CN114307955B - Method for restoring organic pollutants in farmland soil by combining biological carbon with biological degradation - Google Patents
Method for restoring organic pollutants in farmland soil by combining biological carbon with biological degradation Download PDFInfo
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Abstract
The invention discloses a method for restoring organic pollutants in farmland soil by combining biological degradation with charcoal, which comprises the following steps: s1, preparing corn straw biomass charcoal; s2, preparing bamboo charcoal; s2-1, sampling, S2-2, primary treatment, S2-3, secondary treatment, S2-4, pyrolysis, S2-5 and a compound preparation; s3, applying corn straw biomass charcoal CB300 and bamboo charcoal BB700 at one time; s3-1, primary treatment, S3-2, extraction water treatment, S3-3, secondary treatment, S3-4 and circulation; s4, applying microbial nutrient solution for the second time; the method can effectively prevent and control migration and accumulation of PAHs from the flooded soil to the rice, DOC (polyunsaturated fatty acid) is more easily dissolved out by low molecular weight organic acid mainly secreted by the root system of the rice under the stress of the PAHs, meanwhile, anaerobic degradation of the PAHs by soil microorganisms in the flooded soil is promoted, and bamboo charcoal mainly adsorbs and fixes pollutants to inhibit reduction of the PAHs in the soil and reduces the biological effectiveness of the PAHs, so that the effect of preventing and controlling the pollutants is improved.
Description
Technical Field
The invention relates to the technical field of organic pollutant treatment, in particular to a method for restoring organic pollutants in farmland soil by combining biological degradation with charcoal.
Background
The organic pollutants refer to pollutants composed of natural organic substances existing in the forms of carbohydrates, proteins, amino acids, fats and the like and some other biodegradable artificially synthesized organic substances. Can be divided into two categories of natural organic pollutants and artificially synthesized organic pollutants. Polycyclic Aromatic Hydrocarbons (PAHs) are one of organic pollutants and are divided into natural sources and artificial sources, wherein the natural sources mainly come from the biosynthesis process of land, aquatic plants and microorganisms, and polycyclic aromatic hydrocarbons also exist in natural fires of forests and grasslands, eruptions of volcanoes and fossil fuels, lignin and bottom sludge; man-made sources are formed primarily by incomplete combustion or pyrolysis of various fossil fuels (e.g., coal, petroleum, natural gas, etc.), wood, paper, and other hydrocarbon-containing compounds under reducing conditions. Polycyclic Aromatic Hydrocarbons (PAHs) can cause various damages to the human body, such as damages to the respiratory system, the circulatory system and the nervous system, and damages to the liver and the kidney, due to toxicity, genetic toxicity, mutagenicity and carcinogenicity. And are therefore identified as the major organic pollutants affecting human health. As the number of rings increases, the chemical structure changes and the hydrophobicity increases, the electrochemical stability, durability, anti-biodegradation capacity and carcinogenicity increase, and the volatility decreases as the molecular weight increases.
In agricultural production, Polycyclic Aromatic Hydrocarbons (PAHs) are usually concentrated to crops through plant roots and enter food chains, and thus, degradation of PAHs in paddy fields should be enhanced. The biomass charcoal has wide sources, large specific surface area and rich functional groups, and is considered as a high-efficiency and high-quality adsorption material. The root exudates secreted by crops have a great influence on the environmental behavior of organic pollutants in the soil, especially in the rhizosphere. Therefore, the adsorption mechanism of the biomass charcoal to the PAHs needs to be further defined, and the optimal degradation adsorption effect needs to be found.
The different biomass charcoals have different adsorption effects on organic pollutants, the application of the biomass charcoals in soil is widely accepted, and besides the adsorption of pollutants, the biomass charcoals can also improve soil acid-base balance, increase soil organic matters, maintain soil fertility, improve microbial populations and help to weaken greenhouse effect to a certain extent. However, the adsorption-degradation mechanism of Polycyclic Aromatic Hydrocarbons (PAHs) needs to be further studied. For example, patent CN109835881B discloses a modified biochar, a biochar-based organic fertilizer, and a preparation method and application thereof, and belongs to the technical field of organic fertilizers. According to the modified charcoal, the peach wood residues are crushed and sieved, the obtained peach wood residue powder is mixed with graphene oxide, the mixture is pyrolyzed for 2-3 hours at 550-600 ℃ under the protection of nitrogen, the mixture is soaked in a potassium permanganate solution and then pyrolyzed for 0.4-0.6 hour at 550-600 ℃, and impurities are removed through washing to obtain the modified charcoal. The biochar-based organic fertilizer is prepared by fermenting the following raw materials in parts by weight: 30-40 parts of modified biochar, 60-80 parts of cow dung, 15-25 parts of decomposed vinasse, 10-20 parts of peanut shell powder, 6-8 parts of wood vinegar, 4-6 parts of beet molasses, 3-5 parts of a rhodotorula mucilaginosa fermenting agent and 0.08-0.12 part of composite cellulase. The biochar-based organic fertilizer achieves the effects of soil cultivation and yield increase, and meanwhile, the biochar-based organic fertilizer is easy to obtain raw materials, low in cost, advanced in process and capable of being produced in a large scale. However, the invention patent does not relate to the adsorption and degradation effects on organic pollutants in soil, such as Polycyclic Aromatic Hydrocarbons (PAHs) and the like, and has a narrow application range and needs further improvement.
Disclosure of Invention
Aiming at the problems, the invention provides a method for restoring organic pollutants in farmland soil by combining biological degradation with charcoal.
