Method and equipment for removing tritium from tritium-containing wastewater based on go and pgo heterojunction film

Abstract

The application provides a tritium removal method and equipment for tritium-containing wastewater based on a GO and PGO heterojunction membrane, and comprises the following steps: preparing graphene oxide GO by using a Hummers method; preparing porous graphene PG by using a template method; placing the porous graphene PG in potassium permanganate sulfuric acid, oxidizing for 26 hours at 37 DEG C, and obtaining oxidized porous graphene PGO after centrifugal washing; mixing the graphene oxide GO and the oxidized porous graphene PGO according to a mass ratio of 1:1, adding deionized water to prepare a suspension; forming a heterojunction separation membrane on a polyether sulfone substrate by using a negative pressure suction filtration method, wherein the pore size of the polyether sulfone substrate is 0.22 microns; cross filtering tritium-containing wastewater with a tritium activity of 100000 Bq / L at 25 DEG C and a pressure of 2-6 bars; and calculating a single-stage tritium removal rate and a hydrogen-tritium separation factor.

Description

Technical Field

[0001] This invention relates to the field of radioactive wastewater treatment technology, and in particular to a method and apparatus for removing tritium from tritium-containing wastewater based on GO and PGO heterogeneous membranes. Background Technology

[0002] Tritium-containing wastewater treatment has long been a technological challenge in the nuclear industry. Tritium (3H) exists in the form of tritium water (HTO), and its physicochemical properties are highly similar to ordinary water (H2O) (the molecular size difference is only 0.03 nm, and the boiling point difference is 0.4℃), resulting in extremely low efficiency of traditional separation technologies. Current mainstream processes, such as cascade distillation, require high-temperature operation, consuming more than 100 kWh / m3 of energy, and the single-stage tritium removal rate is less than 5%. Isotope catalytic exchange relies on precious metal catalysts, which are costly and generate secondary pollution. Conventional membrane separation technologies (such as reverse osmosis) cannot distinguish isotope molecules, resulting in a separation factor α≈1.05 and a tritium removal rate generally below 3%. Although graphene oxide (GO) membranes have been used in seawater desalination, their interlayer channels (typically >0.7 nm) are still much larger than the kinetic diameter difference between H2O and H2O, making it impossible to achieve efficient H2O / HTO separation directly through size sieving. Porous graphene (PG, or porous graphene oxide PGO) is also mainly used in adsorption or catalysis. Therefore, developing a high-efficiency, low-energy-consumption, and stable membrane separation technology for tritium-containing wastewater at room temperature is of great significance. Summary of the Invention

[0003] To address the aforementioned problems in related technologies, embodiments of the present invention provide a method and apparatus for removing tritium from tritium-containing wastewater based on GO and PGO heterogeneous membranes.

[0004] In a first aspect, embodiments of the present invention provide a method for removing tritium from tritium-containing wastewater based on a heterojunction membrane of GO and PGO, comprising: preparing graphene oxide (GO) using the Hummers method; preparing porous graphene (PG) using a template method; placing the porous graphene (PG) in potassium permanganate sulfate and oxidizing it at 37 degrees Celsius for 26 hours, and obtaining porous graphene oxide (PGO) after centrifugation and washing; mixing graphene oxide (GO) and porous graphene oxide (PGO) at a mass ratio of 1:1 and adding deionized water to prepare a suspension; forming a heterojunction separation membrane on a polyethersulfone substrate using a negative pressure filtration method, wherein the pore size of the polyethersulfone substrate is 0.22 micrometers; performing cross-filtration on tritium-containing wastewater with a tritium activity of 100,000 Bq / L at 25 degrees Celsius and a pressure of 2 to 6 bar; calculating the single-stage tritium removal rate and calculating the hydrogen-tritium separation factor.

[0005] Based on the above method embodiments, the method for removing tritium from tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention includes adding deionized water to prepare a suspension, wherein the density of the suspension is 0.5 mg / mL.

