CN106276788A - A kind of supercritical water gasification hydrogen production device and method of the coal of residual liquid recirculation - Google Patents
A kind of supercritical water gasification hydrogen production device and method of the coal of residual liquid recirculation Download PDFInfo
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- CN106276788A CN106276788A CN201610570395.8A CN201610570395A CN106276788A CN 106276788 A CN106276788 A CN 106276788A CN 201610570395 A CN201610570395 A CN 201610570395A CN 106276788 A CN106276788 A CN 106276788A
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
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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
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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
- C10J3/48—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
- 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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
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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
- Y02P20/10—Process efficiency
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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 present invention relates to the supercritical water gasification hydrogen production system and method for the coal of a kind of residual liquid recirculation, this system belongs to the clean and effective of coal and converts category, the feature of this system is by charging system, heating system, response system, piece-rate system and blood circulation are constituted, and blood circulation includes regenerator, high-pressure separator, filter, High Temperature High Pressure plunger displacement pump, high temperature mass flowmenter, heater and reactor, realize the supercritical water gasification residual liquid of coal in the circulation within gasification system, both the energy in residual liquid can have been reclaimed, the organic substance in residual liquid can be made again again to gasify, improve the carbon gasification rate of coal.The invention provides efficient, clean gasification of coal, relative to traditional coal gasifying process, it is low that this device and method has gasification temperature, and hydrogen percentage composition is high, the outstanding advantages that energy utilization efficiency is high.
Description
Technical field
The invention belongs to clear energy sources and convert field and coal chemical technology, particularly to the coal of a kind of residual liquid recirculation
Supercritical water gasification hydrogen production apparatus and method.
Background technology
Hydrogen production from coal gasification will be the main technological route of following hydrogen economy, and coal hydrogen manufacturing is to solve the development Hydrogen Energy primary stage
The main path of hydrogen source problem, has important strategic importance.And the supercritical water gasification hydrogen production the most promising coal that is one
Conversion process efficient, clean.Supercritical water has excellent physicochemical properties, and supercritical water has low compared with the water under normality
Dielectric constant, the weak hydrogen bond of the few intensity of quantity, polarity is greatly reduced, and a lot of Organic substances and gas are soluble in supercritical
In water, therefore gasification reaction can be carried out in single_phase system, thus substantially increases reaction rate.It addition, supercritical water
Ionic product is several orders of magnitude higher than under normality, and therefore supercritical water is also good acidic group/base catalysis reaction medium.Surpass and face
These characteristics of boundary's water make the supercritical water gasification of coal have the advantage that, and coal adaptability is strong, be swift in response, rate of gasification
High, gasification product hydrogen content height, aerogenesis calorific value height, coke generate less, product hydrogen rate is high, can obtain hydrogen rich gas at a lower temperature
Body, pollutant containing N, S are got rid of with liquid phase.
Modell (US4113446) of america's MIT in 1978 et al. proposes the use solid such as coal, timber or liquid first
Organic material reacts generation high heat value gas in supercritical water, and in material, 80% is converted into gas, and 20% is converted into liquid, several
Coke is not had to generate.University of Melbourne combines with Australia Commonwealth Scientific and Industrial Research Organisation and publishes an article
(International Journal of Hydrogen Energy, 2009,34 (8): 3342-3350) Study on Coal is at supercritical
Non-catalyzed gasification in water, the conclusion drawn is: when reactor inner transmission matter heat transfer condition is bad, the conversion ratio distance thermodynamics of coal
Equilibrium point has bigger gap.Chinese Academy of Sciences's Shanxi coalification Bi Jicheng (ZL 200310109657.3) and Xi'an Communications University
Guo Liejin (ZL 200510041633.8) has built pipe flow reactor respectively, and has investigated coal gasification characteristic within the system.
In order to solve coking, the blockage problem easily occurred in pipe flow reactor, Xi'an Communications University Guo Lie brocade (ZL
200710017691.6) invent supercritical water fluid bed reactor.
