CN101214920A - System and device for preparing hydrogen from coke-oven gas by using mixed conductor oxygen-permeating film reactor - Google Patents
System and device for preparing hydrogen from coke-oven gas by using mixed conductor oxygen-permeating film reactor Download PDFInfo
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- CN101214920A CN101214920A CNA2008100324132A CN200810032413A CN101214920A CN 101214920 A CN101214920 A CN 101214920A CN A2008100324132 A CNA2008100324132 A CN A2008100324132A CN 200810032413 A CN200810032413 A CN 200810032413A CN 101214920 A CN101214920 A CN 101214920A
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- oxygen
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- oven gas
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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
- Y02P20/10—Process efficiency
- Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
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Abstract
The invention relates to a system device of preparing hydrogen by coke oven gas catalysis, partial oxidization reformation gas with a dense mixed conductor oxygen permeable film reactor, and belongs to the technical field of coke oven coal hydrogen making process. The key and important main device adopted by the coke oven gas hydrogen making device of the invention is the mixed conductor oxygen permeable film reactor which consists of the ceramic oxygen permeable film, an upper space and a lower space separated by the oxygen permeable film (the air side space on the upper side and the reformed coal side space on the lower side), and an outer shell; the system device includes the following systems: (1) an oxygen air supply system; (2) a coke oven gas supply system; (3) an output system of reacted product after being oxidized and reformed; (4) other auxiliary devices. The system device of the invention can convert all energetic components in large amount of coke oven gas into hydrogen, so that the quantity of the hydrogen prepared by the coke oven gas is doubled. Because the oxygen is supplied by the mixed conductor oxygen permeable film, the cost may be 50 percent lower than that of oxygen making through an air separation method.
Description
Technical field
The present invention relates to a kind ofly utilize fine and close temperature to close the conductor oxygen-permeable membrane reactor to realize that coke-oven gas catalysis, partial oxidation reformation coal gas to produce the system and device of hydrogen, belong to hydrogen production from coke oven gas Technology field.
Background technology
Along with development of human society, the energy system that the mankind depend on for existence is also constantly taking place to change.Hydrogen is considered to one of desirable energy of 21st century, has caused that people pay attention to widely.At present, realize the extensive utilization of Hydrogen Energy, the technology of preparing that exploitation possesses mass-producing and economy is to compel one of key issue to be solved.Hydrogen Energy belongs to secondary energy, can only be transformed and be obtained by other energy.At present; in the method for various hydrogen manufacturing; though utilizing renewable energy source hydrogen manufacturing such as sun power, wind energy, underground heat is optimal pattern, utilize these renewable energy sources not possess mass-producing and economy now by the Hydrogen Energy of methods such as photodissociation, pyrolysis, electrolysis or microbiological degradation preparation.The maturation method that can be used at present scale hydrogen manufacturing in the world mainly is water electrolysis and fossil energy hydrogen manufacturing (coal, Sweet natural gas and liquid fossil energy).If utilize water electrolysis hydrogen producing, water electrolysis 1Nm
3H
2Theoretical power consumption be 2.95kWh, actual power consumption 5～6kWh, commodity valency are 4～6 yuan/Nm
3H
2, i.e. 45～65 yuan/kgH
2, far above the price of utilizing fossil energy hydrogen manufacturing.More various preparation methods take a broad view of domestic resource status and characteristics, can realize that the most possible approach of economy of large scale hydrogen manufacturing is to utilize the containing that coking produces can furnace gas nearly mid-term.The composition of coke-oven gas is the percentage ratio meter by volume, mainly is H
2(accounting for 53～59%), CH
4(accounting for 25～30%) secondly is CO (about 6%), CO
2(about 2.5%), N
2(about 4%), O
2(about 0.5%), C
mH
n(about 2.5%).National coke oven by-product purified gas total resources was 79,900,000,000 Nm in 2003
3, by 2005, the total coal gas amount of coke oven by-product was up to about 96,600,000,000 Nm
3Quite a lot of independently coke-oven plant is owing to can not find suitable purposes, and a large amount of coal gas is burnt in vain by the mode of point " day lamp ", or directly enters atmosphere, causes the waste of the energy and the pollution of environment.According to the statistics of Shanxi Province Environmental Protection Agency, 8,000 ten thousand tons of Shanxi Province's year coking in 2004 produce about more than 300 hundred million Nm of coke-oven gas
3, its mid point " day lamp " discharging 20,000,000,000 Nm are arranged approximately
3Adsorb (PSA) technology to the original H in the coke oven purified gas by transformation at present
2It has been the industrialization process of comparative maturity that component is separated with purifying hydrogen manufacturing.Only reclaimed the original H in the furnace gas in this technology
2Component.Except hydrogen, also contain CH in the coke-oven gas
4, CO and C
mH
nDeng containing the energy component,, the amount that obtains hydrogen from coke-oven gas is significantly improved if these contain and can component transform the hydrogen that obtains through suitable reforming process in the coke-oven gas.
