CN110586616A - Efficient inhibition method for dioxin regeneration in fly ash high-temperature thermal treatment process - Google Patents
Efficient inhibition method for dioxin regeneration in fly ash high-temperature thermal treatment process Download PDFInfo
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- 238000007669 thermal treatment Methods 0.000 title claims abstract description 32
- 238000000034 method Methods 0.000 title claims abstract description 29
- 230000008929 regeneration Effects 0.000 title claims abstract description 22
- 238000011069 regeneration method Methods 0.000 title claims abstract description 22
- HGUFODBRKLSHSI-UHFFFAOYSA-N 2,3,7,8-tetrachloro-dibenzo-p-dioxin Chemical compound O1C2=CC(Cl)=C(Cl)C=C2OC2=C1C=C(Cl)C(Cl)=C2 HGUFODBRKLSHSI-UHFFFAOYSA-N 0.000 title claims abstract 5
- 230000005764 inhibitory process Effects 0.000 title abstract description 6
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- KVGZZAHHUNAVKZ-UHFFFAOYSA-N 1,4-Dioxin Chemical compound O1C=COC=C1 KVGZZAHHUNAVKZ-UHFFFAOYSA-N 0.000 description 49
- 239000007789 gas Substances 0.000 description 14
- 239000010813 municipal solid waste Substances 0.000 description 11
- 230000009467 reduction Effects 0.000 description 10
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- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical group O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 2
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- 229910052801 chlorine Inorganic materials 0.000 description 2
- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
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- 229920000742 Cotton Polymers 0.000 description 1
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- 150000001336 alkenes Chemical class 0.000 description 1
- CSDREXVUYHZDNP-UHFFFAOYSA-N alumanylidynesilicon Chemical compound [Al].[Si] CSDREXVUYHZDNP-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
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- 235000012215 calcium aluminium silicate Nutrition 0.000 description 1
- WNCYAPRTYDMSFP-UHFFFAOYSA-N calcium aluminosilicate Chemical compound [Al+3].[Al+3].[Ca+2].[O-][Si]([O-])=O.[O-][Si]([O-])=O.[O-][Si]([O-])=O.[O-][Si]([O-])=O WNCYAPRTYDMSFP-UHFFFAOYSA-N 0.000 description 1
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- 229940043430 calcium compound Drugs 0.000 description 1
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- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 229910052742 iron Inorganic materials 0.000 description 1
- JEIPFZHSYJVQDO-UHFFFAOYSA-N iron(III) oxide Inorganic materials O=[Fe]O[Fe]=O JEIPFZHSYJVQDO-UHFFFAOYSA-N 0.000 description 1
- 229910052976 metal sulfide Inorganic materials 0.000 description 1
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- 230000004048 modification Effects 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- 235000021317 phosphate Nutrition 0.000 description 1
- 150000003013 phosphoric acid derivatives Chemical class 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000002952 polymeric resin Substances 0.000 description 1
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- 238000010248 power generation Methods 0.000 description 1
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- 239000010703 silicon Substances 0.000 description 1
- 239000000377 silicon dioxide Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
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Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B09—DISPOSAL OF SOLID WASTE; RECLAMATION OF CONTAMINATED SOIL
- B09B—DISPOSAL OF SOLID WASTE NOT OTHERWISE PROVIDED FOR
- B09B3/00—Destroying solid waste or transforming solid waste into something useful or harmless
- B09B3/40—Destroying solid waste or transforming solid waste into something useful or harmless involving thermal treatment, e.g. evaporation
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- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Processing Of Solid Wastes (AREA)
Abstract
The invention relates to an incineration treatment technology of municipal domestic waste, in particular to a high-efficiency inhibition method for dioxin regeneration in a high-temperature thermal treatment process of fly ash. Comprises the following steps: the method comprises the following steps: drying and grinding the sludge, and adding the sludge into the waste incineration fly ash; step two: stirring the fly ash and the sludge to realize the full and uniform mixing of the fly ash and the sludge; step three: then the mixture of the fly ash and the sludge is subjected to high-temperature thermal treatment in heating equipment, and the treatment time, namely the final temperature retention time is 10 min-6 h; step four: after the mixture of the fly ash and the sludge is subjected to high-temperature heat treatment, the obtained residue is collected after being cooled. The method can effectively inhibit the regeneration of the dioxin in the tail gas and obviously improve the degradation efficiency of the dioxin in the fly ash.
