CN100482575C - Solid fuel continuous non-oxdiation hydrogen preparation method and device - Google Patents
Solid fuel continuous non-oxdiation hydrogen preparation method and device Download PDFInfo
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- CN100482575C CN100482575C CNB2006100664224A CN200610066422A CN100482575C CN 100482575 C CN100482575 C CN 100482575C CN B2006100664224 A CNB2006100664224 A CN B2006100664224A CN 200610066422 A CN200610066422 A CN 200610066422A CN 100482575 C CN100482575 C CN 100482575C
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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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Abstract
An apparatus for preparing H2 by continuous non-oxygen gasification of solid fuel is composed of a spray-bed or fluidized-bed gasifying reactor made up of high-strength alloy and with thin-wall quartz tube liner, and a continuous feeder for feeding solid fuel and absorbent power. Its process features that the high-pressure N2 is used as the carrying gas of slid fuel and CO2 absorbent powder, and water steam is used as gasifying gas.
Description
Technical field
The invention belongs to clear energy sources and transform field and coal chemical technology, be particularly related to for example coal of a kind of solid fuel, under the effect of catalyzer, with the water vapour reaction generation hydrogen of High Temperature High Pressure, produced simultaneously carbonic acid gas is all absorbed by the base absorption agent, realizes the method for continous way hydrogen manufacturing.
The invention still further relates to the device of realizing aforesaid method.
Technical background
Hydrogen Energy with its cleaning, efficient, utilize plurality of advantages such as various informative, more and more win people's favor, be expected to become in future and lay equal stress on electric power and one of terminal energy sources that complementary is main.Hydrogen is secondary energy, need produce from primary energy source.With solid fuels such as coals is that raw material hydrogen manufacturing becomes first-selection: the coal reserves are the primary energy source that China is top dog than horn of plenty, and its cleaning efficiently utilizes difficulty big, are that China's efficiency of energy utilization is low, the major cause that environmental problem is outstanding.The new way of exploitation coal hydrogen manufacturing is the means that effectively solve the energy environment problem, has the strategic importance of reality.
At present, more sophisticated is fossil oil hydrogen manufacturing and water electrolysis hydrogen producing technology, wherein producing hydrogen with raw materials such as coal, oil is the topmost method of current hydrogen manufacturing, it comprises steps such as gasification, scavenging process, the conversion of CO component and hydrogen purification, and it is more to produce in the process power consumption, and hydrogen production efficiency is low, equipment is more complicated also, less economical, main towards the application of hydrogen as industrial chemicals, can't satisfy extensive, efficient, the cheap requirement that hydrogen uses as the energy.The water electrolysis hydrogen production technology is ripe, but electricity itself is the high-quality energy, and the efficient itself of being come by the primary energy source conversion is just not high, therefore can not satisfy the requirement that hydrogen uses as the energy.Having started with hydrogen at present is the research boom of energy source use.
In recent years, their biomass hydrogen preparation research has been reported in the Shanghai Communications University, Xi'an, but on the high temperature flow reactor of the long term operation of its design, has realized that the 0.1M Mierocrystalline cellulose is at 650 ℃, 25Mpa is gasified totally, and true biomass (sawdust and a small amount of Xylo-Mucine) gasification efficiency reaches 95%.But the content of hydrogen has much room for improvement in the gaseous product.
Be that raw material is produced and also proposed a lot of new notions and possible path for transformation aspect the hydrogen with coal.
On the research basis of using for reference high pressure hydro-thermal biomass hydrogen preparation, Japan has proposed the HyPr-RING experimental reserch program(me), under the condition of supercritical water, coal is given hydrogen transmission ofenergy by the circulation of water-hydrogen-water and then is utilized by the user, and self be oxidized to carbonic acid gas, shift out from reaction system by the circulation of calcium oxide-lime carbonate-calcium oxide again.WangJie etc. have further studied when low-rank coal gasifies in the supercritical water, Ca (OH)
2Effect, think Ca (OH)
2Have very strong katalysis, and think that the calcium carbon ratio 0.6 o'clock carbon dioxide absorption relatively fully.
