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CN117776166A - Method for preparing graphene quantum dots from retired graphite - Google Patents

Method for preparing graphene quantum dots from retired graphite Download PDF

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Publication number
CN117776166A
CN117776166A CN202410003094.1A CN202410003094A CN117776166A CN 117776166 A CN117776166 A CN 117776166A CN 202410003094 A CN202410003094 A CN 202410003094A CN 117776166 A CN117776166 A CN 117776166A
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graphite
solution
graphene quantum
quantum dots
retired
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CN117776166B (en
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侯红帅
罗定中
纪效波
邹国强
邓文韬
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Central South University
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Central South University
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    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02WCLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00Technologies for solid waste management
    • Y02W30/50Reuse, recycling or recovery technologies
    • Y02W30/84Recycling of batteries or fuel cells

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Abstract

The invention relates to a method for preparing graphene quantum dots by retired graphite, which comprises the following steps: ball milling and activating the retired graphite to obtain activated retired graphite; adding activated retired graphite into a mixed solution of concentrated nitric acid and concentrated sulfuric acid to uniformly disperse graphite, and then carrying out hydrothermal reaction in a closed reaction container while stirring; after the reaction is completed, cooling to room temperature, diluting the solution in the reaction container with deionized water, adding hot alkali solution to make the solution neutral, centrifuging, performing solid-liquid separation, removing unreacted graphite, and collecting a first solution; cooling the collected first solution, performing solid-liquid separation, and collecting a second solution; dialyzing the second solution by using a dialysis bag, and drying the obtained liquid to obtain graphene quantum dots; the method can effectively convert retired graphite into graphene quantum dots, has high conversion rate, avoids pollution of waste graphite to the environment, and realizes high-value recycling of low-value waste resources.

Description

Method for preparing graphene quantum dots from retired graphite
Technical Field
The invention relates to the technical field of waste battery recovery, in particular to a method for preparing graphene quantum dots by retired graphite.
Background
The lithium ion battery is used as a green and environment-friendly secondary power supply, and has been widely applied to the fields of 3C products, electric automobiles and the like by virtue of the characteristics of high energy density, long cycle life, no memory effect and the like. The lithium ion power battery is generally composed of a shell, a positive electrode material, a negative electrode material, an Al/Cu current collector, a diaphragm, electrolyte and the like. Graphite is widely used in negative electrode materials of lithium ion batteries due to its characteristics of good conductivity, high reversible lithium storage capacity, long and stable platform, etc. The lithium ion battery industry rapidly develops and simultaneously generates a large amount of waste graphite, and the contained graphite belongs to solid waste and faces the problems of low recovery economic value and serious environmental pollution. If the waste graphite is made into high-quality graphene quantum dots, the economic benefit of graphite cathode recovery can be improved, and environmental pollution can be avoided. Moreover, the cost of the raw materials of the waste graphite is far lower than that of the high-purity graphite, and the waste graphite is suitable for being used as the raw material for producing the graphene quantum dots. As disclosed in chinese patent 201811358813.2, a method for preparing graphene quantum dots by using waste lithium ion batteries is disclosed, in which, after removing a current collector of a negative plate, the obtained graphite-containing mixed solution is heated and filtered, and then microwave digestion, dialysis and molecular sieve elution are sequentially performed to obtain graphene quantum dots; however, the conversion rate of graphite in the method is low (about 16-18%), which causes a great deal of waste of retired graphite.
Disclosure of Invention
Based on the technical problems in the prior art, the inventor finds that the interlayer spacing of the recycled retired graphite is larger than that of the pure graphite through research, and the recycled retired graphite can be easily oxidized and prepared into uniform graphene quantum dots through a specific method after activation.
In order to achieve the above object, the technical scheme of the present invention is as follows:
a method for preparing graphene quantum dots by retired graphite comprises the following steps:
s1, performing ball milling activation on retired graphite to obtain activated retired graphite;
s2, adding the activated retired graphite into a mixed solution of concentrated nitric acid and concentrated sulfuric acid to uniformly disperse the graphite, and then carrying out hydrothermal reaction in a sealed reaction container while stirring;
s3, after the reaction is completed, cooling to room temperature, diluting the solution in the reaction container by deionized water, adding an alkali solution to make the solution neutral, centrifuging, performing solid-liquid separation, removing unreacted graphite, and collecting a first solution;
s4, cooling the first solution collected in the step S3, performing solid-liquid separation, and collecting a second solution;
and S5, dialyzing the second solution by using a dialysis bag, and drying the obtained liquid to obtain the graphene quantum dots.
