CN114854454A - Self-heating coal supercritical water thermochemical reduction hydrogen production reactor and method - Google Patents
Self-heating coal supercritical water thermochemical reduction hydrogen production reactor and method Download PDFInfo
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- CN114854454A CN114854454A CN202210454070.9A CN202210454070A CN114854454A CN 114854454 A CN114854454 A CN 114854454A CN 202210454070 A CN202210454070 A CN 202210454070A CN 114854454 A CN114854454 A CN 114854454A
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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
- C10J3/725—Redox processes
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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
- C10J2300/0913—Carbonaceous raw material
- C10J2300/093—Coal
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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
- C10J2300/16—Integration of gasification processes with another plant or parts within the plant
- C10J2300/1603—Integration of gasification processes with another plant or parts within the plant with gas treatment
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/54—Improvements relating to the production of bulk chemicals using solvents, e.g. supercritical solvents or ionic liquids
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Abstract
The invention provides a self-heating supercritical water thermochemical reduction hydrogen production reactor and a method for coal, comprising the following steps: the reaction section main body is internally and coaxially provided with a partition plate in a tubular structure; the lower end of the clapboard is arranged in a sealing way, and the upper end of the clapboard is arranged in an opening way; the lower end of the clapboard is connected with an outlet pipe of the oxidation section; the bottom of the reaction section main body is connected with a lower end cover, and the top of the reaction section main body is connected with an upper end cover; the lower end cover is provided with a supercritical water inlet, the upper end cover is provided with an oxygen adding pipe, and the oxygen adding pipe extends into the partition plate; the middle lower part of the reaction section main body is provided with a charging pipe for charging coal slurry. The invention integrates gasification and oxidation by a reactor in the form of a sleeve, the annular area formed by the outside of the clapboard and the main body of the reaction section is a gasification area, the inside of the clapboard is an oxidation area, and the two areas are communicated at the opening at the upper end of the clapboard. The heat released by the reaction in the oxidation zone is transferred to the gasification zone through the partition plate, so that the coupling self-heating of gasification and hydrogen oxidation is realized, and the economic investment of external heating equipment is reduced.
Description
Technical Field
The invention belongs to the field of clean conversion and utilization of coal and renewable resources, and particularly relates to a gasification and hydrogen oxidation coupled self-heating coal supercritical water thermal chemical reduction hydrogen production reactor and a method.
Background
In the current energy structure of China, the proportion of coal in primary energy is still higher than 60%. The traditional coal utilization mode and the existing large-scale clean coal utilization technology can not generate a large amount of dust and NO inevitably x 、SO x And the like. The supercritical water gasification technology utilizes the excellent physical and chemical properties of supercritical water to discharge N, S compounds in the coal in a liquid phase form, thereby fundamentally preventing NO x 、SO x And the like.
In the past decades, numerous scholars at home and abroad carry out a great deal of research on the supercritical water gasification technology, so that the technology is rapidly developed. The supercritical water deep ploughing technology in a multi-phase flow national key laboratory of power engineering of the university of Sian traffic for many years obtains pioneering achievements in the fields of reactor design, disclosure of gasification mechanism, screening and preparation of catalysts, industrial scale amplification of systems and the like, and applies or authorizes a large number of patents. In 2007, a coal and biomass supercritical water fluidized bed gasification/partial oxidation hydrogen production device and method (ZL200710017691.6) are invented, the problems of low material heating rate, reactor slagging and blockage and the like of a tubular reactor are solved, and high-concentration biomass efficient gasification is achieved. In 2016, the invention provides the device and the method (ZL201610570689.0) for online discharging the residue in the supercritical water gasification furnace, so that the successful slag discharge of the supercritical water gasification furnace is realized, and the continuous and stable operation of the gasification furnace is not influenced. However, the gasification reaction is an endothermic process, and requires a large amount of heat to be added to maintain the temperature required for the gasification reaction. Therefore, the laboratory also proposes a technical route of coal gasification before oxidation: coal is gasified in supercritical water to produce H 2 Introducing oxygen into the mixture, oxidizing the combustible gas in supercritical water, and oxidizing to release great amount of combustible gasThe heat can provide heat for the gasification and the system. In 2018, a system and a method (201810509004.0) for measuring the combustion characteristics of hydrogen in a supercritical mixed working medium are applied, the combustion rate of the hydrogen in the supercritical mixed working medium under different conditions is measured, the kinetic parameters of the reaction are obtained, and the method has important guiding significance for the coupling design of gasification-oxidation reaction.