The prospect 21 (Vision 21) that has started in the U.S. about the basic ideas of hydrogen manufacturing is in the works: fuel is vaporized chemical with oxygen, purification then, conversion, separation, with coal fired power generation efficient reach 60%, natural gas power efficient reaches 75%, coal hydrogen production efficiency 75% is a target, key technology wherein comprises the novel gasification technology that adapts to various fuel, high efficiency separation O
2With N
2, CO
2With H
2Membrane technique etc.Further proposed the Futuregen project again in 2003: setting up one is the demonstration power station (275MW) of product with hydrogen and electricity, has embodied the thinking of hydrogen as main force's energy.Prospect 21 and Futuregen are devoted to integrate multiple modern technique, and development is in the system that significant improvement is all arranged aspect efficient, environment compatibility and the economy.
At the target that prospect 21 is formulated, GE company has proposed the hydrogen manufacturing notion of AGC, and it constitutes three fluidized-bed reactors, coal and water vapour reactive moieties gasification in first reactor, and the carbonic acid gas of generation is by carbon-dioxide absorbent CAM (CO
2Absorption Material) absorbs, form hydrogen-rich gaseous product; The semicoke of gained is transported to next reactor and finishes gasification with water vapour in this reactor.Simultaneous reaction also has the reduction of oxygen transport material OTM (Oxygen Transfer Material) and the regeneration of carbon-dioxide absorbent in second reactor, and its heat comes the sensible heat since the next flowable materials of the 3rd reactor.Second reactor bed temperature wants height to be beneficial to CO
2Release, form rich CO
2Product.In the 3rd reactor, OTM consumes airborne oxygen by the intensive oxygenizement, and the warm air of the deoxidation that obtains enters the mechanism of qi acting.The high heat that reaction produces is along with material mobile passes to reactor 1 and reactor 2 for gasification and regeneration.
U.S. Las Alamos laboratory has proposed the notion of anaerobism coal hydrogen manufacturing, employing hydrogen is vaporized chemical, in gasifying reactor, generate methane earlier with the coal reaction, methane generates carbonic acid gas and hydrogen with steam reaction again in the next stage reactor, exist carbon-dioxide absorbent with carbon dioxide absorption herein, obtain pure hydrogen.A hydrogen part that obtains is returned vapourizing furnace as unstripped gas, and another part is delivered to fuel cell power generation, and fuel battery waste heat is used for carbon-dioxide absorbent is regenerated.Calculating shows that total system has very high efficient, but equipment such as main operation and fuel cell have been proposed very high requirement.
Summary of the invention
The purpose of this invention is to provide a kind of solid fuel continuous non-oxdiation hydrogen preparation method.
Another purpose of the present invention is to provide a kind of device that is used to realize aforesaid method.
For achieving the above object, solid fuel continuous non-oxdiation hydrogen preparation method provided by the invention, be that solid fuel and carbon-dioxide absorbent are joined in high pressure fluidized-bed gasification furnace or the spouted bed gasification furnace of high pressure continuously, with water vapour as fluidizing agent and vaporized chemical, with KOH or Ca (OH)
2Or the mixture of the two is as carbon-dioxide absorbent, and directly all gasifications produce high-purity hydrogen through gas solid separation, gas-liquid separation and purification; Reacted carbon-dioxide absorbent is collected at the gas-solid separator place, sends in the calcining furnace and calcines, and activation generates carbon-dioxide absorbent, is sent back to vapourizing furnace and carbon dioxide reaction again;
Wherein carbon-dioxide absorbent and solid-fuelled stoichiometric ratio are 0.6～5.0.
Wherein the continuous add-on of solid fuel and carbon-dioxide absorbent is 2g/min～40g/min.
Wherein the add-on of water vapour is 80g/min～600g/min.
Wherein the temperature of calcining furnace is 800 ℃～1000 ℃.
The device that is used to realize aforesaid method provided by the invention comprises gasifying reactor and continuous-feeding device; Wherein:
The gasifying reactor steam-gas inlet is connected with the steam generator outlet, and the steam generator water inlet connects a water tank;
Combination is connected by pipeline the continuous-feeding device with relief valve by storage bin, feed buncher, and the nitrogen inlet of continuous-feeding device is connected with the nitrogen buffer tank outlet, adds solid fuel and absorption agent powder in the highly compressed reactor continuously and stably;
The outlet of nitrogen gas generation device is connected with the nitrogen buffer tank import;
The product outlet of gasifying reactor is connected with the gas-solid separator import;
The solid outlet of gas-solid separator connects the solid collection storehouse;
The pneumatic outlet of gas-solid separator is connected with water cooler;
The outlet of water cooler is connected with the gas-liquid separator import;
The liquid exit of gas-liquid separator is connected with the liquid collection tank import;
The pneumatic outlet of gas-liquid separator is connected with the gas collector import.