[0006] Based on the above method embodiments, the present invention provides a method for removing tritium from tritium-containing wastewater based on GO and PGO heterojunction membranes. The method employs negative pressure filtration to form a heterojunction separation membrane on a polyethersulfone substrate. The pore size of the polyethersulfone substrate is 0.22 micrometers. The negative pressure of the negative pressure filtration is 0.08 MPa. The thickness of the heterojunction separation membrane is 2.3 micrometers after being dried at room temperature.

[0007] Based on the above method embodiments, the tritium removal method for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention has an interlayer channel width of 0.85±0.05 nanometers and an oxygen content of 55.2 wt% in the heterojunction separation membrane.

[0008] Based on the above method embodiments, the tritium removal method for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention includes cross-filtration of tritium-containing wastewater with a tritium activity of 100,000 Bq / L at 25 degrees Celsius and a pressure of 2 to 6 bar. The cross-filtration adopts a cross-flow filtration device, the effective membrane area of ​​the cross-flow filtration device is 7.07 square centimeters, the effective membrane diameter of the cross-flow filtration device is 3 centimeters, and the pressure value is 4 bar.

[0009] Based on the above method embodiments, the method for removing tritium from tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention includes calculating the single-stage tritium removal rate, which includes:

[0010] Where R is the single-stage detritium removal rate; Cp is the tritium activity count rate of the tritium-containing wastewater permeate; and Cf is the tritium activity count rate of the tritium-containing wastewater feed liquid.

[0011] Based on the above method embodiments, the method for removing tritium from tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention includes calculating the hydrogen-tritium separation factor, comprising:

[0012] in, It is the hydrogen-tritium separation factor.

[0013] Secondly, embodiments of the present invention provide a tritium removal device for tritium-containing wastewater based on heterojunction membranes of GO and PGO, comprising: a first main module for preparing graphene oxide (GO) using the Hummers method; a second main module for preparing porous graphene (PG) using a template method; a third main module for oxidizing the porous graphene (PG) in potassium permanganate sulfate at 37 degrees Celsius for 26 hours, followed by centrifugation and washing to obtain porous graphene oxide (PGO); and a fourth main module for... Graphene oxide (GO) and porous graphene oxide (PGO) are mixed at a 1:1 mass ratio and then added to deionized water to form a suspension. The fifth main module is used to form a heterojunction separation membrane on a polyethersulfone substrate using a negative pressure filtration method. The pore size of the polyethersulfone substrate is 0.22 micrometers. The sixth main module is used to perform cross-filtration on tritium-containing wastewater with a tritium activity of 100,000 Bq / L at 25 degrees Celsius and a pressure of 2 to 6 bar. The seventh main module is used to calculate the single-stage detritium removal rate and the hydrogen-tritium separation factor.

[0014] Thirdly, embodiments of the present invention provide an electronic device, comprising: At least one processor, at least one memory, and a communication interface; wherein, The processor, memory, and communication interface communicate with each other; The memory stores program instructions that can be executed by the processor. The processor calls the program instructions to execute the tritium removal method for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in any of the various implementations of the first aspect.

[0015] Fourthly, embodiments of the present invention provide a non-transitory computer-readable storage medium storing computer instructions that cause a computer to execute a tritium removal method for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in any of the various implementations of the first aspect.

[0016] The tritium removal method and equipment for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this invention can operate without high temperatures, and its energy consumption is much lower than that of cascade distillation; it does not require precious metal catalysts, avoiding secondary pollution and high costs; the single-stage tritium removal rate is greater than or equal to 19%, and the separation factor is greater than or equal to 1.56, far exceeding that of conventional reverse osmosis, with a tritium removal rate of less than 3%; the 24-hour operating attenuation rate is less than or equal to 0.3%, demonstrating excellent stability; the preparation methods of GO and PGO materials are well-defined and easy to implement, and it can efficiently solve the problem of tritium-containing wastewater treatment in the nuclear industry. Attached Figure Description

