以表压计为0.01~0.3Pa,气相线速为0.5~1.5m/s,质量空速为0.5~2h-1In the above scheme, the conditions of the riser reactor: the reaction temperature is 580~720℃, the reaction pressure is 0.01~0.3MPa in gauge pressure, and the gas phase linear velocity is 3~10m/s; the fluidized bed reactor conditions: The reaction temperature is 580-720°C, the reaction pressure is 0.01-0.3Pa in gauge pressure, the gas phase linear velocity is 0.5-1.5m/s, and the mass space velocity is 0.5-2h -1 .

所述的再生催化剂碳含量质量比例低于0.2%。The carbon content of the regenerated catalyst is less than 0.2% by mass.

所述含有石脑油的原料的转化方法,其特征在于,包括以下步骤:The transformation method of the raw material containing naphtha is characterized in that, comprises the following steps:

a)含有石脑油的原料与催化剂在提升管反应器中接触反应后,通入流化床反应器,经流化床反应器扩大段分离,得到产品气I和经预积碳的催化剂;所述经预积碳的催化剂下行至所述流化床反应器的反应段;a) after the raw material containing naphtha and the catalyst are contacted and reacted in the riser reactor, they are passed into the fluidized bed reactor and separated through the enlarged section of the fluidized bed reactor to obtain product gas I and the catalyst through pre-carbon deposition; The pre-carbonized catalyst descends to the reaction section of the fluidized bed reactor;

b)将含有石脑油和/或甲醇的原料从所述流化床反应器的底部输入,上行至所述流化床反应器的反应段与所述经积碳的催化剂接触,得到产品气II和待再生催化剂;所述待再生催化剂下行进入再生器再生后,得到再生催化剂;b) inputting the raw material containing naphtha and/or methanol from the bottom of the fluidized bed reactor, and going up to the reaction section of the fluidized bed reactor to contact with the carbon deposited catalyst to obtain product gas II and the catalyst to be regenerated; after the catalyst to be regenerated goes down into the regenerator for regeneration, the regenerated catalyst is obtained;

c)所述再生催化剂返回所述提升管反应器中;c) returning the regenerated catalyst to the riser reactor;

其中,产品气I和产品气II混合输出,经分离,得到烯烃、芳烃和汽油。Among them, product gas I and product gas II are mixed and output, and after separation, olefins, aromatics and gasoline are obtained.

可选地,所述烯烃包括乙烯、丙烯、丁烯。Optionally, the olefin includes ethylene, propylene, butene.

可选地,所述芳烃包括苯、甲苯、二甲苯。Optionally, the aromatic hydrocarbons include benzene, toluene, and xylene.

可选地,所述提升管反应器的条件:反应温度为580~720℃,反应压力以表压计为0.01~0.3MPa,气相线速为3~10m/s;Optionally, the conditions of the riser reactor: the reaction temperature is 580-720° C., the reaction pressure is 0.01-0.3 MPa in gauge pressure, and the gas phase linear velocity is 3-10 m/s;

所述流化床反应器条件:反应温度580~720℃,反应压力以表压计为0.01~0.3Pa,气相线速为0.5~1.5m/s,甲醇和/或石脑油的总质量空速为0.5~2h-1。其中,甲醇和石脑油的比例可以任意调变。The conditions of the fluidized bed reactor: the reaction temperature is 580-720°C, the reaction pressure is 0.01-0.3Pa in gauge pressure, the gas phase linear velocity is 0.5-1.5m/s, and the total mass of methanol and/or naphtha is empty. The speed is 0.5~2h -1 . Among them, the ratio of methanol and naphtha can be adjusted arbitrarily.

可选地,所述提升管反应器中的反应温度的上限选自590℃、600℃、610℃、620℃、630℃、640℃、650℃、660℃、670℃、680℃、690℃、700℃、710℃或720℃;下限选自580℃、590℃、600℃、610℃、620℃、630℃、640℃、650℃、660℃、670℃、680℃、690℃、700℃或710℃。Optionally, the upper limit of the reaction temperature in the riser reactor is selected from 590°C, 600°C, 610°C, 620°C, 630°C, 640°C, 650°C, 660°C, 670°C, 680°C, 690°C , 700°C, 710°C or 720°C; the lower limit is selected from 580°C, 590°C, 600°C, 610°C, 620°C, 630°C, 640°C, 650°C, 660°C, 670°C, 680°C, 690°C, 700°C °C or 710 °C.

可选地,所述提升管反应器中的反应压力以表压计上限选自0.02MPa、0.05MPa、0.08MPa、0.1MPa、0.15MPa、0.2MPa、0.25MPa或0.3MPa;下限选自0.01MPa、0.02MPa、0.05MPa、0.08MPa、0.1MPa、0.15MPa、0.2MPa或0.25MPa。Optionally, the upper limit of the reaction pressure in the riser reactor is selected from 0.02MPa, 0.05MPa, 0.08MPa, 0.1MPa, 0.15MPa, 0.2MPa, 0.25MPa or 0.3MPa in gauge pressure; the lower limit is selected from 0.01MPa , 0.02MPa, 0.05MPa, 0.08MPa, 0.1MPa, 0.15MPa, 0.2MPa or 0.25MPa.