Although the supercritical water gasification technology has the advantages of high gasification rate, high hydrogen content of products, strong adaptability of coal types and the like, and is developed greatly in the past decades, the traditional electric heating and novel solar heating modes are adopted to supply heat for gasification reaction, equipment and operation investment are increased, and the industrial popularization of the technology is restricted. However, the current research on gasification-oxidation coupling technology is mainly divided into a gasification reactor and an oxidation reactor, and the design of separating the two reactors causes high material cost and insufficient integration level of the reactors.
Disclosure of Invention
The invention aims to overcome the problems and provide an autothermal coal supercritical water thermochemical reduction hydrogen production reactor and a method, so that gasification and hydrogen oxidation are coupled for self-heating, and the economic investment of external heating equipment is reduced.
The invention is realized by the following technical scheme:
an autothermal coal supercritical water thermochemical reduction hydrogen production reactor comprising: the reaction section main body is internally and coaxially provided with a partition plate in a tubular structure; the lower end of the clapboard is arranged in a sealing way, and the upper end of the clapboard is arranged in an opening way; the lower end of the clapboard is connected with an outlet pipe of the oxidation section;
the bottom of the reaction section main body is connected with a lower end cover, and the top of the reaction section main body is connected with an upper end cover; the lower end cover is provided with a supercritical water inlet, the upper end cover is provided with an oxygen adding pipe, and the oxygen adding pipe extends into the partition plate; the middle lower part of the reaction section main body is provided with a charging pipe for charging coal slurry.
Preferably, the upper end and the lower end of the baffle plate extend out of the main body of the reaction section.
Preferably, the oxygen adding pipes are arranged in a plurality, and the depth of each oxygen adding pipe extending into the partition board is different.
Furthermore, the depth of each oxygen adding pipe extending into the partition plate is gradually increased according to equal intervals.
Furthermore, each oxygenation pipe is evenly arranged on the circumference coaxial with the partition plate.
Furthermore, the outlets of the oxygen adding pipes are all horizontally directed to the axis of the partition plate.
Preferably, the upper end and the lower end of the clapboard are connected with the reaction section main body through ribs.
Preferably, the lower end of the reaction section main body is provided with a slag discharge conduit.
Preferably, the thickness of the partition plate is 2-5 mm.
A self-heating coal supercritical water thermal chemical reduction hydrogen production method is based on the reactor, supercritical water is added into a reaction section main body from a supercritical water inlet, normal temperature coal slurry is added into the reaction section main body from a feeding pipe, and oxygen is introduced into a partition plate from an oxygen adding pipe; supercritical water rises along an annular gasification area formed by the partition plate and the reaction section main body, is mixed with normal-temperature coal slurry and flows into coal particles to carry out supercritical water gasification of the coal slurry and generate mixed liquid rich in hydrogen; the mixed liquor turns to enter an oxidation zone in the clapboard when continuously rising to the upper end cover, and generates oxidation reaction with oxygen, and finally flows out of the reactor through an outlet pipe of the oxidation section.
Compared with the prior art, the invention has the following beneficial effects:
the invention integrates gasification and oxidation by a reactor in the form of a sleeve, the annular area formed by the outside of the clapboard and the main body of the reaction section is a gasification area, the inside of the clapboard is an oxidation area, and the two areas are communicated at the opening at the upper end of the clapboard. The heat released by the reaction in the oxidation zone is transferred to the gasification zone through the partition plate, so that the coupling self-heating of gasification and hydrogen oxidation is realized, and the economic investment of external heating equipment is reduced. The invention integrates the gasification reactor and the oxidation reactor into one reactor, thereby reducing the material cost of the reactor, improving the integration level of the reactor and saving the space.
Furthermore, the depths of the oxygen adding pipes inserted into the oxidation zone are different, so that the staged gradual oxygen adding of the oxidation zone can be realized, and the purpose of controllable and complete oxidation of gasification products is achieved. And the temperature of the gasification zone and the oxidation zone in the reactor can be directionally regulated and controlled by regulating the oxygen inlet position and flow of the oxidant and the flow of the coal slurry.
Furthermore, the outlet of each oxygen adding pipe horizontally points to the axis of the partition plate, so that the oxidant and the gasified mixed liquid can be fully mixed, and the uniform oxidation of the gasified product can be realized.
