CN1277740C - Process of catalyzing and gasifying fresh substance by solid thermophore for preparing hydrogen-rich gas - Google Patents
Process of catalyzing and gasifying fresh substance by solid thermophore for preparing hydrogen-rich gas Download PDFInfo
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- CN1277740C CN1277740C CNB031337996A CN03133799A CN1277740C CN 1277740 C CN1277740 C CN 1277740C CN B031337996 A CNB031337996 A CN B031337996A CN 03133799 A CN03133799 A CN 03133799A CN 1277740 C CN1277740 C CN 1277740C
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- 239000007789 gas Substances 0.000 title claims abstract description 24
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- 238000000034 method Methods 0.000 title abstract description 23
- 230000008569 process Effects 0.000 title abstract description 13
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- 239000003054 catalyst Substances 0.000 claims abstract description 34
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- 230000003197 catalytic effect Effects 0.000 claims abstract description 18
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- 238000011069 regeneration method Methods 0.000 claims abstract description 15
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 19
- 239000000969 carrier Substances 0.000 claims description 14
- 229910052799 carbon Inorganic materials 0.000 claims description 13
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 12
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/584—Recycling of catalysts
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- Hydrogen, Water And Hydrids (AREA)
Abstract
本发明涉及在生物质中提取氢气的方法，尤其是一种固体热载体催化气化生物质制取富氢气体的方法。由固体热载体催化剂与生物质混合加热、生物质快速热解、催化气化、催化剂固体颗粒加热再生循环构成。催化剂作为固体热载体，在连续再生过程中同时也积蓄了生物质气化所需的热量。该工艺装置由移动床反应器、加料器、再生提升管、催化剂储槽等组成。本发明使生物质中的氢最大程度地转化为产品氢气，催化剂连续无切换再生解决了催化剂快速失活问题，焦油产量少，操作简单，产气纯度高，是极具潜力的新工艺。
The invention relates to a method for extracting hydrogen from biomass, in particular to a method for preparing hydrogen-rich gas by catalytically gasifying biomass with a solid heat carrier. It is composed of solid heat carrier catalyst and biomass mixed heating, biomass rapid pyrolysis, catalytic gasification, catalyst solid particle heating regeneration cycle. As a solid heat carrier, the catalyst also accumulates the heat required for biomass gasification during the continuous regeneration process. The process device is composed of moving bed reactor, feeder, regeneration riser, catalyst storage tank and so on. The invention maximizes the conversion of hydrogen in biomass into product hydrogen, and the continuous non-switching regeneration of the catalyst solves the problem of rapid catalyst deactivation. The method has low tar output, simple operation and high gas purity, and is a new process with great potential.
Description
Technical field
The present invention relates to a kind of method of extracting hydrogen in biomass, especially a kind of solid thermal carriers catalytic gasification biomass are produced the method for hydrogen-rich gas.
Background technology
Hydrogen is a kind of important chemical material, also is the clean fuel that can be used for fuel cell and oil engine simultaneously.Hydrogen is mainly derived from two approach, the i.e. conversion of water electrolysis and hydrocarbon polymer.The main technique of hydrogen manufacturing at present is the water vapor catalytic reforming of Sweet natural gas (methane), lower carbon number hydrocarbons or petroleum naphtha, and the partial oxidation of heavy oil residual oil and gasification also are alternative technology.Be subjected to the restriction of raw material supplying based on the process for making hydrogen of Sweet natural gas or other fossil oils, in the long term, hydrogen feedstock should be based on renewable resources.
Biomass (comprising timber, agricultural crop straw etc.) are important renewable resources, are world's fourth largest energy, and 14% primary energy source is being provided.China's 1998 output of being only agricultural crop straw just reach 8.1 hundred million tons, are equivalent to 3.9 hundred million tons of standard coals, account for 32.1% of total output of primary energy.Biomass are different from coal and oil as the sun power carrier, and its S content is relatively very low, and the clean discharging of energy conversion process greenhouse gases is zero.Hydrogen producing technology based on biomass is eco-friendly Sustainable development technology.
