CN103204464A - Cellular oxygen carrier chemical-looping reforming reactor - Google Patents
Cellular oxygen carrier chemical-looping reforming reactor Download PDFInfo
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- CN103204464A CN103204464A CN2013101083238A CN201310108323A CN103204464A CN 103204464 A CN103204464 A CN 103204464A CN 2013101083238 A CN2013101083238 A CN 2013101083238A CN 201310108323 A CN201310108323 A CN 201310108323A CN 103204464 A CN103204464 A CN 103204464A
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Abstract
The invention discloses a cellular oxygen carrier chemical-looping reforming reactor. The cellular oxygen carrier chemical-looping reforming reactor comprises a reactor main body which comprises an outer wall and an outer heating barrel, wherein cellular oxygen carriers are formed in the outer wall and the outer heating barrel and are jointed with the outer wall and the inner wall of the outer heating barrel, and cellular pore paths parallel to the outer wall and a main shaft of the outer heating barrel are arranged in the cellular oxygen carrier and are pairwise spaced; and the tops of the outer wall and the outer heating barrel are connected with a top gas collecting region through upper flanges, the bottoms of the outer wall and the outer heating barrel are connected with a bottom gas storage region through lower flanges, a tail gas outlet is connected outside the top gas collecting region, a tee-junction gas inlet is connected outside the bottom gas storage region, and the bottom gas storage region is internally provided with a radiation type gas pre-distribution device connected with the tee-junction gas inlet. The cellular oxygen carriers have the advantages of having heat storage function, being capable of helping the reactor to maintain reaction temperature, alleviating the thermal load of external heating equipment and being beneficial to the stable proceeding of reaction.
Description
Technical field
The present invention relates to fuel clean burning, functional materials, environmental protection technical field, particularly a kind ofly can carry out CH efficiently, at low cost
4The cellular oxygen carrier reactor reformed of chemical chain.
Background technology
Methane is the main component of Sweet natural gas, coal-seam gas and gas hydrate, exhaustion day by day along with petroleum resources, the abundant relatively methane resource of reserves will become one of back petroleum times tool substitute energy of wishing, exploration shows that China's coal-seam gas reserves are about 35,000,000,000,000 m
3, the Sweet natural gas prospective reserves reaches 43,000,000,000,000 m
3, therefore, research and development are economical, the methane conversion technology has great strategic importance efficiently.And be that an important channel of liquid fuel and chemical is to be synthetic gas (H with methane conversion at first with methane conversion
2+ CO), through means such as Fischer-Tropsch synthesize synthetic gas further is converted into liquid fuel and chemical again, so synthetic gas is gas chemical industry's important intermediate.
Traditional gas renormalizing is by methane and water vapour (steam methane reforming, SMR) or CO2 (carbon dioxide reforming, CDR) reforming reaction takes place and generate synthetic gas, again by liquid fuels such as synthetic gas hydrogen manufacturing, methyl alcohol, synthetic ammonia and gasoline etc.SMR and CDR are strong thermo-negative reaction, the equipment bulky complex, and the process cost costliness, wherein synthesis gas preparation accounts for the 60%-70% of whole gas chemical industry's gross investment and production cost.Therefore, research is more economical, the methane conversion technology just seems extremely urgent more efficiently.
It is a kind of methane preparing synthetic gas technology that development in recent years is got up that methane chemistry chain is reformed, and its essence is methane portion oxidation synthesis gas.It is the principle of reacting according to chemical looping that the chemistry chain is reformed, and utilizes the lattice oxygen in the metal oxide molecule as oxygen source methane portion oxidation to be become synthetic gas; Then, the metal oxide that loses lattice oxygen oxidation by air again recovers lattice oxygen, finishes the chain type circulating reaction.As seen, at methane chemistry chain reformation and methane steam or CO
2Reformation is compared, and has saved pure oxygen and has prepared link, is the thermopositive reaction of a gentleness, can realize high conversion and the H of methane under the condition of less energy-consumption
2, CO highly selective, have less investment, efficient height, low power consumption and other advantages, but also avoided methane directly to contact the danger that may blast with gas phase oxygen.
