CN109437604B - Method for realizing sensible heat recovery and tail gas utilization of burnt lime by utilizing methane reforming - Google Patents
Method for realizing sensible heat recovery and tail gas utilization of burnt lime by utilizing methane reforming Download PDFInfo
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- CN109437604B CN109437604B CN201811347885.7A CN201811347885A CN109437604B CN 109437604 B CN109437604 B CN 109437604B CN 201811347885 A CN201811347885 A CN 201811347885A CN 109437604 B CN109437604 B CN 109437604B
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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
- C04B2/00—Lime, magnesia or dolomite
- C04B2/10—Preheating, burning calcining or cooling
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- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
- C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
- C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
- C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/02—Processes for making hydrogen or synthesis gas
- C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
- C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
- C01B2203/0238—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a carbon dioxide reforming step
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- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/12—Feeding the process for making hydrogen or synthesis gas
- C01B2203/1205—Composition of the feed
- C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
- C01B2203/1235—Hydrocarbons
- C01B2203/1241—Natural gas or methane
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Abstract
A method for realizing the sensible heat recovery and tail gas utilization of burnt lime by utilizing methane reforming. Methane and carbon dioxide from tail gas are introduced into the lime kiln from bottom to top from a cooling zone at the lower part of the lime kiln, the methane and the carbon dioxide absorb sensible heat of burnt lime, the temperature of the sensible heat is gradually increased, the lime is initially cooled, the methane and the carbon dioxide are subjected to reforming reaction at the temperature of 700-1150 ℃ and in a space region, the reforming reaction absorbs a large amount of heat and is superposed with gas convection heat exchange, and further rapid cooling of high-temperature burnt lime is realized to improve the activity of the high-temperature burnt lime. The reformed product is the synthesis gas rich in carbon monoxide and hydrogen, can be used for the working procedures of chemical synthesis, combustion power generation, iron ore reduction and the like, and simultaneously realizes the quick cooling and sensible heat recovery of the burnt lime and reduces the emission of carbon dioxide. The method has simple process and low cost, and has better economic benefit and environmental protection benefit on the premise of ensuring high-efficiency production of the lime kiln and high quality of lime.
Description
Technical Field
The invention mainly belongs to the fields of clean and efficient utilization of coal, energy conservation and environmental protection, and particularly relates to a method for realizing sensible heat recovery of calcined lime and resource utilization of carbon dioxide by utilizing methane reforming, which is used for improving the quality of lime in a lime kiln, reducing the energy consumption in the lime calcination process and realizing the resource utilization of carbon dioxide in tail gas.
Background
Lime is one of important flux and slagging material in steel production, and large and medium-sized steel enterprises in China basically have lime production facilities. The lime industry scale of China reaches 2.5 hundred million tons by 2015, the actual capacity is 2.3 hundred million tons, and the lime capacity of China is steadily increased to 2.5 hundred million tons by 2020. Along with the improvement of the steel smelting process level in China, the lime production technology level is correspondingly improved, and the lime production technology level comprises the selection, mining, transportation and processing of limestone, the type selection and improvement of a kiln and the like. But still has the problems of high energy consumption, large discharge, uneven product quality and the like. The average thermal efficiency of the lime kiln is less than 40%, most of the lime kiln is mainly made of coal, and the standard coal of a lime unit reaches 145kg/t, so that the pollutant emission is serious. In addition, the mineral raw materials can emit a large amount of carbon dioxide in the lime roasting process, and the emission of carbon dioxide in the lime industry accounts for more than 2% of the national emission due to the energy consumption of the mineral raw materials. The energy-saving and emission-reducing work of the lime industry mainly comprises the aspects of furnace and kiln structure optimization, waste heat utilization (tail gas and burnt lime), kiln gas thickening and recycling and the like.