可选地,所述提升管反应器中的气相线速的上限选自3m/s、4m/s、5m/s、6m/s、7m/s、8m/s、9m/s或10m/s;下限选自2m/s、3m/s、4m/s、5m/s、6m/s、7m/s、8m/s或9m/s。Optionally, the upper limit of the linear velocity of the gas phase in the riser reactor is selected from 3m/s, 4m/s, 5m/s, 6m/s, 7m/s, 8m/s, 9m/s or 10m/s ; the lower limit is selected from 2m/s, 3m/s, 4m/s, 5m/s, 6m/s, 7m/s, 8m/s or 9m/s.

可选地,所述流化床反应器中的反应温度的上限选自590℃、600℃、610℃、620℃、630℃、640℃、650℃、660℃、670℃、680℃、690℃、700℃、710℃或720℃;下限选自580℃、590℃、600℃、610℃、620℃、630℃、640℃、650℃、660℃、670℃、680℃、690℃、700℃或710℃。Optionally, the upper limit of the reaction temperature in the fluidized bed reactor is selected from 590°C, 600°C, 610°C, 620°C, 630°C, 640°C, 650°C, 660°C, 670°C, 680°C, 690°C ℃, 700℃, 710℃ or 720℃; the lower limit is selected from 580℃, 590℃, 600℃, 610℃, 620℃, 630℃, 640℃, 650℃, 660℃, 670℃, 680℃, 690℃, 700°C or 710°C.

可选地,所述流化床反应器中的反应压力以表压计上限选自0.02MPa、0.05MPa、0.08MPa、0.1MPa、0.15MPa、0.2MPa、0.25MPa或0.3MPa;下限选自0.01MPa、0.02MPa、0.05MPa、0.08MPa、0.1MPa、0.15MPa、0.2MPa或0.25MPa。Optionally, the upper limit of the reaction pressure in the fluidized bed reactor is selected from 0.02MPa, 0.05MPa, 0.08MPa, 0.1MPa, 0.15MPa, 0.2MPa, 0.25MPa or 0.3MPa in gauge pressure; the lower limit is selected from 0.01 MPa, 0.02MPa, 0.05MPa, 0.08MPa, 0.1MPa, 0.15MPa, 0.2MPa or 0.25MPa.

可选地,所述流化床反应器中的气相线速的上限选自1m/s或1.5m/s;下限选自0.5m/s或1m/s。Optionally, the upper limit of the linear velocity of the gas phase in the fluidized bed reactor is selected from 1 m/s or 1.5 m/s; the lower limit is selected from 0.5 m/s or 1 m/s.

可选地,所述流化床反应器中的总质量空速的上限选自1h-1、1.5h-1、或2h-1;下限选自0.5h-1、1h-1或1.5h-1Optionally, the upper limit of the total mass space velocity in the fluidized bed reactor is selected from 1h -1 , 1.5h -1 , or 2h -1 ; the lower limit is selected from 0.5h -1 , 1h -1 or 1.5h -1 1 .

可选地,所述提升管反应器和所述流化床反应器进料量的质量比为1:9~9:1。Optionally, the mass ratio of the feed amount of the riser reactor and the fluidized bed reactor is 1:9-9:1.

可选地,所述提升管反应器和所述流化床反应器进料量的质量比为1:9、1:7、1:5、1:3、1:1、3:1、5:1、9:1及任意两个比值之间的范围值。Optionally, the mass ratio of the feed amount of the riser reactor and the fluidized bed reactor is 1:9, 1:7, 1:5, 1:3, 1:1, 3:1, 5 :1, 9:1, and the range between any two ratios.

可选地,步骤a)包括:含有石脑油的原料与催化剂在提升管中接触反应,所得包括经预反应的催化剂和产品气I的物流上行至流化床反应器;包括催化剂和产品气I的物流在流化床反应器的扩大段分离,所述产品气I进入产品气出口管线,所述经预反应的催化剂下行至所述流化床反应器的反应段。Optionally, step a) includes: the raw material containing naphtha is contacted and reacted with the catalyst in the riser, and the obtained stream including the pre-reacted catalyst and the product gas I ascends to the fluidized bed reactor; including the catalyst and the product gas The stream of I is separated in the expansion section of the fluidized bed reactor, the product gas I enters the product gas outlet line, and the pre-reacted catalyst descends to the reaction section of the fluidized bed reactor.

可选地,步骤b)包括:将含有石脑油和甲醇的原料从所述流化床反应器的底部输入,上行至所述流化床反应器的反应段与所述经预反应的催化剂接触,得到产品气II和待再生催化剂;所述产品气II上行至流化床反应器的扩大段进入产品气出口管线;所述待再生催化剂下行至所述流化床反应器的汽提段,经待生斜管、提升管进入再生器再生。Optionally, step b) includes: inputting the raw material containing naphtha and methanol from the bottom of the fluidized bed reactor, and ascending to the reaction section of the fluidized bed reactor and the pre-reacted catalyst contact to obtain product gas II and the catalyst to be regenerated; the product gas II goes up to the expansion section of the fluidized bed reactor and enters the product gas outlet pipeline; the catalyst to be regenerated goes down to the stripping section of the fluidized bed reactor , enter the regenerator through the inclined tube and the riser to be regenerated.

