CN111620431A - Application of adsorbed-desorbed waste biochar in degradation of persistent organic pollutants by activated persulfate - Google Patents
Application of adsorbed-desorbed waste biochar in degradation of persistent organic pollutants by activated persulfate Download PDFInfo
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- CN111620431A CN111620431A CN202010527056.8A CN202010527056A CN111620431A CN 111620431 A CN111620431 A CN 111620431A CN 202010527056 A CN202010527056 A CN 202010527056A CN 111620431 A CN111620431 A CN 111620431A
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
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- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
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- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/72—Copper
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- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/755—Nickel
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
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Abstract
The invention relates to application of adsorbed-desorbed waste biochar in activating persulfate to degrade persistent organic pollutants, which takes the adsorbed-desorbed waste biochar as a catalyst, adds the adsorbed-desorbed waste biochar into organic pollutant wastewater, and simultaneously adds persulfate to degrade and remove the persistent organic pollutants in the wastewater. The method not only enables the waste biochar to be better recycled and utilized, saves resources, but also has high chemical stability, low metal ion dissolution and higher persulfate activation capacity, changes waste into valuable, can be recycled, is used for treating the wastewater containing organic pollutants by using a heterogeneous persulfate oxidation technology, and has high organic matter removal rate.
Description
Technical Field
The invention relates to application of adsorbed-desorbed waste biochar in activating persulfate to degrade persistent organic pollutants, and belongs to the technical field of waste resource utilization and environment and chemistry.
Background
In recent years, with the industry of ChinaThe rapid development of the method, a large amount of organic pollutants which are difficult to degrade, such as medical compounds, pesticides, dyes and the like, are discharged into the environment through different ways, so that the water resource of China is influenced by different degrees, and the health of human bodies, animals and plants is directly threatened. Conventional physicochemical and biological techniques are not effective in removing these persistent organic contaminants and therefore require advanced treatment processes to achieve removal. Sulfate radical (SO) generated by advanced oxidation technology based on activated persulfate4 -) The advantages of high oxidation-reduction potential, simple generation, wide pH application and the like become a new technology for treating persistent organic pollutants.
The current persulfate activation methods comprise heat treatment, microwave treatment, transition metal ion catalytic activation and the like. The transition metal activation method is widely concerned due to mild reaction conditions and simple operation. But the introduced metal ions need to be further treated after the reaction is finished, so that the operation cost is increased, and the metal pollution risk in the effluent is increased. The heterogeneous persulfate activation technology realizes the separation of the catalyst and the active component, and avoids the introduction of free metal ions into the water body, so a great deal of research is focused on developing novel high-efficiency heterogeneous catalysts. The method for preparing the heterogeneous catalyst comprises a precipitation method, an impregnation method, a calcination method and the like, and the prepared catalyst can effectively activate persulfate, has complex preparation process and higher cost and wastes resources.
For a long time, the problem of heavy metal pollution of water in China is very prominent, and the method has important threats to the environment and the human health. The enrichment of heavy metals by adopting a solid adsorbent is one of important components and effective means for removing the heavy metals in water. The biochar has the characteristics of high efficiency, low cost, simplicity and convenience in operation, environmental friendliness and the like, is widely used, and is continuously and widely concerned by researchers. However, the regeneration and reuse of the adsorbed biochar is also called as a problem, and the adsorbent for adsorbing heavy metals is finally changed into solid waste, which is called as secondary pollution, and no better treatment method is available at present. After being absorbed into the biochar, the heavy metal has good chemical stability, is not easy to leach, cannot be effectively treated, can only be stacked, and seriously pollutes the environment.
Based on the problems facing today: the biochar adsorbing heavy metals cannot be effectively treated, so that the environment is seriously polluted; the preparation process of the persulfate activating catalyst is complex and high in cost, and a novel mode for activating persulfate is urgently needed to be developed and used for degrading persistent organic pollutants.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides the application of the waste biochar after adsorption-desorption in the degradation of persistent organic pollutants by activating persulfate.
