CN1482056A - Method for producing hydrogen-rich gas by catalytic gasification of biomass with solid heat carrier - Google Patents
Method for producing hydrogen-rich gas by catalytic gasification of biomass with solid heat carrier Download PDFInfo
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- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 45
- 239000001257 hydrogen Substances 0.000 title claims abstract description 45
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 44
- 238000002309 gasification Methods 0.000 title claims abstract description 34
- 239000007787 solid Substances 0.000 title claims abstract description 29
- 239000007789 gas Substances 0.000 title claims abstract description 28
- 230000003197 catalytic effect Effects 0.000 title claims abstract description 15
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- 239000003054 catalyst Substances 0.000 claims abstract description 57
- 238000006243 chemical reaction Methods 0.000 claims abstract description 35
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 9
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- 238000001833 catalytic reforming Methods 0.000 claims description 3
- 229910052500 inorganic mineral Inorganic materials 0.000 claims description 3
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- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 2
- 239000010796 biological waste Substances 0.000 claims description 2
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- 238000002156 mixing Methods 0.000 description 7
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 6
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- 240000007594 Oryza sativa Species 0.000 description 2
- 235000007164 Oryza sativa Nutrition 0.000 description 2
- 244000018633 Prunus armeniaca Species 0.000 description 2
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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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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 invention relates to a method for extracting hydrogen from biomass, in particular to a method for preparing hydrogen-rich gas by catalyzing and gasifying biomass with a solid heat carrier.
Background
Hydrogen is an important chemical feedstock and also a clean fuel for fuel cells and internal combustion engines. Hydrogen mainly originates from two routes, namely water electrolysis and hydrocarbon conversion. The main process for producing hydrogen at present is steam catalytic reforming of natural gas (methane), low carbon hydrocarbon or naphtha, and partial oxidation and coal gasification of heavy oil residual oil are also alternative processes. Hydrogen production processes based on natural gas or other fossil fuels are constrained by the supply of raw materials, which in the long run should be based on renewable resources.
Biomass (including wood, crop straw, etc.) is an important renewable resource, the fourth largest energy source in the world, providing 14% of primary energy. In 1998, the yield of crop straws reaches 8.1 hundred million tons, which is equivalent to 3.9 hundred million tons of standard coal and accounts for 32.1 percent of the total amount of primary energy production. The biomass as a solar carrier is different from coal and petroleum, the S content is relatively low, and the net emission of greenhouse gases in the energy conversion process is zero. The biomass-based hydrogen production technology is an environment-friendly sustainable development technology.
The biomass wood fuel has the following typical mass composition: c48%, O45%, H6% and small amount of N, S and minerals. Considering the major elements, the molecular composition of biomass can be expressed as CH1.5O0.7Based on this, the theoretical yield of hydrogen can be calculated. If the biomass reacts with a hydrogen-containing substance, the hydrogen yield is 6% above the maximum hydrogen content of the biomass. A typical process is steam gasification of biomass: (1)
the maximum hydrogen yield of 165gH can be calculated by the reaction route2V (kg biomass).
(1) And (2) the net thermal effect of the reaction is endothermic, and additional heat must be supplied to complete the reaction. The required heat can be provided by partial combustion of the biomass. The biomass used to provide the heat required for the reaction during gasification is as high as 30-40%, and the hydrogen in this portion of the biomass is lost as water:
reaction (1) is H2O-biomass reaction ratio C-O2And C-CO2Slow reaction, high reaction temp and high steam content2The O-biomass reacts at a rate and shortens the residence time of its products. Therefore, hydrogen yield, energy consumption, reactor type and investment in biomass hydrogen production are mutually restricted.
