CN113526662A - Preparation method and application of novel quinone mediator material - Google Patents
Preparation method and application of novel quinone mediator material Download PDFInfo
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- CN113526662A CN113526662A CN202110873196.5A CN202110873196A CN113526662A CN 113526662 A CN113526662 A CN 113526662A CN 202110873196 A CN202110873196 A CN 202110873196A CN 113526662 A CN113526662 A CN 113526662A
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/28—Anaerobic digestion processes
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F2003/001—Biological treatment of water, waste water, or sewage using granular carriers or supports for the microorganisms
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F2003/001—Biological treatment of water, waste water, or sewage using granular carriers or supports for the microorganisms
- C02F2003/003—Biological treatment of water, waste water, or sewage using granular carriers or supports for the microorganisms using activated carbon or the like
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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
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
Abstract
The invention discloses a preparation method and application of a novel quinone mediator material. The invention takes the sewage plant residual sludge-based biochar as a carrier, and the anthraquinone compound is connected to the surface of the biochar in a chemical bond combination mode, so that the loaded anthraquinone compound is not easy to fall off from the surface of the biochar, has high stability and can be recycled. The loaded material is applied to an anaerobic bioreactor to catalyze the anaerobic biotransformation of pollutants, so that the treatment efficiency is improved. The preparation method provided by the invention has the advantages of simple process, strong adaptability, large-scale production, realization of resource utilization of excess sludge, and high efficiency of treatment of printing and dyeing wastewater.
Description
Technical Field
The invention belongs to the field of sewage treatment and sewage treatment materials, and particularly relates to a preparation method and application of a novel quinone mediator material.
Background
With the development of economy, the printing and dyeing industry has a very important position in the world economy and daily life. But at the same time, a large amount of colored printing and dyeing wastewater is generated, and the discharge of the printing and dyeing wastewater poses great threat to the water environment. Azo dyes are one of dyes, and because molecules contain azo-N ═ N-chromophoric groups, the azo dyes are named as azo dyes, have wide color spectrum, uniform variety, high yield and wide application and are positioned at the head of various dyes, and if wastewater containing reactive azo dyes can be effectively treated, the problem of treating most of dye wastewater is easily solved.
The biological method is the most widely applied method for treating printing and dyeing wastewater at present, particularly the anaerobic and aerobic combined process is the most effective method for treating the wastewater, and the reduction broken bond reaction becomes the rate-limiting step of the whole mineralization process of the azo dye due to the lower oxidation-reduction potential and the complex structure and space obstruction of dye molecules. Therefore, the transfer of the azo dye from the reduction donor from the initial electron donor (co-metabolite) to the final electron acceptor is generally the controlling step in the anaerobic reduction of azo dyes.
Certain quinone group containing compounds are effective in accelerating the bioreductive conversion process of azo dyes. The redox mediator containing quinone group has high water solubility, and is easy to eliminate with water after being added directly into the reaction system, resulting in secondary pollution and high cost.
Disclosure of Invention
Aiming at the current situation, the invention provides a preparation method and application of a novel quinone mediator material, aiming at loading a soluble quinone mediator in a non-soluble carrier material to prepare the novel quinone mediator material, wherein the non-soluble carrier material is biochar prepared from excess sludge.
In order to achieve the technical purpose, the invention provides the following technical scheme:
a method of preparing a quinone mediator material, the method comprising the steps of:
dipping the pretreated sludge-based biochar in a hydrochloric acid solution containing zinc chloride for modification, taking out after standing reaction, cleaning to be neutral, and drying to obtain modified sludge-based biochar;
adding the modified sludge-based biochar into an anthraquinone compound solution for reaction, cleaning the surface of the modified sludge-based biochar, and drying to obtain the quinone mediator material.
Further, the sludge-based biochar is prepared by drying the residual sludge subjected to gravity concentration, pyrolyzing at high temperature under the condition of air isolation, cooling, grinding and sieving.
Further, the residual sludge is concentrated by gravity at 4 ℃ and dried at 40-60 ℃.