The typical quality group of biomass wooden fuel becomes: C 48%, and O 45%, H 6% and small amount of N, S and mineral substance.Consider principal element, the molecular composition of biomass can be expressed as CH
1.5O
0.7, can calculate the theoretical yield of hydrogen on this basis.If biomass and hydrogenous material reaction, then the hydrogen productive rate is higher than biomass maximum hydrogen content 6%.The water vapor gasification that typical process is biomass:
Can calculate maximum hydrogen output 165gH by above reaction path
2/ (kg biomass).
(1), (2) reaction net heat effect is heat absorption, fully must extra heat supply for reaction is carried out.Can by the biomass partial combustion to provide heat requirement.The biological quality that is used to reaction institute heat requirement is provided in gasification is up to 30-40%, and the hydrogen in this part biomass runs off with the form of water:
Reaction (1) is H
2C-O is compared in the reaction of O-biomass
2And C-CO
2Reaction is slow, and rising temperature of reaction, increase water vapor amount can be accelerated H
2O-biomass speed of response also shortens residence time of its product.Therefore, hydrogen productive rate, energy consumption, type of reactor and investment are mutual restriction in the biomass hydrogen preparation process.
General catalytic pyrolysis of biomass/gasifying reactor form is fixed bed and fluidized-bed at present, sees that from obtaining the hydrogen-rich gas purpose all there is deficiency separately in they.Catalyzer closely contacts with biomass in the fixed bed, helps producing hydrogen-rich gas, but fixed bed is difficult to reach fast pyrogenation, and the catalyst deactivation problem is outstanding; Fluidized-bed is relative dilute phase system, and the density variation of solid catalyst and biomass also can be brought outstanding problem.Since the eighties, scientists has been carried out a large amount of research trials in order to solve two kinds of reactors defective separately, wherein the improvement of fixed bed is concentrated on research to catalyst activity and anti-carbon aspect, wish to find that the novel and effective catalyzer reduces carbon distribution and prolongs the active time, and the improvement of fluidized-bed is concentrated on the fluidizing medium that the searching physical strength is fit to, traditional fluidized-bed fluidizing medium is husky, and its physical strength reaches requirement substantially.Developed the fluidizing medium with catalytic performance afterwards gradually, and attempted using rhombspar, its catalytic performance is excellent, but physical strength can't adapt to fluidized-bed.And the physical strength of the nearest peridotites of studying and catalytic performance all can satisfy the requirement of fluidized-bed.At burner of fluidized-bed downstream addition, be exclusively used in the area carbon of burn off catalyzer in order to solve this shortcoming of the rapid inactivation of fluid catalyst.Improvement on the other hand to fluidized-bed is to have developed circulating fluidized bed CFB (Circulating fluidized Bed), be characterized in realizing utilizing the circulation of fluidizing medium to realize the cycling and reutilization of whole system heat, but its fluidizing medium only serves as thermal barrier, whole gasification is not had quicken or optimization function.Also there is quite a few focus to be placed on the exploitation of fluidized-bed and fixed bed coupling technology, utilizes the advantage of fast pyrogenation of fluidized-bed and strong point that fixed bed tar transforms to solve two kinds of reactors defective separately.Domestic correlative study report is obviously less and concentrate on on-catalytic gasifying biomass aspect, and representational is that Guangzhou Energy Resource Inst., Chinese Academy of Sciences is the ciculation fluidized bed gasifying apparatus of raw material with the fine particle biomass material.Although the improvement of conventional apparatus and technology is devoted in the research work of a large amount of biology systems matter hydrogen, but still do not find more efficiently technology, no matter be fixed bed or fluidized-bed, the required heat of system all is that the partial combustion by biomass provides, thereby consumed part hydrogen in the biomass, reduced the hydrogen productive rate.This shows, answer the new Biomass Catalytic Gasification of active development to produce the hydrogen-rich gas processing method.
Summary of the invention
In order to overcome the deficiency of producing at present in the hydrogen-rich gas processing method, the present invention proposes a kind of new Biomass Catalytic Gasification preparing hydrogen-rich gas method, be solid thermal carriers catalytic gasification biomass hydrogen preparation technology, constitute by biomass and catalyst mix heating, biomass fast pyrogenation, catalytic gasification, catalyst solid particle regeneration circulation, make the hydrogen in the biomass be converted into purpose product hydrogen to greatest extent.