Following problem demanding prompt solution is there is at present: discharge from reactor in the technique of the supercritical water gasification hydrogen production of coal
Reaction residue temperature higher, the heat of current supercritical water gasification technique is reclaimed by regenerator mostly, but according to being
System calculation of thermodynamics, energy loss is mainly derived from heat transfer process, and high temperature residual liquid to have and can reclaim having of gasification further
Machine material, again gasifies it and is possible not only to improve coal slurry gasification efficiency, and system can be made close to zero-emission.
Summary of the invention
The present invention proposes the supercritical water gasification hydrogen production device and method of the coal of a kind of residual liquid recirculation.Not only can be more
Reclaim well the heat of supercritical water gasification residual liquid, and coal rate of gasification in supercritical water can be improved further.System
Simple, convenient, efficient.
The technical solution used in the present invention is:
A kind of supercritical water gasification hydrogen production device of the coal of residual liquid recirculation, including reactor, regenerator, heater, with
And high-pressure separator, wherein, regenerator, heater and reactor form closed-loop path, water flow through successively regenerator, heater and
Reactor, in reactor with material hybrid reaction after, return regenerator, the outlet connection of the tube side of described regenerator has described
High-pressure separator, the liquid outlet of this high-pressure separator is connected to the entrance of heater by branch road, the gas of high-pressure separator
It is connected to gas flowmeter after cooling;In reactor, after supercritical water and material reaction, the mixture of generation divides through high pressure
Separating from device, wherein, hydrogen-rich gas is discharged from gas outlet and measures through gas flowmeter, and highly pressurised liquid then passes through liquid
Outlet carries out gasification reaction in branch road comes back to reactor.
Further, the liquid outlet of described high-pressure separator is connected to the entrance of heater by branch road, and this branch road is at least
Including High Temperature High Pressure plunger displacement pump, the front end of this High Temperature High Pressure plunger displacement pump connects filter, the rear end of this High Temperature High Pressure plunger displacement pump
Connect and have the 3rd mass flowmenter.
Further, supercritical water enters into regenerator by the shell-side inlet of regenerator, is then flowed out by shell-side outlet,
After converging with the liquid outlet branch road of high-pressure separator, it is connected to the entrance of heater.
Further, the gas outlet of described high-pressure separator connects cooler, and the outlet of cooler connects low pressure separator,
The gas outlet of low pressure separator connects gas flowmeter, and described low pressure separator is further provided with slag-drip opening.
Further, the outlet of described cooler connects counterbalance valve, hydrogen-rich gas in cooler after cooling, through the back of the body
Pressure valve enters into low pressure separator.
Further, water and material are entered in regenerator and reactor by the first and second plunger displacement pumps respectively.
Further, this device has farther included monitoring system, to control the pressure of whole device, temperature, flow
System, this monitoring system includes the first pressure transducer and the first mass flow being arranged between the first plunger displacement pump and regenerator
Meter, the second pressure transducer being arranged between the second plunger displacement pump and reactor and the second mass flowmenter.
The hydrogen production process of the supercritical water gasification hydrogen production device of the coal of a kind of residual liquid recirculation, comprises the following steps:
(1) coal gasification reaction: open the first plunger displacement pump, water flows through regenerator, heater, reactor, regenerator, height successively
Pressure separator, cooler, counterbalance valve, low pressure separator, discharged by low pressure separator outlet;Heater adds with reactor
Thermal, makes system reach required pressure and temperature;Opening the second plunger displacement pump, coal slurry is transported in reactor, starts coal
Supercritical water gasification reaction;
(2) residual liquid process recycling: open High Temperature High Pressure plunger displacement pump, makes residual liquid along High Temperature High Pressure plunger displacement pump, heater, anti-
Device, regenerator, high-pressure separator, filter is answered to form closed-loop path, by the first high-pressure plunger pump and High Temperature High Pressure plunger displacement pump
Flow is adjusted to the flow condition needed for system stability;
(3) after gasification reaction terminates, it is first shut off the feeding device of the second plunger displacement pump, treats that device runs a period of time continuously
Rear closedown heater and the heater of reactor, slowly regulate counterbalance valve after system is lowered the temperature and carry out blood pressure lowering.
