CN116789123A

CN116789123A - Method for preparing graphene

Info

Publication number: CN116789123A
Application number: CN202210242118.XA
Authority: CN
Inventors: 杨盛贤
Original assignee: Qujing Huajin Rainforest Technology Co ltd
Current assignee: Qujing Huajin Rainforest Technology Co ltd
Priority date: 2022-03-13
Filing date: 2022-03-13
Publication date: 2023-09-22

Abstract

The invention discloses a preparation method of graphene, and belongs to the technical field of nano materials. According to the method, firstly, a reducing agent is added into graphene oxide solution, reduction is carried out by a chemical method, then the reduced product is dispersed, and finally, various impurities are removed through filtration and replacement of different solvents (liquids), so that graphene is uniformly dispersed in various solvents (liquids). The method has the advantages that the graphene is uniformly dispersed in various solvents (liquids), various impurities in the graphene are removed efficiently, and the preparation cost of the graphene is reduced. The graphene prepared by the method has the advantages of high purity, good dispersion uniformity, good dispersion stability, high repeatability and possibility of application and popularization.

Description

Method for preparing graphene

Technical Field

The invention belongs to the technical field of new material preparation, and particularly provides a method for preparing graphene.

Background

Graphene is a single-layer two-dimensional material composed of closely packed carbon atoms. The carbon atom having 4 valence electrons, 3 of which are sp ² The hybridization forms sigma bond, the sigma bond is connected with other three carbon atoms to form a hexagonal structure, and the 4 th non-bonded electron forms pi bond perpendicular to the plane. Based on the crystal structure of graphene, the graphene has particularly excellent optical, electrical and mechanical properties, such as super-strong mechanical properties, extremely high carrier mobility, extremely high heat conduction performance, good optical properties and the like.

Although graphene has many excellent characteristics, two problems exist in practical application, namely, how to uniformly disperse graphene in various solvents (liquids); and secondly, how to purify the prepared graphene.

Graphene is easy to agglomerate, cannot be dispersed in water, cannot be widely dispersed in various organic solutions, can be only dispersed in a small amount of N, N-dimethylformamide and N-methylpyrrolidone in an unstable manner, can be hardly dispersed in other solutions, and the difficulty in dispersion greatly limits the application. The reason why graphene is difficult to disperse in a solution is that pi-pi action between carbon atoms and van der waals force between sheets make it difficult to disperse graphene, and agglomeration is an inherent property of graphene. Graphene is easily agglomerated in different systems, resulting in a number of properties that are excellent on the nanoscale that are significantly reduced or even vanished with the agglomeration of graphene sheets. Therefore, developing a solution in which graphene is uniformly dispersed in different solvents (liquids) is of great importance, and is an important condition for promoting application and development of graphene.

The existing solution is to modify graphene, and disperse the modified graphene in a solution, so that different application systems generally have different characteristics, and the graphene needs to be modified in a targeted manner. The common modification means are: covalent bond modification, non-covalent bond modification, surfactant addition, and the like. However, the modification can reduce the performance of the graphene, and new impurities can be introduced, so that the pure unmodified graphene has the best performance.

A large amount of impurities can be introduced in the preparation process of the graphene, the quality of the graphene can be reduced by residual impurities, the subsequent application is seriously influenced, and the difficulty in purification is always a great difficulty in preventing the application of the graphene. In the preparation of graphene, graphene oxide is generally produced by using reagents such as graphite powder, sulfuric acid, nitrate, chlorate, potassium permanganate, hydrochloric acid, phosphoric acid and the like, and the graphene oxide is reduced to obtain graphene. Elements such as sodium, potassium, manganese, sulfur, nitrogen, chlorine, phosphorus and the like are inevitably introduced into the graphene, and a large amount of residual reducing agent is also introduced. It is very difficult to remove impurity elements such as sodium, potassium, manganese, sulfur, nitrogen, chlorine, phosphorus, etc. and residual reducing agents in graphene. Many downstream applications have high purity requirements for graphene, and the impurity content in graphene needs to be strictly controlled, so purification is of great importance.

The common purification modes include centrifugation, dialysis, filtration and the like, but all have defects of different degrees. Comprising the following steps: incomplete impurity removal, more residual impurities, long time, more water consumption, complicated working procedures and high purification cost. The centrifugation has the advantages that the pH value is low in the initial stage, the impurity content is high, the centrifugation layering is easy, the pH value is increased in the later stage, the solution is not easy to delaminate, the impurities cannot be effectively separated from graphene, a plurality of impurity ions are arranged in graphene oxide sheets, the graphene cannot be rapidly centrifugally separated, and the large-scale high-speed centrifuge cannot be used for purifying the graphene in a long-term and large-scale centrifugation manner in industry. The dialysis has the advantages of long time, large amount of consumed pure water, frequent replacement of dialysis medium, high cost and limitation of large-scale production of graphene oxide. The filter cake can block the flow of the solution, and has the advantages of low speed, long time, low efficiency, high cost, complex process and incapability of thoroughly removing impurities. In addition, the reducing agent added during the reduction process, as well as the manner of modification and addition of the surfactant, also faces difficulties in removing the residual reagent, and in secondary purification.

Therefore, based on the prior art, a person skilled in the art needs to research an efficient, convenient and low-cost method, and the following two points are achieved in the process of preparing graphene: (1) So that the graphene is uniformly dispersed in various solvents (liquids); and (2) efficiently removing various impurities in the graphene.

Disclosure of Invention

Aiming at the defects of the prior art, the invention aims to provide a method for preparing graphene, which simultaneously achieves the following two points in the process of preparing graphene: (1) So that the graphene is uniformly dispersed in various solvents (liquids); and (2) efficiently removing various impurities in the graphene.

The specific principle of action of the invention is as follows.

The principle of uniformly dispersing graphene in a solution is as follows: (1) After chemical reduction, unreacted reducing agent, chemical reduction products and other small molecules are adsorbed on the surface of the graphene through interactions of hydrogen bonds, van der Waals forces, intermolecular forces and the like, so that the graphene is uniformly dispersed in the solution; (2) After chemical reduction, adding a dispersing agent into the graphene solution, wherein the dispersing agent has a dispersing effect in the presence of one or more of the following independent existence or simultaneous existence: the first case is that the dispersing agent reacts with various chemical substances in the graphene solution after chemical reduction to generate gas, the second case is that the dispersing agent is decomposed to generate gas, and the third case is that a plurality of dispersing agents react with each other to generate gas. The generated gas is one or a mixture of several gases: oxygen, carbon dioxide, nitrogen, ammonia, hydrogen, ozone, fluorine, chlorine, bromine, nitrogen monoxide, nitrogen dioxide, chlorine dioxide. The generated gas is adsorbed on the surface of the graphene, so that agglomeration is avoided, and the graphene is kept uniformly dispersed in the solution; (3) After the dispersing agent is added, substances which keep the graphene uniformly dispersed become gas and various small molecules.

The principle of removing impurities in graphene is as follows: the gas adsorbed on the surface keeps the dispersion of the graphene, and the solvent (liquid) can smoothly flow through the inner space of the material, so that various impurities in the solution are taken away during filtration, and the impurities in the graphene solution are removed. Removed impurities include, but are not limited to: (1) impurities contained in graphite powder; (2) The preparation method comprises the steps of introducing sodium, potassium, manganese, sulfur, nitrogen, chlorine, phosphorus and other impurity elements into reagents such as sulfuric acid, nitrate, chlorate, potassium permanganate, hydrochloric acid, phosphoric acid and the like used in the preparation of graphene oxide; (3) unreacted reducing agent, chemical reduction product; (4) impurities introduced in preparing the graphene solution. The method is simple, quick and efficient, and is beneficial to reducing the production cost of graphene.

The invention can lead the graphene to be evenly dispersed in different solvents (liquid) according to the following principle: the solution in which graphene is uniformly dispersed in the first solvent (liquid) is replaced with the second solvent (liquid) by utilizing the mutual solubility of the solvents (liquids), and a solution in which graphene is uniformly dispersed in the second solvent (liquid) is obtained.

The principle of the invention for adjusting the concentration of the graphene solution is as follows: for the uniformly dispersed graphene solution, a certain amount of solvent (liquid) is newly added, or the excessive solvent (liquid) is removed by filtration, so that the concentration of the solution can be conveniently adjusted. Wherein the concentration of the single-layer graphene solution is generally 0.1 mg/mL to 10 mg/mL, the concentration of the few-layer graphene solution is generally 1 mg/mL to 20 mg/mL, and the concentration of the multi-layer graphene solution is generally 5 mg/mL to 200 mg/mL. By measuring the concentration of the solution, the dispersion uniformity of the graphene in the solution is good.

The invention is realized by the following technical scheme, which comprises the following steps:

firstly, adding a reducing agent into a graphene oxide solution to react to obtain a chemically reduced graphene solution;

secondly, adding the solution obtained in the first step into a dispersing agent, mixing and reacting to obtain a solution containing impurities, wherein the solution contains graphene uniformly dispersed;

and thirdly, adding the solution obtained in the second step into a solvent (liquid), filtering and replacing to remove impurities in the graphene solution, and obtaining a solution with uniformly dispersed graphene after removing the impurities.

Preferably, the meaning of the solvent (liquid) in the present invention is as follows: according to the general rule, a liquid containing one component is called a solvent, and a liquid containing two or more components is called a solution.

Preferably, the graphene oxide in the first step is used as a mixture of one or more of the following: single-layer graphene oxide, few-layer graphene oxide, and multi-layer graphene oxide.

Preferably, the solvent (liquid) for preparing the graphene oxide solution in the first step is a common public solvent (liquid), and one or more of the following are commonly used for mixing: water, methanol, ethanol, propanol, acetone, N-dimethylformamide, N-dimethylacetamide, N-methylpyrrolidone.

Preferably, in the first step, the concentration of the graphene oxide solution is 0.05-100 mg/mL according to different types of actually used graphene oxide, and the common concentration is as follows: 0.05 mg/mL, 0.1 mg/mL, 0.2 mg/mL, 0.3 mg/mL, 0.4 mg/mL, 0.5 mg/mL, 0.6 mg/mL, 0.7 mg/mL, 0.8 mg/mL, 0.9 mg/mL, 1 mg/mL, 1.5 mg/mL, 2 mg/mL, 2.5 mg/mL, 3 mg/mL, 4 mg/mL, 5 mg/mL, 6 mg/mL, 7 mg/mL, 8 mg/mL, 9 mg/mL, 10 mg/mL, 11 mg/mL, 12 mg/mL, 13 mg/mL, 14 mg/mL, 15 mg/mL, 20 mg/mL, 30 mg/mL, 40 mg/mL, 50 mg/mL, 60 mg/mL, 70 mg/mL, 80 mg/mL, 90 mg/mL, and 100/mL.

Preferably, in the first step, according to the specific graphene oxide used, a surfactant may be added when preparing the solution, where the surfactant is one or more of the following: polyvinylpyrrolidone, polyethylenimine, dodecyltrimethylammonium bromide, tetradecyltrimethylammonium bromide, hexadecyltrimethylammonium bromide, octadecyltrimethylammonium bromide, sodium dodecylbenzenesulfonate, sodium dodecylsulfate, sodium dodecylsulfonate, alkylphenol ethoxylates, triton x-100, polyethylene glycol, aqueous ammonia, N-diethylpropiolate, octadecylamine, gum arabic, cyclodextrin, DNA. The mass ratio of graphene oxide to surfactant is 1 (0-50), and the mass ratio is as follows: 1:0, 1:0.05, 1:0.06, 1:0.07, 1:0.08, 1:0.09, 1:0.1, 1:0.15, 1:0.2, 1:0.25, 1:0.3, 1:0.35, 1:0.4, 1:0.45, 1:0.5, 1:0.55, 1:0.6, 1:0.65, 1:0.7, 1:0.75, 1:0.8, 1:0.85, 1:0.9, 1:0.95, 1:1, 1:1.1, 1:1.2, 1:1.3, 1:1.4, 1:1.5, 1:1.6, 1:1.7, 1:1.8, 1:1.9, 1:2, 1:2.1, 1:2.2, 1:2.3, 1:2.4, 1:4, 1:2.8, 1:2.3, 1:2.9, 1:2.5, 1:2.6, 1:1.3, 1:4.3, 1:2.3, 1.3, 1:2.3, 3, and the like; 1:2.5, 1:2.6, 1:2.7, 1:2.8, 1:2.9, 1:3, 1:3.1, 1:3.2, 1:3.3, 1:3.4, 1:3.5, 1:3.6, 1:3.7, 1:3.8, 1:3.9, 1:4, 1:4.1, 1:4.2, 1:4.3, 1:4.4, 1:4.5, 1:4.6, 1:4.7, 1:4.8, 1:4.9, 1:5, 1:6, 1:7, 1:8, 1:9, 1:10, 1:11, 1:12, 1:13, 1:14, 1:15, 1:20, 1:25, 1:30, 1:35, 1:40.

