CN110982558B - Method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on chemical chain technology - Google Patents
Method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on chemical chain technology Download PDFInfo
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
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- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/72—Other features
- C10J3/82—Gas withdrawal means
- C10J3/84—Gas withdrawal means with means for removing dust or tar from the gas
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- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
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- C01B2210/0028—Separation of the specific gas from gas mixtures containing a minor amount of this specific gas
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- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
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- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
- C10J2300/0913—Carbonaceous raw material
- C10J2300/093—Coal
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- C10J2300/00—Details of gasification processes
- C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
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Abstract
The invention discloses a method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on a chemical chain technology, which comprises the following steps: the system comprises a fuel reactor, an oxygen reactor, a first gas-solid separation device, a second gas-solid separation device, a first flow control device, a second flow control device and an air separation device; the calcium oxide captures carbon dioxide in the fuel reactor, releases carbon dioxide in the oxygen reactor, and the carbon dioxide reacts with coke to generate carbon monoxide under the action of the catalyst, wherein the oxygen and the carbon dioxide are used as a fluidizing medium and are also used as reaction raw materials. The method has the advantages of simple flow, convenient operation, scientific and easily obtained process raw materials, low cost, high carbon utilization efficiency, less pollutants and environmental friendliness.
Description
Technical Field
The invention relates to the technical field of energy and chemical industry, in particular to a method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on a chemical chain technology.
Background
The synthesis gas uses carbon monoxide and hydrogen as main components and is used as a raw material gas of chemical raw materials. The raw material range of the synthesis gas is wide, and the synthesis gas can be generated by gasifying solid fuels such as coal or coke, can be prepared from light hydrocarbons such as natural gas and naphtha, and can be produced from heavy oil by a partial oxidation method. However, in the past, the production of syngas, whether coal or natural gas as fuel, has produced large amounts of carbon dioxide, and thus, the removal of carbon dioxide or the conversion of carbon dioxide to carbon monoxide in the syngas production process is desirable to further improve system efficiency, reduce emissions, and protect the environment.
The calcium-based chemical-looping carbon capture technology is a carbon dioxide capture technology which is widely researched at present, a carbon dioxide capture device after calcium circulation combustion of a demonstration device level is available in the world, hydrogen with high purity (> 85%) can be produced and carbon dioxide can be captured in a hydrogen production process of coal gasification or methane wet reforming process and calcium circulation coupling, however, how to dispose the captured carbon dioxide becomes a new problem, pure oxygen is needed in a calcium oxide regeneration process, and the pure oxygen is only used for combusting coke to provide heat to regenerate the calcium oxide and capture the carbon dioxide, so that the system efficiency is reduced, therefore, the process is combined with a synthesis gas production process, the added value of the product produced by the whole device can be better increased, and the fuel can be efficiently utilized.
In other processes or devices for preparing hydrogen and carbon monoxide by gasifying coal or biomass based on chemical chain technology (CN103113917, CN208234855, CN101638590, CN107325846, and CN101975395), no method for in-situ conversion of carbon dioxide into carbon monoxide is mentioned or solved, and the device has a more complex structural design, which results in higher cost.
Disclosure of Invention
The technical problem to be solved by the invention is to provide a method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on a chemical chain technology, so that the aim of converting carbon dioxide trapped in a calcium cycle coal gasification process into carbon monoxide in situ is fulfilled, and synthesis gas (hydrogen and carbon monoxide) with adjustable proportion is directly obtained.
In order to solve the technical problems, the invention provides a device for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on a chemical looping technology, which comprises: the system comprises a fuel reactor, an oxygen reactor, a first gas-solid separation device, a second gas-solid separation device, a first flow control device, a second flow control device and an air separation device; the calcium carbonate bed material loaded with iron or nickel enters an oxygen reactor through a first gas-solid separation device and a first control flow device to generate calcium oxide bed material loaded with iron or nickel, and the calcium oxide bed material loaded with iron or nickel enters a fuel reactor through a second gas-solid separation device and a second control flow device to generate calcium carbonate bed material loaded with iron or nickel again; the bed material is circulated between two reactors, wherein steam and coal or biomass are fed into a fuel reactor and hydrogen is produced, and oxygen is fed into an oxygen reactor and carbon monoxide is produced, wherein the oxygen is supplied from an air separation unit, which separates nitrogen from oxygen in the air to obtain pure oxygen.
