CN113155679B - Experimental device and experimental method for simulating adsorption and migration of radioactive nuclide in rock mass fracture - Google Patents
Experimental device and experimental method for simulating adsorption and migration of radioactive nuclide in rock mass fracture Download PDFInfo
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N13/00—Investigating surface or boundary effects, e.g. wetting power; Investigating diffusion effects; Analysing materials by determining surface, boundary, or diffusion effects
Abstract
An experimental device and an experimental method for simulating the adsorption and migration of radioactive nuclides in a rock mass fracture are disclosed, wherein the experimental device comprises a variable-rate liquid supply adjusting device, an adsorption and migration rock pillar device, an automatic collection and effluent device, a pressure and temperature sensor, a barometer and a gas bottle; the experimental method is that an undisturbed rock mass column containing a single crack is placed into an adsorption migration rock mass column device, and the device is subjected to ventilation sealing treatment by using an air bottle. The variable-rate liquid supply adjusting device is connected with the adsorption migration rock pillar device to provide the synthetic underground water solution for the adsorption migration rock pillar device. The effluent liquid of the whole process is automatically collected by an automatic effluent collecting device. The method can be used for researching the adsorption migration rule of the nuclide under the joint action of the water and rock in the surrounding rock fracture, and simultaneously developing condition experiments and parallel experiments of different influence factors, thereby playing a vital role in simulating and predicting the migration distribution of the nuclide.
Description
Technical Field
The invention relates to the technical field of radionuclide adsorption migration and retention, in particular to an experimental device and an experimental method for simulating the radionuclide adsorption migration in a rock mass fracture.
Background
In order to deal with the increasing leakage risk of nuclear waste, at present, deep geological processing libraries or underground laboratories are selected to be established in all nuclear countries in the world, and the nuclear waste is deeply buried in underground rock stratums to be effectively isolated from biospheres. However, during long-term storage of nuclear waste, the storage tanks may be leaked due to corrosion or geological environmental changes, and radioactive nuclides (Pu, U, Se, Sr, Am, Cs, Eu, Tc, etc.) are released into the surrounding rock. In practical situations, the permeability of the surrounding rock is low, but the permeability of cracks and broken zones existing in the surrounding rock is high, so that nuclides in the surrounding rock mainly migrate in the cracks or broken zones of the surrounding rock along with the underground water flow to the outside and finally enter a biosphere, thereby threatening ecological safety and human health. Therefore, the research on the adsorption migration rule of the nuclide under the joint action of the water and rock in the fracture of the surrounding rock is very important.
At present, a vertical or horizontal packed column is established mainly for powdery rock minerals in a laboratory for developing a nuclide adsorption migration simulation process, so that when natural rocks are crushed for researching an adsorption migration rule, although data related to adsorption migration behaviors or mechanisms can be quantitatively provided, the crushing is considered to be a main reason for increasing the adsorption capacity of the rocks, because extra surfaces and reaction sites are generated, the crushing degree is different, and the adsorption capacity is different, so that the traditional powdery mineral research is too ideal, and larger errors can exist when experimental data are used for predicting the actual adsorption migration change rule of the simulated nuclides in surrounding rocks, and the experimental data are not suitable for actual conditions. Therefore, a set of device is needed to be invented to research the solute transport rule of the radionuclide in the surrounding rock fractures, and the device has great research value in the aspects of simulation and prediction of nuclide transport distribution characteristics.
Disclosure of Invention
The invention provides an experimental device and an experimental method for simulating the adsorption and migration of radioactive nuclides in a rock mass fracture.
An experimental device for simulating the adsorption and migration of radioactive nuclides in a rock mass fracture comprises a variable-rate liquid supply adjusting device, an adsorption and migration rock pillar device, an automatic collection and effluent device, a pressure sensor, a temperature sensor, a barometer and a gas bottle;
the variable-rate liquid supply adjusting device consists of a liquid supply bottle, a synthetic underground aqueous solution, a liquid supply pipe and a peristaltic pump, wherein the synthetic underground aqueous solution is filled in the liquid supply bottle and enters the device for adsorbing and migrating the rock pillar through the liquid supply pipe;
the rock pillar adsorption and migration device is a core area of the whole device and comprises a pressure chamber top cover, a pressure chamber bottom cover, a sample piece top cover, a sample piece lower seat, a water permeable plate, a first quick-plug connector, a second quick-plug connector, a sample rock pillar, a transparent latex film, an organic glass cover, organic glass, a support, a first upright post, a second upright post, a first hexagon nut, a second hexagon nut, a gas inlet pipe, a gas outlet pipe, an adjustable telescopic rod and an adjusting rod; the pressure chamber bottom cover is connected with the sample lower seat, the first quick-plug connector is embedded into the sample lower seat, the adjustable telescopic rod is externally connected with the sample top cover, the pressure chamber top cover and the second upright post, the second upright post is fixed with the adjustable telescopic rod through a second hexagon nut, the adjustable telescopic rod is internally connected with the adjusting rod and the second quick-plug connector, the first upright post and the organic glass cover are connected between the pressure chamber top cover and the pressure chamber bottom cover and fixed through the first hexagon nut, a gas inlet pipe and a gas outlet pipe are embedded into the pressure chamber top cover and the pressure chamber bottom cover, the gas inlet pipe is externally connected with a gas gauge and a gas bottle, the gas valve is used for controlling the gas transportation, and the gas outlet pipe is externally connected with a gas valve for controlling the gas output; the synthetic groundwater solution is conveyed into the sample rock mass column through the first quick-connection plug, the sample lower seat and the water permeable plate by the pressure sensor and the temperature sensor which are externally connected with the liquid supply pipe, flows through the adjusting rod and the second quick-connection plug and then flows into the automatic collecting and effluent device;
the automatic collection and effluent device comprises an effluent pipe, an effluent liquid, a sample collection test tube and an automatic part collector; the automatic collecting and flowing device automatically collects the liquid flowing out of the adsorption and migration rock pillar device into the sample collecting test tube at regular time;
the sample rock mass column contains a single fracture;
the pressure sensor and the temperature sensor monitor the temperature and the pressure of the synthesized underground water solution in the liquid supply pipe in real time before the synthesized underground water solution flows into the adsorption and migration rock pillar device;
the gas bottle can provide sufficient gas for the device for adsorbing and transferring the rock mass, and the gas pressure meter provides pressure data of the gas in real time.