可选地,步骤c)包括:再生催化剂经再生器汽提段、再生斜管返回所述提升管反应器中。Optionally, step c) includes: returning the regenerated catalyst to the riser reactor through the regenerator stripping section and the regeneration inclined pipe.

可选地,所述再生催化剂碳含量质量比例低于0.5%。Optionally, the carbon content of the regenerated catalyst is less than 0.5% by mass.

可选地,所述再生催化剂碳含量质量比例低于0.2%。Optionally, the carbon content of the regenerated catalyst is less than 0.2% by mass.

可选地,所述再生催化剂碳含量质量比例低于0.1%。Optionally, the carbon content of the regenerated catalyst is less than 0.1% by mass.

可选地,所述催化剂为含有石脑油催化裂解活性微球催化剂;所述微球催化剂的直径为30~300μm。Optionally, the catalyst is a microsphere catalyst containing naphtha catalytic cracking activity; the diameter of the microsphere catalyst is 30-300 μm.

可选地,所述微球催化剂中的分子筛的重量含量为10~50%。Optionally, the weight content of the molecular sieve in the microsphere catalyst is 10-50%.

可选地,所述微球催化剂中分子筛的重量含量的上限选自20%、30%、40%或50%;上限选自10%、20%、30%或40%。Optionally, the upper limit of the weight content of molecular sieve in the microsphere catalyst is selected from 20%, 30%, 40% or 50%; the upper limit is selected from 10%, 20%, 30% or 40%.

可选地,所述微球催化剂的直径优选50~150μm。Optionally, the diameter of the microsphere catalyst is preferably 50-150 μm.

可选地,所述催化剂为含有ZSM-5分子筛的微球催化剂。Optionally, the catalyst is a microsphere catalyst containing ZSM-5 molecular sieve.

可选地,所述微球催化剂的成型包括:将含有分子筛和粘结剂的浆料喷雾干燥成型。Optionally, the forming of the microsphere catalyst includes: spray-drying the slurry containing the molecular sieve and the binder.

可选地,所述的石脑油馏程在20~200℃之间。Optionally, the distillation range of the naphtha is between 20 and 200°C.

作为一种实施方式,所述的方法,包括以下步骤:含有石脑油的原料进入提升管反应器与催化剂接触,生成的产物I和催化剂物流进入流化床反应器扩大段分离,产物I进产品气出口管线,催化剂进入流化床反应器反应段,含有石脑油和/或甲醇的原料通过流化床反应器进料口进入流化床反应器反应段与催化剂反应,生成的产物II进入产品气出口管线,催化剂下行进入流化床反应器汽提段,经过汽提后,通过待生斜管、提升管,进入再生器,经过再生的催化剂通过再生器汽提段、再生斜管进入提升管反应器;产品气经过产品气出口管线进入分离系统,得到包括烯烃、芳烃和汽油的产物。As an embodiment, the described method comprises the following steps: the raw material containing naphtha enters the riser reactor to contact with the catalyst, the generated product I and the catalyst stream enter the fluidized bed reactor expansion section for separation, and the product I enters the The product gas outlet pipeline, the catalyst enters the reaction section of the fluidized bed reactor, the raw material containing naphtha and/or methanol enters the reaction section of the fluidized bed reactor through the feed port of the fluidized bed reactor and reacts with the catalyst to generate product II After entering the product gas outlet pipeline, the catalyst descends into the stripping section of the fluidized bed reactor. After stripping, it enters the regenerator through the inclined tube to be regenerated and the riser. The regenerated catalyst passes through the stripping section of the regenerator and the inclined tube for regeneration. Enter the riser reactor; the product gas enters the separation system through the product gas outlet line to obtain products including olefins, aromatics and gasoline.

可选地,所述方法,烯烃、芳烃和汽油的质量收率可调变。Optionally, in the method, the mass yields of olefins, aromatics and gasoline can be adjusted.

可选地,烯烃的质量收率为42~72%,芳烃的质量收率为16~24%,汽油的质量收率为6~21%。Optionally, the mass yield of olefins is 42-72%, the mass yield of aromatics is 16-24%, and the mass yield of gasoline is 6-21%.

本申请能产生的有益效果包括:The beneficial effects that this application can produce include:

1)本申请的装置提升管反应器和流化床反应器,可同时也可单独进行石脑油的催化裂解反应。1) The riser reactor and the fluidized bed reactor of the device of the present application can simultaneously or independently carry out the catalytic cracking reaction of naphtha.

2)本申请可以通过调整提升管反应器和流化床反应器的进料比例可以在较大范围内调控产物组分含量。2) In the present application, the content of product components can be regulated in a wide range by adjusting the feed ratio of the riser reactor and the fluidized bed reactor.