In some embodiments, in step S1, during the ball milling process, the ball milling rotational speed is 300-800rpm/min; the ball milling time is 1-6h.
In some embodiments, in step S2, the volume ratio of concentrated nitric acid to concentrated sulfuric acid is 1:2-6.
In some embodiments, the concentrated nitric acid concentration is 65-68%; the concentration of the concentrated sulfuric acid is 95-98%.
In some embodiments, in step S2, the solid to liquid ratio of graphite to mixed solution is 1g:40-80mL.
In some embodiments, in step S2, the hydrothermal reaction temperature is 90-120 ℃; the reaction time is 12-24h.
In some embodiments, in step S3, the base comprises at least one of sodium carbonate, sodium bicarbonate, sodium hydroxide, potassium carbonate, potassium bicarbonate, potassium hydroxide, magnesium hydroxide, zinc hydroxide, magnesium carbonate, lithium carbonate, aqueous ammonia.
In some embodiments, in step S3, a hot sodium carbonate solution is added to the solution, followed by dropwise heating of the sodium hydroxide solution until the solution is neutral; wherein the temperature of the hot sodium carbonate solution is 60-80 ℃, and the concentration of the sodium carbonate solution is as follows: 3.0-3.9mol/L.
In some embodiments, the temperature of the hot sodium hydroxide is 70-90℃and the concentration of sodium hydroxide solution is 45-50mol/L.
In some embodiments, in step S1, the retired graphite is obtained by the following method:
soaking the negative electrode of the waste battery in ethanol, and washing off electrolyte; then soaking with NMP, heating to 70-90 ℃, preserving heat for 4-6 hours, taking out the negative electrode, scraping graphite from the current collector, then putting the graphite into ethanol for ultrasonic treatment, standing and drying after ultrasonic treatment is completed, and obtaining retired graphite.
In some embodiments, graphite is sonicated in ethanol for 1-2 hours, with a resting time of 84-96 hours, with ethanol being exchanged every 12 hours.
In some embodiments, the graphene quantum dots are dried at 90-120 ℃ for 24-48 hours. Compared with the prior art, the invention has the following beneficial effects:
the inventor finds that the layer spacing of the recycled retired graphite is larger than that of pure graphite, based on the fact, the retired graphite is used as a raw material, after being activated, the graphene quantum dots are obtained through oxidation by a specific oxidant and subsequent treatment, high-value recycling of low-value waste resources is achieved, solid waste pollution caused by the waste graphite to the environment is avoided, and the retired graphite is activated before oxidation, so that the conversion rate of the retired graphite is improved, and the yield of the graphene quantum dots can reach more than 58%.
In addition, compared with normal-temperature alkali liquor, the alkali liquor used in the process of neutralizing the acid solution is heated first, the dosage is less, the volume of the waste liquor to be treated is smaller, saturated micromolecular salt can be separated out through cooling, the dialysis time and the water changing times are reduced, and the subsequent treatment procedures are further simplified.
Drawings
Fig. 1 is a TEM image of a graphene quantum dot material prepared in example 1 of the present invention;
fig. 2 is an XRD pattern of the graphene quantum dot material prepared in example 1 of the present invention;
FIG. 3 is an XPS C1s spectrum of the graphene quantum dot material prepared in example 1 of the present invention;
FIG. 4 is an XPS O1s spectrum of the graphene quantum dot material prepared in example 1 of the present invention;
fig. 5 is an FTIR diagram of a graphene quantum dot material prepared in example 1 of the present invention.
Detailed Description
In the following description, numerous specific details are set forth in order to provide a thorough understanding of the present invention. The invention may be embodied in many other forms than described herein and similarly modified by those skilled in the art without departing from the spirit or scope of the invention, which is therefore not limited to the specific embodiments disclosed below.
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. The terminology used herein in the description of the invention is for the purpose of describing particular embodiments only and is not intended to be limiting of the invention.
