CN114426876B - Conversion method of raw oil - Google Patents
Conversion method of raw oil Download PDFInfo
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- CN114426876B CN114426876B CN202011187111.XA CN202011187111A CN114426876B CN 114426876 B CN114426876 B CN 114426876B CN 202011187111 A CN202011187111 A CN 202011187111A CN 114426876 B CN114426876 B CN 114426876B
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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
- C10G55/00—Treatment of hydrocarbon oils, in the absence of hydrogen, by at least one refining process and at least one cracking process
- C10G55/02—Treatment of hydrocarbon oils, in the absence of hydrogen, by at least one refining process and at least one cracking process plural serial stages only
- C10G55/06—Treatment of hydrocarbon oils, in the absence of hydrogen, by at least one refining process and at least one cracking process plural serial stages only including at least one catalytic cracking step
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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
- C10G2300/201—Impurities
- C10G2300/202—Heteroatoms content, i.e. S, N, O, P
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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
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4006—Temperature
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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
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4012—Pressure
-
- 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
- C10G2300/40—Characteristics of the process deviating from typical ways of processing
- C10G2300/4018—Spatial velocity, e.g. LHSV, WHSV
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- Oil, Petroleum & Natural Gas (AREA)
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- General Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Production Of Liquid Hydrocarbon Mixture For Refining Petroleum (AREA)
Abstract
The present disclosure relates to a conversion method of raw oil, in which liquefied gas in reaction oil gas is subjected to adsorption desulfurization treatment by using a passivated regenerated desulfurization adsorbent in a raw oil conversion process to obtain a material containing the desulfurized liquefied gas, and then the material is subjected to absorption stabilization treatment. Because the activity of the passivated regenerated desulfurization adsorbent is low, the method disclosed by the invention can effectively avoid the conversion of unsaturated olefins in liquefied gas in reaction oil gas into saturated alkanes during desulfurization treatment, and can at least partially improve the yield of unsaturated olefins in liquefied gas while carrying out desulfurization treatment on the liquefied gas, thereby improving the yield of unsaturated olefins in reaction oil gas.
Description
Technical Field
The present disclosure relates to the field of petrochemical technology, and in particular, to a method for converting raw oil.
Background
Catalytic cracking is an important feedstock conversion means that converts feedstock into petroleum products such as liquefied gas, gasoline, and diesel under the action of heat and a catalyst. The liquefied gas produced by the conversion of the raw oil in the catalytic cracking process contains a large amount of sulfides, which mainly exist in the form of hydrogen sulfide, mercaptan, thioether and the like. With the development of petrochemical technology and the increasing perfection of related environmental regulations, sulfide removal in liquefied gas has become an important content in the technical field of petrochemical industry.
In the related art, sulfur compounds in liquefied gas are removed by adsorption by using a desulfurization adsorbent in the presence of hydrogen. However, in the above-described method, a part of olefins in the liquefied gas react with hydrogen to form saturated alkanes, which may lower the yield of olefins in the liquefied gas.
Disclosure of Invention
The purpose of the present disclosure is to provide a conversion method of raw oil.
In order to achieve the above object, the present disclosure provides a conversion method of raw oil, the method comprising the steps of:
s1, under the catalytic cracking condition, the raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas is separated from the reaction oil gas;
s2, carrying out desulfurization treatment on the liquefied gas to obtain a material containing the liquefied gas after desulfurization treatment, and carrying out absorption stabilization treatment on the material containing the liquefied gas after desulfurization treatment;
the desulfurization treatment is performed in one or two modes:
mode one: transferring a spent desulfurization adsorbent into a regenerator for complete burning regeneration to obtain a complete regeneration desulfurization adsorbent, separating gasoline from the reaction oil gas, introducing the gasoline into the bottom of a rapid bed desulfurization reactor, contacting the complete regeneration desulfurization adsorbent with the complete regeneration desulfurization adsorbent in the rapid bed desulfurization reactor for passivation to obtain a passivated regeneration desulfurization adsorbent, introducing the passivated regeneration desulfurization adsorbent into a bubbling bed desulfurization reactor, contacting the passivated regeneration adsorbent with liquefied gas and gas containing hydrogen in the bubbling bed desulfurization reactor for adsorption desulfurization reaction to obtain a reacted material, introducing the gas phase in the reacted material into a settling section at the upper part of the rapid bed desulfurization reactor from the top of the bubbling bed desulfurization reactor, introducing the solid phase in the reacted material into a passivation section at the lower part of the rapid bed desulfurization reactor from the lower part of the bubbling bed desulfurization reactor, and guiding the liquefied material containing treated gas from the top of the settling section at the upper part of the rapid bed desulfurization reactor;
mode two: transferring the spent desulfurization adsorbent into a regenerator for incomplete burning regeneration to obtain a passivated regenerated desulfurization adsorbent, introducing the passivated regenerated desulfurization adsorbent into a rapid bed desulfurization reactor, contacting the passivated regenerated desulfurization adsorbent with liquefied gas and hydrogen-containing gas in the rapid bed reactor, performing adsorption desulfurization reaction to obtain reacted materials, and leading out the materials containing the liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor.
Optionally, when the passivated regenerated desulfurization adsorbent is subjected to an adsorption desulfurization reaction with liquefied gas and a gas containing hydrogen, the conditions of the adsorption desulfurization reaction include: the temperature is 200-550 ℃, the pressure is 0.3-3MPa, and the weight hourly space velocity of the liquefied gas is 0.1-50h -1 The weight ratio of the hydrogen to the liquefied gas is 1:100-5000;
preferably, when the passivated regenerated desulfurization adsorbent is subjected to an adsorption desulfurization reaction with liquefied gas and a gas containing hydrogen, the conditions of the adsorption desulfurization reaction include: the temperature is 350-500 ℃, the pressure is 0.5-2MPa, and the weight hourly space velocity of the liquefied gas is 1-20h -1 The weight ratio of the hydrogen to the liquefied gas is 1:500-2000.