Preferably, the reducing agent in the first step is one or more of the following mixtures: organic acids, borohydride, citrate, ascorbate, alcohols, saccharides, amino acids, sulfur-containing reducing agents, nitrogen-containing reducing agents, reducing plant extracts, metals, inorganic acids, bases. The reducing agents commonly used are one or more of the following: ascorbic acid, oxalic acid, gallic acid, citric acid, tannic acid, tartaric acid, formic acid, acetic acid, propionic acid, butyric acid, valeric acid, caproic acid, oxalic acid, malonic acid, succinic acid, adipic acid, maleic acid, benzoic acid, phenylacetic acid, phthalic acid, terephthalic acid, fatty acids, acrylic acid, trifluoroacetic acid, dehydroascorbic acid, gul Le Tangsuan, threonic acid, lithium borohydride, sodium borohydride, potassium borohydride, rubidium borohydride, aluminum borohydride, beryllium borohydride, calcium borohydride, zinc borohydride, magnesium borohydride, cesium borohydride, strontium borohydride, barium borohydride, cuprous borohydride, titanium borohydride, zirconium borohydride, yttrium borohydride, manganese borohydride, iron borohydride, nickel borohydride, borane, lithium citrate, magnesium citrate, aluminum citrate, potassium citrate, calcium citrate ammonium citrate, ferric citrate, ferrous citrate, nickel citrate, cobalt citrate, manganese citrate, chromium citrate, cupric citrate, zinc citrate, barium citrate, lithium ascorbate, sodium ascorbate, magnesium ascorbate, aluminum ascorbate, potassium ascorbate, calcium ascorbate, ammonium ascorbate, ferrous ascorbate, nickel ascorbate, cobalt ascorbate, manganese ascorbate, chromium ascorbate, copper ascorbate, zinc ascorbate, barium ascorbate, stannous ascorbate, methanol, benzyl alcohol, ethanol, ethylene glycol, propanol, isopropanol, butanol, sorbitol, monosaccharides (glucose, fructose, galactose), disaccharides (sucrose, lactose, maltose), oligosaccharides (cyclodextrin), polysaccharides (chitosan), L-cysteine, L-glutathione, thiourea dioxide, ethanethiol, thiophene, lawsen reagent, lithium persulfate, sodium persulfate, potassium persulfate, ammonium persulfate, ammonia water, hydrazine (hydrazine), hydrazine hydrate (hydrazine hydrate), ammonia borane, phenylhydrazine, urea, hydroxylamine hydrochloride, pyrrole, pyridine, benzylamine, p-phenylenediamine, ethylenediamine, dimethylketoxime, lithium nitrite, sodium nitrite, magnesium nitrite, aluminum nitrite, potassium nitrite, calcium nitrite, ammonium nitrite, iron nitrite, ferrous nitrite, nickel nitrite, cobalt nitrite, manganese nitrite, chromium nitrite, copper nitrite, barium nitrite, zinc nitrite, silver nitrite, tea extract, rose extract, iron tree leaf extract, orange peel extract, ginkgo leaf extract, lithium, sodium, magnesium, aluminum, potassium, calcium, beryllium, iron, zinc, tin, lithium aluminum hydride, sulfuric acid, hydrofluoric acid, hydrochloric acid, hydrobromic acid, hydroiodic acid, phosphoric acid, nitric acid, carbonic acid, lithium hydroxide, sodium hydroxide, potassium hydroxide.

Preferably, the mass ratio of graphene oxide to reducing agent in the first step is 1 (1-200), and the mass ratio is 1:1, 1:2, 1:3, 1:4, 1:5, 1:6, 1:7, 1:8, 1:9, 1:10, 1:11, 1:12, 1:13, 1:14, 1:15, 1:16, 1:17, 1:18, 1:19, 1:20, 1:25, 1:30, 1:35, 1:40, 1:45, 1:50.

Preferably, the time of the chemical reduction reaction in the first step is 0 to 120 hours. The common usage is: 1, 1.5, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 50, 52, 54, 56, 58, 60, 64, 68, 72, 76, 80, 84, 88, 92, 96, 100, 104, 108, 112, 116, 120.

Preferably, the chemical reduction reaction temperature in the first step is-10 ℃ to 100 ℃, and is usually: -10 ℃, -5 ℃, 0 ℃, 5 ℃, 10 ℃, 15 ℃, 20 ℃, 25 ℃, 30 ℃, 35 ℃, 40 ℃, 45 ℃, 50 ℃, 80 ℃, 85 ℃, 90 ℃, 95 ℃.

Preferably, the stirring speed of the chemical reduction reaction in the first step is 0-3000 r/min. The usual rotational speeds are: 0 r/min (i.e. standing), 10 r/min, 20 r/min, 30 r/min, 40 r/min, 50 r/min, 60 r/min, 70 r/min, 80 r/min, 90 r/min, 100 r/min, 110 r/min, 120 r/min, 130 r/min, 140 r/min, 150 r/min, 180 r/min, 200 r/min, 240 r/min, 300 r/min, 500 r/min, 600 r/min, 700 r/min, 800 r/min, 900 r/min, 1000 r/min.

Preferably, the chemical reduction reaction in the first step can adjust relevant parameters of the type of the reducing agent, the quality of the reducing agent, the reaction time, the reaction temperature and the stirring rotation speed during the experiment.

Preferably, the dispersant in the second step is one or more of the following: peroxides, superoxides, percarbonates, persulfates, permanganates and permanganates, manganates, ferrates and ferrates, chlorates and chlorates, carbonates, bicarbonates, bisulphates, ammonium salts, dichromates and bichromates, iodic acids and iodates, bromic and bromates, nitrous acids and nitrites, metals, metal hydrides, acids, bases, perborates, halogen intermetallics. Commonly used dispersants are one or more of the following mixtures: hydrogen peroxide, lithium peroxide, sodium peroxide, potassium peroxide, calcium peroxide, magnesium peroxide, zinc peroxide, strontium peroxide, barium peroxide, lead peroxide, urea hydrogen peroxide complex, 2-dihydro propane, 2, 5-dimethyl-2, 5-dihydro hexane, 2-bis- (t-butyl peroxide) propane, 2-bis- (t-butyl peroxide) butane, 2, 5-dimethyl-2, 5-bis- (t-butyl peroxide) hexane, 2-bis- (4, 4-di-t-butyl cyclohexyl peroxide) propane, 2, 5-dimethyl-2, 5-bis- (2-ethylhexanoyl peroxide) hexane 2, 5-dimethyl-2, 5-bis- (3, 5-trimethylhexanoyl) hexane, 2, 5-dimethyl-2, 5-bis- (benzoyl peroxide) hexane, 1-bis- (t-butyl peroxide) cyclohexane, 1-bis- (t-butyl peroxide) -3, 5-trimethylcyclohexane, acetyl sulfonyl peroxide cyclohexane bis- (1-hydroxycyclohexane) peroxide, 3,3,6,6,9,9-hexamethyl-1, 2,4, 5-tetraoxycyclononane, 2, 5-dimethyl-2, 5-bis- (tert-butyl peroxide) -3-hexyne, isopropyl hydroperoxide, 1, 3-tetramethylbutyl hydroperoxide, cumene hydroperoxide, diisopropyl (yl) benzene hydroperoxide, di-tert-butylisopropyl (yl) benzene hydroperoxide pinane, menthane hydroperoxide, tetralin hydroperoxide, di-tert-butyl peroxide, tert-butylbenzene peroxide, tert-butylisopropyl (yl) benzene peroxide, 1, 3-bis- (2-tert-butylisopropyl) benzene peroxide, 1, 4-bis- (2-tert-butylisopropyl) benzene peroxide, diisopropylbenzene peroxide, isobutylmethylketone peroxide, methylethylketone peroxide, acetylacetone peroxide, cyclohexanone peroxide, methylcyclohexanone peroxide, diacetone peroxide, acetyl peroxide, propionyl peroxide, isobutyryl peroxide, n-octanoyl peroxide n-nonanoyl peroxide, isononyl peroxide, decanoyl peroxide, dodecanoyl peroxide, benzoyl peroxide, di- (2-methylbenzoyl) peroxide, di- (2-chlorobenzoyl) peroxide, di- (2, 4-dichlorobenzoyl) peroxide, acetyl benzoyl peroxide, peroxyformic acid, peroxyacetic acid, succinic acid peroxide, azelaic acid diperoxide, dodecanedioic acid diperoxide, benzoyl peroxide, 3-chlorobenzoic acid peroxide, terephthalic acid, t-butylterephthalic acid, t-butyl peroxyacetate, t-butyl peroxydiethyl acetate, ethyl 3, 3-bis- (t-butyl peroxybutyrate, tert-butyl peroxyisobutyrate, n-butyl 4, 4-bis- (tert-butyl peroxypivalate), tert-butyl peroxypivalate, isopropyl peroxypivalate, tert-butyl peroxy2-ethylhexanoate 1, 3-tetramethylbutyl peroxy3, 5-trimethylhexanoate, tert-butyl peroxyneodecanoate, tert-amyl peroxyneodecanoate, isopropyl peroxyneodecanoate, tert-butyl peroxybutenoate, tert-butyl peroxymaleic acid, tert-butyl peroxybenzoate, tert-butyl peroxyphthalate, bis- (tert-butyl peroxyphthalate), tert-butyl peroxyisopropyl carbonate, tert-butyl peroxyoctadecanoyl carbonate 2, 4-trimethylpentyl-2-peroxy phenoxyacetate, 3-tert-butyl-3-o-hydroxymethylbenzoate, diethyl peroxydicarbonate, di-n-propyl peroxydicarbonate, diisopropyl peroxydicarbonate, di-n-butyl peroxydicarbonate, di-sec-butyl peroxydicarbonate, di- (2-ethylhexyl) peroxydicarbonate, di (isotridecyl) peroxydicarbonate, ditetradecyl peroxydicarbonate, dioctadecyl peroxydicarbonate, dicyclohexyl peroxydicarbonate, di- (4-tert-butylcyclohexyl) peroxydicarbonate, diphenyl peroxydicarbonate, bis- (2-phenoxyethyl) peroxydicarbonate, bis- (3, 5-trimethyl-1, 2-dioxolane), pinene peroxide, chenopodium oil, sodium superoxide, potassium superoxide, lithium percarbonate sodium percarbonate, potassium percarbonate, ammonium percarbonate, calcium percarbonate, aluminum percarbonate, magnesium percarbonate, lithium persulfate, sodium persulfate, potassium persulfate, ammonium persulfate, permanganate, lithium permanganate sodium permanganate, potassium permanganate, ammonium permanganate, calcium permanganate, zinc permanganate, magnesium permanganate, silver permanganate, barium permanganate, lithium manganate, sodium manganate, potassium manganate, ferrate, lithium ferrate, sodium ferrate, potassium ferrate, perchloric acid, lithium perchlorate, sodium perchlorate, potassium perchlorate, magnesium perchlorate, ammonium perchlorate, calcium perchlorate, barium perchlorate, strontium perchlorate, lead perchlorate ferrous perchlorate, silver perchlorate, chloric acid, lithium chlorate, sodium chlorate, potassium chlorate, magnesium chlorate, ammonium chlorate, cesium chlorate, strontium chlorate, barium chlorate, calcium chlorate, copper chlorate, zinc chlorate, silver chlorate, chlorous acid, lithium chlorite, sodium chlorite, potassium chlorite, magnesium chlorite, ammonium chlorite, calcium chlorite, hypochlorous acid, lithium hypochlorite, sodium hypochlorite, potassium hypochlorite, magnesium hypochlorite, calcium hypochlorite, ammonium hypochlorite, barium hypochlorite, chlorine dioxide, lithium carbonate, sodium carbonate, potassium carbonate, ammonium carbonate, calcium carbonate, magnesium carbonate, aluminum carbonate, iron carbonate, copper carbonate, silver carbonate, lithium bicarbonate, sodium bicarbonate, potassium bicarbonate, magnesium bicarbonate, calcium bicarbonate, barium bicarbonate, lithium bisulfate, sodium bisulfate, potassium bisulfate, magnesium bisulfate, calcium bisulfate, ammonium bicarbonate, ammonium nitrate, ammonium hypochlorite, ammonium nitrite, ammonium sulfate, ammonium bisulfate, ammonium fluoride, ammonium chloride, ammonium iodide, ammonium bromide, dichromic acid, lithium dichromate, sodium dichromate, potassium dichromate, ammonium dichromate, magnesium dichromate, silver dichromate, cesium dichromate, barium dichromate, aluminum dichromate, copper dichromate, zinc dichromate, chromium trioxide, periodic acid, ammonium periodate, barium periodate, sodium paraperiodate, sodium metaperiodate, potassium periodate, potassium paraperiodate, potassium metaperiodate, iodic acid, diiodide, ammonium iodate, sodium iodate, potassium iodate-in-iodic acid, potassium iodate-diiodidate, lithium iodate, calcium iodate, strontium iodate, barium iodate, manganese iodate, iron iodate, zinc iodate, silver iodate, cadmium iodate, lead iodate, sodium bromate, potassium bromate, magnesium bromate, strontium bromate, barium bromate, zinc bromate, silver, cadmium bromate lead bromate, hydrobromic acid, sodium bromate, potassium bromate, nitrous acid, lithium nitrite, sodium nitrite, magnesium nitrite, aluminum nitrite, potassium nitrite, calcium nitrite, ammonium nitrite, ferric nitrite, ferrous nitrite, nickel nitrite, cobalt nitrite, manganese nitrite, chromium nitrite, copper nitrite, barium nitrite, zinc nitrite, silver nitrite, lithium, sodium, magnesium, aluminum, potassium, calcium, beryllium, iron, zinc lithium hydride, sodium hydride, aluminum hydride, magnesium hydride, potassium hydride, calcium hydride, barium hydride, nickel hydride, copper hydride, zinc hydride, ascorbic acid, oxalic acid, gallic acid, citric acid, tannic acid, tartaric acid, formic acid, acetic acid, propionic acid, butyric acid, valeric acid, caproic acid, enanthic acid, caprylic acid, oxalic acid, malonic acid, succinic acid, adipic acid, maleic acid, 2-methylbutyric acid, 2-ethylbutyric acid, 2-ethylhexanoic acid, myristic acid, oleic acid, benzoic acid, phenylacetic acid, phthalic acid, terephthalic acid, fatty acid, acrylic acid, trifluoroacetic acid, dehydroascorbic acid, palo Le Tangsuan, threonic acid, sulfuric acid, hydrofluoric acid, hydroiodic acid, hydrobromic acid, hydrochloric acid, phosphoric acid, nitric acid, carbonic acid, aqueous ammonia, lithium hydroxide, sodium hydroxide, potassium hydroxide, barium perborate, sodium perborate, potassium perborate, rubidium perborate, cesium perborate, calcium perborate, barium perborate, iodine fluoride, bromine monofluoride, chlorine monofluoride, iodine chloride, bromine chloride, iodine bromide, iodine trifluoride, bromine trifluoride, chlorine trifluoride, iodine pentafluoride, bromine pentafluoride, chlorine pentafluoride, iodine heptafluoride.