The currently available forms of biomass catalytic pyrolysis/gasification reactors are fixed and fluidized beds, each of which has disadvantages for the purpose of obtaining hydrogen-rich gas. The catalyst in the fixed bed is in close contact with the biomass, which is beneficial to producing hydrogen-rich gas, but the fixed bed is difficult to achieve fast pyrolysis, and the problem of catalyst deactivation is prominent; fluidized beds are relatively dilute phase systems and the density differences between the solid catalyst and the biomass can also present significant problems. Since the 80 s, scientists have made extensive research attempts to solve the drawbacks of each of the two reactors, wherein the improvement of the fixed bed has focused on the research on the activity and anti-carbon deposition of the catalyst, and hopefully, the discovery of a new and effective catalyst for reducing carbon deposition and prolonging the activity time, while the improvement of the fluidized bed has focused on finding a fluidizing medium with suitable mechanical strength, which is sand as the conventional fluidizing medium, and which basically meets the requirements. Later, fluidized media with catalytic properties were developed, and attempts were made to use dolomite, which has very good catalytic properties but mechanical strength not compatible with the fluidized bed. The mechanical strength and catalytic performance of olivine, which have been studied recently, meet the requirements of fluidized beds. In order to solve the defect of rapid deactivation of the fluidized bed catalyst, a burner is additionally arranged at the downstream of the fluidized bed and is specially used for burning off the surface carbon deposit of the catalyst. Another improvement of the fluidized bed is the development of a circulating fluidized bed cfb (circulating fluidized bed), which is characterized in that the circulation of the fluidizing medium is utilized to realize the circulation and the reuse of the heat of the whole system, but the fluidizing medium only serves as a heat carrier and has no acceleration or optimization effect on the whole gasification process. There has also been a considerable amount of work focusing on the development of a combined fluidized and fixed bed process that takes advantage of the fast pyrolysis advantages of the fluidized bed and the tar conversion advantages of the fixed bed to address the drawbacks of each of the two reactors. Related research reports in China are obviously few and are concentrated on the aspect of non-catalytic biomass gasification, and the typical circulating fluidized bed gasification device takes fine-particle biomass materials as raw materials for Guangzhou energy research of Chinese academy of sciences. Although much research on biomass hydrogen production has been devoted to improving conventional devices and processes, no more efficient process has been found, and the heat required for the system, whether it be a fixed bed or a fluidized bed, is provided by partial combustion of the biomass, thereby consuming some of the hydrogen from the biomass and reducing the hydrogen yield. Therefore, a new process for preparing hydrogen-rich gas by catalytic gasification of biomass should be actively developed.
Disclosure of Invention
In order to overcome the defects of the prior process for preparing the hydrogen-rich gas, the invention provides a novel method for preparing the hydrogen-rich gas by catalyzing and gasifying biomass, namely a process for preparing the hydrogen by catalyzing and gasifying the biomass by using a solid heat carrier.
The technical scheme adopted by the invention for solving the technical problems is as follows: the biomass is closely contacted with a solid heat carrier in a solid catalyst heat carrier circulation system to perform a fast pyrolysis gasification reaction, the ratio of the solid heat carrier catalyst to the biomass is 1-8: 1, the reaction temperature is about 700-850 ℃, the pressure is 0-0.02 MPa, the ratio of water vapor to the biomass is 0.2-2, the biomass pyrolysis tar is further subjected to a catalytic reforming reaction with the water vapor under the action of the solid catalyst to generate a hydrogen-rich gas containing no tar or little tar, and the product gas is obtained through a separation and purification system. The catalyst particles are also heat carriers, and the heat required by biomass pyrolysis gasification is accumulated while the catalyst particles are continuously regenerated by burning carbon deposited on the surface of the catalyst and gasification product charcoal, so that the circulation for preparing hydrogen-rich gas is completed, and the regeneration lifting temperature is controlled to be 800-950 ℃. The biomass is various crops or biological wastes such as apricot seeds, beanstalk, rice straw, rice hull and the like with the particle size of less than 5-10 mm and the moisture content of less than 20% after crushing, drying or natural air drying treatment, and can also be light coal.
The solid heat carrier catalyst can be natural minerals (dolomite, olivine and the like) and Ni-loaded modified catalysts thereof, perovskite structure Ni-based catalysts, industrial load type Ni-based catalysts and the like.
The activating agents of the carbon deposited on the surface of the combustion catalyst and the gasification product charcoal are air, oxygen-enriched air, hot flue gas and the like.
The reaction temperature range of the main reactor is about 700-850 ℃, the pressure is 0-0.02 MPa, and the steam/biomass ratio range is 0.2-2. The reaction effect is better when the reaction temperature range is about 750-800 ℃ and the ratio of the water vapor to the biomass ranges from 0.4 to 1.2.
The catalyst and part of unreacted biomass charcoal from the moving bed reactor enter a heatingregeneration activation stage from the bottom of a regeneration riser, and the temperature of the regeneration riser is controlled to be 800-950 ℃.
