CN111939866B - Method for efficiently treating household garbage leachate and preparing modified aluminum-iron-based adsorbent - Google Patents

Method for efficiently treating household garbage leachate and preparing modified aluminum-iron-based adsorbent Download PDF

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CN111939866B
CN111939866B CN202010925426.3A CN202010925426A CN111939866B CN 111939866 B CN111939866 B CN 111939866B CN 202010925426 A CN202010925426 A CN 202010925426A CN 111939866 B CN111939866 B CN 111939866B
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iron
aluminum
domestic garbage
garbage leachate
ferric chloride
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黄涛
宋东平
杜晶
金俊勋
刘龙飞
周璐璐
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Zhejiang Chuxiao Environmental Technology Co ltd
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Changshu Institute of Technology
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    • B01J20/02Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
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    • B01J20/28057Surface area, e.g. B.E.T specific surface area
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    • CCHEMISTRY; METALLURGY
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    • C02F2101/30Organic compounds
    • CCHEMISTRY; METALLURGY
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    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/06Contaminated groundwater or leachate

Abstract

The invention discloses a method for efficiently treating domestic garbage leachate and preparing a modified aluminum-iron-based adsorbent, which comprises the following steps: weighing aluminum ash and waste scrap iron, mixing and mechanically grinding to obtain activated aluminum-iron mixed powder; respectively weighing hydrochloric acid aqueous solution and activated aluminum iron mixed powder, and mixing and stirring to obtain iron chloride aluminum mixed slurry; respectively measuring domestic garbage leachate and aluminum ferric chloride mixed slurry, mixing and stirring, carrying out low-temperature plasma irradiation, and carrying out solid-liquid separation to respectively obtain a domestic garbage leachate purified solution and polyaluminum ferric chloride slurry; and drying the polyaluminum ferric chloride slurry, grinding to obtain polyaluminum ferric chloride powder, sintering the polyaluminum ferric chloride powder, and cooling to normal temperature to obtain the modified aluminum ferric-based adsorbent. The invention not only purifies the domestic garbage leachate, but also realizes the modification of the ferric aluminum oxide. The method can remove the highest 98 percent of COD, 99 percent of ammonia nitrogen, 99 percent of total phosphorus and 99 percent of lead in the landfill leachate, and the maximum specific surface area of the obtained iron aluminum oxide adsorbent can be 478m 2 /g。

Description

Method for efficiently treating household garbage leachate and preparing modified aluminum-iron-based adsorbent
Technical Field
The invention relates to the field of harmless treatment and recycling of hazardous wastes, in particular to a method for efficiently treating domestic garbage leachate and preparing a modified aluminum-iron-based adsorbent.
Background
The landfill leachate is a highly polluted liquid generated by rainwater leaching and scouring and microorganism anaerobic action in the process of landfill. Landfill leachate generated in landfill sites accounts for 15% -30% of the total amount of all sources. If the landfill leachate is discharged randomly without being reasonably treated, the soil, water (including surface water and underground water) and atmospheric environment around the discharge area are seriously polluted. The pollutant components in the landfill leachate are complex and have quite high concentration.
Generally, the landfill leachate mainly has the following characteristics: the pollutant has complex types, higher concentration, large change of water quantity and water quality, high ammonia nitrogen content, heavy metal pollutant existence and strong odor. If the landfill leachate is directly discharged into an urban sewage treatment system, the system load is seriously increased, and a large amount of non-degradable toxic pollutants are carried into the activated sludge, so that the activated sludge is inactivated and poisoned. The development of suitable landfill leachate disposal technology has become a hot topic in current environmental management. At present, the domestic and foreign treatment method of landfill leachate mainly comprises a filtration method, an evaporation method, a membrane separation method, a coagulating sedimentation method and an advanced oxidation method. However, the methods have the problems of overgrowth of the purification process, low purification efficiency of leachate, high yield of secondary solid-liquid dangerous waste, high difficulty in disposal of the secondary solid-liquid dangerous waste and the like.
Therefore, the research and development of the secondary waste which is simple in process, can realize the efficient purification of the landfill leachate and can realize the resource utilization of the landfill leachate in the treatment process is the key for solving the current treatment problem of the landfill leachate.
Disclosure of Invention
The purpose of the invention is as follows: the invention aims to solve the technical problem of providing a method for efficiently treating domestic garbage leachate and preparing a modified aluminum-iron-based adsorbent. The invention combines the treatment process of the domestic garbage percolate and the preparation process of the modified aluminum-iron adsorbent into a whole, thereby not only purifying the domestic garbage percolate, but also realizing the modification of the aluminum-iron oxide, and the specific surface area of the aluminum-iron oxide adsorbent prepared by the inventionCan be 478m at maximum 2 /g。
The invention also aims to solve the technical problem of providing a modified aluminum-iron-based adsorbent with high specific surface area.