Example 1
A preparation method for preparing graphene quantum dots from retired graphite comprises the following steps:
firstly, soaking the negative electrode of the waste battery in ethanol for 24 hours, washing off electrolyte, then soaking the negative electrode of the waste battery in NMP (N-methylpyrrolidone) for 12 hours, heating the solution to 80 ℃, preserving heat for 5 hours, then taking out the negative electrode of the waste battery, and scraping graphite from copper foil; placing the waste graphite into ethanol, performing ultrasonic treatment for 2 hours, standing for 84 hours, and replacing the ethanol every 12 hours; picking out the crushed copper foil in the waste graphite, and placing the crushed copper foil in a blast drying oven to be dried for 24 hours at 90 ℃; drying to obtain retired graphite;
ball milling retired graphite at 500rpm/min for 2 hr, and adding concentrated HNO 3 And H 2 SO 4 In the mixed solution (the volume ratio of concentrated nitric acid (68%) to concentrated sulfuric acid (98%) is 1:3, the total volume of the solution is 60 ml), stirring for 30min, and then ultrasonic treatment is carried out for 30min until the retired graphite is uniformly dispersed in the mixed solution; then, the mixed solution is heated to 90 ℃ in a sealed high-pressure reaction kettle, and is stirred at the speed of 300rpm/min for hydrothermal reaction for 24 hours; after the reaction is completed, naturally cooling to room temperature,after dilution with 20mL deionized water (DI), na was used 2 CO 3 (20g) Heating and dissolving in 50mL of deionized water, pouring into the mixed solution to neutralize a part of acid, heating and dissolving in 30mL of water by using NaOH (55 g), and dropwise adding until the pH of the mixed solution is adjusted to be neutral; and after centrifugation and filtration, firstly standing for 24 hours to cool and separate out a large amount of supersaturated salt in the system, then further dialyzing in a dialysis bag to remove small molecular salt, and freeze-drying liquid obtained after dialysis to obtain graphene quantum dot powder.
Through detection, the yield of the graphene quantum dots reaches 58%.
And carrying out TEM test and XRD test on the obtained graphene quantum dot material, wherein the detection results are shown in figures 1 and 2. Fig. 1 is a TEM diagram of the graphene quantum dot material, and fig. 2 is an XRD diagram of the graphene quantum dot material.
As shown in FIG. 1, the graphene quantum dot material obtained in the embodiment has the particle size of 2-5nm, is uniformly distributed, and has no obvious agglomeration phenomenon.
As shown in fig. 2, the diffraction peak at 26.6 ° of the graphite after acid oxidation disappeared, indicating that the two-dimensional structure of the graphite was destroyed, and the graphite was successfully exfoliated to synthesize GQDs.
As shown in fig. 3, the high resolution C1s fine spectrum can be split into three peaks at 284.8, 286.5 and 288.3eV, corresponding to C-C/c= C, C-O and O-c=o bonds, respectively.
As shown in FIG. 4, O1s XPS spectrum showed 4 types of peaks at 531.1, 531.5, 532.4 and 535.6eV belonging to O-C= O, C-O, C-OH and H, respectively 2 O。
The functional groups of GQDs were detected by Fourier infrared transformation (FT-IR). As shown in FIG. 5, 1105 and 1619cm -1 The peaks at which are ascribed to stretching vibrations of the C-O and O-c=o groups; 3433cm -1 The broad absorption band at this point indicates the typical stretching vibration of the hydroxyl groups in GQDs. Thus, it is shown that GQDs formed after oxidative exfoliation contain rich oxygen-containing functional groups.
Example 2
A preparation method for preparing graphene quantum dots from retired graphite comprises the following steps:
firstly, soaking the negative electrode of the waste battery in ethanol for 48 hours, washing off electrolyte, then soaking the negative electrode of the waste battery in NMP (N-methylpyrrolidone) for 24 hours, heating the solution to 90 ℃, preserving heat for 6 hours, then taking out the negative electrode of the waste battery, and scraping graphite from copper foil; putting the waste graphite into ethanol, performing ultrasonic treatment for 2 hours, standing for 96 hours, and changing the ethanol every 12 hours; picking out the crushed copper foil in the waste graphite, and placing the crushed copper foil in a blast drying oven to be dried for 24 hours at 90 ℃; drying to obtain retired graphite;
ball milling retired graphite at 700rpm/min for 2 hr, and adding concentrated HNO 3 And H 2 SO 4 In the mixed solution (the volume ratio of concentrated nitric acid (68%) to concentrated sulfuric acid (98%) is 1:4, the total volume of the solution is 50 ml), stirring for 30min, and then ultrasonic treatment is carried out for 30min until the retired graphite is uniformly dispersed in the mixed solution; then, the mixed solution is heated to 120 ℃ in a sealed high-pressure reaction kettle, and stirred for hydrothermal reaction for 24 hours at the speed of 300 rpm/min; after the reaction was completed, it was naturally cooled to room temperature, diluted with 20mL deionized water (DI), and then first with Na 2 CO 3 (20g) Heating and dissolving in 50mL of deionized water, pouring into the mixed solution to neutralize a part of acid, heating and dissolving in 30mL of water by using NaOH (55 g), and dropwise adding until the pH of the mixed solution is adjusted to be neutral; and after centrifugation and filtration, standing for one day, cooling and separating out a large amount of supersaturated salt in the system, further dialyzing in a dialysis bag to remove small molecular salt, and freeze-drying liquid obtained after dialysis to obtain graphene quantum dot powder.