3)本申请提供一种含有石脑油原料的转化方法,产物为低碳烯烃、轻质芳烃和高品质汽油,产物比例可调节。该方法通过采用包括石脑油的原料同时进入提升管反应器和流化床反应器,反应产物在流化床反应器顶部出口汇合后进入分离系统,得到低碳烯烃、轻质芳烃和高品质汽油;催化剂由再生器经提升管反应器进入流化床反应器,完成催化裂解后回到再生器再生。该方法提高了石脑油催化裂解产物调变范围,提高了装置抵御市场波动风险的能力。3) The present application provides a conversion method containing naphtha raw materials, the products are low-carbon olefins, light aromatic hydrocarbons and high-quality gasoline, and the product ratio can be adjusted. In the method, the raw materials including naphtha are simultaneously fed into the riser reactor and the fluidized bed reactor, and the reaction products are merged at the top outlet of the fluidized bed reactor and then enter the separation system to obtain low-carbon olefins, light aromatics and high-quality Gasoline; the catalyst enters the fluidized bed reactor from the regenerator through the riser reactor, and returns to the regenerator for regeneration after the catalytic cracking is completed. The method improves the modulation range of the naphtha catalytic cracking product and improves the ability of the device to resist the risk of market fluctuations.

附图说明Description of drawings

图1为本申请所述装置的流程示意图。FIG. 1 is a schematic flowchart of the device described in the present application.

部件和附图标记列表:List of parts and reference numbers:

1:提升管反应器进料口,2:提升管反应器,3:流化床反应器,4:流化床反应器进料口,5:流化床反应器汽提段进气口,6:提升管提升器进口,7:产品气出口管线,8:烟气出口管线,9:再生器,10:再生空气入口,11:再生器汽提段进气口,12:再生斜管,13:待生斜管,14:流化床反应器扩大段,15:流化床反应器反应段,16:流化床反应器汽提段,17:再生器扩大段,18:再生器再生段,19:再生器汽提段,20:提升管20。1: feed inlet of riser reactor, 2: riser reactor, 3: fluidized bed reactor, 4: feed inlet of fluidized bed reactor, 5: inlet of stripping section of fluidized bed reactor, 6: Riser riser inlet, 7: Product gas outlet line, 8: Flue gas outlet line, 9: Regenerator, 10: Regeneration air inlet, 11: Regenerator stripping section inlet, 12: Regeneration inclined pipe, 13: Inclined pipe to be grown, 14: Expanded section of fluidized bed reactor, 15: Reacted section of fluidized bed reactor, 16: Stripping section of fluidized bed reactor, 17: Expanded section of regenerator, 18: Regeneration of regenerator Section, 19: Regenerator stripping section, 20: Riser 20.

具体实施方式Detailed ways

下面结合实施例详述本申请,但本申请并不局限于这些实施例。The present application will be described in detail below with reference to the examples, but the present application is not limited to these examples.

如无特别说明,本申请的实施例中的原料均通过商业途径购买。Unless otherwise specified, the raw materials in the examples of this application are all purchased through commercial channels.

实施例中,催化剂为“含有石脑油催化裂解活性的微球”,所述催化剂根据专利CN200710118286.3的方法制备。In the embodiment, the catalyst is "microspheres containing naphtha catalytic cracking activity", and the catalyst is prepared according to the method of patent CN200710118286.3.

本申请的实施例中分析方法如下:The analytical method in the embodiment of the application is as follows:

利用安捷伦气相色谱进行产物分析。Product analysis was performed using Agilent gas chromatography.

本申请的实施例中转化率、选择性计算如下:In the embodiment of the application, conversion rate, selectivity are calculated as follows:

本申请的实施例中,烯烃收率、芳烃收率、甲烷收率都基于质量进行计算:In the embodiment of this application, the olefin yield, aromatics yield, and methane yield are all calculated based on mass:

烯烃收率=(产物中烯烃质量含量*产物质量流率)/(产物质量流率+生焦率);芳烃收率=(产物中芳烃质量含量*产物质量流率)/(产物质量流率+生焦率);甲烷收率=(产物中甲烷质量含量*产物质量流率)/(产物质量流率+生焦率)。Olefin yield=(olefin mass content in product*product mass flow rate)/(product mass flow rate+coking rate); aromatics yield=(aromatic mass content in product*product mass flow rate)/(product mass flow rate + coke formation rate); methane yield=(methane mass content in product*product mass flow rate)/(product mass flow rate+ coke formation rate).