The technical scheme is as follows: in order to solve the technical problems, the invention provides a method for efficiently treating domestic garbage leachate and preparing a modified aluminum-iron-based adsorbent, which comprises the following steps:
1) Respectively weighing aluminum ash and waste scrap iron, mixing, and mechanically grinding for 2-6 hours to obtain activated aluminum-iron mixed powder;
2) Respectively weighing hydrochloric acid aqueous solution and activated aluminum-iron mixed powder, mixing, and stirring for 6-24 hours to obtain aluminum-iron chloride mixed slurry;
3) Respectively measuring domestic garbage leachate and aluminum ferric chloride mixed slurry, mixing, stirring, carrying out low-temperature plasma irradiation for 3-12 hours, centrifuging, and carrying out solid-liquid separation to respectively obtain domestic garbage leachate purified liquid and polyaluminum ferric chloride slurry;
4) Drying and grinding the polyaluminum ferric chloride slurry at 50-150 ℃ to obtain polyaluminum ferric chloride powder, sintering the polyaluminum ferric chloride powder for 3-9 hours, and cooling to normal temperature to obtain the modified aluminum ferric absorbent.
Wherein the mass ratio of the aluminum ash to the scrap iron in the step 1) is 2-4: 1.
Wherein the concentration of the hydrochloric acid aqueous solution in the step 2) is 2-6M.
Wherein, the liquid-solid ratio of the hydrochloric acid aqueous solution to the activated aluminum-iron mixed powder in the step 2) is 10-30: 1mL/g.
Wherein the volume ratio of the domestic garbage percolate to the aluminum ferric chloride mixed slurry in the step 3) is 1-3: 1.
Wherein, the acting voltage of the low-temperature plasma in the step 3) is 10-50 kV, and the acting atmosphere of the low-temperature plasma is oxygen.
Wherein the sintering temperature in the step 4) is 300-600 ℃.
The invention also discloses the modified aluminum-iron-based adsorbent prepared by the method.
The reaction mechanism of the present invention: after mixing aluminium ash and scrap iron bits, because the particle size distribution difference, the aluminium ash collides and extrudees with scrap iron bits each other in grinding process, will produce stronger impact and shearing force each other to lead to the particle diameter to diminish, granule specific surface area grow. Mixing the hydrochloric acid aqueous solution with the activated aluminum-iron mixed powder, and gradually dissolving aluminum ash and waste iron filings into liquid along with the continuous consumption of hydrogen ions in the stirring process to generate aluminum ions and iron ions. After the domestic garbage leachate is mixed with aluminum ferric chloride, the introduced aluminum ions and iron ions in the mixed liquor can reduce the zeta potential of the colloid in the garbage leachate, and the colloid in the leachate is induced to form alum floc so as to realize settlement. During the low-temperature plasma irradiation process, oxygen in the atmosphere is dissociated and ionized in the discharge channel to generate oxygen radicals. The oxygen free radicals can convert part of ammonia nitrogen in the landfill leachate into nitrogen and nitrate, and can also realize the decomposition and mineralization of part of organic pollutants in the landfill leachate through oxidation. The oxygen free radicals can also combine with hydrogen ions to form hydrogen peroxide. The oxygen radicals may also oxidize chloride ions to chlorine gas and hypochlorous acid. Hydrogen peroxide, chlorine and hypochlorous acid can further enhance the decomposition of organic pollutants. Meanwhile, the oxygen free radicals can induce the aluminum and the iron in the aluminum chloride-iron mixed slurry to generate a hydrolytic polymerization reaction to generate a polymeric aluminum-iron coagulant. The polymeric aluminum-iron coagulant can further adsorb pollutants in the landfill leachate through the adsorption bridging action and the net capturing action, so that the purification of the landfill leachate is realized. During the sintering process, the polyaluminum ferric chloride powder is oxidized and decomposed to generate aluminum ferric oxide powder. Meanwhile, organic matters adsorbed in the polyaluminium chloride iron powder are subjected to oxidative decomposition in a high-temperature environment to generate carbon dioxide gas. Carbon dioxide gas is rapidly released from the iron aluminum oxide powder, thereby further increasing the specific surface area of the iron aluminum oxide powder. Elements such as phosphorus, nitrogen, heavy metals and the like adsorbed on the polyaluminium chloride iron powder are quickly oxidized and fused into the alumina iron powder in the oxidative decomposition process of the polyaluminium chloride iron powder, so that the surface modification of the alumina iron is realized, and the surface adsorption active sites of the alumina iron are increased.
Has the advantages that: compared with the prior art, the invention has the following remarkable advantages:
(1) The invention disposes the domestic garbage percolateThe process is combined with the preparation process of the modified aluminum-iron adsorbent, so that the domestic garbage leachate is purified, and the modification of the aluminum-iron oxide is realized. The method can remove the highest 98 percent of COD, 99 percent of ammonia nitrogen, 99 percent of total phosphorus and 99 percent of lead in the landfill leachate, and the maximum specific surface area of the obtained iron aluminum oxide adsorbent can be 478m 2 The removal rate of heavy metal contaminants by iron alumina adsorbents is much higher than commercial alumina and iron oxide.