Described device, wherein gasifying reactor is high pressure fluidized-bed gasification furnace or the spouted bed gasification furnace of high pressure.
Described device, wherein gasifying reactor liner thin-walled silica tube.
Described device wherein is connected a throttling valve between the outlet of the steam-gas inlet of gasifying reactor and steam generator.
Described device wherein is connected with volume pump between steam generator water inlet and the water tank.
Described device, wherein gas-solid separator adopts whirlwind separator.
Innovative point of the present invention is: with the delivering gas of high pressure nitrogen as solid fuel and carbon-dioxide absorbent powder, realize the continous way gasification; Adopt highly compressed fluidized-bed or spouted bed to replace traditional gasification reacting furnace, use water vapour as gasifying gas, while carbonic acid gas quilt is absorption reaction all, and the productive rate of hydrogen is improved greatly; In gasification, the carbonic acid gas of generation is by the carbon-dioxide absorbent total overall reaction, all discharges in calcining furnace, treated after, can realize zero release.
Description of drawings
Fig. 1 is the structural representation of apparatus of the present invention.
Fig. 2 is the structural representation of continuous-feeding device 3 among Fig. 1.
Embodiment
Please in conjunction with Fig. 1 and Fig. 2.Solid fuel continuous non-oxdiation hydrogen preparation device provided by the invention, comprise spouted bed or fluidized bed gasification reactor 1 and continuous-feeding device 3: described reactor 1 liner thin-walled silica tube, to avoid corrosion and the wearing and tearing of reactive material to described gasifying reactor 1 wall; Steam generator 2 is supplied with high compressed steam by throttling valve by following direction gasifying reactor 1, and water tank 10 is connected with steam generator 2 through volume pump 9; Described continuous-feeding device 3 by above or below through behind the throttling valve to gasifying reactor 1 in adding solid fuel and carbon-dioxide absorbent powder; Described continuous-feeding device adopts the method for high-pressure sealed feed bin, the star-like wheeled inventory control of class, is connected with the high pressure in the balanced reaction device with nitrogen buffer tank 4, and nitrogen gas generation device 5 adds nitrogen continuously to nitrogen buffer tank, keeps the pressure equilibrium of system; Outlet in the described gasifying reactor 1 is connected with gas-solid separator 6; The below outlet of described gas-solid separator 6 connects solid collection storehouse 11; The top outlet of described gas-solid separator 6 is connected with water cooler 7; The outlet of described water cooler 7 is connected with gas-liquid separator 8; The below outlet of described gas-liquid separator 8 is connected with liquid collection tank 13; The top outlet of described gas-liquid separator 8 is connected with gas collector 12.
Described continuous-feeding device 3 is formed by connecting by pipeline by storage bin 3-1, feed buncher 3-2 and relief valve 3-3 combination: (carbon-dioxide absorbent can be KOH or Ca (OH) to store needed solid fuel of gasification reaction and carbon-dioxide absorbent powder in the described storage bin 3-1
2Or the mixture of aforementioned the two arbitrary proportion), nitrogen buffer tank 4 is connected with storage bin 3-1 upper inlet through throttling valve; Described feed buncher 3-2 is installed in the bottom of storage bin 3-1, and 3-3 is connected with relief valve; Described relief valve 3-3 is connected with nitrogen snubber 4 by Y-tube, can guarantee the pressure after storage bin 3-1 internal pressure is slightly larger than relief valve 3-3, makes solid fuel and carbon-dioxide absorbent powder fall feed buncher 3-2 place.
