CN110002953A - A kind of process and device of static bed coal gasification synthesis of methanol with joint production LNG - Google Patents

A kind of process and device of static bed coal gasification synthesis of methanol with joint production LNG Download PDF

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CN110002953A
CN110002953A CN201910362106.9A CN201910362106A CN110002953A CN 110002953 A CN110002953 A CN 110002953A CN 201910362106 A CN201910362106 A CN 201910362106A CN 110002953 A CN110002953 A CN 110002953A
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gas
unit
methanol
synthesis
coal gasification
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钱宇
顾竞芳
杨思宇
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South China University of Technology SCUT
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South China University of Technology SCUT
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    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C29/00Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
    • C07C29/15Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
    • C07C29/151Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
    • C07C29/1516Multisteps
    • C07C29/1518Multisteps one step being the formation of initial mixture of carbon oxides and hydrogen for synthesis
    • CCHEMISTRY; METALLURGY
    • C07ORGANIC CHEMISTRY
    • C07CACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C29/00Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
    • C07C29/15Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
    • C07C29/151Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
    • C07C29/152Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases characterised by the reactor used
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/02Fixed-bed gasification of lump fuel
    • C10J3/06Continuous processes
    • C10J3/16Continuous processes simultaneously reacting oxygen and water with the carbonaceous material
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/02Fixed-bed gasification of lump fuel
    • C10J3/20Apparatus; Plants
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    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72Other features
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72Other features
    • C10J3/82Gas withdrawal means
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10LFUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/10Working-up natural gas or synthetic natural gas
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00Details of gasification processes
    • C10J2300/09Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913Carbonaceous raw material
    • C10J2300/093Coal
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00Details of gasification processes
    • C10J2300/09Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953Gasifying agents
    • C10J2300/0959Oxygen
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00Details of gasification processes
    • C10J2300/09Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953Gasifying agents
    • C10J2300/0973Water
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00Details of gasification processes
    • C10J2300/16Integration of gasification processes with another plant or parts within the plant
    • C10J2300/1603Integration of gasification processes with another plant or parts within the plant with gas treatment
    • C10J2300/1612CO2-separation and sequestration, i.e. long time storage
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00Details of gasification processes
    • C10J2300/16Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656Conversion of synthesis gas to chemicals
    • C10J2300/1662Conversion of synthesis gas to chemicals to methane (SNG)
    • CCHEMISTRY; METALLURGY
    • C10PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10JPRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00Details of gasification processes
    • C10J2300/16Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656Conversion of synthesis gas to chemicals
    • C10J2300/1665Conversion of synthesis gas to chemicals to alcohols, e.g. methanol or ethanol

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  • Chemical Kinetics & Catalysis (AREA)
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  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Low-Molecular Organic Synthesis Reactions Using Catalysts (AREA)

Abstract

The invention belongs to the energy and chemical technology field, and in particular to a kind of process and device of static bed coal gasification synthesis of methanol with joint production LNG.This method separates hydrogen, carbon monoxide, methane content in synthesis gas by circularly cooling unit and cryogenic separation unit, available LNG product, process has better unit product income, and by remaining synthesis gas combined production of methanol platform chemicals, the hydrocarbon utilization of resources is optimized, coal gas project low status of project profitability due to SNG price continues at a low price is alleviated.In addition, the carbon dioxide that part acid gas removes is used for synthetic reaction by methanol synthesis unit by the present invention, to meet the hydrogen-carbon ratio of methanol synthesis reaction, WGS unit, process emission reduction are saved, so that this technical process ratio reduces by 18% CO2 emissions with scale coal gas project.

Description

A kind of process and device of static bed coal gasification synthesis of methanol with joint production LNG
Technical field
The invention belongs to the energy and chemical technology field, and in particular to a kind of static bed coal gasification synthesis of methanol with joint production LNG Process and device.
Background technique
Natural gas is the energy products that a kind of calorific value is high, pollution is few.In China, urban heat supplying, communications and transportation etc. Natural gas consumption demand is big, and the channels such as gas field gas production, inlet natural gas are sometimes insufficient, cause urban " winter gas It is waste " the case where.Therefore natural gas from coal project is released rapidly throughout our country.But with this kind of number of entry and investment On be continuously increased, produce structure on problem further expose.
In general, during natural gas from coal, in producing synthesis gas from coal containing 10%~20% methane, which can To be exported as gas product.But since synthesis gas needs part that water gas shift reaction occurs, to improve itself hydrogen Carbon ratio example meets the needs of methanation reaction.CO and H predominantly therein2O is converted to H by reforming reaction2And CO2, this Original 2.3~2.7 or so synthesis gas hydrogen-carbon ratio is adjusted to 3.1 or so by process, but also results in the wave of CO active principle Take and the increase of system carbon emission.Meanwhile thus obtained coal-based gas product is after dehydration, due to can not be temporary It deposits, needs to transport in time through piping, but with the decline of non-heating season natural gas consumption demand, it is also possible to face limited production and adjust Whole situation.
