CN112495373A - Manganese-containing soil low-temperature denitration catalyst and preparation method thereof - Google Patents
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Abstract
The invention aims to solve the problems in the prior art and provides a manganese-containing soil low-temperature denitration catalyst and a preparation method thereof. The method utilizes the polluted manganese-containing soil in the manganese ore area to carry out active substance loading modification treatment, and can achieve very excellent denitration activity.
Description
Technical Field
The invention relates to the field of atmospheric nitrogen oxide pollution control, and particularly relates to a manganese-containing soil low-temperature denitration catalyst and a preparation method thereof.
Background
Manganese-containing soil is a solid waste. The smelting activity of manganese is the main cause of soil pollution in a manganese ore area, and the harm of the soil pollution has the characteristics of long-term property and irreversible transformation. And heavy metals in the manganese-containing soil continuously pollute underground water and surface water along with runoff and can enter the bodies of animals or human bodies through food chains to harm health.
Furthermore, Nitrogen Oxides (NO)x) Second only to inhalable particles and SO2The emission of one of the main atmospheric pollutants poses a great threat to human health and living environment. With the continuous and high-speed development of industry and urbanization in China, the emission of nitrogen oxides is continuously increased, and the nitrogen oxides become the air pollutants which are mainly controlled. The SCR selective catalytic reduction technology is the most main flue gas NO at presentxThe principle of the removal is NH3Is a reducing agent, selectively catalyzes and reduces nitrogen oxides in the flue gas under the action of a catalyst to finally generate nontoxic and harmless N2And H2And O. The most widely used SCR catalyst in industry is TiO2As a carrier, loading an active component V2O5The prepared vanadium-titanium catalyst. Such catalysts are expensive and not suitable for low temperature flue gases. Therefore, the research on the low-temperature denitration catalyst which is low in cost, simple in preparation process and excellent in performance at low temperature has great significance.
Disclosure of Invention
The invention aims to solve the problems in the prior art and provides a manganese-containing soil low-temperature denitration catalyst and a preparation method thereof. The method utilizes the polluted manganese-containing soil in the manganese ore area to carry out active substance loading modification treatment, and can achieve very excellent denitration activity.
The manganese-containing soil low-temperature denitration catalyst is characterized by comprising the following steps of:
1) collecting manganese-containing soil at different positions in a manganese ore area, screening the collected manganese-containing soil, and drying a sample with a certain particle size range to obtain a manganese-containing soil carrier;
2) taking inorganic salt of rare earth element cerium as an active component;
taking the manganese-containing soil obtained in the step 1) as a carrier, weighing the active component according to the manganese content in the carrier, and dissolving the weighed active component in water to obtain a precursor solution;
3) dipping the manganese-containing soil obtained in the step 1) into the precursor solution obtained in the step 2);
4) calcining the product obtained in the step 3) in an air atmosphere, and cooling to obtain the manganese-containing soil low-temperature denitration catalyst.
Further, the manganese ore area in the step 1) is located in the Yangxi town of Xishan county, Chongqing city, the manganese-containing soil is the polluted waste of the manganese ore area, the particle size range is 20-100 meshes, the drying temperature is 90-110 ℃, the drying time is 6-10 hours, and the low-temperature denitration catalyst for the manganese-containing soil takes the manganese-containing soil as a carrier;
further, the inorganic salt of the rare earth element cerium in the step 2) is cerium nitrate, the active component is weighed according to the manganese content in the carrier, and the molar mass ratio of manganese to cerium is Mn: Ce ═ 1: 1. 1.5: 1. 2: 1;
further, the manganese-containing soil low-temperature denitration catalyst and the preparation method thereof are characterized in that the manganese-containing soil mainly comprises the following components in percentage by mass: SiO 2255-60％、MnO 5-10％、Al2O315-20％、FeO 5-10％、CaO 1-5％、K2O1-5％、P≤1％、Na≤1％。
Further, after dipping the precursor solution in the manganese-containing soil in the step 3), carrying out ultrasonic treatment and standing, then carrying out water bath evaporation to dryness, and finally carrying out drying treatment;
the ultrasonic frequency is 40KHz, and the ultrasonic time range is 30-60 min;
the water bath time is 1-3 h, and the water bath temperature is 40-60 ℃;
the drying temperature is 90-110 ℃, and the drying time is 6-10 h;
further, the product in the step 4) is calcined in an air atmosphere:
in the calcining treatment process, the temperature of the muffle furnace is increased to 300-500 ℃ from room temperature at the heating rate of 5-10 ℃/min, and the muffle furnace is naturally cooled to room temperature after being calcined for 2-4 h.
