CN114772961B - Process for producing cement and carbon monoxide by co-pyrolysis of cement raw material and solid-phase carbon - Google Patents
Process for producing cement and carbon monoxide by co-pyrolysis of cement raw material and solid-phase carbon Download PDFInfo
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- CN114772961B CN114772961B CN202210478399.9A CN202210478399A CN114772961B CN 114772961 B CN114772961 B CN 114772961B CN 202210478399 A CN202210478399 A CN 202210478399A CN 114772961 B CN114772961 B CN 114772961B
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B7/00—Hydraulic cements
- C04B7/36—Manufacture of hydraulic cements in general
- C04B7/38—Preparing or treating the raw materials individually or as batches, e.g. mixing with fuel
- C04B7/42—Active ingredients added before, or during, the burning process
- C04B7/428—Organic materials
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B7/00—Hydraulic cements
- C04B7/36—Manufacture of hydraulic cements in general
- C04B7/38—Preparing or treating the raw materials individually or as batches, e.g. mixing with fuel
- C04B7/42—Active ingredients added before, or during, the burning process
- C04B7/421—Inorganic materials
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B7/00—Hydraulic cements
- C04B7/36—Manufacture of hydraulic cements in general
- C04B7/43—Heat treatment, e.g. precalcining, burning, melting; Cooling
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- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B7/00—Hydraulic cements
- C04B7/36—Manufacture of hydraulic cements in general
- C04B7/43—Heat treatment, e.g. precalcining, burning, melting; Cooling
- C04B7/44—Burning; Melting
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
- C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
- C10J3/58—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels combined with pre-distillation of the fuel
- C10J3/60—Processes
Abstract
The invention discloses a process for producing cement and carbon monoxide by co-pyrolysis of cement raw materials and a solid-phase carbon source, which comprises the following steps: mixing cement raw materials with solid-phase carbon sources to form mixed raw materials, and then sending the mixed raw materials into a pyrolysis furnace; heating the mixed raw materials and carrying out coupling reduction thermal decomposition under the action of a gasifying agent to obtain a thermal solid-phase decomposition product and decomposition gas; sending the solid-phase decomposition product into a cement mineralization sintering section to generate cement clinker; the decomposed gas is sent to the next working procedure for recycling. Compared with the prior art, the invention has the following advantages: according to the scheme, the gasification reaction of coal or organic matters and the decomposition reaction of cement raw materials are organically combined, the characteristics that the gasification reaction and the decomposition reaction of cement raw materials can mutually promote are utilized, the energy consumption is reduced from the source, the emission of carbon dioxide and nitrogen oxides in the cement industry is reduced, the environment-friendly design of cement production is realized through chemical coupling with energy, the development bottleneck of the existing cement rearrangement industry under the 'double carbon' target is broken through, and the energy transformation and the structural adjustment of the cement industry are promoted.
Description
Technical Field
The invention relates to the technical field of cement production, in particular to a cement and carbon monoxide production process capable of saving energy, reducing consumption and reducing carbon emission.
Background
The cement industry is one of the largest sources of carbon dioxide emissions worldwide, accounting for about 7% of the world's carbon emissions. The mixed combustion of calcium carbonate and coal to produce calcium oxide and carbon dioxide is the main reaction of cement clinker production, and high temperature (> 900 ℃) and high energy consumption and high emission of carbon dioxide and nitrogen oxides are the pain points of the reaction. However, high concentrations of carbon dioxide can cause the calcium oxide to re-react with the carbon dioxide to form calcium carbonate (reverse reaction), thereby inhibiting calcium carbonate decomposition, increasing process operating temperatures, and further increasing nitrogen oxide emissions and system energy consumption. Therefore, the traditional cement raw material decomposition process cannot meet the modern green low-carbon development requirements.
At present, partial replacement of coal by biomass is one of important means for reducing emission in the cement industry as fuel for decomposing calcium carbonate (main component of cement raw material). However, fuel replacement strategies have limited carbon dioxide emissions in the cement industry due to the large amount of carbon dioxide released by the calcium carbonate decomposition reaction itself, while high temperature combustion air also generates large amounts of nitrogen oxides. The novel low-temperature cement raw material decomposition strategy is explored, so that the energy consumption and the emission of carbon dioxide and nitrogen oxides are reduced, and the method has great significance on synergism, low carbon and pollution reduction of the cement industry.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a process for producing cement and carbon monoxide by co-pyrolysis of cement raw materials and a solid-phase carbon source. In the scheme, the gasification reaction of coal or solid organic matters and the decomposition reaction of cement raw materials are organically combined, and the characteristics of mutual promotion of the gasification reaction and the decomposition reaction of the cement raw materials are utilized, so that the carbon emission is effectively reduced, the energy consumption is reduced, and the green production is realized.
