CN108587674B - Millisecond pyrolysis-gasification coupling process for heavy oil double-reaction tube semicoke circulating bed - Google Patents
Millisecond pyrolysis-gasification coupling process for heavy oil double-reaction tube semicoke circulating bed Download PDFInfo
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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
- C10G9/00—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils
- C10G9/28—Thermal non-catalytic cracking, in the absence of hydrogen, of hydrocarbon oils with preheated moving solid material
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/46—Gasification of granular or pulverulent flues in suspension
- C10J3/54—Gasification of granular or pulverulent fuels by the Winkler technique, i.e. by fluidisation
- C10J3/56—Apparatus; Plants
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
- C10J3/723—Controlling or regulating the gasification process
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
- C10J3/82—Gas withdrawal means
- C10J3/84—Gas withdrawal means with means for removing dust or tar from the gas
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0956—Air or oxygen enriched air
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0959—Oxygen
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0953—Gasifying agents
- C10J2300/0973—Water
- C10J2300/0976—Water as steam
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J2300/00—Details of gasification processes
- C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
- C10J2300/1807—Recycle loops, e.g. gas, solids, heating medium, water
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Abstract
The invention provides a millisecond pyrolysis-gasification coupling process for a semicoke circulating bed of a heavy oil double-reaction tube. Spraying preheated heavy oil into the upper part of the descending reaction tube from a feed inlet of the descending reaction tube by using a high-efficiency atomizing nozzle, and mixing, heating, vaporizing and pyrolyzing the oil mist and high-temperature semicoke millisecond flowing down from a return feeder; after oil gas and coking, semicoke flows downwards to a gas-solid quick separator at the bottom of the descending reaction tube at a high speed for gas-solid separation; oil gas enters a fractionating tower for separation, oil slurry returns to be mixed with heavy oil for recycling, and the rest oil is output as a product; after coking, the semicoke enters the lower part of the riser gasification reactor to perform gasification reaction with oxidant and steam, and the generated synthesis gas and high-temperature semicoke flow upwards to a graded gas-solid separator at the top of the riser gasification reactor to perform gas-solid separation; the large and medium particle high-temperature semicoke flows into the top of the descending reaction pipe to participate in circulation and cracking of heavy oil, the medium and small particles return to the lower part of the riser gasification reactor through the circulating pipe to continuously participate in gasification reaction, and the synthesis gas is output as a product after heat exchange.
Description
1. Field of the invention
The invention provides a millisecond pyrolysis-gasification coupling process for a semicoke circulating bed of a heavy oil double-reaction tube, belonging to the field of heavy oil processing.
2. Background of the invention
The lightening of heavy oil is one of the important problems in petroleum processing in all countries of the world today. The residual oil content in most crude oil in China is high, the light oil content is low, and in recent years, the heavy oil (heavy oil) yield is continuously increased and the problem of light oil is more prominent due to the introduction of part of foreign heavy crude oil. The heavy oil processing method is usually catalytic cracking, solvent deasphalting, viscosity reduction, coking, thermal cracking, heavy oil hydrogenation and other methods, in general, the method is not limited to hydrogenation and decarburization, wherein the heavy oil decarburization processing is the main mode of petroleum refining at present, and the reasonable utilization of decarburization is not solved all the time. The heavy oil solid phase carrier circulating cracking process mainly comprises heavy oil catalytic cracking, flexible coking, fluid coking, heavy oil fluid modification and the like. The catalytic cracking of heavy oil is carried out, except for the obtained target products (gasoline, diesel oil and olefin chemical raw materials), the removed carbon residue is combusted in a regenerator to release heat, one part of the heated catalyst is used as a heat source for cracking, one part of the heated catalyst is used for heating by a heat collector to generate steam to be sent out or generate electricity, the reaction temperature is lower by about 500-650 ℃, the requirements on the content of the carbon residue and heavy metals of the heavy oil raw material are higher, and the poor-quality heavy oil is difficult to meet the requirements; the reaction temperature of the flexible coking and the fluid coking of the inferior heavy oil is low, about 450-600 ℃, the coking gasoline, the diesel oil and the coking wax oil used as a catalytic raw material are mainly produced, the coke combustion part is circulated as a heat carrier, and the part is gasified to produce synthesis gas, but the cracking time is too long, and the yield of light oil is low; the inferior heavy oil fluidization modification (such as ART process developed by Engerhardd, HCC process of Luoyang petrochemical institute, etc.) adopts the circulating fluidized bed technology similar to the heavy oil catalytic cracking process, the reaction temperature is about 400-600 ℃, the cracking time is short, the yield of light oil is higher, but the popularization and application are limited due to excessive carbon residue removal amount and difficult external heat extraction design.