Through detection, the yield of the graphene quantum dots is 56.7 percent by the method of the embodiment.
The graphene quantum dots obtained by the method have the particle size of 3-8nm, are uniformly distributed and have no obvious agglomeration.
Comparative example 1
A method for preparing graphene quantum dots from ordinary graphite, comprising the following steps:
adding graphite powder into concentrated HNO 3 And H 2 SO 4 In the mixed solution (the volume ratio of the concentrated nitric acid (68%) and the concentrated sulfuric acid (98%) is 1:3, the total volume of the solution is 60 ml),stirring for 30min, and then performing ultrasonic treatment for 30min until the retired graphite is uniformly dispersed in the mixed solution; subsequently, the mixed solution is heated to 90 ℃ in a sealed high-pressure reaction kettle, and is stirred at the speed of 300rpm/min for hydrothermal reaction for 24 hours; after the reaction was completed, it was naturally cooled to room temperature, diluted with 20mL deionized water (DI), and then first with Na 2 CO 3 (20g) Heating and dissolving in 50mL of deionized water, pouring into the mixed solution to neutralize a part of acid, heating and dissolving in 30mL of water by using NaOH (55 g), and dropwise adding until the pH of the mixed solution is adjusted to be neutral; and after centrifugation and filtration, firstly standing for 24 hours to cool and separate out a large amount of supersaturated salt in the system, then further dialyzing in a dialysis bag to remove small molecular salt, and freeze-drying liquid obtained after dialysis to obtain graphene quantum dot powder.
Through detection, the yield of the graphene quantum dots is 25% in the method of the comparative example.
The graphene quantum dots obtained by the method of the comparative example have the particle size of 5-10nm and no obvious agglomeration.
Comparative example 2
A preparation method for preparing graphene quantum dots from retired graphite comprises the following steps:
firstly, soaking the negative electrode of the waste battery in ethanol for 48 hours, washing off electrolyte, then soaking the negative electrode of the waste battery in NMP (N-methylpyrrolidone) for 24 hours, heating the solution to 90 ℃, preserving heat for 6 hours, then taking out the negative electrode of the waste battery, and scraping graphite from copper foil; putting the waste graphite into ethanol, performing ultrasonic treatment for 2 hours, standing for 96 hours, and changing the ethanol every 12 hours; picking out the crushed copper foil in the waste graphite, and placing the crushed copper foil in a blast drying oven to be dried for 24 hours at 90 ℃; drying to obtain retired graphite;
ball milling the retired graphite at a rotating speed of 700rpm/min for 2 hours, and standing for 24 hours;
adding the retired graphite subjected to ball milling and standing into concentrated HNO 3 And H 2 SO 4 In the mixed solution (the volume ratio of concentrated nitric acid (68%) to concentrated sulfuric acid (98%) is 1:3, the total volume of the solution is 60 ml), stirring for 30min, and then ultrasonic treatment is carried out for 30min until the retired graphite is uniformly dispersed in the mixed solution; the mixed solution is then subjected to a high pressure in a sealHeating to 120 ℃ in a reaction kettle, and stirring for hydrothermal reaction for 24 hours at the speed of 300 rpm/min; after the reaction was completed, it was naturally cooled to room temperature, diluted with 20mL deionized water (DI), and then first with Na 2 CO 3 (20g) Heating and dissolving in 50mL of deionized water, pouring into the mixed solution to neutralize a part of acid, heating and dissolving in 30mL of water by using NaOH (55 g), and dropwise adding until the pH of the mixed solution is adjusted to be neutral; and after centrifugation and filtration, standing for one day, cooling and separating out a large amount of supersaturated salt in the system, further dialyzing in a dialysis bag to remove small molecular salt, and freeze-drying liquid obtained after dialysis to obtain graphene quantum dot powder.
Through detection, the yield of the graphene quantum dots is 48.7%.
The graphene quantum dots obtained by the method have the particle size of 3-9nm, are uniformly distributed and have no obvious agglomeration.