The invention is realized by the following technical scheme: the process for producing cement and carbon monoxide by co-pyrolysis of cement raw materials and solid-phase carbon sources is characterized by comprising the following steps:
mixing cement raw materials with solid-phase carbon sources to form mixed raw materials, and then sending the mixed raw materials into a pyrolysis furnace; heating the mixed raw materials and carrying out coupling reduction thermal decomposition under the action of a gasifying agent to obtain a thermal solid-phase decomposition product and decomposition gas; sending the solid-phase decomposition product into a cement mineralization sintering section to generate cement clinker, grinding the cement clinker, and blending to obtain finished cement; the decomposed gas is collected and then recycled, and can be sent to a synthesis gas blending system to blend synthesis gas or raw materials for combustion heat supply or chemical production;
the decomposed gas contains at least carbon monoxide.
The calcium salt in the cement raw material has obvious catalysis on the gasification reaction of coal, and meanwhile, the calcium oxide has obvious catalysis on the gasification of solid organic matters (mainly biomass), under the catalysis of a calcium salt catalyst, solid-phase carbon source substances are gasified into reducing gas containing hydrogen elements in the presence of a gasifying agent; meanwhile, the reducing gas containing hydrogen element is combined with carbon dioxide generated by decomposing the cement raw material, so that the carbon dioxide decomposed from the cement raw material is rapidly consumed, the reaction balance is promoted to move rightwards, the in-situ self-catalysis can effectively reduce the decomposition temperature of calcium carbonate, and the calcium oxide can be generated by co-thermal decomposition with biomass under the condition of 600 ℃ in experiments. The process is a coupling reduction thermal decomposition process of the cement raw material and the solid-phase carbon source, and through the reaction process, the decomposition temperature of the raw material in the traditional cement manufacturing process can be effectively reduced, nitrogen oxides generated at high temperature can be effectively avoided, carbon dioxide can be effectively converted into carbon monoxide, and carbon emission is reduced.
The applicant innovatively designs a green cement chemical industry technical route for producing carbon monoxide by coupling, reducing and thermally decomposing cement raw materials and biomass. In the route, the solid-phase carbon source is gasified to generate reducing molecules such as hydrogen, methane and the like, the reducing atmosphere provides the reducing atmosphere for decomposing calcium carbonate in the cement raw material, the low-temperature pyrolysis of the calcium carbonate is promoted to prepare calcium oxide, the decomposition temperature of the calcium carbonate can be reduced, and meanwhile, carbon dioxide in-situ reduction is realized to generate carbon monoxide, namely, carbon dioxide generated by decomposing the calcium carbonate reacts with reducing gas to generate carbon monoxide, so that the aim of carbon emission reduction is fulfilled. In the process, the cement raw material has good catalytic action on biomass gasification, components such as calcium carbonate and the like can effectively catalyze the pyrolysis of biomass, and meanwhile, the raw material is also used as a raw material to participate in production, so that the effect of in-situ self-catalysis is effectively achieved, and the decomposition of the cement raw material and the pyrolysis of the biomass can be mutually coupled and have a mutual synergistic effect.
Compared with the traditional cement raw material thermal decomposition process, the whole decomposition process of the scheme generates no thermal nitrogen oxide at low temperature. The coupling design of the calcium carbonate thermal decomposition reaction and the biomass directional gasification reaction can realize the source consumption reduction and emission reduction of the cement industry, and provides a revolutionary technology for cement production and biomass resource utilization.
In the coupling reduction thermal decomposition process, the gasifying agent and the solid-phase carbon source are gasified to obtain the reducing gas containing hydrogen, such as hydrogen, low-molecular hydrocarbon and the like.
The solid-phase carbon source is simple substance carbon or solid organic matter, which is not only used for reacting with gasifying agent to generate hydrogen-containing reducing micromolecular gas in the whole process, but also can provide heat for the co-pyrolysis process by participating in oxidation reaction.