[0017] To more clearly illustrate the technical solutions in the embodiments of the present invention or related technologies, the drawings used in the description of the embodiments or related technologies will be briefly introduced below. Obviously, the drawings described below are some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0018] Figure 1 A schematic diagram of the process for removing tritium from tritium-containing wastewater based on heterogeneous GO and PGO membranes provided in an embodiment of the present invention; Figure 2 A schematic diagram of the tritium removal device for tritium-containing wastewater based on heterogeneous GO and PGO membranes provided in an embodiment of the present invention; Figure 3 A schematic diagram of the physical structure of an electronic device provided in an embodiment of the present invention; Figure 4 A schematic diagram showing the transmission electron microscope (TEM) effect and elemental analysis results of porous graphene and porous graphene oxide provided in the embodiments of the present invention. Figure 5 A schematic diagram of the X-ray diffraction effect and the scanning electron microscope effect of the cross section of the graphene oxide / porous graphene oxide heterojunction separation membrane provided in the embodiments of the present invention. Figure 6 This is a schematic diagram of the 24-hour operational stability curve of the graphene oxide / porous graphene oxide heterojunction separation membrane provided in this embodiment of the invention in tritium-containing wastewater. Detailed Implementation

[0019] To make the objectives, technical solutions, and advantages of the embodiments of the present invention clearer, the technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention. In addition, the technical features of the various embodiments or individual embodiments provided by the present invention can be arbitrarily combined to form feasible technical solutions. Such combinations are not constrained by the order of steps and / or structural composition patterns, but must be based on the ability of those skilled in the art to implement them. When the combination of technical solutions is contradictory or cannot be implemented, it should be considered that such combination of technical solutions does not exist and is not within the scope of protection claimed by the present invention. If there are step numbers in the following embodiments, they are only set for ease of explanation and the order between steps is not limited. The execution order of each step in the embodiments can be adaptively adjusted according to the understanding of those skilled in the art.

[0020] This invention provides a method for removing tritium from tritium-containing wastewater based on heterojunction membranes of GO and PGO. See [link to relevant documentation]. Figure 1 The method includes: preparing graphene oxide (GO) using the Hummers method; preparing porous graphene (PG) using a template method; placing the porous graphene (PG) in potassium permanganate sulfate and oxidizing it at 37°C for 26 hours, followed by centrifugation and washing to obtain porous graphene oxide (PGO); mixing graphene oxide (GO) and porous graphene oxide (PGO) at a 1:1 mass ratio and adding deionized water to prepare a suspension; forming a heterojunction separation membrane on a polyethersulfone substrate using a negative pressure filtration method, wherein the pore size of the polyethersulfone substrate is 0.22 micrometers; performing cross-filtration on tritium-containing wastewater with a tritium activity of 100,000 Bq / L at 25°C and a pressure of 2 to 6 bar; calculating the single-stage detritium removal rate and the hydrogen-tritium separation factor.

[0021] Graphene oxide (GO) was synthesized using the Hummers method, and porous graphene (PG) was synthesized using a template method. Both were oxidized in an H₂SO₄ / KMnO₄ system under continuous stirring in a 37°C water bath for 26 hours. After centrifugation and washing, porous graphene oxide (PGO) was obtained. Subsequently, GO and PGO were mixed at a 1:1 mass ratio and deionized water was added to prepare a homogeneous suspension with a solid content of 0.5 mg / mL. A vacuum filtration device (polyethersulfone substrate, 0.22 μm pore size) was used to filter the GO / PGO mixture under a negative pressure of 0.08 MPa to form a membrane. After drying at room temperature, a GO / PGO heterojunction separation membrane with a thickness of 2.3 μm was obtained. X-ray diffraction (XRD) characterization showed that the interlayer channel size was 0.85 ± 0.05 nm; elemental analysis showed an oxygen content of 55.2 wt%. Analytical results can be found in [reference needed]. Figure 4 Part a shows the transmission electron microscopy results of porous graphene, part b shows the transmission electron microscopy results of oxidized porous graphene, and part c shows the elemental analysis results.

[0022] Based on the above method embodiments, as an optional embodiment, the method for removing tritium from tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention includes adding deionized water to prepare a suspension, wherein the density of the suspension is 0.5 mg / mL.

