CN115477372A - Preparation method and application of carbon nanotube loaded phosphorus nitride electrode material - Google Patents
Preparation method and application of carbon nanotube loaded phosphorus nitride electrode material Download PDFInfo
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/469—Treatment of water, waste water, or sewage by electrochemical methods by electrochemical separation, e.g. by electro-osmosis, electrodialysis, electrophoresis
- C02F1/4691—Capacitive deionisation
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/66—Treatment of water, waste water, or sewage by neutralisation; pH adjustment
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B60/00—Obtaining metals of atomic number 87 or higher, i.e. radioactive metals
- C22B60/02—Obtaining thorium, uranium, or other actinides
- C22B60/0204—Obtaining thorium, uranium, or other actinides obtaining uranium
- C22B60/0217—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes
- C22B60/0252—Obtaining thorium, uranium, or other actinides obtaining uranium by wet processes treatment or purification of solutions or of liquors or of slurries
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B7/00—Working up raw materials other than ores, e.g. scrap, to produce non-ferrous metals and compounds thereof; Methods of a general interest or applied to the winning of more than two metals
- C22B7/006—Wet processes
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/04—Treating liquids
- G21F9/06—Processing
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
- C02F2001/46133—Electrodes characterised by the material
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
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Abstract
The invention discloses a preparation method and application of a carbon nano tube loaded phosphorus nitride electrode material. The carbon nano tube loaded phosphorus nitride electrode material has a wide application range, uranium enrichment and recovery are realized when the carbon nano tube loaded phosphorus nitride electrode material is used for uranium-containing wastewater treatment, the carbon nano tube loaded phosphorus nitride electrode material is used as a composite carbon electrode material which is simple and convenient to synthesize, the advantages of high adsorption capacity, high adsorption rate and the like are shown in the uranium-containing wastewater treatment process, and uranium ions can be rapidly extracted from a water body.
Description
Technical Field
The invention relates to the technical field of capacitive deionization, in particular to a preparation method and application of a carbon nano tube loaded phosphorus nitride electrode material.
Background
The process of industrial modernization promotes the adjustment of world energy structures, and the proportion of clean green energy is continuously increased. The continuous increase of nuclear power capacity alleviates the contradiction between energy shortage and economic development. The proliferation of the nuclear industry also brings a number of issues that need to be addressed urgently. The demand of uranium ores is increasing, and as a uranium-depleted country in China, the uranium ores are highly dependent on the outside, and export of the uranium ores as strategic reserve resources is restricted by many countries. The mining mode of uranium ores in China is mainly a leaching method. The uranium mining process can produce a large amount of uranium-bearing waste water, and these waste waters can invade soil, move along with groundwater and surface water. Uranium has extremely high biological toxicity, chemical toxicity and radioactivity, and can produce destructive influence on the natural environment and human social activities along with the enrichment of an ecological chain. However, most of the prior uranium-bearing wastewater treatment technologies have the defects of high cost, long period, lack of selectivity and the like. Therefore, the research on how to economically and efficiently remove uranium ions from uranium-containing wastewater selectively can reduce the harm of the uranium-containing wastewater to the natural environment and improve the utilization rate of uranium ores.