Summary of the invention
To solve the disadvantage that existing natural gas from coal (SNG) technology and shortcoming, the primary purpose of the present invention is that mentioning A kind of device for coal through lurgi gasifier fixed bed crushed coal pressure gasifying methanol with joint production LNG.
Another object of the present invention is to provide a kind of processes using above-mentioned apparatus methanol with joint production LNG.The party Method is in view of the higher feature of methane content in lurgi gasifier gasification raw gas, after carrying out the processing such as coal washing gas and acid gas removing, Increase cryogenic separation unit during original coal gas, the methane content in separating synthetic gas obtains the liquid of high added value Natural gas (LNG), as output of products.Remaining synthesis gas needs not move through WGS unit, at this time effective group in synthesis gas (the H divided2-CO2)/(CO+CO2) ratio is in the hydrogen-carbon ratio requirement of methanol synthesis reaction, it is 2.0~2.2.Therefore, it is obtaining After LNG product, water gas shift reaction and methanation reaction are saved, increases methanol synthesis reaction, system coproduction LNG can be made With two kinds of products of methanol.The transformation process facilitates the CO2 emission of reduction system, improves carbon utilization rate and obtains To higher unit product income.
To achieve the above object, The technical solution adopted by the invention is as follows:
A kind of device of static bed coal gasification synthesis of methanol with joint production LNG, including air gas separation unit, coal gasification unit, acid Gas removal unit, circularly cooling unit, cryogenic separation unit and methanol synthesis unit;
The air gas separation unit is equipped with air intake, nitrogen outlet and oxygen outlet, and wherein oxygen outlet passes through pipe Road is connected with the oxygen intake of coal gasification unit, and nitrogen outlet is connected by pipeline with the nitrogen inlet of circularly cooling unit It connects;
The coal gasification unit is equipped with feed coal entrance, oxygen intake and the outlet of coal gasification crude synthesis gas, wherein coal gas Change crude synthesis gas outlet to be connected by pipeline with the coal gasification crude synthesis gas entrance of acid gas removal unit;
Acid gas removal unit is equipped with synthesis gas from coal gasification outlet, sulfide outlet and carbon dioxide outlet, wherein titanium dioxide Carbon outlet is connected by pipeline with the carbon dioxide entrance of methanol synthesis unit, and synthesis gas from coal gasification outlet passes through pipeline and depth The synthesis gas from coal gasification entrance of cold separative unit is connected;
Cryogenic separation unit is equipped with synthesis gas from coal gasification entrance, N2Gas entrance, N2Gas outlet, liquified natural gas outlet and first Alcohol syngas outlet, wherein methyl methanol syngas outlet are connected by pipeline with methanol synthesis unit, N2Gas entrance and N2Gas outlet Respectively with the N of circularly cooling unit2Outlet and N2Gas outlet is connected;
Wherein, circularly cooling unit is the refrigerating plant of one group of nitrogen circulation loop.In cryogenic separation unit The low-pressure nitrogen (0.3~0.6MPa of operating pressure, 30~40 DEG C of operation temperature) of condensing zone is cooled into nitrogen through compressor compresses Gas (3~6MPa of operating pressure, 40~50 DEG C of operation temperature), returns again to main heat exchanger and is condensed into liquid nitrogen, most afterwards through circularly cooling Throttle valve in unit reduces temperature, returns in cryogenic separation unit and provides cooling capacity again for scrubbing section and the area rectifying Zai Fei.Separately Outside, the liquid nitrogen that coal gasification unit air separation plant is supplemented may be that condenser provides part cooling capacity.
Preferably, the coal gasification unit uses lurgi gasifier fixed bed broken coal pressurized coal gasification furnace.
Preferably, the device of the static bed coal gasification synthesis of methanol with joint production LNG further includes methanol rectification unit, methanol The methanol crude product outlet of synthesis unit is connected by pipeline with methanol rectification unit.
Preferably, the circularly cooling unit includes sequentially connected compressor, heat exchanger and expanding machine.
Preferably, the cryogenic separation unit includes molecular sieve zone, concentrates heat transfer zone, is scrubbing section, the area rectifying Zai Fei, cold Coagulation zone and product compressional zone.
It is furthermore preferred that the CH in scrubbing tower and the area rectifying Zai Fei in the cryogenic separation unit, in scrubbing section4-CO Rectifying column is packed tower, and design pressure is 4~6MPa, and the condenser in condensing zone is adopted with the reboiler in the area rectifying Zai Fei Use aluminum plate-fin heat exchanger.