Furthermore, the upper end of the partition plate is opened, so that the pressure of the inner side oxidation area and the outer side annular gasification area of the partition plate is balanced, the partition plate only needs to bear high temperature and does not need to bear pressure, and therefore the partition plate can be made of thin sheets, materials can be saved, the heat conduction and heat resistance of the partition plate can be reduced, the heat released by the inner side oxidation reaction of the partition plate can be conducted to the outer side gasification area, and the gasification of coal slurry is supported.
According to the method, supercritical water enters the reactor from a supercritical water inlet, and because the lower end of the partition plate is sealed, the supercritical water rises along an annular gasification area formed by the partition plate and the reaction section main body and is mixed with normal-temperature coal slurry entering the reactor through the feeding pipe. The supercritical water fluidizes coal particles in the annular drainage basin, so that the coal slurry is heated rapidly, and the supercritical water gasification of the coal slurry is carried out to generate CO and CH 4 、H 2 And the like. The mixed liquid continuously rises, because the upper end cover is sealed, the mixed liquid turns to and enters the oxidation zone in the partition plate, and is subjected to oxidation reaction with the oxidant entering through the oxygen adding pipe, and the released heat is conducted to the annular gasification zone through the partition plate, so that the coupling self-heating of gasification and hydrogen oxidation is realized, and the economic investment of external heating equipment is reduced.
Drawings
FIG. 1 is a structural diagram of a self-heating coal supercritical water thermal chemical reduction hydrogen production reactor with gasification and hydrogen oxidation coupled according to the present invention;
FIG. 2 is a schematic view of the circumferential installation structure of the partition plate and the main body of the reaction section in FIG. 1;
FIG. 3 is an enlarged view of an upper portion of the reactor of FIG. 1;
fig. 4 is a plan view of the circumferential position of the oxygen adding pipe and the partition plate in fig. 1.
The reference numbers in the figures are: 1-reaction section main body, 2-lower end cover, 3-slag discharge conduit, 4-charging pipe, 5-upper end cover, 6-oxygenation pipe, 7-clapboard, 8-oxidation section outlet pipe, 21-supercritical water inlet, 22-air distribution plate and 71-rib.
Detailed Description
For a further understanding of the invention, reference will now be made to the following examples, which are provided to illustrate further features and advantages of the invention, and are not intended to limit the scope of the invention as set forth in the following claims.
As shown in figure 1, the gasification and hydrogen oxidation coupled self-heating coal supercritical water thermal chemical reduction hydrogen production reactor comprises a reaction section main body 1, a partition plate 7 in a tubular structure is coaxially arranged in the reaction section main body 1, the lower end of the partition plate 7 is sealed, the upper end of the partition plate 7 is opened, an annular area between the partition plate 7 and the reaction section main body 1 forms a gasification area, and an oxidation area is arranged in the partition plate 7. An oxidation section outlet pipe 8 is connected to the lower right part of the baffle 7.
Referring to fig. 3 and 2, in one embodiment, the partition 7 extends beyond the main body 1 at both the upper and lower ends thereof. The oxidation zone at the inner side of the clapboard 7 is communicated with the gasification zone at the outer side of the reactor, the pressure at the inner side and the outer side of the clapboard 7 is balanced, and the clapboard can be made of thin plates with the thickness of 2-5 mm. The partition plate is made of the thin plate, so that materials can be saved, the heat conduction and heat resistance of the partition plate can be reduced, the heat released by oxidation reaction on the inner side of the partition plate can be conducted to an outer gasification area, and the gasification of coal slurry is supported.
The upper and lower ends of the partition 7 are connected to the main body of the reaction section by ribs 71. Referring to fig. 2, in the embodiment of the present invention, the partition plate 7 is in a circular tube shape and is coaxially arranged with the reaction section main body 1, and the upper and lower ends of the partition plate 7 are respectively welded to the inner wall of the reaction section main body through 3 ribs uniformly arranged in the circumferential direction.
The lower end of the reaction section main body 1 is connected with a lower end cover 2, and the upper end is connected with an upper end cover 5. The lower end cover 2 is provided with a supercritical water inlet 21, the upper end cover 5 is provided with an oxygen adding pipe 6, and the oxygen adding pipe 6 extends into the clapboard 7.