Further, the high-temperature pyrolysis conditions are as follows: putting the sludge-based biochar into a tubular furnace, and pyrolyzing for 60-180min at the temperature of 350-950 ℃ in the atmosphere of carbon dioxide and nitrogen gas.
Further, grinding the cooled sludge-based biochar until the cooled sludge-based biochar passes through a 1-2mm sieve.
Further, the pretreatment is to use deionized water to clean the surface of the sludge-based biochar to be neutral and then dry the biochar.
Further, the content of zinc chloride in the hydrochloric acid solution is 250g/L, and the mass fraction of the hydrochloric acid is 37%.
Further, the modification conditions are as follows: the temperature is 25-35 ℃, and the time is 36-48 h.
Further, the anthraquinone compound is anthraquinone 2 sodium sulfonate (AQS), and the concentration of the solution is 1000 mg/L. The anthraquinone compounds may also be benzoquinone, anthraquinone and naphthoquinone compounds containing sulfonate groups.
The reaction is carried out in a shaking table at the temperature of 25-35 ℃ and the rotating speed of 80-120rpm for 48 h. The drying temperature is 40-60 ℃.
The invention also discloses application of the quinone mediator material obtained by the preparation method in a dye wastewater treatment technology.
Compared with the prior art, the invention has the beneficial effects that:
the invention provides a preparation method of a novel quinone mediator material, which adopts sludge biochar prepared by taking excess sludge as a substrate and modifies the surface of the sludge biochar so that the biochar has higher surface loading performance, a more developed void structure and more surface functional groups and provides an effective material for biological treatment for treating azo dye pollution. For sewage treatment facilities, the treatment cost of excess sludge accounts for about 20-30% of the operation cost of the sewage treatment facilities, so that the preparation of the excess sludge into a biochar material to improve the operation treatment effect of sewage plants is an ideal treatment mode of energy internal circulation.
The method adopts a pretreatment mode of hydrochloric acid solution containing zinc chloride to improve the efficiency of loading the anthraquinone compound on the sludge-based biochar, thereby realizing strong biocatalysis efficiency, and the main action mechanism is that chlorine atoms replace hydroxyl functional groups (-OH) on the surface of the biochar to form chlorine substituent groups, and then sulfonic groups in anthraquinone 2 sodium sulfonate are combined with the chlorine substituent groups to form a covalent structure, so that the stability is high. The anthraquinone 2 sodium sulfonate can effectively avoid secondary pollution after being fixed on the biochar, can be recycled, has excellent economy and environmental friendliness, has excellent mechanical properties, can be used as a filler to be placed in a bioreactor, and can strengthen the anaerobic biological treatment effect of azo dyes.
The preparation method provided by the invention has the advantages of simple process, strong adaptability, large-scale production, realization of resource utilization of excess sludge, and high efficiency of treatment of printing and dyeing wastewater.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings needed in the embodiments will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and it is obvious for those skilled in the art to obtain other drawings without creative efforts.
FIG. 1 is a Fourier transform infrared spectrum of a modified sludge-based biochar and quinone mediator material prepared in example 1;
FIG. 2 is a scanning electron microscope image of the surface of the modified sludge-based biochar and quinone mediator material prepared in example 1;
FIG. 3 is an X-ray diffraction pattern of the modified sludge-based biochar and quinone mediator material prepared in example 1;
FIG. 4 is a graph showing the measurement of electron transfer capacity of the modified sludge-based biochar and quinone mediator materials prepared in example 1;
FIG. 5 illustrates the use of the quinone mediator material prepared in example 1 for anaerobic biological treatment of reactive Red 2 in a bioreactor (AnSBR);
FIG. 6 is an illustration of the use of the quinone mediator material prepared in example 1 for anaerobic biological treatment of reactive Red 2 dye in an upflow fixed bed biofilm reactor (UAFB).
Detailed Description
Reference will now be made in detail to various exemplary embodiments of the invention, the detailed description should not be construed as limiting the invention but as a more detailed description of certain aspects, features and embodiments of the invention.