The technical scheme of the invention is as follows:
the method for restoring organic pollutants in farmland soil by combining biological degradation with charcoal comprises the following steps:
s1, preparing corn straw biomass charcoal: taking corn straws, sun-drying for 2d, washing for 3 times by using distilled water, drying for 6-10h in an oven, crushing by using a crusher, sieving by using a 60-80 mesh screen, heating the corn straw powder to 200 ℃ at a heating rate of 10-15 ℃/min in a tubular furnace, preserving heat for 1h, then heating to 300 ℃ at a heating rate of 20 ℃/min, preserving heat for 2-3h, cooling to room temperature, taking out, and washing for 3 times by using deionized water to obtain corn straw biomass charcoal CB 300;
s2, bamboo charcoal preparation: taking wild alpine moso bamboos, naturally drying for 3d, soaking in biomass degradation liquid for degradation for 12-24h, drying in an oven for 6-10h, crushing by using a crusher, sieving by using a 60-80 mesh sieve, heating alpine moso bamboo powder to 1000 ℃ at a heating rate of 20-25 ℃/min in a tubular furnace, and carrying out thermal insulation pyrolysis for 1-2h to obtain bamboo charcoal BB 700;
s3, one application: setting up a phytotron greenhouse above the soil of the marsh crop farmland affected by the polycyclic aromatic hydrocarbon PAHs, applying the corn straw biomass charcoal CB300 obtained in the step S1 and the bamboo charcoal BB700 obtained in the step S2 to the soil, wherein the mass ratio of the applied corn straw biomass charcoal CB300 in the soil is 0.5-1.5%, and the mass ratio of the applied bamboo charcoal BB700 in the soil is 0.4-1%;
s4, secondary application: and (5) continuously applying a microbial nutrient solution to the soil of the marsh crop farmland to which the corn straw biomass charcoal CB300 and the bamboo charcoal BB700 are applied 60-90 days after the step S3 is finished, and continuously culturing for 150 days to observe the content of the Polycyclic Aromatic Hydrocarbons (PAHs) in the soil.
Further, the drying temperature in the oven in the steps S1 and S2 is 70-80 ℃. The aim of uniform drying is achieved.
Further, the growth year of the wild alpine moso bamboo obtained in the step S2 is 3 to 5 years. The raw materials with qualified quality can ensure that the obtained biomass charcoal has good performance.
Further, in the step S2, the mass ratio of the wild alpine moso bamboo to the biomass degradation liquid is 1: 3. the biomass degradation liquid is used for pretreating biomass raw materials, so that certain organic nutrients can be provided, and the prepared biomass charcoal has a certain repairing effect on soil.
Further, the preparation method of the biomass degradation liquid in the step S2 includes:
s2-1, sampling: grinding 5 weight parts of rice hull, sieving with 80-100 mesh sieve, air drying, and keeping water content of rice hull powder at 1-5 wt%;
s2-2, primary treatment: adding the rice hull powder into 6-9 parts by weight of hydrogen peroxide solution with mass concentration of 5%, stirring for 1-2h at 40-45 ℃, filtering and drying;
s2-3, secondary treatment: adding the rice hull powder obtained in the step S2-2 after primary treatment into 6-8 parts by weight of humic acid solution with mass concentration of 10%, stirring for 0.5-1h at 75-85 ℃, washing for 2-3 times by using deionized water, filtering and drying until the water content is 1-5 wt%;
s2-4, pyrolysis: placing the rice hull powder obtained in the step S2-3 after the secondary treatment in a tubular furnace, heating to 700-750 ℃ at the temperature rising speed of 25-35 ℃/min, and preserving heat for 10-15min under the nitrogen atmosphere to obtain rice hull biochar;
s2-5, compound preparation: and (4) mixing the rice hull biochar obtained in the step (S2-4) with 1.8-2.3 parts by weight of calcium hydroxide solution, and stirring for 5-10min to obtain a biomass degradation liquid. Organic nutrients in the biomass degradation liquid are coated on the surface of the biomass charcoal after pyrolysis, and a synergistic effect can be achieved on removal of organic pollutants in soil.
Further, the mass concentration of the calcium hydroxide solution in the step S2-5 is 60 wt%. The calcium hydroxide solution is added to facilitate the mixing with the rice husk biochar, so that the lignin content in the wild high mountain moso bamboo is reduced, and the wild high mountain moso bamboo is fully pyrolyzed.
Further, the swamp crops in step S3 are rice. The method is beneficial to improving the soil ecology of the aged rice and promoting the growth of the rice.
Further, in the step S3, the corn stalk biomass charcoal CB300 is applied to a position 10-15cm below the surface layer of the soil by a manual shovel, and a certain amount of nitrogen fertilizer is applied at the same time, wherein the mass ratio of the corn stalk biomass charcoal CB300 to the nitrogen fertilizer is 4: 1-1.5, then applying bamboo charcoal BB700 to a position 12-18cm below the surface layer of soil through an injector, adjusting the daytime temperature to 28-32 ℃, the nighttime temperature to 25-27 ℃ and the humidity to 39-43% in a phytotron greenhouse after applying, keeping the soil in a dry state after 15-20 days, and then performing soil dry-wet alternate management, wherein the soil dry-wet alternate management specifically comprises the following steps:
s3-1, primary water injection: injecting deionized water into the soil, enabling the initial water level to be 2-3cm above the surface of the soil, keeping for 6h, then inserting a water pumping pipe 5cm below the soil to pump water with the liquid level height of 0.5cm, continuously pumping water with the liquid level height of 0.5cm after 12h until no water is accumulated on the surface of the soil, at the moment, the soil is in a wet and partially dry state, and keeping field water pumped each time for later use;
s3-2, treatment of extracted water: independently treating the field water extracted each time in the step S3-1 in batches, firstly filtering the field water to remove impurities, injecting the field water into an oxidation pond for oxidation treatment, introducing ozone into the oxidation pond and continuously stirring, wherein the introduced ozone amount is 2-5mg/L, the stirring speed is 85-130r/min, and the duration is 6h, then introducing the field water subjected to oxidation treatment into a glass pipeline filled with the pretreated polypropylene adsorption resin, and the weight part ratio of the field water subjected to oxidation treatment to the polypropylene adsorption resin is 60: 1, collecting purified field water at the flow rate of 5L/min to obtain a plurality of parts of purified field water;
s3-3, secondary water injection: after the water injection for one time of step S1-3 is finished for 48 hours, reinjecting the purified field water obtained in the step S3-2, injecting one copy of field water each time, wherein the time interval of each injection is 24 hours, continuously injecting deionized water after all injection is finished to ensure that the water level is kept the same as the initial water level in the step S3-1, and at the moment, the soil is in a flooded state;
s3-4, circulation: and repeating the steps of S3-1 primary water injection, S3-2 water extraction treatment and S3-3 secondary water injection for 2 times, and keeping the soil in a flooded state. The degradation effect of the biomass charcoal on heavy metals and organic pollutants in soil is promoted by alternately managing the dryness and the wetness of the soil.