Optionally, in the first aspect, when the fully regenerated desulfurization adsorbent is contacted with the gasoline for passivation, the passivation condition includes: the temperature is 300-550 ℃, the pressure is 0.3-3MPa, and the weight hourly space velocity of the gasoline is 0.1-50h -1 ；
Preferably, in the first aspect, when the fully regenerated desulfurization adsorbent is contacted with the gasoline for passivation, the passivation conditions include: the temperature is 350-500 ℃, the pressure is 0.5-2MPa, and the weight hourly space velocity of the gasoline is 1-10h -1 。
Optionally, in the first mode, the weight ratio of the fully regenerated desulfurization adsorbent to the gasoline is 2-30:1, preferably 5-20:1.
optionally, in the second mode, the weight ratio of the passivated regenerated desulfurization adsorbent to the liquefied gas is 2-60:1, preferably 10-40:1.
optionally, the carbon number of the gasoline is C5-C12; the sulfur content in the gasoline is more than 10 mug/g;
the carbon number of the liquefied gas is C3-C4; the sulfur content in the liquefied gas is more than 10 mug/g;
the hydrogen-containing gas is hydrogen and/or a refinery gas containing hydrogen; preferably, the sulfur content in the hydrogen-containing refinery gas is greater than 10 μg/g.
Optionally, the desulfurization adsorbent comprises a carrier and an active component supported on the carrier; the carrier contains 10 to 90wt% of zinc oxide, 5 to 30wt% of aluminum oxide and 5 to 85wt% of silica based on the total weight of the carrier; the active component accounts for 5-30wt% of the total weight of the desulfurization adsorbent; the active component is one or more oxides selected from cobalt, nickel, iron, manganese, copper, molybdenum, tungsten, silver, tin and vanadium.
Optionally, in the first aspect, the conditions for complete coke burn regeneration include: the temperature is 200-800 ℃, the pressure is 0.1-2.5 MPa, the gas linear velocity of the oxygen-containing gas is 0.1-2.0 m/s, and the consumption of the oxygen-containing gas ensures that the carbon content in the regenerated desulfurization adsorbent is 0.01-1.0 wt%;
preferably, the conditions for the complete char regeneration include: the temperature is 400-600 ℃, the pressure is 0.1-1.5 MPa, and the consumption of the oxygen-containing gas is such that the carbon content in the regenerated desulfurization adsorbent is 0.1-0.5 wt%.
Optionally, in the second mode, the condition of incomplete coke burn regeneration includes: the temperature is 200-800 ℃, the pressure is 0.1-2.5 MPa, the linear velocity of the oxygen-containing gas is 0.1-2.0 m/s, and the amount of the oxygen-containing gas is such that the carbon content in the passivated regenerated desulfurization adsorbent is 0.01-2.0 wt%;
preferably, the conditions for the incomplete coke burn regeneration include: the temperature is 400-600 ℃, the pressure is 0.1-1.5 MPa, and the oxygen-containing gas is used in an amount that the carbon content in the passivated regenerated desulfurization adsorbent is 1.0-1.5 wt%.
Optionally, in the first mode, the completely regenerated desulfurization adsorbent is directly led into the rapid bed desulfurization reactor from the fluidized bed regenerator without reduction to contact with gasoline for passivation;
in the second mode, the passivated regenerated desulfurization adsorbent is directly led into the rapid bed desulfurization reactor from the regenerator without reduction, and is contacted with liquefied gas and gas containing hydrogen to perform adsorption desulfurization reaction.
Through the technical scheme, in the raw oil conversion process, the liquefied gas in the reaction oil gas is subjected to adsorption desulfurization treatment by using the passivated regenerated desulfurization adsorbent, so that a material containing the liquefied gas after desulfurization treatment is obtained, and then the material is subjected to absorption stabilization treatment. Because the activity of the passivated regenerated desulfurization adsorbent is low, the method disclosed by the invention can effectively avoid the conversion of unsaturated olefins in liquefied gas in reaction oil gas into saturated alkanes during desulfurization treatment, and can at least partially improve the yield of unsaturated olefins in liquefied gas while carrying out desulfurization treatment on the liquefied gas, thereby improving the yield of unsaturated olefins in reaction oil gas.
Additional features and advantages of the present disclosure will be set forth in the detailed description which follows.
Drawings
The accompanying drawings are included to provide a further understanding of the disclosure, and are incorporated in and constitute a part of this specification, illustrate the disclosure and together with the description serve to explain, but do not limit the disclosure. In the drawings:
FIG. 1 schematically illustrates a schematic diagram of an apparatus for applying a method according to an embodiment of the present disclosure;
fig. 2 schematically illustrates another apparatus structure for applying the method according to the embodiment of the present disclosure.
Description of the reference numerals
1. Liquefied gas of catalytic cracker 2
3. Gasoline 4 preheating furnace
5. Bubbling bed desulfurization reactor 6 fast bed desulfurization reactor
7. Regenerator 8 lock hopper
Detailed Description
Specific embodiments of the present disclosure are described in detail below with reference to the accompanying drawings. It should be understood that the detailed description and specific examples, while indicating and illustrating the disclosure, are not intended to limit the disclosure.
