CN101570315B - Method and device for producing hydrogen through biomass gasification by using single fluidized bed and two-step method - Google Patents
Method and device for producing hydrogen through biomass gasification by using single fluidized bed and two-step method Download PDFInfo
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Abstract
The invention belongs to the field of energy. Biomass is used as a raw material, and is added with catalyst calcium carbonate/magnesium carbonate of a carbonate system to react in a fluidized bed; a biomass gasification process is divided into two processes, namely a biomass burning process and a biomass pyrolysis and gasification process, and the two processes work alternately in turn, wherein the burning process comprises that catalyst calcium carbonate/magnesium carbonate granules are added into the fluidized bed, simultaneously air is supplied to the fluidized bed, the air supply to the furnace is stopped when the temperature of the bed layer is raised to a predetermined temperature, and the burning process is finished; then the biomass burning process turns to the gasification process, namely vapor and biomass are supplied to the fluidized bed to obtain hydrogen-rich gas with extremely low tar content; and after the hydrogen-rich gas is washed and purified by coal gas, the hydrogen-rich gas is converted into H2 and CO2 in a CO conversion device, then the gas is desulfurized and compressed, and the H2 is extracted from the gas in a variable pressure adsorption device. The method achieves that the gasification and burning two processes and the cyclic regeneration of a catalyst are finished in the same fluidized bed gasification furnace, the investment is saved, and the running cost is low.
Description
Technical field
The invention belongs to energy field, relate to method and device that a kind of single fluidized bed two step method gasifying biomass is produced hydrogen.
Background technology
The energy is the basic substance of human society survival and development, and consuming excessively of fossil resource causes oil shortage and climate warming, become the significant problem that influences the human society sustainable development, and seeking the oil replacement product becomes whole world common recognition.Biomass energy has environmental friendliness and recyclability, satisfying the Future Society energy demand, will play an important role in the particularly traffic demand for fuel.Hydrogen is the following clean energy carrier of the ideal of generally acknowledging, seeking extensive, cleaning and cheap biomass hydrogen preparation technology is important directions of oil fuel alternate.Biomass hydrogen preparation mainly comprises thermochemical process and bioprocess, and biomass are utilized photodissociation and the fermentation of microorganism, because efficient is low, enzyme liberating is difficult, also is difficult to carry out commercial applications.And the hydrogen manufacturing of biomass thermal chemical transformation because and traditional fossil class hydrogen production process more approaching, the characteristics that efficient is high help large-scale industrial production, help the reduction of hydrogen manufacturing cost, are technology and the very feasible hydrogen production process of giving priority at present.The present invention relates to a kind of hydrogen production process in this field.But biomass pyrogenation gasification prepares in the hydrogen process separately at present, a large amount of tar that low temperature generates have down become an important factor that influences combustion gas quality and hydrogen richness, and therefore taking with water vapour is that gasifying process such as vaporized chemical, high-temperature gasification and increase catalyzer are the directions of present foreign biomolecule matter gasification hydrogen-producing technical study development.As 200310108667.5 patents, it adopts double-fluidized-bed, i.e. fluid-bed combustion furnace, a fluidized-bed gasification furnace with coal or biomass and CaO adding, is cooked vaporized chemical with water vapor and is gasified in vapourizing furnace, burn in roasting kiln with oxygen, material circulates by the device for transporting objects between two stoves, so just realizes that CaO produces hydrogen in the directed gasification of vapourizing furnace, simultaneously CaO and CO
2Produce CaCO through carbonation reaction
3, enter by device for transporting objects then that roasting kiln burns and calcination reaction, CaCO
3Calcine generation CaO after not only but also be admitted to vapourizing furnace as CO
2Receptor.So just realized the cyclic regeneration of CaO.200410064682.9 patents and for example, it is similar with 200310108667.5 patent ultimate principles, all is that employing is double-fluidized-bed, and just its material-transporting system has adopted fly-ash separator, as realizing the circulation of material between two stoves, also realized the cyclic regeneration of CaO simultaneously.But because the restriction of thermal barrier quantity and temperature, the temperature of general pyrolytic gasification bed can not be very high, thereby gasification efficiency is lower, coke and thermal barrier all at high temperature circulate during on the other hand owing to operation, be difficult to quantitative control, bed temperature variation and unstable takes place easily, and these reasons have limited the practicality of double bed evaporating method.