Preferably, the fuel reactor and the oxygen reactor are both fluidized beds, and the flow patterns are both fast fluidized beds or pneumatic conveying beds.
Preferably, the first gas-solid separation device and the second gas-solid separation device are both one of an inertial separator and a cyclone separator, and the first gas-solid separation device and the second gas-solid separation device separate gas and solid particles generated in the reactor.
Preferably, the first control flow device and the second control flow device are each one of a V-valve, a U-valve, an L-valve, an H-valve and a J-valve, and the first control flow device and the second control flow device control bed material transfer and prevent gas channeling between reactors.
Preferably, the bed material mainly comprises calcium oxide and is loaded with iron or nickel, and the main loading method is an impregnation method.
Correspondingly, the method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on a chemical chain technology comprises the following steps:
(1) feeding coal or biomass particles with the particle size of 0.1-10mm into the bottom of a fuel reactor, lifting calcium oxide bed material particles with the particle size of 0.07-0.7mm and loaded with iron or nickel to the top of the fuel reactor, wherein in the lifting process, the iron or nickel plays a role of catalysis, the calcium oxide adsorbs carbon dioxide to generate calcium carbonate, hydrogen with the concentration of 85% is separated in a first gas-solid separation device, the temperature of the fuel reactor is controlled to be 600-800 ℃, and the inside of the reactor is in a reducing atmosphere;
(2) controlling the temperature of an oxygen reactor to be 700-950 ℃, feeding calcium carbonate bed material particles loaded with iron or nickel into the bottom of the oxygen reactor, lifting the calcium carbonate bed material particles to the top of the oxygen reactor by oxygen, heating the calcium carbonate to decompose the calcium carbonate into calcium oxide and carbon dioxide in the lifting process, reacting the carbon dioxide, coke and oxygen together to generate carbon monoxide, and separating the carbon monoxide with the concentration of 85% in a first gas-solid separation device;
(3) according to the steps (1) and (2), iron and nickel are used as catalysts for the reaction, and simultaneously, carbon deposit generated in the fuel reactor and oxygen in the oxygen reactor are subjected to partial oxidation reaction to generate carbon monoxide.
Preferably, the coal or biomass fuel particles include bituminous coal, gas coal and lignite, or are replaced by biomass particles or other carbonaceous solid waste particles.
The invention has the beneficial effects that: the invention can capture carbon dioxide while producing hydrogen by coal or biomass gasification, can directly convert the captured carbon dioxide into carbon monoxide in situ, and can produce hydrogen and carbon monoxide which are needed most in the chemical process by converting solid fuels such as coal or biomass and the like by using the double fluidized bed reactor, and can obtain synthesis gas with adjustable carbon-hydrogen ratio according to actual needs.
Drawings
FIG. 1 is a schematic structural diagram of the apparatus of the present invention.
Wherein, 1, a fuel reactor; 2. an oxygen reactor; 3. a first gas-solid separation device; 4. a second gas-solid separation device; 5. a second control flow device; 6. a first control flow device; 7. an air separation plant.
Detailed Description
As shown in fig. 1, an apparatus for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on chemical looping technology comprises: the system comprises a fuel reactor, an oxygen reactor, a first gas-solid separation device, a second gas-solid separation device, a first flow control device, a second flow control device and an air separation device; the calcium carbonate bed material loaded with iron or nickel enters an oxygen reactor through a first gas-solid separation device and a first control flow device to generate calcium oxide bed material loaded with iron or nickel, and the calcium oxide bed material loaded with iron or nickel enters a fuel reactor through a second gas-solid separation device and a second control flow device to generate calcium carbonate bed material loaded with iron or nickel again; the bed material is circulated between two reactors, wherein steam and coal or biomass are fed into a fuel reactor and hydrogen is produced, and oxygen is fed into an oxygen reactor and carbon monoxide is produced, wherein the oxygen is supplied from an air separation unit, which separates nitrogen from oxygen in the air to obtain pure oxygen.