(2) The method has the advantages of simple treatment and preparation process, easy realization of the treatment and preparation process and wide source of the required raw materials.
Drawings
FIG. 1 is a flow chart of the present invention;
FIG. 2 is a view of a low-temperature plasma processing apparatus.
Detailed Description
The invention is further described below with reference to the figures and examples.
It should be noted that the landfill leachate of the invention is taken from the sanitary landfill of the domestic garbage of Qinglongshan mountain in the continuous Yunyong city. The mass concentration of COD in the landfill leachate is 1456mg/L, the concentration of ammonia nitrogen is 945mg/L, the total phosphorus is 198mg/L, and lead ions (Pb) are contained 2+ )14mg/L。
Aluminum ash was obtained from Heng-Johntong high temperature furnace, north, jiang, of Steheny, and mainly contained 24.43% Al, 60.34% Al 2 O 3 、6.51%SiO 2 、3.36%Na 2 O、2.32%MgO、1.68%CaO、1.36%MnO。
Scrap iron obtained from Honda scrap Metal recovery, guangzhou, inc., mainly comprises 43.34% Fe, 36.38% Fe 2 O 3 、4.28%SiO 2 、3.64%P2O5、2.36%CaO。
Example 1 influence of the ratio of the mass of aluminum ash to the mass of scrap iron on the specific surface area of landfill leachate purification and modified ferro-aluminum adsorbent
Respectively weighing the aluminum ash and the waste scrap iron according to the mass ratio of the aluminum ash to the waste scrap iron of 1: 1, 1.5: 1, 1.8: 1, 2: 1, 3:1, 4:1, 4.5: 1, 5: 1 and 6: 1, mixing, and mechanically grinding for 2 hours to obtain nine groups of activated aluminum iron mixed powder. Mixing water and hydrochloric acid, and stirring uniformly to prepare a hydrochloric acid aqueous solution, wherein the concentration of the hydrochloric acid aqueous solution is 2M. Respectively weighing the hydrochloric acid aqueous solution and the activated aluminum-iron mixed powder according to the liquid-solid ratio of the hydrochloric acid aqueous solution to the activated aluminum-iron mixed powder of 10: 1mL/g, mixing, and stirring for 6 hours to obtain nine groups of aluminum-iron chloride mixed slurry. Respectively measuring domestic garbage leachate and aluminum ferric chloride mixed slurry according to the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry of 1: 1, mixing, stirring, carrying out low-temperature plasma irradiation for 3 hours, centrifuging, and carrying out solid-liquid separation to respectively obtain nine groups of domestic garbage leachate purified liquids and nine groups of polyaluminum ferric chloride slurries, wherein the low-temperature plasma action voltage is 10kV, and the low-temperature plasma action atmosphere is oxygen. And drying and grinding the nine groups of polyaluminium chloride iron slurry at 50 ℃ to obtain nine groups of polyaluminium chloride iron powder. And sintering the nine groups of polyaluminium chloride iron powder for 3 hours, and cooling to normal temperature to obtain nine groups of modified aluminum iron adsorbents, wherein the sintering temperature is 300 ℃.
COD concentration detection and COD removal rate calculation: the concentration of Chemical Oxygen Demand (COD) in the landfill leachate is measured according to the national standard bichromate method for measuring water quality chemical oxygen demand (GB 11914-1989); the COD removal rate is calculated according to the formula (1), wherein R COD As the removal rate of COD, c Q And c t The COD concentration (mg/L) of the landfill leachate before and after treatment are respectively shown.
Figure BDA0002666587100000041
Detecting the ammonia nitrogen concentration and calculating the ammonia nitrogen removal rate: the concentration of ammonia nitrogen in the landfill leachate is measured according to salicylic acid spectrophotometry for measuring ammonia nitrogen in water (HJ 536-2009); the ammonia nitrogen removal rate is calculated according to the formula (2), wherein R N For ammonia nitrogen removal, c N0 The initial concentration (mg/L) of ammonia nitrogen in the landfill leachate before treatment, c Nt The residual ammonia nitrogen concentration (mg/L) in the treated landfill leachate is adopted.
Figure BDA0002666587100000042
And (3) detecting the concentration of total phosphorus and calculating the removal rate of the total phosphorus: the concentration of total phosphorus in the landfill leachate is measured according to the determination of total phosphorus in water quality (GB 1893-89); the total phosphorus removal was calculated according to formula (3), where R p As a total phosphorus removal rate, c p0 Is the initial concentration (mg/L), c, of total phosphorus in the landfill leachate before treatment pt The residual concentration (mg/L) of the total phosphorus in the landfill leachate after treatment is adopted.