The invention introduces the waste biochar which adsorbs heavy metal ions for multiple times and is desorbed into a persulfate system for activating sulfate to generate sulfate radical free radical (SO)4 -) The method has the advantages of degrading persistent organic pollutants, solving the problem that the biochar adsorbing heavy metals cannot be effectively treated, providing a new way for activating persulfate, being simple to operate and low in cost, effectively helping to solve environmental problems and realizing waste utilization.
The invention is realized by the following technical scheme:
the application of the adsorbed-desorbed waste biochar in the degradation of persistent organic pollutants by activated persulfate comprises the following steps:
adding the waste biochar subjected to adsorption-desorption into organic pollutant wastewater by using the waste biochar subjected to adsorption-desorption as a catalyst, simultaneously adding persulfate, uniformly mixing, reacting under a shaking condition that the temperature is 25-45 ℃ and the pH is 2.0-11.0, and degrading to remove persistent organic pollutants in the wastewater, wherein the mass-to-volume ratio of the catalyst to the organic pollutant wastewater is (1-5): (10-100), and the unit: g/L; the waste biochar after adsorption-desorption is biogas residue biochar after heavy metal ions are adsorbed-desorbed for multiple times.
According to the invention, the biogas residue biochar after multiple adsorption and desorption of heavy metal ions is preferably biochar obtained by adsorbing heavy metals in heavy metal wastewater by using the biogas residue biochar, then desorbing, adsorbing heavy metal ions in the heavy metal wastewater by using the desorbed biochar, then desorbing, repeatedly adsorbing and desorbing for 3-6 times, and drying.
According to the invention, in the preferable application of the activated persulfate to degrade the persistent organic pollutants, the biochar obtained by adsorbing heavy metals in the heavy metal wastewater by the biogas residue biochar for one time has almost the same effect as the biochar obtained by adsorbing and desorbing for 3-6 times for multiple times.
The desorption process is carried out according to the conventional techniques in the art, and the present invention preferably employs sodium hydroxide for desorption.
Preferably, according to the present invention, the heavy metal ions are copper and/or nickel ions.
According to the invention, the mass volume ratio of the catalyst to the organic pollutant wastewater is (1-3) to (3-30), and the unit is as follows: g/L.
Further preferably, the mass volume ratio of the catalyst to the organic pollutant wastewater is (1-3) to (8-20), and the unit is as follows: g/L, most preferably, the mass volume ratio of the catalyst to the organic pollutant wastewater is 1:10, unit: g/L.
According to the invention, the organic pollutant wastewater is preferably medical wastewater, dye wastewater or paper-making wastewater.
According to the invention, the particle size of the waste biochar after adsorption-desorption is 40-100 nm.
According to a preferred embodiment of the invention, the persulfate is potassium persulfate and/or oxone.
According to the invention, the persulfate is preferably added in an amount of 0.5 to 3 mmol/L.
Most preferably, the addition amount of the persulfate is 1 mmol/L.
According to the invention, the pH value of the organic pollutant wastewater is 6-9.
According to the invention, the preferred oscillation speed is 120-160 r/min, and the reaction time is 1-2 hours.
According to the invention, the biogas residue biochar is preferably prepared by the following method:
(1) washing the biogas residues with water, drying, grinding and sieving to obtain dry biogas residue powder;
(2) calcining and carbonizing the dry biogas residue powder to obtain biogas residue biochar.
According to the invention, the biogas residue in the step (1) is preferably biogas residue obtained by anaerobic fermentation of corn straw, wheat straw, rice straw or a mixture thereof at the fermentation temperature of 30-55 ℃ for 25-45 days.
According to the invention, in the step (1), the biogas residue is preferably washed by soaking in tap water for 24h, draining, and then washing with deionized water for 3 times, wherein the drying temperature is 60-80 ℃.