Summary of the invention
The purpose of this invention is to provide a kind of single fluidized bed two step method gasifying biomass and produce the device and method of hydrogen, it hockets the catalytic pyrolysis gasification process of biomass and the combustion processes of biomass in same fluidized-bed successively, to produce the apparatus and method of hydrogen-rich gas.Can realize biomass reduced investment, the mass-producing hydrogen manufacturing purpose that running cost is low, level of automation is high with this method.
Realize that the above-mentioned purpose technical scheme is: be raw material with biomass, and the catalyzer carbonic acid calcium/magnesiumcarbonate that adds carbonate system reacts in fluidized-bed, and biomass gasification process is divided into two processes: the combustion processes of biomass and biomass pyrogenation gasification process.The work that hockets successively of two processes, wherein combustion processes is to add catalyzer carbonic acid calcium/hydrotalcite particle in fluidized-bed, simultaneously air-supplied, at this moment the stove internal adsorption is in lip-deep carbon deposit of lime carbonate/hydrotalcite particle and air generation combustion reactions, the catalyzer of inactivation is regenerated, coke granule makes lime carbonate/hydrotalcite particle that calcination reaction take place in fluidized-bed simultaneously, discharge carbonic acid gas, lime carbonate/hydrotalcite particle then is sintered into calcium oxide/magnesium oxide, bed temperature is raise rapidly, stop in stove air-suppliedly when bed temperature rises to preset temperature, combustion processes finishes.Change gasification over to, at this moment infeed water vapour and biomass to fluidized-bed, the high temperature oxidation calcium/magnesium oxide particle after the calcination and regeneration and the biomass of adding are under fluidized state, the catalytic cracking reaction of pyrolytic gasification reaction and tar takes place under the water vapour effect, generate coke granule, carbonic acid gas in simultaneous oxidation calcium/magnesium oxide and the gas-phase product is cured reaction and generates lime carbonate/magnesiumcarbonate, and to obtain the extremely low hydrogen-rich gas of tar content, bed temperature descends rapidly.When temperature drops to preset temperature, stop in bed, to infeed water vapour, gasification finishes, and fluidized-bed enters combustion processes again.Gasifying biomass and two processes of burning are alternately back and forth carried out work in same fluidized-bed gasification furnace like this, and meanwhile catalyzer carbonic acid calcium/magnesiumcarbonate has also been realized cyclic regeneration in same stove, finally reaches the purpose of producing hydrogen-rich gas.The hydrogen-rich gas of producing out removes dust, tar, H through gas washing, refining plant
2Behind S, the KCl etc., enter the CO changing device, CO is transformed into H
2And CO
2, again by the further desulfurization of smart thionizer, be forced into 0.8MPa (this pressure can be adjusted as required) through gas compressor after desulfurization finishes after, enter transformation absorption PSA-H
2Device, the PSA-H that the unstripped gas of sending into is made up of a plurality of absorption towers
2Operation is extracted H
2PSA-H
2The stripping gas of device is rich in CH
4Can be used for producing and life.Product gas H
2Purify to 99.99% back and comparatively exporting to the user under stable flow rate and the pressure.
The raw material that infeeds in the wherein said combustion processes can comprise suitable coal, and adding proportion is to account for 0～20% of biomass.The catalyzer that adds is granular lime carbonate/magnesiumcarbonate, and adding proportion is to account for 10～30% of biomass.
The operating temperature range of fluidized-bed gasification furnace is: 800～1000 ℃.Combustion processes: 800 ℃～1000 ℃, gasification: 1000 ℃～800 ℃.
Single fluidized bed two step method gasification hydrogen production plant of the present invention, comprise fluidized-bed gasification furnace body and auxiliary equipment, high temperature cyclone separator 4, waste heat boiler and vapor superheater 5, air reversing valve 1-1, steam reversing valve 2-1, flue gas reversing valve 1-2, combustion gas reversing valve 2-2, roots blower 13, fly-ash separator 12, air preheater 11, washing, purifying desulfurizer 6, and hydrogen generating system: carbon monoxide conversion device 7, smart desulfurizer 8, hydrogen gas compressor 9, pressure-swing absorption apparatus 10; Wherein fluidized-bed gasification furnace 3 is provided with two screw feeding devices, i.e. biomass feeding device 1 and catalyzer, coal feeding device 2, and be provided with ash discharge slag device 14 in vapourizing furnace 3 bottoms.At the fluidized-bed gasification furnace entrance end with air reversing valve 1-1, steam reversing valve 2-1, exit end flue gas reversing valve 1-2, combustion gas reversing valve 2-2 is a tie point, and equipment is connected to two work systems, the i.e. firing system of vapourizing furnace and gasification system.Its firing system comprises: the roots blower 13 of Lian Jieing, air preheater 11 successively, air reversing valve 1-1, fluidized-bed gasification furnace body 3, high temperature cyclone separator 4, waste heat boiler and vapor superheater 5, flue gas reversing valve 1-2, air preheater 11, fly-ash separator 12; Gasification system comprises successively the waste heat boiler that connects and vapor superheater 5, steam reversing valve 2-1, fluidized-bed gasification furnace body 3, high temperature cyclone separator 4, waste heat boiler and vapor superheater 5, combustion gas reversing valve 2-2, washing, purifying desulfurizer 6; Washing, purifying desulfurizer 6 backs connect hydrogen generating system, promptly continuous successively carbon monoxide conversion device 7, smart desulfurizer 8, hydrogen gas compressor 9, pressure-swing absorption apparatus 10.