It is worth explaining that the manganese-containing soil is contaminated solid waste in the smelting process of manganese ores, contains rich manganese elements, is high in mechanical strength and simple in preparation method, has excellent denitration activity, is improved after being treated by loading active substances, is low in preparation cost, and has the advantages of being an excellent high-efficiency low-temperature denitration catalyst.
The manganese-containing soil is subjected to drying treatment after plants and large stone impurities are simply removed, excellent denitration activity is shown, and the activity is further improved after active substances are loaded. Therefore, the invention provides the manganese-containing soil low-temperature denitration catalyst and the preparation method thereof through resource and harmless utilization of the manganese-containing soil, effectively reduces the secondary pollution of nitrogen oxides, and can be applied to treatment of waste gas discharged from garbage incineration plants, sintering plants, cement plants and the like.
Drawings
FIG. 1 shows the curve of denitration activity of manganese-containing soil catalyst with different preparation methods along with the change of temperature
Detailed Description
The present invention is further illustrated by the following examples, but it should not be construed that the scope of the above-described subject matter is limited to the following examples. Various substitutions and alterations can be made without departing from the technical idea of the invention and the scope of the invention is covered by the present invention according to the common technical knowledge and the conventional means in the field.
Example 1:
1) collecting manganese-containing soil at different positions in a manganese ore area, screening the collected manganese-containing soil, and drying a sample with a certain particle size range to obtain a manganese-containing soil carrier;
the manganese ore area is positioned in the Luxi town of Xishan county in Chongqing city;
the manganese-containing soil is polluted waste of a manganese ore area;
the particle size range is 40-100 meshes;
the drying temperature is 100 ℃, and the drying time is 6 hours;
the low-temperature denitration catalyst for the manganese-containing soil takes the manganese-containing soil as a carrier;
2) taking inorganic salt of rare earth element cerium as an active component;
taking the manganese-containing soil obtained in the step 1) as a carrier, weighing the active component according to the manganese content in the carrier, and dissolving the weighed active component in water to obtain a precursor solution;
the inorganic salt of the rare earth element cerium is cerium nitrate;
the manganese content of the manganese-containing soil is MnO of 8.2%;
the molar mass ratio of the manganese to the cerium is Mn to Ce as 1: 1;
3) dipping the manganese-containing soil obtained in the step 1) into the precursor solution obtained in the step 2); after dipping the manganese-containing soil into the precursor solution, carrying out ultrasonic treatment and standing, then evaporating to dryness in a water bath, and finally carrying out drying treatment;
the ultrasonic frequency is 40KHz, and the ultrasonic time range is 30 min;
the water bath time is 2 hours, and the water bath temperature is 60 ℃;
the drying treatment temperature is 100 ℃, and the drying time is 10 hours;
4) calcining the product obtained in the step 3) in an air atmosphere, and cooling to obtain the manganese-containing soil low-temperature denitration catalyst.
In the calcining treatment process, the temperature of the muffle furnace is increased to 500 ℃ from room temperature at the heating rate of 5 ℃/min, and the low-temperature denitration catalyst for the manganese-containing soil is obtained after calcining for 4 hours and then naturally cooling to room temperature.
Example 2:
the catalyst was prepared according to the method of example 1, with the only difference that: the molar mass ratio of manganese to cerium in the step 2) is Mn to Ce being 1.5: 1;
example 3:
the catalyst was prepared according to the method of example 1, with the only difference that: the molar mass ratio of manganese to cerium in the step 2) is Mn: Ce ═ 2: 1;
control experiment:
collecting manganese-containing soil at different positions in a manganese ore area, screening the collected manganese-containing soil, and drying a sample with a certain particle size range to obtain a low-temperature denitration catalyst for the manganese-containing soil;
the manganese ore area is positioned in the Luxi town of Xishan county in Chongqing city;
the manganese-containing soil is polluted waste of a manganese ore area;
the particle size range is 40-100 meshes;
the drying temperature is 100 ℃, and the drying time is 6 hours;
the low-temperature denitration catalyst for the manganese-containing soil takes the manganese-containing soil as a carrier.
And (3) comparative analysis:
evaluation of catalyst Performance: 2g of each of the manganese-containing soil catalysts prepared in examples 1 to 3 and the control experiment were placed in a fixed bed reactor, and simulated flue gas was introduced and the temperature was raised from room temperature to 250 ℃. The simulated flue gas consists of 500ppm of NO, 5 vol.% of O2500ppm of NH3And balance gas N2And (4) forming. The curve of the denitration activity of the manganese-containing soil low-temperature denitration catalyst with different preparation methods along with the change of the temperature is shown in figure 1, and the experimental results are shown in the following table.