Fig. 1 and 2 show schematic diagrams of two apparatuses applying the methods according to the embodiments of the present disclosure, respectively. It should be noted that fig. 1 and 2 are only examples of apparatuses to which the methods of the embodiments of the present disclosure may be applied to help those skilled in the art understand the technical content of the present disclosure, but do not mean that the methods of the embodiments of the present disclosure may not be used in other apparatuses, environments, or scenarios.
The device shown in fig. 1 works as follows: in the catalytic cracking unit 1, raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas 2 and gasoline 3 are separated from the reaction oil gas; the liquefied gas 2 is preheated by a preheating furnace 4 and then is led into a bubbling bed desulfurization reactor 5; after the gasoline 3 is preheated by a preheating furnace 4, the gasoline is led into a rapid bed desulfurization reactor 6; transferring the spent desulfurization adsorbent into a regenerator 7 for complete burning regeneration to obtain a complete regenerated desulfurization adsorbent; transferring the obtained completely regenerated desulfurization adsorbent into a rapid bed desulfurization reactor 6, enabling the completely regenerated desulfurization adsorbent to be in contact with gasoline 3, and passivating to obtain a passivated regenerated desulfurization adsorbent; introducing the passivated regenerated desulfurization adsorbent into a bubbling bed desulfurization reactor 5, enabling the regenerated desulfurization adsorbent to be in contact with liquefied gas 2 and gas containing hydrogen in the bubbling bed desulfurization reactor 5, and performing adsorption desulfurization reaction to obtain a reacted material; introducing the gas phase in the reacted material from the top of the bubbling bed desulfurization reactor 5 into a settling section at the upper part of the rapid bed desulfurization reactor 6, and introducing the solid phase in the reacted material from the lower part of the bubbling bed desulfurization reactor 5 into a passivation section at the lower part of the rapid bed desulfurization reactor 6; guiding out a material containing liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor 6, and guiding out a spent desulfurization adsorbent from a passivation section at the lower part of the rapid bed desulfurization reactor 6; and (3) carrying out absorption stabilization treatment on the liquefied gas-containing material after desulfurization treatment, and introducing the spent desulfurization adsorbent into a regenerator 7 through a lock hopper 8 to carry out complete burning regeneration treatment.
The device shown in fig. 2 works as follows: in the catalytic cracking unit 1, raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas 2 is separated from the reaction oil gas; the liquefied gas 2 is preheated by a preheating furnace 4 and then is led into a rapid bed desulfurization reactor 6; transferring the spent desulfurization adsorbent into a regenerator 7 for incomplete burning regeneration to obtain a passivated regenerated desulfurization adsorbent; introducing the passivated regenerated desulfurization adsorbent into a rapid bed desulfurization reactor 6, and contacting the passivated regenerated desulfurization adsorbent with liquefied gas 2 and gas containing hydrogen in the rapid bed reactor 6 to perform adsorption desulfurization reaction to obtain a reacted material; guiding out a material containing liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor 6, and guiding out a spent desulfurization adsorbent from a passivation section at the lower part of the rapid bed desulfurization reactor 6; and (3) carrying out absorption stabilization treatment on the liquefied gas-containing material after desulfurization treatment, and introducing the spent desulfurization adsorbent into a regenerator 7 through a lock hopper 8 to carry out complete burning regeneration treatment.
A first aspect of the present disclosure provides a conversion method of raw oil, the method comprising the steps of: s1, under the catalytic cracking condition, the raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas is separated from the reaction oil gas; s2, carrying out desulfurization treatment on the liquefied gas to obtain a material containing the liquefied gas after desulfurization treatment, and carrying out absorption stabilization treatment on the material containing the liquefied gas after desulfurization treatment; the desulfurization treatment is performed in one or two modes:
mode one: transferring a spent desulfurization adsorbent into a regenerator for complete burning regeneration to obtain a complete regeneration desulfurization adsorbent, separating gasoline from the reaction oil gas, introducing the gasoline into the bottom of a rapid bed desulfurization reactor, contacting the complete regeneration desulfurization adsorbent with the complete regeneration desulfurization adsorbent in the rapid bed desulfurization reactor for passivation to obtain a passivated regeneration desulfurization adsorbent, introducing the passivated regeneration desulfurization adsorbent into a bubbling bed desulfurization reactor, contacting the passivated regeneration adsorbent with liquefied gas and gas containing hydrogen in the bubbling bed desulfurization reactor for adsorption desulfurization reaction to obtain a reacted material, introducing the gas phase in the reacted material into a settling section at the upper part of the rapid bed desulfurization reactor from the top of the bubbling bed desulfurization reactor, introducing the solid phase in the reacted material into a passivation section at the lower part of the rapid bed desulfurization reactor from the lower part of the bubbling bed desulfurization reactor, and guiding the liquefied material containing treated gas from the top of the settling section at the upper part of the rapid bed desulfurization reactor;
mode two: transferring the spent desulfurization adsorbent into a regenerator for incomplete burning regeneration to obtain a passivated regenerated desulfurization adsorbent, introducing the passivated regenerated desulfurization adsorbent into a rapid bed desulfurization reactor, contacting the passivated regenerated desulfurization adsorbent with liquefied gas and hydrogen-containing gas in the rapid bed reactor, performing adsorption desulfurization reaction to obtain reacted materials, and leading out the materials containing the liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor.