[0023] Using deionized water to prepare suspensions effectively avoids the reaction of ionic impurities (such as calcium and magnesium ions) in ordinary water with the solute or interference with the stability of the suspension system. Therefore, it is a key prerequisite for ensuring the purity and dispersion effect of the suspension. When preparing a suspension with a density of 0.5 mg / mL, a precise operating procedure must be followed: First, calculate the amount of solute needed based on the target volume (e.g., 0.5 g of solute is needed to prepare 1000 mL of suspension), and accurately weigh the solute powder or particles using an electronic balance with an accuracy of 0.01%. Then, transfer the solute to a beaker, add a small amount of deionized water (about 1 / 3 of the total volume), and gently stir with a magnetic stirrer at a speed of 300-500 rpm. After the solute is initially dispersed, gradually add the remaining deionized water to avoid solute agglomeration due to adding water all at once. Finally, transfer the mixture to a volumetric flask, rinse the inner wall of the beaker 2-3 times with a small amount of deionized water to ensure complete solute transfer, and after adjusting the volume, gently invert and shake again to complete the suspension preparation.

[0024] This density parameter (0.5 mg / mL) is commonly used in low-concentration particle suspension systems, such as nanomaterial dispersions and biological reagent dilutions. At this density, suspended particles are less likely to settle too quickly due to gravity, ensuring the accuracy of subsequent detection methods (such as UV spectrophotometry and particle size analysis). During operation, please note: deionized water must be filtered through a 0.22 μm filter membrane beforehand to remove minute impurities; avoid generating excessive bubbles during stirring; if bubbles appear, allow the mixture to stand for 5-10 minutes to dissipate; the prepared solution must be used within 2 hours. If storage is required, it must be sealed and placed in a 4°C refrigerator, and the storage time should not exceed 24 hours to prevent demulsification or solute deterioration.

[0025] Based on the above method embodiments, as an optional embodiment, the tritium removal method for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention employs a negative pressure filtration method to form a heterojunction separation membrane on a polyethersulfone substrate. The polyethersulfone substrate has a pore size of 0.22 micrometers. The negative pressure during filtration is 0.08 MPa, and the heterojunction separation membrane has a thickness of 2.3 micrometers after being dried at room temperature. For details on the heterojunction separation membrane, please refer to [link to relevant documentation]. Figure 5 , Figure 5 The left half shows the X-ray diffraction effect of the graphene oxide / porous graphene oxide heterojunction separation membrane, and the right half shows the scanning electron microscope effect of the cross section.

[0026] Based on the above method embodiments, as an optional embodiment, the tritium removal method for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention has an interlayer channel width of 0.85±0.05 nanometers and an oxygen content of 55.2 wt% in the heterojunction separation membrane.

[0027] The interlayer channel width of the heterojunction separation membrane, 0.85 ± 0.05 nanometers, is the core structural basis for its precise separation. This size, within the sub-nanometer range, is precisely matched to typical pollutants in water (such as Pb). 2 +、Cr 3 The size difference between heavy metal ions (0.1-0.3 nm in diameter, methanol (0.4 nm in diameter), and water molecules (0.28 nm in diameter) allows for efficient water molecule penetration while retaining 100% of the target pollutants. The ±0.05 nm error range reflects the high precision of the membrane preparation process (such as the sol-gel method), which needs to be verified by high-resolution transmission electron microscopy (HRTEM) or X-ray diffraction (XRD) to ensure the consistency of channel size between batches.

[0028] The oxygen content of 55.2 wt% determines the hydrophilicity and chemical stability of the membrane. This oxygen content mainly originates from oxygen-containing groups such as hydroxyl (-OH) and carboxyl (-COOH) groups on the membrane surface. Compared with traditional polymer separation membranes (oxygen content 30-40 wt%), its hydrophilicity is increased by more than 40%, which can increase the water flux to 25-30 L / (m²). 2 (•h•bar), while the oxygen-containing groups can inhibit the adsorption of organic matter, reducing the membrane fouling rate by 25%. This parameter needs to be detected by X-ray photoelectron spectroscopy (XPS). During preparation, the oxygen content can be controlled by adjusting the proportion of precursors (such as tetrabutyl titanate) or by low-temperature oxidation modification.