In order to solve the potential threat of uranium-containing wastewater to human life, researchers develop a series of uranium removal technologies, such as membrane separation, ion exchange, chemical precipitation, adsorption and other separation means. However, the method has the limitations of poor low-concentration removal capability, easy generation of secondary pollution, difficult treatment of residual medicament, high energy consumption, limited ion exchange capacity, low adsorption efficiency, easy pollution of membranes and the like. Electrochemical methods are becoming an effective and simple method for removing heavy metals from water as a new water treatment technology. Electro-adsorption means that substances dissolved in liquid are adsorbed on electrodes, and surface bonding is promoted by an electric field. A typical electro-adsorption module consists of two electrodes through which micro-saline passes. Electrosorption is induced by polarizing the electrodes with an applied bias. Conventionally, electrodes for electro-adsorption are made of an electrically conductive non-ferroelectric material, such as porous carbon. During charging, to satisfy charge neutrality, oppositely charged ions are attracted to the polarized electrode by coulomb forces and accumulate charge on the electrode surface, as in a capacitor. At the surface of the polarizing electrode, the ions form an electric double layer. The removal of ions from a solution using this phenomenon is called Capacitive Deionization (CDI). In turn, discharges the electrodes. Upon discharge, ions are released and the electrodes are regenerated. Because the CDI process stores charge, the energy used in the electrosorption process can be partially recovered, making it potentially more energy efficient than other ion removal techniques. In recent years, the definition of CDI is expanded, and a novel electrode material based on faradaic principles such as ion intercalation, redox reaction and pseudocapacitance appears, so that not only is the adsorption performance greatly improved, but also the ion selectivity is enhanced. In radioactive waste waters, the uranium is predominantly in the form of hexavalent uranyl cations (UO) 2 2+ ) Exist in the form of (1). Therefore, CDI technology can be used to extract uranium from wastewater. So far, the research of the CDI technology for removing uranium from wastewater is still in the initial stage, mainly focusing on carbon materials, such as graphene, activated carbon, carbon nanotubes and the like, and the uranium adsorption capacity is maintained between 200 and 500mg g -1 Meanwhile, the application of the CDI technology in uranium-containing wastewater is limited due to the lower adsorption capacity.
Disclosure of Invention
The invention aims to provide a preparation method and application of a carbon nano tube loaded phosphorus nitride electrode material, and particularly relates to application of the carbon nano tube loaded phosphorus nitride electrode material in extraction of uranium ions in sewage.
In order to achieve the above purpose, the invention adopts the following technical scheme,
firstly, the invention provides a preparation method of a carbon nano tube loaded phosphorus nitride electrode material, which comprises the following steps:
step (1): uniformly dispersing the carbon nano tube in deionized water, heating to 90-100 ℃ in an oil bath, and reacting for 8-10h to obtain a hydroxylated carbon nano tube;
step (2): adding the hydroxylated carbon nano tube into an organic solvent, and uniformly stirring to obtain a mixture A;
and (3): adding hexachlorocyclotriphosphazene into the mixture A, performing ultrasonic treatment, adding sodium amide, and continuing ultrasonic treatment to obtain a mixture B;
and (4): putting the mixture B into a high-pressure reaction kettle, heating to 150-250 ℃, and reacting for 8-10h to obtain a carbon nano tube loaded phosphorus nitride crude product;
and (5): and (3) putting the carbon nano tube loaded phosphorus nitride crude product into a centrifuge, washing for 3 times by using absolute ethyl alcohol, and then putting the centrifuge into a freeze drying instrument for drying for 8-36h to obtain the carbon nano tube loaded phosphorus nitride electrode material.
Preferably, in the step (2), the organic solvent is a benzene solution.
Preferably, in the step (3), the mass ratio of the hexachlorocyclotriphosphazene to the hydroxylated carbon nanotube is 2:1-8:1.
preferably, in the step (3), the ultrasonic time is 30min.
Preferably, in the step (4), the heating temperature is 180 to 220 ℃.
Secondly, the invention also provides a preparation method of the asymmetric capacitance deionization module containing the carbon nano tube loaded with the phosphorus nitride electrode material, which comprises the following steps:
(a) Preparing a cathode electrode: uniformly mixing the prepared carbon nanotube-loaded phosphorus nitride electrode material serving as an active substance with conductive carbon black, adding absolute ethyl alcohol, uniformly stirring, adding a binder, and uniformly stirring; coating the obtained mixture on graphite paper, wherein the coating thickness is 100-600 mu m, and drying the coated graphite paper at 40-80 ℃ for 2-24h to obtain a cathode electrode for capacitive deionization, wherein the active substance is phosphorus nitride loaded by a carbon nano tube;
(b) Preparing an anode electrode: uniformly mixing active carbon serving as an active substance with conductive carbon black, adding absolute ethyl alcohol, uniformly stirring, adding a binder, and uniformly stirring; coating the obtained mixture on graphite paper, wherein the coating thickness is 100-600 mu m, and drying the coated graphite paper at 40-80 ℃ for 2-24h to obtain an anode electrode for capacitive deionization with active substances as activated carbon;
(c) Assembling an asymmetric capacitance deionization module: and sequentially assembling the current collector, the titanium strip, the cathode electrode for capacitive deionization of phosphorus nitride loaded by carbon nano tubes with active substances, non-woven fabric, a silica gel gasket, the non-woven fabric, the anode electrode for capacitive deionization with active substances of activated carbon, the titanium strip and the current collector to obtain the asymmetric capacitive deionization module of the carbon nano tube loaded phosphorus nitride electrode material.