图1为本申请含有石脑油的原料转化为低碳烯烃和芳烃的方法采用的装置,该方法包括如下步骤:包括石脑油的原料进入提升管反应器2与催化剂接触,生成的产物和催化剂物流进入流化床反应器扩大段14分离,产物进入产品气出口管线,催化剂进入流化床反应器反应段15,包括石脑油或/和甲醇的原料通过流化床反应器进料口4进入流化床反应器反应段与催化剂反应,生成的产物进入产品气出口管线,催化剂下行进入流化床反应器汽提段16,经过汽提后,通过待生斜管13、提升管20,进入再生器9,经过再生的催化剂通过再生器汽提段19、再生斜管12进入提升管反应器2;产品气经过产品气出口管线进入分离系统,得到不同产物。,Fig. 1 is the device adopted in the method for converting the raw material containing naphtha into light olefins and aromatic hydrocarbons of the application, and the method comprises the following steps: the raw material including naphtha enters the riser reactor 2 to contact with the catalyst, and the generated products and The catalyst stream enters the expansion section 14 of the fluidized bed reactor for separation, the product enters the product gas outlet pipeline, and the catalyst enters the reaction section 15 of the fluidized bed reactor, and the raw materials including naphtha or/and methanol pass through the fluidized bed reactor feed port 4. Enter the reaction section of the fluidized bed reactor to react with the catalyst, the generated product enters the product gas outlet pipeline, and the catalyst descends into the stripping section 16 of the fluidized bed reactor. , enter the regenerator 9, the regenerated catalyst enters the riser reactor 2 through the regenerator stripping section 19 and the regeneration inclined pipe 12; the product gas enters the separation system through the product gas outlet pipeline to obtain different products. ,

实施例1Example 1

如图1所示的装置中,催化剂为含有石脑油催化裂解活性的微球催化剂,催化剂中分子筛的重量含量为30%,粒径范围为50-150微米。包括石脑油的原料进入提升管反应器与催化剂接触,生成的产物和催化剂物流进入流化床反应器扩大段分离,产物进入产品气出口管线,催化剂进入流化床反应器反应段,包括石脑油或/和甲醇的原料通过流化床反应器进料口进入流化床反应器反应段与催化剂反应,生成的产物进入产品气出口管线,催化剂下行进入流化床反应器汽提段,经过汽提后,通过待生斜管、提升管,进入再生器,经过再生的催化剂通过再生器汽提段、再生斜管进入提升管反应器。产品气经过产品气出口管线进入分离系统,得到不同产物。催化剂循环量通过塞阀或滑阀控制。再生催化剂碳含量质量分数低于0.1%。石脑油的组成见表1。提升管反应器的条件:反应温度为700℃,反应压力以表压计为0.01MPa,气相线速为3m/s;流化床反应器条件:反应温度690℃,反应压力以表压计为0.01MPa,气相线速为1m/s,石脑油和甲醇的质量比为2。提升管反应器和流化床反应器进料量的质量比为1:1。保持催化剂循环量稳定,流化床反应器质量空速为1h-1。产品气通过在线色谱分析,烯烃质量收率54%,BTX质量收率为23%,高品质汽油质量收率为15%。In the device shown in Figure 1, the catalyst is a microsphere catalyst containing naphtha catalytic cracking activity, the weight content of molecular sieve in the catalyst is 30%, and the particle size range is 50-150 microns. The raw material including naphtha enters the riser reactor to contact the catalyst, the generated product and catalyst stream enter the expansion section of the fluidized bed reactor for separation, the product enters the product gas outlet line, and the catalyst enters the reaction section of the fluidized bed reactor, including the The raw materials of naphtha or/and methanol enter the reaction section of the fluidized bed reactor through the feed port of the fluidized bed reactor to react with the catalyst, the generated product enters the product gas outlet pipeline, and the catalyst descends into the stripping section of the fluidized bed reactor, After stripping, it enters the regenerator through the inclined tube to be grown and the riser, and the regenerated catalyst enters the riser reactor through the stripping section of the regenerator and the regeneration inclined tube. The product gas enters the separation system through the product gas outlet line to obtain different products. The amount of catalyst circulating is controlled by a plug valve or spool valve. The mass fraction of carbon content of the regenerated catalyst is less than 0.1%. The composition of naphtha is shown in Table 1. Conditions of the riser reactor: the reaction temperature was 700°C, the reaction pressure was 0.01 MPa in gauge pressure, and the gas phase linear velocity was 3 m/s; fluidized bed reactor conditions: the reaction temperature was 690°C, and the reaction pressure was gauged as 0.01MPa, the linear velocity of the gas phase is 1m/s, and the mass ratio of naphtha and methanol is 2. The mass ratio of the feed to the riser reactor and the fluidized bed reactor was 1:1. Keep the catalyst circulation stable, and the mass space velocity of the fluidized bed reactor is 1h -1 . The product gas was analyzed by online chromatography, and the mass yield of olefin was 54%, the mass yield of BTX was 23%, and the mass yield of high-quality gasoline was 15%.