The present invention further provides the processes of static bed coal gasification synthesis of methanol with joint production LNG a kind of, including following step It is rapid:
Air 1 is separated into nitrogen 4 and oxygen 5 by air gas separation unit, and wherein nitrogen 4 enters circularly cooling unit shape At refrigerant and enter cryogenic separation unit, and exchange heat between circularly cooling unit and cryogenic separation unit, oxygen 5 with Raw material lignite 2 and water 3 enter coal gasification unit, coal gasification crude synthesis gas 6 are made by pressure gasification process, coal gasification slightly synthesizes Gas 6 deviates from sulfide 7 by acid gas removal unit, obtains the synthesis gas from coal gasification 10 of carbon dioxide 8, carbon dioxide 9 and cleaning, Wherein carbon dioxide 8 discharges, and carbon dioxide 9 enters methanol synthesis unit, and clean synthesis gas from coal gasification 10 enters cryogenic separation Unit, obtains liquid natural gas 11 and methyl methanol syngas 12 after lock out operation, and methyl methanol syngas 12 enters methanol synthesis unit And it is reacted with carbon dioxide 9 and generates methanol crude product 13.
Preferably, the methanol crude product 13 also obtains methanol product 14 by methanol rectification unit.
It preferably, also include resulting vapor after air separation in the oxygen 5.
Preferably, the reacting furnace temperature of the coal gasification unit is 1000~1500 DEG C, and pressure is 25~42bar.
It is furthermore preferred that the reacting furnace temperature of the coal gasification unit is 1100~1450 DEG C, pressure is 28~42bar.
It is further preferred that the reaction condition in the coal gasification unit are as follows: 650~700 DEG C of gas temperature, lime-ash temperature 450~500 DEG C of degree, 340 DEG C of gasification agent temperature, coal room temperature, steaming oxygen ratio is 4~7, and oxygen coal ratio is 0.5~0.8.
Preferably, the hydrogen-carbon ratio of the coal gasification crude synthesis gas 6 is 2~3, and including 60~70vol.% of following component H2, 20~30vol.%CO and 5~20vol.%CH4
Preferably, the technique used in the acid gas removal unit is aMDEA technique, Gas/Spec technique, Sulfinol technique, Ucasol technique or Flexsorb technique.
It is furthermore preferred that the solvent of process selection used is aMDEA-1, aMDEA-2, Gas/ in the acid gas removal unit Spec-CS, Sulfinol-D, Sulfinol-X, ES-501, ES-701, PS series, one of HP series or CT8-23/25 Or it is two or more, which is able to satisfy the makings technical indicator before China LNG such as deep desulfuration decarburization removal of organic sulfur liquefaction.
Preferably, the amount of the carbon dioxide 9 meets methanol-fueled CLC unstrpped gas component content design requirement.
It is furthermore preferred that volume fraction is the 28 of gas gross after the carbon dioxide 9 is mixed with methyl methanol syngas 12 ~31%.
Preferably, the hydrogen-carbon ratio of the clean synthesis gas from coal gasification 10 is 1.5~3.
It is furthermore preferred that the hydrogen-carbon ratio of the clean synthesis gas from coal gasification 10 is 1.8~2.5.
Preferably, the circularly cooling unit is the swell refrigeration technique of unitary system cryogen.
It is furthermore preferred that the low temperature cold position that the swell refrigeration technique of the unitary system cryogen is supplied to cryogenic unit is -150 ~-200 DEG C, pressure is 30~50bar, and shaft power is 12000~15000kW, and steam consumption quantity is 45~60t/h, is imitated in constant entropy In the case that rate is 50%~85%, the outlet band liquid measure of expanding machine is 5~10vol.%.
It is further preferred that the swell refrigeration technique of the unitary system cryogen uses single-stage expansion refrigeration process, second level Concatenated nitrogen expansion refrigeration process, the nitrogen expansion refrigeration process of dual temperature area parallel connection, nitrogen-methane blended swell refrigeration technique or One or more of methane swell refrigeration technique.
Still more preferably, the logistics progress in the circularly cooling unit is that nitrogen a passes through circularly cooling unit In nitrogen compressor generate high temperature and pressure nitrogen b, high temperature and pressure nitrogen b by expanding machine generate cooling capacity, through in cryogenic separation unit Concentration heat transfer zone in exchange heat after formed nitrogen c, nitrogen c return circularly cooling unit in carry out circularly cooling.
Preferably, the ice chest outlet temperature of the cryogenic separation unit is -150~-250 DEG C, 11 He of liquid natural gas The yield of methyl methanol syngas 12 changes with the variation of outlet temperature.
It is furthermore preferred that the rectifier unit that the area rectifying Zai Fei uses includes low-temperature fractionating tower in the cryogenic separation unit With column plate type rectifying column, wherein the internals of low-temperature fractionating tower are 125Y, 250Y or 350Y type structured packing, operation pressure drop is to pass The 40%~80% of system sieve-plate tower, column plate type rectifying column are one or more kinds of in JCPT, valve tower version or JCV float valve.