Preferably, in the step (a), the binder is a mixed solution of polyvinyl butyral and polyvinyl pyrrolidone.
Preferably, the mass ratio of the polyvinyl butyral to the polyvinyl pyrrolidone in the mixed solution is 2.
The invention further provides a method for applying the asymmetric capacitive deionization module containing the carbon nano tube loaded with the phosphorus nitride electrode material to uranium ion extraction, and the method comprises the following steps:
and (2) connecting the assembled asymmetric capacitance deionization module containing the carbon nano tube loaded phosphorus nitride electrode material with a power supply, a peristaltic pump and 100mL uranium-containing waste liquid through hoses, pumping the uranium-containing waste liquid into a channel between two electrodes at a certain flow rate through the peristaltic pump, respectively adsorbing positive and negative ions in the solution to the two electrodes under the action of voltage, adjusting the pH value to be 3-8, setting the power supply voltage to be 0-1.2V, and setting the adsorption time to be 0-420min.
Preferably, the pH value is adjusted by using 1mol/L hydrochloric acid and 1mol/L sodium hydroxide solution.
Preferably, the flow rate of the peristaltic pump is 15mL/min, the voltage is set to be 1.2V, and the adsorption time is 300min.
Compared with the prior art, the invention has the beneficial effects that:
1. the preparation process of the carbon nanotube loaded phosphorus nitride electrode material has the advantages of simple process, short preparation period, wide raw material source, high yield, low cost and the like.
2. The carbon nano tube loaded phosphorus nitride electrode material has a wide application range, can be used for treating uranium-containing wastewater with different initial concentrations and simultaneously has the advantages of recycling the treasure uranium ore resource, and shows the advantages of high adsorption capacity, high adsorption rate and the like in the uranium-containing wastewater treatment process compared with common carbon materials because the carbon nano tube loaded phosphorus nitride is used as a composite carbon material.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings used in the description of the embodiments will be briefly introduced below, and it is obvious that the drawings in the description below are only some embodiments of the present invention, and it is obvious for those skilled in the art that other drawings can be obtained based on these drawings without making any inventive changes.
Fig. 1 is an X-ray diffraction spectrum of the carbon nanotube-supported phosphorus nitride electrode material prepared in the first example;
FIG. 2 is a graph of an infrared absorption spectrum of the carbon nanotube-supported phosphorus nitride electrode material prepared in the first example;
FIG. 3 is a Scanning Electron Microscope (SEM) lens of the carbon nanotube supported phosphorus nitride electrode material prepared in the first embodiment;
FIG. 4 is a diagram of a carbon nanotube-loaded phosphorus nitride electrode sheet fabricated in the second example;
FIG. 5 is a graph showing the change of adsorption capacity with time in the process of electro-adsorption of the carbon nanotube-loaded phosphorus nitride electrode in the third embodiment;
fig. 6 is a comparison graph of adsorption conditions of uranium ions by the carbon nanotube-loaded phosphorus nitride electrode at different pH values in the fourth example;
FIG. 7 is a comparison graph of adsorption of uranium ions by a carbon nanotube-loaded phosphorus nitride electrode at different initial uranium concentrations in example five;
fig. 8 is a graph comparing the adsorption of uranium ions by the carbon nanotube-loaded phosphorus nitride electrode under different applied voltages in example six.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more clearly and completely apparent, the technical solutions in the embodiments of the present invention will be described below with reference to the accompanying drawings in the embodiments of the present invention, and it should be noted that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The first embodiment is as follows: preparing the carbon nano tube loaded phosphorus nitride electrode material.