Further, the pretreatment method of the polypropylene-ethylene adsorption resin in the step S3-2 is as follows: before use, immersing the polystyrene adsorbent resin in an acetone solution with the mass concentration of 30% for 2h, taking out and drying, immersing the polystyrene adsorbent resin in a cyclohexane solution with the mass concentration of 50% for 2h, taking out and washing the polystyrene adsorbent resin for 3 times by using deionized water to obtain the pretreated polystyrene adsorbent resin. The polypropylene ethylene adsorption resin is primarily purified to remove other soluble organic matters in the polypropylene ethylene adsorption resin, so that the treatment effect of organic pollutants in the extracted field water is improved.
Further, in the step S4, the microbial nutrient solution contains the following components in percentage by mass: 3-5% of urea, 0.5-1% of amino acid, 1-2% of starch, 2-3% of glucose, 0.5-2% of chitosan and the balance of water. The bioremediation efficiency of organic pollutants is improved by injecting a microbial nutrient solution.
The beneficial effects of the invention are:
(1) the method for restoring organic pollutants in farmland soil by combining and biodegrading the biochar and the bamboo charcoal is applied to the farmland soil of the marsh crops affected by PAHs (polycyclic aromatic hydrocarbons), so that the migration and accumulation of the PAHs from the flooded soil to the paddy can be effectively prevented and controlled, DOC (docos) can be more easily dissolved out by low-molecular-weight organic acid mainly secreted by the root system of the paddy under the stress of the PAHs, the PAHs in the soil are desorbed by the treatment of the corn stalk charcoal, meanwhile, the anaerobic degradation of the PAHs by soil microorganisms in the flooded soil is promoted, the bamboo charcoal mainly adsorbs and fixes the pollutants to inhibit the reduction of the PAHs in the soil, the biological effectiveness of the PAHs is reduced, and the pollutant prevention and control effect is improved.
(2) The method for restoring the organic pollutants in the farmland soil by the biochar combined biodegradation improves and optimizes the preparation methods of the corn straw biochar and the bamboo charcoal so as to improve the combined effect of the two biochar, optimizes the application formula, adopts a soil dry-wet alternative management method, promotes the adsorption capacity of the biochar to the pollutants compared with the soil by treating and reinjecting the extracted field water, improves the microbial population by injecting ozone, increases the soil nutrition and the degradation effect of soil microbes on the pollutants, improves the treatment effect on the organic pollutants, and can completely degrade the organic pollutants in the soil to a certain extent.
Drawings
FIG. 1 is a process flow diagram of the process of the present invention.
Detailed Description
Example 1
The method for restoring organic pollutants in farmland soil by combining biological degradation with charcoal comprises the following steps:
s1, preparing corn straw biomass charcoal: taking corn straws, drying in the sun for 2d, washing with distilled water for 3 times, drying in an oven for 8h, wherein the drying temperature in the oven is 75 ℃, crushing with a crusher, sieving with a 70-mesh screen, heating the corn straw powder in a tubular furnace at a heating rate of 13 ℃/min to 200 ℃, preserving heat for 1h, then heating at a heating rate of 20 ℃/min to 300 ℃, preserving heat for 2.5h, cooling to room temperature, taking out, washing with deionized water for 3 times, and obtaining corn straw biomass charcoal CB 300;
s2, bamboo charcoal preparation: taking wild alpine moso bamboos with the growth years of 4 years, naturally drying for 3d, soaking in biomass degradation liquid for degradation for 18h, wherein the mass ratio of the wild alpine moso bamboos to the biomass degradation liquid is 1: 3, drying for 8 hours in an oven at the drying temperature of 75 ℃, crushing by using a crusher, sieving by using a 70-mesh screen, heating the alpine moso bamboo powder to 1000 ℃ at the heating rate of 23 ℃/min in a tubular furnace, and carrying out thermal insulation pyrolysis for 1.5 hours to obtain bamboo charcoal BB 700;
the preparation method of the biomass degradation liquid comprises the following steps:
s2-1, sampling: grinding and crushing 5 parts by weight of rice husk, sieving by using a 90-mesh sieve, and air-drying and keeping the water content of the rice husk powder at 2 wt%;
s2-2, primary treatment: adding the rice hull powder into 8 parts by weight of hydrogen peroxide solution with the mass concentration of 5%, stirring for 1.5h at 42 ℃, filtering and drying;
s2-3, secondary treatment: adding the rice hull powder obtained in the step S2-2 after primary treatment into 7 parts by weight of humic acid solution with the mass concentration of 10%, stirring for 0.8h at the temperature of 80 ℃, washing for 3 times by using deionized water, filtering and drying until the water content is 2 wt%;
s2-4, pyrolysis: placing the rice hull powder obtained in the step S2-3 after the secondary treatment in a tubular furnace, heating to 720 ℃ at the heating rate of 30 ℃/min, and preserving heat for 12min under the nitrogen atmosphere to obtain rice hull biochar;
s2-5, compound preparation: mixing the rice hull biochar obtained in the step S2-4 with 2 parts by weight of calcium hydroxide solution with the mass concentration of 60wt%, and stirring for 6min to obtain biomass degradation liquid;
s3, one application: setting up a phytotron greenhouse above the soil of the rice farmland of the marsh crops affected by the polycyclic aromatic hydrocarbon PAHs, applying the corn straw biomass charcoal CB300 obtained in the step S1 and the bamboo charcoal BB700 obtained in the step S2 to the soil, wherein the mass ratio of the applied corn straw biomass charcoal CB300 in the soil is 1%, and the mass ratio of the applied bamboo charcoal BB700 in the soil is 0.6%;
s4, secondary application: at 75d after the step S3 is finished, continuously applying a microbial nutrient solution to the soil of the marsh crop rice farmland which is applied with the corn stalk biomass charcoal CB300 and the bamboo charcoal BB700, wherein the microbial nutrient solution comprises the following components in percentage by mass: 4% of urea, 0.8% of amino acid, 1.5% of starch, 2.5% of glucose, 0.6% of chitosan and the balance of water, and continuously culturing for 150 days to observe the content of Polycyclic Aromatic Hydrocarbons (PAHs) in the soil.