The solid organic matters are biomass raw materials such as straw, wood, bamboo and the like, or solid combustible matters such as plastics, rubber, resin and the like, in particular waste recycled combustible matters; the elemental carbon may be coal, coke, or the like. In practice the liquid phase carbon source material can also promote the decomposition of the cement raw meal during the co-pyrolysis process, but this solution is not economical given the high cost of using the liquid phase carbon source material (mainly petroleum).
When the solid-phase carbon source is a solid organic matter, the gasifying agent is one or more of water vapor, oxygen and carbon dioxide. The solid organic matter contains carbon and hydrogen elements, and can undergo pyrolysis, oxidation, reduction reforming and other reactions under the action of the gasifying agent to obtain carbon monoxide, hydrogen and low-molecular hydrocarbons. Hydrogen and low molecular hydrocarbons are capable of reacting with carbon dioxide to convert them to carbon monoxide.
When the solid-phase carbon source is simple substance carbon, the gasifying agent is steam, carbon monoxide and hydrogen are generated in the gasifying reaction process, the hydrogen reacts with carbon dioxide generated by decomposing calcium carbonate, the carbon dioxide is converted into carbon monoxide, carbon emission reduction is realized, and the carbon monoxide generated in the process can be sent to a synthesis gas preparation process or used for other purposes.
According to the setting of reaction conditions and the proportion of materials, the decomposed gas also contains one or more of hydrogen, methane and carbon dioxide. The solid-phase carbon source and gasifying agent are gasified under the catalysis of calcium, the generated micromolecular hydrogen-containing reducing gases are mainly hydrogen and methane, under certain conditions, the micromolecular reducing gases are not consumed in the reaction with carbon dioxide and can be sent to the next working procedure as decomposed gases, the carbon dioxide is not consumed in the reaction, impurity gases can be removed in a targeted manner in the resource utilization stage of a synthesis gas preparation working procedure and the like, and the contents of all components are prepared to meet the actual gas requirement.
As a further improvement to the above scheme, the temperature in the pyrolysis furnace is between 600 ℃ and 1300 ℃.
The carbon dioxide generated by decomposing the calcium carbonate in the cement raw material under the reducing atmosphere can be quickly converted into carbon monoxide, so that the balance of the decomposition reaction of the calcium carbonate is effectively promoted to shift right, the low-temperature decomposition of the calcium carbonate is promoted to prepare the calcium oxide, the decomposition temperature of the calcium carbonate can be reduced, and the decomposition reaction can be carried out in the environment of as low as 600 ℃. Meanwhile, the calcium oxide or calcium carbonate serving as a catalyst in the whole co-pyrolysis process has a wider temperature tolerance range, and can effectively realize coupling reduction thermal decomposition below the melting point of the calcium carbonate. And coking is easy due to high temperature.
As a further improvement to the above-mentioned scheme, the mass ratio of the solid-phase carbon source to the cement raw meal is in the range of 0.05-10.
As a further improvement to the above, hydrogen and/or methane is also fed into the pyrolysis furnace. Carbon dioxide can be converted into carbon monoxide under the action of reducing gases such as hydrogen and methane, and the applicant can ensure a reducing atmosphere by feeding hydrogen or methane into the pyrolysis furnace, further promote the decomposition of calcium carbonate and reduce the dosage of solid-phase carbon sources.
As a further improvement to the above scheme, hydrogen and oxygen are sourced from an electrolytic water production process, and electric energy of the electrolytic water production process is sourced from cement waste heat for power generation.
Compared with the prior art, the invention has the following advantages: according to the scheme, the decomposition of the cement raw material is coupled with the renewable biomass gasification, and the reducing gases such as hydrogen and methane generated by the biomass gasification are utilized to convert carbon dioxide in situ to produce carbon monoxide, so that the forward progress of the calcium carbonate decomposition reaction is promoted, and the decomposition temperature is reduced; meanwhile, the cement raw materials such as calcium carbonate and the like can catalyze biomass gasification in situ, and the two materials are mutually cooperated to realize low-temperature reduction thermal decomposition of the calcium carbonate and produce important chemical raw materials-carbon monoxide, so that carbon dioxide is avoided as much as possible. At present, research and report on coupling of calcium carbonate decomposition and biomass gasification do not exist, cement raw material and biomass reduction thermal decomposition equipment are developed by exploring the characteristics of calcium carbonate reduction thermal decomposition under mixed atmosphere, in-situ catalytic biomass gasification regulation and control mechanism and energy coupling rule in the co-pyrolysis process, and original breakthrough of the environment-friendly cement chemical engineering innovation technology for decomposing calcium carbonate at low temperature and producing carbon monoxide is realized. The project implementation reduces energy consumption from the source, reduces emission of carbon dioxide and nitrogen oxide in the cement industry, is coupled with energy chemical industry, and has important scientific significance and social and economic benefits for promoting green design of chemical engineering reform technology, breaking through the development bottleneck of the existing cement rearrangement industry under the 'double carbon' target, and promoting energy transformation and cement industry structure adjustment.
