CN110548391A - Catalytic oxidation system for treating benzene organic matters by manganese-based catalyst prepared based on waste ternary electrode material - Google Patents
Catalytic oxidation system for treating benzene organic matters by manganese-based catalyst prepared based on waste ternary electrode material Download PDFInfo
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- CN110548391A CN110548391A CN201910643681.6A CN201910643681A CN110548391A CN 110548391 A CN110548391 A CN 110548391A CN 201910643681 A CN201910643681 A CN 201910643681A CN 110548391 A CN110548391 A CN 110548391A
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8668—Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/76—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
- B01J23/84—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36 with arsenic, antimony, bismuth, vanadium, niobium, tantalum, polonium, chromium, molybdenum, tungsten, manganese, technetium or rhenium
- B01J23/889—Manganese, technetium or rhenium
- B01J23/8892—Manganese
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Abstract
2 2The invention discloses a catalytic oxidation system for treating benzene organic matters by using a manganese-based catalyst prepared based on waste ternary electrode materials, which comprises a first air pump, a second air pump, an air distribution system, a benzene organic matter generating device, a buffer device, a preheating device and a catalytic reaction device, wherein the system loads organic matters in the benzene organic matter generating device out of the buffer device by using the first air pump, adjusts the second air pump to dilute the loaded organic matters, and then the diluted organic matters enter the preheating device after stabilization, and then the catalytic reaction device is loaded with the manganese-based catalyst prepared based on the waste ternary electrode materials by using honeycomb cordierite as a carrier to enable the organic matters to be catalytically degraded.
Description
Technical Field
The invention belongs to the technical field of waste gas treatment, and particularly relates to a catalytic oxidation system for treating benzene organic matters by using a manganese-based catalyst prepared based on waste ternary electrode materials.
background
In recent years, frequent haze has seriously affected the surrounding environment and human health, and people attract extensive attention, one of the major causes of frequent haze is the release of toxic and harmful gases, wherein the generation of VOCs occupies an important proportion, and various regulatory regulations and standards are issued by the ministry of ecological environment to limit the emission of polluted gases. In the emission of VOCs, the proportion of waste gas that the chemical industry produced is the biggest, and the waste gas that the chemical industry produced has characteristics such as composition complicacy, concentration is big, unstability, it is most effective to the waste gas that the chemical industry produced, the technique that uses the most extensively is direct thermal combustion and thermal catalytic oxidation, direct thermal combustion needs extra fuel of adding, because the temperature of its burning is than, also than higher to the requirement of equipment material, cause its running cost greatly increased, direct combustion under the high temperature can produce thermal type nitrogen oxide and cause secondary pollution in addition, in addition there is incomplete combustion phenomenon. In comparison, the catalytic oxidation temperature of the thermal catalytic oxidation is low, no additional fuel is needed, no secondary pollution problem exists, the operation cost is low, the organic waste gas generated in the chemical industry does not need to be concentrated and can be directly used for catalytic combustion, the operation cost of the thermal catalytic oxidation is increased by selecting the noble metal, compared with the noble metal, the general transition metal oxide also has a good catalytic degradation effect, the performance of the catalyst obtained by compounding the general transition metal can be comparable with that of the noble metal, and the selection of the catalyst is critical to the whole technology. The waste lithium battery is widely applied at present and faces the problem of large quantity of scrapped, the anode material contains a large quantity of valuable metal elements, and the waste ternary electrode material is applied to the preparation of the catalytic oxidation catalyst, so that the recovery procedure of the battery anode material is simplified, the cost of catalytic oxidation degradation is reduced, the purpose of treating wastes with processes of wastes is achieved, the catalytic oxidation technology can play an important role in industrial waste gas treatment, and the advantages are achieved.
disclosure of Invention
The system can reduce the reaction activation energy of the oxidation reaction of the organic matters through the high-efficiency catalyst, further reduce the reaction temperature, improve the reaction rate, degrade the organic matters into H 2 O and CO 2, reduce the energy consumed by the oxidation system for treating organic waste gas, and improve the degradation rate.
the technical scheme of the invention is specifically introduced as follows.