Example 2
This embodiment is substantially the same as embodiment 1, except that: step S1 different preparation methods of the corn straw biomass charcoal.
S1, preparing corn straw biomass charcoal: taking corn straws, sun-drying for 2d, washing for 3 times by using distilled water, drying for 6h in an oven, drying at 70 ℃ in the oven, crushing by using a crusher, sieving by using a 60-mesh screen, heating the corn straw powder to 200 ℃ at a heating rate of 10 ℃/min in a tubular furnace, preserving heat for 1h, heating to 300 ℃ at a heating rate of 20 ℃/min, preserving heat for 2h, cooling to room temperature, taking out, and washing for 3 times by using deionized water to obtain the corn straw biomass charcoal CB 300.
Example 3
This embodiment is substantially the same as embodiment 1, except that: step S1 is different in preparation method of corn straw biomass charcoal.
S1, preparing corn straw biomass charcoal: taking corn straws, sun-drying for 2d, washing for 3 times by using distilled water, drying for 10h in an oven, wherein the drying temperature in the oven is 80 ℃, crushing by using a crusher, sieving by using an 80-mesh screen, heating the corn straw powder to 200 ℃ at a heating rate of 15 ℃/min in a tubular furnace, preserving heat for 1h, then heating to 300 ℃ at a heating rate of 20 ℃/min, preserving heat for 3h, cooling to room temperature, taking out, and washing for 3 times by using deionized water to obtain the corn straw biomass charcoal CB 300.
Example 4
This embodiment is substantially the same as embodiment 1, except that: step S2 the preparation method of bamboo charcoal is different.
S2, bamboo charcoal preparation: taking wild alpine moso bamboos with the growth years of 3 years, naturally drying for 3d, soaking in biomass degradation liquid for degradation for 12h, wherein the mass ratio of the wild alpine moso bamboos to the biomass degradation liquid is 1: and 3, drying for 6 hours in an oven at the drying temperature of 70 ℃, crushing by using a crusher, sieving by using a 60-mesh screen, heating the alpine moso bamboo powder to 1000 ℃ in a tubular furnace at the heating rate of 20 ℃/min, and carrying out thermal insulation pyrolysis for 1 hour to obtain the bamboo charcoal 700 BB.
Example 5
This embodiment is substantially the same as embodiment 1, except that: step S2 the preparation method of bamboo charcoal is different.
S2, preparing bamboo charcoal: taking wild alpine moso bamboos with the growth years of 5 years, naturally drying for 3d, soaking in biomass degradation liquid for degradation for 24h, wherein the mass ratio of the wild alpine moso bamboos to the biomass degradation liquid is 1: and 3, drying for 10 hours in an oven, wherein the drying temperature in the oven is 80 ℃, crushing by using a crusher, sieving by using an 80-mesh screen, heating the alpine moso bamboo powder to 1000 ℃ at the heating rate of 25 ℃/min in a tubular furnace, and carrying out thermal insulation pyrolysis for 2 hours to obtain the bamboo charcoal 700 BB.
Example 6
This embodiment is substantially the same as embodiment 1, except that: the preparation methods of the biomass degradation liquid are different.
The preparation method of the biomass degradation liquid comprises the following steps:
s2-1, sampling: grinding and crushing 5 parts by weight of rice husk, sieving by using a 80-mesh sieve, and air-drying while keeping the water content of the rice husk powder at 1 wt%;
s2-2, primary treatment: adding the rice hull powder into 6 parts by weight of hydrogen peroxide solution with the mass concentration of 5%, stirring for 1h at 40 ℃, filtering and drying;
s2-3, secondary treatment: adding the rice hull powder obtained in the step S2-2 after primary treatment into 6 parts by weight of humic acid solution with the mass concentration of 10%, stirring for 0.5h at the temperature of 75 ℃, washing for 2 times by using deionized water, filtering and drying until the water content is 1 wt%;
s2-4, pyrolysis: placing the rice hull powder obtained in the step S2-3 after the secondary treatment in a tubular furnace, heating to 700 ℃ at the heating rate of 25 ℃/min, and preserving heat for 10min under the nitrogen atmosphere to obtain the rice hull biochar;
s2-5, compound preparation: and (5) mixing the rice hull biochar obtained in the step (S2-4) with 1.8 parts by weight of a calcium hydroxide solution with the mass concentration of 60wt%, and stirring for 5min to obtain a biomass degradation solution.
Example 7
This embodiment is substantially the same as embodiment 1, except that: the preparation methods of the biomass degradation liquid are different.
The preparation method of the biomass degradation liquid comprises the following steps:
s2-1, sampling: grinding and crushing 5 parts by weight of rice husk, sieving by using a 100-mesh sieve, and air-drying while keeping the water content of the rice husk powder at 5 wt%;
s2-2, primary treatment: adding the rice hull powder into 9 parts by weight of hydrogen peroxide solution with the mass concentration of 5%, stirring for 2 hours at the temperature of 45 ℃, filtering and drying;
s2-3, secondary treatment: adding the rice hull powder subjected to primary treatment obtained in the step S2-2 into 8 parts by weight of humic acid solution with the mass concentration of 10%, stirring for 1h at 85 ℃, washing for 3 times by using deionized water, filtering and drying until the water content is 5 wt%;
s2-4, pyrolysis: placing the rice hull powder obtained in the step S2-3 after the secondary treatment in a tube furnace, heating to 750 ℃ at the heating rate of 35 ℃/min, and preserving heat for 15min in the nitrogen atmosphere to obtain rice hull biochar;
s2-5, compound preparation: and (4) mixing the rice hull biochar obtained in the step (S2-4) with 2.3 parts by weight of a calcium hydroxide solution with the mass concentration of 60wt%, and stirring for 10min to obtain a biomass degradation liquid.