Referring to fig. 3, the oxygen adding pipe 6 is directly welded to the upper end cap. Preferably, a plurality of oxygen adding pipes 6 can be arranged, the depths of the oxygen adding pipes 6 extending into the partition plate 7 are respectively different, and the intervals are equal (namely, the depths of the oxygen adding pipes 6 extending into the partition plate 7 are gradually increased according to equal intervals), so that the staged gradual oxygen adding in the oxidation zone can be realized, and the purpose of controllable and complete oxidation of gasification products is achieved. And the temperature of the gasification zone and the oxidation zone in the reactor can be directionally regulated and controlled by regulating the oxygen inlet position and flow of the oxidant and the flow of the coal slurry.
Referring to fig. 4, the oxygenation tubes 6 are positioned in a circular tube formed by the partition plates 7, and are uniformly arranged on a circumference with a certain diameter, and the circumference is coaxial with the partition plates 7. The outlet of each oxygen adding pipe 6 points horizontally to the axis of the clapboard 7.
The lower end of the main body 1 of the reaction section is provided with a slag discharge conduit 3 from which solid phase residue formed in the reaction process is discharged out of the reactor. The middle lower part of the reaction section main body 1 is provided with a feed pipe 4, and the feed pipe 4 is connected with a coal slurry feeder.
The upper end cover 5 comprises a second clamping plate, an upper end cover upper end, an upper end cover lower end, a second gasket and a second bolt, the upper end cover upper end and the upper end cover lower end are fixedly connected through the second clamping plate, the second gasket is arranged between a step surface of the upper end cover and the inner surface of the second clamping plate, and the second bolt penetrates through the second clamping plate to tightly push the second gasket. The lower end of the upper end cover is welded with the upper end of the reaction section main body 1.
The lower end cover 2 comprises a first clamping plate, an upper end of the lower end cover, a lower end of the lower end cover, a first gasket and a first bolt, the upper end of the lower end cover and the lower end of the lower end cover are fixedly connected through the clamping plate, the gasket is arranged between a step surface of the lower end cover and the inner surface of the clamping plate, and the bolt penetrates through the clamping plate to tightly push the gasket. An air distribution plate 22 is arranged between the upper end of the lower end cover and the lower end of the lower end cover. The upper end of the lower end cover is welded with the lower end of the reaction section main body 1. And a through hole for the outlet pipe 8 of the oxidation section to penetrate out is arranged on the side wall of the upper end of the lower end cover.
The structural design of the end cover of the invention facilitates the disassembly and cleaning of the reactor.
The invention relates to a gasification and hydrogen oxidation coupled self-heating coal supercritical water thermal chemical reduction hydrogen production reactor, which comprises the following working processes: at the beginning of the experiment, supercritical water heated to 700 ℃ enters the lower end cover 2 from the supercritical water inlet 21 and then enters the reactor through the lower cover cloth air plate 22. Because the lower end of the clapboard 7 is sealed,supercritical water rises along an annular gasification area formed by the partition plates 7 and the reaction section main body 1 and is mixed with normal-temperature coal slurry entering the reactor through the feed pipe 4. The supercritical water fluidizes coal particles in the annular drainage basin, so that the coal slurry is heated rapidly, and the supercritical water gasification of the coal slurry is carried out to generate CO and CH 4 、H 2 And the like. The mixed liquid continuously rises, because the upper end cover is sealed, the mixed liquid turns to enter an oxidation zone in the partition plate 7, partial hydrogen in the mixed liquid and an oxidant entering through the oxygen adding pipe 6 are subjected to oxidation reaction, and released heat is conducted to the annular gasification zone through the partition plate 7, so that the coupling self-heating of gasification and hydrogen oxidation is realized. And finally, the mixed liquid flows out of the reactor through an outlet pipe of the oxidation section at the lower end, and enters a downstream device for heat recovery, separation and analysis of products. The residue generated in the operation process is discharged through the slag discharge conduit.
The invention adopts the reactor in the form of a sleeve, integrates the originally separated gasification reactor and the oxidation reactor into one reactor, reduces the material cost of the reactor, ensures that the integration level of the reactor is higher, and saves the space. Meanwhile, the oxidation zone can support the reaction of the gasification zone as an internal heat source, so that energy self-coupling is realized, and the investment of external heating equipment and the power consumption of an external heat source are reduced.