It is to be understood that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention. Further, for numerical ranges in this disclosure, it is understood that each intervening value, between the upper and lower limit of that range, is also specifically disclosed. Every smaller range between any stated value or intervening value in a stated range and any other stated or intervening value in a stated range is encompassed within the invention. The upper and lower limits of these smaller ranges may independently be included or excluded in the range.
Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs. Although only preferred methods and materials are described herein, any methods and materials similar or equivalent to those described herein can be used in the practice or testing of the present invention. All documents mentioned in this specification are incorporated by reference herein for the purpose of disclosing and describing the methods and/or materials associated with the documents. In case of conflict with any incorporated document, the present specification will control.
It will be apparent to those skilled in the art that various modifications and variations can be made in the specific embodiments of the present disclosure without departing from the scope or spirit of the disclosure. Other embodiments will be apparent to those skilled in the art from consideration of the specification. The specification and examples are exemplary only.
As used herein, the terms "comprising," "including," "having," "containing," and the like are open-ended terms that mean including, but not limited to.
Example 1
Taking the residual sludge back, concentrating at 4 deg.C for 24 hr, drying at 60 deg.C, weighing 20g dry sludge, placing in crucible boat, and pyrolyzing in pyrolysis furnace with CO as environmental gas2The flow rate is 0.8L/min, the heating rate is 5 ℃/min, the temperature is 550 ℃, the temperature is reduced to room temperature, and then the sludge-based biochar is ground through a sieve of 1-2mm to obtain the sludge-based biochar.
And cleaning the prepared sludge-based biochar to be neutral by deionized water, and drying for 24h at the temperature of 60 ℃. Weighing 5g of sludge-based biochar, soaking the sludge-based biochar in 50mL of hydrochloric acid with the mass fraction of 37%, wherein the content of zinc chloride in a hydrochloric acid solution is 250g/L, the reaction condition is 30 ℃, standing for 48 hours, separating the sludge-based biochar from the hydrochloric acid solution containing the zinc chloride after the reaction is finished, repeatedly washing the sludge-based biochar to be neutral by using deionized water, and drying at the temperature of 60 ℃ to obtain the modified sludge-based biochar.
And (2) placing the modified sludge-based biochar in a sodium anthraquinone 2 sulfonate solution with the concentration of 1000mg/L, carrying out reaction in a shaking table under the conditions of 30 ℃, 120rpm and 48 hours, washing the surface to be neutral by deionized water after the reaction is finished, and drying at the temperature of 60 ℃ to obtain the quinone mediator material.
FIG. 1 is a Fourier transform infrared spectrum of the modified sludge-based biochar and quinone mediator material prepared in this example. As can be seen from the figure, the modified sludge-based biochar and the quinone mediator material are both in the range of 3420-3440cm-1、1700-1750cm-1、1630-1650cm-1And 1420--1There appeared characteristic peaks representing oxygen-containing functional groups (carboxyl, aldehyde, ketone and quinonyl groups), respectively, at 1215cm-1Is sulfonic group (-SO) in anthraquinone 2 sodium sulfonate3) The characteristic peak of the anthraquinone 2 sodium sulfonate shows that the anthraquinone 2 sodium sulfonate is successfully loaded on the surface of the biochar.
FIG. 2 is a scanning electron microscope image of the surface of the modified sludge-based biochar and quinone mediator materials prepared in this example. The surface of the modified sludge-based biochar is rough, the surface morphology presents a granular structure, the granular structure of the surface of the material loaded with the quinone mediator becomes smaller, the surface becomes rougher, and a pore structure appears, which shows that the modified sludge-based biochar provides a more favorable surface structure for the loading of the quinone mediator.