A catalytic oxidation system for treating benzene organic matters by using a manganese-based catalyst prepared based on waste ternary electrode materials comprises a first air pump, a second air pump, an air distribution system, a benzene organic matter generating device, a first buffer device, a preheating device, a catalytic reaction device and a second buffer device; the first air pump is sequentially connected with the benzene system organic matter generating device and the first buffer device through the air distribution system and used for loading the benzene system organic matters into the first buffer device, and the second air pump is connected with the first buffer device through the air distribution system and used for diluting the loaded benzene system organic matters; the first buffer device is connected with the preheating device and the catalytic reaction device sequentially through a pipeline and is used for heating benzene organic matters through the preheating device and then enabling the benzene organic matters to enter the catalytic reaction device for catalytic oxidation reaction, and degrading the benzene organic matters; the catalytic reaction device adopts a tubular reactor, the tubular reactor is heated by a second thermocouple, the second thermocouple is connected with the second temperature controller, and a supported manganese-based catalyst prepared based on waste ternary electrode materials is arranged in the tubular reactor; and the degraded benzene organic matters are discharged from the discharge port after passing through the second buffer device.
In the invention, the concentration of the benzene series organic matters entering the preheating device is 300-2500mg/m 3, and further the concentration of the benzene series organic matters is 1200 ~ 2500-2500 mg/m 3.
In the present invention, the benzene-series organic substance includes benzene and toluene.
In the invention, the supported manganese-based catalyst prepared based on the waste ternary electrode material takes honeycomb cordierite as a carrier; the preparation method comprises the following steps:
(1) Placing the honeycomb cordierite into a drying box to be dried for 10-12 hours at the temperature of 100-110 ℃;
(2) Dissolving 0.5 ~ 1g of waste lithium battery ternary positive electrode material LiNi 1- x - y Co x Mn y O 2 by using 30 ~ 50ml of aqua regia to prepare required impregnation liquid;
(3) placing the carrier dried in the step (1) into the impregnation liquid prepared in the step (2) for impregnation for 3-4 hours;
(4) Treating the impregnated sample in an oven at a temperature of 100-110 ℃ for 10-12 hours;
(5) The catalyst is treated and activated in a muffle furnace at 1150 ~ 1250 ℃ to prepare the catalytic oxidation catalyst.
In the invention, the temperature in the preheating device is 100-200 ℃; the temperature in the catalytic reaction device is 175-375 ℃.
-1in the invention, the air distribution amount of the first air pump is between 0 and 10L/min, the air distribution amount of the second air pump is between 0 and 50L/min, and the space velocity in the catalytic reaction device is 5000-.
Compared with the prior art, the invention has the beneficial effects that:
The invention can reduce the degradation temperature of the benzene organic matters, and compared with the traditional combustion process, the reaction system is more energy-saving.
The active component of the catalyst adopted by the invention is the composite metal oxide prepared based on the waste lithium battery ternary cathode material NCM, and the catalyst has the characteristics of low price, reproducibility and higher benzene organic matter degradation rate compared with the traditional noble metal catalyst.
The invention selects the honeycomb cordierite as the carrier to carry out activity test, and has the characteristics of high mechanical strength, small pressure drop, good heat resistance and the like compared with the traditional carrier.
Drawings
FIG. 1 is a schematic structural diagram of a catalytic oxidation system for treating organic waste gas.
Fig. 2 is a cross-sectional view of a honeycomb cordierite carrier.
reference numbers in the figures: 1-a first air pump, 2-a second air pump, 3-a gas distribution system, 4-a benzene series organic matter generating device, 5-a first buffer device, 6-a ceramic heat accumulator, 7-a first temperature control instrument, 8-a second temperature control instrument, 9-a tubular reactor, 10-a second buffer device, 11-a tubular furnace, 12-a discharge port, 13-a sampling port, 14-a honeycomb cordierite carrier, 15-a first thermocouple and 16-a second thermocouple.
Detailed Description
The technical scheme of the invention is explained in detail in the following by combining the drawings and the embodiment.
The present invention provides a catalytic oxidation system (fig. 1) capable of efficiently treating benzene-based organic compounds, comprising:
The device comprises a first air pump 1, a second air pump 2, an air distribution system 3, a benzene organic matter generating device 4 and a first buffer device 5; the benzene-series organic matter generator 4 includes a temperature control system, which maintains a low temperature, for example, 1 ℃, through the temperature control system to ensure that the benzene-series organic matter in the benzene-series organic matter generator 4 maintains a liquid state. Meanwhile, the benzene series organic matters carried out only by the air (the first air pump 1) cannot meet the experimental requirements, and the concentration of the carried benzene series organic matters is regulated by diluting the carried benzene series organic matters with another air flow (the second air pump 2). The flow of the air pump is intelligently controlled by a computer so as to adjust the concentration of the benzene organic matters in the first buffer device 5.
in the embodiment, a first air pump 1 (0-10L/min) for blowing liquid toluene 3 and a second air pump 2 (0-50L/min) for blowing air are used for controlling the gas concentration, toluene in a benzene organic matter generating device 4 in a temperature control system is loaded into a first buffer device by adjusting the first air pump 1, the loaded toluene is diluted by adjusting the second air pump 2, the concentration of a target degradation product toluene is controlled, the total flow of gas is 12L/min, and the toluene gas concentration is maintained at 1500mg/m 3.