Utilize composite conductor oxygen-permeating film reactor and correlation technique, can directly from air, dynamically obtain pure oxygen, realize the coupling of methane portion oxidation process in oxygen sepn process and the coal gas, thereby reduced energy consumption, facility investment and running cost greatly.
Fine and close composite conductor oxygen-permeating film is the important mineral membrane of a class in high-temperature gas separation and the membrane catalytic reaction, why be called the mixed conductor mould material and be meant that this material has the characteristics of electronics and oxygen conduction simultaneously, the power that oxygen transmits in film is that the oxygen partial pressure of film both sides is poor, as long as the film both sides exist oxygen partial pressure poor, airborne oxygen will be transferred to the reaction side of membrane reactor continually.
Composite conductor oxygen-permeating film is fine and close fully stupalith, oxygen is pressed transmission with ionic shape in composite conductor oxygen-permeating film, oxygen permeable film is 100% to the diffusion selectivity of oxygen in theory, be that this type of film can only transmit oxonium ion, other gas molecule (as airborne nitrogen) is can not transmit in the past, this has the difference of essence with inorganic porous membrane on transporting mechanism, and the high oxygen permeating amount of this type of material can be suitable with the infiltration capacity of microporous membrane.
Owing in mixed conductor material, have oxonium ion transmission and reverse electric transmission simultaneously, so this type of film and solid electrolyte dense film also are not quite similar, do not need to add the loop during mixed conductor membrane work and offset the reverse potential that produces under the solid electrolyte dense film condition of pure ionophore, make the development and design of membrane reactor convenient like this.
Summary of the invention
The purpose of this invention is to provide a kind of composite conductor oxygen-permeating film reactor that utilizes and realize that coke-oven gas catalysis, partial oxidation reformation coal gas are to produce the system and device of hydrogen.
A kind of system and device for preparing hydrogen from coke-oven gas that utilizes fine and close composite conductor oxygen-permeating film reactor of the present invention, the feature of this system and device is to adopt most important agent set composite conductor oxygen-permeating film reactor, and it is that the air side space of upside and the reformation coal gas side space and the body skin of downside are formed by oxygen permeable film, two spaces up and down of being separated by oxygen permeable film; Described system and device is provided with following each system:
A. be delivered to the air side spatial oxygen source air feed system of oxygen-permeable membrane reactor upside: this system includes oxygen source gas inlet, compressor, high temperature air waste heat recoverer, well heater, bypass heat control valve and pipeline;
B. be delivered to the reformation coal gas spatial coke-oven gas feed system of oxygen-permeable membrane reactor downside: this system includes gas entry, compressor, first preheater bypass heat control valve and pipeline, dry desulfurization device, high temperature air waste heat recoverer, bypass heat control valve and pipeline, preheater of reformation coal gas.
C. react the output system of after product through oxidation and reformation: this output system includes interchanger of reformation coal gas, reformation coal gas secondary heat exchange device, high-temperature water gas conversion device, condenser, low temperature water gas changing device, condenser, gas-liquid separator, pressure-swing absorption apparatus, high purity H outlet and CO
2The tail gas outlet;
D. other auxiliary equipments: the water pump that send the water inlet place; Graywater outlet pipe by the gas-liquid separator discharge.