A method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on a chemical chain technology comprises the following steps:
(1) feeding coal or biomass particles with the particle size of 0.1-10mm into the bottom of a fuel reactor, lifting calcium oxide bed material particles with the particle size of 0.07-0.7mm and loaded with iron or nickel to the top of the fuel reactor, wherein in the lifting process, the iron or nickel plays a role of catalysis, the calcium oxide adsorbs carbon dioxide to generate calcium carbonate, hydrogen with the concentration of 85% is separated in a first gas-solid separation device, the temperature of the fuel reactor is controlled to be 600-800 ℃, and the inside of the reactor is in a reducing atmosphere;
(2) controlling the temperature of the oxygen reactor to 700-950 ℃, feeding the calcium carbonate bed material particles loaded with iron or nickel into the bottom of the oxygen reactor, lifting the calcium carbonate bed material particles to the top of the oxygen reactor by oxygen, and heating and decomposing the calcium carbonate into calcium oxide and carbon dioxide in the lifting process. The carbon dioxide, coke and oxygen react together to generate carbon monoxide, and the carbon monoxide with the concentration of 85% is separated in a first gas-solid separation device;
(3) according to the steps (1) and (2), iron and nickel are used as catalysts for the reaction, and meanwhile, carbon deposit generated in the fuel reactor can also be partially oxidized with oxygen in the oxygen reactor to generate carbon monoxide.
Example 1:
the process method comprises a fuel reactor, an oxygen reactor, a first gas-solid separation device, a second gas-solid separation device, a first flow control device, a second flow control device and an air separation device; the calcium carbonate bed material loaded with iron or nickel enters an oxygen reactor through a first gas-solid separation device and a first control flow device to generate calcium oxide bed material loaded with iron or nickel, and the calcium oxide bed material loaded with iron or nickel enters a fuel reactor through a second gas-solid separation device and a second control flow device to generate calcium carbonate bed material loaded with iron or nickel again; the bed material circulates between two reactors, in which steam and coal or biomass are fed into a fuel reactor and hydrogen is produced, and oxygen is fed into an oxygen reactor and carbon monoxide is produced.
The fuel reactor and the oxygen reactor described in this example are both fluidized beds, and the flow patterns are both fast bed flow patterns or pneumatic transport bed flow patterns.
In this embodiment, the gas-solid separation device is one of an inertial separator and a cyclone separator, and the gas-solid separation device separates gas and solid particles generated in the reactor.
In the embodiment, the first flow control device and the second flow control device are all one of a V valve, a U valve, an L valve, an H valve and a J valve, and the flow control devices control bed material transmission and prevent gas back-flowing between reactors.
The bed material used in this example was mainly composed of calcium oxide and loaded with iron or nickel, and the main loading method was impregnation.
The process method for directly preparing hydrogen and carbon monoxide by using the device is characterized by comprising the following specific process steps:
(1) feeding coal or biomass particles with the particle size of 0.1-10mm into the bottom of a fuel reactor, lifting calcium oxide bed material particles with the particle size of 0.07-0.7mm and loaded with iron or nickel to the top of the fuel reactor, wherein in the lifting process, the iron or nickel plays a role of catalysis, the calcium oxide adsorbs carbon dioxide to generate calcium carbonate, hydrogen with the concentration of 85% is separated in a first gas-solid separation device, the temperature of the fuel reactor is controlled to be 600-800 ℃, and the inside of the reactor is in a reducing atmosphere;
(2) controlling the temperature of the oxygen reactor to 700-950 ℃, feeding the calcium carbonate bed material particles loaded with iron or nickel into the bottom of the oxygen reactor, lifting the calcium carbonate bed material particles to the top of the oxygen reactor by oxygen, and heating and decomposing the calcium carbonate into calcium oxide and carbon dioxide in the lifting process. The carbon dioxide, coke and oxygen react together to generate carbon monoxide, and the carbon monoxide with the concentration of 85% is separated in a first gas-solid separation device;
(3) according to the steps (1) and (2), iron and nickel are used as catalysts for the reaction, and meanwhile, carbon deposit generated in the fuel reactor can also be partially oxidized with oxygen in the oxygen reactor to generate carbon monoxide.