Example 8
This embodiment is substantially the same as embodiment 1, except that: the biomass charcoal application amount and the microorganism nutrient solution are different between the first application and the second application.
S3, one application: setting up a phytotron greenhouse above the soil of the rice farmland of the marsh crops affected by the polycyclic aromatic hydrocarbon PAHs, applying the corn straw biomass charcoal CB300 obtained in the step S1 and the bamboo charcoal BB700 obtained in the step S2 to the soil, wherein the mass ratio of the applied corn straw biomass charcoal CB300 in the soil is 0.5%, and the mass ratio of the applied bamboo charcoal BB700 in the soil is 0.4%;
s4, secondary application: and (5) continuously applying a microbial nutrient solution to the soil of the marsh crop rice farmland which is applied with the corn straw biomass carbon CB300 and the bamboo charcoal BB700 60 days after the step S3 is finished, wherein the microbial nutrient solution comprises the following components in percentage by mass: 3% of urea, 0.5% of amino acid, 1% of starch, 2% of glucose, 0.5% of chitosan and the balance of water, and continuously culturing for 150 days to observe the content of Polycyclic Aromatic Hydrocarbons (PAHs) in the soil.
Example 9
This embodiment is substantially the same as embodiment 1, except that: the biomass charcoal application amount and the microorganism nutrient solution are different between the first application and the second application.
S3, one application: setting up a phytotron greenhouse above the soil of the rice farmland of the marsh crops affected by the polycyclic aromatic hydrocarbon PAHs, applying the corn straw biomass charcoal CB300 obtained in the step S1 and the bamboo charcoal BB700 obtained in the step S2 to the soil, wherein the mass ratio of the corn straw biomass charcoal CB300 in the soil is 1.5%, and the mass ratio of the bamboo charcoal BB700 in the soil is 1%;
s4, secondary application: and (5) continuously applying a microbial nutrient solution to the soil of the rice farmland of the marsh crops with the corn straw biomass carbon CB300 and the bamboo charcoal BB700 at 90d after the step S3 is finished, wherein the microbial nutrient solution comprises the following components in percentage by mass: 5% of urea, 1% of amino acid, 2% of starch, 3% of glucose, 2% of chitosan and the balance of water, and continuously culturing for 150 days to observe the content of Polycyclic Aromatic Hydrocarbons (PAHs) in the soil.
Example 10
This embodiment is substantially the same as embodiment 1, except that: step S3 also includes adding a quantity of nitrogen fertilizer at one application.
Apply maize straw living beings charcoal CB300 in the following 13cm position of soil top layer through artifical shovel that turns over, apply a quantitative nitrogenous fertilizer simultaneously, maize straw living beings charcoal CB300 is 4 with the mass ratio of nitrogenous fertilizer: 1.2, bamboo charcoal BB700 was applied by syringe 15cm below the surface of the soil.
Example 11
This embodiment is substantially the same as embodiment 1, except that: step S3 also includes adding a quantity of nitrogen fertilizer at one application.
The corn straw biomass charcoal CB300 is applied to the position 10cm below the surface layer of the soil through a manual turning shovel, a certain amount of nitrogen fertilizer is applied at the same time, and the mass ratio of the corn straw biomass charcoal CB300 to the nitrogen fertilizer is 4: 1, bamboo charcoal BB700 was applied by syringe at a position 12cm below the surface of the soil.
Example 12
This embodiment is substantially the same as embodiment 1, except that: step S3 also includes adding a quantity of nitrogen fertilizer at one application.
Apply maize straw living beings charcoal CB300 in the following 15cm position of soil top layer through artifical shovel that turns over, apply a quantitative nitrogenous fertilizer simultaneously, maize straw living beings charcoal CB300 is 4 with the mass ratio of nitrogenous fertilizer: 1.5, bamboo charcoal BB700 was applied by syringe at a location 18cm below the surface of the soil.
Example 13
This embodiment is substantially the same as embodiment 1, except that: step S3 further includes performing soil wet-dry alternation management when the soil is applied once.
Adjusting the daytime temperature and the nighttime temperature in the artificial climate greenhouse to be 30 ℃, the nighttime temperature to be 26 ℃ and the humidity to be 41%, wherein the soil is in a drought state after the soil lasts for 18 days, and then performing soil dry-wet alternation management, wherein the soil dry-wet alternation management specifically comprises the following steps:
s3-1, primary water injection: injecting deionized water into the soil, enabling the initial water level to be located 2.5cm above the surface of the soil, keeping for 6 hours, then inserting a water pumping pipe into the position 5cm below the soil to pump water with the liquid level height of 0.5cm, continuously pumping the water with the liquid level height of 0.5cm after 12 hours until no water is accumulated on the surface of the soil, enabling the soil to be in a wet and partially dry state, and keeping field water pumped each time for later use;
s3-2, treating the extracted water: separately treating the field water extracted each time in the step S3-1 in batches, firstly filtering the field water to remove impurities, injecting the field water into an oxidation pond for oxidation treatment, introducing ozone into the oxidation pond and continuously stirring, wherein the introduced ozone amount is 3mg/L, the stirring speed is 100r/min, and the duration is 6 hours, then introducing the field water subjected to oxidation treatment into a glass pipeline filled with pretreated polypropylene adsorption resin, and the weight ratio of the field water subjected to oxidation treatment to the polypropylene adsorption resin is 60: 1, collecting purified field water at the flow rate of 5L/min to obtain a plurality of parts of purified field water; the pretreatment method of the polypropylene-ethylene adsorption resin comprises the following steps: immersing the polypropylene ethylene adsorption resin in an acetone solution with the mass concentration of 30% for 2h before use, taking out and drying, immersing the polypropylene ethylene adsorption resin in a cyclohexane solution with the mass concentration of 50% for 2h, taking out and washing the polypropylene ethylene adsorption resin for 3 times by using deionized water to obtain the pretreated polypropylene ethylene adsorption resin;
s3-3, secondary water injection: after the water injection for one time of step S1-3 is finished for 48 hours, reinjecting the purified field water obtained in the step S3-2, injecting one copy of field water each time, wherein the time interval of each injection is 24 hours, continuously injecting deionized water after all injection is finished to ensure that the water level is kept the same as the initial water level in the step S3-1, and at the moment, the soil is in a flooded state;
s3-4, circulation: and repeating the steps of S3-1 primary water injection, S3-2 water extraction treatment and S3-3 secondary water injection for 2 times, and keeping the soil in a flooded state.