Most of CO into before cryogenic separation device, in synthesis gas from coal gasificationx,SOxBe removed, but there is still a need for into One step removes CO2, water and methanol to be to meet separation requirement.Clean synthesis gas from coal gasification 10 enters the molecule of cryogenic separation device Sieve area, CO2, water and methanol is adsorbed by adsorbent;Purified synthesis gas leave molecular sieve zone sequentially enter concentrate heat transfer zone with Scrubbing section largely contains CH4It is washed with the synthesis gas of CO, subsequently into the CH in the area rectifying Zai Fei4In-CO rectifying column, tower top goes out Implication (about 50~90% or so) containing a large amount of CO, tower bottom are LNG product of the CO content less than 1%, and LNG product is after overcompression It is transported to storage tank.
It is further preferred that the logistics progress in the cryogenic separation unit is, clean synthesis gas from coal gasification 10 is passed through Over-molecular sieve removes CO2, meet cryogenic separation requirement after first alcohol and water, obtain synthesis gas d, synthesis gas d is by concentrating heat transfer zone Heat exchange obtains synthesis gas e, and synthesis gas e enters scrubbing tower, and the tower top outlet of scrubbing tower is the methanol-fueled CLC that methane content is lower than 1% Gas f, methyl methanol syngas f obtain methyl methanol syngas 12 after cold recovery, into methanol synthesis unit;The tower bottom group of scrubbing tower It as methane and carbon monoxide stream stock g, is introduced into rectifying column and is separated, the tower top outlet gas h of rectifying column is by condensation The heat exchanger in area obtains rich CO gas i and condensate liquid j, and gas i obtains gas k after the heat exchanger re-heat of concentration heat transfer zone, It sends out and cold is mixed to get methyl methanol syngas 12 with methyl methanol syngas f backward;Phegma l of the condensate liquid j a part as rectifying column, Another part enters scrubbing tower as phegma m.The stream stock n that the tower bottom of rectifying column is separated mainly contains methane content, warp After concentrating the heat exchanger in heat transfer zone, enters back into product compressional zone and obtain liquid natural gas 11;Stream stock o is to take heat steam, is passed through Heat steam p is obtained after crossing heat exchange.
The process of static bed coal gasification synthesis of methanol with joint production LNG of the present invention in addition to carry out above-mentioned restriction it Outside, other technological parameters are carried out referring to ordinary skill in the art means.
Compared with prior art, the present invention has the following advantages and beneficial effects:
(1) methane content is high in the synthesis gas from coal gasification for the lurgi gasifier that coal gas project is selected, and the present invention passes through Circularly cooling unit and cryogenic separation unit separate hydrogen, carbon monoxide, methane content in synthesis gas, available LNG product, process have better unit product income, and by remaining synthesis gas combined production of methanol platform chemicals, optimize carbon Coal gas project low status of project profitability due to SNG price continues at a low price is alleviated in the hydrogen utilization of resources.
(2) traditional coal gas project needs to meet downstream product by acid gas removal unit and gas conversion unit Suitable composition, the carbon dioxide product of acid gas removal unit removing are partly or entirely expelled directly out system in addition to partial oxidation, lead to While crossing gas shift reaction raising hydrogen-carbon ratio, a large amount of CO2 emission is produced, this partial CO 2 is often It is directly discharged in atmosphere, reduces the utilization rate of coal resources.The present invention is removed part acid gas by methanol synthesis unit Carbon dioxide to meet the hydrogen-carbon ratio of methanol synthesis reaction save WGS unit for synthetic reaction, process subtracts Row, so that this technical process ratio reduces by 18% CO2 emissions with scale coal gas project.
Detailed description of the invention
Fig. 1 is the process schematic representation of natural gas from coal in the prior art.Prior art device include air gas separation unit, Coal gasification unit, WGS unit, acid gas removal unit and methane synthesis unit.1~11 is logistics number, wherein 1 It is oxygen for air, 4,2 be feed coal, and 3 be water, and 5 be raw gas synthesis gas, and 6 be transformation synthesis gas, and 7 be to remove sulfide, 8 It is Clean synthesis gas for carbon dioxide removal, 9,10 be natural gas from coal.
Fig. 2 is the schematic device of static bed coal gasification synthesis of methanol with joint production LNG in the present invention, including air separation list Member, coal gasification unit, acid gas removal unit, circularly cooling unit, cryogenic separation unit, methanol synthesis unit and methanol essence Evaporate unit.
Fig. 3 is the process schematic diagram of static bed coal gasification synthesis of methanol with joint production LNG in the present invention.1~13 is logistics Number, wherein 1 is air, 4 be nitrogen, and 5 be oxygen, and 2 be feed coal, and 3 be water, and 6 be coal gasification crude synthesis gas, and 7 be abjection sulphur Compound, 8 be carbon dioxide, and 9 be carbon dioxide, and 10 be clean synthesis gas from coal gasification, and 11 be liquid natural gas, and 12 close for methanol It is methanol crude product at gas, 13,14 be methanol product.