Preferably, the mass ratio of the dispersant to the initial graphene oxide in the second step is (1-1000): 1, which is usually: 5:1, 10:1, 15:1, 20:1, 25:1, 30:1, 35:1, 40:1, 45:1, 50:1, 55:1, 60:1, 65:1, 70:1, 75:1, 80:1, 85:1, 90:1, 95:1, 100:1, 110:1, 120:1, 130:1, 140:1, 150:1, 160:1, 170:1, 180:1, 190:1, 200:1, 210:1, 220:1, 230:1, 240:1, 250:1, 260:1, 270:1, 280:1, 290:1, 300:1, 350:1, 400:1, 450:1, 500:1.

Preferably, the reaction time in the second step is 1 minute to 120 hours, and is usually: 1 min, 2 min, 3 min, 4 min, 5 min, 6 min, 7 min, 8 min, 9 min, 10 min, 15 min, 20 min, 25 min, 30 min, 35 min, 40 min, 45 min, 50 min, 55 min, 60 min, 65 min, 70 min, 75 min, 80 min, 85 min, 90 min, 95 min, 100 min, 105 min, 110 min, 115 min, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 31, 32, 33, 34, 35, 36, 37, 38, 39, 40, 41, 42, 43, 44, 45, 46, 47, 48, 50, 52, 54, 56, 58, 60, 64, 68, 72, 76, 80, 84, 88, 92, 96, 100, 104, 108, 112, 116, 120.

Preferably, the reaction temperature in the second step is-10 ℃ to 100 ℃, and is usually: -10 ℃, -5 ℃, 0 ℃, 5 ℃, 10 ℃, 15 ℃, 20 ℃, 25 ℃, 30 ℃, 35 ℃, 40 ℃, 45 ℃, 50 ℃, 55 ℃, 60 ℃, 65 ℃, 70 ℃, 75 ℃, 80 ℃, 85 ℃, 90 ℃, 95 ℃.

Preferably, the stirring speed of the reaction in the second step is 0-3000 r/min, and is usually: 0 r/min (i.e. standing), 10 r/min, 20 r/min, 30 r/min, 40 r/min, 50 r/min, 60 r/min, 70 r/min, 80 r/min, 90 r/min, 100 r/min, 110 r/min, 120 r/min, 130 r/min, 140 r/min, 150 r/min, 180 r/min, 200 r/min, 240 r/min, 300 r/min, 500 r/min, 600 r/min, 700 r/min, 800 r/min, 900 r/min, 1000 r/min.

Preferably, the dispersing agent in the second step is present singly or in combination of two or more of the following: the first case is that the dispersing agent reacts with various chemical substances in the graphene solution after chemical reduction to generate gas, the second case is that the dispersing agent is decomposed to generate gas, and the third case is that a plurality of dispersing agents react with each other to generate gas. The generated common gas is one or a mixture of the following components: oxygen, carbon dioxide, nitrogen, ammonia, hydrogen, ozone, fluorine, chlorine, bromine, nitrogen monoxide, nitrogen dioxide, chlorine dioxide. The reaction also produces soluble products. Typical examples of the dispersing action of the dispersant are as follows: (1) The reducing agent is ascorbic acid, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen. (2) The reducing agent is ascorbic acid, the dispersing agent is sodium percarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (3) The reducing agent is ascorbic acid, the dispersing agent is sodium carbonate, and the generated gas is as follows: carbon dioxide. (4) The reducing agent is ascorbic acid, the dispersing agent is hydrogen peroxide and sodium carbonate, and the generated gas is as follows: oxygen, carbon dioxide. (5) The reducing agent is ascorbic acid, the dispersing agent is sodium bicarbonate, and the generated gas is as follows: carbon dioxide. (6) The reducing agent is ascorbic acid, the dispersing agent is hydrogen peroxide and sodium bicarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (7) The reducing agent is oxalic acid, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen. (8) The reducing agent is oxalic acid, the dispersing agent is sodium percarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (9) The reducing agent is oxalic acid, the dispersing agent is sodium carbonate, and the generated gas is as follows: carbon dioxide. (10) The reducing agent is oxalic acid, the dispersing agent is hydrogen peroxide and sodium carbonate, and the generated gas is as follows: oxygen, carbon dioxide. (11) The reducing agent is oxalic acid, the dispersing agent is sodium bicarbonate, and the generated gas is as follows: carbon dioxide. (12) The reducing agent is oxalic acid, the dispersing agent is hydrogen peroxide and sodium bicarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (13) The reducing agent is citric acid, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen. (14) The reducing agent is citric acid, the dispersing agent is sodium percarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (15) The reducing agent is citric acid, the dispersing agent is sodium carbonate, and the generated gas is as follows: carbon dioxide. (16) The reducing agent is citric acid, the dispersing agent is hydrogen peroxide and sodium carbonate, and the generated gas is as follows: oxygen, carbon dioxide. (17) The reducing agent is citric acid, the dispersing agent is sodium bicarbonate, and the generated gas is as follows: carbon dioxide. (18) The reducing agent is citric acid, the dispersing agent is hydrogen peroxide and sodium bicarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (19) The reducing agent is sodium ascorbate, sodium oxalate and sodium citrate, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen. (20) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen. (21) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is sodium percarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (22) The reducing agent is ascorbic acid and citric acid, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen. (23) The reducing agent is ascorbic acid and citric acid, the dispersing agent is sodium percarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (24) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is hydrogen peroxide and sodium carbonate, and the generated gas is as follows: oxygen, carbon dioxide. (25) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is hydrogen peroxide and sodium bicarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (26) The reducing agent is ascorbic acid, the dispersing agent is potassium dichromate and ammonium sulfate, and the generated gas is as follows: oxygen, nitrogen. (27) The reducing agent is ascorbic acid, the dispersing agent is potassium permanganate, and the generated gas is as follows: oxygen. (28) The reducing agent is ascorbic acid, the dispersing agent is potassium ferrate, and the generated gas is as follows: oxygen. (29) The reducing agent is ascorbic acid, the dispersing agent is sodium persulfate, and the generated gas comprises: oxygen. (30) The reducing agent is ascorbic acid, the dispersing agent is potassium chlorate, and the generated gas is as follows: oxygen. (31) The reducing agent is ascorbic acid, the dispersing agent is potassium perchlorate, and the generated gas is as follows: oxygen. (32) The reducing agent is ascorbic acid, the dispersing agent is calcium hydride, and the generated gas is as follows: hydrogen gas. (33) The reducing agent is ascorbic acid, the dispersing agent is potassium dichromate, and the generated gas is as follows: oxygen. (34) The reducing agent is ascorbic acid and hydrazine hydrate, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen, nitrogen. (35) The reducing agent is ammonia water, sodium borohydride and ascorbic acid, the dispersing agent is hydrogen peroxide, and the generated gas is: oxygen, nitrogen. (36) The reducing agent is ascorbic acid, the dispersing agent is hydrogen peroxide and potassium permanganate, and the generated gas is as follows: oxygen. (37) The reducing agent is ascorbic acid, the dispersing agent is ammonium persulfate, and the generated gas comprises: oxygen, ammonia. (38) The reducing agent is ascorbic acid, the dispersing agent is potassium manganate and hydrogen peroxide, and the generated gas is as follows: oxygen. (39) The reducing agent is ascorbic acid, the dispersing agent is sodium perborate and sodium bicarbonate, and the generated gas is as follows: oxygen, carbon dioxide. (40) The reducing agent is ammonia water, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen, nitrogen. (41) The reducing agent is ammonia water and glucose, the dispersing agent is ascorbic acid and hydrogen peroxide, and the generated gas is as follows: oxygen, nitrogen. (42) The reducing agent is ammonia water and glucose, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen, nitrogen. (43) The reducing agent is ammonia water and glucose, the dispersing agent is ammonium chloride and sodium nitrite, and the generated gas is as follows: nitrogen gas. (44) The reducing agent is ammonia water and glucose, the dispersing agent is ammonium bicarbonate, and the generated gas is as follows: carbon dioxide, ammonia. (45) The reducing agent is ammonia water and glucose, the dispersing agent is ammonium nitrite, and the generated gas is as follows: nitrogen gas. (46) The reducing agent is ammonia water and hydrazine hydrate, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen, nitrogen. (47) The reducing agent is ammonia water and sodium borohydride, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen, nitrogen. (48) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is aluminum, and the generated gas is as follows: hydrogen gas. (49) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is hydrogen chloride and aluminum, and the generated gas is as follows: hydrogen gas. (50) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is sodium bicarbonate and aluminum, and the generated gas is as follows: carbon dioxide, hydrogen. (51) The reducing agent is ammonia water and glucose, the dispersing agent is sodium hydroxide and aluminum, and the generated gas is as follows: hydrogen gas. (52) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is sodium percarbonate, hydrogen chloride and aluminum, and the generated gas is as follows: oxygen, carbon dioxide, hydrogen. (53) The reducing agent is ascorbic acid and citric acid, the dispersing agent is zinc, and the generated gas is as follows: hydrogen gas. (54) The reducing agent is ascorbic acid and citric acid, the dispersing agent is hydrogen peroxide and zinc, and the generated gas is as follows: the reducing agent of oxygen and hydrogen (55) is ascorbic acid, the dispersing agent is hydrogen peroxide, hydrogen chloride and zinc, and the generated gases are as follows: oxygen, hydrogen. (56) The reducing agent is ammonia water and glucose, the dispersing agent is hydrogen peroxide and zinc, and the generated gas is as follows: oxygen, nitrogen, hydrogen. (57) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is sodium carbonate and zinc, and the generated gas is as follows: carbon dioxide, hydrogen. (58) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is sodium carbonate, hydrogen peroxide and zinc, and the generated gas is as follows: oxygen, carbon dioxide, hydrogen. (59) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is sodium carbonate, hydrogen chloride and zinc, and the generated gas is as follows: carbon dioxide, hydrogen. (60) The reducing agent is ascorbic acid, oxalic acid and zinc, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: hydrogen and oxygen. (61) The reducing agent is hydroiodic acid, the dispersing agent is hydrogen peroxide, and the generated gas is as follows: oxygen. (62) The reducing agent is ascorbic acid, the dispersing agent is hydrogen chloride and sodium chlorite, and the generated gas is as follows: chlorine dioxide. (63) The reducing agent is ascorbic acid, the dispersing agent is sodium bicarbonate, sodium bisulfate, hydrogen chloride and sodium chlorite, and the generated gases are as follows: carbon dioxide, chlorine dioxide. (64) The reducing agent is ascorbic acid and oxalic acid, the dispersing agent is sodium bicarbonate, hydrogen chloride and sodium chlorite, and the generated gas is as follows: carbon dioxide, chlorine dioxide. The general examples set forth above are merely illustrative of the principles of the present invention, and the experimental protocols that are actually used are not limited to those set forth above. All experiments performed in accordance with the principles of the present invention and with the various reagents exemplified herein are included within the scope of the present invention.