Example 14
This embodiment is substantially the same as embodiment 1, except that: step S3 further includes performing soil wet-dry alternation management when the soil is applied once.
Adjusting the daytime temperature of 28 ℃, the nighttime temperature of 25 ℃ and the humidity of 39% in the artificial climate greenhouse, keeping the soil in a drought state after 15 days, and then performing soil dry-wet alternate management, wherein the soil dry-wet alternate management specifically comprises the following steps:
s3-1, primary water injection: injecting deionized water into the soil, enabling the initial water level to be 2cm above the surface of the soil, keeping for 6h, then inserting a water pumping pipe 5cm below the soil to pump water with the liquid level height of 0.5cm, continuously pumping water with the liquid level height of 0.5cm after 12h until no water is accumulated on the surface of the soil, enabling the soil to be in a wet and partially dry state, and keeping field water pumped each time for later use;
s3-2, treating the extracted water: separately treating the field water extracted each time in the step S3-1 in batches, firstly filtering the field water to remove impurities, injecting the field water into an oxidation pond for oxidation treatment, introducing ozone into the oxidation pond and continuously stirring, wherein the introduced ozone amount is 2mg/L, the stirring speed is 85r/min, and the duration is 6 hours, then introducing the field water subjected to oxidation treatment into a glass pipeline filled with pretreated polypropylene adsorption resin, and the weight ratio of the field water subjected to oxidation treatment to the polypropylene adsorption resin is 60: 1, collecting purified field water at the flow rate of 5L/min to obtain a plurality of parts of purified field water; the pretreatment method of the polypropylene-ethylene adsorption resin comprises the following steps: immersing the polypropylene ethylene adsorption resin in an acetone solution with the mass concentration of 30% for 2 hours before use, taking out and drying, immersing the polypropylene ethylene adsorption resin in a cyclohexane solution with the mass concentration of 50% for 2 hours, taking out and washing the polypropylene ethylene adsorption resin for 3 times by using deionized water to obtain the pretreated polypropylene ethylene adsorption resin;
s3-3, secondary water injection: after the water injection for one time of step S1-3 is finished for 48 hours, reinjecting the purified field water obtained in the step S3-2, injecting one copy of field water each time, wherein the time interval of each injection is 24 hours, continuously injecting deionized water after all injection is finished to ensure that the water level is kept the same as the initial water level in the step S3-1, and at the moment, the soil is in a flooded state;
s3-4, circulation: and repeating the steps of S3-1 primary water injection, S3-2 water extraction treatment and S3-3 secondary water injection for 2 times, and keeping the soil in a flooded state.
Example 15
This embodiment is substantially the same as embodiment 1, except that: step S3 further includes performing soil wet and dry alternation management when the application is performed once.
Adjusting the daytime temperature of 32 ℃, the nighttime temperature of 27 ℃ and the humidity of 43% in the artificial climate greenhouse, keeping the soil in a drought state after 20 days, and then performing soil dry-wet alternate management, wherein the soil dry-wet alternate management specifically comprises the following steps:
s3-1, primary water injection: injecting deionized water into the soil, enabling the initial water level to be located 3cm above the surface of the soil, keeping for 6h, then inserting a water pumping pipe 5cm below the soil to pump water with the liquid level height of 0.5cm, continuously pumping water with the liquid level height of 0.5cm after 12h until no water is accumulated on the surface of the soil, enabling the soil to be in a wet and partially dry state, and keeping field water pumped each time for later use;
s3-2, treating the extracted water: separately treating the field water extracted each time in the step S3-1 in batches, firstly filtering the field water to remove impurities, injecting the field water into an oxidation pond for oxidation treatment, introducing ozone into the oxidation pond and continuously stirring, wherein the introduced ozone amount is 5mg/L, the stirring speed is 130r/min, and the duration is 6h, then introducing the field water subjected to oxidation treatment into a glass pipeline filled with pretreated polyethylene-propylene adsorption resin, and the weight ratio of the field water subjected to oxidation treatment to the polyethylene-propylene adsorption resin is 60: 1, collecting purified field water at the flow rate of 5L/min to obtain a plurality of parts of purified field water; the pretreatment method of the polystyrene adsorbent resin comprises the following steps: immersing the polypropylene ethylene adsorption resin in an acetone solution with the mass concentration of 30% for 2h before use, taking out and drying, immersing the polypropylene ethylene adsorption resin in a cyclohexane solution with the mass concentration of 50% for 2h, taking out and washing the polypropylene ethylene adsorption resin for 3 times by using deionized water to obtain the pretreated polypropylene ethylene adsorption resin;
s3-3, secondary water injection: after the water injection for one time of step S1-3 is finished for 48 hours, reinjecting the purified field water obtained in the step S3-2, injecting one copy of field water each time, wherein the time interval of each injection is 24 hours, continuously injecting deionized water after all injection is finished to ensure that the water level is kept the same as the initial water level in the step S3-1, and at the moment, the soil is in a flooded state;
s3-4, circulation: and repeating the steps of S3-1 primary water injection, S3-2 water extraction treatment and S3-3 secondary water injection for 2 times, and keeping the soil in a flooded state.
Experimental example 1
To verify the efficiency of extraction of PAHs from rice and the accuracy of the method of the present invention, experiments were conducted based on the data given in examples 1-13 to determine the concentrations of PAHs in soil and rice, which were calculated on a dry weight basis and expressed as arithmetic mean, and the biomass of roots, stems and leaves and seeds of rice of examples 1-5 was first examined and compared with comparative examples 1-3, in which no biomass charcoal was applied and corn stalk biomass charcoal CB300 and bamboo charcoal BB700 were applied alone, and the results are shown in Table 1.