Description
Technical Field
The invention relates to an incineration treatment technology of municipal solid waste, in particular to a technology for efficiently inhibiting dioxin regeneration in a high-temperature thermal treatment process of incineration fly ash of municipal solid waste, which is a fly ash dioxin detoxification technology with low cost and high efficiency.
Background
In recent years, the urban domestic garbage incineration power generation technology in China is rapidly developed, the garbage incineration amount is increased year by year, 2011 + 2017, 5 years, the annual treatment amount of the garbage incineration in China is remarkably increased from 2599 ten thousand tons/year to 8463 ten thousand tons/year, and is more than three times. Fly ash generated by waste incineration is definitely classified as dangerous waste by most countries including China because of being rich in dioxin, heavy metals and chlorine salt, and the harmless treatment and resource utilization of the fly ash are always difficult in industry. In 2017, the fly ash yield of China is about 500 million tons, however, compared with smoke, the fly ash has less attention, only about 10-20% of fly ash in China is reasonably treated at present, and more than 50% of fly ash treated in a landfill site does not meet the leaching standard of China. Therefore, exploring and developing a novel fly ash harmless disposal technology and a resource utilization mode are very important for eliminating the threat of a large amount of fly ash to the environment and promoting the development of the waste incineration industry.
At present, most developed countries in the world generally adopt a fly ash disposal strategy of landfill storage, while Japan mainly realizes the harmless and resource pretreatment of fly ash by a high-temperature melting vitrification method, and the fly ash disposal mode of China mainly comprises landfill after cement solidification and cement kiln cooperative disposal. Although the cement solidification can inhibit the leaching of heavy metals in the fly ash, the cement solidification cannot degrade dioxin in the fly ash, and the solidified fly ash has obvious capacity increase, is not beneficial to transportation and landfill, and does not have the condition of subsequent resource utilization. The cement kiln co-treatment is a main way for recycling the fly ash, but because the chlorine is strictly controlled by cement, the addition amount of the fly ash is very low, and therefore, the cement kiln can only realize the limited recycling of the fly ash.
The high-temperature thermal treatment (such as sintering, melting, vitrification and the like) of the household garbage incineration fly ash can realize the high-efficiency solidification of heavy metals, the high-efficiency degradation of dioxin and the preparation of environment-friendly stable materials. The glassy residue obtained after melting the fly ash is clearly specified as general solid waste in the european union waste catalogue, and has the condition of subsequent resource utilization. In addition, the relevant standard 'technical requirement for vitrified treatment products of solid wastes' in China is also applied, and is expected to formally take effect in the near future. Therefore, the high-temperature thermal treatment technology of the fly ash is a main method for overcoming the problem of fly ash treatment in China in the future. However, fly ash is rich in catalytic metals, organics, carbon and chlorine, which are easily migrated to the gas phase at high temperature, resulting in regeneration of dioxin at low temperature stage. To date, there is no effective solution to this problem, which severely hinders the development of high temperature thermal disposal techniques for fly ash and the elimination of dioxins in the environment.
Therefore, based on the above background, the present invention provides a method for efficiently suppressing the regeneration of dioxin during the high-temperature thermal treatment of fly ash.
Disclosure of Invention
The invention aims to solve the technical problem of overcoming the defects of the prior art and provides a high-efficiency inhibition method for dioxin regeneration in the high-temperature thermal treatment process of fly ash.
In order to solve the technical problem, the solution of the invention is as follows:
the method for efficiently inhibiting the regeneration of dioxin in the high-temperature thermal treatment process of the fly ash is provided, and comprises the following steps:
the method comprises the following steps: drying and grinding the sludge, and adding the sludge into the waste incineration fly ash;
step two: stirring the fly ash and the sludge to realize the full and uniform mixing of the fly ash and the sludge;
step three: then the mixture of the fly ash and the sludge is subjected to high-temperature thermal treatment in heating equipment, and the treatment time, namely the final temperature retention time is 10 min-6 h;
step four: after the mixture of the fly ash and the sludge is subjected to high-temperature heat treatment, the obtained residue is collected after being cooled.
As an improvement, in the first step, the water content of the domestic sludge is lower than 40%, and the particle size is 0.01 mu m-10 mm.
As an improvement, in the first step, the water content of the waste incineration fly ash is lower than 30%, and the particle size is 0.01-1000 microns.
As an improvement, in the first step, the mass of the sludge dry basis accounts for 5-85% of the total dry basis mass of the mixture.