Preferably, in the step (2), the calcination and carbonization are to heat the dry biogas residue powder to 700 ℃ at a speed of 10 ℃/min in a nitrogen atmosphere, keep the temperature for 2h, then turn to room temperature, take out the dry biogas residue powder, soak the dry biogas residue powder in 1mol/L HCl for 12h, then wash the dry biogas residue powder to be neutral by deionized water, and finally dry the dry biogas residue powder at 70 ℃ to obtain the biogas residue charcoal.
The invention has the technical characteristics and advantages that:
1. the method for degrading persistent organic pollutants by activating persulfate by using biogas residue biochar after multiple adsorption-desorption of heavy metal ions as a catalyst for the first time realizes high-efficiency and high-value utilization of the waste biochar, provides a new idea for recycling the biochar after adsorption of heavy metal ions, avoids secondary pollution of the waste biochar after adsorption of heavy metal ions, finds a resource road for the waste biochar, relieves the pressure of solid waste treatment, and protects the environment. The method not only enables the waste biochar to be better recycled and utilized, saves resources, but also has high chemical stability, low metal ion dissolution and higher persulfate activation capacity, changes waste into valuable, can be recycled, is used for treating the wastewater containing organic pollutants by using a heterogeneous persulfate oxidation technology, and has high organic matter removal rate.
2. The biogas residue biochar after multiple adsorption-desorption of heavy metal ions is used as a catalyst and applied to the degradation of persistent organic pollutants by activating persulfate, the catalyst can be repeatedly utilized, and meanwhile, in the reaction of activating persulfate, the biogas residue biochar has higher degradation rate on different organic pollutants. The method provides a new technology for removing the organic pollutants which are difficult to degrade in the wastewater, provides a new idea for resource utilization of the waste biochar, realizes the repeated utilization of the catalyst, and has important significance for environmental protection.
3. The application method disclosed by the invention has the advantages of wide application range of pH, good treatment effect when the pH is 2.0-11.0, mild conditions, capability of being carried out at room temperature, small using amount, large treatment amount and large-scale popularization and application.
Drawings
FIG. 1 is a TEM image and a TEM-mapping image of the biogas residue biochar catalyst after 3 times of Cu ion adsorption-desorption, wherein the mass percentage of Cu ions in the catalyst is 3%;
FIG. 2 is a TEM image and a TEM-mapping image of the biogas residue biochar catalyst after 3 times of nickel ion adsorption-desorption, wherein the mass percentage of nickel ions in the catalyst is 3%;
fig. 3 is a graph showing the degradation effect of norfloxacin by activating persulfate through different biogas residue biochar catalysts, which is respectively as follows: after 3 times of Cu ion adsorption-desorption, the Cu ion mass percentage content is 3% and 6% of biogas residue biochar, and after 3 times of nickel ion adsorption-desorption, the nickel ion mass percentage content is 3% and 6% of biogas residue biochar;
fig. 4 is a graph showing the effect of adding different biogas residue biochar catalysts on the degradation and removal of organic pollutants, wherein a is biogas residue biochar with 3% of Cu ions by mass after 3 times of Cu ion adsorption-desorption, b is biogas residue biochar with 6% of Cu ions by mass after 3 times of Cu ion adsorption-desorption, c is biogas residue biochar with 3% of nickel ions by mass after 3 times of nickel ion adsorption-desorption, and d is biogas residue biochar with 6% of nickel ions by mass after 3 times of nickel ion adsorption-desorption;
FIG. 5 is a graph showing the effect of removing organic pollutants by degrading a pH biogas residue biochar catalyst; a is biogas residue biochar with the Cu ion mass percentage of 3% after 3 times of Cu ion adsorption-desorption, b is biogas residue biochar with the Cu ion mass percentage of 6% after 3 times of Cu ion adsorption-desorption, c is biogas residue biochar with the nickel ion mass percentage of 3% after 3 times of nickel ion adsorption-desorption, and d is biogas residue biochar with the nickel ion mass percentage of 6% after 3 times of nickel ion adsorption-desorption;
fig. 6 is a metal dissolution diagram of different biogas residue biochar catalysts in the process of activating persulfate to degrade norfloxacin, wherein a is biogas residue biochar with the mass percentage of 3% and 6% of Cu ions after 3 times of adsorption-desorption of Cu ions, and b is biogas residue biochar with the mass percentage of 3% and 6% of nickel ions after 3 times of adsorption-desorption of nickel ions;
FIG. 7 is a diagram showing the recycling effect of different biogas residue biochar catalysts.