Figure BDA0002666587100000043
Detecting the concentration of lead ions and calculating the removal rate: the lead ion concentration in the landfill leachate is measured according to inductively coupled plasma emission spectrometry (HJ 776-2015) for measuring 32 elements in water quality. The lead ion removal rate was calculated according to the formula (4) wherein R pb Is the lead ion removal rate, c Pb0 Is the initial concentration (mg/L) of lead ions in the landfill leachate before treatment, c Pbt The lead ion concentration (mg/L) in the treated landfill leachate is obtained.
Figure BDA0002666587100000044
Specific surface detection of the modified aluminum-iron adsorbent: the specific surface area of the modified ferroaluminum adsorbent is detected by a specific surface area and pore size measuring instrument (Jing Gao, model: JW-BK 300C), and a calculation model is a BET specific surface area (single point).
The removal rate of COD, ammonia nitrogen, total phosphorus and lead ions in the landfill leachate and the specific surface area result of the adsorbent are shown in the table 1.
TABLE 1 influence of the ratio of the mass of aluminum ash to the mass of scrap iron on the specific surface area of the modified ferro-aluminum adsorbent for purifying landfill leachate
Figure BDA0002666587100000051
As can be seen from Table 1, when the mass ratio of the aluminum ash to the scrap iron pieces is less than 2: 1 (as in Table 1, the mass ratio of the aluminum ash to the scrap iron pieces = 1.8: 1,Lower values not listed in table 1 and 1: 1, 1: 1), less aluminum ash, poor grinding effect after mixing the aluminum ash and the waste scrap iron, reduction of aluminum ions and iron ions dissolved in dilute hydrochloric acid, poor zeta potential reduction effect of colloid in leachate, reduction of generation amount of polymeric aluminum-iron coagulant, reduction of pollutants adsorbed on the coagulant, and significant reduction of removal rate of COD, ammonia nitrogen, total phosphorus and lead in landfill leachate and specific surface area of modified aluminum-iron adsorbent along with reduction of mass ratio of the aluminum ash to the waste scrap iron. When the mass ratio of the aluminum ash to the waste iron filings is equal to 2-4: 1 (as shown in table 1, the mass ratio of the aluminum ash to the waste iron filings is = 2: 1, 3:1, 4: 1), after the aluminum ash and the waste iron filings are mixed, due to the difference of particle size distribution, the aluminum ash and the waste iron filings collide and extrude with each other in the grinding process, so that strong collision force and shearing force are generated, the particle size is reduced, and the specific surface area of the particles is increased. Mixing the hydrochloric acid aqueous solution with the activated aluminum-iron mixed powder, and gradually dissolving aluminum ash and waste iron filings into liquid along with the continuous consumption of hydrogen ions in the stirring process to generate aluminum ions and iron ions. After the domestic garbage leachate is mixed with aluminum ferric chloride, the introduced aluminum ions and iron ions in the mixed liquor can reduce the zeta potential of the colloid in the garbage leachate, and the colloid in the leachate is induced to form alum floc so as to realize settlement. The oxygen free radicals can induce the aluminum and the iron in the aluminum chloride-iron mixed slurry to generate hydrolysis polymerization reaction to generate a polymeric aluminum-iron coagulant. The polymeric aluminum-iron coagulant can further adsorb pollutants in the landfill leachate through the adsorption bridging action and the net capturing action, so that the purification of the landfill leachate is realized. Organic matters adsorbed in the polyaluminium chloride iron powder are oxidized and decomposed under a high-temperature environment to generate carbon dioxide gas. Carbon dioxide gas is rapidly released from the iron aluminum oxide powder, thereby further increasing the specific surface area of the iron aluminum oxide powder. The COD removal rate of the final landfill leachate is more than 86 percent, the ammonia nitrogen removal rate is more than 88 percent, the phosphorus removal rate is more than 90 percent, the lead removal rate is more than 85 percent, and the specific surface area of the modified aluminum-iron adsorbent is more than 424m 2 /g。
When the mass ratio of the aluminum ash to the waste iron filings is greater than 4:1 (as shown in table 1, when the mass ratio of the aluminum ash to the waste iron filings is = 4.5: 1, 5: 1, 6: 1 and higher values not listed in table 1), too much aluminum ash is generated, the grinding effect of the mixed aluminum ash and the waste iron filings is poor, aluminum ions and iron ions dissolved in dilute hydrochloric acid are reduced, the zeta potential reduction effect of colloid in leachate is poor, the generation amount of the polyaluminum-iron coagulant is reduced, and pollutants adsorbed on the coagulant are reduced, so that the removal rate of COD, ammonia nitrogen, total phosphorus and lead in the garbage leachate and the specific surface area of the modified aluminum-iron adsorbent are remarkably reduced along with the further increase of the mass ratio of the aluminum ash to the waste iron filings. Therefore, in summary, the benefit and the cost are combined, when the mass ratio of the aluminum ash to the scrap iron is equal to 2-4: 1, the purification effect of the landfill leachate is most favorably improved, and the specific surface area of the modified aluminum-iron adsorbent is most favorably improved.