In addition, as the national environmental protection requirements are higher and higher, petroleum refining enterprises need a large amount of hydrogen to hydrofining light oil products so as to produce qualified vehicle fuels, but at present, each refining enterprise is lack of a large amount of cheap hydrogen sources.
How to use heavy oil most economically, most cleanly, most reasonably and maximally and realize no slag is a major problem to be solved by petroleum workers in China.
3. Summary of the invention
The invention aims to overcome the defects of the existing heavy oil processing technology and develop a millisecond pyrolysis-gasification coupling process of a heavy oil double-reaction-tube semicoke circulating bed, which can produce light oil products, can obtain a large amount of cheap hydrogen resources and realize no slag in heavy oil processing.
The technical scheme of the invention is as follows:
the invention aims to produce light oil products by pyrolyzing heavy oil by semicoke through double-pipe circulation, gasify the semicoke part after coking to produce synthesis gas to prepare hydrogen, solve the problem of excessive heat of combustion regeneration circulation of a semicoke riser by utilizing steam gasification heat absorption, and realize no slag in heavy oil processing. The method is characterized in that heavy oil preheated to 180-350 ℃ is sprayed into the upper part of a descending reaction tube from a feed inlet of the descending reaction tube by a high-efficiency atomizing nozzle, and oil mist is mixed, heated, vaporized and pyrolyzed with 800-1100 ℃ high-temperature semi-coke millisecond flowing from a double-control return feeder; after oil gas and coking, semicoke flows downwards to a gas-solid quick separator at the bottom of the descending reaction tube at a high speed for gas-solid separation; oil gas enters a fractionating tower from a pyrolysis gas outlet for separation, oil slurry returns to be mixed with heavy oil for recycling, and other pyrolysis gasoline and diesel oil, liquefied gas and pyrolysis dry gas are output as intermediate products; after being stripped, the coked semicoke enters the lower part of the lifting pipe gasification reactor through a flow controller to perform gasification reaction with oxidant and steam, and after the reaction temperature is 850-1200 ℃, the generated synthesis gas and high-temperature semicoke flow upwards at high speed to a synthesis gas fractional separator at the top of the lifting pipe gasification reactor to perform gas-solid separation; and the separated large and medium particle high-temperature semicoke flows into a double-regulation return feeder, part of the high-temperature large and medium particle semicoke flows into the top of a descending reaction tube according to the tar ratio of 1-10 to participate in circulation and cracking of heavy oil, the rest of the large and medium particle semicoke and medium and small particle semicoke powder returns to the lower part of a riser gasification reactor through a circulating tube to continuously participate in gasification reaction, and the synthesis gas is output as a product after heat exchange, so that the slag-free processing of the heavy oil is realized.
The oxidant is oxygen, air or oxygen-enriched air, preferably oxygen.
The synthesis gas grading separator is one or a combination of more of an inertial separator, a horizontal inertial cyclone separator and a vertical cyclone separator.
The present invention will be described in detail with reference to examples.
4. Description of the drawings
FIG. 1 is a schematic process diagram of the present invention.
The drawing of FIG. 1 is set forth below:
1. the system comprises a synthesis gas grading separator, 2, a double-control return feeder, 3, a high-efficiency atomizing nozzle, 4, a descending reaction tube, 5, a gas-solid quick separator, 6, a pyrolysis gas outlet, 7, a flow regulator, 8, a steam inlet, 9, an oxidant inlet, 10, a lift tube gasification reactor, 11, a heat exchanger, 12, a synthesis gas outlet, 13, a circulating tube
The process features of the present invention are described in detail below with reference to the accompanying drawings and examples.