As an improvement, in the second step, the fly ash and the sludge are fully stirred and are stirred by a ball mill or a stirrer.
As an improvement, the stirring time in the second step is 1-60 min.
As an improvement, the treatment atmosphere of the fly ash and sludge mixture in the third step is any one of the following: air, nitrogen or an atmosphere with an oxygen content of 70-99%; the heating equipment is any one of the following: an electric heating furnace, a microwave heating furnace, an incinerator, an electric heating rotary kiln or a plasma melting furnace; the high-temperature heat treatment temperature is 600-1600 ℃.
As an improvement, the cooling mode in the fourth step is any one of the following modes: slow furnace cooling, air quenching or water quenching.
As an improvement, the sludge is urban domestic sludge.
The high-temperature heat treatment amount of the fly ash and sludge mixture is 1 kg-50 t/h.
Description of the inventive principles:
in the high-temperature thermal treatment process of the municipal solid waste incineration fly ash, more than 95% of dioxin in the fly ash solid particles is degraded, the degradation path is mainly the decomposition of a dioxin molecular ring structure and is accompanied with dechlorination, and degradation products comprise chlorobenzene, chlorophenol, micromolecular olefin, carbon oxide and the like. However, a significant dioxin regeneration phenomenon occurs in the tail gas at a low temperature range (200 to 600 ℃), thereby significantly reducing the overall reduction efficiency of dioxin. The regeneration route of dioxin is mainly synthesized from the beginning, and the regeneration amount of dioxin is increased along with the increase of the processing temperature along with the chlorination reaction. The most critical factors influencing the regeneration of dioxin are catalytic metals such as Cu, Fe, Cr, Zn and the like in fly ash. In the thermal treatment process, carbon matrixes in the fly ash are decomposed, and dioxin is generated in a gas phase under the action of catalytic metal. The municipal domestic sludge contains high content of P, N, S and other elements, and the elements have obvious inhibition effect on the generation of dioxin. In the synergistic high-temperature thermal treatment process of the fly ash and the sludge, nitrogen-containing and sulfur-containing compounds in the sludge are decomposed to generate NH3And SO2And the like, which have an inhibitory effect on the generation of dioxins. In addition, the method can be used for producing a composite materialS, P and N in the sludge can react with catalytic metals in the thermal treatment process to generate compounds with stable forms, such as metal sulfides, sulfates, phosphates, metal nitride compounds and the like, so that the catalytic metals for promoting the synthesis of dioxin are passivated, and the regeneration of the dioxin is effectively inhibited. The fly ash contains high content of calcium compound, and the inorganic component of the sludge is SiO2、Al2O3And Fe2O3Mainly, the fly ash is similar to the main components of clay, and is matched with the sludge with high silicon-aluminum content for use, so that the solid-waste synergistic complementation can be realized, the property of the prepared building material is further improved, and the resource quality of the fly ash is obviously improved.
Compared with the prior art, the invention has the following advantages:
(1) according to the invention, by the cooperative high-temperature thermal treatment of the municipal solid waste incineration fly ash and the municipal domestic sludge, the regeneration of dioxin in tail gas can be effectively inhibited, and the degradation efficiency of the dioxin in the fly ash is remarkably improved;
(2) the sludge and the fly ash are treated cooperatively, the treatment problem of the fly ash and the sludge is solved, and the heat generated by burning the sludge in the thermal treatment process reduces the energy consumption of the thermal treatment of the fly ash;
(3) the sludge contains high-content elements such as silicon and aluminum, and the like, and the elements can react with high-content calcium in the fly ash in the high-temperature thermal treatment process of the fly ash to generate minerals such as calcium aluminosilicate and the like, so that the resource quality of thermal treatment residues can be obviously improved;
(4) the method provided by the invention has the advantages of low cost and environment-friendly process, and realizes the synergistic complementation by matching different solid wastes, thereby reducing the emission of pollutants such as dioxin and the like and improving the resource quality of the product.
Detailed Description
A method for efficiently inhibiting the regeneration of dioxin in the high-temperature thermal treatment process of fly ash comprises the following steps:
the method comprises the following steps: directly adding the sludge into the waste incineration fly ash;
step two: stirring the fly ash and the sludge to realize the full and uniform mixing of the fly ash and the sludge;
step three: then the mixture of the fly ash and the sludge is subjected to high-temperature thermal treatment in heating equipment, namely the final temperature retention time is 10 min-6 h;
step four: after the mixture of the fly ash and the sludge is subjected to high-temperature heat treatment, the obtained residue is collected after being cooled.