Example 2 volume ratio of domestic garbage leachate and aluminum ferric chloride mixed slurry to garbage leachate purification and specific surface influence of modified aluminum ferric adsorbent
And weighing the aluminum ash and the waste scrap iron according to the mass ratio of the aluminum ash to the waste scrap iron of 4:1, mixing, and mechanically grinding for 4 hours to obtain the activated aluminum-iron mixed powder. Mixing water and hydrochloric acid, and stirring uniformly to prepare a hydrochloric acid aqueous solution, wherein the concentration of the hydrochloric acid aqueous solution is 4M. Respectively weighing the hydrochloric acid aqueous solution and the activated aluminum-iron mixed powder according to the liquid-solid ratio of the hydrochloric acid aqueous solution to the activated aluminum-iron mixed powder of 20: 1mL/g, mixing, and stirring for 15 hours to obtain aluminum-iron chloride mixed slurry. According to the volume ratio of 0.5: 1, 0.7: 1, 0.9: 1, 1: 1, 2: 1, 3:1, 3.2: 1, 3.5: 1 and 4:1 of the mixed slurry of the domestic garbage percolate and the ferric aluminum chloride, respectively measuring the mixed slurry of the domestic garbage percolate and the ferric aluminum chloride, mixing, stirring, carrying out low-temperature plasma irradiation for 7.5 hours, centrifuging, and carrying out solid-liquid separation to respectively obtain nine groups of domestic garbage percolate purifying solutions and nine groups of polymerized ferric aluminum chloride slurries, wherein the low-temperature plasma action voltage is 30kV, and the low-temperature plasma action atmosphere is oxygen. And drying and grinding the nine groups of polyaluminium chloride iron slurry at the temperature of 100 ℃ to obtain nine groups of polyaluminium chloride iron powder. And sintering the nine groups of polyaluminum ferric chloride powders for 6 hours, and cooling to normal temperature to obtain nine groups of modified aluminum ferric adsorbents, wherein the sintering temperature is 450 ℃. The COD concentration detection and the calculation of the COD removal rate, the ammonia nitrogen concentration detection and the calculation of the ammonia nitrogen removal rate, the total phosphorus concentration detection and the calculation of the total phosphorus removal rate, the lead ion concentration detection and the calculation of the removal rate and the specific surface detection of the modified aluminum-iron adsorbent are the same as those in the embodiment 1.
The results of removing COD, ammonia nitrogen, total phosphorus and lead ions and the specific surface area of the adsorbent in the landfill leachate are shown in Table 2.
TABLE 2 influence of volume ratio of domestic garbage leachate and aluminum ferric chloride mixed slurry on garbage leachate purification and specific surface area of modified aluminum ferric adsorbent
Figure BDA0002666587100000071
As can be seen from table 2, when the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry is less than 1: 1 (as in table 2, when the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry = 0.9: 1, 0.7: 1, 0.5: 1, and lower values not listed in table 2), the domestic garbage leachate is less, the consumption of hydrogen ions in the aluminum ferric chloride mixed slurry after the domestic garbage leachate is mixed with the aluminum ferric chloride mixed slurry is less, the efficiency of the oxygen radical to induce the hydrolysis polymerization reaction of aluminum and iron is reduced, the generated polyaluminum ferric chloride is reduced, the pollutant adsorption is reduced, and the removal rate of COD, ammonia nitrogen, total phosphorus and lead in the garbage leachate and the specific surface of the modified aluminum ferric chloride adsorbent are all significantly reduced along with the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry. When the volume ratio of the household garbage leachate to the aluminum ferric chloride mixed slurry is equal to 1-3: 1 (as shown in table 2, when the volume ratio of the household garbage leachate to the aluminum ferric chloride mixed slurry is = 1: 1, 2: 1, 3: 1), after the household garbage leachate and the aluminum ferric chloride are mixed, aluminum ions and iron ions introduced into the mixed solution can reduce zeta potential of colloids in the garbage leachate, and the colloids in the leachate are induced to form alum flocs, so that sedimentation is realized. During the low-temperature plasma irradiation process, oxygen in the atmosphere is dissociated and ionized in the discharge channel to generate oxygen radicals. The oxygen free radicals can induce the aluminum and the iron in the aluminum chloride-iron mixed slurry to generate hydrolysis polymerization reaction to generate a polymeric aluminum-iron coagulant. The polymeric aluminum iron coagulant can further adsorb pollutants in the landfill