Preferably, the reaction in the second step can adjust relevant parameters of the type of the dispersant, the quality of the dispersant, the reaction time, the reaction temperature and the stirring rotation speed in the experimental process.

Preferably, the filtration and displacement in the third step is performed in one or more of the following combinations: normal pressure filtration, reduced pressure filtration, gravity filtration, vacuum filtration, centrifugal filtration, dialysis, and soaking replacement.

Preferably, in the third step, the filtering and replacing are performed according to the different sheet diameter and the number of layers of the graphene, and the used equipment is one or more of the following combinations: a filter screen, a filter membrane, a filter bag and a filter paper with the mesh number of 10-5000 meshes. The usual mesh numbers are: 200 mesh, 250 mesh, 300 mesh, 350 mesh, 400 mesh, 450 mesh, 500 mesh, 550 mesh, 600 mesh, 650 mesh, 700 mesh, 750 mesh, 800 mesh, 1000 mesh.

Preferably, the filtering and replacing in the third step remove impurities in the graphene solution, wherein the impurity removal standard is that the impurity content in the graphene solution meets the requirement standard of downstream application on the impurity content in the graphene. Removed impurities include, but are not limited to: impurities in the graphite powder, impurities introduced during preparation of graphene, impurities introduced during reduction of graphene, and impurities introduced during preparation of a graphene solution.

Preferably, the filtration and displacement in the third step may be performed by using only one solvent (liquid), or may be performed by using a plurality of solvents (liquids) in sequence. By utilizing the mutual solubility of solvents (liquids), graphene uniformly dispersed in one solvent (liquid) is fully replaced by different solvents (liquids) in sequence, and uniformly dispersed in other solvents (liquids), so that a solution in which graphene is uniformly dispersed in different solvents (liquids) is sequentially obtained.

Preferably, the solvent (liquid) used for the filtration and displacement in the third step is one of the following three: an inorganic solvent (liquid), an organic solvent (liquid), and a mixed solution of the inorganic solvent (liquid) and the organic solvent (liquid).

Preferably, the inorganic solvent (liquid) used for the filtration and displacement in the third step is any one of the following: water, a solution formed by adding solute to water.

Preferably, one of the inorganic solutions used for the filtration and displacement in the third step is a solution formed by adding a solute to water, and the solute is one or more of the following: lithium chloride, sodium chloride, magnesium chloride, aluminum chloride, potassium chloride, calcium chloride, ammonium chloride, ferric chloride, ferrous chloride, nickel chloride, cobalt chloride, manganese chloride, chromium chloride, copper chloride, zinc chloride, barium chloride, tin chloride, stannous chloride, lithium fluoride, sodium fluoride, magnesium fluoride, aluminum fluoride, potassium fluoride, calcium fluoride, ammonium fluoride, ferric fluoride, ferrous fluoride, nickel fluoride cobalt fluoride, manganese fluoride, chromium fluoride, copper fluoride, zinc fluoride, barium fluoride, tin fluoride, stannous fluoride, lithium sulfate, sodium sulfate, magnesium sulfate, aluminum sulfate, potassium sulfate, ammonium sulfate ferric sulfate, ferrous sulfate, nickel sulfate, cobalt sulfate, manganese sulfate, chromium sulfate, copper sulfate, zinc sulfate, tin sulfate, stannous sulfate, lithium nitrate, sodium nitrate, magnesium nitrate, aluminum nitrate potassium nitrate, calcium nitrate, ammonium nitrate, iron nitrate, ferrous nitrate, nickel nitrate, cobalt nitrate, manganese nitrate, chromium nitrate, copper nitrate, barium nitrate, zinc nitrate, tin nitrate, stannous nitrate, lithium carbonate, sodium carbonate, potassium carbonate, ammonium carbonate, lithium bicarbonate, sodium bicarbonate, magnesium bicarbonate, potassium bicarbonate, calcium bicarbonate, ammonium bicarbonate, lithium acetate, sodium acetate, magnesium acetate, aluminum acetate, potassium acetate, calcium acetate, ammonium acetate, iron acetate, ferrous acetate, nickel acetate, cobalt acetate, manganese acetate, chromium acetate, copper acetate, zinc acetate, barium acetate, tin acetate, stannous acetate, the surfactant added in the first step described in [0020], the reducing agent used in the first step described in [0021], the dispersing agent used in the second step described in [0027 ].