Described gasifying reactor 1 uses high-intensity alloy manufacturing, and its intensity reaches: can bear 800 ℃ high temperature and the high pressure of 20MPa simultaneously, its inner replaceable different inner member is so that require to realize different gas-solid contact forms according to reaction; It is required to supply with reaction that described vapour generator 2 can produce the controlled vapour stream of stable quality; Described continuous-feeding device 3 can add solid fuel and absorption agent powder continuously and stably in the highly compressed reactor, require the solid powder drying, and the pipe coupling transition of feeding system is smooth, and whole feeding system is equipped with vibrator; Described gas-solid separator 6 adopts whirlwind separator.
Solid fuel continuous non-oxdiation hydrogen preparation device provided by the invention, its advantage are to realize the continous way gasification with the delivering gas of high pressure nitrogen as solid fuel and carbon-dioxide absorbent powder; Adopt highly compressed fluidized-bed or spouted bed to replace traditional gasification reacting furnace, use water vapour as gasifying gas, while carbonic acid gas quilt is absorption reaction all, and the productive rate of hydrogen is improved greatly; In gasification, the carbonic acid gas of generation is by the carbon-dioxide absorbent total overall reaction, all discharges in calcining furnace, treated after, can realize zero release.
Working process of the present invention is as follows:
1) at first volume pump 9 is opened, the water in the water tank 10 joins in the steam generator 2 after metering, and steam generator begins heating then, is 500 ℃～750 ℃ to producing temperature, and pressure is the overheated steam of 5MPa～20MPa.
2) open nitrogen gas generator 5 simultaneously and supply with nitrogen, to reaching the pressure that the nitrogen snubber sets (10MPa～30MPa) to nitrogen snubber 4.Open the valve that is communicated with of nitrogen snubber 4 and continuous-feeding device 3, reach set(ting)value (10MPa～30MPa) to storage bin 3-1 internal pressure.Regulate relief valve 3-3, the pressure after making storage bin 3-1 internal pressure a little more than relief valve 3-3.
3) open the valve that is communicated with gasifying reactor 1 and steam generator 2, in reactor, add the water vapour of design temperature, open gas-solid separator 6, water cooler 7 and gas-liquid separator 8 simultaneously.
4) behind the temperature-stable, open feed buncher 3-2 in gasifying reactor 1, the adjusting feeding coal is 2g/min～40g/min.
5) the solid fuel continuous non-oxdiation hydrogen preparation device enters steady running.
Solid fuel and the carbon-dioxide absorbent flow with 2g/min～40g/min is joined in high pressure fluidized-bed gasification furnace or the spouted bed gasification furnace of high pressure continuously, wherein carbon-dioxide absorbent and solid fuel chemistry equivalence ratio are 0.6～5.0, with water vapour as fluidizing agent and vaporized chemical, wherein the flow of water vapour is selected between 80g/min～600g/min according to the solid-fuelled amount that adds, directly all gasifications produce high-purity hydrogen through gas solid separation, gas-liquid separation and purification; Reacted carbon-dioxide absorbent is collected at the gas-solid separator place, sends in the calcining furnace temperature lower calcination at 800 ℃～1000 ℃ again, and activation generates carbon-dioxide absorbent, is sent back to vapourizing furnace and carbon dioxide reaction again.
Claims (6)
1, a kind of solid fuel continuous non-oxdiation hydrogen preparation method, solid fuel and carbon-dioxide absorbent are joined in high pressure fluidized-bed gasification furnace or the spouted bed gasification furnace of high pressure continuously, carbon-dioxide absorbent and solid-fuelled stoichiometric ratio are between 0.6～5.0, the continuous add-on of solid fuel and carbonic acid gas is 2g/min～40g/min, with water vapour as fluidizing agent and vaporized chemical, the add-on of water vapour is 80g/min～600g/min, with KOH or Ca (OH)
2Or the mixture of the two is as carbon-dioxide absorbent, and directly all gasifications produce high-purity hydrogen through gas solid separation, gas-liquid separation and purification; Reacted carbon-dioxide absorbent is collected at the gas-solid separator place, sends in the calcining furnace temperature lower calcination at 800 ℃～1000 ℃ again, and activation generates carbon-dioxide absorbent, is sent back to vapourizing furnace and carbon dioxide reaction again.