leachate through the adsorption bridging action and the net capturing action, so that the purification of the landfill leachate is realized. During the sintering process, the polyaluminium chloride iron powderOxidative decomposition occurs to produce iron aluminum oxide powder. Meanwhile, organic matters adsorbed in the polyaluminium chloride iron powder are subjected to oxidative decomposition in a high-temperature environment to generate carbon dioxide gas. Carbon dioxide gas is rapidly released from the iron aluminum oxide powder, thereby further increasing the specific surface area of the iron aluminum oxide powder. Elements such as phosphorus, nitrogen, heavy metals and the like adsorbed on the polyaluminium chloride iron powder are quickly oxidized and fused into the alumina iron powder in the oxidative decomposition process of the polyaluminium chloride iron powder, so that the surface modification of the alumina iron is realized, and the surface adsorption active sites of the alumina iron powder are increased. The COD removal rate of the final landfill leachate is more than 92 percent, the ammonia nitrogen removal rate is more than 92 percent, the phosphorus removal rate is more than 93 percent, the lead removal rate is more than 91 percent, and the specific surface area of the modified aluminum-iron adsorbent is more than 436m 2 (ii) in terms of/g. When the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry is greater than 3:1 (as shown in table 1, the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry is = 3.2: 1, 3.5: 1, and 4: 1), the domestic garbage leachate is too much, the zeta potential reduction effect of colloid in the leachate is poor, and the removal efficiency of pollutants in the domestic garbage leachate is poor, so that the removal rates of COD, ammonia nitrogen, total phosphorus, and lead in the landfill leachate are all remarkably reduced along with the further increase of the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry. Therefore, in summary, the benefit and the cost are combined, when the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry is equal to 1-3: 1, the purification effect of the landfill leachate is favorably improved, and the specific surface area of the modified aluminum ferric adsorbent is favorably improved.
Example 3 influence of Low-temperature plasma irradiation time on landfill leachate purification and specific surface area of modified ferroaluminum adsorbent
And weighing the aluminum ash and the waste scrap iron according to the mass ratio of the aluminum ash to the waste scrap iron of 4:1, mixing, and mechanically grinding for 6 hours to obtain the activated aluminum-iron mixed powder. Mixing water and hydrochloric acid, and stirring uniformly to prepare a hydrochloric acid aqueous solution, wherein the concentration of the hydrochloric acid aqueous solution is 6M. Respectively weighing the hydrochloric acid aqueous solution and the activated aluminum-iron mixed powder according to the liquid-solid ratio of the hydrochloric acid aqueous solution to the activated aluminum-iron mixed powder of 30:1mL/g, mixing, and stirring for 24 hours to obtain aluminum-iron chloride mixed slurry. Respectively measuring domestic garbage leachate and aluminum ferric chloride mixed slurry according to the volume ratio of 3:1 of the domestic garbage leachate and the aluminum ferric chloride mixed slurry, mixing, stirring, carrying out low-temperature plasma irradiation for 1.5, 2, 2.5, 3, 7.5, 12, 13, 14 and 15 hours, centrifuging, and carrying out solid-liquid separation to respectively obtain nine groups of domestic garbage leachate purification solutions and nine groups of polyaluminum ferric chloride slurries, wherein the low-temperature plasma action voltage is 50kV, and the low-temperature plasma action atmosphere is oxygen. And drying and grinding the nine groups of polyaluminum ferric chloride slurries at 150 ℃ to obtain nine groups of polyaluminum ferric chloride powders. And sintering the nine groups of polyaluminium chloride iron powder for 9 hours, and cooling to normal temperature to obtain nine groups of modified aluminum iron adsorbents, wherein the sintering temperature is 600 ℃.
The COD concentration detection and the calculation of the COD removal rate, the ammonia nitrogen concentration detection and the calculation of the ammonia nitrogen removal rate, the total phosphorus concentration detection and the calculation of the total phosphorus removal rate, the lead ion concentration detection and the calculation of the removal rate and the detection of the specific surface area of the modified aluminum-iron adsorbent are the same as those in the embodiment 1.
The results of removing COD, ammonia nitrogen, total phosphorus and lead ions and the specific surface area of the adsorbent in the landfill leachate are shown in Table 3.