The ultimate principle of utilizing the oxygen permeable film oxygen supply to realize that methane portion oxidation is reformed in the coke-oven gas is as follows:
Fine and close composite conductor oxygen-permeating film one side is a coke-oven gas, and opposite side is an air, and airborne oxygen is penetrated into the coke-oven gas side through oxygen permeable film and methane generation partial oxidation reaction wherein generates carbon monoxide and hydrogen.Owing to the oxygen on oxygen permeable film surface is consumed very soon, make that the oxygen partial pressure on coke-oven gas side oxygen permeable film surface is very low (to be generally 10 at the partial oxidation reaction of coke-oven gas side methane
-22Normal atmosphere), and the oxygen partial pressure on air side oxygen permeable film surface very high (being oxygen partial pressure 0.21 normal atmosphere in the air), all the time there is a very big oxygen partial pressure difference motivating force like this in the oxygen permeable film both sides, the oxygen of air side can penetrate oxygen permeable film is participated in methane in the coke-oven gas to the coke-oven gas side partial oxidation reaction continuously, for the heat release of adjustment member oxidation reaction process, can in reaction system, penetrate an amount of water vapour.
The reaction mechanism that methane portion oxidation is reformed in the coke-oven gas is as follows:
The partial oxidation reaction of methane: CH
4+ 1/2O
2=CO+2H
2, so-called partial oxidation reaction is with respect to complete oxidation CH
4+ 1/2O
2=CO+2H
2, methane is oxidized to intermediate product CO and H in the partial oxidation reaction
2, promptly for hydrogen manufacturing, make hydrogen in the reaction product, rather than be completely oxidized to water and carbonic acid gas.
Because the partial oxidation reaction of methane is a thermopositive reaction CH
4+ 1/2O
2=CO+2H
2(Δ H=-36KJ), for making full use of heat, long-pending heat and the temperature of eliminating reactor raise, and produce more hydrogen simultaneously, add an amount of water vapour in reactor, because the steam reforming reaction of methane is instead (CH of a heat absorption
4+ H
2O=CO+3H
2Δ H=206KJ).
The advantage of system and device for preparing hydrogen from coke-oven gas of the present invention is: can component as much as possible all be converted into hydrogen all containing in a large amount of coke-oven gas, the amount that makes coke-oven gas make hydrogen significantly improves.Owing to come oxygen supply with composite conductor oxygen-permeating film, its cost might reduce nearly 50% than air separation legal system oxygen.
The present invention adopts methyl hydride catalyzed partial oxidation reformation technology in the composite conductor oxygen-permeating film reactor, compare with methane portion oxidation reforming method under the traditional direct oxygen supply, saved the preparation (low ternperature separation process or pressure-swing adsorption process) of pure oxygen, reaction can directly dynamically obtain pure oxygen from air, realize the coupling of oxygen sepn process and methane portion oxidation process, thereby reduced energy consumption, facility investment and running cost greatly.Because the oxygen in the composite conductor oxygen-permeating film reactor is by the oxygen diffusion control; thereby prevented to exist in the fixed bed reaction possibility of blast; significantly alleviate and in fixed-bed reactor, carry out the temperature runaway problem that the methane portion oxidation reforming reaction is produced; protect catalyzer, prolonged life of catalyst.
Be provided with multistage, multi-section position heat exchange unit in the native system device; made full use of the used heat of reformation coal gas and high temperature oxygen-denuded air; add an amount of water vapour in the methane reforming process, improved the oxygen gesture of oxygen permeable film reformation lateral balance system, can effectively prevent carbon distribution and protection oxygen permeable film.
Referring to Fig. 1, the system and device for preparing hydrogen from coke-oven gas that is provided with composite conductor oxygen-permeating film reactor of the present invention, adopted most important agent set composite conductor oxygen-permeating film reactor, it is that the air side space 9b of upside and reformation coal gas side space 9a people's shell 10 of downside are formed by oxygen permeable film 9, two spaces up and down of being separated by oxygen permeable film; Described system and device has following each system:
(1) be delivered to the oxygen source air feed system of the air side space 9b of oxygen-permeable membrane reactor upside: this system includes oxygen source gas inlet 18, compressor 19, high temperature air waste heat recoverer 6, well heater 20, bypass heat control valve and pipeline 21;
(2) be delivered to the coke-oven gas feed system of the reformation coal gas space 9a of oxygen-permeable membrane reactor downside: this system includes gas entry 1, compressor 2, first preheater 3 bypass heat control valves and pipeline 4, dry desulfurization device 5, high temperature air waste heat recoverer 6, bypass heat control valve and pipeline 8, preheater 7 of reformation coal gas.