Regarding the cooling of burnt lime, the patent "lime kiln waste heat cooling system CN 201120436645.1" discloses a lime kiln waste heat cooling system, which mainly adopts forced convection cooling of a blower to improve the cooling speed of the lime kiln discharging area, accelerate lime discharging and promote lime production efficiency. The process is a mainstream process adopted in the existing lime production, but the concentration of carbon dioxide in tail gas is low, the difficulty in resource utilization of carbon dioxide is high, and the cost is high.
Regarding the recovery of the tail gas waste heat, the patent "a beam lime kiln waste heat recovery system CN 201610547868.2", "lime kiln tail gas waste heat utilization system CN 201620779912.8", "gas preheating device based on gas burning lime kiln tail gas CN 201220221618.7" and the like all disclose tail gas waste heat recovery methods with similar principles, which are used for preheating gas and combustion air or performing waste heat power generation, so that the power consumption of the lime kiln is reduced, and the economic benefit is improved. However, the quality benefit of the waste heat, i.e. the high-quality sensible heat and the low-quality sensible heat are mixed and recycled, and the problem of resource utilization of carbon dioxide in the tail gas is not considered in the waste heat recovery.
The mass fraction of carbon dioxide in the tail gas of the traditional lime kiln is low (about 18-25%), and the components contain more impurities, so that during recycling, impurities such as dust must be removed firstly, and then purification is carried out, and the investment and operation cost are higher than those of the industries such as petrochemical industry and the like. Nevertheless, in the middle of the 90's of the last century, 2 sets of devices for pressure swing adsorption and hot potassium process absorption were successively built in Shao steel, and a lime kiln carbon dioxide recovery device was also built in the former Wu-Shang-Steel works. At present, the recovery of carbon dioxide in lime kiln tail gas is listed in the overall construction plan in a steel branch plant newly built in Zhanjiang by Bao steel, and both Tai steel and saddle steel begin research and feasibility research work on the recovery and utilization of carbon dioxide resources.
Based on a sleeve lime kiln, in order to concentrate and enrich tail gas, a circulating roasting lime kiln using carbon dioxide as a circulating medium (such as "a lime kiln device CN201810438781.0 using circulating hot air" and "a lime kiln flue gas recirculation system CN 201810221778.3") has been proposed in recent years, and the purpose of enriching carbon dioxide can also be achieved by using pure oxygen for combustion. But the problem is how to achieve rapid cooling of the burnt high-temperature quicklime. If carbon dioxide is used as cooling gas, calcium carbonate can be regenerated from quick lime; if the traditional air cooling is adopted, the concentration of carbon dioxide in the tail gas is greatly diluted. In order to ensure the implementation of the new lime roasting process, the invention of a new cooling process for roasting lime is urgently needed.
Disclosure of Invention
Aiming at a circulating roasting lime kiln using carbon dioxide or flue gas with high carbon dioxide concentration as a circulating medium, the invention aims to solve the technical problems that: in addition to ensuring uniform and stable roasting, the production of the active lime needs to consider how to realize the rapid cooling of the burnt quicklime at high temperature (about 1150 ℃) to below 700 ℃ so as to ensure the high activity of the burnt quicklime; on the basis of realizing cooling, how to realize the efficient recycling of the sensible heat of lime; on the basis of realizing lime cooling, how to obtain tail gas with high carbon dioxide concentration and simultaneously avoid the reaction between the oxidation of the carbon dioxide and the burnt lime. Therefore, a new cooling process technology for burning lime must be developed, heat recovery can be realized, and the tail gas resource utilization is facilitated, so that the high efficiency, energy conservation and emission reduction of the lime production process are realized.
The invention provides a method for realizing sensible heat recovery and tail gas resource utilization of burnt lime by utilizing methane reforming, which is characterized in that methane and carbon dioxide are introduced into a lime kiln from the bottom to the top in a cooling zone at the lower part of the lime kiln, the cooling and sensible heat recovery of the burnt lime are realized by utilizing the heat absorption of the methane reforming reaction, and the obtained products are high-quality quick lime and synthesis gas rich in carbon monoxide and hydrogen.