Step (1): taking 100mg of multi-walled carbon nanotubes, uniformly dispersing the carbon nanotubes in deionized water, heating to 90-100 ℃ in an oil bath, and reacting for 10 hours to obtain hydroxylated carbon nanotubes;
step (2): adding the obtained hydroxylated carbon nano tube into a benzene solution, and uniformly stirring to obtain a mixture A;
and (3): adding 500mg of hexachlorocyclotriphosphazene into the mixture A, performing ultrasonic treatment for 30min, then adding 300mg of sodium amide, and continuing the ultrasonic treatment for 30min to obtain a mixture B;
and (4): putting the mixture B into a high-pressure reaction kettle, heating to 220 ℃, and reacting for 12 hours to obtain a carbon nano tube loaded phosphorus nitride crude product;
and (5): and (3) putting the carbon nano tube loaded phosphorus nitride crude product into a centrifuge, washing for 3 times by using absolute ethyl alcohol, and putting the product into a freeze drying instrument for drying for 8-36h to obtain the carbon nano tube loaded phosphorus nitride electrode material.
Fig. 1 is an X-ray diffraction spectrum of the carbon nanotube-supported phosphorus nitride electrode material prepared in the first example. As shown in fig. 1, the peak of the diffraction peak at 2 θ =26 ° represents that the carbon nanotube is still better in crystallinity and conductivity after being compounded with phosphorus nitride.
Fig. 2 is an infrared absorption spectrum of the carbon nanotube-supported phosphorus nitride electrode material prepared in example one. As shown in FIG. 2, 3280cm in the figure -1 The wide absorption peak is attributed to-OH stretching vibration of the carbon nanotube surface after hydroxylation of the carbon nanotube, 1213cm -1 AttributionCharacteristic peaks at P = N and P-N, 921cm -1 The peak belongs to a P-O-C bond generated after the substitution reaction of-OH on the surface of the carbon nano tube and hexachlorocyclotriphosphazene P-Cl. The appearance of the above absorption peaks indicates that the phosphorus nitride is successfully combined with the carbon nanotube.
Fig. 3 is a scanning electron microscope image of the carbon nanotube-supported phosphorus nitride electrode material prepared in the first embodiment. As shown in fig. 3, the carbon nanotubes and the phosphorus nitride nanotubes are tightly bonded together, giving the phosphorus nitride good electrical conductivity.
The second embodiment: and preparing the asymmetric capacitance deionization module of the carbon nano tube loaded phosphorus nitride electrode material.
(a) Preparing a cathode electrode: uniformly mixing the obtained carbon nanotube-loaded phosphorus nitride electrode material serving as an active substance with conductive carbon black and a binder in a mass ratio of 8; subsequently, the resulting mixture was coated on graphite paper with a film thickness of 300 μm; drying the coated graphite paper at 60 ℃ for 8h to obtain a cathode electrode for capacitive deionization with an active substance of carbon nanotube-loaded phosphorus nitride, as shown in fig. 4;
(b) Preparing an anode electrode: uniformly mixing activated carbon serving as an active substance with conductive carbon black, adding absolute ethyl alcohol, uniformly stirring, adding a binder, and uniformly stirring; coating the obtained mixture on graphite paper, wherein the coating thickness is 100-600 mu m, and drying the coated graphite paper at 40-80 ℃ for 2-24h to obtain an anode electrode for capacitive deionization with active substances as activated carbon;
(c) Assembling an asymmetric capacitance deionization module: and sequentially assembling the current collector, the titanium strip, the cathode electrode for capacitive deionization of phosphorus nitride loaded by carbon nano tubes with active substances, non-woven fabric, a silica gel gasket, the non-woven fabric, the anode electrode for capacitive deionization with active substances of activated carbon, the titanium strip and the current collector to obtain the asymmetric capacitive deionization module of the carbon nano tube loaded phosphorus nitride electrode material.
In this example, the carbon nanotubes support a phosphorus nitride electrode material: conductive carbon black: the mass ratio of the binder is 8:1:1-7:2:1.
Example three: the asymmetric capacitive deionization module of the carbon nanotube-loaded phosphorus nitride electrode material is applied to uranium ion extraction.