5. Detailed description of the preferred embodiments
In the embodiment 1, the high-efficiency atomizing nozzle (3) sprays heavy oil preheated to 180-350 ℃ into the upper part of the descending reaction tube (4) from a feed inlet of the descending reaction tube (4), oil mist is mixed, heated, vaporized and pyrolyzed with 800-1100 ℃ high-temperature semi-coke millisecond flowing from the double-control return feeder (2), and the pyrolysis reaction temperature is 480-850 ℃; after oil gas and coking, semicoke flows downwards to a gas-solid rapid separator (5) at the bottom of the descending reaction tube (4) at a high speed for gas-solid separation; oil gas enters a fractionating tower from a pyrolysis gas outlet (6) for separation, oil slurry returns to be mixed with heavy oil for recycling, and other pyrolysis gasoline, diesel oil, liquefied gas and pyrolysis dry gas are output as intermediate products; after coking, semi-coke enters the lower part of a lifting pipe gasification reactor (10) through a flow regulator (7) after steam stripping to perform gasification reaction with oxygen and water vapor entering from a steam inlet (8) and an oxidant inlet (9), the reaction temperature is 850-1200 ℃, and the generated synthesis gas and the high-temperature semi-coke flow upwards at a high speed to a synthesis gas fractional separator (1) at the top of the lifting pipe gasification reactor (10) to perform gas-solid separation; separated large and medium particle high-temperature semicoke flows into a double-regulation return feeder (2), part of the high-temperature large and medium particle semicoke flows into the top of a descending reaction pipe (4) according to the tar ratio of 1-10 to participate in circulation and cracking of heavy oil, the rest of large and medium particle semicoke and medium and small particle semicoke powder returns to the lower part of a riser gasification reactor (10) through a circulating pipe (13) to continuously participate in gasification reaction, and the synthesis gas is subjected to heat exchange through a heat exchanger (11) and then is output as a product from a synthesis gas outlet (12), so that the slag-free processing of the heavy oil is realized.
Example 2 the oxygen in example 1 was changed to oxygen enriched air, and the rest were the same.
In example 3, the oxygen gas in example 1 was replaced with air, and the rest was the same.
According to the millisecond pyrolysis-gasification coupling process for the semicoke circulating bed of the heavy oil double-reaction tube, through semicoke double-tube circulation, 20% of residual carbon heavy oil is pyrolyzed quickly at high temperature and ultrashort contact by using the descending reaction tube to produce light oil, and the yield of the light oil is relatively improved by more than 10 percent; the lift pipe gasification reactor is used for gasifying the coke part to produce the synthesis gas to prepare hydrogen, the steam gasification heat absorption is used for solving the problem of surplus heat of semicoke combustion circulation, the equipment structure is simple, and the coking strength is high; the semicoke, high-temperature steam and an oxidant are subjected to riser gasification regeneration to produce synthesis gas to prepare hydrogen, and the problem that the coke gasification regeneration rate is not matched with the coke production rate of heavy oil cracking is solved through the returning material circulation gasification of a part of large and medium particle semicoke and medium and small particle semicoke powder circulation pipe; the hydrogen cost is greatly reduced (about 50%), the gasification intensity is high, the equipment volume is small, the steel consumption is low, and the fixed investment is greatly reduced; the normal pressure operation is simple, the start and stop are convenient, the continuity is good, and the oil type adaptability is strong; the petroleum resource is fully and effectively utilized, and the slag-free processing of the heavy oil is realized.