Advantage of the present invention:
(1) in single fluidized bed because whole gasification is decomposed into combustion processes and pyrolytic gasification process, be oxygenant in combustion processes with the air, and the pyrolytic gasification process is vaporized chemical with the pure water vapor, thereby can obtains high-quality hydrogen-rich gas.Because without oxygen generating plant, reduced investment, running cost are low.
(2) because production process is divided into two processes, can regulates respectively and make up, to obtain best product gas component according to the characteristics of process.The low grade coal that can select poor activity for use as combustion processes is as raw material, and the pyrolytic gasification process can select for use the biomass that are easy to gasify as raw material, helps the mixing gasifying and the reasonable resources utilization of two raw materials like this.
(3) adopt the two-step approach gasification, realized that carbonate system (Wingdale, rhombspar etc.) catalyzer is at single fluidized bed cyclic regeneration.
Adopting carbonate system (Wingdale, rhombspar etc.) is catalyzer, burn at single fluidized bed internal combustion stage blowing air, deactivated catalyzer is regenerated, on the other hand, the high temperature that the coke burning produces impels catalyzer to carry out calcining and decomposing, makes Wingdale, rhombspar etc. be sintered into CaO/MgO.Combustion phases enters gasifying stage after finishing, and the CaO/MgO that is sintered into, biomass, coal and water vapor generation strong reaction make biomass moment generation pyrolysis and water-gas reaction, generate H
2, CO, CO
2, CH
4, C
nH
mAnd tar, catalytic pyrolysis takes place rapidly in the tar that the CaO/MgO catalyzer produces pyrolysis in the furnace charge, and catalyzed reaction CO+H takes place under the CaO/MgO catalyst action simultaneously
2→ CO
2+ H
2, CO wherein
2Then be cured reaction, generate CaCO with CaO/MgO
3/ MgCO
3After gasifying stage finishes, the CaCO of generation
3/ MgCO
3Enter combustion phases again in same bed, carry out calcination and regeneration, constantly circulation comes and goes, and has realized carbonate system (Wingdale, the rhombspar etc.) recycling of catalyzer in single fluidized bed.
Description of drawings
Accompanying drawing is single fluidized bed two step method process for making hydrogen flow process and device thereof, wherein has: 1, biomass silo and screw feeding device 2, catalyzer, coal charge storehouse and screw feeding device 3, fluidized-bed gasification furnace 4, high temperature cyclone separator 5, waste heat boiler and vapor superheater 6, washing, purifying desulfurizer 7, carbon monoxide conversion device 8, smart desulfurizer 9, hydrogen gas compressor 10, pressure-swing absorption apparatus 11, air preheater 12, fly-ash separator 13, roots blower 14, ash discharge slag device 1-1, air reversing valve 1-2, flue gas reversing valve 2-1, steam reversing valve 2-2, the combustion gas reversing valve
Embodiment
Single fluidized bed two step method gasification hydrogen production plant of the present invention is a core with fluidized-bed gasification furnace 3, and fluidized-bed gasification furnace 3 is provided with two screw feeding devices, i.e. biomass feeding device 1 and coal feeding device 2, and ash discharge slag device 14.At the fluidized-bed gasification furnace entrance end with air reversing valve 1-1, steam reversing valve 2-1, exit end flue gas reversing valve 1-2, combustion gas reversing valve 2-2 is a tie point, and equipment is connected to two work systems, the i.e. firing system of vapourizing furnace and gasification system.Its firing system comprises: the roots blower 13 of Lian Jieing, air preheater 11 successively, air reversing valve 1-1, fluidized-bed gasification furnace body 3, high temperature cyclone separator 4, waste heat boiler and vapor superheater 5, flue gas reversing valve 1-2, air preheater 11, fly-ash separator 12, and be provided with ash discharge slag device 14 in vapourizing furnace 3 bottoms; Gasification system comprises successively the waste heat boiler that connects and vapor superheater 5, steam reversing valve 2-1, fluidized-bed gasification furnace body 3, high temperature cyclone separator 4, waste heat boiler and vapor superheater 5, combustion gas reversing valve 2-2, washing, purifying desulfurizer 6; Washing, purifying desulfurizer 6 backs connect hydrogen generating system, promptly continuous successively carbon monoxide conversion device 7, smart desulfurizer 8, hydrogen gas compressor 9, pressure-swing absorption apparatus 10.