The technical solution adopted for the present invention to solve the technical problems is: biomass closely contact with solid thermal carriers in solid catalyst thermal barrier circulating system, the fast pyrogenation gasification reaction takes place, the quality of solid thermal carriers catalyzer and biomass is 1: 1～8: 1 than scope, range of reaction temperature is 700 ℃～850 ℃, pressure is 0～0.02MPa, water vapor/biomass quality is 0.2～2.0 than scope, biomass pyrolytic tar further under the effect of solid catalyst with water vapor generation catalytic reforming reaction, generation does not contain tar or tar content hydrogen-rich gas seldom, gets product gas through the isolation of purified system.Granules of catalyst also is a thermal barrier simultaneously, by the surface of combustioncatalysts in riser tube gentleization of carbon deposit product charcoal, make granules of catalyst in cyclic regeneration, also put aside the required heat of biomass pyrogenation gasification, to finish the circulation of producing hydrogen-rich gas, regeneration promotes temperature and is controlled at 800 ℃～950 ℃.Various agricultural crop straws or biomass wastes such as granularity＜5～10mm that described biomass are dried for process is broken or natural air drying is handled, the almond of moisture content＜20%, beanstalk, straw, rice husk, or year light coal.
Described solid thermal carriers catalyzer is natural mineral rhombspar, peridotites and load Ni modified catalyst thereof, perovskite structure Ni is catalyst based, industrial load type Ni is catalyst based etc.
The activator of described combustioncatalysts surface gentleization of carbon deposit product charcoal is air, oxygen-rich air and hot flue gas etc.
The range of reaction temperature of main reactor is 700 ℃～850 ℃, and pressure is 0～0.02MPa, and water vapor/biomass quality is 0.2～2.0 than scope.At range of reaction temperature is 750 ℃～800 ℃, and water vapor/biomass quality is 0.4～1.2 o'clock than scope, and reaction effect is better.
The catalyzer and the unreacted biomass charcoal of part that come out from moving-burden bed reactor enter the thermal regeneration activation stage from regeneration riser tube bottom, and the regeneration riser temperature is controlled at 800 ℃～950 ℃.
Implement solid thermal carriers circulation device of the present invention, comprise feed system (screw feeder, electromagnetic adjustable speed motor, water pump, vaporizer etc.), reactive system (moving-burden bed reactor, riser tube, mixing container) and auxiliary isolation of purified system.Described solid thermal carriers circulation device, the charging opening of its biomass and catalyzer is positioned at the top of main reactor, adds reactor by screw feeder; Used water vapor is added by the main reactor top, and its charging opening is positioned at biomass and catalyzer charging opening below.Reactor according to claim 1 is characterized in that the complete and stream of solid thermal carriers catalyzer, biomass, unreacted biomass charcoal, vaporized chemical and product gas in reactor.Described tempering tank, there is a baffle plate its inside, and effect is that the solid catalyst that makes to come out from riser tube and semicoke etc. rest on and continue circulation the tempering tank, and is unlikely to be taken out of reactor by flue gas.
Here, granules of catalyst also is a thermal barrier simultaneously.By combustioncatalysts surface gentleization of carbon deposit product charcoal, make granules of catalyst in cyclic regeneration, also put aside the required heat of gasifying biomass.Because gasification institute heat requirement is to realize by the charcoal of combustioncatalysts carbon deposit and poor hydrogen, this makes hydrogen in the biomass be converted into purpose product hydrogen to greatest extent becomes possibility.Catalyzer and the heating of biomass short mix have overcome the shortcoming that biomass heat up at a slow speed in the general first kind catalysis gasification technique.The outstanding feature of novel process also shows widely adaptability to raw material, aspects such as turndown ratio, low investment and running cost, atmospheric operation, environmental friendliness flexibly.This technology also is applicable to a year light coal.
The invention has the beneficial effects as follows:
1) solid thermal carriers catalyst gasified bio-matter circulating system can realize comprising the independent operating control of each technological process such as solid catalyst heating, catalyzer and the heating of biomass short mix, biomass fast pyrogenation, gasifying biomass and condition very easily.