In the first step, the water content of the domestic sludge is lower than 40%, and the particle size is 0.01 mu m-10 mm. The water content of the waste incineration fly ash is lower than 30%, and the particle size is 0.01-1000 mu m. The proportion of the dry basis weight of the sludge to the total dry basis weight of the mixture is 5-85%.
And in the second step, the fly ash and the sludge are fully stirred and are stirred by a ball mill or a stirrer. And in the second step, the stirring time is 1-60 min.
In the third step, the treatment atmosphere of the fly ash and sludge mixture is any one of the following: air, nitrogen or an atmosphere with an oxygen content of 70-99%; the heating equipment is any one of the following: an electric heating furnace, a microwave heating furnace, an incinerator, an electric heating rotary kiln or a plasma melting furnace; the high-temperature heat treatment temperature is 600-1600 ℃.
The cooling mode in the fourth step is any one of the following modes: slow furnace cooling, air quenching or water quenching.
Example (b): taking municipal solid waste incineration fly ash (with the water content of 3 percent and the average grain diameter of 50 mu m) in a bag-type dust collector of a circulating fluidized bed municipal solid waste incineration power plant for later use; municipal sludge from a municipal sewage treatment plant was taken, dried in an oven under an air atmosphere at 105 ℃ until the water content of the sludge was about 5%, and then ball-milled using a planetary ball mill until the average particle size was about 100. mu.m. Then, the fly ash and the sludge are ball-milled and mixed for 1min in a planetary ball mill according to the working conditions shown in the table 1, the mixed material is subjected to high-temperature heat treatment in a high-temperature tube furnace, the treatment temperatures are 600 ℃, 1100 ℃ and 1600 ℃, the heating rate is 20 ℃/min, the treatment times are 10min, 1h and 6h respectively, the air atmosphere is provided, and the air flow rate is 0.5L/min. In the high-temperature heat treatment process, dioxin in tail gas is absorbed by XAD-II type high polymer resin and toluene. Taking out the residue after heat treatment after cooling along with the tube furnace, and weighing the residue for countingCalculating the mass loss rate W of the sample after heat treatmentloss. And finally, extracting and purifying dioxin in the original fly ash, the original sludge, the thermal treatment residues, the resin and the toluene according to US EPA Method 1613 standard of the environmental protection agency, and detecting the content of the dioxin in the purified sample in a high-resolution gas chromatography-mass spectrometer. After detection, dioxin (resin + toluene) in the tail gas was normalized on the basis of the original sample mass (20g) in a unified manner. Degradation Rate (Eff) of Total Dioxin concentrationC) And toxicity equivalent concentration degradation rate (Eff)TEQ) The calculation is performed by equation (1):
in the formula, COriginalAnd CFixing deviceThe total dioxin concentration (pg/g) or toxicity equivalent concentration (pg I-TEQ/g), C, in the original sample and the residue after heat treatment, respectivelyQi (Qi)Is the normalized total dioxin concentration (pg/g) or toxicity equivalent concentration (pg I-TEQ/g) in the tail gas.
TABLE 1 fly ash and sludge synergistic high temperature thermal treatment regime
The results of dioxin reduction after the high-temperature heat treatment of fly ash and sludge are shown in table 2. The initial dioxin concentrations in the fly ash are 33010pg/g and 594pg I-TEQ/g respectively, and the dioxin concentrations in the sludge are obviously lower than those in the fly ash, namely 1078pg/g and 11pg I-TEQ/g. The fly ash is directly subjected to high-temperature thermal treatment under the condition of not adding sludge, dioxin in a solid phase is effectively degraded, however, a very obvious dioxin regeneration phenomenon appears in tail gas, the total amount of the dioxin in residue and the tail gas after treatment at the temperature of 600 ℃, 1100 ℃ and 1600 ℃ is 23801pg/g and 512pg I-TEQ/g (600 ℃), 131739pg/g and 2066pg I-TEQ/g (1100 ℃), 165134pg/g and 2732pg I-TEQ/g (1600 ℃), the total reduction rate of the dioxin at the temperature of 1100 ℃ and 1600 ℃ is negative, and the reduction rates of the total concentration and the toxicity equivalent concentration are-299 and-248%, and-400 and-360% respectively.