Compared with prior art, the present invention at least has the advantages that the present invention liquid discharge at high-pressure separator
Connect further between mouth and heater and have branch road, so, the gas-liquid mixed produced in reactor, separate through high-pressure separator
After, hydrogen-rich gas is discharged from gas outlet, and highly pressurised liquid then carries out gasification reaction in branch road comes back to reactor.Not only return
Receive the energy in residual liquid in course of reaction, improved the carbon gasification efficiency of coal, and provide a coal at supercritical for reactor
The free radical source of Efficient Conversion in water.
Accompanying drawing explanation
The present invention will be further described for embodiment in conjunction with the following drawings:
Fig. 1 is the supercritical water gasification device schematic diagram of the coal of the residual liquid recirculation of the present invention.
Detailed description of the invention
The present invention relates to the supercritical water gasification hydrogen production system of the coal of a kind of residual liquid recirculation, this system belongs to the cleaning of coal
Efficient Conversion category, this system is mainly made up of charging system, heating system, response system, piece-rate system and blood circulation, follows
Loop systems includes regenerator, high-pressure separator, filter, High Temperature High Pressure plunger displacement pump, high temperature mass flowmenter, heater and reaction
Device, it is achieved the supercritical water gasification residual liquid of coal, in the circulation within gasification system, both can reclaim the energy in residual liquid, the most permissible
Make the organic substance in residual liquid again gasify, improve the carbon gasification rate of coal.The invention provides the gas of efficient, clean coal
Change method, relative to traditional coal gasifying process, it is low that this device and method has gasification temperature, and hydrogen percentage composition is high, energy profit
With the high outstanding advantages of efficiency.
The present invention includes the charging system of the double feeder of double pump carried continuously for the high pressure of high concentration coal slurry;Including producing
The high and low pressure gas and water separator that thing separates;Including holding concurrently when the heater of water preheating with residual liquid pipe flow reactor;High including high temperature
Pressure circulation plunger displacement pump, filter, heater, reactor, high-pressure separator are in interior blood circulation.
Referring to shown in Fig. 1, the present invention is the supercritical water fluid bed gasification hydrogen-producing system of the coal of a kind of residual liquid recirculation,
Including first high-pressure plunger pump the 1, second high-pressure plunger pump 2, High Temperature High Pressure plunger displacement pump the 3, first mass flowmenter the 4, second mass
Effusion meter 5, High Temperature High Pressure mass flowmenter 6, reactor 7, regenerator 8, heater 9, filter 10, high-pressure separator 11, cold
But device 12, counterbalance valve 13, low pressure separator 14, wet gas flow meter 15 and multiple pressure, temperature measuring equipment and control
Valve.
Wherein, the outlet of the first high-pressure plunger pump 1 connects the first mass flowmenter 4 entrance, and the first mass flowmenter 4 exports
Connect the shell-side inlet of regenerator 8, the shell-side outlet of regenerator 8 and the outlet of the 3rd mass flowmenter 6 and the entrance of heater 9
It is respectively connected with, the supercritical water entrance of the outlet coupled reaction device 7 of heater 9.