The assembled asymmetric capacitance deionization module of the carbon nanotube-containing loaded phosphorus nitride electrode material is connected with a power supply, a peristaltic pump and 100mL uranium-containing wastewater with uranium concentration of 175mg/L are connected through a hose, a solution containing uranium ions is pumped into a channel between two electrodes at a certain flow rate through the peristaltic pump, the adsorption time is 420min under the action of 1.2V voltage, and anions and cations in the solution are respectively adsorbed to the two electrodes. Fig. 5 is a graph of a curve of the change of the adsorption capacity with time of the carbon nanotube-loaded phosphorus nitride electrode in the electro-adsorption process, as shown in fig. 5, the carbon nanotube-loaded phosphorus nitride cathode electrode can effectively remove 96.58% of uranium ions in uranium-containing wastewater, and the adsorption capacity reaches 1179.72mg/g. The calculation formula of the adsorption capacity is shown as the following formula I:
Q t ＝((C 0 -C t )V)/m (1)
Q t : adsorption capacity; c 0 : an initial concentration; ct: equilibrium concentration; v: volume of solution; m: carbon nanotube-supported phosphorus nitride.
Example four: and testing the condition that the carbon nano tube loaded phosphorus nitride electrode material adsorbs uranium under different pH value environments.
The carbon nanotube-supported phosphorus nitride electrode was subjected to electro-adsorption in an environment of pH =3 to 8, the initial concentration of uranium (100 mg/L) and the electro-adsorption time were 240min, and other conditions were the same as those in the third example. Fig. 6 is a comparison graph of the adsorption conditions of the carbon nanotube-loaded phosphorus nitride electrode on uranium ions under different pH values in the fourth embodiment, and as shown in fig. 6, the results show that the adsorption of uranium ions is facilitated when the pH value of the solution is 5, and the adsorption capacity of the carbon nanotube-loaded phosphorus nitride electrode on uranium is 182.62mg/g.
Example five: and testing the adsorption experiment of the carbon nano tube loaded phosphorus nitride electrode on uranium ions under different initial uranium concentrations.
Taking 100mL of uranium-containing wastewater with uranium concentration of 100-600mg/L, pumping the uranium-containing wastewater into a channel between two electrodes at a certain flow rate by a peristaltic pump, and performing electro-adsorption for 300min under the action of voltage with the pH value of 5,1.2V. Fig. 7 is a comparison graph of the adsorption of the carbon nanotube-loaded phosphorus nitride electrode to uranium ions at different initial uranium concentrations in example five, and as shown in fig. 7, the adsorption capacity of the carbon nanotube-loaded phosphorus nitride electrode to uranium ions increases with the increase of the initial concentration, and gradually reaches saturation after the initial concentration is 400 mg/L.
Example six: and testing the adsorption condition of the carbon nanotube-loaded phosphorus nitride electrode copper on uranium ions under different applied voltages.
The adsorption experiment of the carbon nanotube loaded phosphorus nitride electrode on uranium ions under different applied voltages comprises the following specific steps: taking 100mL of uranium-containing wastewater with uranium concentration of 185mg/L, pumping the uranium-containing wastewater into a channel between two electrodes at a certain flow rate by a peristaltic pump, and performing electro-adsorption for 300min under the action of voltage with the pH value of 5 and 0-1.2V. Fig. 8 is a comparison graph of adsorption of uranium ions by the carbon nanotube-loaded phosphorus nitride electrode under different applied voltages in example six, and as shown in fig. 8, when the voltage is 1.2V, the adsorption capacity of the carbon nanotube-loaded phosphorus nitride electrode to uranium ions is 614.09mg/g at most.
Finally, it should be noted that: the above examples are only intended to illustrate the technical solution of the present invention, and not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention.