Claims (3)
1. The millisecond pyrolysis-gasification coupling process for the semicoke circulating bed of the heavy oil double reaction tubes is technically characterized in that heavy oil preheated to 180-350 ℃ is sprayed into the upper part of a descending reaction tube from a feed inlet of the descending reaction tube by an atomizing nozzle, oil mist is mixed, heated, vaporized and pyrolyzed with high-temperature semicoke millisecond of 800-1100 ℃ flowing from a double-control return feeder, and the pyrolysis reaction temperature is 480-850 ℃; after oil gas and coking, semicoke flows downwards to a gas-solid quick separator at the bottom of the descending reaction tube at a high speed for gas-solid separation; oil gas enters a fractionating tower from a pyrolysis gas outlet for separation, oil slurry returns to be mixed with heavy oil for recycling, and other pyrolysis gasoline and diesel oil, liquefied gas and pyrolysis dry gas are output as intermediate products; after being stripped, the coked semicoke enters the lower part of a lifting pipe gasification reactor through a flow controller to perform gasification reaction with an oxidant and steam, the reaction temperature is 850-1200 ℃, and the generated synthesis gas and the high-temperature semicoke flow upwards at high speed to a synthesis gas fractional separator at the top of the lifting pipe gasification reactor to perform gas-solid separation; and the separated large and medium particle high-temperature semicoke flows into a double-regulation return feeder, part of the high-temperature large and medium particle semicoke flows into the top of a descending reaction tube according to the tar ratio of 1-10 to participate in circulation and cracking of heavy oil, the rest of the large and medium particle semicoke and medium and small particle semicoke powder returns to the lower part of a riser gasification reactor through a circulating tube to continuously participate in gasification reaction, and the synthesis gas is output as a product after heat exchange, so that the slag-free processing of the heavy oil is realized.
2. The coupled process for millisecond pyrolysis-gasification of a circulating bed of semi-coke in a heavy oil double reaction tube as claimed in claim 1, wherein the oxidant is one of oxygen, air and oxygen-enriched air.
3. The millisecond pyrolysis-gasification coupled process of the circulating bed of semicoke in the heavy oil double reaction tube as claimed in claim 1, wherein the syngas classifier is one or more of a combination of a horizontal inertial cyclone separator and a vertical cyclone separator.
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| CN112538381B (en) | 2019-09-23 | 2022-02-25 | 中国石油大学(北京) | Method and device for co-production of heavy oil lightening and synthesis gas |
| CN112538372B (en) | 2019-09-23 | 2022-02-22 | 中国石油大学(北京) | Integrated method and device for co-producing synthesis gas by catalytic cracking of heavy oil |
| CN112538382B (en) * | 2019-09-23 | 2022-02-22 | 中国石油大学(北京) | Integrated method and device for heavy oil catalytic cracking coupled coke catalytic gasification |
| CN112538370B (en) | 2019-09-23 | 2022-02-25 | 中国石油大学(北京) | Method and device for coupling hydro-pressurized catalytic cracking of heavy oil with coke gasification |
| CN112538376B (en) * | 2019-09-23 | 2022-02-25 | 中国石油大学(北京) | Integrated method and device for heavy oil cracking coupling coke catalytic gasification |
| CN112538367B (en) | 2019-09-23 | 2022-02-22 | 中国石油大学(北京) | Heavy oil cracking-gasification coupling reaction device |
| WO2021118741A1 (en) * | 2019-12-11 | 2021-06-17 | Exxonmobil Chemical Patents Inc. | Processes and systems for converting a hydrocarbon-containing feed |
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| CN102559240A (en) * | 2012-01-17 | 2012-07-11 | 马俊杰 | Dual-cycle mode catalytic cracking reaction regenerative system production technology and device |
| CN102965138A (en) * | 2012-11-16 | 2013-03-13 | 中国石油大学(华东) | Double-reaction-tube semi-coke circulating bed pyrolysis, gasification and coupling process of heavy oil |
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| US9187700B2 (en) * | 2012-01-13 | 2015-11-17 | United Technologies Corporation | Method for reducing coke deposition |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN102559240A (en) * | 2012-01-17 | 2012-07-11 | 马俊杰 | Dual-cycle mode catalytic cracking reaction regenerative system production technology and device |
| CN102965138A (en) * | 2012-11-16 | 2013-03-13 | 中国石油大学(华东) | Double-reaction-tube semi-coke circulating bed pyrolysis, gasification and coupling process of heavy oil |
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