FIG. 3 is an X-ray diffraction pattern of the modified sludge-based biochar and quinone mediator materials prepared in this example. As can be seen from the figure, the quinone (531.2eV), the carbonyl (532.5eV), the hydroxyl (533.7eV) and the carboxyl (534.3-535.4eV) have oscillation peaks, after the anthraquinone is loaded, the contents of the carboxyl, the hydroxyl, the carbon and the quinone on the surface of the quinone-based material are respectively 3.35%, 2.73%, 47.21% and 46.70%, the contents of the corresponding groups on the surface of the modified sludge-based biochar are respectively 3.90%, 27.54%, 43.98% and 24.58%, the contents of the quinone and the carbonyl on the surface of the modified sludge-based biochar are respectively increased by 47.34 and 6.83% after the anthraquinone 2 sodium sulfonate is loaded, and the content of the hydroxyl after the loading is reduced by 90.05%, which shows that the anthraquinone 2 sodium sulfonate is loaded on the surface of the modified sludge-based biochar and replaces the original hydroxyl structure.
FIG. 4 is a graph showing the electron transfer capacity measurements for biochar and quinone mediator materials prepared in this example. As can be seen from the figure, the electron gaining capacity of the biochar is 0.528 and 0.972mmole before the anthraquinone 2 sodium sulfonate is loaded-g-1Electron capacities of 0.269 and 0.760mmole, respectively-g-1After the anthraquinone 2 sodium sulfonate is loaded, the electronic capacity and the electron donating capacity are respectively improved by 45.68 percent and 64.61 percent. The electron gaining and losing capacity of the biochar before and after loading is the sum of the absolute values of the electron gaining capacity and the electron losing capacity, the sum of the absolute values of the electron gaining capacity and the electron losing capacity is 0.937 and 2.114 respectively, the electron gaining and losing capacity is improved by 55.68 percent, and the quinone mediator material has good electron transfer capacity.
Test example 1
And (3) testing the treatment effect of the biochar-based anthraquinone (BC-AQS) mediator on the reactive red 2 dye wastewater. The quinone mediator material prepared in example 1 is placed into an anaerobic sequencing batch reactor (AnSBR) (as shown in figure 5), stirring blades are arranged at the middle lower part of the reactor, the quinone mediator material is added into the reactor and naturally sinks to the bottom, the adding concentration is 20g/L, the particle size is 1-2mm, pre-acclimated anaerobic flocculent sludge (MLSS is 4000mg/L) is added into a reaction system, a water outlet is arranged at the lower part of the side of the reactor, a water inlet is arranged at the upper part of the side of the reactor, an exhaust hole and a sampling port are arranged at the top of the reactor, and the sampling port extends to the position below the reaction liquid level to realize the water sealing function. The hydraulic retention time of the reactor is 24h, the water is drained for 10min, the water is filled for 10min, the sedimentation is carried out for 30min, the rest time is the mixing and stirring in the reaction system, the stirring speed is 30rpm, and the temperature is controlled at 30 ℃. The quinone mediator material is naturally deposited inside the reaction system, and has no requirement on AnSBR structure, so that the application method has wide application foreground in sewage treating facility upgrading and reconstruction. The comparison result of the biodegradation experiment on the active red 2 during the actual operation of the reactor shows that when the inlet water concentration of the active red 2 is 100-400mg/L, the average decolorization rates of the quinone mediator material added in the reaction system and the quinone mediator material not added are 81-92% and 22-39% respectively, which indicates that the biochar-based quinone mediator material can enhance the biological treatment of azo dyes and can remarkably accelerate the extracellular electron transfer process of microorganisms on the surface of the biochar-based quinone mediator material.
Test example 2
The quinone mediator material prepared in example 1 was placed in an upflow fixed bed biofilm reactor (UAFB) for biological treatment experiments with reactive red 2 dye (as shown in fig. 6). The UAFB reactor bottom that uses is equipped with the water inlet, upper portion is equipped with the venthole, the side top is the delivery port, side upper portion is equipped with interior backward flow mouth, the sample connection is for preventing packing layer bottom from blockking up, packing layer bottom is equipped with the cobblestone bed course, the bed course height accounts for about 10% of total bed course, cobblestone upper portion is quinone mediator material packing layer, the packing layer lateral part is equipped with three solid packing sample connection from top to bottom, the sample connection extends to the outside, the sample connection is outside and packing layer middle are equipped with the insulated column, prevent to pack to get into and cause the regional short circuit of treatment in the sample connection, the influence is to the aassessment of quinone mediator packing actual performance, packing layer upper portion is equipped with the ORP electrode, the reactor lateral part is equipped with liquid sample connection. The particle size of the quinone mediator in the filler layer is 2-3mm, after the quinone mediator is filled into a reactor, the filler is inoculated by a sludge beating and film hanging method, the formation time of the biological film is shortened, the anaerobic sludge is anaerobic flocculent sludge which is acclimated in advance, after 7 days of acclimation, the sludge is completely discharged, the acclimation of the biological film is started, the reactor adopts an internal circulation mode to improve the ascending flow rate to 1m/L, the biological film is formed after 15 days of culture, the concentration of influent activated red 2 is 400mg/L, after long-term operation, the removal rate of the reactive system to the activated red 2 can reach 83-95%, and the reactive red 2 has a good decoloration effect.