It is pointed out that traditional methane reforming circulating fluid bed reactor needs constantly to drive catalyzer and circulates fast, not only energy consumption is bigger, and is also very serious to the wearing and tearing of equipment, is difficult for realizing isothermal operation simultaneously.And a kind of good methane reforming reaction apparatus is not only wanted to realize fuel reforming efficiently, also should be taken into account the energy consumption of device and the isothermal operation of reaction.
Summary of the invention
The object of the present invention is to provide a kind of novel methane reforming reaction device, do not need the preparation of pure oxygen, do not need to promote catalyzer and circulate answering between the device, cut down the consumption of energy, reaction temperature and, realize the operation of isothermal easily, reach the purpose that the highly effective and safe of raw material utilizes.
For realizing above purpose, the present invention has taked following technical scheme: a kind of cellular oxygen carrier chemistry chain reforming reactor, use cellular oxygen carrier reactor alternately to realize the reformation of methane and the regenerative response of oxygen carrier, comprise reactor body, described reactor body comprises outer wall and outer heating cylindrical shell, be formed with cellular oxygen carrier in outer wall and the outer heating cylindrical shell, cellular oxygen carrier is connected heating cylinder inboard wall outside outer wall reaches, be provided with the cellular duct parallel with outer wall and outer heating cylindrical shell main shaft in the cellular oxygen carrier, described cellular duct in twos at interval; Described outer wall and outer heating cylindrical shell top are connected with the top gas collecting region by upper flange, the bottom is connected with atmosphere storage district, bottom by lower flange, described top gas collecting region is externally connected with the tail gas outlet, be used for connecting heat-exchange equipment and synthetic gas cleaning system, store or enter synthesizing section after the synthetic gas pressurization after purifying, atmosphere storage district, bottom is externally connected with the threeway gas inlet, be used for connecting respectively atmosphere storage, pressurization and treating plant are provided with in the bottom atmosphere storage district and are connected with the threeway gas inlet and distribute for the gas that the threeway gas inlet is entered again, make gas enter the radiation formula gas pre-distributor in cellular duct uniformly and stably.
Cellular oxygen carrier is fixed in the middle of the reactor, inlet gas through with pre-distributor after alternately enter oxygen carrier and carry out fuel reforming, gas purging, air regenesis.When fuel feeds reactor, fuel under the state of no oxygen by the lattice oxygen partial oxidation on the cellular oxygen carrier wall, obtain crude synthesis gas after the reformation, when air reaction, airborne gaseous oxygen molecule and the honeycomb oxygen carrier reaction that is reduced, fill up the lattice oxygen room on oxygen carrier surface, make oxygen carrier be recovered lattice oxygen by oxidation again, generally, oxygen carrier oxidation by air process is a heat release thermopositive reaction, and heat is except a part is taken away by tail gas, and another part is stored in the cellular oxygen carrier, offer the required heat of methane reforming, thus guarantee reaction continue carry out.The inert gas purge residual gas that hockets in air reaction and fuel reaction gap guarantees that reaction safety carries out.
Fuel, air alternately carries out the transmission of lattice oxygen and heat by the oxygen carrier duct, realizes the reformation of fuel.Cellular duct oxygen carrier, material forms for the composite transition metal oxide compacting sintering.
The reactor outer wall is cylindrical, the whole hearth-type heating of outside employing, the upper gas collection device is connected with top, reactor top and the bottom with the pre-distribution apparatus of lower gas entrance, cellular oxygen carrier is fixed in the middle of the reactor, limit wall and the clamping of reactor outer wall phase are convenient to the oxygen carrier life-span to change whole cellular oxygen carrier when using up.
Oxygen carrier is whole to be cylindrical, and by many cellular passages of centre isometrical distribution to the periphery, each passage is parallel with main shaft.Polynuclear plane has a large amount of rooms and bigger surface-area, absorption that can be reversible when high temperature and transmission oxygen, fuel is had advantages of high catalytic activity, have good thermodynamic stability and suitable physical strength, negatively charged ion, electronics, room are demonstrated the transport properties of mixed type.