Preferably, one of the organic solvents (liquids) used in the filtration and displacement in the third step is one or more of the following: hydrocarbon solvents (liquids), halogenated hydrocarbon solvents (liquids), alcohol solvents (liquids), phenol solvents (liquids), ether solvents (liquids), aldehyde solvents (liquids), ketone solvents (liquids), ester solvents (liquids), acid and acid anhydride solvents (liquids), amine solvents (liquids), amide solvents (liquids), nitrile solvents (liquids), nitrogen-containing compound solvents (liquids), sulfur-containing compound solvents (liquids). The common organic solvents (liquids) are one or more of the following mixtures: CBrF ₃ 、CClF ₃ 、CCl ₂ F ₂ 、CCl ₃ F、CCl ₄ 、CCl ₄ S、CF ₄ 、CS ₂ 、CHBrCl ₂ 、CHBr ₂ Cl、CHBr ₃ 、CHCl ₂ F、CHCl ₃ 、CHF ₃ 、CHF ₃ O ₃ S、CH ₂ ClBr、CH ₂ Br ₂ 、CH ₂ Cl ₂ 、CH ₂ O、CH ₂ O ₂ 、CH ₃ Br、CH ₃ Cl、CH ₃ I、CH ₃ NCO、CH ₃ ON、CH ₃ NO ₂ 、CH ₄ O、CH ₅ N、CH ₆ ClN ₃ O、CH ₆ N ₂ 、C ₂ Cl ₂ F ₄ 、C ₂ Cl ₃ F ₃ 、C ₂ Cl ₄ 、C ₂ Cl ₄ F ₂ 、C ₂ Cl ₆ 、C ₂ HCl ₂ F ₃ 、C ₂ HCl ₂ N、C ₂ HCl ₃ 、C ₂ HO ₂ Cl ₃ 、C ₂ HCl ₅ 、C ₂ HF ₃ O ₂ 、C ₂ H ₂ Br ₄ 、C ₂ H ₂ ClF ₃ 、C ₂ H ₂ ClN、C ₂ H ₂ Cl ₂ 、C ₂ H ₂ Cl ₂ O、C ₂ H ₂ O ₂ Cl ₂ 、C ₂ H ₂ Cl ₄ 、C ₂ H ₂ F ₂ 、C ₂ H ₂ O ₄ 、C ₂ H ₃ Cl、C ₂ H ₃ ClF ₂ 、C ₂ H ₃ ClO、C ₂ H ₃ ClO ₂ 、C ₂ H ₃ O ₂ Cl、C ₂ H ₃ Cl ₃ 、C ₂ H ₃ F ₃ O、C ₂ H ₃ N、C ₂ H ₄ 、C ₂ H ₄ BrCl、C ₂ H ₄ Br ₂ 、C ₂ H ₄ Cl ₂ 、C ₂ H ₄ Cl ₂ O、C ₂ H ₄ F ₂ 、C ₂ H ₄ O、C ₂ H ₄ O ₂ 、C ₂ H ₄ O ₂ S、C ₂ H ₄ O ₃ 、C ₂ H ₅ Br、C ₂ H ₅ BrO、C ₂ H ₅ Cl、C ₂ H ₅ ClO、C ₂ H ₅ N、C ₂ H ₅ ON、C ₂ H ₅ NO ₂ 、C ₂ H ₆ 、C ₂ H ₆ N ₂ O、C ₂ H ₆ O、C ₂ H ₆ O ₂ 、C ₂ H ₆ OS、C ₂ H ₆ O ₂ S、C ₂ H ₆ O ₄ S、C ₂ H ₆ S、C ₂ H ₇ N、C ₂ H ₇ NO、C ₂ H ₇ O ₄ P、C ₂ H ₈ N ₂ 、C ₃ Cl ₂ F ₄ O、C ₃ F ₆ O、C ₃ H ₃ F ₃ O、C ₃ H ₃ N、C ₃ H ₄ Cl ₂ 、C ₃ H ₄ O、C ₃ H ₄ O ₂ 、C ₃ H ₄ O ₃ 、C ₃ H ₄ N ₂ 、C ₃ H ₅ BrO、C ₃ H ₅ BrO ₂ 、C ₃ H ₅ Br ₂ Cl、C ₃ H ₅ Br ₃ 、C ₃ H ₅ Cl、C ₃ H ₅ OCl、C ₃ H ₅ ClO ₂ 、C ₃ H ₅ Cl ₃ 、C ₃ H ₅ N、C ₃ H ₅ NO、C ₃ H ₆ 、C ₃ H ₆ Br ₂ 、C ₃ H ₆ Br ₂ O、C ₃ H ₆ ClNO、C ₃ H ₆ Cl ₂ 、C ₃ H ₆ Cl ₂ O、C ₃ H ₆ O、C ₃ H ₆ O ₂ 、C ₃ H ₆ O ₃ 、C ₃ H ₆ O ₃ S、C ₃ H ₇ Br、C ₃ H ₇ Cl、C ₃ H ₇ ClO、C ₃ H ₇ ClO ₂ 、C ₃ H ₇ I、C ₃ H ₇ N、C ₃ H ₇ ON、C ₃ H ₇ NO ₂ 、C ₃ H ₇ NO ₃ 、C ₃ H ₈ 、C ₃ H ₈ O、C ₃ H ₈ O ₂ 、C ₃ H ₈ O ₃ 、C ₃ H ₈ S、C ₃ H ₉ BO ₃ 、C ₃ H ₉ N、C ₃ H ₉ NO、C ₃ H ₉ O ₄ P、C ₃ H ₁₀ N ₂ 、C ₄ Cl ₆ 、C ₄ F ₆ O ₃ 、C ₄ H ₄ N ₂ 、C ₄ H ₄ O、C ₄ H ₄ S、C ₄ H ₅ Cl、C ₄ H ₅ N、C ₄ H ₅ NO ₂ 、C ₄ H ₆ 、C ₄ H ₆ Cl ₂ O ₂ 、C ₄ H ₆ O、C ₄ H ₆ O ₂ 、C ₄ H ₆ O ₃ 、C ₄ H ₆ O ₄ 、C ₄ H ₆ O ₄ Pb·3H ₂ O、C ₄ H ₇ N、C ₄ H ₇ NO、C ₄ H ₇ ClO ₂ 、C ₄ H ₈ 、C ₄ H ₈ Cl ₂ 、C ₄ H ₈ O、C ₄ H ₈ OCl ₂ 、C ₄ H ₈ O ₂ 、C ₄ H ₈ O ₂ S、C ₄ H ₈ O ₃ 、C ₄ H ₈ S、C ₄ H ₉ Br、C ₄ H ₉ Cl、C ₄ H ₉ ClO、C ₄ H ₉ I、C ₄ H ₉ N、C ₄ H ₉ NO、C ₄ H ₉ NO ₂ 、C ₄ H ₁₀ 、C ₄ H ₁₀ N ₂ O、C ₄ H ₁₀ O、C ₄ H ₁₀ O ₂ 、C ₄ H ₁₀ O ₂ S、C ₄ H ₁₀ O ₃ 、C ₄ H ₁₀ O ₄ S、C ₄ H ₁₀ S、C ₄ H ₁₁ N、C ₄ H ₁₁ NO、C ₄ H ₁₁ NO ₂ 、C ₄ H ₁₁ O ₄ P、C ₄ H ₁₂ Si、C ₄ H ₁₃ N ₃ 、C ₄ H ₁₉ NO ₂ 、C ₅ Cl ₆ 、C ₅ H ₄ O ₂ 、C ₅ H ₅ N、C ₅ H ₆ 、C ₅ H ₆ O、C ₅ H ₆ O ₂ 、C ₅ H ₇ NO ₂ 、C ₅ H ₈ 、C ₅ H ₈ O、C ₅ H ₈ O ₂ 、C ₅ H ₈ O ₃ 、C ₅ H ₉ BrO ₂ 、C ₅ H ₉ ClO ₂ 、C ₅ H ₉ N、C ₅ H ₉ ON、C ₅ H ₉ O、C ₅ H ₁₀ 、C ₅ H ₁₀ Cl ₂ 、C ₅ H ₁₀ N ₂ 、C ₅ H ₁₀ O、C ₅ H ₁₀ O ₂ 、C ₅ H ₁₀ O ₃ 、C ₅ H ₁₀ O ₄ 、C ₅ H ₁₁ Br、C ₅ H ₁₁ Cl、C ₅ H ₁₁ I、C ₅ H ₁₁ N、C ₅ H ₁₁ NO、C ₅ H ₁₁ NO ₂ 、C ₅ H ₁₁ NO ₃ 、C ₅ H ₁₂ 、C ₅ H ₁₂ N ₂ 、C ₅ H ₁₂ ON ₂ 、C ₅ H ₁₂ O、C ₅ H ₁₂ O ₂ 、C ₅ H ₁₂ O ₃ 、C ₅ H ₁₂ O ₄ 、C ₅ H ₁₂ S、C ₅ H ₁₃ N、C ₅ H ₁₃ NO、C ₅ H ₁₃ NO ₂ 、C ₆ F ₆ 、C ₆ H ₂ Cl ₄ 、C ₆ H ₃ ClN ₂ O ₄ 、C ₆ H ₃ Cl ₃ 、C ₆ H ₃ Cl ₃ O、C ₆ H ₄ BrCl、C ₆ H ₄ Br ₂ 、C ₆ H ₄ ClNO ₂ 、C ₆ H ₄ Cl ₂ 、C ₆ H ₄ Cl ₂ O、C ₆ H ₄ N ₂ O ₄ 、C ₆ H ₅ Br、C ₆ H ₅ BrO、C ₆ H ₅ Cl、C ₆ H ₅ ClO、C ₆ H ₅ F、C ₆ H ₅ I、C ₆ H ₅ NO ₂ 、C ₆ H ₆ 、C ₆ H ₆ ClN、C ₆ H ₆ O、C ₆ H ₆ O ₂ 、C ₆ H ₆ OS、C ₆ H ₆ O ₃ 、C ₆ H ₇ N、C ₆ H ₈ N ₂ 、C ₆ H ₈ O、C ₆ H ₈ O ₂ 、C ₆ H ₈ O ₄ 、C ₆ H ₁₀ 、C ₆ H ₁₀ O、C ₆ H ₁₀ O ₂ 、C ₆ H ₁₀ O ₃ 、C ₆ H ₁₀ O ₄ 、C ₆ H ₁₁ N、C ₆ H ₁₁ ON、C ₆ H ₁₂ 、C ₆ H ₁₂ ClO、C ₆ H ₁₂ Cl ₂ O ₂ 、C ₆ H ₁₂ Cl ₃ O ₄ P、C ₆ H ₁₂ O、C ₆ H ₁₂ O ₂ 、C ₆ H ₁₂ O ₂ S、C ₆ H ₁₂ O ₃ 、C ₆ H ₁₂ O ₄ 、C ₆ H ₁₃ Br、C ₆ H ₁₃ Cl、C ₆ H ₁₃ N、C ₆ H ₁₃ NO、C ₆ H ₁₄ 、C ₆ H ₁₄ O、C ₆ H ₁₄ O ₂ 、C ₆ H ₁₄ O ₃ 、C ₆ H ₁₄ O ₄ 、C ₆ H ₁₄ O ₆ 、C ₆ H ₁₅ O ₃ B、C ₆ H ₁₅ N、C ₆ H ₁₅ NO、C ₆ H ₁₅ NO ₂ 、C ₆ H ₁₅ NO ₃ 、C ₆ H ₁₅ O ₄ P、C ₆ H ₁₈ NOP、C ₆ H ₁₈ N ₄ 、C ₆ H ₁₈ OSi ₂ 、C ₇ H ₄ Cl ₃ F、C ₇ H ₅ Cl ₃ 、C ₇ H ₅ F ₃ 、C ₇ H ₅ N、C ₇ H ₅ N ₃ O ₆ 、C ₇ H ₆ Cl ₂ 、C ₇ H ₆ O、C ₇ H ₆ O ₂ 、C ₇ H ₇ Br、C ₇ H ₇ BrO、C ₇ H ₇ Cl、C ₇ H ₇ NO、C ₇ H ₇ NO ₂ 、C ₇ H ₇ NO ₃ 、C ₇ H ₈ 、C ₇ H ₈ O、C ₇ H ₈ O ₂ 、C ₇ H ₈ O ₃ 、C ₇ H ₉ N、C ₇ H ₁₀ O ₃ 、C ₇ H ₁₂ 、C ₇ H ₁₂ O、C ₇ H ₁₂ O ₂ 、C ₇ H ₁₂ O ₄ 、C ₇ H ₁₂ O ₅ 、C ₇ H ₁₃ N、C ₇ H ₁₄ 、C ₇ H ₁₄ O、C ₇ H ₁₄ O ₂ 、C ₇ H ₁₄ O ₃ 、C ₇ H ₁₄ O ₄ 、C ₇ H ₁₅ Br、C ₇ H ₁₆ 、C ₇ H ₁₆ O、C ₇ H ₁₆ O ₂ 、C ₇ H ₁₆ O ₃ 、C ₇ H ₁₆ O ₄ 、C ₇ H ₁₇ N、C ₇ H ₁₈ N ₂ 、C ₈ H ₄ F ₆ 、C ₈ H ₆ 、C ₈ H ₇ N、C ₈ H ₈ 、C ₈ H ₈ O、C ₈ H ₈ O ₂ 、C ₈ H ₈ O ₃ 、C ₈ H ₉ NO、C ₈ H ₉ NO ₃ 、C ₈ H ₉ O、C ₈ H ₁₀ 、C ₈ H ₁₀ O、C ₈ H ₁₀ O ₂ 、C ₈ H ₁₁ N、C ₈ H ₁₂ 、C ₈ H ₁₂ O ₄ 、C ₈ H ₁₄ O、C ₈ H ₁₄ O ₂ 、C ₈ H ₁₄ O ₂ N ₂ 、C ₈ H ₁₄ O ₃ 、C ₈ H ₁₄ O ₄ 、C ₈ H ₁₄ O ₅ 、C ₈ H ₁₄ O ₆ 、C ₈ H ₁₅ N、C ₈ H ₁₆ 、C ₈ H ₁₆ O、C ₈ H ₁₆ O ₂ 、C ₈ H ₁₆ O ₃ 、C ₈ H ₁₆ O ₄ 、C ₈ H ₁₇ Cl、C ₈ H ₁₈ 、C ₈ H ₁₈ O、C ₈ H ₁₈ O ₂ 、C ₈ H ₁₈ O ₃ 、C ₈ H ₁₈ O ₄ 、C ₈ H ₁₈ O ₅ 、C ₈ H ₁₉ N、C ₈ H ₁₉ O ₃ P、C ₈ H ₁₉ O ₄ P、C ₈ H ₂₀ O ₄ Si、C ₈ H ₂₃ N ₅ 、C ₈ H ₂₄ O ₄ Si ₄ 、C ₉ H ₆ N ₂ O ₂ 、C ₉ H ₆ O ₂ 、C ₉ H ₇ N、C ₉ H ₇ NO、C ₉ H ₈ 、C ₉ H ₈ O、C ₉ H ₉ N、C ₉ H ₁₀ 、C ₉ H ₁₀ O、C ₉ H ₁₀ O ₂ 、C ₉ H ₁₀ O ₃ 、C ₉ H ₁₂ 、C ₉ H ₁₂ O、C ₉ H ₁₂ O ₂ 、C ₉ H ₁₃ N、C ₉ H ₁₄ O、C ₉ H ₁₄ O ₆ 、C ₉ H ₁₆ 、C ₉ H ₁₆ O、C ₉ H ₁₆ O ₂ 、C ₉ H ₁₆ O ₄ 、C ₉ H ₁₇ N、C ₉ H ₁₈ 、C ₉ H ₁₈ O、C ₉ H ₁₈ O ₂ 、C ₉ H ₁₈ O ₄ 、C ₉ H ₂₀ 、C ₉ H ₂₀ O、C ₉ H ₂₀ O ₂ 、C ₉ H ₂₀ O ₃ 、C ₉ H ₂₁ N、C ₉ H ₂₁ NO ₃ 、C ₁₀ H ₇ Br、C ₁₀ H ₇ Cl、C ₁₀ H ₈ 、C ₁₀ H ₁₀ O、C ₁₀ H ₁₀ O ₂ 、C ₁₀ H ₁₀ O ₄ 、C ₁₀ H ₁₁ N、C ₁₀ H ₁₂ 、C ₁₀ H ₁₂ O、C ₁₀ H ₁₂ O ₂ 、C ₁₀ H ₁₂ O ₃ 、C ₁₀ H ₁₃ NO、C ₁₀ H ₁₄ 、C ₁₀ H ₁₄ O、C ₁₀ H ₁₄ NO ₅ PS、C ₁₀ H ₁₅ N、C ₁₀ H ₁₆ 、C ₁₀ H ₁₆ ClN、C ₁₀ H ₁₆ O、C ₁₀ H ₁₆ O ₈ N ₂ 、C ₁₀ H ₁₈ 、C ₁₀ H ₁₈ O、C ₁₀ H ₁₈ O ₄ 、C ₁₀ H ₁₉ N、C ₁₀ H ₂₀ 、C ₁₀ H ₂₀ O、C ₁₀ H ₂₀ O ₂ 、C ₁₀ H ₂₀ O ₄ 、C ₁₀ H ₂₁ N、C ₁₀ H ₂₂ 、C ₁₀ H ₂₂ O、C ₁₀ H ₂₂ O ₂ 、C ₁₀ H ₂₂ O ₃ 、C ₁₀ H ₂₂ O ₄ 、C ₁₀ H ₂₂ O ₅ 、C ₁₀ H ₂₂ S、C ₁₀ H ₂₃ N、C ₁₀ H ₂₃ NO、C ₁₁ H ₁₀ 、C ₁₁ H ₁₂ O ₂ 、C ₁₁ H ₁₄ O、C ₁₁ H ₁₄ O ₂ 、C ₁₁ H ₁₄ O ₃ 、C ₁₁ H ₁₆ 、C ₁₁ H ₁₆ O、C ₁₁ H ₁₇ N、C ₁₁ H ₂₀ 、C ₁₁ H ₂₀ O、C ₁₁ H ₂₀ O ₂ 、C ₁₁ H ₂₀ O ₄ 、C ₁₁ H ₂₁ N、C ₁₁ H ₂₂ 、C ₁₁ H ₂₂ O、C ₁₁ H ₂₂ O ₂ 、C ₁₁ H ₂₄ 、C ₁₁ H ₂₄ O、C ₁₂ H ₁₀ 、C ₁₂ H ₁₀ O、C ₁₂ H ₁₂ 、C ₁₂ H ₁₄ O ₄ 、C ₁₂ H ₁₆ 、C ₁₂ H ₁₆ O、C ₁₂ H ₁₆ O ₂ 、C ₁₂ H ₁₆ O ₃ 、C ₁₂ H ₁₈ 、C ₁₂ H ₂₀ O ₄ 、C ₁₂ H ₂₀ O ₇ 、C ₁₂ H ₂₂ 、C ₁₂ H ₂₂ O、C ₁₂ H ₂₂ O ₄ 、C ₁₂ H ₂₂ O ₆ 、C ₁₂ H ₂₃ N、C ₁₂ H ₂₄ 、C ₁₂ H ₂₄ O、C ₁₂ H ₂₄ O ₂ 、C ₁₂ H ₂₅ Br、C ₁₂ H ₂₅ Cl、C ₁₂ H ₂₆ 、C ₁₂ H ₂₆ O、C ₁₂ H ₂₆ O ₃ 、C ₁₂ H ₂₆ S、C ₁₂ H ₂₇ O ₃ B、C ₁₂ H ₂₇ N、C ₁₂ H ₂₇ O ₄ P、C ₁₃ H ₁₀ O、C ₁₃ H ₁₀ O ₃ 、C ₁₃ H ₁₂ 、C ₁₃ H ₁₈ O、C ₁₃ H ₂₀ 、C ₁₃ H ₂₀ O、C ₁₃ H ₂₂ O ₂ 、C ₁₃ H ₂₄ 、C ₁₃ H ₂₄ O、C ₁₃ H ₂₅ N、C ₁₃ H ₂₆ 、C ₁₃ H ₂₆ O、C ₁₃ H ₂₆ O ₂ 、C ₁₃ H ₂₈ 、C ₁₄ H ₁₀ 、C ₁₄ H ₁₂ O ₂ 、C ₁₄ H ₁₂ O ₃ 、C ₁₄ H ₁₄ 、C ₁₄ H ₁₄ O、C ₁₄ H ₂₀ O、C ₁₄ H ₂₂ 、C ₁₄ H ₂₃ N、C ₁₄ H ₂₆ 、C ₁₄ H ₂₆ O、C ₁₄ H ₂₆ O ₄ 、C ₁₄ H ₂₇ N、C ₁₄ H ₂₈ 、C ₁₄ H ₂₈ O、C ₁₄ H ₂₈ O ₂ 、C ₁₄ H ₃₀ 、C ₁₄ H ₃₀ O、C ₁₅ H ₂₂ O、C ₁₅ H ₂₄ 、C ₁₅ H ₂₄ O、C ₁₅ H ₂₇ N ₃ O、C ₁₅ H ₂₈ 、C ₁₅ H ₂₈ O、C ₁₅ H ₂₈ O ₂ 、C ₁₅ H ₂₉ N、C ₁₅ H ₃₀ 、C ₁₅ H ₃₀ O、C ₁₅ H ₃₀ O ₂ 、C ₁₅ H ₃₂ 、C ₁₅ H ₃₂ O、C ₁₅ H ₃₃ O ₃ B、C ₁₅ H ₃₃ N、C ₁₆ H ₁₀ 、C ₁₆ H ₂₂ O ₄ 、C ₁₆ H ₂₄ O、C ₁₆ H ₂₆ 、C ₁₆ H ₂₇ N、C ₁₆ H ₃₀ 、C ₁₆ H ₃₀ O、C ₁₆ H ₃₁ N、C ₁₆ H ₃₂ 、C ₁₆ H ₃₂ O、C ₁₆ H ₃₂ O ₂ 、C ₁₆ H ₃₄ 、C ₁₆ H ₃₄ O、C ₁₆ H ₃₅ N、C ₁₆ H ₃₅ O ₄ P、C ₁₇ H ₂₈ 、C ₁₇ H ₃₂ 、C ₁₇ H ₃₃ N、C ₁₇ H ₃₄ 、C ₁₇ H ₃₄ O、C ₁₇ H ₃₄ O ₂ 、C ₁₇ H ₃₆ 、C ₁₇ H ₃₆ O、C ₁₈ H ₁₂ 、C ₁₈ H ₁₅ O ₄ P、C ₁₈ H ₁₈ O ₅ 、C ₁₈ H ₃₀ 、C ₁₈ H ₃₂ O ₇ 、C ₁₈ H ₃₄ 、C ₁₈ H ₃₄ O ₂ 、C ₁₈ H ₃₄ O ₄ 、C ₁₈ H ₃₅ N、C ₁₈ H ₃₆ 、C ₁₈ H ₃₆ O、C ₁₈ H ₃₆ O ₂ 、C ₁₈ H ₃₇ N、C ₁₈ H ₃₇ NO、C ₁₈ H ₃₈ 、C ₁₈ H ₃₈ O、C ₁₈ H ₃₉ N、C ₁₉ H ₁₆ 、C ₁₉ H ₂₀ O ₄ 、C ₁₉ H ₃₂ 、C ₁₉ H ₃₆ 、C ₁₉ H ₃₆ O ₂ 、C ₁₉ H ₃₈ 、C ₁₉ H ₃₈ O、C ₁₉ H ₃₈ O ₂ 、C ₁₉ H ₄₀ 、C ₂₀ H ₃₂ O、C ₂₀ H ₃₄ 、C ₂₀ H ₃₆ O ₄ 、C ₂₀ H ₃₈ 、C ₂₀ H ₃₈ O ₂ 、C ₂₀ H ₄₀ 、C ₂₀ H ₄₀ O、C ₂₀ H ₄₂ 、C ₂₀ H ₄₃ N、C ₂₁ H ₂₁ O ₄ P、C ₂₁ H ₃₆ 、C ₂₁ H ₄₂ O ₄ 、C ₂₁ H ₄₄ 、C ₂₂ H ₃₄ O ₂ 、C ₂₁ H ₄₀ 、C ₂₁ H ₄₂ 、C ₂₂ H ₄₂ O ₂ 、C ₂₂ H ₄₂ O ₄ 、C ₂₂ H ₄₂ 、C ₂₂ H ₄₄ 、C ₂₂ H ₄₄ O ₂ 、C ₂₂ H ₄₆ 、C ₂₃ H ₄₄ 、C ₂₃ H ₄₆ 、C ₂₃ H ₄₆ O ₂ 、C ₂₃ H ₄₈ 、C ₂₄ H ₃₈ O ₄ 、C ₂₄ H ₄₆ 、C ₂₄ H ₄₈ 、C ₂₄ H ₅₀ 、C ₂₄ H ₅₁ O ₄ P、C ₂₅ H ₄₈ 、C ₂₅ H ₄₈ O ₄ 、C ₂₅ H ₅₀ 、C ₂₅ H ₅₂ 、C ₂₆ H ₄₂ O ₄ 、C ₂₆ H ₄₆ 、C ₂₆ H ₅₀ 、C ₂₆ H ₅₀ O ₄ 、C ₂₆ H ₅₂ 、C ₂₆ H ₅₄ 、C ₂₇ H ₃₆ O ₂ 、C ₂₇ H ₅₂ 、C ₂₇ H ₅₄ 、C ₂₇ H ₅₆ 、C ₂₈ H ₅₄ 、C ₂₈ H ₅₆ 、C ₂₈ H ₅₈ 、C ₂₉ H ₅₆ 、C ₂₉ H ₅₈ 、C ₂₉ H ₆₀ 、C ₃₀ H ₅₄ 、C ₃₀ H ₅₈ 、C ₃₀ H ₆₀ 、C ₃₀ H ₆₂ 、C ₅₇ H ₁₀₄ O ₉ Polyethylene glycol (common molecular weight is 100-6000, common examples are PEG-100, PEG-200, PEG-300, PEG-400, PEG-500, PEG-600, PEG-800, PEG-1000, PEG-1500, PEG-2000, PEG-4000, PEG-6000), pine oil, turpentine, camphoroil, petroleum ether, gasoline, kerosene, solvent naphtha, liquid paraffin, diesel oil, heavy oil, aviation kerosene, lubricating oil, silicone oil, no. 6 solvent oil, no. 70 solvent oil, no. 120 solvent oil, no. 170 solvent oil, no. 200 solvent oil, no. 260 solvent oilSolvent oil, fusel oil, corn oil, rapeseed oil, olive oil, palm oil, cottonseed oil, peanut oil, soybean oil, coconut oil, tea seed oil, sesame oil, rice bran oil, castor oil, linseed oil, safflower oil, cottonseed oil, walnut oil, grape seed oil, pumpkin seed oil, sunflower seed oil, orange oil, perilla oil, almond oil, lemon oil, sea buckthorn oil, evening primrose oil, glass chicory oil, sesame seed oil, hemp oil, linseed oil, camellia seed oil, camellia oil, peony seed oil, lard, tallow, sheep oil, chicken oil, duck oil, whale oil, deep sea fish oil. According to the general rules of disclosure, there are two cases of chemical substances expressed by the above formulas: (1) A formula represents a single structure chemical; (2) Isomers of the same formula but different structures, each formula comprising all isomers of the same formula, are shown in the present specification as representing all isomers associated therewith. The mixing of the organic solvents (liquids) includes the following two cases: (1) Mixing organic solvents (liquids) of different molecular formulas with each other; (2) Organic solvent (liquid) formed by mixing isomers with the same molecular formula.