Detailed Description
The present invention is further illustrated by the following examples, but is not limited thereto.
The biogas residues used in the examples were obtained from Shandong Baoli Biochemical energy GmbH.
In the examples, the preparation of biogas residue biochar:
(1) soaking the biogas residue after anaerobic fermentation in tap water for 24h, draining, washing with deionized water for 3 times, oven drying at 105 deg.C in oven, crushing, sieving with 100 mesh sieve, and keeping.
(2) And (3) putting 10g of dry biogas residue powder into a porcelain boat for compaction, putting the porcelain boat into a tube furnace, heating to 700 ℃ at the speed of 10 ℃/min under the nitrogen atmosphere, keeping the temperature for 2h, then bringing the porcelain boat to the room temperature, taking the porcelain boat out, soaking the porcelain boat in 1mol/L HCl for 12h, then washing the porcelain boat to be neutral by deionized water, and finally drying the porcelain boat at 70 ℃ to obtain the biogas residue carbon.
Example 1:
the application of the waste biochar subjected to adsorption-desorption in the degradation of persistent organic pollutants by activating persulfate, wherein the waste biochar is biogas residue biochar with the mass percentage of Cu ions of 3% after 3 times of Cu ion adsorption-desorption, and the application steps are as follows:
adding the waste biochar subjected to adsorption-desorption into organic pollutant wastewater by using the waste biochar subjected to adsorption-desorption as a catalyst, simultaneously adding persulfate, wherein the adding amount of the persulfate is 1mmol/L, uniformly mixing, and then reacting under the oscillation condition that the temperature is 28 ℃ and the pH is 2.0-11.0 to degrade and remove persistent organic pollutants in the wastewater, wherein the mass-to-volume ratio of the catalyst to the organic pollutant wastewater is 1:10, unit: g/L.
Example 2:
the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants as described in example 1 is different from the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants: the mass volume ratio of the catalyst to the organic pollutant wastewater is 1:20, unit: g/L.
Example 3:
the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants as described in example 1 is different from the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants: the waste biochar is biogas residue biochar with the mass percentage of Cu ions of 6% after 3 times of Cu ion adsorption-desorption.
Example 3:
the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants as described in example 1 is different from the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants: the waste biochar is biogas residue biochar with the nickel ion mass percentage of 3% after 3 times of nickel ion adsorption-desorption, and the mass volume ratio of the catalyst to the organic pollutant wastewater is 1:10, unit: g/L.
Example 4:
the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants as described in example 1 is different from the application of the waste biochar after adsorption-desorption in the activated persulfate degradation persistent organic pollutants: the waste biochar is biogas residue biochar with the mass percentage of nickel ions of 6 percent after 3 times of nickel ion adsorption-desorption, and the mass volume ratio of the catalyst to the organic pollutant wastewater is 1:20, unit: g/L.
Experimental example:
1. examples 1 to 4, TEM and TEM-mapping of the waste biochar used are shown in fig. 1 and 2, respectively, and it can be seen from fig. 1(a) and 2(a) that the biogas residue biochar catalyst has a graphite sheet structure; as can be seen from the TEM-mapping images of FIG. 1 and FIG. 2, copper ions and nickel ions are uniformly distributed in the biogas residue biochar.