The chemical reaction performed in step (1) described in this example includes:
CaO+CO2→CaCO3
coal/biomass+heat→gases+tar+char
C+H2O→CO+H2
C+2H2O→CO2+2H2
CO+H2O→CO2+H2
Tars+H2O→gases+hydrocarbons
hydrocarbons+H2O→H2+CO2+CO。
the chemical reaction performed in step (2) described in this example includes:
CaCO3→CaO+CO2
2C+O2→2CO
C+CO2→2CO。
the chemical reaction performed in step (3) described in this example includes:
2C+O2→2CO。
Claims (6)
1. a method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on a chemical chain technology is characterized by comprising the following steps:
(1) feeding coal or biomass particles with the particle size of 0.1-10mm into the bottom of a fuel reactor, lifting calcium oxide bed material particles with the particle size of 0.07-0.7mm and loaded with iron or nickel to the top of the fuel reactor, wherein in the lifting process, the iron or nickel plays a role of catalysis, the calcium oxide adsorbs carbon dioxide to generate calcium carbonate, hydrogen with the concentration of 85% is separated in a first gas-solid separation device, the temperature of the fuel reactor is controlled to be 600-800 ℃, and the inside of the reactor is in a reducing atmosphere;
(2) controlling the temperature of an oxygen reactor to be 700-950 ℃, feeding calcium carbonate bed material particles loaded with iron or nickel into the bottom of the oxygen reactor, lifting the calcium carbonate bed material particles to the top of the oxygen reactor by oxygen, heating the calcium carbonate to decompose the calcium carbonate into calcium oxide and carbon dioxide in the lifting process, reacting the carbon dioxide, coke and oxygen together to generate carbon monoxide, and separating the carbon monoxide with the concentration of 85% in a first gas-solid separation device;
(3) according to the steps (1) and (2), iron and nickel are used as catalysts for the reaction, and simultaneously, carbon deposit generated in the fuel reactor and oxygen in the oxygen reactor are subjected to partial oxidation reaction to generate carbon monoxide.
2. The method for direct production of hydrogen and carbon monoxide by coal or biomass gasification based on chemical looping technology as claimed in claim 1, wherein the coal comprises bituminous coal, gas coal and lignite.
3. The method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on chemical looping technology according to claim 1, wherein the device for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on chemical looping technology is utilized, and the device comprises: the system comprises a fuel reactor, an oxygen reactor, a first gas-solid separation device, a second gas-solid separation device, a first flow control device, a second flow control device and an air separation device; the calcium carbonate bed material loaded with iron or nickel enters an oxygen reactor through a first gas-solid separation device and a first control flow device to generate calcium oxide bed material loaded with iron or nickel, and the calcium oxide bed material loaded with iron or nickel enters a fuel reactor through a second gas-solid separation device and a second control flow device to generate calcium carbonate bed material loaded with iron or nickel again; the bed material is circulated between two reactors, wherein steam and coal or biomass are fed into a fuel reactor and hydrogen is produced, and oxygen is fed into an oxygen reactor and carbon monoxide is produced, wherein the oxygen is supplied from an air separation unit, which separates nitrogen from oxygen in the air to obtain pure oxygen.
4. The method for direct production of hydrogen and carbon monoxide by coal or biomass gasification based on chemical looping technology as claimed in claim 3, wherein the fuel reactor and the oxygen reactor are both fluidized beds, and the flow pattern is either fast fluidized bed or pneumatic transport bed.
5. The method for directly preparing hydrogen and carbon monoxide by coal or biomass gasification based on chemical looping technology as claimed in claim 3, wherein the first gas-solid separation device and the second gas-solid separation device are both one of inertial separator and cyclone separator, and the first gas-solid separation device and the second gas-solid separation device separate gas and solid particles generated in the reactor.
6. The method for direct production of hydrogen and carbon monoxide by coal or biomass gasification based on chemical looping technology as claimed in claim 3, wherein the first control flow device and the second control flow device are each one of V valve, U valve, L valve, H valve and J valve, and the first control flow device and the second control flow device control bed material transfer and prevent gas channeling between reactors.
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