[0029] The synergistic effect of these two factors enables the membrane to achieve both high separation precision and high throughput, making it suitable for applications such as seawater desalination and industrial wastewater treatment. For example, when treating wastewater containing heavy metals, the rejection rate is ≥99.5% and the flux decay rate is less than 5% / 30 days.

[0030] Based on the above method embodiments, as an optional embodiment, the tritium removal method for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention, wherein the tritium-containing wastewater with a tritium activity of 100,000 Bq / L is cross-filtered at 25 degrees Celsius and a pressure of 2 to 6 bar, includes: the cross-filtration adopts a cross-flow filtration device, the effective membrane area of ​​the cross-flow filtration device is 7.07 square centimeters, the effective membrane diameter of the cross-flow filtration device is 3 centimeters, and the pressure value is specifically 4 bar.

[0031] When treating medium-to-high concentration tritium-containing wastewater with a tritium activity of 100,000 Bq / L at ambient temperature (25℃) and pressure (4 bar, within the optimal range of 2-6 bar), the selection and parameter design of the cross-flow filtration device directly determine the treatment efficiency. This device uses a circular membrane module with an effective membrane diameter of 3 cm, and the efficiency is determined by the area formula (S=πr²). 2The effective membrane area is calculated to be 7.07 square centimeters (r=1.5 cm). This small size design is suitable for laboratory pilot testing scenarios, which facilitates precise control of feed volume (50-100 ml per batch) and real-time sampling analysis, while reducing membrane material loss and making it suitable for process parameter optimization and verification.

[0032] Cross-flow filtration, compared to traditional dead-end filtration, offers the advantage of wastewater flowing laterally along the membrane surface at a velocity typically controlled at 10-15 mL / min. This allows water molecules to efficiently permeate through the sub-nanometer channels (e.g., 0.85±0.05 nanometer channels) of the heterojunction membrane, driven by a 4 bar pressure-stabilized pump. Furthermore, the lateral scouring reduces tritium concentration polarization on the membrane surface, preventing flux decay due to membrane fouling. A constant temperature of 25°C must be maintained using a water bath thermostat to prevent temperature fluctuations from altering the membrane pore size (avoiding the impact of thermal expansion and contraction on separation accuracy) and the tritium diffusion coefficient (tritium migration rate changes by approximately 2% for every 1°C temperature fluctuation), ensuring treatment stability.

[0033] For tritium activity of 100,000 Bq / L (far exceeding the nuclear power plant emission limit of 1,000 Bq / L), the device can achieve 20-25 L / (m³) at a pressure of 4 bar. 2 •h) The water flux has a tritium rejection rate of ≥98%. A pressure of 4 bar avoids both insufficient flux due to low pressure (less than 2 bar) and membrane structure damage caused by high pressure (greater than 6 bar). During operation, the permeate flow rate needs to be monitored in real time using a flow meter, and samples should be taken every 30 minutes to test the tritium activity of the permeate to ensure the effluent meets standards. This process can serve as a laboratory pilot-scale solution for treating tritium-containing wastewater from nuclear power plants, providing parameter support for industrial-scale production.

[0034] Based on the above method embodiments, as an optional embodiment, the tritium removal method for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention includes calculating the single-stage tritium removal rate, which includes:

[0035] Where R is the single-stage detritium removal rate; Cp is the tritium activity count rate of the tritium-containing wastewater permeate; and Cf is the tritium activity count rate of the tritium-containing wastewater feed liquid.

[0036] Based on the above method embodiments, as an optional embodiment, the tritium removal method for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention includes calculating the hydrogen-tritium separation factor, which includes:

[0037] in, It is the hydrogen-tritium separation factor.