Comparative example 3
A preparation method for preparing graphene quantum dots from retired graphite comprises the following steps:
firstly, soaking the negative electrode of the waste battery in ethanol for 24 hours, washing off electrolyte, then soaking the negative electrode of the waste battery in NMP (N-methylpyrrolidone) for 12 hours, heating the solution to 80 ℃, preserving heat for 5 hours, then taking out the negative electrode of the waste battery, and scraping graphite from copper foil; placing the waste graphite into ethanol, performing ultrasonic treatment for 2 hours, standing for 84 hours, and replacing the ethanol every 12 hours; picking out the crushed copper foil in the waste graphite, and placing the crushed copper foil in a blast drying oven to be dried for 24 hours at 90 ℃; drying to obtain retired graphite;
ball milling retired graphite at 500rpm/min for 2 hr, and adding concentrated HNO 3 And H 2 SO 4 In the mixed solution (the volume ratio of concentrated nitric acid (68%) to concentrated sulfuric acid (98%) is 1:3, the total volume of the solution is 60 ml), stirring for 30min, and then ultrasonic treatment is carried out for 30min until the retired graphite is uniformly dispersed in the mixed solution; then, heating the mixed solution to 90 ℃ in a sealed high-pressure reaction kettle, and carrying out hydrothermal reaction for 24 hours; after the reaction was completed, it was naturally cooled to room temperature, diluted with 20mL deionized water (DI), and then first with Na 2 CO 3 (20g) Heating and dissolving in 50mLPouring ionized water into the mixed solution to neutralize a part of acid in the mixed solution, heating and dissolving the mixed solution in 30mL of water by using NaOH (55 g), and dropwise adding until the pH value of the mixed solution is adjusted to be neutral; and after centrifugation and filtration, firstly standing for 24 hours to cool and separate out a large amount of supersaturated salt in the system, then further dialyzing in a dialysis bag to remove small molecular salt, and freeze-drying liquid obtained after dialysis to obtain graphene quantum dot powder.
Through detection, the yield of the graphene quantum dots is 42%.
The graphene quantum dots obtained by the method have the particle size of 4-9nm, are uniformly distributed and have no obvious agglomeration.
The technical features of the above-described embodiments may be arbitrarily combined, and all possible combinations of the technical features in the above-described embodiments are not described for brevity of description, however, as long as there is no contradiction between the combinations of the technical features, they should be considered as the scope of the description.
The above examples illustrate only a few embodiments of the invention, which are described in detail and are not to be construed as limiting the scope of the invention. It should be noted that it will be apparent to those skilled in the art that several variations and modifications can be made without departing from the spirit of the invention, which are all within the scope of the invention. Accordingly, the scope of protection of the present invention is to be determined by the appended claims.

Claims (10)

1.一种退役石墨制备石墨烯量子点的方法,其特征在于,包括以下步骤:1. A method of preparing graphene quantum dots from decommissioned graphite, characterized by comprising the following steps: S1、将退役石墨进行球磨活化后,得到活化退役石墨;S1. After ball milling and activating the retired graphite, the activated retired graphite is obtained; S2、将所述活化退役石墨加入浓硝酸和浓硫酸的混合溶液中,使石墨分散均匀,然后在密封反应容器中边搅拌边进行水热反应;S2. Add the activated decommissioned graphite into a mixed solution of concentrated nitric acid and concentrated sulfuric acid to disperse the graphite evenly, and then perform a hydrothermal reaction while stirring in a sealed reaction vessel; S3、反应完成后,冷却至室温,然后用去离子水稀释反应容器中的溶液,接着加入热碱溶液使溶液呈中性,离心,固液分离,去除未反应的石墨,收集第一溶液;S3. After the reaction is completed, cool to room temperature, then dilute the solution in the reaction vessel with deionized water, then add hot alkali solution to make the solution neutral, centrifuge, separate solid and liquid, remove unreacted graphite, and collect the first solution; S4、将步骤S3收集的第一溶液进行冷却,析出用热碱中和后的过饱和盐,固液分离,收集第二溶液;S4. Cool the first solution collected in step S3, precipitate the supersaturated salt neutralized with hot alkali, separate the solid and liquid, and collect the second solution; S5、将第二溶液用透析袋透析,得到的液体干燥后,得到石墨烯量子点。