In the embodiment of the disclosure, in the conversion process of raw oil, liquefied gas in reaction oil gas is subjected to adsorption desulfurization treatment by using a passivated regenerated desulfurization adsorbent to obtain a material containing the desulfurized liquefied gas, and then the material is subjected to absorption stabilization treatment. Because the passivated regenerated desulfurization adsorbent has low activity, the method disclosed by the invention can effectively avoid that unsaturated olefin (such as C2-C4 olefin, preferably propylene) in liquefied gas in reaction oil gas is converted into saturated alkane (such as C2-C4 alkane, preferably propane) during desulfurization treatment, and can at least partially improve the yield of the unsaturated olefin in the liquefied gas and further improve the yield of the unsaturated olefin in the reaction oil gas when the liquefied gas is subjected to desulfurization treatment.
In addition, in the first mode, the gasoline is utilized to carry out passivation treatment on the completely regenerated desulfurization adsorbent, at least part of sulfides in the gasoline can be removed, the yield of olefins in the gasoline is improved, and the octane number of the gasoline is improved. The embodiment of the disclosure realizes the recycling of the desulfurization adsorbent, and has the advantages of high efficiency and good effect of removing sulfides in the liquefied gas, and no alkaline residue and other wastes are generated in the desulfurization process.
According to the present disclosure, when the passivated regenerated desulfurization adsorbent is subjected to an adsorption desulfurization reaction with liquefied gas and hydrogen-containing gas, the conditions of the adsorption desulfurization reaction may vary within a certain range, for example, the conditions of the adsorption desulfurization reaction may include: the temperature is 200-550deg.C, and the pressure is0.3-3MPa, and the weight hourly space velocity of the liquefied gas is 0.1-50h -1 The weight ratio of the hydrogen to the liquefied gas is 1:100-5000.
Preferably, when the passivated regenerated desulfurization adsorbent is subjected to an adsorption desulfurization reaction with liquefied gas and a gas containing hydrogen, the conditions of the adsorption desulfurization reaction may include: the temperature is 350-500 ℃, the pressure is 0.5-2MPa, and the weight hourly space velocity of the liquefied gas is 1-20h -1 The weight ratio of the hydrogen to the liquefied gas is 1:500-2000. Under the preferred conditions, the embodiment of the disclosure can further avoid the conversion of unsaturated olefins in the liquefied gas into saturated alkanes, which is beneficial to further improving the yield of unsaturated olefins in the liquefied gas.
According to the present disclosure, in the first aspect, when the fully regenerated desulfurization adsorbent is contacted with the gasoline for passivation, the passivation conditions may include: the temperature is 300-550 ℃, the pressure is 0.3-3MPa, and the weight hourly space velocity of the gasoline is 0.1-50h -1 The method comprises the steps of carrying out a first treatment on the surface of the Preferably, in the first aspect, when the fully regenerated desulfurization adsorbent is contacted with the gasoline for passivation, the passivation conditions may include: the temperature is 350-500 ℃, the pressure is 0.5-2MPa, and the weight hourly space velocity of the gasoline is 1-10h -1 。
According to the present disclosure, in the first aspect, the weight ratio of the fully regenerated desulfurization adsorbent to the gasoline may be 2 to 30:1, preferably 5-20:1. in the second mode, the weight ratio of the passivated regenerated desulfurization adsorbent to the liquefied gas may be 2 to 60:1, preferably 10-40:1.
according to the present disclosure, the gasoline may have a carbon number of C5-C12; the sulfur content in the gasoline may be greater than 10 μg/g; the carbon number of the liquefied gas can be C3-C4; the sulphur content in the liquefied gas may be greater than 10 μg/g; the hydrogen-containing gas may be hydrogen and/or a refinery gas containing hydrogen; preferably, the sulfur content in the hydrogen-containing refinery gas may be greater than 10 μg/g.
In the embodiment of the disclosure, the refinery gas containing hydrogen is used as the gas containing hydrogen, so that at least part of sulfides in the refinery gas can be removed, residual hydrogen in the refinery gas is fully utilized, production resources are saved, and production cost is reduced.
According to the present disclosure, the desulfurization adsorbent may contain a carrier and an active component supported on the carrier; the support may contain 10 to 90wt% zinc oxide, 5 to 30wt% aluminum oxide and 5 to 85wt% silica, based on the total weight of the support; the active component can account for 5-30wt% of the total weight of the desulfurization adsorbent; the active component can be an oxide of one or more selected from cobalt, nickel, iron, manganese, copper, molybdenum, tungsten, silver, tin and vanadium.
According to the present disclosure, in the first aspect, the conditions for the complete scorch regeneration may include: the temperature is 200-800 ℃, the pressure is 0.1-2.5 MPa, the gas linear velocity of the oxygen-containing gas is 0.1-2.0 m/s, and the consumption of the oxygen-containing gas ensures that the carbon content in the regenerated desulfurization adsorbent is 0.01-1.0 wt%; preferably, the conditions for the complete char regeneration may include: the temperature is 400-600 ℃, the pressure is 0.1-1.5 MPa, and the consumption of the oxygen-containing gas is such that the carbon content in the regenerated desulfurization adsorbent is 0.1-0.5 wt%.
According to the present disclosure, in the second mode, the condition of the incomplete coke burn regeneration may include: the temperature is 200-800 ℃, the pressure is 0.1-2.5 MPa, the linear velocity of the oxygen-containing gas is 0.1-2.0 m/s, and the amount of the oxygen-containing gas is such that the carbon content in the passivated regenerated desulfurization adsorbent is 0.01-2.0 wt%; preferably, the possible conditions for the incomplete coke burn regeneration include: the temperature is 400-600 ℃, the pressure is 0.1-1.5 MPa, and the oxygen-containing gas is used in an amount that the carbon content in the passivated regenerated desulfurization adsorbent is 1.0-1.5 wt%.