Detailed Description
The following describes in detail the examples of the present invention, which are implemented on the premise of the technical solution of the present invention, and detailed embodiments and specific operation procedures are given, but the scope of protection of the present invention is not limited to the following examples. The mass of biomass components in the following examples is referred to as dry weight.
Example 1
Mixing calcium carbonate with wood dust powder of 0.05 times, 0.1 times, 0.5 times, 1 times, 2 times and 10 times respectively, preparing samples, and carrying out coupling reduction thermal decomposition reaction on each sample at 600 ℃, 650 ℃, 700 ℃, 750 ℃, 800 ℃, 850 ℃, 1200 ℃ and 1300 ℃ under the condition that steam is used as a gasifying agent to obtain a thermosetting phase decomposition product and decomposition gas. Analysis of the solid phase decomposition products revealed that calcium oxide could be obtained.
Mixing cement raw materials and biomass raw materials according to the proportion, sending the mixture into a decomposing furnace, carrying out co-pyrolysis under the action of water vapor, collecting solid-phase decomposition products and decomposed gas, sending the solid-phase decomposition products into a cement mineralization sintering section to generate cement clinker, grinding the cement clinker, preparing the cement clinker to obtain finished cement, sending the decomposed gas into a synthesis gas preparing system, and preparing the synthesis gas according to the requirement after removing impurities. The hydrogen in the synthesis gas can come from an electrolytic water process, and the electric energy can come from a cement waste heat power generation process. At first, when the biomass consumption is low, carbon dioxide exists in the decomposed gas, and as the biomass consumption is increased, the carbon dioxide gradually disappears, and small molecular hydrocarbons such as hydrogen, methane and the like begin to appear in the decomposed gas.
Example 2
Mixing calcium carbonate with 0.1 times, 0.7 times, 1.4 times, 2 times and 5 times of rice straw powder respectively, preparing samples, and carrying out coupling reduction thermal decomposition reaction on each sample at 630 ℃, 680 ℃, 730 ℃, 780 ℃, 830 ℃, 880 ℃, 930 ℃ and 1300 ℃ under the condition that oxygen is taken as a gasifying agent to obtain a thermosetting phase decomposition product and decomposition gas. Analysis of the solid phase decomposition products revealed that calcium oxide could be obtained.
Mixing cement raw materials and biomass raw materials according to the proportion, sending the mixture into a decomposing furnace, carrying out co-pyrolysis under the action of oxygen, collecting solid-phase decomposition products and decomposed gas, sending the solid-phase decomposition products into a cement mineralization sintering section to generate cement clinker, grinding the cement clinker, preparing the cement clinker to obtain finished cement, and directly using the decomposed gas as fuel for the calcination process or other heat supply requiring a heat supply process.
In the process, oxygen reacts with biomass to generate steam, carbon monoxide or carbon dioxide, and the steam can promote biomass gasification reaction to obtain hydrogen or other small molecular hydrocarbons, and the reducing gas containing hydrogen elements reacts with the carbon dioxide to convert the hydrogen into the carbon monoxide.
Example 3
Mixing calcium carbonate with 0.2 times, 0.8 times, 1.2 times, 3 times and 10 times of rice straw powder respectively, preparing samples, and carrying out coupling reduction thermal decomposition reaction on each sample at 630 ℃, 650 ℃, 680 ℃, 700 ℃, 750 ℃, 800 ℃, 900 ℃ and 1300 ℃ under the condition that carbon dioxide is used as a gasifying agent to obtain a thermosetting phase decomposition product and decomposition gas. Analysis of the solid phase decomposition products revealed that calcium oxide could be obtained.
Mixing cement raw materials and biomass raw materials according to the proportion, sending the mixture into a decomposing furnace, carrying out co-pyrolysis under the action of carbon dioxide, collecting solid-phase decomposition products and decomposed gas, sending the solid-phase decomposition products into a cement mineralization sintering section to generate cement clinker, grinding the cement clinker, preparing the cement clinker to obtain finished cement, collecting the decomposed gas, and removing impurities to obtain carbon monoxide, and using the carbon monoxide as a chemical raw material.