During operation, fuel (CH
4), air, rare gas element (N
2) alternately enter reactor through the threeway gas inlet of reactor bottom.At first from the fuel (CH of bottom
4) enter the radiation formula gas pre-distributor through entrance, after sparger was uniformly dispersed, fuel and oxygen carrier reacted, and the lattice oxygen in the oxygen carrier makes CH
4Partial oxidation generates CO and H
2Be the synthetic gas of main ingredient, behind gas collector, discharged by outlet, after waste heat boiler obtains heat, behind the isolation of purified system purification, obtain purer synthetic gas; Behind the reaction certain hour, close the fuel air mouth, open the rare gas element outlet, rare gas element enters reactor through the radiation formula gas pre-distributor, purge unreacting gas remaining in the oxygen carrier, outlet tail gas enters atmosphere behind waste heat boiler or interchanger recovery heat; After purging is finished, close inert gas entrance, open gas inlet, airborne gaseous oxygen and oxygen carrier reaction are recovered the lattice oxygen in the oxygen carrier, and carry out thermal exchange with oxygen carrier, guarantee reaction continue carry out, outlet tail gas enters atmosphere behind waste heat boiler or interchanger recovery heat, so alternately feed fuel, rare gas element, air, and reaction cycle is carried out.
The present invention adopts cellular oxygen carrier reactor to carry out methane chemistry chain and reforms and produce synthetic gas, by oxygen carrier to CH
4Carry out the transmission of lattice oxygen and heat, need not the pure oxygen preparation, do not need to drive the quick circulation of solid particulate, can under the condition of less energy-consumption, realize high conversion and the H of methane
2, CO highly selective, be easy to simultaneously to realize to continue and the operation of isothermal, solved expensive that current reaction unit exists, high energy consumption is difficult for the problem of constant temperature method.
The present invention compared with prior art has following advantage: 1) methane chemistry chain is reformed and traditional water vapor or CO
2Reformation is compared, and has saved water vapour and pure oxygen prepares link, and cost significantly reduces; 2) be easy to the isothermal operation of realization response, but also avoided methane directly to contact the danger that to blast with gas phase oxygen; 3) do not need to drive granules of catalyst and circulate in reactor, energy waste is low, and service life of equipment is long.When 4) oxygen carrier is regenerated, replace air as using water vapour, steam cracking can generate comparatively pure hydrogen, can be used for fuel cell.5) cellular oxygen carrier has heat accumulation function in reaction, can help reactor to keep temperature of reaction, alleviates the thermal load of outer heating equipment, stable the carrying out that is conducive to react.
Description of drawings
Fig. 1 a is oxygen carrier channel flow synoptic diagram ();
Fig. 1 b is oxygen carrier channel flow synoptic diagram (two);
Fig. 2 is cellular oxygen carrier schematic cross-section;
Fig. 3 is cellular oxygen carrier reactor synoptic diagram;
Description of reference numerals: 1, threeway gas inlet; 2, radiation formula gas pre-distributor; 3, bottom atmosphere storage district; 4, lower flange; 5, outer wall and outer heating cylindrical shell; 6, cellular oxygen carrier; 7, cellular oxygen carrier duct; 8, upper flange; 9, top gas collecting region; 10, tail gas outlet.
Embodiment
Below in conjunction with the drawings and specific embodiments content of the present invention is described in further details.
As shown in Figure 3, a kind of cellular oxygen carrier chemistry chain reforming reactor, whole reactor is cylindrical, comprise reactor body, reactor body comprises for the outer wall of control reactor reaction temperature and outer heating cylindrical shell 5, be formed with cellular oxygen carrier 6 in outer wall and the outer heating cylindrical shell 5, airborne gaseous oxygen, partial reaction heat in the lattice oxygen that fuel is required and the fuel reaction district advances exchange by cellular oxygen carrier 6, cellular oxygen carrier synoptic diagram such as Fig. 1, shown in Figure 2, cellular oxygen carrier 6 is connected heating cylindrical shell 5 inwalls outside outer wall reaches, be provided with the cellular duct 7 parallel with outer wall and outer heating cylindrical shell 5 main shafts in the cellular oxygen carrier 6, cellular duct 7 in twos at interval; Outer wall and outer heating cylindrical shell 5 tops are connected with top gas collecting region 9 by upper flange 8, the bottom is connected with atmosphere storage district, bottom 3 by lower flange 4, top gas collecting region 9 is externally connected with tail gas outlet 10, be used for to connect heat-exchange equipment and synthetic gas cleaning systems such as waste heat boiler, the synthetic gas pressurized storage after the purification or enter synthesizing section; Atmosphere storage district, bottom 3 is externally connected with threeway gas inlet 1, be used for connecting respectively storage, pressurization and the treating plant of gas with various, be provided with in the bottom atmosphere storage district 3 and be connected with threeway gas inlet 1 and distribute, make gas to enter the radiation formula gas pre-distributor 2 in cellular duct 7 uniformly and stably again for the gas that threeway gas inlet 1 is entered.