The results in the table show that 1) when the manganese-containing soil is not loaded with active substances, the manganese-containing soil has excellent denitration activity in the low temperature range of 75-250 ℃, and the denitration activity at 150-200 ℃ reaches more than 98%. 2) The loading of active element cerium has obvious promotion on the activity of the manganese-containing soil, wherein when the molar mass ratio of manganese to cerium is Mn: Ce is 1.5: the effect is optimal at 1 time, and the denitration activity at 125-250 ℃ reaches more than 99%, which shows that the manganese-containing soil low-temperature denitration catalyst prepared by the manganese-containing soil low-temperature denitration catalyst and the preparation method thereof provided by the patent has a great application prospect.
Claims (6)
1. The manganese-containing soil low-temperature denitration catalyst is characterized by comprising the following steps of:
1) collecting manganese-containing soil at different positions in a manganese ore area, screening the collected manganese-containing soil, and drying a sample with a certain particle size range to obtain a manganese-containing soil carrier;
2) taking inorganic salt of rare earth element cerium as an active component;
taking the manganese-containing soil obtained in the step 1) as a carrier, weighing the active component according to the manganese content in the carrier, and dissolving the weighed active component in water to obtain a precursor solution;
3) dipping the manganese-containing soil obtained in the step 1) into the precursor solution obtained in the step 2);
4) calcining the product obtained in the step 3) in an air atmosphere, and cooling to obtain the manganese-containing soil low-temperature denitration catalyst.
2. The manganese-containing soil low-temperature denitration catalyst and the preparation method thereof as claimed in claim 1, wherein the manganese ore region is located in the lukexi town of Xiushan county, Chongqing, the manganese-containing soil is the polluted waste of the manganese ore region, the particle size range is 20-100 meshes, the drying temperature is 90-110 ℃, the drying time is 6-10 h, and the manganese-containing soil low-temperature denitration catalyst takes manganese-containing soil as a carrier.
3. The manganese-containing soil low-temperature denitration catalyst and the preparation method thereof as claimed in claim 1 or 2, characterized in that the inorganic salt of rare earth element cerium is cerium nitrate, the active component is weighed according to the manganese content in the carrier, and the molar mass ratio of manganese to cerium is Mn: Ce ═ 1: 1. 1.5: 1. 2: 1.
4. the manganese-containing soil low-temperature denitration catalyst and the manganese-containing soil low-temperature denitration catalyst according to claim 3The preparation method is characterized in that the manganese-containing soil comprises the following main components in percentage by mass: SiO 22 55-60％、MnO 5-10％、Al2O3 15-20％、FeO 5-10％、CaO 1-5％、K2O 1-5％、P≤1％、Na≤1％。
5. The manganese-containing soil low-temperature denitration catalyst and the preparation method thereof according to claim 1 or 3, characterized in that after dipping the manganese-containing soil into the precursor solution, the precursor solution is subjected to ultrasonic treatment, is subjected to standing, is subjected to water bath evaporation to dryness, and is finally subjected to drying treatment;
the ultrasonic frequency is 40KHz, and the ultrasonic time range is 30-60 min;
the water bath time is 1-3 h, and the water bath temperature is 40-60 ℃;
the drying temperature is 90-110 ℃, and the drying time is 6-10 h.
6. The manganese-containing soil low-temperature denitration catalyst and the preparation method thereof according to claim 1, wherein in the step 4), the product is calcined in an air atmosphere:
in the calcining treatment process, the temperature of the muffle furnace is increased to 300-500 ℃ from room temperature at the heating rate of 5-10 ℃/min, and the muffle furnace is naturally cooled to room temperature after being calcined for 2-4 h.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113134355A (en) * | 2021-04-29 | 2021-07-20 | 国网山东省电力公司电力科学研究院 | Cobalt ion contaminated soil-based catalyst and preparation method and application thereof |
| CN115501748A (en) * | 2021-08-31 | 2022-12-23 | 嘉兴沃特泰科环保科技股份有限公司 | Denitration agent and preparation method thereof |
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| CN113134355A (en) * | 2021-04-29 | 2021-07-20 | 国网山东省电力公司电力科学研究院 | Cobalt ion contaminated soil-based catalyst and preparation method and application thereof |
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| CN115501748A (en) * | 2021-08-31 | 2022-12-23 | 嘉兴沃特泰科环保科技股份有限公司 | Denitration agent and preparation method thereof |
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