After the gas is stabilized, the toluene passing through the gas distribution system 3 enters a ceramic heat accumulator 6 in the preheating device, the temperature of the toluene serving as a target pollutant is raised by a first thermocouple 15 connected with a first temperature controller 7, the selected ceramic heat accumulator 6 is a cylinder, the diameter of the cross section of the selected ceramic heat accumulator is 20 cm, and the aperture of a honeycomb hole in the heat accumulator is 0.5 cm; the ceramic heat accumulator 6 selected in the system has the characteristics of high strength, high temperature resistance, corrosion resistance, wear resistance and the like. The temperature in the preheating device is between 100 ℃ and 200 ℃.
The preheated gas enters a catalytic reaction device, the device selects a tubular reactor 9 as the catalytic reaction device, the tubular reactor 9 is a quartz tube, the length of the tube is 450 mm, the inner diameter is 22 mm, the outer diameter is 25 mm, the volume is 168 mL, a catalyst is placed in the quartz tube, the quartz tube is heated by the tubular furnace, the bed temperature of the quartz tube is tested by a second thermocouple 16, and the thermocouple 16 is connected with a second temperature controller 8 to control the heating temperature of the tubular furnace to the bed;
In the embodiment, the specific preparation method of the manganese-based catalyst prepared from the waste ternary electrode material as the catalyst placed in the tubular reactor 9 is as follows:
Placing cordierite in a drying oven at the temperature of 110 ℃ for drying for 10 hours, dissolving 1g of waste lithium battery ternary positive electrode material LiNi 1- x - y Co x Mn y O 2 by 50ml of aqua regia to prepare a required impregnation liquid, placing a dried carrier in the prepared impregnation liquid for impregnation for 3 hours, then treating the impregnated catalyst in an oven at the temperature of 100 ℃ for 10 hours, and finally treating and activating in a muffle furnace at the temperature of 1200 ℃ to prepare the catalytic oxidation catalyst.
In the embodiment, 1g of ternary cathode material LiNi 1- x - y Co x Mn y O 2 of electric waste lithium batteries is calcined in an electric furnace and then placed in 50ml of aqua regia, and the metal element content is measured by ICP-AES after microwave digestion treatment, wherein the manganese accounts for 66.49%, the nickel accounts for 16.11%, the cobalt accounts for 7.94%, the lithium accounts for 7.69%, and the aluminum content is a small amount of 1.78%.
The degraded toluene gas enters the residual organic gas in the tail gas through a second buffer device 10 with active carbon
And (4) removing by adsorption.
After the system is stabilized, respectively sampling inlet and outlet gases, wherein the inlet concentration is sampled through a sampling port 13, and the outlet concentration is sampled through a discharge port 12; the performance of the organic exhaust gas catalytic oxidation system was evaluated by measuring the gas concentration by a gas chromatograph after sampling with a sampling needle.
environmental condition influence factor test
The temperature in the preheating device is set to be 150 ℃, and the measurement is carried out after the catalytic degradation reaction device stably runs for 10 min. The gas concentration is controlled to be maintained stably by changing the regulating valves of the two paths of gas pumps.
The invention controls the temperature in a catalytic reaction device to be 375 ℃ and the concentration of inlet air to be 1500mg/m 3, respectively sets space velocities with certain intervals under the unchanged condition, the reaction system is sampled and analyzed at the front end and the rear end of the reactor after running stably for 10min, and the toluene conversion efficiency is measured under the conditions that the space velocities are 5372.5, 5732.5, 7643.3, 9554.1 and 12420.4 h -1, respectively, the result shows that the toluene conversion rate is highest and can reach more than 85 percent when the space velocity is 5732.5h -1, and the degradation rate of the prepared catalyst to toluene is reduced to a certain degree when the space velocity is increased.
The required inlet gas concentration is obtained by adjusting the flow rate of the air pump, the temperature of the catalytic reaction device is controlled at 375 ℃, the airspeed is controlled at 5732.5h -1, the inlet and the outlet of the catalytic reaction device are respectively sampled after the catalytic reaction device operates stably, and the conversion rate difference of methylbenzene is less than 4% and has small difference when the concentration is the highest and the concentration is the lowest through gas chromatography analysis after sampling under the condition that the inlet gas concentration gradient of the catalytic reaction device is 319.9, 982.4, 1622.7 and 2311.2 mg/m 3.