The carbon dioxide reacts with the biomass to produce steam and carbon monoxide, the steam can promote the biomass gasification reaction to obtain hydrogen or other small molecular hydrocarbons, and the reducing gas containing hydrogen elements reacts with the carbon dioxide to convert the reducing gas into the carbon monoxide.
In examples 1-3, the effective gasifying agent component water vapor may be considered, and thus oxygen, carbon dioxide and water vapor may be used interchangeably or in combination.
Example 4
Mixing calcium carbonate with coke powder of 0.05 times, 0.1 times, 0.3 times, 0.7 times, 1 times, 3 times and 10 times respectively, preparing samples, and carrying out coupling reduction thermal decomposition reaction on each sample at 600 ℃, 650 ℃, 700 ℃, 750 ℃, 800 ℃, 850 ℃, 900 ℃, 1200 ℃ and 1300 ℃ under the condition that water vapor is used as a gasifying agent to obtain a thermosetting phase decomposition product and decomposition gas. Analysis of the solid phase decomposition products revealed that calcium oxide could be obtained.
Mixing cement raw materials and coal or coke according to the proportion, sending the mixture into a decomposing furnace, carrying out co-pyrolysis under the action of water vapor, collecting solid-phase decomposition products and decomposed gas, sending the solid-phase decomposition products into a cement mineralization sintering section to generate cement clinker, grinding the cement clinker, preparing the cement clinker to obtain finished cement, sending the decomposed gas into a synthesis gas preparing system, and preparing synthesis gas according to the requirement after removing impurities. The hydrogen in the synthesis gas can come from an electrolytic water process, and the electric energy can come from a cement waste heat power generation process. At the beginning when the amount of coal or coke is low, carbon dioxide exists in the decomposed gas, and as the biomass dosage increases, the carbon dioxide gradually disappears, and hydrogen begins to appear in the decomposed gas.
The foregoing description of the preferred embodiments of the invention is not intended to be limiting, but rather is intended to cover all modifications, equivalents, and alternatives falling within the spirit and principles of the invention.
Claims (6)
1. The process for producing cement and carbon monoxide by co-pyrolysis of cement raw materials and solid-phase carbon sources is characterized by comprising the following steps:
mixing cement raw materials with solid-phase carbon sources to form mixed raw materials, and then sending the mixed raw materials into a pyrolysis furnace; heating the mixed raw materials and carrying out coupling reduction thermal decomposition at the temperature of a pyrolysis furnace of 600-900 ℃ under the action of a gasifying agent to obtain a thermal solid-phase decomposition product and decomposition gas; sending the solid-phase decomposition product into a cement mineralization sintering section to generate cement clinker, grinding the cement clinker, and blending to obtain finished cement; the decomposed gas is collected and then recycled;
the decomposed gas at least comprises carbon monoxide; the gasifying agent and the solid-phase carbon source are gasified to obtain the reducing gas containing hydrogen;
the cement raw material comprises calcium carbonate, the solid-phase carbon source is one or more of straw, wood, bamboo and plastic, and the gasifying agent is one or more of water vapor and oxygen.
2. A process for the co-pyrolysis of cement raw meal and a solid carbon source to produce cement and carbon monoxide according to claim 1, wherein: the decomposed gas also contains one or more of hydrogen, methane and carbon dioxide.
3. A process for the co-pyrolysis of cement raw meal and a solid carbon source to produce cement and carbon monoxide according to claim 1, wherein: the temperature in the pyrolysis furnace is 600-880 ℃.
4. A process for the co-pyrolysis of cement raw meal and a solid carbon source to produce cement and carbon monoxide according to claim 1, wherein: the mass ratio of the solid-phase carbon source to the cement raw material is in the range of 0.05-10.
5. A process for the co-pyrolysis of cement raw meal and a solid carbon source to produce cement and carbon monoxide according to claim 1, wherein: and hydrogen and/or methane are/is also introduced into the pyrolysis furnace.
6. The process for producing cement and carbon monoxide by co-pyrolysis of a cement raw material and a solid carbon source according to claim 5, wherein: the hydrogen and the oxygen are sourced from an electrolytic water production process, and the electric energy of the electrolytic water production process is sourced from cement waste heat to generate electricity.
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