The invention is realized by the following technical scheme:
(1) introducing carbon dioxide and methane at room temperature or after preheating from the lower part of a lime kiln in a countercurrent manner, gradually heating the carbon dioxide and the methane, gradually lowering the temperature of lime, enabling the temperature of the lime to be higher than the temperature of introduced gas, enabling the volume flow of the carbon dioxide and the volume flow of the methane to be the same, and enabling the total flow of raw material gas to be 40-80 m3T lime。
(2) When the temperature of the raw material gas reaches 700 ℃, the raw material gas interacts with the supported catalyst, carbon dioxide and methane are converted into carbon monoxide and hydrogen, the raw material gas per cubic meter absorbs 5000-6000 kJ of heat at the same time, the temperature of lime is correspondingly and rapidly reduced, and a high-quality product with the activity degree of more than 320 is formed.
Further, the used carbon dioxide is from the tail gas of the lime kiln, the mixed feed gas consisting of the carbon dioxide and methane enters the lime kiln from the lower part of the lime kiln through a heat exchange pipeline for heat exchange, the heat exchange rate is regulated and controlled by regulating the pipe diameter and the shape of a heat exchange pipe, an alumina honeycomb porous material is arranged in the pipeline positioned in the 700-1150 ℃, and a reforming catalyst is loaded in the porous material.
Furthermore, the gas obtained after reforming can be used for the working procedures of chemical synthesis, combustion power generation, iron ore reduction and the like, and H can be improved by mixing and blending with coke oven gas2the/CO thereby improves the efficiency of the catalyst for chemical synthesis and iron ore reduction.
The invention has the beneficial technical effects that:
the invention can ensure the smooth implementation of the new process of the circulating roasting lime kiln using carbon dioxide as a circulating medium, realize the rapid cooling of the burnt high-temperature quicklime, obtain the quicklime with high activity and the tail gas with high carbon dioxide concentration, and provide possibility for reducing the purification cost of carbon dioxide and the subsequent utilization thereof. Meanwhile, by means of the reforming reaction of methane and carbon dioxide, the reformed gas with high carbon monoxide and hydrogen concentration is obtained while the quick cooling of the high-temperature quicklime is realized, and the sensible heat of the lime is recovered. The sensible heat recovered by the process accounts for about 50% of the total sensible heat of the burnt lime, and the carbon dioxide recycled accounts for about 10% of the total amount of the carbon dioxide released by the calcination decomposition of the limestone. The invention essentially converts the high-temperature sensible heat of the burnt lime into chemical energy of reformed gas and fixes partial carbon dioxide. The process is easy to implement and popularize, has low cost, and has better economic benefit and environmental protection benefit on the premise of ensuring high-efficiency production of the lime kiln and high quality of lime.
Drawings
Fig. 1 is a schematic flow chart of a method for recovering sensible heat of burnt lime and utilizing tail gas by utilizing methane reforming in the embodiment of the invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
On the contrary, the invention is intended to cover alternatives, modifications, equivalents and alternatives which may be included within the spirit and scope of the invention as defined by the appended claims. Furthermore, in the following detailed description of the present invention, certain specific details are set forth in order to provide a better understanding of the present invention. It will be apparent to one skilled in the art that the present invention may be practiced without these specific details.
Example 1
For a circulating roasting lime kiln taking 1000 tons of carbon dioxide produced per day as a circulating medium, the mixed raw material gas of methane and carbon dioxide at room temperature enters a cooling area of the lime kiln from a pipeline near a discharge port at the bottom of the lime kiln, and the total gas flow is 40m3And/t lime. The pipe diameter of the air inlet pipeline gradually becomes thicker along with the increase of the depth of the air inlet pipeline entering the kiln body so as to increase the heat exchange area. The inlet pipe is led out of the kiln body at a position which is close to the lime roasting finishing height and is about 1150 ℃. Alumina honeycomb porous materials are filled in the 700-1150 ℃ region in the pipeline to increase the heat exchange area, and the region is also the region where methane and carbon dioxide are subjected to reforming reaction. The gas conversion rate is close to 80 percent, the reformed gas is discharged out of the kiln through a pipeline, and the obtained gas flow rate is 76m3And/t lime is used for synthesizing the raw material gas of the methanol after heat exchange to about 220 ℃. The composition of the gas obtained after reforming is shown in table 1, and the recovered heat can be used for steam production. The lime obtained had an activity of 340. After long-time operation, the filled alumina honeycomb porous material is found to have carbon precipitation to a certain degree near a high-temperature area.