TABLE 1 Rice parts biomass of examples 1-5 and comparative examples 1-3
As can be seen from the data in Table 1, in comparison with the comparative examples 1-5 and 1, the addition of two kinds of biomass charcoal leads the yield of roots, stems and leaves and seeds of rice to be increased remarkably, which indicates that the addition of two kinds of biomass charcoal has a large change in the physicochemical properties of soil, the C, N content in the soil is relatively highest, and thus the increase of the yield of rice is facilitated, and the addition of the biochar can reduce the degree of toxicity of toxic substances in the soil to plants to a certain extent. Comparing examples 1-5 with comparative examples 2 and 3, it can be found that the rice is promoted by adding two kinds of biomass charcoal better than by adding only one kind of biomass charcoal, wherein the yield is improved by applying the corn stalk biomass charcoal CB300 alone similar to the result of adding two kinds of biomass, and the yield is improved by applying the bamboo charcoal BB700 alone slightly. Comparing examples 1 to 5, it can be seen that when two kinds of biomass charcoals are prepared, proper pyrolysis temperature and pyrolysis time are adopted, and the particle size of raw materials is limited, and these factors can have some effects on the effect of the biomass charcoals, but not main effects, and the preparation parameters in example 1 are selected as the optimal ones.
Experimental example 2
The PAHs content of the roots, stems and leaves and seeds of the rice in the examples 1, 6-9 were measured and compared with that of the comparative examples 1-3 in which no biomass charcoal was applied and corn stalk biomass charcoal CB300 and bamboo charcoal BB700 were applied alone, and the results are shown in Table 2.
TABLE 2 contents of PAHs in respective portions of paddy rice of examples 1, 6 to 9 and comparative examples 1 to 3
| Examples | Root microgram/kg | Mu g/kg of stem and leaf | Grain mu g/kg |
| Example 1 | 253.3 | 27.7 | 9.6 |
| Example 6 | 257.4 | 28.8 | 10.0 |
| Example 7 | 259.5 | 28.1 | 10.3 |
| Example 8 | 260.2 | 29.4 | 10.1 |
| Example 9 | 252.6 | 27.8 | 9.5 |
| Comparative example 1 | 392.6 | 37.8 | 12.5 |
| Comparative example 2 | 286.7 | 30.9 | 10.8 |
| Comparative example 3 | 278.1 | 29.8 | 10.6 |
As can be seen from the data in Table 2, PAHs are more easily enriched at the roots of rice rather than edible parts, the enrichment content of PAHs in the overground parts of rice is not obviously different between the examples and the comparative examples, compared with the examples 1, 6-9 and the comparative example 1, the addition of two biomass charcoals can effectively prevent and control the accumulation of PAHs from soil to the roots of rice, wherein the prevention and control effect in the example 1 is the best, which indicates that the improvement of bamboo charcoal performance is facilitated through the parameter adjustment of the preparation method of the biomass degradation liquid, and simultaneously, the enrichment of PAHs is also greatly influenced, the addition of the biomass charcoals has a certain inhibition effect on the enrichment of PAHs in soil when the proportion is larger, but when the application amount is too much, the C content in soil is possibly too high, the normal growth of rice is influenced, the yield of rice is not favorable, and the cost is also changed and accordingly, the selection of the appropriate application amount is very important, the carbon/soil mass ratio given in example 1 for one application was optimal.
Experimental example 3
The total amount of PAHs in the soil of examples 1, 10-15 was measured and compared with comparative example 1 without any application of biomass charcoal, and the results are shown in Table 3.
TABLE 3 Total amount of PAHs in soil of examples 1, 10 to 15 and comparative example 1
As can be seen from the data in table 3, in comparative examples 1, 10 to 12 and comparative example 1, when the corn stalk biomass charcoal CB300 is applied, a certain amount of nitrogen fertilizer is applied to facilitate the growth of rice and simultaneously to achieve a certain effect of adsorbing and fixing the total PAHs in the soil, but if the applied nitrogen fertilizer is too high, the content of N in the soil is increased, the rice grows too fast, and the yield of the rice is not good, so the nitrogen fertilizer application amount in the preferred example 10 is optimal;
it can be seen from comparison of examples 1, 13-15 and comparative example 1 that under the effect of the soil wet-dry alternate management method, the total amount of effective PAHs in the soil can be significantly reduced, because the PAHs in the soil can be converted to a residue state by applying two biomass charcoals while performing the soil wet-dry alternate management, so that the microbial degradation process of the PAHs in the soil can be accelerated, and the rapid reduction of pollutants can be effectively promoted;
in conclusion of the 3 experimental examples, it can be concluded that, in the soil of the farmland polluted by PAHs for a long time, a certain amount of corn stalk carbon or bamboo charcoal is added to effectively prevent and control migration and accumulation of PAHs from flooded soil to rice, DOC is more easily dissolved out by low molecular weight organic acids mainly secreted by rice root systems under the stress of PAHs, and desorption of PAHs can be more effectively promoted by corn stalk biomass carbon CB300, so that applying a certain amount of corn stalk biomass carbon CB300 and then applying bamboo charcoal BB700 is more beneficial to PAHs desorption; meanwhile, under the action of a soil dry-wet alternative management method, the degradation of PAHs is facilitated, so that the whole soil treatment idea of adsorption-desorption-degradation promotion is realized, and the treatment of organic pollutants in soil and the growth of crops can be well promoted.