2, be used to realize the device of the described method of claim 1, comprise gasifying reactor and continuous-feeding device; Wherein:
The gasifying reactor steam-gas inlet is connected with the steam generator outlet, and the steam generator water inlet connects a water tank;
Combination is connected by pipeline the continuous-feeding device with relief valve by storage bin, feed buncher, and the nitrogen inlet of continuous-feeding device is connected with the nitrogen buffer tank outlet, adds solid fuel and absorption agent powder in gasifying reactor continuously and stably;
Described gasifying reactor is high pressure fluidized-bed gasification furnace or the spouted bed gasification furnace of high pressure;
The outlet of nitrogen gas generation device is connected with the nitrogen buffer tank import;
The product outlet of gasifying reactor is connected with the gas-solid separator import;
The solid outlet of gas-solid separator connects the solid collection storehouse;
The pneumatic outlet of gas-solid separator is connected with water cooler;
The outlet of water cooler is connected with the gas-liquid separator import;
The liquid exit of gas-liquid separator is connected with the liquid collection tank import;
The pneumatic outlet of gas-liquid separator is connected with the gas collector import.
3. device as claimed in claim 2, wherein gasifying reactor liner thin-walled silica tube.
4. device as claimed in claim 2 wherein is connected a throttling valve between the outlet of the steam-gas inlet of gasifying reactor and steam generator.
5. device as claimed in claim 2 wherein is connected with volume pump between steam generator water inlet and the water tank.
6, device as claimed in claim 2, wherein gas-solid separator adopts whirlwind separator.
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| CNB2006100664224A CN100482575C (en) | 2006-03-30 | 2006-03-30 | Solid fuel continuous non-oxdiation hydrogen preparation method and device |
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| CNB2006100664224A CN100482575C (en) | 2006-03-30 | 2006-03-30 | Solid fuel continuous non-oxdiation hydrogen preparation method and device |
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| CN101045525A CN101045525A (en) | 2007-10-03 |
| CN100482575C true CN100482575C (en) | 2009-04-29 |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103045308B (en) * | 2012-12-29 | 2014-12-03 | 中国科学院工程热物理研究所 | Power generation method and system based on step conversion of hydrocarbon components of coal |
| CN104030240B (en) * | 2014-06-11 | 2016-04-20 | 南京理工大学 | The device and method of hydrogen making and carbonic acid gas while of utilizing double-fluidized-bed |
| CN105540697B (en) * | 2016-01-21 | 2018-10-19 | 西南石油大学 | The processing unit and method of a kind of high temperature and pressure to waste liquid of drilling |
| CN113060703A (en) * | 2021-04-27 | 2021-07-02 | 西安热工研究院有限公司 | Novel system and method for catalytic hydrogen production by steam under high-temperature and high-pressure working conditions |
| CN114262631A (en) * | 2021-11-18 | 2022-04-01 | 杨家华 | Novel method and device for producing hydrogen by using solid oxide and water |
Citations (4)
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|---|---|---|---|---|
| CN1407948A (en) * | 1999-12-09 | 2003-04-02 | 加利福尼亚大学董事会 | Hydrogen production from carbonaceous material |
| CN1544309A (en) * | 2003-11-12 | 2004-11-10 | 浙江大学 | Oxygen needless hydrogen making method from solid fuel without waste gas discharging |
| WO2005037708A1 (en) * | 2003-10-22 | 2005-04-28 | Intercedo Pte Ltd. | A device for creating energy |
| CN2931446Y (en) * | 2006-03-30 | 2007-08-08 | 中国科学院工程热物理研究所 | Solid fuel continuous non-oxygen gasification hydrogen production device |
-
2006
- 2006-03-30 CN CNB2006100664224A patent/CN100482575C/en active Active
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1407948A (en) * | 1999-12-09 | 2003-04-02 | 加利福尼亚大学董事会 | Hydrogen production from carbonaceous material |
| WO2005037708A1 (en) * | 2003-10-22 | 2005-04-28 | Intercedo Pte Ltd. | A device for creating energy |
| CN1544309A (en) * | 2003-11-12 | 2004-11-10 | 浙江大学 | Oxygen needless hydrogen making method from solid fuel without waste gas discharging |
| CN2931446Y (en) * | 2006-03-30 | 2007-08-08 | 中国科学院工程热物理研究所 | Solid fuel continuous non-oxygen gasification hydrogen production device |
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| 煤制氢零排放系统. 肖云汉.《工程热物理学报》，第22卷第1期. 2001 * |
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