TABLE 1 reformed gas composition
Example 2
For a pure oxygen combustion roasting lime kiln (the fuel is converter gas) with the daily yield of 1000 tons, mixed raw material gas of methane and carbon dioxide preheated to 200 ℃ enters a cooling area of the lime kiln from a pipeline near a discharge port at the bottom of the lime kiln, and the total gas flow is 80m3And/t lime. The pipe diameter of the air inlet pipeline gradually becomes thicker along with the increase of the depth of the air inlet pipeline entering the kiln body so as to increase the heat exchange area. The inlet pipe is led out of the kiln body at a position which is close to the lime roasting finishing height and is about 1150 ℃. And filling an alumina honeycomb porous material carrying a nickel-based catalyst in a 700-1150 ℃ interval in the pipeline to increase the heat exchange area and promote reforming conversion. The gas conversion rate is close to 96 percent, the reformed gas is discharged out of the kiln through a pipeline, and the obtained gas flow rate is 157m3And (2) exchanging heat for lime to about 220 ℃, and supplementing carbon dioxide to 5% to obtain the raw material gas for synthesizing the methanol. The composition of the gas obtained after reforming is shown in table 1, and the recovered heat can be used for preheating methane and carbon dioxide gas. The activity of the obtained lime is 360. No carbon precipitation phenomenon occurs after long-time operation.
TABLE 2 reformed gas composition
Claims (3)
1. A method for realizing sensible heat recovery and tail gas utilization of burnt lime by utilizing methane reforming is characterized in that methane and carbon dioxide are introduced into a lime kiln from bottom to top from a cooling zone at the lower part of the lime kiln, the cooling and sensible heat recovery of the burnt lime are realized by utilizing the heat absorption of the methane reforming reaction, and the obtained products are high-quality quicklime and synthesis gas rich in carbon monoxide and hydrogen;
the main production process flow is as follows:
(1) introducing carbon dioxide and methane at room temperature or after preheating from the lower part of the lime kiln in a countercurrent mannerThe temperature of the alkane is gradually increased, the temperature of the lime is gradually reduced, the temperature of the lime is higher than the temperature of the introduced gas, the volume flow of the carbon dioxide and the volume flow of the methane are the same, and the total flow of the raw material gas is 40-80 m3T lime;
(2) when the temperature of the raw material gas reaches 700 ℃, the raw material gas interacts with the supported catalyst, carbon dioxide and methane are converted into carbon monoxide and hydrogen, the raw material gas per cubic meter absorbs 5000-6000 kJ of heat at the same time, the temperature of lime is correspondingly and rapidly reduced, and a high-quality product with the activity degree of more than 320 is formed.
2. The method for realizing sensible heat recovery and tail gas utilization of burnt lime by utilizing methane reforming as claimed in claim 1, wherein the used carbon dioxide is from the tail gas of a lime kiln, the mixed feed gas consisting of the carbon dioxide and the methane enters the lime kiln from the lower part of the lime kiln through a heat exchange pipeline for heat exchange, the heat exchange rate is regulated and controlled by regulating the pipe diameter and the shape of a heat exchange pipe, an alumina honeycomb porous material is arranged in a pipeline positioned in a 700-1150 ℃ region, and a reforming catalyst is loaded in the porous material.
3. The method as claimed in claim 1, wherein the reformed gas is used in chemical synthesis, combustion power generation, and iron ore reduction processes, and is mixed with coke oven gas to increase H2the/CO thereby improves the efficiency of the catalyst for chemical synthesis and iron ore reduction.
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