表1石脑油组成Table 1 Naphtha Composition

组成(wt%)Composition (wt%) 石脑油(IBP-150℃)Naphtha (IBP-150℃) 石脑油(IBP-180℃)Naphtha (IBP-180℃) 正构烷烃n-alkanes 4141 3535 异构烷烃isoparaffin 24twenty four 2929 环烷烃Naphthenic 1515 2828 芳烃Aromatic hydrocarbons 1414 77

实施例2Example 2

按照实施例1所述的条件和步骤,催化剂为含有石脑油催化裂解活性的微球,催化剂中分子筛的重量含量为30%,粒径范围为50-150微米。所述的再生催化剂碳含量质量分数低于0.5%。提升管反应器的条件:反应温度为680℃,反应压力以表压计为0.01MPa,气相线速为3m/s;流化床反应器条件:反应温度670℃,反应压力以表压计为0.01MPa,气相线速为1m/s,石脑油和甲醇的质量比为10。提升管反应器和流化床反应器进料量的质量比为9:1。保持催化剂循环量稳定,流化床反应器质量空速为0.5h-1。产品气通过在线色谱分析,烯烃质量收率45%,BTX质量收率为18%,高品质汽油质量收率为13%。According to the conditions and steps described in Example 1, the catalyst is a microsphere containing naphtha catalytic cracking activity, the weight content of molecular sieve in the catalyst is 30%, and the particle size range is 50-150 microns. The carbon content mass fraction of the regenerated catalyst is less than 0.5%. Conditions of the riser reactor: the reaction temperature was 680°C, the reaction pressure was 0.01 MPa in gauge pressure, and the gas phase linear velocity was 3 m/s; fluidized bed reactor conditions: the reaction temperature was 670°C, and the reaction pressure was gauged as 0.01MPa, the linear velocity of the gas phase is 1m/s, and the mass ratio of naphtha and methanol is 10. The mass ratio of the feed to the riser reactor and the fluidized bed reactor was 9:1. Keep the catalyst circulation stable, and the mass space velocity of the fluidized bed reactor is 0.5h -1 . The product gas was analyzed by online chromatography, and the mass yield of olefin was 45%, the mass yield of BTX was 18%, and the mass yield of high-quality gasoline was 13%.

实施例3Example 3

按照实施例1所述的条件和步骤,催化剂为含有石脑油催化裂解活性的微球,催化剂中分子筛的重量含量为30%,粒径范围为50-150微米。所述的再生催化剂碳含量质量分数低于0.5%。提升管反应器的条件:反应温度为680℃,反应压力以表压计为0.01MPa,气相线速为3m/s;流化床反应器条件:反应温度670℃,反应压力以表压计为0.01MPa,气相线速为1m/s,石脑油和甲醇的质量比为0.5。提升管反应器和流化床反应器进料量的质量比为1:9。保持催化剂循环量稳定,流化床反应器质量空速为1.5h-1。产品气通过在线色谱分析,烯烃质量收率72%,BTX质量收率为16%,高品质汽油质量收率为6%。According to the conditions and steps described in Example 1, the catalyst is a microsphere containing naphtha catalytic cracking activity, the weight content of molecular sieve in the catalyst is 30%, and the particle size range is 50-150 microns. The carbon content mass fraction of the regenerated catalyst is less than 0.5%. Conditions of the riser reactor: the reaction temperature was 680°C, the reaction pressure was 0.01 MPa in gauge pressure, and the gas phase linear velocity was 3 m/s; fluidized bed reactor conditions: the reaction temperature was 670°C, and the reaction pressure was gauged as 0.01MPa, the linear velocity of the gas phase is 1m/s, and the mass ratio of naphtha and methanol is 0.5. The mass ratio of the feed to the riser reactor and the fluidized bed reactor was 1:9. Keep the catalyst circulation stable, and the mass space velocity of the fluidized bed reactor is 1.5h -1 . The product gas was analyzed by online chromatography, and the mass yield of olefin was 72%, the mass yield of BTX was 16%, and the mass yield of high-quality gasoline was 6%.

实施例4Example 4

按照实施例1所述的条件和步骤,催化剂为含有石脑油催化裂解活性的微球,催化剂中分子筛的重量含量为30%,粒径范围为50-150微米。所述的再生催化剂碳含量质量分数低于0.5%。提升管反应器的条件:反应温度为720℃,反应压力以表压计为0.01MPa,气相线速为3m/s;流化床反应器条件:反应温度700℃,反应压力以表压计为0.01MPa,气相线速为1m/s,石脑油和甲醇的质量比为50。提升管反应器和流化床反应器进料量的质量比为1:1。保持催化剂循环量稳定,流化床反应器质量空速为1.0h-1。产品气通过在线色谱分析,烯烃质量收率42%,BTX质量收率为24%,高品质汽油质量收率为21%。According to the conditions and steps described in Example 1, the catalyst is a microsphere containing naphtha catalytic cracking activity, the weight content of molecular sieve in the catalyst is 30%, and the particle size range is 50-150 microns. The carbon content mass fraction of the regenerated catalyst is less than 0.5%. Conditions of the riser reactor: the reaction temperature was 720°C, the reaction pressure was 0.01 MPa in gauge pressure, and the gas phase linear velocity was 3 m/s; fluidized bed reactor conditions: the reaction temperature was 700°C, and the reaction pressure was gauged as 0.01MPa, the linear velocity of the gas phase is 1m/s, and the mass ratio of naphtha and methanol is 50. The mass ratio of the feed to the riser reactor and the fluidized bed reactor was 1:1. Keep the catalyst circulation stable, and the mass space velocity of the fluidized bed reactor is 1.0h -1 . The product gas was analyzed by online chromatography, and the mass yield of olefin was 42%, the mass yield of BTX was 24%, and the mass yield of high-quality gasoline was 21%.