According to the first aspect of the present disclosure, the completely regenerated desulfurization adsorbent may be directly introduced from the fluidized bed regenerator into the rapid bed desulfurization reactor to contact with gasoline without reduction, and be passivated; in the second mode, the passivated regenerated desulfurization adsorbent may be directly introduced from the regenerator into the rapid bed desulfurization reactor without reduction, and contacted with liquefied gas and gas containing hydrogen to perform adsorption desulfurization reaction.
The present disclosure is further illustrated by the following examples, but the present disclosure is not limited thereby.
The desulfurization adsorbent referred to in examples and comparative examples of the present disclosure was FCAS-20 adsorbent, and its chemical composition and physicochemical properties are shown in Table 1, which was produced by China institute of petrochemical and petrochemical industries.
TABLE 1
The gasoline involved in examples and comparative examples of the present disclosure is catalytic gasoline derived from the division company of Yanshan, petrochemical industry, and its composition and physicochemical properties are shown in table 2.
TABLE 2
The liquefied gas referred to in examples and comparative examples of the present disclosure is a catalytically cracked liquefied gas, which is derived from the division company of Yanshan, petrochemical industry, and its composition and physicochemical properties are shown in table 3.
TABLE 3 Table 3
The rapid bed desulfurization reactors referred to in examples and comparative examples of the present disclosure were hollow cylinders having a height of 2.6 m and a diameter of 39 mm, and the upper portions thereof were communicated with a reservoir tank through a 2.4 m long transfer pipe, and the height of the extended distance given position thereof was 1.3 m.
The rapid bed desulfurization reactors referred to in the examples and comparative examples of the present disclosure were of a cylindrical structure having a height of 4 m and a diameter of 39 mm, and the bubbling bed reactor was of a cylindrical structure having a height of 2.6 m and a diameter of 30 mm.
Example 1
This example is intended to illustrate the conversion process of the feedstock oil of the present disclosure, including the following operations.
(1) In a catalytic device, raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas and gasoline are separated from the reaction oil gas;
(2) Preheating liquefied gas in a preheating furnace, and introducing the preheated liquefied gas into a bubbling bed desulfurization reactor; preheating gasoline by a preheating furnace, and then introducing the preheated gasoline into a rapid bed desulfurization reactor;
(3) Transferring the spent desulfurization adsorbent into a regenerator for complete burning regeneration to obtain the complete regenerated desulfurization adsorbent, wherein the conditions of complete burning regeneration comprise: the temperature is 550 ℃, the pressure is 1.0MPa, the gas linear velocity of the oxygen-containing gas is 1.0m/s, and the amount of the oxygen-containing gas is such that the carbon content in the regenerated desulfurization adsorbent is 0.1 wt%;
(4) Transferring the obtained completely regenerated desulfurization adsorbent into a rapid bed desulfurization reactor, enabling the completely regenerated desulfurization adsorbent to be in contact with gasoline, and passivating to obtain passivated regenerated desulfurization adsorbent, wherein the weight ratio of the completely regenerated desulfurization adsorbent to the gasoline is 12: the passivation conditions include: the temperature is 400 ℃, the pressure is 1.0MPa, and the weight hourly space velocity of the gasoline is 2.6h -1 ；
(5) Introducing the passivated regenerated desulfurization adsorbent into a bubbling bed desulfurization reactor, enabling the regenerated desulfurization adsorbent to be in contact with liquefied gas and gas containing hydrogen in the bubbling bed desulfurization reactor, and performing adsorption desulfurization reaction to obtain a reacted material, wherein the adsorption desulfurization reaction conditions comprise: the temperature is 360 ℃, the pressure is 1.0MPa, and the weight hourly space velocity of the liquefied gas is 3.5h -1 The weight ratio of the hydrogen to the liquefied gas is 1:1000;
(6) Introducing the gas phase in the obtained reacted material from the top of the bubbling bed desulfurization reactor into a settling section at the upper part of the rapid bed desulfurization reactor, and introducing the solid phase in the reacted material from the lower part of the bubbling bed desulfurization reactor into a passivation section at the lower part of the rapid bed desulfurization reactor; guiding out a material containing liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor, and guiding out a spent desulfurization adsorbent from a passivation section at the lower part of the rapid bed desulfurization reactor;
(7) Carrying out absorption stabilization treatment on the material containing the liquefied gas after desulfurization treatment; and introducing the spent desulfurization adsorbent into a regenerator through a lock hopper to perform complete coke burning regeneration treatment.
Physical and chemical analysis was performed on the material subjected to the absorption stabilization treatment in this example, and the sulfur content, the olefin content and the octane number were measured, and the measurement results are shown in table 4.
Example 2
The conversion of the feedstock was carried out as in example 1, except that: in step (4), the passivation conditions include: the temperature is 440 ℃, the pressure is 2.0MPa, and the weight hourly space velocity of the gasoline is 1.3h -1 The method comprises the steps of carrying out a first treatment on the surface of the In the step (5), the conditions for the adsorption desulfurization reaction include: the temperature is 400 ℃, the pressure is 2.0MPa, and the weight hourly space velocity of the liquefied gas is 1.8h -1 The weight ratio of the hydrogen to the liquefied gas is 1:1000.
physical and chemical analysis was performed on the material subjected to the absorption stabilization treatment in this example, and the sulfur content, the olefin content and the octane number were measured, and the measurement results are shown in table 4.