The above examples are merely illustrative of the present invention and are not intended to limit the present invention. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. A self-heating coal supercritical water thermal chemical reduction hydrogen production reactor is characterized by comprising: the reaction section comprises a reaction section main body (1), wherein a partition plate (7) in a tubular structure is coaxially arranged in the reaction section main body (1); the lower end of the clapboard (7) is arranged in a sealing way, and the upper end is arranged in an opening way; the lower end of the clapboard (7) is connected with an outlet pipe (8) of the oxidation section;
the bottom of the reaction section main body (1) is connected with a lower end cover (2), and the top is connected with an upper end cover (5); a supercritical water inlet (21) is arranged on the lower end cover (2), an oxygen adding pipe (6) is arranged on the upper end cover (5), and the oxygen adding pipe (6) extends into the partition plate (7); the middle lower part of the reaction section main body (1) is provided with a feed pipe (4) for feeding coal slurry.
2. The reactor for hydrogen production by supercritical water thermochemical reduction of coal as per claim 1, wherein the upper and lower ends of the partition (7) are extended out of the main body (1) of the reaction section.
3. The self-heating coal supercritical water thermal chemical reduction hydrogen production reactor according to claim 1, characterized in that a plurality of oxygen adding pipes (6) are provided, and the depth of each oxygen adding pipe (6) extending into the partition (7) is different.
4. The self-heating coal supercritical water thermal chemical reduction hydrogen production reactor according to claim 3, characterized in that the depth of each oxygen adding pipe (6) extending into the baffle (7) is gradually increased at equal intervals.
5. The autothermal coal supercritical water thermal chemical reduction hydrogen production reactor of claim 3, characterized in that the individual oxygen adding tubes (6) are uniformly arranged on a circumference coaxial with the baffle (7).
6. The self-heating coal supercritical water thermal chemical reduction hydrogen production reactor according to claim 3, characterized in that the outlet of each oxygen adding pipe (6) is horizontally directed to the axis of the baffle (7).
7. The self-heating coal supercritical water thermal chemical reduction hydrogen production reactor according to claim 1, characterized in that the upper end and the lower end of the baffle (7) are connected with the reaction section main body (1) through ribs (71).
8. The self-heating coal supercritical water thermal chemical reduction hydrogen production reactor according to claim 1, characterized in that the lower end of the reaction section main body (1) is provided with a slag discharge conduit (3).
9. The self-heating coal supercritical water thermal chemical reduction hydrogen production reactor according to claim 1, characterized in that the thickness of the baffle (7) is 2-5 mm.
10. A self-heating coal supercritical water thermal chemical reduction hydrogen production method is characterized in that, based on the reactor of any one of claims 1 to 9, supercritical water is added into the reaction section main body (1) from a supercritical water inlet (21), normal temperature coal slurry is added into the reaction section main body (1) from a feeding pipe (4), and oxygen is introduced into a partition plate (7) from an oxygen adding pipe (6); supercritical water rises along an annular gasification area formed by the partition plate (7) and the reaction section main body (1), is mixed with normal-temperature coal slurry and flows into coal particles to perform supercritical water gasification of the coal slurry to generate mixed liquid rich in hydrogen; when the mixed liquor continuously rises to the upper end cover, the mixed liquor turns to enter an oxidation area in the clapboard (7) and is subjected to oxidation reaction with oxygen, and finally, the mixed liquor flows out of the reactor through an outlet pipe (8) of the oxidation section.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN115353909A (en) * | 2022-08-17 | 2022-11-18 | 西安交通大学 | Supercritical water porous medium hydrogen oxidation exothermic reactor and working method thereof |
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| US20090206007A1 (en) * | 2008-02-20 | 2009-08-20 | Air Products And Chemicals, Inc. | Process and apparatus for upgrading coal using supercritical water |
| US20150240172A1 (en) * | 2012-09-13 | 2015-08-27 | Big Dutchman International Gmbh | Apparatus and method for generating fuel gas from a solid combustible |
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| CN115353909A (en) * | 2022-08-17 | 2022-11-18 | 西安交通大学 | Supercritical water porous medium hydrogen oxidation exothermic reactor and working method thereof |
| CN115353909B (en) * | 2022-08-17 | 2024-03-26 | 西安交通大学 | Supercritical water porous medium hydrogen oxidation exothermic reactor and working method thereof |
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| CN114854454B (en) | 2023-04-14 |
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