In conclusion, the biochar material is pretreated by the zinc chloride hydrochloride solution, so that the load rate of the quinone mediator is improved, the treatment of the azo dye is accelerated in an anaerobic biological reaction system, and the treatment of pollutants is promoted while the content of a biological membrane is easily formed on the surface of the material.
Example 2
Taking the residual sludge back, concentrating at 4 deg.C for 24 hr, drying at 40 deg.C, weighing 20g dry sludge, placing in crucible boat, and pyrolyzing in pyrolysis furnace with N as ambient gas2The flow rate is 0.8L/min, the heating rate is 5 ℃/min, and the temperature is 950 ℃. And cooling to room temperature, and grinding the mixture through a sieve with the diameter of 1-2mm to obtain the sludge-based biochar.
And cleaning the prepared sludge-based biochar to be neutral by deionized water, and drying for 24 hours at the temperature of 40 ℃. Weighing 5g of sludge-based biochar, soaking the sludge-based biochar in 50mL of hydrochloric acid with the mass fraction of 37%, wherein the content of zinc chloride in a hydrochloric acid solution is 250g/L, the reaction condition is 35 ℃, standing for 48 hours, separating the sludge-based biochar from the hydrochloric acid solution containing the zinc chloride after the reaction is finished, repeatedly washing the sludge-based biochar to be neutral by using deionized water, and drying at the temperature of 40 ℃ to obtain the modified sludge-based biochar.
Placing the modified sludge-based biochar in naphthoquinone (2-hydroxy-1, 4-naphthoquinone) solution with the concentration of 1000mg/L, carrying out reaction in a shaking table under the conditions of 35 ℃, 120rpm and 48 hours, washing the surface to be neutral by deionized water after the reaction is finished, and drying at 40 ℃ to obtain the quinone mediator material.
The removal rate of reactive red 2 in the UAFB reactor using the quinone mediator material was 93%.
Example 3
Taking the residual sludge back, concentrating at 4 deg.C for 24 hr, drying at 50 deg.C, weighing 20g dry sludge, placing in crucible boat, and pyrolyzing in pyrolysis furnace with N as ambient gas2The flow rate is 0.8L/min, the heating rate is 5 ℃/min, and the temperature is 300 ℃. And cooling to room temperature, and grinding the mixture through a sieve with the diameter of 1-2mm to obtain the sludge-based biochar.
And cleaning the prepared sludge-based biochar to be neutral by deionized water, and drying for 24 hours at the temperature of 50 ℃. Weighing 5g of sludge-based biochar, soaking the sludge-based biochar in 50mL of hydrochloric acid with the mass fraction of 37%, wherein the content of zinc chloride in a hydrochloric acid solution is 250g/L, the reaction condition is 25 ℃, standing for 36h, separating the sludge-based biochar from the hydrochloric acid solution containing the zinc chloride after the reaction is finished, repeatedly washing the sludge-based biochar to be neutral by using deionized water, and drying at the temperature of 50 ℃ to obtain the modified sludge-based biochar.
And (2) placing the modified sludge-based biochar in an anthraquinone solution with the concentration of 1000mg/L, carrying out reaction in a shaking table under the conditions of 25 ℃, 80rpm and 48h, washing the surface to be neutral by deionized water after the reaction is finished, and drying at the temperature of 50 ℃ to obtain the quinone mediator material.