The outlet of the second high-pressure plunger pump 2 connects the second mass flowmenter 5 entrance, and the outlet of the second mass flowmenter 5 is even
Connecing the material inlet of reactor 7, the outlet of reactor 7 connects the tube side entrance of regenerator 8, and the tube side outlet of regenerator 8 connects
The entrance of high-pressure separator 11;The liquid-phase outlet of high-pressure separator 11 connects the entrance of filter 10, and the outlet of filter 10 is even
Connecing the entrance of High Temperature High Pressure plunger displacement pump 3, the outlet of High Temperature High Pressure plunger displacement pump 3 connects the entrance of the 3rd mass flowmenter 6, the 3rd matter
The outlet of amount effusion meter 6 and the outlet of regenerator 8 connect the entrance of heater 9.The deslagging of high-pressure separator 11 exports residue
Discharge system, the gas-phase product outlet of high-pressure separator 11 connects the entrance of cooler 12, and the outlet of cooler 12 connects back pressure
The entrance of valve 13, the outlet of counterbalance valve 13 connects the entrance of low pressure separator 14, and the gaseous phase outlet of low pressure separator 14 connects wet
The entrance of formula gas flowmeter 15.
The operating procedure of the supercritical water gasification hydrogen production device of the coal of described system is as follows:
1) configuration coal slurry: add coal, additive and catalyst in a reservoir, is stirring evenly and then adding into water, stands a timing
Between, the coal slurry forming stable homogeneous is standby.
2) coal gasification reaction process: open the first plunger displacement pump 1 make water flow through successively the first mass flowmenter 4, regenerator 8,
Heater 9, reactor 7, regenerator 8, high-pressure separator 11, cooler 12, counterbalance valve 13, low pressure separator 14, divided by low pressure
Discharge from device outlet.Screw the heater of counterbalance valve 13 heater 9 and reactor 7, make system reach required pressure
Power and temperature.Open the second plunger displacement pump 2 simultaneously and coal slurry is transported to reactor.By charging system by reacted for coal slurry device 7
Entrance is sent in supercritical water fluid bed reactor, starts the supercritical water gasification reaction of coal.
3) residual liquid process recycling: open High Temperature High Pressure plunger displacement pump 3 and make residual liquid along High Temperature High Pressure plunger displacement pump the 3, the 3rd mass
Effusion meter 6, heater 9, reactor 7, regenerator 8, high-pressure separator 11, filter 10 form closed-loop path, by the first high pressure
The flow of plunger displacement pump 1 and High Temperature High Pressure plunger displacement pump 3 is adjusted to the flow condition needed for system stability.
4) terminate course of reaction: after gasification reaction terminates, be first shut off the feeding device of the second plunger displacement pump 2, treat that device is even
Reforwarding row closes the heater of heater 9 and reactor 7 after one hour, after system is lowered the temperature, slowly regulation counterbalance valve drops
Pressure.
Compared to prior art, the method have the advantages that
(1) native system make use of the physicochemical properties that supercritical water is excellent, can realize the height of coal at a lower temperature
Effect, clean conversion.This technique and the method economic advantages when processing the brown coal of high-moisture highlight.
(2) high-pressure separator realizes hydrogen-rich gaseous product separation from system at high temperature under high pressure, and highly pressurised liquid is then
It is re-entered in reactor by pump and carries out gasification reaction.
(3) with High Temperature High Pressure plunger displacement pump, filter, heater, reactor, regenerator, the residual liquid of high-pressure separator composition
Closed circuit, is possible not only to realize reclaiming the energy in residual liquid, improves the carbon gasification efficiency of coal, and can be that reactor provides
The free radical source of one coal Efficient Conversion in supercritical water.
Claims (8)
1. the supercritical water gasification hydrogen production device of the coal of a residual liquid recirculation, it is characterised in that: include reactor (7), backheat
Device (8), heater (9), and high-pressure separator (11), wherein, regenerator (8), heater (9) and reactor (7) are formed and close
Closing loop, water flows through regenerator (8), heater (9) and reactor (7) successively, with material hybrid reaction in reactor (7)
After, returning regenerator (8), the tube side outlet connection of described regenerator (8) has described high-pressure separator (11), and this high pressure separates
The liquid outlet of device (11) is connected to the entrance of heater (9) by branch road, and the gas of high-pressure separator (11) connects after cooling
It is connected to gas flowmeter (15);In reactor, after supercritical water and material reaction, the mixture of generation divides through high-pressure separator
From, wherein, hydrogen-rich gas is discharged from gas outlet and measures through gas flowmeter, and highly pressurised liquid is then by liquid outlet warp
Branch road comes back to carry out in reactor gasification reaction.