2. Degradation experiments
The degradation method comprises the following steps: the application of the biogas residue biochar catalyst in the degradation of norfloxacin comprises the following specific application methods:
(1) preparing 10mg/L norfloxacin solution, putting 50mL into a conical flask, adding 0.05mmol of potassium hydrogen persulfate, adding 5mg of metal-loaded biogas residue biochar catalyst (taking the catalyst used in examples 1-4 and a blank control as 5 groups of experiments), putting into a constant-temperature water bath oscillator, and oscillating at the oscillation speed of 140r/min and the reaction temperature of 25 ℃ for 120 min.
(2) Taking 1mL of sample in a sampling tube at different reaction time points, adding 0.5mL of ethanol, stopping the catalytic reaction, filtering by using a filter membrane, and measuring the concentration of the residual norfloxacin by using high performance liquid chromatography; meanwhile, another 1mL of the solution was taken out of the sampling tube at different reaction times, filtered through a filter membrane, and then the metal ion elution concentration was measured.
(3) And collecting the reacted catalyst, drying and carrying out the next catalytic degradation experiment (the reaction conditions are the same as the above).
And (3) testing results: the degradation effect of the different biogas residue biochar catalysts for activating persulfate to degrade norfloxacin is shown in fig. 3, and as can be seen from fig. 3, the degradation efficiency of the biogas residue biochar catalysts for activating persulfate to norfloxacin can reach more than 90%, and the higher the metal ion loading is, the higher the degradation efficiency is.
The effect of the addition of different biogas residue biochar catalysts on the degradation and removal of organic pollutants is shown in fig. 4. It can be seen from the figure that the degradation removal rate of the organic pollutants is improved along with the increase of the adding amount of the biogas residue biochar catalyst. However, when the amount of the organic contaminant added is more than 0.1g/L, the removal rate of the organic contaminant is not satisfactory, the degradation removal rate is slowly improved with respect to the amount of 0.1g/L, and the subsequent amount of the organic contaminant added is preferably 1g/L from the viewpoint of quality-cost.
The effect of the pH biogas residue biochar catalyst on the removal of organic pollutants by degradation is shown in fig. 5, and it can be seen from the graph that the removal rate of organic pollutants by degradation increases with the increase of pH in the range of pH 2-10, and the removal rate slightly decreases when the pH is higher than 10. But generally speaking, the biogas residue biochar catalyst can effectively degrade and remove organic pollutants in a wider pH range.
FIG. 6 is a metal dissolution diagram of different biogas residue biochar catalysts in the process of activating persulfate to degrade norfloxacin. As can be seen from FIG. 4, in the use process of the biogas residue biochar catalyst, the adsorbed and fixed heavy metal ions are slightly dissolved out and are far lower than the national emission standard. The catalyst has good chemical stability and practical application prospect.
FIG. 7 is a diagram showing the recycling effect of different biogas residue biochar catalysts. The metal-loaded biogas residue biochar catalysts used in examples 1-4 all showed higher catalytic activity in the fourth repeated test, and the removal rate of norfloxacin by the four catalysts in the fourth repeated test is still higher than 80%, which indicates that the metal-loaded biogas residue biochar catalysts have good stability in the reaction reminding and can be recycled.
The present invention is not limited to the above-described embodiments, which are merely exemplary and intended to illustrate the present invention, but are not to be construed as limiting the present invention.
Claims (10)
1. The application of the adsorbed-desorbed waste biochar in the degradation of persistent organic pollutants by activated persulfate comprises the following steps:
adding the waste biochar subjected to adsorption-desorption into organic pollutant wastewater by using the waste biochar subjected to adsorption-desorption as a catalyst, simultaneously adding persulfate, uniformly mixing, reacting under a shaking condition that the temperature is 25-45 ℃ and the pH is 2.0-11.0, and degrading to remove persistent organic pollutants in the wastewater, wherein the mass-to-volume ratio of the catalyst to the organic pollutant wastewater is (1-5): (10-100), and the unit: g/L; the waste biochar after adsorption-desorption is biogas residue biochar after heavy metal ions are adsorbed-desorbed for multiple times.