(3) through the output system of oxidation and reformation reaction after product: this output system includes interchanger 7 of reformation coal gas, reformation coal gas secondary heat exchange device 11, high-temperature water gas conversion device 12, condenser 13, low temperature water gas changing device 14, condenser 15, gas-liquid separator 16, pressure-swing absorption apparatus 17, high purity H outlet 25 and CO
2 Tail gas outlet 26;
(4) other auxiliary equipments: the water pump 24 that send water inlet 23 places; Graywater outlet pipe 27 by gas-liquid separator 16 discharges.
The actual operation process of composite conductor oxygen-permeating film reactor system and device for preparing hydrogen from coke-oven gas of the present invention also is that the process for making hydrogen flow process of present embodiment is as described below:
Process for making hydrogen schema referring to Fig. 1.
The coke-oven gas of removing most impurity 1 compressed machine 2 pressurizations that from coking, come, at first enter the first preheater 3 of coke-oven gas of bypass temperature adjustment pipe 4, conversion gas heat exchange with high-temperature water gas conversion device 12, be elevated to about 300 ℃ from normal temperature, the coke-oven gas of sulfur-bearing is again by containing the dry desulfurization device 5 of cobalt or nickel molybdate catalyst, a spot of conversion of olefines is a methane in the coke-oven gas in device 5, and inorganic sulfur and organosulfur are removed simultaneously.Coke-oven gas after the purification mixes with the water vapor that reformation coal gas secondary heat exchange device 11 produces, enter in the high temperature off-air heat regenerator 6 of bypass temperature adjustment pipe 8 and interchanger 7 of reformation coal gas respectively and carry out heat exchange from the high temperature off-air of film both sides in the densification mixing oxygen permeable film reforming reactor and reformation coal gas and heat up, temperature is brought up to 800 ℃.The gas mixture of high temperature coke oven coal gas and steam enters among the reformation coal gas side space 9a of the membrane reactor that is made of fine and close composite conductor oxygen-permeating film 9 and body skin 10, in reformation coal gas side space 9a coke-oven gas with carry out partial oxidation reaction by the pure oxygen that oxygen permeable film 9 infeeds at reformation side space 9a by the air side space 9b of membrane reactor, mainly be H in the gas after the conversion
2And CO, also have a spot of CH
4, H
2O, CO
2And N
2In the reformation coal gas side space 9a of membrane reactor, be filled with the all-in-one-piece catalyzer of vesicular structure for partial oxidation reaction of methane, and the catalyzer for partial oxidation reaction of methane of the reformation coal gas side space 9a surface-coated identical component of oxygen permeable film 9.
The reformation coal gas that comes out from oxygen-permeable membrane reactor reformation side space 9a cools to 350～400 ℃ through interchanger 7 of reformation coal gas and reformation coal gas secondary heat exchange device 11 successively, enters then and makes most of CO process water gas shift reaction generation H in the reformation coal gas in the high-temperature water gas conversion device 12
2And CO
2, the water vapour that needs in the high temperature shift device 12 can be produced by reformation coal gas secondary heat exchange device 11 and condenser 13.Interchanger here and condenser can adopt waste heat boiler.Coal gas behind the high-temperature water gas conversion successively through coke-oven gas just preheater 3 and condenser 13 further cool to about 200 ℃, the conversion coal gas after the cooling enters low temperature water gas changing device 14 again, makes that remaining CO is converted to H in the coal gas
2Water vapour required in the low temperature water gas changing device 14 can be produced by condenser 13 and condenser 15 heat exchange.The main component of the coal gas that comes out from low temperature water gas changing device 14 is H
2, CO
2And water vapour, also have a spot of CH
4, CO and N
2Enter condenser 15 and gas-liquid separator 16 through the coal gas after the low temperature shift, utilize again from water inlet 23, cooling condenser 13 and the condenser 15 that water out 27 can be recycled to water pump 24 from the graywater that gas-liquid separator comes out.The dry gas that comes out from gas-liquid separator enters pressure-swing absorption apparatus 17 to be separated to purify and obtains highly purified hydrogen 25 and rich CO
2Tail gas 26.Rich CO
2Tail gas 26 can as the preparation high-purity CO
2Unstripped gas.