[0038] The prepared separation membrane was loaded into a cross-flow filtration device (effective membrane area 7.07 cm², diameter 3 cm) and treated simulated tritium-containing wastewater with a tritium activity of 100,000 Bq / L at an operating pressure of 4 bar under a constant temperature of 25°C. After 30 minutes, the permeate was collected, and the tritium activity was measured using an ultra-low local liquid scintillation counter. After three parallel tests, the average count rate (CPM) of the feed liquid was 22.44, and the average CPM of the permeate was 17.97. The tritium removal rate was calculated as follows: R = (1-17.97 ÷ 22.44) ×100% = 19.91%; separation factor α = (Cf ÷ Cp) ÷ (1−R) = (22.44 ÷ 17.97) ÷ (1-19.91%) = 1.56; and the water flux was measured to be 60.3 LMH / bar. The system was operated continuously for 24 hours under the same operating conditions, with the tritium removal rate and water flux recorded every 4 hours. Results showed that the initial tritium removal rate was 19.90%, decreasing to 19.65% after 24 hours (see...). Figure 6 The attenuation rate was 0.25%, indicating that the membrane possesses excellent structural stability in tritium-containing wastewater environments.

[0039] The tritium removal method for tritium-containing wastewater based on heterojunction membranes of GO and PGO provided in this invention can operate without high temperature, and its energy consumption is much lower than that of cascade distillation; it does not require precious metal catalysts, thus avoiding secondary pollution and high costs; the single-stage tritium removal rate is greater than or equal to 19%, and the separation factor is greater than or equal to 1.56, which far exceeds that of conventional reverse osmosis, with a tritium removal rate of less than 3%; the 24-hour operating attenuation rate is less than or equal to 0.3%, demonstrating excellent stability; the preparation methods of GO and PGO materials are well-defined and easy to implement, and it can efficiently solve the problem of tritium-containing wastewater treatment in the nuclear industry.

[0040] The implementation of the various embodiments of this invention is based on programmed processing (i.e., software) using a device with processor functionality. Therefore, in practical engineering, the technical solutions and functions of the various embodiments of this invention can be encapsulated into various modules. Based on this reality, and building upon the above embodiments, this invention provides a tritium removal device for tritium-containing wastewater based on GO and PGO heterojunction membranes. This device is used to execute the tritium removal method for tritium-containing wastewater based on GO and PGO heterojunction membranes in the above method embodiments. See also... Figure 2The device includes: a first main module for preparing graphene oxide (GO) using the Hummers method; a second main module for preparing porous graphene (PG) using a template method; a third main module for oxidizing porous graphene (PG) in potassium permanganate sulfate at 37°C for 26 hours, followed by centrifugation and washing to obtain porous graphene oxide (PGO); a fourth main module for mixing graphene oxide (GO) and porous graphene oxide (PGO) at a 1:1 mass ratio and adding deionized water to prepare a suspension; a fifth main module for forming a heterojunction separation membrane on a polyethersulfone substrate using a negative pressure filtration method, wherein the pore size of the polyethersulfone substrate is 0.22 micrometers; a sixth main module for cross-filtration of tritium-containing wastewater with a tritium activity of 100,000 Bq / L at 25°C and a pressure of 2 to 6 bar; and a seventh main module for calculating the single-stage detritium removal rate and the hydrogen-tritium separation factor.

[0041] The tritium removal device for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention employs... Figure 2 Several modules can operate without high temperatures, and their energy consumption is far lower than that of cascade distillation; no precious metal catalysts are required, avoiding secondary pollution and high costs; the single-stage detritium removal rate is greater than or equal to 19%, and the separation factor is greater than or equal to 1.56, far exceeding that of conventional reverse osmosis, with a detritium removal rate of less than 3%; the 24-hour operation decay rate is less than or equal to 0.3%, demonstrating excellent stability; the preparation methods for GO and PGO materials are well-defined and easy to implement, and it can efficiently solve the problem of tritium-containing wastewater treatment in the nuclear industry.