2. The application of claim 1, wherein the biogas residue biochar after multiple adsorption-desorption of heavy metal ions is biochar obtained by adsorbing heavy metals in heavy metal wastewater by using biogas residue biochar, then desorbing, adsorbing heavy metal ions in heavy metal wastewater by using the desorbed biochar, then desorbing, repeating the adsorption and desorption for 3-6 times, and drying.
3. Use according to claim 2, wherein the heavy metal ions are copper and/or nickel ions.
4. The use of claim 1, wherein the mass-to-volume ratio of the catalyst to the organic pollutant wastewater is (1-3) to (10-30) in units of: g/L.
5. The use of claim 1, wherein the mass-to-volume ratio of the catalyst to the organic pollutant wastewater is (1-3) to (8-20) in units of: g/L, most preferably, the mass volume ratio of the catalyst to the organic pollutant wastewater is 1:10, unit: g/L.
6. The use of claim 1, wherein the organic pollutant wastewater is medical wastewater, dye wastewater or paper-making wastewater, and the particle size of the adsorbed and desorbed waste biochar is 40-100 nm.
7. Use according to claim 1, wherein the persulfate is potassium persulfate and/or oxone, and the persulfate is added in an amount of 0.5-3mmol/L, and most preferably the persulfate is added in an amount of 1 mmol/L.
8. The application of claim 1, wherein the pH of the organic pollutant wastewater is 6-9, the shaking speed is 120-160 r/min, and the reaction time is 1-2 hours.
9. The use of claim 1, wherein the biogas residue biochar is prepared by the following method:
(1) washing the biogas residues with water, drying, grinding and sieving to obtain dry biogas residue powder;
(2) calcining and carbonizing the dry biogas residue powder to obtain biogas residue biochar.
10. The application of claim 9, wherein the biogas residue in the step (1) is obtained by anaerobic fermentation of corn stalks, wheat straw stalks, rice straw stalks or a mixture thereof at a fermentation temperature of 30-55 ℃ and a retention time of 25-45 days; in the step (1), the washing of the biogas residues is to soak the biogas residues in tap water for 24 hours and then drain the biogas residues, and then wash the biogas residues for 3 times by using deionized water, wherein the drying temperature is 60-80 ℃; in the step (2), the calcination carbonization is to put dry biogas residue powder into a tube furnace, heat the powder to 700 ℃ at a speed of 10 ℃/min under the nitrogen atmosphere, keep the temperature for 2h, then turn the temperature to room temperature, take the powder out, soak the powder in 1mol/L HCl for 12h, then wash the powder to be neutral by deionized water, and finally dry the powder at 70 ℃ to obtain the biogas residue biochar.
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| CN114471588A (en) * | 2021-12-27 | 2022-05-13 | 南京林业大学 | Carbon material and preparation method and application thereof |
| CN114163061A (en) * | 2022-02-14 | 2022-03-11 | 浙江浙能技术研究院有限公司 | Method for efficiently degrading organic matters in wastewater by virtue of hydrothermal persulfate catalytic oxidation |
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| CN115285971A (en) * | 2022-08-30 | 2022-11-04 | 云南中医药大学 | Polygonatum kingianum residue biochar and application thereof |
| CN115285971B (en) * | 2022-08-30 | 2023-12-26 | 云南中医药大学 | Polygonatum kingianum dreg biochar and application thereof |
| CN115624956A (en) * | 2022-10-13 | 2023-01-20 | 青岛科技大学 | Preparation method of efficient recyclable biogas residue carbon-based cation adsorbent |
| CN115999604A (en) * | 2022-12-15 | 2023-04-25 | 广东省科学院生态环境与土壤研究所 | Method for preparing efficient core-shell structure catalyst by taking tail end waste residue recovered from waste ternary lithium battery as raw material, product and application |
| CN117861621A (en) * | 2024-01-24 | 2024-04-12 | 安徽科凌沃特水处理技术有限公司 | Biochar/polyaluminum chloride composite adsorbent |
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