The removal rate of reactive red 2 in the UAFB reactor using the quinone mediator material was 84%.
Comparative example 1
The difference from example 1 is that the modified sludge-based biochar is replaced by sludge-based biochar. The prepared quinone mediator material is put into an upflow fixed bed biofilm reactor (UAFB) to carry out a biological treatment experiment of the reactive red 2 dye, and the result shows that the removal rate of the reactive red 2 is 63 percent, and the removal rate is obviously reduced.
Comparative example 2
The difference from example 1 is that, in the biological treatment experiment of the reactive red 2 dye, the anthraquinone 2 sodium sulfonate solution is directly added into the upflow fixed bed biofilm reactor (UAFB), and the result shows that the removal rate of the reactive red 2 is 98%, but the anthraquinone 2 sodium sulfonate flows out with water, which causes secondary pollution.
Comparative example 3
The difference from example 1 is that the biological treatment experiment of the reactive red 2 dye was carried out in an upflow fixed bed biofilm reactor (UAFB) without the addition of the quinone mediator material, and as a result, the removal rate of the reactive red 2 was found to be 33%, and the removal rate was significantly decreased.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included therein.
Claims (10)
1. A preparation method of a quinone mediator material is characterized by comprising the following steps:
dipping the pretreated sludge-based biochar in a hydrochloric acid solution containing zinc chloride for modification, cleaning to be neutral, and drying to obtain modified sludge-based biochar;
and adding the modified sludge-based biochar into an anthraquinone compound solution for reaction, cleaning and drying to obtain the quinone mediator material.
2. The preparation method according to claim 1, wherein the sludge-based biochar is prepared by drying the residual sludge after gravity concentration, pyrolyzing the dried residual sludge at high temperature under the condition of air isolation, cooling, grinding and sieving.
3. The method according to claim 2, wherein the excess sludge is concentrated by gravity at 4 ℃ and dried at 40-60 ℃.
4. The method according to claim 2, wherein the pyrolysis conditions are: carbon dioxide atmosphere, temperature 300-.
5. The method of claim 2, wherein the cooled sludge-based biochar is ground to pass through a 1-2mm sieve.
6. The method according to claim 1, wherein the pretreatment is drying after washing to neutrality.
7. The preparation method according to claim 1, wherein the content of zinc chloride in the hydrochloric acid solution is 250g/L, and the mass fraction of the hydrochloric acid is 37%.
8. The method according to claim 1, wherein the modification conditions are: the temperature is 25-35 ℃, and the time is 36-48 h.
9. The production method according to claim 1, wherein the anthraquinone compound is sodium anthraquinone-2 sulfonate; the reaction conditions are as follows: the temperature is 25-35 ℃, the rotating speed is 80-120rpm, and the time is 48 h.
10. Use of a quinone mediator material obtained by the method of any one of claims 1 to 9 in a dye wastewater treatment technology.
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| CN114772746A (en) * | 2022-04-06 | 2022-07-22 | 中国海洋大学 | Method for removing soluble organic nitrogen in rainwater runoff |
| CN114772721A (en) * | 2022-04-11 | 2022-07-22 | 中国农业大学 | Method for promoting anaerobic degradation of polycyclic aromatic hydrocarbon in wastewater by using biochar |
| CN114686344A (en) * | 2022-06-06 | 2022-07-01 | 中国农业科学院农业环境与可持续发展研究所 | Methane production system based on recoverable composite mediator enhanced anaerobic digestion |
| CN114920233A (en) * | 2022-07-20 | 2022-08-19 | 中国农业科学院农业环境与可持续发展研究所 | Preparation method and application of quinone-based modified biochar |
| CN114920233B (en) * | 2022-07-20 | 2022-09-30 | 中国农业科学院农业环境与可持续发展研究所 | Preparation method and application of quinone-based modified biochar |
| CN115651140A (en) * | 2022-12-29 | 2023-01-31 | 中国农业科学院农业环境与可持续发展研究所 | Three-dimensional carbon-based copolymerized composite material and preparation method and application thereof |
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Application publication date: 20211022 |