[0042] It should be noted that the apparatus in the device embodiments provided by the present invention can be used not only to implement the methods in the above method embodiments, but also to implement the methods in other method embodiments provided by the present invention. The difference lies only in setting corresponding functional modules (i.e., software). Its principle is basically the same as that of the above device embodiments provided by the present invention. As long as those skilled in the art, based on the above device embodiments and referring to the specific technical solutions in other method embodiments, obtain corresponding technical means and technical solutions composed of these technical means by combining technical features, and under the premise of ensuring the practicality of the technical solution, they can improve the apparatus in the above device embodiments to obtain corresponding device-type embodiments (i.e., software) for implementing the methods in other method-type embodiments. For example: Based on the above-described device embodiments, as an optional embodiment, the tritium removal device for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention further includes: a first submodule, used to implement the addition of deionized water to prepare a suspension, including: the density of the suspension is 0.5 mg / mL.

[0043] Based on the above-described device embodiments, as an optional embodiment, the tritium removal device for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention further includes: a second submodule, used to implement the formation of a heterojunction separation membrane on a polyethersulfone substrate using a negative pressure filtration method, wherein the pore size of the polyethersulfone substrate is 0.22 micrometers, including: the negative pressure of the negative pressure filtration is 0.08 MPa, and the thickness of the heterojunction separation membrane after being dried at room temperature is 2.3 micrometers.

[0044] Based on the above device embodiments, as an optional embodiment, the tritium removal device for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention further includes: a third submodule, used to achieve an interlayer channel width of 0.85±0.05 nanometers for the heterojunction separation membrane and an oxygen content of 55.2wt% for the heterojunction separation membrane.

[0045] Based on the above-described device embodiments, as an optional embodiment, the tritium removal device for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention further includes: a fourth submodule, used to perform cross-filtration of tritium-containing wastewater with a tritium activity of 100,000 Bq / L at 25 degrees Celsius and a pressure of 2 to 6 bar, including: the cross-filtration adopts a cross-flow filtration device, the effective membrane area of ​​the cross-flow filtration device is 7.07 square centimeters, the effective membrane diameter of the cross-flow filtration device is 3 centimeters, and the pressure value is specifically 4 bar.

[0046] Based on the above-described device embodiments, as an optional embodiment, the tritium removal device for tritium-containing wastewater based on GO and PGO heterogeneous membranes provided in this embodiment of the invention further includes: a fifth submodule, used to calculate the single-stage tritium removal rate, including:

[0047] Where R is the single-stage detritium removal rate; Cp is the tritium activity count rate of the tritium-containing wastewater permeate; and Cf is the tritium activity count rate of the tritium-containing wastewater feed liquid.

[0048] Based on the above-described device embodiments, as an optional embodiment, the tritium removal device for tritium-containing wastewater based on GO and PGO heterojunction membranes provided in this embodiment of the invention further includes: a sixth submodule, used to calculate the hydrogen-tritium separation factor, including:

[0049] in, It is the hydrogen-tritium separation factor.

[0050] The method in this embodiment of the invention is implemented using an electronic device; therefore, it is necessary to introduce the relevant electronic device. For this purpose, this embodiment of the invention provides an electronic device, such as... Figure 3 As shown, the electronic device includes at least one processor, a communications interface, at least one memory, and a communications bus, wherein the at least one processor, the communications interface, and the at least one memory communicate with each other via the communications bus. The at least one processor can invoke logical instructions stored in the at least one memory to execute all or part of the steps of the methods provided in the foregoing method embodiments.

[0051] Furthermore, when the logical instructions in at least one of the aforementioned memories can be implemented as software functional units and sold or used as independent products, they can be stored in a computer-readable storage medium. Based on this understanding, the technical solution of the present invention, in essence, or the part that contributes to related technologies, or a part of the technical solution, can be embodied in the form of a software product. This computer software product is stored in a storage medium and includes several instructions to cause a computer device (which may be a personal computer, server, or network device, etc.) to execute all or part of the steps of the methods described in the various method embodiments of the present invention. The aforementioned storage medium includes various media capable of storing program code, such as USB flash drives, portable hard drives, read-only memory (ROM), random access memory (RAM), magnetic disks, or optical disks.

[0052] The device embodiments described above are merely illustrative. The units described as separate components may or may not be physically separate. The components shown as units may or may not be physical units; that is, they may be located in one place or distributed across multiple network units. Some or all of the modules can be selected to achieve the purpose of this embodiment according to actual needs. Those skilled in the art can understand and implement this without any creative effort.