实施例5Example 5

按照实施例1所述的条件和步骤,催化剂为含有石脑油催化裂解活性的微球,催化剂中分子筛的重量含量为30%,粒径范围为50-150微米。所述的再生催化剂碳含量质量分数低于0.5%。提升管反应器的条件:反应温度为720℃,反应压力以表压计为0.01MPa,气相线速为3m/s;流化床反应器条件:反应温度700℃,反应压力以表压计为0.01MPa,气相线速为1m/s,石脑油和甲醇的质量比为1。提升管反应器和流化床反应器石脑油进料量的质量比为1:1。保持催化剂循环量稳定,流化床反应器总质量空速为1.0h-1。产品气通过在线色谱分析,烯烃质量收率61%,BTX质量收率为19%,高品质汽油质量收率为9%。According to the conditions and steps described in Example 1, the catalyst is a microsphere containing naphtha catalytic cracking activity, the weight content of molecular sieve in the catalyst is 30%, and the particle size range is 50-150 microns. The carbon content mass fraction of the regenerated catalyst is less than 0.5%. Conditions of the riser reactor: the reaction temperature was 720°C, the reaction pressure was 0.01MPa in gauge pressure, and the gas phase linear velocity was 3m/s; fluidized bed reactor conditions: the reaction temperature was 700°C, and the reaction pressure was gauged as 0.01MPa, the linear velocity of the gas phase is 1m/s, and the mass ratio of naphtha and methanol is 1. The mass ratio of the naphtha feed to the riser reactor and the fluidized bed reactor was 1:1. To keep the catalyst circulation stable, the total mass space velocity of the fluidized bed reactor is 1.0h -1 . The product gas was analyzed by online chromatography, and the mass yield of olefin was 61%, the mass yield of BTX was 19%, and the mass yield of high-quality gasoline was 9%.

实施例6Example 6

按照实施例1所述的条件和步骤,催化剂为含有石脑油催化裂解活性的微球,催化剂中分子筛的重量含量为10%,粒径范围为50~150微米。所述的再生催化剂碳含量质量分数低于0.5%。流化床反应器的反应段的催化剂床层高径比为0.3。提升管反应器的条件:反应温度为680℃,反应压力以表压计为0.01MPa,气相线速为3m/s;流化床反应器条件:反应温度670℃,反应压力以表压计为0.01MPa,气相线速为1m/s,石脑油和甲醇的质量比为10。提升管反应器和流化床反应器进料量的质量比为9:1。保持催化剂循环量稳定,流化床反应器质量空速为0.5h-1。产品气通过在线色谱分析,烯烃质量收率42%,BTX质量收率为17%,高品质汽油质量收率为15%。According to the conditions and steps described in Example 1, the catalyst is a microsphere containing naphtha catalytic cracking activity, the weight content of molecular sieve in the catalyst is 10%, and the particle size range is 50-150 microns. The carbon content mass fraction of the regenerated catalyst is less than 0.5%. The height-diameter ratio of the catalyst bed in the reaction section of the fluidized bed reactor was 0.3. Conditions of the riser reactor: the reaction temperature was 680°C, the reaction pressure was 0.01 MPa in gauge pressure, and the gas phase linear velocity was 3 m/s; fluidized bed reactor conditions: the reaction temperature was 670°C, and the reaction pressure was gauged as 0.01MPa, the linear velocity of the gas phase is 1m/s, and the mass ratio of naphtha and methanol is 10. The mass ratio of the feed to the riser reactor and the fluidized bed reactor was 9:1. Keep the catalyst circulation stable, and the mass space velocity of the fluidized bed reactor is 0.5h -1 . The product gas was analyzed by online chromatography, and the mass yield of olefin was 42%, the mass yield of BTX was 17%, and the mass yield of high-quality gasoline was 15%.