Cellular oxygen carrier is made by composite transition metal oxide, have a large amount of oxygen rooms on the structure and have bigger specific surface area, by the isometrical evenly distributed cylindrical bore of middle mind-set periphery, duct and axially parallel, absorption that can be reversible when high temperature and transmission oxygen, fuel such as methane had advantages of high catalytic activity, have good thermodynamic stability and suitable physical strength, negatively charged ion, electronics, room are demonstrated the transport properties of mixed type, therefore, suiting to carry out chemical chain in the oxygen carrier reactor reforms.Existing experiment shows that the composition metal thing can be reformed for the chemical chain of methane enough lattice oxygen are provided, and has outstanding structural stability and good oxidation reduction cycle reactive behavior.
In sum, this device has adopted cellular oxygen carrier and air, the methane alternation response design carry out methane reforming and produce synthetic gas, transmit lattice oxygen and heat by cellular oxygen carrier, in operational process, only need the air input of fuel metering gas reactor entrance 1, gas flow rate and temperature of reaction can realize the stable isothermal operation that continues, do not need the pure oxygen preparation, do not need to drive the required big energy consumption of granules of catalyst circulation, prolonged the work-ing life of reactor wall, avoided methane directly to contact the danger that to blast with gas phase oxygen, it is big to have solved the energy consumption that exists in the current fluidized-bed reactor preferably, easy to wear, fluctuation of service, the problem that temperature each point fluctuation is bigger, as in the reactor during oxygen carrier regeneration with the water replaces air, also can obtain comparatively pure hydrogen, can be used for fuel cell.
Embodiment one:
Choosing LaFeO3 is the oxygen carrier material, makes reactor oxygen carrier 6 behind the high temperature compacting sintering.Oxygen carrier is cylindrical, diameter 1000mm, high 2000mm, in diameter is arranged is the cellular duct 7 of 3mm, the duct is parallel with the cylinder main shaft.Oxygen carrier is connected in reactor outer wall 5, and (904L) makes by the high temperature resistant stainless steel material, and the reactor outer wall provides heat by the hearth-type heating system.Reactor bottom atmosphere storage district 3, reactor head plenum zone 9 diameter 1000mm, high 300mm.Reactor bottom gas inlet 1 is controlled by three-way solenoid valve.
During operation, open the outer heating of reactor system, 850 ℃-900 ℃ of control reactors, fuel (CH
4), air, rare gas element (N2) alternately enter reactor through the threeway gas inlet 1 of reactor bottom.At first open N in the reactor bottom gas inlet 1
2 Purge 5 minutes, gas flow 80L/h closes N2 afterwards, opens the fuel inlet in 1, from the CH of reactor bottom
4Enter radiation formula gas pre-distributor 2, gas flow 120L/h after advancing sparger and being uniformly dispersed, flows from bottom to top at the cellular oxygen carrier passage 7 in the pressure lower edge of self, fuel and oxygen carrier 6 react during high temperature, and lattice oxygen is come partial oxidation reformation CH in the use oxygen carrier
4, generate CO and H
2Be the synthetic gas of main ingredient, methane conversion surpasses 90%, CO and H
2Near 1:2, synthetic gas is discharged by outlet 10 behind plenum zone 9, after waste heat boiler obtains heat, obtains purer synthetic gas behind the isolation of purified system purification, stores or enter synthesizing section after the pressurization; React after 30 minutes, close fuel air, open N2 gas entrance, purged remaining unreacting gas 5 minutes, tail gas is discharged through top exit 10, and the gas after the discharge enters atmosphere behind waste heat boiler or interchanger recovery heat; After purging is finished, close inert gas entrance, open the gas inlet in 1, air enters reactor through gas distributor 2, cellular oxygen carrier road, pressure lower edge 7 at self flows from bottom to top, flow is 180L/h, airborne gaseous oxygen and oxygen carrier 6 react during high temperature, and the lattice oxygen in the oxygen carrier 6 is recovered, and carry out thermal exchange with oxygen carrier, promote reaction continue carry out, reaction times is 10 minutes, and tail gas is discharged through exporting 10, enters atmosphere again behind waste heat boiler or interchanger recovery heat, so alternately feed fuel, rare gas element, air, reaction continue circulation and carry out.See accompanying drawing 4.