The solid heat carrier circulating device comprises a feeding system (a spiral feeder, an electromagnetic speed regulating motor, a steam pump, a vaporizer and the like), a reaction system (a moving bed reactor, a riser and a mixing tank) and an auxiliary separation and purification system. The biomass and catalyst feeding ports of the solid heat carrier circulating device are positioned at the top of the main reactor and are added into the reactor through a spiral feeder; the steam is also added from the top of the main reactor, and the feeding ports are positioned below the biomass and catalyst feeding ports. The reactor of claim 1, wherein the solid heat carrier catalyst, the biomass, the unreacted biomass charcoal, the gasifying agent and the product gas are all in parallel flow in the reactor, and a gas production channel is arranged in the reactor and leads from the bottom to the upper part of the moving bed so as to lead the produced gas out of the reactor. The mixing tank is internally provided with a baffle plate which is used for enabling the solid catalyst, the semicoke and the like coming out of the riser to stay in the mixing tank for continuous circulation and not to be carried out of the reactor by the flue gas.
The catalyst particles are also heat carriers here. The catalyst particles continuously regenerate and accumulate heat required for biomass gasification by burning carbon deposits on the surface of the catalyst and charcoal of gasification products. Since the heat required for gasification is achieved by burning catalyst coke and hydrogen-depleted charcoal, it is possible to maximize the conversion of the hydrogen in the biomass to the desired product hydrogen. The catalyst and the biomass are quickly mixed and heated, and the defect of slow temperature rise of the biomass in the first catalytic gasification process is overcome. The outstanding characteristics of the new process are also reflected in the aspects of wide raw material adaptability, flexible operation flexibility, low investment and operation cost, normal pressure operation, environmental friendliness and the like. The process is also suitable for light coal.
The invention has the beneficial effects that:
1) the solid heat carrier catalyst catalytic gasification biomass circulation system can very conveniently realize independent operation control of various technological processes and conditions including solid catalyst heating, catalyst and biomass rapid mixing heating, biomass rapid pyrolysis, biomass gasification and the like.
2) The solid catalyst is used as a heat carrier, and heat required by biomass pyrolysis and gasification reaction is provided by burning catalyst carbon deposit and biomass charcoal, so that the maximum conversion of hydrogen in the biomass into product hydrogen is possible.
3) The solid heat carrier heating method realizes the rapid temperature rise, pyrolysis and gasification of biomass particles, and is favorable for improving the biomass carbon conversion rate and inhibiting the carbon deposition of a catalyst.
4) The biomass is rapidly pyrolyzed, catalytically gasified, pyrolyzed tar/hydrocarbon in-situ catalytic steam reforming, and the heating of a solid heat carrier and the non-switching regeneration of a catalyst are continuously carried out at the same time. The continuous non-switching regeneration of the catalyst solves the problem of rapid inactivation of the catalyst in the process.
5) And the solid heat carrier catalyst, the biomass, the gasifying agent and the pyrolysis and gasification reaction product in the whole circulating systemare in full parallel flow. The adoption of the flow of the full parallel flow moving bed reactor can effectively reduce the load of product separation and purification, and creates conditions for the optimization of the structure and the operation of a reaction device in the continuous cycle process in engineering.
Drawings
The technical solution is further explained below with reference to the drawings and the embodiments:
FIG. 1 is a flow chart of the present invention
1. Biomass tank 2 and catalyst replenishing tank
3. 4, a spiral feeder 5, a vaporizer 6 and a water vapor pump
7. Gas production channel 8, falling bed reactor 9 and lifting pipe
10. Mixing tank 11, baffle 12, cyclone
Detailed Description
Biomass enters the falling bed reactor from the biomass tank 1 through the screw feeder 4 and is mixed with the catalyst circulated back from the mixing tank 10. The steam is pumped into the reactor by a pump, the three are subjected to fast pyrolysis and steam reforming catalytic reaction in the falling bed reactor 8, the produced gas is discharged out of the reactor through a channel 7, and is analyzed and collected after being treated by a separation and purification system. The reaction residue (including charcoal/char residue, solid dust and catalyst) is recycled to the bottom of the riser. Air or supplementary fuel gas is added into the riser tube from the bottom of the riser tube 9 and used as an activating agent to burn off charcoal and carbon deposit on the surface of the catalyst, and the catalyst is regenerated, and simultaneously the heat is collected to ensure that the surface temperature of the catalyst meets the requirement required by the reaction. When the mixture is circulated to the mixing tank 10, part of the flue gas and solid dust generated by the reaction is discharged from the reaction system through the cyclone 12, and the rest of the catalyst and part of the semicoke enter the falling bed reactor for continuous circulation.