Preferably, one of the organic solvents (liquids) used for the filtration and displacement in the third step is a solution of a solute as described in [0041] added to the organic solvent (liquid), and the solute is a solute as described in [0040 ].

Preferably, the mixed solution of the inorganic solvent (liquid) and the organic solvent (liquid) used in the filtration and replacement in the third step is a mixed solution of the inorganic solvent (liquid) described in [0039] and the organic solvent (liquid) described in [0041 ]. The mass ratio of the inorganic solvent (liquid) to the organic solvent (liquid) in the mixed solution is 1 (0-100), and the common mass ratio is: 1:0, 1:0.01, 1:0.02, 1:0.03, 1:0.04, 1:0.05, 1:0.06, 1:0.07, 1:0.08, 1:0.09, 1:0.1, 1:0.15, 1:0.2, 1:0.25, 1:0.3, 1:0.35, 1:0.4, 1:0.45, 1:0.5, 1:0.55, 1:0.6, 1:0.65, 1:0.7, 1:0.75, 1:0.8, 1:0.85, 1:0.9, 1:0.95, 1:1, 1:1.1, 1:1.2, 1:1.3, 1:1.4, 1:1.5, 1:1.6, 1:1.7, 1:1.8, 1:1.9, 1:2, 1:2.2, 1:2.5, 1:1:0.8, 1:0.3, 1:2.2.2, 1:2.5, 1:2.1.2.3, 1:2.2.1.2, 1:2.1.2.5, 1:2.2.1.2.1.0.9; 1:2.8, 1:2.9, 1:3, 1:3.1, 1:3.2, 1:3.3, 1:3.4, 1:3.5, 1:3.6, 1:3.7, 1:3.8, 1:3.9, 1:4, 1:4.1, 1:4.2, 1:4.3, 1:4.4, 1:4.5, 1:4.6, 1:4.7, 1:4.8, 1:4.9, 1:5, 1:6, 1:7, 1:8, 1:9, 1:10, 1:11, 1:12, 1:13, 1:14, 1:15, 1:20, 1:25, 1:30, 1:35, 1:40, 1:45, 1:50, 1:55, 1:60, 1:65, 1:70, 1:75, 1:80, 1:85, 1:90, 1:100.

Preferably, the mixed solution of the inorganic solvent (liquid) and the organic solvent (liquid) used in the filtration and displacement in the third step further comprises a solution formed by adding a solute to the mixed solution described in [0043], wherein the solute is the solute described in [0040 ].

Preferably, the filtering and replacing in the third step further comprises uniformly dispersing graphene in the first solvent (liquid), and replacing with the second solvent (liquid) to obtain a solution in which graphene is uniformly dispersed in the second solvent (liquid). The second solvent (liquid) used for replacement is one of the following three: the mixed solution of the inorganic solvent (liquid), the organic solvent (liquid) and the organic solvent (liquid) is the solution described in [0039], [0040], [0041], [0042], [0043], [0044 ].