Example 3
This example is intended to illustrate the conversion process of the feedstock oil of the present disclosure, including the following operations.
(1) In a catalytic cracking device, raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas is separated from the reaction oil gas;
(2) Preheating liquefied gas in a preheating furnace, and introducing the preheated liquefied gas into a rapid bed desulfurization reactor; transferring the spent desulfurization adsorbent into a regenerator to perform incomplete coking regeneration to obtain a passivated regenerated desulfurization adsorbent, wherein the conditions of the incomplete coking regeneration comprise: the temperature is 530 ℃, the pressure is 0.3MPa, the linear velocity of the oxygen-containing gas is 1.0m/s, and the amount of the oxygen-containing gas is such that the carbon content in the passivated regenerated desulfurization adsorbent is 1.0 wt%;
(3) Introducing the obtained passivated regenerated desulfurization adsorbent into a rapid bed desulfurization reactor, and contacting the passivated regenerated desulfurization adsorbent with liquefied gas and gas containing hydrogen in the rapid bed reactor to perform adsorption desulfurization reaction to obtain reacted materials, wherein the weight ratio of the passivated regenerated desulfurization adsorbent to the liquefied gas is 24: the conditions of the adsorption desulfurization reaction include: the temperature is 400 ℃, the pressure is 1.0MPa, and the weight hourly space velocity of the liquefied gas is 2.6h -1 The weight ratio of the hydrogen to the liquefied gas is 1:1000;
(4) Guiding out the material containing the liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor, and guiding out the spent desulfurization adsorbent from a passivation section at the lower part of the rapid bed desulfurization reactor;
(5) And (3) carrying out absorption stabilization treatment on the material containing the liquefied gas after desulfurization treatment, and introducing a spent desulfurization adsorbent into a regenerator through a lock hopper to carry out incomplete burning regeneration treatment.
Physical and chemical analysis was performed on the material subjected to the absorption stabilization treatment in this example, and the sulfur content and the olefin content were measured, and the measurement results are shown in table 4.
Example 4
The conversion of the feedstock was carried out as in example 3, except that: in the step (3), the conditions for the adsorption desulfurization reaction include: the temperature is 430 ℃, the pressure is 2.0MPa, and the weight hourly space velocity of the liquefied gas is 1.3h -1 The weight ratio of the hydrogen to the liquefied gas is 1:1000.
physical and chemical analysis was performed on the material subjected to the absorption stabilization treatment in this example, and the sulfur content and the olefin content were measured, and the measurement results are shown in table 4.
Comparative example 1
(1) In a catalytic device, raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, liquefied gas and gasoline are separated from the reaction oil gas, and the liquefied gas and the gasoline are preheated by a preheating furnace and then are led into a rapid bed desulfurization reactor;
(2) Transferring the spent desulfurization adsorbent into a regenerator for complete burning regeneration to obtain the complete regenerated desulfurization adsorbent, wherein the conditions of complete burning regeneration comprise: the temperature is 550 ℃, the pressure is 1.0MPa, the gas linear velocity of the oxygen-containing gas is 1.0m/s, and the amount of the oxygen-containing gas is such that the carbon content in the regenerated desulfurization adsorbent is 0.1 wt%;
(3) Transferring the obtained completely regenerated desulfurization adsorbent into a rapid bed desulfurization reactor, enabling the completely regenerated desulfurization adsorbent to be in contact with gasoline, liquefied gas and gas containing hydrogen to perform adsorption desulfurization reaction to obtain reacted materials, wherein the adsorption desulfurization reaction stripsThe piece includes: the temperature is 360 ℃, the pressure is 1.0MPa, and the weight hourly space velocity of the liquefied gas is 3.5h -1 The weight ratio of the hydrogen to the liquefied gas is 1:1000;
(4) Guiding out the material containing the liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor, and guiding out the spent desulfurization adsorbent from a passivation section at the lower part of the rapid bed desulfurization reactor;
(5) Carrying out absorption stabilization treatment on the material containing the liquefied gas after desulfurization treatment; and introducing the spent desulfurization adsorbent into a regenerator through a lock hopper to perform complete coke burning regeneration treatment.
Physical and chemical analysis was performed on the material subjected to the absorption stabilization treatment in this comparative example, and the sulfur content, the olefin content and the octane number were measured, and the measurement results are shown in table 4.
Comparative example 2
(1) In a catalytic cracking device, raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas is separated from the reaction oil gas;
(2) Preheating liquefied gas in a preheating furnace, and introducing the preheated liquefied gas into a rapid bed desulfurization reactor; transferring the spent desulfurization adsorbent into a regenerator for complete burning regeneration to obtain the complete regenerated desulfurization adsorbent, wherein the conditions of complete burning regeneration comprise: the temperature is 550 ℃, the pressure is 1.0MPa, the linear velocity of the oxygen-containing gas is 1.0m/s, and the amount of the oxygen-containing gas is such that the carbon content in the passivated regenerated desulfurization adsorbent is 0.1 wt%;
(3) Introducing the obtained fully regenerated desulfurization adsorbent into a rapid bed desulfurization reactor, and contacting the fully regenerated desulfurization adsorbent with liquefied gas and gas containing hydrogen in the rapid bed reactor to perform adsorption desulfurization reaction to obtain reacted materials, wherein the weight ratio of the fully regenerated desulfurization adsorbent to the liquefied gas is 24: the conditions of the adsorption desulfurization reaction include: the temperature is 400 ℃, the pressure is 1.0MPa, and the weight hourly space velocity of the liquefied gas is 2.6h -1 The weight ratio of the hydrogen to the liquefied gas is 1:1000;
(4) Guiding out the material containing the liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor, and guiding out the spent desulfurization adsorbent from a passivation section at the lower part of the rapid bed desulfurization reactor;
(5) And (3) carrying out absorption stabilization treatment on the material containing the liquefied gas after desulfurization treatment, and introducing a spent desulfurization adsorbent into a regenerator through a lock hopper to carry out complete burning regeneration treatment.