Fig. 4 be cryogenic separation unit of the invention schematic device, including molecular sieve zone, concentrate heat transfer zone, scrubbing section, Rectifying and the area Zai Fei, condensing zone and product compressional zone.
Fig. 5 is the logistics schematic diagram of circularly cooling unit and cryogenic separation unit of the invention, wherein a is nitrogen, and b is High temperature and pressure nitrogen, c are nitrogen, and d is clean synthesis gas, and e is synthesis gas, and f is the methyl methanol syngas of methane content, and g is Carbon monoxide, h are tower top outlet gas, and i is richness CO gas, and j is condensate liquid, and k is the gas after heat exchanger re-heat, and l and m are reflux Liquid, n are tower bottom stream stock, and o is to take heat steam, and p is to remove heat steam.
Specific embodiment
Below with reference to embodiment and attached drawing, the present invention is described in further detail, but embodiments of the present invention are unlimited In this.For not specifically specified technological parameter, routine techniques progress can refer to.
Embodiment 1
The present embodiment provides the processes and device of a kind of static bed coal gasification synthesis of methanol with joint production LNG.
(1) device of static bed coal gasification synthesis of methanol with joint production LNG includes air gas separation unit, coal gasification unit, acid Gas removal unit, circularly cooling unit, cryogenic separation unit and methanol synthesis unit;
The air gas separation unit is equipped with air intake, nitrogen outlet and oxygen outlet, and wherein oxygen outlet passes through pipe Road is connected with the oxygen intake of coal gasification unit, and nitrogen outlet is connected by pipeline with the nitrogen inlet of circularly cooling unit It connects;
The coal gasification unit is equipped with feed coal entrance, oxygen intake and the outlet of coal gasification crude synthesis gas, wherein coal gas Change crude synthesis gas outlet to be connected by pipeline with the coal gasification crude synthesis gas entrance of acid gas removal unit;
Acid gas removal unit is equipped with synthesis gas from coal gasification outlet, sulfide outlet and carbon dioxide outlet, wherein titanium dioxide Carbon outlet is connected by pipeline with the carbon dioxide entrance of methanol synthesis unit, and synthesis gas from coal gasification outlet passes through pipeline and depth The synthesis gas from coal gasification entrance of cold separative unit is connected;
Cryogenic separation unit is equipped with synthesis gas from coal gasification entrance, N2Gas entrance, N2Gas outlet, liquified natural gas outlet and first Alcohol syngas outlet, wherein methyl methanol syngas outlet are connected by pipeline with methanol synthesis unit, N2Gas entrance and N2Gas outlet Respectively with the N of circularly cooling unit2Outlet and N2Gas outlet is connected;
Further, the coal gasification unit uses lurgi gasifier fixed bed broken coal pressurized coal gasification furnace.
Further, the device of the static bed coal gasification synthesis of methanol with joint production LNG further includes methanol rectification unit, first The methanol crude product outlet of alcohol synthesis unit is connected by pipeline with methanol rectification unit.
Further, the circularly cooling unit includes sequentially connected compressor, heat exchanger and expanding machine.
Further, the cryogenic separation unit include molecular sieve zone, concentrate heat transfer zone, scrubbing section, the area rectifying Zai Fei, Condensing zone and product compressional zone.
Further, the CH in scrubbing tower and the area rectifying Zai Fei in the cryogenic separation unit, in scrubbing section4- CO rectifying column is packed tower, and design pressure is 4~6MPa, and the condenser in condensing zone and the reboiler in the area rectifying Zai Fei are equal Using aluminum plate-fin heat exchanger.
(2) process is as follows:
Air 1 is separated into nitrogen 4 and oxygen 5 by air gas separation unit, and wherein nitrogen 4 enters circularly cooling unit shape At refrigerant and enter cryogenic separation unit, and exchange heat between circularly cooling unit and cryogenic separation unit, oxygen 5 with Raw material lignite 2 and water 3 enter coal gasification unit, coal gasification crude synthesis gas 6 are made by pressure gasification process, coal gasification slightly synthesizes Gas 6 deviates from sulfide 7 by acid gas removal unit, obtains the synthesis gas from coal gasification 10 of carbon dioxide 8, carbon dioxide 9 and cleaning, Wherein carbon dioxide 8 discharges, and carbon dioxide 9 enters methanol synthesis unit, and clean synthesis gas from coal gasification 10 enters cryogenic separation Unit, obtains liquid natural gas 11 and methyl methanol syngas 12 after lock out operation, and methyl methanol syngas 12 enters methanol synthesis unit And it is reacted with carbon dioxide 9 and generates methanol crude product 13.
Preferably, the methanol crude product 13 also obtains methanol product 14 by methanol rectification unit.
It preferably, also include resulting vapor after air separation in the oxygen 5.
For the technique used in the acid gas removal unit for aMDEA technique, the solvent of selection is aMDEA-1.