Embodiment two
Because each embodiment operating process is identical with device, concrete implementation and operation process is identical with embodiment one, repeats no more herein, only lists implementation condition and result of implementation in following table.
Embodiment three
Because each embodiment operating process is identical with device, concrete implementation and operation process is identical with embodiment one, repeats no more herein, only lists implementation condition and result of implementation in following table.
Above-listed detailed description is at the specifying of possible embodiments of the present invention, and this embodiment is not in order to limiting claim of the present invention, and the equivalence that all the present invention of disengaging do is implemented or change, all should be contained in the claim of this case.
Claims (1)
1. cellular oxygen carrier chemistry chain reforming reactor, comprise reactor body, reactor body comprises for the outer wall of control reactor reaction temperature and outer heating cylindrical shell (5), be formed with cellular oxygen carrier (6) in outer wall and the outer heating cylindrical shell (5), cellular oxygen carrier (6) is connected heating cylindrical shell (5) inwall outside outer wall reaches, be provided with the cellular duct (7) parallel with outer wall and outer heating cylindrical shell (5) main shaft in the cellular oxygen carrier (6), cellular duct (7) are the interval in twos; Outer wall and outer heating cylindrical shell (5) top are connected with top gas collecting region (9) by upper flange (8), the bottom is connected with atmosphere storage district (3), bottom by lower flange (4), top gas collecting region (9) is externally connected with tail gas outlet (10), atmosphere storage district, bottom (3) is externally connected with threeway gas inlet (1), is provided with in the bottom atmosphere storage district (3) to be connected with threeway gas inlet (1) and to distribute, make gas to enter the radiation formula gas pre-distributor (2) in cellular duct (7) uniformly and stably again for the gas that threeway gas inlet (1) is entered.
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| CN104129754A (en) * | 2014-07-09 | 2014-11-05 | 中国科学院广州能源研究所 | Biomass pyrolysis and chemical chain hydrogen production coupled continuous reaction device and method for producing hydrogen gas with biomass pyrolysis and chemical chain hydrogen production coupled continuous reaction device |
| CN107847893A (en) * | 2015-07-07 | 2018-03-27 | 泰恩河畔纽卡斯尔大学 | Chemical cyclization |
| CN108855109A (en) * | 2018-07-02 | 2018-11-23 | 西北大学 | A kind of chemical chain partial oxidation methane preparing synthetic gas carrier of oxygen and its preparation method and application |
| CN109092374A (en) * | 2018-09-14 | 2018-12-28 | 昆明理工大学 | A kind of preparation method of the honeycomb carrier of oxygen |
| CN113217986A (en) * | 2021-04-30 | 2021-08-06 | 董荣华 | Chemical heat accumulator and heating system adopting same |
| CN114408865A (en) * | 2022-03-01 | 2022-04-29 | 浙江浙能技术研究院有限公司 | Chemical chain methane reforming hydrogen production device |
| CN114477086A (en) * | 2022-01-27 | 2022-05-13 | 北京联力源科技有限公司 | Methanol steam reforming hydrogen production device and starting method thereof |
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| CN113217986A (en) * | 2021-04-30 | 2021-08-06 | 董荣华 | Chemical heat accumulator and heating system adopting same |
| CN114477086A (en) * | 2022-01-27 | 2022-05-13 | 北京联力源科技有限公司 | Methanol steam reforming hydrogen production device and starting method thereof |
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Application publication date: 20130717 |