During this device operation; by screw feeding device 1 biomass are joined in the fluidized-bed gasification furnace 3; join in the fluidized-bed gasification furnace 3 with catalyzer carbonic acid calcium particle or with coal by coal feeding device 2; through air preheater 11, air reversing valve 1-1 sends into fluidized-bed gasification furnace 3 to roots blower 13 with air, burns under fluidized state with the particulate material of biomass coke in the stove and coal, catalyzer; bed temperature is risen rapidly; at this moment, calcium carbonate granule decomposes through high-temperature calcination, discharges CO
2, calcium carbonate granule then is sintered into calcium oxide, and high temperature oxidation calcium particle and remaining coke that the burning back generates provide catalyzer and thermal source for next step biomass pyrogenation gasification.The high-temperature flue gas that produces carries out just separating through high temperature cyclone separator 4, and granules of catalyst under separating and carbon containing ash particle return utilization again in the stove through the material-returning device of high temperature cyclone separator 4.And flue gas enters waste heat boiler and vapor superheater 5 carries out heat exchange, cools to 400 ℃ after flue gas reversing valve 1-2 enters air preheater 11 and fly-ash separator 12, enters in the atmosphere after the purification.When bed temperature rises to preset temperature, air reversing valve 1-1, flue gas reversing valve 1-2 closes in succession, and combustion processes finishes.And steam reversing valve 2-1, combustion gas reversing valve 2-2 opens in succession to fluidized-bed gasification furnace 3 and infeeds water vapour, and vapourizing furnace changes the pyrolytic gasification process over to.At this moment biomass feeding device 1 adds the biological particles material to vapourizing furnace 3, make raw material under fluidized state, under the effect of catalyst oxidation calcium particle, react with water vapour generation pyrolytic gasification, generate the hydrogen-rich gas that does not contain tar, simultaneously, calcium oxide particle is cured reaction with carbonic acid gas again, emits heat, generate calcium carbonate granule, and quicken the carrying out of biomass-making H-H reaction.Because above-mentioned reaction is thermo-negative reaction generally, make temperature decline in the stove, when temperature drops to preset temperature, gasifying stage finishes, steam reversing valve 2-1, and combustion gas reversing valve 2-2 closes in succession, air reversing valve 1-1, flue gas reversing valve 1-2 opens in succession, and vapourizing furnace changes combustion processes again over to.The hydrogen-rich gas that gasification produces enters waste heat boiler and vapor superheater 5 after high temperature cyclone separator 4 roughing out, the heat exchange cooling is after combustion gas reversing valve 2-2, enter washing, purifying desulfurizer 6, carbon monoxide conversion device 7, behind the smart desulfurizer 8, by hydrogen gas compressor 9 input pressure-swing absorption apparatuss 10, produce the hydrogen supply user at last.In gasification, required steam gasification agent can be satisfied by the water vapour that waste heat boiler 5 produces.
In whole biomass hydrogen preparation process, two processes alternately back and forth reach the purpose of producing hydrogen.In combustion processes, add calcium carbonate granule (or coal) and air, fluidized-bed is in 800～1000 ℃ of temperature rise periods, and this process calcium carbonate granule calcining and decomposing generates calcium oxide particle, improves bed temperature, for next step biomass pyrogenation gasification is prepared.In the pyrolytic gasification process, add biomass and water vapour, fluidized-bed is in 1000～800 ℃ temperature-fall period, make biomass under the effect of catalyzer, carry out the pyrolytic gasification reaction, be cured reaction with carbonic acid gas again simultaneously, emit heat, generate calcium carbonate granule, and the carrying out that quickens the biomass-making H-H reaction, thereby obtain the extremely low hydrogen-rich gas of tar content, through the separable pure hydrogen gas that goes out more than 99% of CO conversion, pressure-swing absorption apparatus.Following table is the experimental data of a plurality of embodiment, wherein S/B=water vapour/biomass: biomass: corn cob;
Above-mentioned experiment method only is used to illustrate the technical program, and is not limited.