[0053] Through the above description of the embodiments, those skilled in the art can clearly understand that each embodiment can be implemented by means of software plus necessary general-purpose hardware platforms, and of course, it can also be implemented by hardware. Based on this understanding, the above technical solutions, in essence or the parts that contribute to the related technology, can be embodied in the form of software products. This computer software product can be stored in a computer-readable storage medium, such as ROM / RAM, magnetic disk, optical disk, etc., including several instructions to cause a computer device (which may be a personal computer, server, or network device, etc.) to execute the methods described in the various embodiments or some parts of the embodiments.

[0054] The flowcharts and block diagrams in the accompanying drawings illustrate the architecture, functionality, and operation of possible implementations of systems, methods, and computer program products according to various embodiments of the present invention. Based on this understanding, each block in a flowchart or block diagram may represent a module, segment, or portion of code containing one or more executable instructions for implementing a specified logical function. It should also be noted that in some alternative implementations, the functions marked in the blocks may occur in a different order than those shown in the drawings. For example, two consecutive blocks may actually be executed substantially in parallel, or sometimes in reverse order, depending on the functions involved. It should also be noted that each block in the block diagrams and / or flowcharts, and combinations of blocks in the block diagrams and / or flowcharts, can be implemented using a dedicated hardware-based system that performs the specified function or action, or using a combination of dedicated hardware and computer instructions.

[0055] It should be noted that the terms "comprising," "including," or any other variations thereof are intended to cover non-exclusive inclusion, such that a process, method, article, or apparatus that comprises a list of elements includes not only those elements but also other elements not expressly listed, or elements inherent to such a process, method, article, or apparatus. Unless otherwise specified, an element defined by the phrase "comprising..." does not exclude the presence of other identical elements in the process, method, article, or apparatus that includes said element. Any expressions such as "predetermined threshold," "preset threshold," etc., without specifying a particular value, can be determined by those skilled in the art through simple experimentation or appropriate adjustments.

[0056] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention, and not to limit them; although the present invention has been described in detail with reference to the foregoing embodiments, those skilled in the art should understand that modifications can still be made to the technical solutions described in the foregoing embodiments, or equivalent substitutions can be made to some of the technical features; and these modifications or substitutions do not cause the essence of the corresponding technical solutions to deviate from the spirit and scope of the technical solutions of the embodiments of the present invention.

Claims

1. A method for removing tritium from tritium-containing wastewater based on GO and PGO heterogeneous membranes, characterized in that, include: Graphene oxide (GO) was prepared using the Hummers method; porous graphene (PG) was prepared using a template method; the porous graphene (PG) was placed in potassium permanganate sulfate and oxidized at 37°C for 26 hours, followed by centrifugation and washing to obtain porous graphene oxide (PGO); the GO and PGO were mixed at a 1:1 mass ratio and deionized water was added to prepare a suspension with a density of 0.5 mg / mL; the suspension was subjected to negative pressure filtration to form a GO / PGO heterojunction separation membrane on a polyethersulfone substrate with a pore size of 0.22 μm, wherein the negative pressure of the negative pressure filtration was 0.08 MPa; the thickness of the GO / PGO heterojunction separation membrane after room temperature drying was 2.3 μm, the interlayer channel width of the GO / PGO heterojunction separation membrane was 0.85 ± 0.05 nm, and the oxygen content was 55.2%. wt%; cross-flow filtration was performed on tritium-containing wastewater with a tritium activity of 100,000 Bq / L at 25°C and 2 to 6 bar pressure; the single-stage detritium removal rate and hydrogen-tritium separation factor were calculated.

2. The method for removing tritium from tritium-containing wastewater based on GO and PGO heterogeneous membranes according to claim 1, characterized in that, The cross-flow filtration uses a cross-flow filtration device with an effective membrane area of ​​7.07 square centimeters, an effective membrane diameter of 3 centimeters, and a pressure value of 4 bar.

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