S5. Dialyze the second solution with a dialysis bag, and dry the obtained liquid to obtain graphene quantum dots. 2.根据权利要求1所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S1中,球磨过程中,球磨转速为300-800rpm/min;球磨时间为1-6h。2. The method for preparing graphene quantum dots from decommissioned graphite according to claim 1, characterized in that in step S1, during the ball milling process, the ball milling speed is 300-800rpm/min; the ball milling time is 1-6h. 3.根据权利要求1所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S2中,浓硝酸和浓硫酸的体积比为1:2-6。3. The method for preparing graphene quantum dots from decommissioned graphite according to claim 1, characterized in that in step S2, the volume ratio of concentrated nitric acid and concentrated sulfuric acid is 1:2-6. 4.根据权利要求1所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S2中,石墨和混合溶液的固液比为1g:40-80mL。4. The method for preparing graphene quantum dots from decommissioned graphite according to claim 1, characterized in that in step S2, the solid-liquid ratio of graphite and mixed solution is 1g:40-80mL. 5.根据权利要求1所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S2中,水热反应温度为90-120℃;反应时间为12-24h。5. The method for preparing graphene quantum dots from decommissioned graphite according to claim 1, characterized in that in step S2, the hydrothermal reaction temperature is 90-120°C; the reaction time is 12-24h. 6.根据权利要求1所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S3中,所述碱包括碳酸钠、碳酸氢钠、氢氧化钠、碳酸钾、碳酸氢钾、氢氧化钾、氢氧化镁、氢氧化锌、碳酸镁、碳酸锂、氨水中的至少一种。6. The method for preparing graphene quantum dots from decommissioned graphite according to claim 1, characterized in that, in step S3, the alkali includes sodium carbonate, sodium bicarbonate, sodium hydroxide, potassium carbonate, potassium bicarbonate, hydrogen At least one of potassium oxide, magnesium hydroxide, zinc hydroxide, magnesium carbonate, lithium carbonate, and ammonia. 7.根据权利要求1所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S3中,先用热碳酸钠溶液加入溶液中,接着滴加热氢氧化钠溶液直至溶液呈中性;其中,热碳酸钠溶液的温度为60-80℃,碳酸钠溶液的浓度为:3.0-3.9mol/L;和/或,热氢氧化钠的温度为70-90℃,氢氧化钠溶液的浓度为45-50mol/L。7. The method for preparing graphene quantum dots from decommissioned graphite according to claim 1, characterized in that in step S3, hot sodium carbonate solution is first added to the solution, and then the sodium hydroxide solution is heated dropwise until the solution becomes neutral; Wherein, the temperature of the hot sodium carbonate solution is 60-80°C, and the concentration of the sodium carbonate solution is: 3.0-3.9mol/L; and/or, the temperature of the hot sodium hydroxide solution is 70-90°C, and the concentration of the sodium hydroxide solution is is 45-50mol/L. 8.根据权利要求1所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S4中,将收集的第一溶液进行冰水浴冷却,冰水浴的温度为3-10℃,冰水浴时间为6-10h。8. The method for preparing graphene quantum dots from decommissioned graphite according to claim 1, characterized in that in step S4, the collected first solution is cooled in an ice-water bath, and the temperature of the ice-water bath is 3-10°C. The time is 6-10h. 9.根据权利要求1-7任一项所述的退役石墨制备石墨烯量子点的方法,其特征在于,步骤S1中,退役石墨由以下方法得到:9. The method for preparing graphene quantum dots from decommissioned graphite according to any one of claims 1 to 7, characterized in that, in step S1, decommissioned graphite is obtained by the following method: 将废弃电池的负极放入乙醇中浸泡,洗去电解液;然后用NMP浸泡后,升温至70-90℃,保温4-6h后取出负极,将石墨从集流体上刮下来,然后放入乙醇中超声,超声完成后,静置,干燥,得到退役石墨。Soak the negative electrode of the discarded battery in ethanol to wash away the electrolyte; then soak it in NMP, heat it to 70-90°C, keep it warm for 4-6 hours, take out the negative electrode, scrape the graphite from the current collector, and put it in ethanol Ultrasonic in medium. After the ultrasonic is completed, let it stand and dry to obtain retired graphite. 10.根据权利要求9所述的退役石墨制备石墨烯量子点的方法,其特征在于,将石墨放入乙醇中超声1-2h,静置时间为84-96h,每隔12h换一次乙醇。10. The method for preparing graphene quantum dots from decommissioned graphite according to claim 9, characterized in that the graphite is placed in ethanol and ultrasonicated for 1-2 hours, the standing time is 84-96 hours, and the ethanol is replaced every 12 hours.
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