The circularly cooling unit uses single-stage expansion refrigeration process.
In the cryogenic separation unit, the rectifier unit that the area rectifying Zai Fei uses includes low-temperature fractionating tower and column plate type essence Evaporate tower, wherein the internals of low-temperature fractionating tower are the structured packing of 125Y type, and column plate type rectifying column is JCPT.
The specific implementation of above-mentioned process is as follows:
The flow of raw material lignite 2 is 580t/h, and the tolerance of the coal gasification crude synthesis gas 6 generated by coal gasification unit is 42350kmol/h removes the carbon dioxide of 4324kmol/h, at this time coal after coal gas water washing using acid gas removal unit The hydrogen-carbon ratio of gasification synthesis gas 10 is 2.45, tolerance 28310kmol/h;
By the molecular sieve of cryogenic separation unit and after concentrating heat transfer zone, washed tower separation methanol closes synthesis gas from coal gasification It is the tower base stream of carbon monoxide and methane at gas and main component.Carbon monoxide and methane further exchange heat and divide through rectifying column From obtaining the LNG product (tower bottom outlet temperature be -91 DEG C, pressure 3.5Mpa) of 4900kmol/h, the top of the distillation column condenser Temperature is -168 DEG C, pressure 3.1MPa, and gasification divides rate 0.75.;Leave the 12 (methane content at this time of methyl methanol syngas of heat transfer zone Less than 1%, 2.24) synthesis gas hydrogen-carbon ratio is;With the 720kmol/h carbon dioxide mix from acid gas removal unit, into first Alcohol synthesis unit (reaction temperature is 246 DEG C, pressure 0.8MPa), the Katalco provided using Johnson Matthey company 51-9 catalyst, at this time synthesis gas total sulfur (H2S+COS), chloride content controls within 20ppm.Obtain methanol crude product 5290kmol/h speeds to put after (40 DEG C of tower top temperature, pressure 7MPa) of methyl methanol syngas periodic off-gases heat exchange.
Embodiment 2
The present embodiment provides the processes and device of a kind of static bed coal gasification synthesis of methanol with joint production LNG.
The process and device is embodied as follows with embodiment 1:
The flow of raw material lignite 2 is 580t/h, and the tolerance of the coal gasification crude synthesis gas 6 generated by coal gasification unit is 42350kmol/h goes out the carbon dioxide of 4324kmol/h after coal gas water washing using acid gas removal unit, at this time coal The hydrogen-carbon ratio of gasification synthesis gas 10 is 2.45, tolerance 28310kmol/h;
Synthesis gas from coal gasification is behind heat transfer zone in over-molecular sieve sum aggregate, washed tower separation methyl methanol syngas and main component For the tower base stream of carbon monoxide and methane.Carbon monoxide and methane further exchange heat and separate through rectifying column, obtain The LNG product (tower bottom outlet temperature is -90.8 DEG C, pressure 3.4MPa) of 4790kmol/h, the top of the distillation column condenser temperature It is -158 DEG C, pressure 3.1MPa, gasification divides rate 0.77;Leaving the methyl methanol syngas 12 of heat transfer zone, (methane content is less than at this time 1%, 2.18) synthesis gas hydrogen-carbon ratio is;With the 720kmol/h carbon dioxide mix from acid gas removal unit, closed into methanol At unit (reaction temperature is 246 DEG C, pressure 0.8MPa), the Katalco 51- provided using Johnson Matthey company 9 catalyst, at this time synthesis gas total sulfur (H2S+COS), chloride content controls within 20ppm.Obtain methanol crude product 5343kmol/h speeds to put after (40 DEG C of tower top temperature, pressure 7MPa) of methyl methanol syngas periodic off-gases heat exchange.
Embodiment 3
The present embodiment provides the processes and device of a kind of static bed coal gasification synthesis of methanol with joint production LNG.
The process and device is embodied as follows with embodiment 1:
The flow of raw material lignite 2 is 580t/h, and the tolerance of the coal gasification crude synthesis gas 6 generated by coal gasification unit is 42350kmol/h goes out the carbon dioxide of 4324kmol/h after coal gas water washing using acid gas removal unit, at this time coal The hydrogen-carbon ratio of gasification synthesis gas 10 is 2.45, tolerance 28310kmol/h;
Synthesis gas from coal gasification is behind heat transfer zone in over-molecular sieve sum aggregate, washed tower separation methyl methanol syngas and main component For the tower base stream of carbon monoxide and methane.Carbon monoxide and methane further exchange heat and separate through rectifying column, obtain The LNG product (tower bottom outlet temperature is -90.8 DEG C, pressure 3.4MPa) of 4790kmol/h, the top of the distillation column condenser temperature It is -153 DEG C, pressure 3.1MPa, gasification divides rate 0.80;Leaving the methyl methanol syngas 12 of heat transfer zone, (methane content is less than at this time 1%, 2.11) synthesis gas hydrogen-carbon ratio is;With the 720kmol/h carbon dioxide mix from acid gas removal unit, closed into methanol At unit (reaction temperature is 246 DEG C, pressure 0.8MPa), the Katalco 51- provided using Johnson Matthey company 9 catalyst, at this time synthesis gas total sulfur (H2S+COS), chloride content controls within 20ppm.Obtain methanol crude product 5542kmol/h speeds to put after (40 DEG C of tower top temperature, pressure 7MPa) of methyl methanol syngas periodic off-gases heat exchange.