TABLE 3 influence of low-temperature plasma irradiation time on landfill leachate purification and specific surface area of modified ferro-aluminum adsorbent
Figure BDA0002666587100000091
As can be seen from table 3, when the low-temperature plasma irradiation time is less than 3 hours (as in table 3, when the low-temperature plasma irradiation time =2.5, 2, 1.5 and lower values not listed in table 3), the low-temperature plasma irradiation time is too short, oxygen radicals, hydrogen peroxide, chlorine and hypochlorous acid generated during the low-temperature plasma irradiation process are reduced, the decomposition of organic pollutants in the landfill leachate is insufficient, and the aluminum and iron in the aluminum-iron chloride mixed slurry undergo hydrolytic polymerization, so that the removal rate of COD, ammonia nitrogen, total phosphorus and lead in the landfill leachate and the specific surface area of the modified aluminum-iron adsorbent are all significantly reduced as the low-temperature plasma irradiation time is reduced. When the low-temperature plasma irradiation time is equal to 3 to 12 hours (as in table 3, low-temperature plasma irradiation time =3, 7.5,12 hours), oxygen in the atmosphere is dissociated and ionized in a discharge channel during the low-temperature plasma irradiation process, and oxygen radicals are generated. The oxygen free radicals can convert part of ammonia nitrogen in the landfill leachate into nitrogen and nitrate, and can also realize the decomposition and mineralization of part of organic pollutants in the landfill leachate through oxidation. The oxygen free radicals can also combine with hydrogen ions to form hydrogen peroxide. The oxygen radicals may also oxidize chloride ions to chlorine gas and hypochlorous acid. The hydrogen peroxide, the chlorine and the hypochlorous acid can further strengthen the decomposition of the organic pollutants. Meanwhile, the oxygen free radicals can induce the aluminum and the iron in the aluminum chloride-iron mixed slurry to generate a hydrolytic polymerization reaction to generate a polymeric aluminum-iron coagulant. The COD removal rate of the final landfill leachate is more than 95 percent, the ammonia nitrogen removal rate is more than 94 percent, the phosphorus removal rate is more than 96 percent, the lead removal rate is more than 95 percent, and the specific surface area of the modified aluminum-iron adsorbent is more than 448m 2 (iv) g. When the low-temperature plasma irradiation time is longer than 12 hours (as in table 3, when the low-temperature plasma irradiation time =13, 14, 15 and higher values not listed in table 3), the removal rate of COD, ammonia nitrogen, total phosphorus and lead and the specific surface of the modified ferro-aluminum adsorbent in the landfill leachate do not change significantly with the further increase of the low-temperature plasma irradiation time. Therefore, in summary, combining the benefit and the cost, when the low-temperature plasma irradiation time is equal to 3-12 hours, the purification effect of the landfill leachate is most favorably improved, and the specific surface area of the modified aluminum-iron adsorbent is most favorably improved.
Different comparative processes of comparative example influence the specific surface area of landfill leachate purification and modified ferro-aluminum adsorbent
The process of the invention comprises the following steps: and weighing the aluminum ash and the waste scrap iron according to the mass ratio of the aluminum ash to the waste scrap iron of 4:1, mixing, and mechanically grinding for 6 hours to obtain the activated aluminum-iron mixed powder. Mixing water and hydrochloric acid, and stirring uniformly to prepare a hydrochloric acid aqueous solution, wherein the concentration of the hydrochloric acid aqueous solution is 6M. Respectively weighing the hydrochloric acid aqueous solution and the activated aluminum-iron mixed powder according to the liquid-solid ratio of the hydrochloric acid aqueous solution to the activated aluminum-iron mixed powder of 30:1mL/g, mixing, and stirring for 24 hours to obtain aluminum-iron chloride mixed slurry. Respectively measuring the domestic garbage leachate and the aluminum ferric chloride mixed slurry according to the volume ratio of 3:1 of the domestic garbage leachate to the aluminum ferric chloride mixed slurry, mixing, stirring, irradiating for 12 hours by using low-temperature plasma, centrifuging, and performing solid-liquid separation to respectively obtain a domestic garbage leachate purified solution and polyaluminum ferric chloride slurry, wherein the low-temperature plasma action voltage is 50kV, and the low-temperature plasma action atmosphere is oxygen. Drying the polyaluminium chloride iron slurry at 150 ℃, and grinding to obtain the polyaluminium chloride iron powder. Sintering the polyaluminum ferric chloride powder for 9 hours, and cooling to normal temperature to obtain the modified aluminum ferric adsorbent, wherein the sintering temperature is 600 ℃.
Comparative process 1: and weighing the aluminum ash and the waste scrap iron according to the mass ratio of the aluminum ash to the waste scrap iron of 4:1, mixing, and mechanically grinding for 6 hours to obtain the activated aluminum-iron mixed powder. Respectively weighing the water and the activated aluminum-iron mixed powder according to the liquid-solid ratio of the water to the activated aluminum-iron mixed powder of 30:1mL/g, mixing, and stirring for 24 hours to obtain iron-aluminum mixed slurry. Respectively measuring the domestic garbage leachate and the aluminum-iron mixed slurry according to the volume ratio of 3:1 of the domestic garbage leachate to the aluminum-iron mixed slurry, mixing, stirring, carrying out low-temperature plasma irradiation for 12 hours, centrifuging, and carrying out solid-liquid separation to respectively obtain a domestic garbage leachate purified liquid and polymerized aluminum-iron slurry, wherein the low-temperature plasma action voltage is 50kV, and the low-temperature plasma action atmosphere is oxygen. And drying the polymerized aluminum iron slurry at 150 ℃, and grinding to obtain the polymerized aluminum iron powder. And sintering the polymeric aluminum-iron powder for 9 hours, and cooling to normal temperature to obtain the comparative adsorbent 1, wherein the sintering temperature is 600 ℃.