Claims (5)
1. single fluidized bed two step method is produced the method for hydrogen, it is characterized in that being:
With biomass is that raw material reacts in fluidized-bed, and biomass gasification process is divided into two processes: the combustion processes of biomass and biomass pyrogenation gasification process; The work that hockets successively of two processes, wherein combustion processes is air-supplied in fluidized-bed, stops in stove air-suppliedly when bed temperature rises to preset temperature, combustion processes finishes; Change gasification over to, at this moment infeed water vapour and biomass to fluidized-bed, to obtain hydrogen-rich gas, bed temperature descends rapidly; Fluidized-bed enters combustion processes again; After the hydrogen-rich gas process gas washing of producing out, the purification, enter the CO changing device again and be transformed into H
2And CO
2, after smart desulfurization, pressurization, enter pressure-swing absorption apparatus again, extract H
2And in combustion processes, in fluidized-bed, add catalyzer carbonic acid calcium/hydrotalcite particle simultaneously.
2. single fluidized bed two step method according to claim 1 is produced the method for hydrogen, it is characterized in that the operating temperature range that is fluidized-bed gasification furnace is: 800～1000 ℃; Combustion processes: 800 ℃～1000 ℃, gasification: 1000 ℃～800 ℃, the catalyzer adding proportion is to account for 10～30% of biomass.
3. single fluidized bed two step method according to claim 1 is produced the method for hydrogen, and it is characterized in that adding simultaneously in the fluidized-bed gasification furnace a certain amount of coal is raw material, and adding proportion is to account for 0～20% of biomass.
4. realize the device of the described method of claim 1, it is characterized in that comprising fluidized-bed gasification furnace body and auxiliary equipment, high temperature cyclone separator (4), waste heat boiler and vapor superheater (5), air reversing valve (1-1), steam reversing valve (2-1), flue gas reversing valve (1-2), combustion gas reversing valve (2-2), roots blower (13), fly-ash separator (12), air preheater (11), washing, purifying desulfurizer (6), and hydrogen generating system: carbon monoxide conversion device (7), smart desulfurizer (8), hydrogen gas compressor (9), pressure-swing absorption apparatus (10); Wherein fluidized-bed gasification furnace is provided with two screw feeding devices, i.e. biomass feeding device (1), coal feeding device (2), and be provided with ash discharge slag device (14) in the fluidized-bed gasification furnace bottom; At the fluidized-bed gasification furnace entrance end with air reversing valve (1-1), steam reversing valve (2-1), exit end flue gas reversing valve (1-2), combustion gas reversing valve (2-2) is a tie point, and equipment is connected to two work systems, the i.e. firing system of vapourizing furnace and gasification system; Its firing system comprises: the roots blower of Lian Jieing (13), air preheater (11) successively, air reversing valve (1-1), the fluidized-bed gasification furnace body, high temperature cyclone separator (4), waste heat boiler and vapor superheater (5), flue gas reversing valve (1-2), air preheater (11), fly-ash separator (12); Gasification system comprises successively the waste heat boiler that connects and vapor superheater (5), steam reversing valve (2-1), fluidized-bed gasification furnace body, high temperature cyclone separator (4), waste heat boiler and vapor superheater (5), combustion gas reversing valve (2-2), washing, purifying desulfurizer (6); Washing, purifying desulfurizer (6) back connects hydrogen generating system, promptly continuous successively carbon monoxide conversion device (7), smart desulfurizer (8), hydrogen gas compressor (9), pressure-swing absorption apparatus (10).
5. device according to claim 4 is characterized in that described fluidized-bed gasification furnace body adopts circulating fluidized bed or bubbling fluidized bed.
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| CN111377398A (en) * | 2018-12-28 | 2020-07-07 | 中国石油化工股份有限公司 | Method for preparing hydrogen and carbon monoxide by biomass pyrolysis and gasification |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111377398A (en) * | 2018-12-28 | 2020-07-07 | 中国石油化工股份有限公司 | Method for preparing hydrogen and carbon monoxide by biomass pyrolysis and gasification |
| CN111377398B (en) * | 2018-12-28 | 2022-02-08 | 中国石油化工股份有限公司 | Method for preparing hydrogen and carbon monoxide by biomass pyrolysis and gasification |
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Granted publication date: 20110601 Termination date: 20200615 |