2) with solid catalyst as thermal barrier, biomass pyrolytic and gasification reaction institute heat requirement are provided by combustioncatalysts carbon deposit and biomass charcoal, making hydrogen in the biomass be converted into product hydrogen to greatest extent becomes possibility.
3) the solid thermal carriers heating method realizes that biological particles is rapidly heated, pyrolytic gasification, helps improving the biomass efficiency of carbon conversion and suppresses catalyst carbon deposit.
4) realize REVIEW ON FAST PYROLYSIS OF BIOMASS FOR BIO-OIL, catalytic gasification, pyrolytic tar/hydro carbons situ catalytic steam reformation, and the nothing of the heating of solid thermal carriers and catalyzer switching regeneration is carried out simultaneously continuously.The continuous nothing of catalyzer is switched regeneration and has then been solved the problem that the catalyzer rapid deactivation brings from technology.
5) solid thermal carriers catalyzer in the whole circulation system, biomass, vaporized chemical, and the pyrolytic gasification reaction product is complete and stream.Adopt complete and the movable bed reactor flow process of drifting can effectively reduce product isolation of purified load, and on engineering, created condition for the optimization of continuous circulation process process reaction apparatus structure and operation.
Description of drawings
Below in conjunction with drawings and Examples the technical program is further specified:
Fig. 1 is a schema of the present invention
1, biomass groove 2, make-up catalyst groove 3,4, feeding screw 5, vaporizer
6, water pump 7, moving-burden bed reactor 8, riser tube 9, tempering tank 10, baffle plate
11, cyclonic separator 12, fly-ash separator 13, gas treating system 14, vacuum pump
Embodiment
Biomass enter moving-burden bed reactor from biomass groove 1 by screw feeder 3, with the catalyst mix that loops back from tempering tank 9.Water vapour is squeezed into reactor by pump, and fast pyrogenation and steam reformation catalyzed reaction take place in moving-burden bed reactor 7 three, and aerogenesis goes out reactor as shown in the figure, collects through isolation of purified system handles post analysis.The aerogenesis exit connects vacuum pump 14, is used for regulation system pressure.Reaction residual (comprising charcoal/cinder, solid dust and catalyzer) is circulated to the riser tube bottom.Air or additional combustion gas add riser tube by riser tube 8 bottoms, burning the carbon deposit of charcoal and catalyst surface, and make catalyst regeneration as activator, assemble heat simultaneously and make the surface temperature of catalyzer reach the reaction necessary requirement.When said mixture was promoted to tempering tank 9, flue gas and solid dust that partial reaction produces went out reactive system via cyclonic separator 11, and remaining catalyzer and part semicoke enter moving-burden bed reactor and continue circulation.
Embodiment 1:
With sieving after the pulverizing of biomass material almond, select for use the biomass of 8～16 order granularities to place the biomass groove.Sieve after the catalyzer rhombspar pulverized certain particle, 12～16 purpose raw ores are calcined in retort furnace, 900 ℃ of calcining temperatures, calcination time 4h puts into catalyst tank afterwards.Start electromagnetic adjustable speed motor, biomass and catalyzer adding are fallen bed bioreactor, control reaction temperature is 750 ℃, and the value of water vapor/biomass mass ratio is 0.8.Aerogenesis is formed and the index of productive rate sees Table 1.
Embodiment 2:
Control reaction temperature is 800 ℃, and all the other are with embodiment 1.
Embodiment 3:
Control reaction temperature is 850 ℃, and all the other are with embodiment 1.
Embodiment 4:
The value of adjusting water vapor/biomass mass ratio is 0.4, and all the other are with embodiment 2.
Embodiment 5:
The value of adjusting water vapor/biomass mass ratio is 1.2, and all the other are with embodiment 2.
Table 1
Claims (6)
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| MX2008005225A (en) * | 2005-10-21 | 2008-09-11 | Taylor Biomass Energy Llc | Process and system for gasification with in-situ tar removal. |
| CN100363249C (en) * | 2006-09-18 | 2008-01-23 | 华东理工大学 | Method for producing hydrogen by catalytic gasification of cellulose waste hydrolysis residue |
| CN101045524B (en) * | 2007-05-04 | 2010-05-19 | 大连理工大学 | Method for producing hydrogen-rich gas by catalytic gasification of solid fuel |
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