The above embodiment is a preferred embodiment of the present invention, but embodiments of the present invention are not by above-described embodiment Limitation, other any changes, modifications, substitutions, combinations, simplifications made without departing from the spirit and principles of the present invention, It should be equivalent substitute mode, be included within the scope of the present invention.

Claims (10)

1. a kind of device of static bed coal gasification synthesis of methanol with joint production LNG, it is characterised in that: including air gas separation unit, coal gas Change unit, acid gas removal unit, circularly cooling unit, cryogenic separation unit and methanol synthesis unit;
The air gas separation unit be equipped with air intake, nitrogen outlet and oxygen outlet, wherein oxygen outlet by pipeline with The oxygen intake of coal gasification unit is connected, and nitrogen outlet is connected by pipeline with the nitrogen inlet of circularly cooling unit;
The coal gasification unit is equipped with feed coal entrance, oxygen intake and the outlet of coal gasification crude synthesis gas, and wherein coal gasification is thick Syngas outlet is connected by pipeline with the coal gasification crude synthesis gas entrance of acid gas removal unit;
Acid gas removal unit is equipped with synthesis gas from coal gasification outlet, sulfide outlet and carbon dioxide outlet, and wherein carbon dioxide goes out Mouth is connected by pipeline with the carbon dioxide entrance of methanol synthesis unit, and synthesis gas from coal gasification outlet passes through pipeline and deep cooling point Synthesis gas from coal gasification entrance from unit is connected;
Cryogenic separation unit is equipped with synthesis gas from coal gasification entrance, N2Gas entrance, N2Gas outlet, liquified natural gas outlet and methanol close It is exported at gas, wherein methyl methanol syngas outlet is connected by pipeline with methanol synthesis unit, N2Gas entrance and N2Gas outlet difference With the N of circularly cooling unit2Outlet and N2Gas outlet is connected.
2. the device of static bed coal gasification synthesis of methanol with joint production LNG according to claim 1, it is characterised in that:
The coal gasification unit uses lurgi gasifier fixed bed broken coal pressurized coal gasification furnace;
The device of the static bed coal gasification synthesis of methanol with joint production LNG further includes methanol rectification unit, methanol synthesis unit The outlet of methanol crude product is connected by pipeline with methanol rectification unit.
3. the device of static bed coal gasification synthesis of methanol with joint production LNG according to claim 1, it is characterised in that:
The circularly cooling unit includes sequentially connected compressor, heat exchanger and expanding machine;
The cryogenic separation unit includes molecular sieve zone, concentrates heat transfer zone, scrubbing section, the area rectifying Zai Fei, condensing zone and product Compressional zone.
4. the device of static bed coal gasification synthesis of methanol with joint production LNG according to claim 3, it is characterised in that: described The CH in scrubbing tower and the area rectifying Zai Fei in cryogenic separation unit, in scrubbing section4- CO rectifying column is packed tower, design pressure Power is 4~6MPa, and the reboiler in condenser and the area rectifying Zai Fei in condensing zone is all made of aluminum plate-fin heat exchanger.
5. a kind of process using the described in any item device synthesis of methanol with joint production LNG of Claims 1 to 4, feature exist In, comprising the following steps: air 1 is separated into nitrogen 4 and oxygen 5 by air gas separation unit, and wherein nitrogen 4 enters circulation system Cold unit forms refrigerant and enters cryogenic separation unit, and is changed between circularly cooling unit and cryogenic separation unit Heat, oxygen 5 and raw material lignite 2 and water 3 enter coal gasification unit, and coal gasification crude synthesis gas 6, coal is made by pressure gasification process Crude synthesis gas 6 gasify by acid gas removal unit abjection sulfide 7, obtains the coal gas of carbon dioxide 8, carbon dioxide 9 and cleaning Be combined to gas 10, wherein carbon dioxide 8 discharge, carbon dioxide 9 enter methanol synthesis unit, clean synthesis gas from coal gasification 10 into Enter cryogenic separation unit, liquid natural gas 11 and methyl methanol syngas 12 are obtained after lock out operation, methyl methanol syngas 12 enters first Alcohol synthesis unit simultaneously reacts generation methanol crude product 13 with carbon dioxide 9.