The regeneration phenomenon of dioxin in tail gas is remarkably inhibited by adding the sludge, and the reduction rates of the total concentration and the toxicity equivalent concentration of the dioxin are respectively 68% and 48%, 70% and 62%, 84 and 82%, 42% and 32% for 85%, 70%, 55% and 5% of the added amount of the sludge at 1100 ℃; under the conditions of 600 ℃ and 1600 ℃, the reduction rates of the total dioxin concentration and the toxicity equivalent concentration are respectively 87 percent, 84 percent and 81 percent for 30 percent of sludge addition. Compared with the working condition that no sludge is added, the dioxin reduction rate is remarkably improved. This shows that, in the high-temperature thermal treatment process of the fly ash, the addition of the sludge can significantly improve the overall reduction effect of dioxin by inhibiting the regeneration of dioxin in the tail gas.
TABLE 2 reduction of dioxins in cooperation with fly ash and sludge by high-temperature thermal treatment
aDioxin content in the solid sample before high-temperature thermal treatment;
bthe total amount of dioxin in the solid residue and tail gas after the high-temperature heat treatment.
It should be noted that, the sludge and the fly ash in this embodiment, and the other conditions are not changed, the experimental conditions are changed into that the fly ash and the sludge are stirred by a stirrer, the mixture of the fly ash and the sludge is disposed in the atmosphere of nitrogen or oxygen content of 70%, 80%, 99%, the high-temperature heat disposing equipment is an electric heating furnace, a microwave heating furnace, an incinerator, an electric heating rotary kiln or a plasma melting furnace, and the cooling mode is air quenching or water quenching, and the experimental results with the same rule can be obtained, so the present invention does not refer to the other embodiments.
Therefore, the method for efficiently inhibiting the regeneration of dioxin in the high-temperature thermal treatment process of the fly ash can realize the efficient inhibition of the regeneration phenomenon of the dioxin in tail gas in the high-temperature thermal treatment process of the fly ash generated by burning urban domestic garbage, thereby obviously improving the overall reduction efficiency of the dioxin and the harmless treatment effect of the fly ash, promoting the preparation of various building materials such as high-activity powder materials, heat-insulating cotton, ceramsite and the like, and being a fly ash treatment technology in the waste burning industry, which has a good commercial application prospect, low investment and operation cost and high efficiency.
Finally, it should be noted that the above-mentioned list is only a specific embodiment of the present invention. It is obvious that the present invention is not limited to the above embodiments, but many variations are possible. All modifications which can be derived or suggested by a person skilled in the art from the disclosure of the present invention are to be considered within the scope of the invention.
Claims (9)
1. A method for efficiently inhibiting the regeneration of dioxin in the high-temperature thermal treatment process of fly ash is characterized by comprising the following steps:
the method comprises the following steps: drying and grinding the sludge, and adding the sludge into the waste incineration fly ash;
step two: stirring the fly ash and the sludge to realize the full and uniform mixing of the fly ash and the sludge;
step three: then the mixture of the fly ash and the sludge is subjected to high-temperature thermal treatment in heating equipment, and the treatment time, namely the final temperature retention time is 10 min-6 h;
step four: after the mixture of the fly ash and the sludge is subjected to high-temperature heat treatment, the obtained residue is collected after being cooled.
2. The method according to claim 1, wherein the water content of the sludge in the first step is less than 40%, and the particle size is 0.01 μm to 10 mm.
3. The method according to claim 1, wherein the fly ash from waste incineration in the first step has a water content of less than 30% and a particle size of 0.01-1000 μm.
4. The method according to claim 1, wherein the proportion of the dry mass of the sludge in the first step to the total dry mass of the mixture is 5-85%.
5. The method according to claim 1, wherein the fly ash and the sludge in the second step are fully stirred by a ball mill or a stirrer.
6. The method according to claim 1, wherein the stirring time in the second step is 1-60 min.
7. The method according to claim 1, wherein the treatment atmosphere of the fly ash and sludge mixture in the third step is any one of the following: air, nitrogen or an atmosphere with an oxygen content of 70-99%; the heating equipment is any one of the following: an electric heating furnace, a microwave heating furnace, an incinerator, an electric heating rotary kiln or a plasma melting furnace; the high-temperature heat treatment temperature is 600-1600 ℃.
8. The method according to claim 1, wherein the cooling mode in the fourth step is any one of the following modes: slow furnace cooling, air quenching or water quenching.
9. The method of claim 1, wherein the sludge is municipal sludge.
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Application publication date: 20191220 |