Comparative process 2: and weighing the aluminum ash and the waste scrap iron according to the mass ratio of the aluminum ash to the waste scrap iron of 4:1, mixing, and mechanically grinding for 6 hours to obtain the activated aluminum-iron mixed powder. Mixing water and hydrochloric acid, and stirring uniformly to prepare a hydrochloric acid aqueous solution, wherein the concentration of the hydrochloric acid aqueous solution is 6M. Respectively weighing the hydrochloric acid aqueous solution and the activated aluminum-iron mixed powder according to the liquid-solid ratio of the hydrochloric acid aqueous solution to the activated aluminum-iron mixed powder of 30:1mL/g, mixing, and stirring for 24 hours to obtain iron-aluminum chloride mixed slurry. Respectively measuring the domestic garbage leachate and the aluminum ferric chloride mixed slurry according to the volume ratio of 3:1 of the domestic garbage leachate to the aluminum ferric chloride mixed slurry, mixing, stirring for 12 hours, centrifuging, and performing solid-liquid separation to respectively obtain the domestic garbage leachate purified liquid and the aluminum ferric chloride slag. Drying the aluminum ferric chloride slag at 150 ℃, and grinding to obtain aluminum ferric chloride slag powder. And sintering the aluminum chloride iron slag powder for 9 hours, and cooling to normal temperature to obtain the contrast adsorbent 2, wherein the sintering temperature is 600 ℃.
The COD concentration detection and the calculation of the COD removal rate, the ammonia nitrogen concentration detection and the calculation of the ammonia nitrogen removal rate, the total phosphorus concentration detection and the calculation of the total phosphorus removal rate, the lead ion concentration detection and the calculation of the removal rate and the detection of the specific surface area of the adsorbent are the same as those in the embodiment 1.
The results of removing COD, ammonia nitrogen, total phosphorus and lead ions and the specific surface area of the adsorbent in the landfill leachate are shown in Table 4.
TABLE 4 influence of different comparative processes on the landfill leachate purification and the specific surface area of the modified ferro-aluminum adsorbent
Figure BDA0002666587100000111
As can be seen from Table 4, the purification effect of landfill leachate and the specific surface area of the adsorbent which can be realized by the process of the invention are far higher than those of the comparative process 1 and the comparative process 2 and are both higher than the sum of the two.

Claims (8)

1. A method for efficiently treating domestic garbage leachate and preparing a modified aluminum-iron-based adsorbent is characterized by comprising the following steps:
1) Respectively weighing aluminum ash and waste scrap iron, mixing, and mechanically grinding for 2 to 6 hours to obtain activated aluminum-iron mixed powder;
2) Respectively weighing a hydrochloric acid aqueous solution and activated aluminum iron mixed powder, mixing, and stirring for 6 to 24 hours to obtain iron aluminum chloride mixed slurry;
3) Respectively measuring domestic garbage leachate and aluminum ferric chloride mixed slurry, mixing, stirring, carrying out low-temperature plasma irradiation for 3 to 12 hours, centrifuging, and carrying out solid-liquid separation to respectively obtain a domestic garbage leachate purified solution and polyaluminum ferric chloride slurry;
4) Drying and grinding the polyaluminum ferric chloride slurry at 50-150 ℃ to obtain polyaluminum ferric chloride powder, sintering the polyaluminum ferric chloride powder for 3-9 hours, and cooling to normal temperature to obtain the modified aluminum-iron-based adsorbent.
2. The method for efficiently disposing domestic garbage leachate and preparing the modified aluminum-iron-based adsorbent according to claim 1, wherein the mass ratio of aluminum ash to scrap iron in the step 1) is 2-4.
3. The method for efficiently disposing domestic garbage leachate and preparing a modified aluminum-iron-based adsorbent according to claim 1, wherein the concentration of the hydrochloric acid aqueous solution in the step 2) is 2-6M.
4. The method for efficiently disposing domestic garbage leachate and preparing the modified aluminum-iron-based adsorbent according to claim 1, wherein the liquid-solid ratio of the hydrochloric acid aqueous solution to the activated aluminum-iron mixed powder in step 2) is 10 to 30:1mL/g.
5. The method for efficiently disposing domestic garbage leachate and preparing a modified aluminum-iron-based adsorbent according to claim 1, wherein the volume ratio of the domestic garbage leachate to the aluminum ferric chloride mixed slurry in the step 3) is 1 to 3.
6. The method for efficiently disposing domestic garbage leachate and preparing the modified aluminum-iron-based adsorbent according to claim 1, wherein the low-temperature plasma action voltage in the step 3) is 10 to 50kV, and the low-temperature plasma action atmosphere is oxygen.
7. The method for efficiently disposing domestic garbage leachate and preparing the modified aluminum-iron-based adsorbent according to claim 1, wherein the sintering temperature in the step 4) is 300-600 ℃.
8. The modified aluminum-iron-based adsorbent prepared by the method of any one of claims 1 to 7.
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