6. the process of synthesis of methanol with joint production LNG according to claim 5, it is characterised in that:
The methanol crude product 13 also obtains methanol product 14 by methanol rectification unit;
The reacting furnace temperature of the coal gasification unit is 1000~1500 DEG C, and pressure is 25~42bar;
The hydrogen-carbon ratio of the coal gasification crude synthesis gas 6 is 2~3, and including 60~70vol.%H of following component2, 20~ 30vol.%CO and 5~20vol.%CH4
The technique used in the acid gas removal unit is aMDEA technique, Gas/Spec technique, Sulfinol technique, Ucasol technique or Flexsorb technique;
The amount of the carbon dioxide 9 meets methanol-fueled CLC unstrpped gas component content design requirement;
The hydrogen-carbon ratio of the clean synthesis gas from coal gasification 10 is 1.5~3;
The circularly cooling unit is the swell refrigeration technique of unitary system cryogen;
The ice chest outlet temperature of the cryogenic separation unit is -150~-250 DEG C, liquid natural gas 11 and methyl methanol syngas 12 Yield change with the variation of outlet temperature.
7. the process of synthesis of methanol with joint production LNG according to claim 6, it is characterised in that:
The reacting furnace temperature of the coal gasification unit is 1100~1450 DEG C, and pressure is 28~42bar;
The solvent of process selection used is aMDEA-1, aMDEA-2, Gas/Spec-CS in the acid gas removal unit, Sulfinol-D, Sulfinol-X, ES-501, ES-701, PS series, HP series or one or both of CT8-23/25 with On;
After the carbon dioxide 9 is mixed with methyl methanol syngas 12, volume fraction is the 28~31% of gas gross;
The hydrogen-carbon ratio of the clean synthesis gas from coal gasification 10 is 1.8~2.5;
The low temperature cold position that the swell refrigeration technique of the unitary system cryogen is supplied to cryogenic unit is -150~-200 DEG C, pressure For 30~50bar, it is 50%~85% in isentropic efficiency that shaft power, which is 12000~15000kW, and steam consumption quantity is 45~60t/h In the case where, the outlet band liquid measure of expanding machine is 5~10vol.%.
8. the process of synthesis of methanol with joint production LNG according to claim 7, it is characterised in that: the cryogenic separation In unit, the rectifier unit that the area rectifying Zai Fei uses includes low-temperature fractionating tower and column plate type rectifying column, wherein low-temperature fractionating tower Internals are 125Y, 250Y or 350Y type structured packing, operation pressure drop is the 40%~80% of traditional sieve-plate tower, column plate type rectifying column It is one or more kinds of in JCPT, valve tower version or JCV float valve.
9. the process of synthesis of methanol with joint production LNG according to claim 7, it is characterised in that:
Reaction condition in the coal gasification unit are as follows: 650~700 DEG C of gas temperature, 450~500 DEG C of ash temperature, gasification 340 DEG C of agent temperature, coal room temperature, steaming oxygen ratio is 4~7, and oxygen coal ratio is 0.5~0.8;
The swell refrigeration technique of the unitary system cryogen is freezed using the nitrogen expansion of single-stage expansion refrigeration process, two-stage tandem In technique, the nitrogen expansion refrigeration process of dual temperature area parallel connection, nitrogen-methane blended swell refrigeration technique or methane swell refrigeration technique One or more.
10. the process of synthesis of methanol with joint production LNG according to claim 7, it is characterised in that: the cryogenic separation Logistics progress in unit is that clean synthesis gas from coal gasification 10 removes CO through over-molecular sieve2, deep cooling point is met after first alcohol and water From requiring, synthesis gas d is obtained, by concentrating heat transfer zone to exchange heat to obtain synthesis gas e, synthesis gas e enters scrubbing tower, washes synthesis gas d The tower top outlet for washing tower is methyl methanol syngas f of the methane content lower than 1%, and methyl methanol syngas f obtains first after cold recovery Alcohol synthesis gas 12, into methanol synthesis unit;The tower bottom group of scrubbing tower becomes methane and carbon monoxide stream stock g, is introduced into essence It evaporates in tower and is separated, the tower top outlet gas h of rectifying column obtains rich CO gas i and condensate liquid j, gas by the heat exchanger of condensing zone For body i by obtaining gas k after concentrating the heat exchanger re-heat of heat transfer zone, submitting is cold to be mixed to get methanol with methyl methanol syngas f backward Synthesis gas 12;Phegma l of the condensate liquid j a part as rectifying column, another part enter scrubbing tower as phegma m, rectifying The stream stock n that the tower bottom of tower is separated mainly contains methane content, after concentrating the heat exchanger in heat transfer zone, enters back into product pressure Contracting area obtains liquid natural gas 11;Stream stock o is to take heat steam, obtains heat steam p after heat exchange.
CN201910362106.9A 2019-04-30 2019-04-30 A kind of process and device of static bed coal gasification synthesis of methanol with joint production LNG Pending CN110002953A (en)

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Application publication date: 20190712