Preferably, in order to meet the requirement of the graphene solution concentration in the application, the method for preparing the graphene can add more solvent (liquid) into the solution or filter and remove the redundant solvent (liquid) in the solution.

Preferably, in order to meet the requirement of drying materials in application, the method for preparing graphene is used for drying in a common mode to obtain dried graphene. Common drying modes include: air drying, natural air drying, freeze drying, vacuum drying, spray drying, microwave drying, and supercritical drying.

Preferably, the graphene prepared by the method can be used in the following fields: lithium ion batteries, sodium ion batteries, potassium ion batteries, magnesium ion batteries, solid state batteries, conductive agents, graphene paper, super capacitors, solar cells, light transmitting coatings, flexible display devices, transparent conductive films, photodetectors, heat dissipating coatings, heat sinks, heat generating sheets, conductive coatings, conductive inks, conductive viscose, antistatic coatings, antistatic plastics, conductive rubber, conductive films, corrosion resistant coatings, metal composites, cable materials, hydrogels, aerogels, 3D printing materials, electromagnetic shielding materials, chemical sensors, biological sensors, blood sensors, gas sensors, drug carriers, medical imaging, building materials, abrasion resistant coatings, reinforced plastics, graphene tires, foaming materials, water impermeable plastics, reinforcing materials, graphene fibers, graphene brake sheets, carbon composites, oil absorbing sponges, seawater desalination, sewage purification, seawater uranium extraction, seawater lithium extraction, separation membranes, ion sieves, masks, catalyst carriers, hydrogen evolution catalysts, oxygen evolution catalysts.

The beneficial effects of the invention are as follows: the invention provides a method for preparing graphene, which can uniformly disperse graphene in various solvents (liquids) while reducing graphene oxide, and can efficiently and conveniently remove various impurities in the graphene. The solvent (liquid) for dispersing the graphene comprises various inorganic solvents (liquids), organic solvents (liquids) and mixed solutions composed of the inorganic solvents (liquids) and the organic solvents (liquids). The impurities removed include: impurities in the graphite powder, impurities introduced in the preparation of graphene oxide, impurities introduced in the reduction of graphene, and impurities introduced in the preparation of graphene solution. The invention is beneficial to improving the quality of graphene, reducing the production cost of graphene and conveniently adjusting the concentration of graphene solution.

The accompanying drawings of the specification.

Fig. 1 is a scanning electron microscope image of graphene oxide.

Fig. 2 is a scanning electron microscope image of graphene.

Fig. 3 is an X-ray diffraction pattern of graphene oxide.

Fig. 4 is an X-ray diffraction pattern of graphene prepared in example 1.

Fig. 5 is a measured value, average value, and standard deviation of the concentration of graphene solution (aqueous solution).

Fig. 6 is a measured value, average value, and standard deviation of the concentration of graphene solution (ethanol solution).

Fig. 7 is a conductivity test result of a graphene solution.

FIG. 8 is a schematic diagram of the steps of the present invention.

Detailed description of the preferred embodiments.

Example 1.

1 g graphene oxide is taken and dissolved in 5L pure water, and is stirred ultrasonically for 2 hours to form 0.2 mg/mL graphene oxide solution.

And adding 20-g ascorbic acid into the solution, uniformly mixing, and standing at 15 ℃ for reaction for 24 hours to obtain a chemically reduced graphene solution.

500 mL of 30% hydrogen peroxide solution was added to the above solution, and the mixture was stirred at a rotation speed of 100 r/min at 15℃for 5 minutes, followed by standing for 24 hours, to obtain a uniformly dispersed graphene solution.

The above solution was filtered using a 350 mesh screen to give a black viscous sample.

And adding pure water into the sample for multiple times, and repeatedly filtering to remove impurities until the conductivity of the filtrate is equal to that of the pure water, so as to obtain a solution in which graphene is uniformly dispersed in the pure water.

Example 2.

Adding 10 g ascorbic acid into the solution, uniformly mixing, and standing at 0 ℃ for reaction for 60 hours to obtain a chemically reduced graphene solution.

60 g sodium percarbonate is added into the solution, the mixture is stirred and reacted for 5 minutes at the rotating speed of 100 r/min at the temperature of 0 ℃, and then the mixture is stirred and reacted for 24 hours at the rotating speed of 10 r/min, so that the uniformly dispersed graphene solution is obtained.

The above solution was filtered using a 300 mesh screen to give a black viscous sample.

And adding ethanol into the solution for multiple times, repeatedly filtering, and replacing water with ethanol to obtain a solution in which graphene is uniformly dispersed in ethanol.

Example 3.

And adding 20-g ascorbic acid into the solution, uniformly mixing, and standing at 5 ℃ for reaction for 24 hours to obtain a chemically reduced graphene solution.

200 ml of 30% hydrogen peroxide solution and 30 g sodium carbonate were added to the above solution, and after stirring and reacting at a rotation speed of 100 r/min for 5 minutes at 5 ℃, the mixture was allowed to stand for 20 hours to obtain a uniformly dispersed graphene solution.

The above solution was filtered using a 400 mesh screen to give a black viscous sample.

And adding ethanol into the sample for multiple times, repeatedly filtering to remove impurities until the conductivity of the filtrate is equal to that of the ethanol, and obtaining a solution in which graphene is uniformly dispersed in the ethanol.

Example 4.

Adding 5 g ascorbic acid and 15 g oxalic acid into the solution, uniformly mixing, and standing at 5 ℃ for reaction for 36 hours to obtain a chemically reduced graphene solution.

Adding 40 g sodium bicarbonate into the solution, stirring at a rotation speed of 100 r/min for reaction for 5 minutes at a temperature of 5 ℃, and standing for reaction for 16 hours to obtain a uniformly dispersed graphene solution.

And adding N-methyl pyrrolidone into the solution for multiple times, repeatedly filtering, and replacing ethanol with the N-methyl pyrrolidone to obtain a solution in which the graphene is uniformly dispersed in the N-methyl pyrrolidone.

Example 5.

And adding 20-g ascorbic acid into the solution, uniformly mixing, and standing at 5 ℃ for reaction for 32 hours to obtain a chemically reduced graphene solution.

60 g potassium dichromate and 20 g ammonium sulfate are added into the solution, and after stirring and reacting for 5 minutes at 20 ℃ and a rotating speed of 100 r/min, the solution is kept stand for 24 hours, so that a uniformly dispersed graphene solution is obtained.

And adding ethyl acetate into the solution for multiple times, repeatedly filtering, and replacing ethanol with ethyl acetate to obtain a solution in which graphene is uniformly dispersed in ethyl acetate.

Example 6.

And adding 35 g ascorbic acid into the solution, uniformly mixing, and standing at 10 ℃ for reaction for 24 hours to obtain a chemically reduced graphene solution.

50 g potassium permanganate is added into the solution, stirred at the rotating speed of 100 r/min for reaction for 5 minutes at the temperature of 20 ℃, and then the mixture is stood for reaction for 24 hours, so that the uniformly dispersed graphene solution is obtained.

And adding gasoline into the solution for multiple times, repeatedly filtering, and replacing ethanol with gasoline to obtain a solution with graphene uniformly dispersed in the gasoline.

Example 7.

And adding 15 g ascorbic acid and 5 g hydrazine hydrate into the solution, uniformly mixing, and standing at 10 ℃ for reaction for 24 hours to obtain a chemically reduced graphene solution.

500 ml of 30% hydrogen peroxide solution was added to the above solution, and the mixture was stirred at 20℃and a rotation speed of 100 r/min for 5 minutes, followed by standing for 24 hours, to obtain a uniformly dispersed graphene solution.

And adding methanol into the solution for multiple times, repeatedly filtering, and replacing ethanol with methanol to obtain a solution in which graphene is uniformly dispersed in the methanol.

And adding acetone into the solution for multiple times, repeatedly filtering, and replacing methanol with acetone to obtain a solution in which graphene is uniformly dispersed in the acetone.

Example 8.

And adding 25 g sodium ascorbate into the solution, uniformly mixing, and standing at 10 ℃ for reaction for 24 hours to obtain a chemically reduced graphene solution.

And adding N, N-dimethylformamide into the solution for multiple times, repeatedly filtering, and replacing water by using the N, N-dimethylformamide to obtain a solution in which the graphene is uniformly dispersed in the N, N-dimethylformamide.

Example 9.

And adding 40-g ascorbic acid into the solution, uniformly mixing, and standing at 0 ℃ for reaction for 28 hours to obtain a chemically reduced graphene solution.

1000 mL of 30% hydrogen peroxide solution was added to the above solution, and after stirring at a rotation speed of 100 r/min at 5℃for 5 minutes, the solution was allowed to stand for 24 hours to obtain a uniformly dispersed graphene solution.

And adding N-methyl pyrrolidone into the solution for multiple times, repeatedly filtering, and replacing water by using the N-methyl pyrrolidone to obtain a solution in which the graphene is uniformly dispersed in the N-methyl pyrrolidone.

Example 10.

20 mL of 25% ammonia water solution and 15 g glucose were added to the above solution, and the mixture was stirred at a stirring speed of 100 r/min at 90℃for 2 hours to obtain a chemically reduced graphene solution.

400 mL of 30% hydrogen peroxide solution was added to the above solution, and after stirring and reacting at a rotation speed of 100 r/min at 5℃for 5 minutes, the solution was allowed to stand for 24 hours to obtain a uniformly dispersed graphene solution.

And placing the sample into carbon dioxide supercritical drying equipment, and replacing ethanol in the sample by using carbon dioxide to obtain the graphene material subjected to carbon dioxide supercritical drying.

Example 11.

Adding a proper amount of ammonia water into the solution, adjusting the pH to be 11, adding 20 g glucose, and stirring at the rotation speed of 600 r/min at the temperature of 90 ℃ for reaction for 2 hours to obtain a chemically reduced graphene solution.

13.5 g ammonium chloride and 17.25 g sodium nitrite are added into the solution, and the mixture is stirred and reacted for 4 hours at the temperature of 85 ℃ and the rotating speed of 100 r/min, so as to obtain the uniformly dispersed graphene solution.

And adding hydrogen peroxide solution into the solution for multiple times, repeatedly filtering, and replacing water by using the hydrogen peroxide solution to obtain a solution in which graphene is uniformly dispersed in the hydrogen peroxide solution.

Example 12.

Adding a proper amount of ammonia water into the solution, adjusting the pH to be 11, adding 15 g glucose, and stirring at the rotation speed of 120 r/min for reaction for 2 hours at the temperature of 90 ℃ to obtain a chemically reduced graphene solution.

And adding 20 g ammonium bicarbonate and 20 g ammonium nitrite into the solution, and stirring at a rotating speed of 30 r/min for reaction for 3 hours at 90 ℃ to obtain a uniformly dispersed graphene solution.

And adding a sodium chloride solution into the solution for multiple times, repeatedly filtering, and replacing water by using the sodium chloride solution to obtain a solution in which the graphene is uniformly dispersed in the sodium chloride solution.

Example 13.

Adding a proper amount of ammonia water into the solution, adjusting the pH to be 11, adding 20 g hydrazine hydrate, and stirring at the rotating speed of 120 r/min at the temperature of 90 ℃ for reaction for 2 hours to obtain a chemically reduced graphene solution.

500 mL of 30% hydrogen peroxide solution was added to the above solution, and the mixture was stirred at a rotation speed of 100 r/min at 20℃for 5 minutes, followed by standing for 24 hours, to obtain a uniformly dispersed graphene solution.

And adding rapeseed oil into the solution for multiple times, repeatedly filtering, and replacing ethanol by utilizing the rapeseed oil to obtain a solution with graphene uniformly dispersed in the rapeseed oil.

Example 14.

Adding 2 g ascorbic acid, 13g oxalic acid and 5 g citric acid into the solution, uniformly mixing, and standing at 10 ℃ for reaction for 32 hours to obtain a chemically reduced graphene solution.

20 g sodium carbonate, 20 mL of 37% hydrogen chloride solution and 15 g aluminum powder are added into the solution, and after stirring and reacting for 15 minutes at the rotating speed of 100 r/min at the temperature of 20 ℃, standing and reacting for 24 hours, the uniformly dispersed graphene solution is obtained.