Example 1:
crushing biomass (apricot kernels), screening, and placing biomass with the granularity of 8-16 meshes in a biomass tank. Crushing the catalyst (dolomite) to a certain particle size, screening, calcining the 12-16-mesh raw ore in a muffle furnace at 900 ℃ for 4h, and then putting the calcined ore into a catalyst tank. Starting an electromagnetic speed regulating motor, adding the biomass and the catalyst into the falling bed reactor, controlling the reaction temperature to be 750 ℃ and the value of the steam/biomass ratio to be 0.8. The gas production composition and yield index are shown in Table 1.
Example 2:
the reaction temperature was controlled to 800 ℃ as in example 1.
Example 3:
the reaction temperature was controlled to 850 ℃ as in example 1.
Example 4:
the steam/biomass ratio was adjusted to a value of 0.4 as in example 2.
Example 5:
the steam/biomass ratio was adjusted to a value of 1.2, as in example 2. TABLE 1
| (g/kg raw material) Substance (Dry) Dry ash-free Base)) | CO | 5.57 | 14.07 | 28.48 | 18.95 | 13.53 |
| CO+H2 | 49.06 | 74.29 | 102.91 | 73.33 | 83.65 |
Claims (6)
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| CNB031337996A CN1277740C (en) | 2003-07-25 | 2003-07-25 | Process of catalyzing and gasifying fresh substance by solid thermophore for preparing hydrogen-rich gas |
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Cited By (22)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1301789C (en) * | 2005-02-25 | 2007-02-28 | 许庆华 | Biomass gasification catalyst and its production method |
| 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 |
| CN101818081A (en) * | 2010-03-23 | 2010-09-01 | 武汉凯迪科技发展研究院有限公司 | Process and system for manufacturing synthesis gas from biomass by carbonization |
| CN101880552A (en) * | 2010-06-29 | 2010-11-10 | 中国科学院广州能源研究所 | A gasification device and method for preparing hydrogen-rich synthesis gas from biomass |
| CN103415591A (en) * | 2011-03-10 | 2013-11-27 | 科伊奥股份有限公司 | Refractory mixed-metal oxides and spinel compositions for thermo-catalytic conversion of biomass |
| CN103468322A (en) * | 2013-07-25 | 2013-12-25 | 易高环保能源研究院有限公司 | Method for preparing hydrogen-rich gas by gasifying water vapor of solid organic matter |
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| CN101312905B (en) * | 2005-10-21 | 2015-07-22 | 泰勒生物质能有限责任公司 | Process and system for gasification with in-situ tar removal |
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| CN105008498A (en) * | 2013-02-05 | 2015-10-28 | 瑞来斯实业公司 | A process for catalytic gasification of carbonaceous feedstock |
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| CN111498806A (en) * | 2020-04-10 | 2020-08-07 | 大连海洋大学 | Method for preparing high-purity hydrogen from biomass and system adopted by method |
| CN112410075A (en) * | 2020-11-25 | 2021-02-26 | 新奥科技发展有限公司 | Coal catalytic gasification system and method |
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| CN115074157A (en) * | 2022-05-16 | 2022-09-20 | 哈尔滨工业大学 | Rotary kiln and moving bed composite gasification device and method thereof |
| CN115228874A (en) * | 2022-05-25 | 2022-10-25 | 海南省智慧环境投资控股有限公司 | Dynamic circulation organic solid waste treatment process |
| CN115926853A (en) * | 2022-12-27 | 2023-04-07 | 华中科技大学 | A self-heating cracked gas catalytic reforming reaction system |
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2003
- 2003-07-25 CN CNB031337996A patent/CN1277740C/en not_active Expired - Fee Related
Cited By (32)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1301789C (en) * | 2005-02-25 | 2007-02-28 | 许庆华 | Biomass gasification catalyst and its production method |
| CN101312905B (en) * | 2005-10-21 | 2015-07-22 | 泰勒生物质能有限责任公司 | 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 |
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