The supercritical water gasification hydrogen production device of the coal of a kind of residual liquid recirculation the most according to claim 1, it is characterised in that:
The liquid outlet of described high-pressure separator is connected to the entrance of heater (9) by branch road, and this branch road at least includes High Temperature High Pressure
Plunger displacement pump (3), the front end of this High Temperature High Pressure plunger displacement pump connects filter (10), and the rear end of this High Temperature High Pressure plunger displacement pump connects to be had
3rd mass flowmenter (6).
The supercritical water gasification hydrogen production device of the coal of a kind of residual liquid recirculation the most according to claim 1, it is characterised in that:
Supercritical water enters into regenerator by the shell-side inlet of regenerator (8), is then flowed out by shell-side outlet, through separating with high pressure
After the liquid outlet branch road of device converges, it is connected to the entrance of heater.
The supercritical water gasification hydrogen production device of the coal of a kind of residual liquid recirculation the most according to claim 1, it is characterised in that:
The gas outlet of described high-pressure separator connects cooler (12), and the outlet of cooler connects low pressure separator, low pressure separator
Gas outlet connect gas flowmeter (15), described low pressure separator is further provided with slag-drip opening.
The supercritical water gasification hydrogen production device of the coal of a kind of residual liquid recirculation the most according to claim 4, it is characterised in that:
The outlet of described cooler connects counterbalance valve, and hydrogen-rich gas after cooling, enters into low pressure through counterbalance valve in cooler
Separator.
The supercritical water gasification hydrogen production device of the coal of a kind of residual liquid recirculation the most according to claim 1, it is characterised in that:
Water and material are entered in regenerator and reactor by the first and second plunger displacement pumps respectively.
The supercritical water gasification hydrogen production device of the coal of a kind of residual liquid recirculation the most according to claim 6, it is characterised in that:
This device has farther included monitoring system, so that the pressure of whole device, temperature, flow are controlled, and this monitoring system bag
Include the first pressure transducer and the first mass flowmenter being arranged between the first plunger displacement pump and regenerator, be arranged on the second plunger
The second pressure transducer between pump and reactor and the second mass flowmenter.
8. the supercritical water gasification hydrogen production of a coal based on a kind of residual liquid recirculation according to any one of claim 1 to 7
The hydrogen production process of device, it is characterised in that: comprise the following steps:
(1) coal gasification reaction: open the first plunger displacement pump (1), water flow through successively regenerator (8), heater (9), reactor (7),
Regenerator (8), high-pressure separator (11), cooler (12), counterbalance valve (13), low pressure separator (14), gone out by low pressure separator
Mouth is discharged;The heater of heater (9) and reactor (7), makes system reach required pressure and temperature;Open second
Plunger displacement pump (2), coal slurry is transported in reactor, starts the supercritical water gasification reaction of coal;
(2) residual liquid process recycling: open High Temperature High Pressure plunger displacement pump, make residual liquid along High Temperature High Pressure plunger displacement pump (3), heater (9),
Reactor (7), regenerator (8), high-pressure separator (11), filter (10) form closed-loop path, by the first high-pressure plunger pump (1)
It is adjusted to the flow condition needed for system stability with the flow of High Temperature High Pressure plunger displacement pump (3);
(3) after gasification reaction terminates, it is first shut off the feeding device of the second plunger displacement pump (2), treats that device runs a period of time continuously
Rear closedown heater (9) and the heater of reactor (7), slowly regulate counterbalance valve after system is lowered the temperature and carry out blood pressure lowering.
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