CN110548391B - 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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- 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
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- 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
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Abstract
The invention discloses a catalytic oxidation system for treating benzene organic matters by using a manganese-based catalyst prepared based on waste ternary electrode materials. The system comprises a first air pump, a second air pump, an air distribution system, a benzene series organic matter generating device, a buffer device, a preheating device and a catalytic reaction device; the system loads organic matters in the benzene series organic matter generating device out through the first air pump, the organic matters enter the buffering device, the second air pump is adjusted to dilute the loaded organic matters, the organic matters enter the preheating device after being stabilized, and then the organic matters are catalytically degraded through the catalytic reaction device which takes honeycomb cordierite as a carrier and is loaded with the manganese-based catalyst prepared based on the waste ternary electrode material. The catalytic oxidation system reduces the reaction activation energy of the oxidation reaction of the organic matters through the manganese-based catalyst prepared based on the waste ternary electrode material, further reduces the reaction temperature, improves the reaction rate, and degrades the organic matters into H2O and CO2The energy consumed by the oxidation system for treating the organic waste gas is reduced, and the degradation rate is improved.
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
In view of the above, the invention aims to provide a catalytic oxidation system for treating benzene organic matters by using a manganese-based catalyst prepared based on waste ternary electrode materials. The system can reduce the reaction activation energy of the organic oxidation reaction through the high-efficiency catalyst, further reduce the reaction temperature, improve the reaction rate and degrade the organic into H2O and CO2The energy consumed by the oxidation system for treating the organic waste gas is reduced, and the degradation rate is improved.
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/m3(ii) a Further, the concentration of the benzene-series organic substance is 1200 to 2500mg/m3。
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 0.5-1 g of waste lithium battery ternary positive electrode material LiNi by using 30-50 ml of aqua regia x y1−−Co x Mn y O2Preparing needed 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) and (3) treating and activating 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 ℃.
In the invention, the air distribution quantity of the first air pump is between 0 and 10L/min, and the air distribution quantity of the second air pump is between 0 and 50L/min; the space velocity in the catalytic reaction device is 5000--1。
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 for controlling gas concentration are used for loading toluene in a benzene organic matter generating device 4 in a temperature control system into a first buffer device by adjusting the first air pump 1, the second air pump 2 is adjusted to dilute the loaded toluene, the concentration of a target degradation product toluene is controlled, the total flow of gas is 12L/min, and the concentration of toluene gas is maintained at 1500mg/m3。
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 for drying at the temperature of 110 ℃ for 10 hours, and dissolving 1g of waste lithium battery ternary positive electrode material LiNi by 50ml of aqua regia x y1−−Co x Mn y O2Preparing needed impregnation liquid, placing the dried carrier in the prepared impregnation liquid for impregnation for 3 hours, then treating the impregnated catalyst in an oven at 100 ℃ for 10 hours, and finally treating and activating in a muffle furnace at 1200 ℃ to prepare the catalytic oxidation catalyst.
In the embodiment, 1g of ternary cathode material LiNi of electric waste lithium battery is taken x y1−−Co x Mn y O2Calcining in 50ml aqua regia in an electric furnace, digesting with microwave, measuring the content of metal elements by ICP-AES, wherein the content of manganese accounts for 66.49%, the content of nickel accounts for 16.11%, the content of cobalt accounts for 7.94%, the content of lithium accounts for 7.69%, and the content of aluminum accounts for 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 the catalytic reaction device to 375 ℃ and the concentration of inlet gas to 1500mg/m3Under the unchanged condition, airspeeds with certain intervals are respectively set, sampling analysis is respectively carried out at the front end and the rear end of the reactor after the reaction system stably runs for 10min, and the airspeeds are 5372.5, 5732.5, 7643.3, 9554.1 and 12420.4 h respectively-1In the case of (2), the toluene conversion efficiency was measured, and the results showed 5732.5h with space velocity-1The highest toluene conversion rate can reach more than 85%, and the toluene degradation rate of the prepared catalyst can be reduced to a certain extent along with the increase of the space velocity.
The required intake air concentration is obtained by adjusting the flow of the air pump, the temperature of the catalytic reaction device is controlled at 375 ℃, and the space velocity is controlled at 5732.5h-1After the catalytic reaction device runs stably, sampling is respectively carried out at the inlet and the outlet of the reaction device, and the inlet gas concentration gradient of the invention is 319.9, 982.4, 1622.7 and 2311.2 mg/m3In the case of (2), after sampling, gas chromatography analysis shows that the difference of the conversion rates of the methylbenzene when the concentration is highest and the concentration is lowest is below 4%, the difference is not large, and the degradation rate of the methylbenzene can reach 80%.
In one embodiment of the invention, the air distribution volume is controlled to be 12L/min, and the space velocity is controlled to be 5732.5h-1The concentration of toluene gas was 1500mg/m3For the organic matter degradation experiment of manganese-based catalyst prepared from waste ternary electrode material by using honeycomb cordierite as carrier and load, the temperature in the catalytic reaction device is set between 175-375 ℃, the gradient of the temperature is set to 25 ℃, the conversion rate of toluene starts to rise from 30% in the process of rising from 250-375 ℃, the toluene tends to be stable at 350 ℃, and the highest degradation efficiency can reach more than 85%.
In one embodiment of the invention, the air distribution volume is controlled to be 12L/min, and the space velocity is controlled to be 5732.5h-1The concentration of toluene gas was 1500mg/m3For honeycomb cordierite without manganese-based catalyst prepared from waste ternary electrode materialThe stone is subjected to an organic matter degradation experiment, the removal of toluene is almost unchanged along with the continuous increase of the temperature within the range of 200-350 ℃, and the highest removal rate of toluene by 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 (6)
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; the degraded benzene organic matters pass through a second buffer device and are discharged from a discharge port; wherein:
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 0.5-1 g of waste lithium battery ternary positive electrode material LiNi by using 30-50 ml of aqua regia x y1−−Co x Mn y O2Preparing needed 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) and (3) treating and activating in a muffle furnace at 1150-1250 ℃ to prepare the catalytic oxidation catalyst.
2. The catalytic oxidation system as set forth in claim 1, wherein the concentration of the benzene-based organic compound entering the preheating device is 300-2500mg/m3。
3. The catalytic oxidation system as set forth in claim 1, wherein the concentration of the benzene-based organic compound entering the preheating device is 1200-2500mg/m3。
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 temperature in the preheating device is 100-200 ℃; the temperature in the catalytic reaction device is 175-375 ℃.
6. The catalytic oxidation system of claim 1, wherein the air distribution capacity of the first air pump is between 0-10L/min, and the air distribution capacity of the second air pump is between 0-50L/min; the space velocity in the catalytic reaction device is 5000--1。
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| WO2012167280A1 (en) * | 2011-06-03 | 2012-12-06 | The Regents Of The University Of California | Manganese oxide and activated carbon fibers for removing particle, voc or ozone from a gas |
| CN105194941A (en) * | 2015-10-15 | 2015-12-30 | 苏州韵蓝环保科技有限公司 | Result-controllable organic waste gas treatment device adopting catalytic combustion |
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