Claims (11)
1. A preparation method of a carbon nanotube loaded phosphorus nitride electrode material is characterized by comprising the following steps:
step (1): uniformly dispersing the carbon nano tube in deionized water, heating to 90-100 ℃ in an oil bath, and reacting for 8-10h to obtain a hydroxylated carbon nano tube;
step (2): adding the hydroxylated carbon nano tube into an organic solvent, and uniformly stirring to obtain a mixture A;
and (3): adding hexachlorocyclotriphosphazene into the mixture A, performing ultrasonic treatment, adding sodium amide, and continuing ultrasonic treatment to obtain a mixture B;
and (4): putting the mixture B into a high-pressure reaction kettle, heating to 150-250 ℃, and reacting for 8-10h to obtain a carbon nano tube loaded phosphorus nitride crude product;
and (5): and (3) putting the carbon nano tube loaded phosphorus nitride crude product into a centrifuge, washing for 3 times by using absolute ethyl alcohol, and then putting the centrifuge into a freeze drying instrument for drying for 8-36h to obtain the carbon nano tube loaded phosphorus nitride electrode material.
2. The production method according to claim 1, wherein in the step (2), the organic solvent is a benzene solution.
3. The method for preparing according to claim 1, wherein in the step (3), the mass ratio of the hexachlorocyclotriphosphazene to the hydroxylated carbon nanotube is 2:1-8:1.
4. the method according to claim 1, wherein in the step (3), the sonication time is 30min.
5. The method according to claim 1, wherein in the step (4), the heating temperature is 180 to 220 ℃.
6. A method for preparing an asymmetric capacitive deionization module containing a carbon nano tube loaded with a phosphorus nitride electrode material is characterized by comprising the following steps:
(a) Preparing a cathode electrode: uniformly mixing the carbon nanotube-supported phosphorus nitride electrode material prepared in claim 1 as an active substance with conductive carbon black, adding absolute ethyl alcohol, uniformly stirring, adding a binder, and uniformly stirring; coating the obtained mixture on graphite paper, wherein the coating film thickness is 100-600 mu m, and drying the coated graphite paper at 40-80 ℃ for 2-24h to obtain a cathode electrode for capacitive deionization, wherein the active substance is carbon nanotube-loaded phosphorus nitride;
(b) Preparing an anode electrode: uniformly mixing active carbon serving as an active substance with conductive carbon black, adding absolute ethyl alcohol, uniformly stirring, adding a binder, and uniformly stirring; coating the obtained mixture on graphite paper, wherein the coating thickness is 100-600 mu m, and drying the coated graphite paper at 40-80 ℃ for 2-24h to obtain an anode electrode for capacitive deionization with active substances as activated carbon;
(c) Assembling an asymmetric capacitance deionization module: and sequentially assembling the current collector, the titanium strip, the cathode electrode for capacitive deionization of phosphorus nitride loaded by carbon nano tubes with active substances, non-woven fabric, a silica gel gasket, the non-woven fabric, the anode electrode for capacitive deionization with active substances of activated carbon, the titanium strip and the current collector to obtain the asymmetric capacitive deionization module of the carbon nano tube loaded phosphorus nitride electrode material.
7. The method according to claim 6, wherein the binder in the step (a) is a mixed solution of polyvinyl butyral and polyvinyl pyrrolidone.
8. The production method according to claim 7, wherein the mass ratio of the polyvinyl butyral to the polyvinyl pyrrolidone in the mixed solution is 2.
9. A method for applying an asymmetric capacitive deionization module containing a carbon nano tube loaded with a phosphorus nitride electrode material to uranium ion extraction is characterized by comprising the following steps:
the asymmetric capacitance deionization module of the carbon nanotube-loaded phosphorus nitride-containing electrode material assembled in claim 6 is connected with a power supply, a peristaltic pump and 100mL uranium-containing waste liquid through hoses, the uranium-containing waste liquid is pumped into a channel between two electrodes through the peristaltic pump at a certain flow rate, under the action of voltage, positive ions and negative ions in the solution are respectively adsorbed to the two electrodes, the pH value is adjusted to be 3-8, the power supply voltage is set to be 0-1.2V, and the adsorption time is 0-420min.
10. The method according to claim 9, wherein the pH is adjusted using 1mol/L hydrochloric acid and 1mol/L sodium hydroxide solution.
11. The method of claim 9, wherein the peristaltic pump flow rate is 15mL/min, the voltage is set at 1.2V, and the adsorption time is 300min.
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