The raw air 18 that oxygen source is provided is through compressor 19 pressurizations, the high temperature off-air heat regenerator 6 and the well heater 20 that enter bypass temperature adjustment pipe 21 carry out heat exchange and heat temperature raising respectively, air after the heating is elevated to about 800 ℃ from normal temperature, high temperature air directly enters among the air side space 9b of the membrane reactor that is made of fine and close composite conductor oxygen-permeating film 9 and body skin 10,, under the motivating force of the oxygen partial pressure of oxygen permeable film 9 both sides, constantly be fed to by oxygen permeable film 9 among the reformation side space 9a of membrane reactor and participate in partial oxidation reaction at airborne oxygen in the 9b of air side space by the air side space 9b of membrane reactor.Raw air and cryogenic desulfurizing and purifying coke-oven gas that the high temperature oxygen-denuded air of discharging from the air side space 9b of membrane reactor enters high temperature off-air heat regenerator 6 and room temperature carry out heat exchange, oxygen-denuded air after the heat exchange is by relief outlet 22 emptyings, or as the raw material of preparation pure nitrogen gas.
Claims (1)
1. system and device for preparing hydrogen from coke-oven gas that utilizes fine and close composite conductor oxygen-permeating film reactor, the feature of this system and device is to adopt most important agent set composite conductor oxygen-permeating film reactor, two spaces up and down that it is separated by oxygen permeable film (9), by oxygen permeable film be the air side space (9b) of upside and downside reformation coal gas side space (9a), reach body skin (10) and formed; Described system and device is provided with following each system:
A. be delivered to the oxygen source air feed system in the air side space (9b) of oxygen-permeable membrane reactor upside: this system includes oxygen source gas inlet (18), compressor (19), high temperature air waste heat recoverer (6), well heater (20), bypass heat control valve and pipeline (21);
B. be delivered to the coke-oven gas feed system in the reformation coal gas space (9a) of oxygen-permeable membrane reactor downside: this system includes gas entry (1), compressor (2), first preheater (3) bypass heat control valve and pipeline (4), dry desulfurization device (5), high temperature air waste heat recoverer (6), bypass heat control valve and pipeline (8), a preheater of reformation coal gas (7).
C. through the output system of oxidation and reformation reaction after product: this output system includes an interchanger of reformation coal gas (7), reformation coal gas secondary heat exchange device (11), high-temperature water gas conversion device (12), condenser (13), low temperature water gas changing device (14), condenser (15), gas-liquid separator (16), pressure-swing absorption apparatus (17), high purity H and exports (25) and CO
2Tail gas outlet (26);
D. other auxiliary equipments: send the water inlet water pump that (23) are located (24); Graywater outlet pipe (27) by gas-liquid separator (16) discharge.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNA2008100324132A CN101214920A (en) | 2008-01-08 | 2008-01-08 | System and device for preparing hydrogen from coke-oven gas by using mixed conductor oxygen-permeating film reactor |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNA2008100324132A CN101214920A (en) | 2008-01-08 | 2008-01-08 | System and device for preparing hydrogen from coke-oven gas by using mixed conductor oxygen-permeating film reactor |
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| CN101214920A true CN101214920A (en) | 2008-07-09 |
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|---|---|---|---|
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104854021A (en) * | 2012-12-13 | 2015-08-19 | 乔治洛德方法研究和开发液化空气有限公司 | Coproduction of oxygen, hydrogen, and nitrogen using ion transport membranes |
| CN117264661A (en) * | 2023-10-16 | 2023-12-22 | 南京工业大学 | Device and method for producing hydrogen by biomass fuel based on inorganic membrane |
-
2008
- 2008-01-08 CN CNA2008100324132A patent/CN101214920A/en active Pending
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104854021A (en) * | 2012-12-13 | 2015-08-19 | 乔治洛德方法研究和开发液化空气有限公司 | Coproduction of oxygen, hydrogen, and nitrogen using ion transport membranes |
| CN117264661A (en) * | 2023-10-16 | 2023-12-22 | 南京工业大学 | Device and method for producing hydrogen by biomass fuel based on inorganic membrane |
| CN117264661B (en) * | 2023-10-16 | 2024-04-26 | 南京工业大学 | Device and method for producing hydrogen by biomass fuel based on inorganic membrane |
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Open date: 20080709 |