Physical and chemical analysis was performed on the material subjected to the absorption stabilization treatment in this comparative example, and the sulfur content and the olefin content were measured, and the measurement results are shown in Table 4.
Comparative example 3
(1) In a catalytic device, raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas and gasoline are separated from the reaction oil gas;
(2) Preheating liquefied gas in a preheating furnace, and introducing the preheated liquefied gas into a bubbling bed desulfurization reactor; preheating gasoline by a preheating furnace, and then introducing the preheated gasoline into a rapid bed desulfurization reactor;
(3) Transferring quartz sand into a rapid bed desulfurization reactor to be contacted with gasoline, wherein the weight ratio of the quartz sand to the gasoline is 12: the conditions in the rapid bed desulfurization reactor include: the temperature is 400 ℃, the pressure is 1.0MPa, and the weight hourly space velocity of the gasoline is 2.6h -1 ；
(4) Continuously introducing quartz sand into a bubbling bed desulfurization reactor, and enabling the quartz sand to be in contact with liquefied gas and gas containing hydrogen in the bubbling bed desulfurization reactor to obtain reacted materials, wherein the conditions in the bubbling bed desulfurization reactor comprise: the temperature is 360 ℃, the pressure is 1.0MPa, and the weight hourly space velocity of the liquefied gas is 3.5h -1 The weight ratio of the hydrogen to the liquefied gas is 1:1000;
(5) Introducing the gas phase in the obtained reacted material from the top of the bubbling bed desulfurization reactor into a settling section at the upper part of the rapid bed desulfurization reactor, and introducing the solid phase in the reacted material from the lower part of the bubbling bed desulfurization reactor into a passivation section at the lower part of the rapid bed desulfurization reactor; leading out a material containing liquefied gas from the top of a settling section at the upper part of the rapid bed desulfurization reactor, and leading out quartz sand from a passivation section at the lower part of the rapid bed desulfurization reactor;
(6) And (3) carrying out absorption stabilization treatment on the material containing the liquefied gas.
Physical and chemical analysis was performed on the material subjected to the absorption stabilization treatment in this comparative example, and the sulfur content, the olefin content and the octane number were measured, and the measurement results are shown in table 4.
TABLE 4 Table 4
As can be seen from table 4, in the conversion process of raw oil, the present disclosure uses a passivated regenerated desulfurization adsorbent to perform adsorption desulfurization treatment on liquefied gas in reaction oil gas, to obtain a material containing the liquefied gas after desulfurization treatment, and then performs absorption stabilization treatment on the material. Because the activity of the passivated regenerated desulfurization adsorbent is low, the method disclosed by the invention can effectively avoid the conversion of unsaturated olefins in liquefied gas in reaction oil gas into saturated alkanes during desulfurization treatment, and can at least partially improve the yield of unsaturated olefins in the liquefied gas and the octane number of product gasoline while carrying out desulfurization treatment on the liquefied gas, thereby improving the yield of unsaturated olefins in the reaction oil gas and the octane number of the product gasoline.
The preferred embodiments of the present disclosure have been described in detail above with reference to the accompanying drawings, but the present disclosure is not limited to the specific details of the above embodiments, and various simple modifications may be made to the technical solutions of the present disclosure within the scope of the technical concept of the present disclosure, and all the simple modifications belong to the protection scope of the present disclosure.
In addition, the specific features described in the foregoing embodiments may be combined in any suitable manner, and in order to avoid unnecessary repetition, the present disclosure does not further describe various possible combinations.
Moreover, any combination between the various embodiments of the present disclosure is possible as long as it does not depart from the spirit of the present disclosure, which should also be construed as the disclosure of the present disclosure.
Claims (16)
1. A process for converting a feedstock, the process comprising the steps of:
s1, under the catalytic cracking condition, the raw oil is contacted with a catalytic cracking catalyst to obtain reaction oil gas, and liquefied gas is separated from the reaction oil gas;
s2, carrying out desulfurization treatment on the liquefied gas to obtain a material containing the liquefied gas after desulfurization treatment, and carrying out absorption stabilization treatment on the material containing the liquefied gas after desulfurization treatment;
the desulfurization treatment is performed in one or two modes:
mode one: transferring a spent desulfurization adsorbent into a regenerator for complete burning regeneration to obtain a complete regeneration desulfurization adsorbent, separating gasoline from the reaction oil gas, introducing the gasoline into the bottom of a rapid bed desulfurization reactor, contacting the complete regeneration desulfurization adsorbent with the complete regeneration desulfurization adsorbent in the rapid bed desulfurization reactor for passivation to obtain a passivated regeneration desulfurization adsorbent, introducing the passivated regeneration desulfurization adsorbent into a bubbling bed desulfurization reactor, contacting the passivated regeneration adsorbent with liquefied gas and gas containing hydrogen in the bubbling bed desulfurization reactor for adsorption desulfurization reaction to obtain a reacted material, introducing the gas phase in the reacted material into a settling section at the upper part of the rapid bed desulfurization reactor from the top of the bubbling bed desulfurization reactor, introducing the solid phase in the reacted material into a passivation section at the lower part of the rapid bed desulfurization reactor from the lower part of the bubbling bed desulfurization reactor, and guiding the liquefied material containing treated gas from the top of the settling section at the upper part of the rapid bed desulfurization reactor;
mode two: transferring the spent desulfurization adsorbent into a regenerator for incomplete burning regeneration to obtain a passivated regenerated desulfurization adsorbent, introducing the passivated regenerated desulfurization adsorbent into a rapid bed desulfurization reactor, contacting the passivated regenerated desulfurization adsorbent with liquefied gas and hydrogen-containing gas in the rapid bed reactor, performing adsorption desulfurization reaction to obtain a reacted material, and guiding out the material containing the liquefied gas after desulfurization treatment from the top of a settling section at the upper part of the rapid bed desulfurization reactor;
in the first mode, the completely regenerated desulfurization adsorbent is directly led into the rapid bed desulfurization reactor from the fluidized bed regenerator without reduction to contact with gasoline for passivation;
in the second mode, the passivated regenerated desulfurization adsorbent is directly led into the rapid bed desulfurization reactor from the regenerator without reduction, and is contacted with liquefied gas and gas containing hydrogen to perform adsorption desulfurization reaction.