And adding chloroform into the solution for multiple times, repeatedly filtering, and replacing ethanol with chloroform to obtain a solution in which graphene is uniformly dispersed in the chloroform.

Example 15.

Adding 10 g hydrazine hydrate and 20 g oxalic acid into the solution, uniformly mixing, and standing at 15 ℃ for reaction for 24 hours to obtain a chemically reduced graphene solution.

50 g sodium bicarbonate and 10 g aluminum powder are added into the solution, and the mixture is stirred and reacted for 24 hours at 15 ℃ and the rotating speed of 100 r/min, so as to obtain the uniformly dispersed graphene solution.

And adding dimethylbenzene into the solution for multiple times, repeatedly filtering, and replacing ethanol with dimethylbenzene to obtain a solution with graphene uniformly dispersed in dimethylbenzene.

Example 16.

Adding 10 g sodium ascorbate, 10 g citric acid and 10 g oxalic acid into the solution, uniformly mixing, and standing at 15 ℃ for reaction for 24 hours to obtain a chemically reduced graphene solution.

10 mL of 37% hydrogen chloride solution and 20 g zinc powder are added into the solution, and after stirring and reacting for 5 minutes at the speed of 100 r/min at the temperature of 20 ℃, the solution is stood for reacting for 24 hours, so as to obtain the uniformly dispersed graphene solution.

Acetonitrile is added to the solution for a plurality of times, and the filtration is repeated, and water is replaced by acetonitrile, so that the solution in which graphene is uniformly dispersed in acetonitrile is obtained.

Example 17.

Adding a proper amount of ammonia water into the solution, adjusting the pH to be 11, adding 20 g glucose, and stirring at the rotation speed of 120 r/min for reaction for 2 hours at the temperature of 90 ℃ to obtain a chemically reduced graphene solution.

400 mL of 30% hydrogen peroxide solution and 20 g zinc powder were added to the above solution, and after stirring and reacting at 20℃and a rotational speed of 100 r/min for 5 minutes, the mixture was allowed to stand for 24 hours to obtain a uniformly dispersed graphene solution.

And adding ethylene glycol into the solution for multiple times, repeatedly filtering, and replacing water by using the ethylene glycol to obtain a solution in which the graphene is uniformly dispersed in the ethylene glycol.

Example 18.

1 g graphene oxide was dissolved in 250 mL of N, N-dimethylformamide and stirred ultrasonically for 2 hours to form a graphene oxide solution of 4 mg/mL.

Adding 1 g ascorbic acid and 4 g sodium borohydride into the solution, and stirring at the rotation speed of 200 r/min at 15 ℃ for reaction for 6 hours to obtain a chemically reduced graphene solution.

50 mL of 30% hydrogen peroxide solution was added to the above solution, and the mixture was stirred at 20℃and a rotation speed of 200 r/min for 5 minutes, followed by standing for 18 hours, to obtain a uniformly dispersed graphene solution.

And adding N, N-dimethylformamide into the solution for multiple times, repeatedly filtering, and removing impurities to obtain a solution in which the graphene is uniformly dispersed in the N, N-dimethylformamide.

Example 19.

Adding 5 g ascorbic acid and 15 g oxalic acid into the solution, uniformly mixing, and standing at 45 ℃ for reaction for 12 hours to obtain a chemically reduced graphene solution.

Adding 40 g sodium bicarbonate into the solution, stirring at a rotating speed of 100 r/min for reaction for 5 minutes at 20 ℃, and standing for reaction for 16 hours to obtain a uniformly dispersed graphene solution.

And adding a mixed solution of methanol and ethanol into the solution for multiple times, repeatedly filtering, and replacing water by using the mixed solution of methanol and ethanol to obtain a solution in which graphene is uniformly dispersed in the mixed solution of methanol and ethanol.

And (3) carrying out spray drying on the solution to obtain the dried graphene.

Summary of the effects of the invention.

The degree of reduction of graphene can be characterized by an X-ray diffraction pattern. The graphene oxide surface contains a large number of oxygen-containing functional groups, and the oxygen-containing functional groups increase the interplanar spacing of the graphene sheets. The interplanar spacing becomes smaller after reduction to remove oxygen-containing functional groups. Bragg's law by crystalline X-ray diffraction: 2dsin theta=nλ, and according to the 2θ angle of the characteristic peak in the spectrum, the interplanar distance d can be calculated, so that the reduction effect of the graphene is judged. The X-ray wavelength used in the detection was 0.15406 nm, and the diffraction order n was 1. Fig. 5 is an X-ray diffraction pattern of graphene oxide, 2θ=12.93°, interplanar spacing d= 0.717858 nm. Fig. 6 is an X-ray diffraction pattern of graphene prepared in example 1, 2θ=25.22°, interplanar spacing d= 0.352841 nm. It is evident that the interplanar spacing d after chemical reduction is reduced, indicating that the oxygen-containing functional groups are removed by chemical reduction and the graphene is reduced.

The uniformity of the dispersion of graphene in a solution can be judged by measuring the mean and standard deviation of the concentration. A total of 12 samples were measured, 7 samples were taken from each group, and the mean and standard deviation of the concentrations were calculated from the measured values. FIG. 5 shows the measurement result of graphene solution (aqueous solution) concentration, wherein the average value of sample concentration is distributed between 5.85 and 6.01 mg/mL, and the standard deviation is between 0.042 and 0.108 mg/mL. FIG. 6 shows the measurement result of the concentration of graphene solution (ethanol solution), wherein the average value of the concentration of a sample is distributed between 5.91 and 6.00 mg/mL, and the standard deviation is between 0.051 and 0.112 mg/mL. And experimental errors are considered, the standard deviation of each sample is small, the concentration is uniform, and the uniformity of the dispersion of graphene in water and ethanol is good. After the dispersing agent is added, the surface of the graphene adsorbs gas, so that more space is reserved between the sheets, and other materials can enter the sheets to form the composite material. After the solution is replaced, a small amount of gas escapes, and the uniformity of dispersion is unchanged. In conclusion, the method is beneficial to compositing graphene with other materials, so that the graphene has more application scenes in downstream industries.

The effect of removing impurities in graphene can be illustrated by the conductivity of a solution, and the lower the conductivity of the solution is, the lower the impurity content is. FIG. 7 shows the conductivity of graphene solution, the conductivity before filtration is high, and the conductivity after multiple filtration is equal to the conductivity of the solution, indicating that impurities in the solution are removed. Removed impurities include, but are not limited to: (1) impurities contained in graphite powder; (2) The preparation method comprises the steps of introducing sodium, potassium, manganese, sulfur, nitrogen, chlorine, phosphorus and other impurity elements into reagents such as sulfuric acid, nitrate, chlorate, potassium permanganate, hydrochloric acid, phosphoric acid and the like used in the preparation of graphene oxide; (3) unreacted reducing agent, chemical reduction product; (4) impurities introduced in preparing the graphene solution. The method is simple, quick and efficient, is beneficial to reducing the production cost of graphene, and is an efficient and feasible purification mode.

In summary, the method for preparing graphene provided by the invention reduces graphene, simultaneously makes graphene uniformly dispersed in various solutions, and can efficiently and conveniently remove various impurities in graphene. The solution for dispersing the graphene comprises various inorganic solvents (liquids), organic solvents (liquids) and mixed solutions consisting of the inorganic solvents (liquids) and the organic solvents (liquids). The impurities removed include: impurities in the graphite powder, impurities introduced during preparation, impurities introduced during reduction, and impurities introduced during preparation of the graphene solution. The invention is beneficial to improving the quality of graphene, reducing the production cost of graphene and conveniently adjusting the concentration of graphene solution.

The invention is not a matter of the known technology.

The above embodiments are provided to illustrate the technical concept and features of the present invention and are intended to enable those skilled in the art to understand the content of the present invention and implement the same, and are not intended to limit the scope of the present invention. All equivalent changes or modifications made in accordance with the spirit of the present invention should be construed to be included in the scope of the present invention.

Claims

1. A method for preparing graphene, comprising the steps of:

2. The method for preparing graphene according to claim 1, wherein the reducing agent in the first step is one or more of the following: organic acids, borohydrides, citrates, ascorbates, alcohols, sugars, amino acids, sulfur-containing reducing agents, nitrogen-containing reducing agents, reducing plant extracts, metals, inorganic acids, bases; the mass ratio of the graphene oxide to the reducing agent is 1 (1-200).

3. The method for preparing graphene according to claim 1, wherein the reaction time of the chemical reduction in the first step is 0 to 120 hours, the reaction temperature is-10 ℃ to 100 ℃, and the stirring speed of the reaction is 0 to 3000 r/min.

4. The method for preparing graphene according to claim 1, wherein the dispersant in the second step is one or more of the following: peroxides, superoxides, percarbonates, persulfates, permanganates and permanganates, manganates, ferrates and ferrates, chlorates and chlorates, carbonates, bicarbonates, bisulphates, ammonium salts, dichromates and bichromates, iodic acids and iodates, bromic and bromates, nitrous acids and nitrites, metals, metal hydrides, acids, bases, perborates, halogen intermetallics.

5. The method for preparing graphene according to claim 1, wherein the mass ratio of the dispersant to the initial graphene oxide in the second step is (1-1000): 1.

6. The method for preparing graphene according to claim 1, wherein the reaction time after adding the dispersing agent into the solution obtained in the first step and mixing is 1 minute-120 hours, the reaction temperature is-10-100 ℃, and the reaction stirring speed is 0-3000 r/min.

7. The method for preparing graphene according to claim 1, wherein the filtration and substitution in the third step is performed by one or more of the following combinations: normal pressure filtration, reduced pressure filtration, gravity filtration, vacuum filtration, centrifugal filtration, dialysis and soaking replacement; the equipment used is one or more of the following combinations: a filter screen, a filter membrane, a filter bag and a filter paper with the mesh number of 10-5000 meshes.

8. The method for preparing graphene according to claim 1, wherein the solvent (liquid) is added for filtration and displacement in the third step, and the solvent (liquid) used is one of the following three types: an inorganic solvent (liquid), an organic solvent (liquid), and a mixed solution of the inorganic solvent (liquid) and the organic solvent (liquid); wherein the inorganic solvent (liquid) is any one of the following: water, a solution formed by adding solute into water; wherein the organic solvent (liquid) is one or more of the following mixture: hydrocarbon solvents (liquids), halogenated hydrocarbon solvents (liquids), alcohol solvents (liquids), phenol solvents (liquids), ether solvents (liquids), aldehyde solvents (liquids), ketone solvents (liquids), ester solvents (liquids), acid and acid anhydride solvents (liquids), amine solvents (liquids), amide solvents (liquids), nitrile solvents (liquids), nitrogen-containing compound solvents (liquids), sulfur-containing compound solvents (liquids), and solutions formed by adding solutes to the above-mentioned various organic solvents (liquids).

9. The method for preparing graphene according to claim 1, wherein the removing of impurities in the graphene solution in the third step means adding solvent (liquid) into the solution containing impurities in which graphene is uniformly dispersed, filtering and replacing until the content of impurities in the graphene solution reaches the required standard of the downstream application on the content of impurities in the graphene solution, and obtaining the solution in which graphene is uniformly dispersed after removing the impurities.

10. The method for preparing graphene according to claim 1, wherein the filtration and displacement in the third step further comprises uniformly dispersing graphene in a solution of the first solvent (liquid), filtering and displacement using the second solvent (liquid) to obtain a solution of graphene uniformly dispersed in the second solvent (liquid), and filtering and displacement using one of the following three solvents (liquid): an inorganic solvent (liquid), an organic solvent (liquid), and a mixed solution composed of the inorganic solvent (liquid) and the organic solution; wherein the inorganic solvent (liquid) is any one of the following: water, a solution formed by adding solute into water; the organic solvent (liquid) is one or more of the following mixed materials: hydrocarbon solvents (liquids), halogenated hydrocarbon solvents (liquids), alcohol solvents (liquids), phenol solvents (liquids), ether solvents (liquids), aldehyde solvents (liquids), ketone solvents (liquids), ester solvents (liquids), acid and acid anhydride solvents (liquids), amine solvents (liquids), amide solvents (liquids), nitrile solvents (liquids), nitrogen-containing compound solvents (liquids), sulfur-containing compound solvents (liquids), and solutions formed by adding solutes to the above-mentioned various organic solvents (liquids).