Claims (7)
1. The method for restoring organic pollutants in farmland soil by combining biological degradation with charcoal is characterized by comprising the following steps:
s1, preparing the corn straw biomass charcoal: taking corn straws, sun-drying for 2d, washing for 3 times by using distilled water, drying for 6-10h in an oven, crushing by using a crusher, sieving by using a 60-80 mesh screen, heating the corn straw powder to 200 ℃ at a heating rate of 10-15 ℃/min in a tubular furnace, preserving heat for 1h, then heating to 300 ℃ at a heating rate of 20 ℃/min, preserving heat for 2-3h, cooling to room temperature, taking out, and washing for 3 times by using deionized water to obtain corn straw biomass charcoal CB 300;
s2, bamboo charcoal preparation: taking wild alpine moso bamboos, naturally drying for 3d, soaking in biomass degradation liquid for degradation for 12-24h, drying in an oven for 6-10h, crushing by using a crusher, sieving by using a 60-80 mesh sieve, heating alpine moso bamboo powder to 1000 ℃ at a heating rate of 20-25 ℃/min in a tubular furnace, and carrying out thermal insulation pyrolysis for 1-2h to obtain bamboo charcoal BB 700;
the preparation method of the biomass degradation liquid in the step S2 comprises the following steps:
s2-1, sampling: grinding 5 weight parts of rice hull, sieving with 80-100 mesh sieve, air drying, and keeping water content of rice hull powder at 1-5 wt%;
s2-2, primary treatment: adding the rice hull powder into 6-9 parts by weight of hydrogen peroxide solution with mass concentration of 5%, stirring for 1-2h at 40-45 ℃, filtering and drying;
s2-3, secondary treatment: adding the rice hull powder obtained in the step S2-2 after primary treatment into 6-8 parts by weight of humic acid solution with mass concentration of 10%, stirring for 0.5-1h at 75-85 ℃, washing for 2-3 times by using deionized water, filtering and drying until the water content is 1-5 wt%;
s2-4, pyrolysis: placing the rice hull powder obtained in the step S2-3 after the secondary treatment in a tubular furnace, heating to 700-750 ℃ at the heating rate of 25-35 ℃/min, and preserving heat for 10-15min under the nitrogen atmosphere to obtain the rice hull biochar;
s2-5, compound preparation: mixing the rice hull biochar obtained in the step S2-4 with 1.8-2.3 parts by weight of calcium hydroxide solution, and stirring for 5-10min to obtain biomass degradation liquid;
s3, one application: setting up a phytotron greenhouse above the soil of the marsh crop farmland affected by the polycyclic aromatic hydrocarbon PAHs, applying the corn straw biomass charcoal CB300 obtained in the step S1 and the bamboo charcoal BB700 obtained in the step S2 to the soil, wherein the mass ratio of the applied corn straw biomass charcoal CB300 in the soil is 0.5-1.5%, and the mass ratio of the applied bamboo charcoal BB700 in the soil is 0.4-1%;
in the step S3, the corn straw biomass charcoal CB300 is applied to a position 10-15cm below the surface layer of the soil through a manual turning shovel, and a certain amount of nitrogen fertilizer is applied at the same time, wherein the mass ratio of the corn straw biomass charcoal CB300 to the nitrogen fertilizer is 4: 1-1.5, then applying bamboo charcoal BB700 to a position 12-18cm below the surface layer of soil through an injector, adjusting the daytime temperature to 28-32 ℃, the nighttime temperature to 25-27 ℃ and the humidity to 39-43% in a phytotron greenhouse after applying, keeping the soil in a dry state after 15-20 days, and then performing soil dry-wet alternate management, wherein the soil dry-wet alternate management specifically comprises the following steps:
s3-1, primary water injection: injecting deionized water into the soil, enabling the initial water level to be 2-3cm above the surface of the soil, keeping for 6h, then inserting a water pumping pipe 5cm below the soil to pump water with the liquid level height of 0.5cm, continuously pumping water with the liquid level height of 0.5cm after 12h until no water is accumulated on the surface of the soil, at the moment, the soil is in a wet and partially dry state, and keeping field water pumped each time for later use;
s3-2, treating the extracted water: separately treating the field water extracted each time in the step S3-1 in batches, firstly filtering the field water to remove impurities, injecting the field water into an oxidation pond for oxidation treatment, introducing ozone into the oxidation pond and continuously stirring, wherein the introduced ozone amount is 2-5mg/L, the stirring speed is 85-130r/min, and the duration time is 6h, then introducing the field water subjected to oxidation treatment into a glass pipeline filled with pretreated polypropylene-ethylene adsorption resin, and the weight ratio of the field water subjected to oxidation treatment to the polypropylene-ethylene adsorption resin is 60: 1, collecting purified field water at the flow rate of 5L/min to obtain a plurality of parts of purified field water;
s3-3, secondary water injection: after the water injection for one time of step S1-3 is finished for 48 hours, reinjecting the purified field water obtained in the step S3-2, injecting one copy of field water each time, wherein the time interval of each injection is 24 hours, continuously injecting deionized water after all injection is finished to ensure that the water level is kept the same as the initial water level in the step S3-1, and at the moment, the soil is in a flooded state;
s3-4, circulation: repeating the steps of S3-1 primary water injection, S3-2 water extraction treatment and S3-3 secondary water injection for 2 times, and keeping the soil in a flooded state;
s4, secondary application: and (5) continuously applying a microbial nutrient solution to the soil of the marsh crop farmland to which the corn straw biomass charcoal CB300 and the bamboo charcoal BB700 are applied 60-90 days after the step S3 is finished, and continuously culturing for 150 days to observe the content of the Polycyclic Aromatic Hydrocarbons (PAHs) in the soil.
2. The method for remediating organic pollutants in farmland soil through biochar combined biodegradation according to claim 1, wherein the drying temperature in the oven in the steps S1 and S2 is 70-80 ℃.
3. The method for remedying the organic pollutant in the farmland soil through the biochar combined biodegradation according to the claim 1, wherein the growth years of the wild alpine moso bamboo obtained in the step S2 are 3-5 years.
4. The method for remedying the organic pollutants in the farmland soil through the biochar combined biodegradation according to claim 1, wherein the mass ratio of the wild alpine moso bamboo to the biomass degradation liquid in the step S2 is 1: 3.
5. the method for remediating organic pollutants in farmland soil through biochar combined biodegradation according to claim 1, wherein the mass concentration of the calcium hydroxide solution in the step S2-5 is 60 wt%.
6. The method for remediating organic pollutants in farmland soil through biochar combined biodegradation according to claim 1, wherein the marsh crop in the step S3 is rice.
7. The method for remediating organic pollutants in farmland soil through biochar combined biodegradation according to claim 1, wherein the mass content percentage of each component in the microbial nutrient solution in the step S4 is as follows: 3-5% of urea, 0.5-1% of amino acid, 1-2% of starch, 2-3% of glucose, 0.5-2% of chitosan and the balance of water.
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