2. The method of claim 1, wherein the conditions of the adsorption desulfurization reaction when the passivated regenerated desulfurization adsorbent is subjected to the adsorption desulfurization reaction with liquefied gas and hydrogen-containing gas include: the temperature is 200-550 ℃, the pressure is 0.3-3MPa, and the weight hourly space velocity of the liquefied gas is 0.1-50h -1 The weight ratio of the hydrogen to the liquefied gas is 1:100-5000.
3. The method of claim 2, wherein the conditions of the adsorption desulfurization reaction when the passivated regenerated desulfurization adsorbent is subjected to the adsorption desulfurization reaction with liquefied gas and hydrogen-containing gas include: the temperature is 350-500 ℃, the pressure is 0.5-2MPa, and the weight hourly space velocity of the liquefied gas is 1-20h -1 The weight ratio of the hydrogen to the liquefied gas is 1:500-2000.
4. The method of claim 1, wherein in the first mode, when the fully regenerated desulfurization adsorbent is contacted with the gasoline for passivation, the passivation conditions include: the temperature is 300-550 ℃, the pressure is 0.3-3MPa, and the weight hourly space velocity of the gasoline is 0.1-50h -1 。
5. The method of claim 4, wherein the partyIn the formula I, when the fully regenerated desulfurization adsorbent is contacted with the gasoline for passivation, the passivation conditions comprise: the temperature is 350-500 ℃, the pressure is 0.5-2MPa, and the weight hourly space velocity of the gasoline is 1-10h -1 。
6. The method of claim 1, wherein in the first mode, the weight ratio of the fully regenerated desulfurization adsorbent to the gasoline is from 2 to 30:1.
7. the method of claim 6, wherein the weight ratio of the fully regenerated desulfurization adsorbent to the gasoline is from 5 to 20:1.
8. the method of claim 1, wherein in the second mode, the weight ratio of the passivated regenerated desulfurization adsorbent to the liquefied gas is from 2 to 60:1.
9. the method of claim 8, wherein the weight ratio of the passivated regenerated desulfurization adsorbent to the liquefied gas is from 10 to 40:1.
10. the method of claim 1, wherein the gasoline has a carbon number of C5-C12; the sulfur content in the gasoline is more than 10 mug/g;
the carbon number of the liquefied gas is C3-C4; the sulfur content in the liquefied gas is more than 10 mug/g;
the hydrogen-containing gas is hydrogen and/or a refinery gas containing hydrogen.
11. The method of claim 10, wherein the sulfur content in the hydrogen-containing refinery-related gas is greater than 10 μg/g.
12. The method of claim 1, wherein the desulfurization adsorbent comprises a carrier and an active component supported on the carrier; the carrier contains 10 to 90wt% of zinc oxide, 5 to 30wt% of aluminum oxide and 5 to 85wt% of silica based on the total weight of the carrier; the active component accounts for 5-30wt% of the total weight of the desulfurization adsorbent; the active component is one or more oxides selected from cobalt, nickel, iron, manganese, copper, molybdenum, tungsten, silver, tin and vanadium.
13. The method of claim 1, wherein in one aspect, the conditions for complete char regeneration comprise: the temperature is 200-800 ℃, the pressure is 0.1-2.5 MPa, the gas linear velocity of the oxygen-containing gas is 0.1-2.0 m/s, and the consumption of the oxygen-containing gas ensures that the carbon content in the regenerated desulfurization adsorbent is 0.01-1.0 wt%.
14. The method of claim 13, wherein the conditions of complete char regeneration comprise: the temperature is 400-600 ℃, the pressure is 0.1-1.5 MPa, and the consumption of the oxygen-containing gas is such that the carbon content in the regenerated desulfurization adsorbent is 0.1-0.5 wt%.
15. The method of claim 1, wherein in mode two, the condition of incomplete coke burn regeneration comprises: the temperature is 200-800 ℃, the pressure is 0.1-2.5 MPa, the linear velocity of the oxygen-containing gas is 0.1-2.0 m/s, and the dosage of the oxygen-containing gas is such that the carbon content in the passivated regenerated desulfurization adsorbent is 0.01-2.0 wt%.
16. The method of claim 15, wherein the conditions of incomplete char regeneration comprise: the temperature is 400-600 ℃, the pressure is 0.1-1.5 MPa, and the oxygen-containing gas is used in an amount that the carbon content in the passivated regenerated desulfurization adsorbent is 1.0-1.5 wt%.
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