实施例7Example 7

按照实施例1所述的条件和步骤,催化剂为含有石脑油催化裂解活性的微球,催化剂中分子筛的重量含量为50%,粒径范围为50~150微米。所述的再生催化剂碳含量质量分数低于0.5%。流化床反应器的反应段的催化剂床层高径比为0.3。提升管反应器的条件:反应温度为680℃,反应压力以表压计为0.01MPa,气相线速为3m/s;流化床反应器条件:反应温度670℃,反应压力以表压计为0.01MPa,气相线速为1m/s,石脑油和甲醇的质量比为10。提升管反应器和流化床反应器进料量的质量比为9:1。保持催化剂循环量稳定,流化床反应器质量空速为0.5h-1。产品气通过在线色谱分析,烯烃质量收率78%,BTX质量收率为22%,高品质汽油质量收率为11%。According to the conditions and steps described in Example 1, the catalyst is a microsphere containing naphtha catalytic cracking activity, the weight content of molecular sieve in the catalyst is 50%, and the particle size range is 50-150 microns. The carbon content mass fraction of the regenerated catalyst is less than 0.5%. The height-diameter ratio of the catalyst bed in the reaction section of the fluidized bed reactor was 0.3. Conditions of the riser reactor: the reaction temperature was 680°C, the reaction pressure was 0.01 MPa in gauge pressure, and the gas phase linear velocity was 3 m/s; fluidized bed reactor conditions: the reaction temperature was 670°C, and the reaction pressure was gauged as 0.01MPa, the linear velocity of the gas phase is 1m/s, and the mass ratio of naphtha and methanol is 10. The mass ratio of the feed to the riser reactor and the fluidized bed reactor was 9:1. Keep the catalyst circulation stable, and the mass space velocity of the fluidized bed reactor is 0.5h -1 . The product gas was analyzed by online chromatography, and the mass yield of olefin was 78%, the mass yield of BTX was 22%, and the mass yield of high-quality gasoline was 11%.

以上所述,仅是本申请的几个实施例,并非对本申请做任何形式的限制,虽然本申请以较佳实施例揭示如上,然而并非用以限制本申请,任何熟悉本专业的技术人员,在不脱离本申请技术方案的范围内,利用上述揭示的技术内容做出些许的变动或修饰均等同于等效实施案例,均属于技术方案范围内。The above are only a few embodiments of the present application, and are not intended to limit the present application in any form. Although the present application is disclosed as above with preferred embodiments, it is not intended to limit the present application. Without departing from the scope of the technical solution of the present application, any changes or modifications made by using the technical content disclosed above are equivalent to equivalent implementation cases and fall within the scope of the technical solution.

Claims (10)

1. A process for converting a naphtha containing feedstock comprising the steps of:
a) after the raw material containing naphtha and the catalyst are in contact reaction in a riser reactor, introducing the raw material into a fluidized bed reactor, and separating the raw material and the catalyst through an expansion section of the fluidized bed reactor to obtain product gas I and the catalyst subjected to pre-deposited carbon; the pre-deposited catalyst descends to the reaction section of the fluidized bed reactor;
b) inputting raw materials containing naphtha and/or methanol from the bottom of the fluidized bed reactor, ascending to a reaction section of the fluidized bed reactor to contact with the carbon deposited catalyst to obtain product gas II and a catalyst to be regenerated; the catalyst to be regenerated is descended into a regenerator to be regenerated, and then a regenerated catalyst is obtained;
c) returning the regenerated catalyst to the riser reactor;
wherein, the product gas I and the product gas II are mixed and output, and are separated to obtain olefin, aromatic hydrocarbon and gasoline.
2. The method of claim 1, wherein the conditions of the riser reactor are: the reaction temperature is 580-720 ℃, the reaction pressure is 0.01-0.3 MPa in terms of gauge pressure, and the gas-phase linear speed is 3-10 m/s;
the fluidized bed reactor conditions: the reaction temperature is 580-720 ℃, the reaction pressure is 0.01-0.3 Pa in terms of gauge pressure, the gas-phase linear speed is 0.5-1.5 m/s, and the total mass space velocity of naphtha and/or methanol is 0.5-2 h-1
3. The method according to claim 1, wherein the mass ratio of the feeding amounts of the riser reactor and the fluidized bed reactor is 1: 9-9: 1.
4. The method of claim 1, wherein step a) comprises: contacting and reacting raw materials containing naphtha and a catalyst in a riser to obtain a material flow which comprises the pre-reacted catalyst and a product gas I and flows upwards to a fluidized bed reactor; the method comprises the steps of separating material flows of a catalyst and a product gas I in an expansion section of a fluidized bed reactor, enabling the product gas I to enter a product gas outlet pipeline, and enabling the pre-reacted catalyst to descend to a reaction section of the fluidized bed reactor.
5. The method of claim 1, wherein step b) comprises: inputting raw materials containing naphtha and methanol from the bottom of the fluidized bed reactor, ascending to a reaction section of the fluidized bed reactor to contact with the pre-reacted catalyst to obtain product gas II and a catalyst to be regenerated; the product gas II ascends to the expansion section of the fluidized bed reactor and enters a product gas outlet pipeline; the catalyst to be regenerated descends to a stripping section of the fluidized bed reactor and enters a regenerator for regeneration through a to-be-regenerated inclined pipe and a riser.
6. The method of claim 1, wherein step c) comprises: the regenerated catalyst returns to the riser reactor through the regenerator stripping section and the regeneration inclined tube.
7. The method according to claim 1, wherein the regenerated catalyst has a carbon content of less than 0.5% by mass.
8. The method of claim 1, wherein the catalyst is a microsphere catalyst comprising naphtha catalytic cracking activity; the diameter of the microspherical catalyst is 30-300 mu m.
9. The method of claim 1, wherein the microspheroidal catalyst has a diameter of 50 to 150 μm.
10. The method according to claim 1, wherein the naphtha boiling range is between 20 and 200 ℃.
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