In one example of the invention, the gas distribution amount is controlled to be 12L/min, the space velocity is 5732.5h -1, the concentration of toluene gas is 1500mg/m 3, the degradation experiment of organic matters is carried out on a manganese-based catalyst which takes honeycomb cordierite as a carrier and takes a load as a waste ternary electrode material, the temperature in a catalytic reaction device is set between 175-375 ℃, the gradient of the temperature is set to be 25 ℃, the conversion rate of toluene starts to rise from 30 percent in the process that the temperature rises from 250-375 ℃, the toluene tends to be stable at 350 ℃, and the degradation efficiency can reach more than 85 percent at most.
In one embodiment of the invention, the gas distribution amount is controlled to be 12L/min, the space velocity is 5732.5h -1, the concentration of toluene gas is 1500mg/m 3, the organic matter degradation experiment is carried out on the honeycomb cordierite which is not loaded with the manganese-based catalyst prepared from the waste ternary electrode material, the toluene removal is almost not changed along with the continuous rising of the temperature within the range of 200 ℃ and 350 ℃, and the highest toluene removal rate of the unloaded cordierite carrier is not more than 5%.
In summary, the catalytic oxidation system for organic pollutants provided by the invention uses benzene organic matters such as toluene as degradation objects, uses the honeycomb ceramic heat accumulator to preheat the organic pollutants, controls the temperature at 100-. Therefore, the invention has the advantages of environmental protection, economy, high efficiency and the like.
Although specific implementations and cases have been set forth for the invention, the above-described embodiments are illustrative, and the scope of the invention is not limited thereto. Those skilled in the art can modify the above-described embodiments within the scope of the present invention.
Claims (7)
1. Catalytic oxidation system for treating benzene organic matters by using manganese-based catalyst prepared based on waste ternary electrode material
characterized in that the device comprises a first air pump, a second air pump, an air distribution system, a benzene series organic matter generating device, a first buffer device, a preheating device, a catalytic reaction device and a second buffer device; the first air pump is sequentially connected with the benzene system organic matter generating device and the first buffer device through the air distribution system and used for loading the benzene system organic matters into the first buffer device, and the second air pump is connected with the first buffer device through the air distribution system and used for diluting the loaded benzene system organic matters; the first buffer device is connected with the preheating device and the catalytic reaction device sequentially through a pipeline and is used for heating benzene organic matters through the preheating device and then enabling the benzene organic matters to enter the catalytic reaction device for catalytic oxidation reaction, and degrading the benzene organic matters; the catalytic reaction device adopts a tubular reactor, the tubular reactor is heated by a second thermocouple, the second thermocouple is connected with the second temperature controller, and a supported manganese-based catalyst prepared based on waste ternary electrode materials is arranged in the tubular reactor; and the degraded benzene organic matters are discharged from the discharge port after passing through the second buffer device.
2. The catalytic oxidation system according to claim 1, wherein the concentration of the benzene-based organic compound entering the preheating device is 300-2500mg/m 3.
3. The catalytic oxidation system according to claim 1, wherein the concentration of the benzene-based organic compound entering the preheating device is 1200-2500mg/m 3.
4. The catalytic oxidation system of claim 1, wherein the benzene-based organic comprises benzene and toluene.
5. The catalytic oxidation system of claim 1, wherein the supported manganese-based catalyst prepared based on the waste ternary electrode material is prepared by using honeycomb cordierite as a carrier; the preparation method comprises the following steps:
(1) Placing the honeycomb cordierite into a drying box to be dried for 10-12 hours at the temperature of 100-110 ℃;
(2) Dissolving 0.5 ~ 1g of waste lithium battery ternary positive electrode material LiNi 1- x - y Co x Mn y O 2 by using 30 ~ 50ml of aqua regia to prepare required impregnation liquid;
(3) Placing the carrier dried in the step (1) into the impregnation liquid prepared in the step (2) for impregnation for 3-4 hours;
(4) Treating the impregnated sample in an oven at a temperature of 100-110 ℃ for 10-12 hours;
(5) The catalyst is treated and activated in a muffle furnace at 1150 ~ 1250 ℃ to prepare the catalytic oxidation catalyst.
6. The catalytic oxidation system of claim 1, wherein the temperature in the preheating device is 100-200 ℃; the temperature in the catalytic reaction device is 175-375 ℃.
-17. The catalytic oxidation system of claim 1, wherein the air distribution amount of the first air pump is 0-10L/min, the air distribution amount of the second air pump is 0-50L/min, and the space velocity in the catalytic reaction device is 5000-.
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