The working process of the invention is as follows:
the peristaltic pump is electrified to rotate, the synthetic underground water solution in the liquid supply pipe is brought into the adsorption and migration rock column device through the air pressure sensor and the temperature sensor, the gas bottle provides an air pressure environment for the whole adsorption and migration rock column device, the liquid flows through the first quick-inserting connector, the sample piece lower seat and the water permeable plate to enter the sample rock column, then flows into the automatic collection effluent device after flowing through the adjusting rod and the second quick-inserting connector, after the liquid collected by the automatic part collector reaches an expected concentration range, the peristaltic pump and the automatic part collector are powered off, and the whole process is terminated.
The designed research object is a complete rock pillar instead of rock mineral powder, so that experimental data for researching the adsorption migration and retention rules of nuclides in surrounding rocks are more realistic; through the design of adjustable rock pillar volume, the limitation of the design of a general rock pillar with fixed volume is broken, rock pillars with different volumes can be flexibly used for adsorption migration experiments, the design enhances the practicability of the device, and is also beneficial for researchers to carry out researches on the aspect of relevant parameter scale effects; the whole device takes in place the sealing treatment measures of the sample rock mass column, and the treatment is carried out by 3 steps: firstly, coating a layer of epoxy resin on the side surface of the single-crack rock mass column; secondly, a layer of transparent latex film is sleeved on the outer layer; and finally, the whole adsorption and migration rock pillar device is sealed and ventilated, so that the air pressure of the whole device stably reaches 2MPa, and the aim of sealing is fulfilled. The device can develop the condition experiment and the parallel experiment of different influence factors simultaneously, and the automatic data collection device can realize real-time automatic collection experimental data, practices thrift the human cost, can repeat the experimentation.
A testing method using the simulation device for radionuclide adsorption and migration in rock fractures, comprising the following steps:
firstly, rock pillar pretreatment and sealing: selecting a sample rock pillar according to experiment requirements, wherein a standard granite rock pillar with the length of 10cm and the diameter of 5cm is taken as an example for explanation; in order to generate a single crack in the granite core, the single crack is pretreated by using a Brazilian splitting method, and after treatment, a sealing measure is taken for the granite core with the single crack, firstly, a layer of epoxy resin with the thickness of 1-3mm is coated on the side surface of the single crack rock body column, and then, a transparent emulsion film with the thickness of 1mm is sleeved on the outer layer of the single crack rock body column;
secondly, assembling the rock pillar device: the whole adsorption and migration rock pillar device C is detachable and recombined; assembling the sample rock cylinder subjected to primary sealing treatment in the first step sequentially according to the sequence of a pressure chamber bottom cover, a first quick-connection plug, a water permeable plate, a sample rock cylinder, organic glass, a support, a first stand column, a sample piece top cover, a pressure chamber top cover, an adjusting rod, an adjustable telescopic rod, a second stand column and a second quick-connection plug; the outside is connected with a gas bottle through a gas inlet pipe, gas is selected according to experiment requirements, and argon is selectively introduced at the position; the first quick-connection plug is externally connected with a liquid supply pipe, the synthetic underground water solution in the liquid supply bottle is led into the first quick-connection plug by a peristaltic pump, the flow rate is set according to the experimental requirements, the flow rate is preliminarily set to be 0.3ml/h, and a group of pressure sensors and temperature sensors are arranged on the liquid supply pipe before leading;
thirdly, ventilating the rock pillar: in order to prevent liquid from overflowing from the side surface of the rock pillar when the liquid is introduced into the single-fracture sample rock pillar, a gas bottle is connected with a gas inlet pipe through a control gas valve, the gas valve of the gas inlet pipe is opened at the same time, so that the gas is conveyed into the whole adsorption migration column device, the gas valve of the gas inlet pipe is closed after the gas is continuously introduced for a few minutes, the gas is continuously introduced, the gas pressure of the whole device is controlled to be about 2MPa through the reading of a gas pressure meter, the gas tightness is observed, and the gas valve is closed if the reading of the gas pressure meter is stabilized to be 2 MPa;
fourthly, initially balancing the water supply of the rock pillar: selecting the synthetic underground water solution according to the experimental requirements, and preparing and synthesizing the synthetic underground water solution according to the ion components of underground water in a depth of 600m of a certain drilled hole in certain northwest China; firstly, measuring the initial concentration and pH of each ion in the prepared and synthesized underground water solution; starting the whole device, setting the flow rate of the peristaltic pump to be 0.3ml/h, wherein the flow rate in the whole process is very slow, further discharging bubbles sealed in the sample rock mass column, and observing the flow rate, the concentration and the pH value of each ion of effluent liquid in the sample collecting test tube at intervals, so as to calculate the real flow rate and the stability of the synthetic underground water solution flowing in the whole sample rock mass column, wherein the process is continued until the flow output of the effluent liquid is stable and the concentration and the pH value of each ion are consistent with the initial measurement result, which indicates that the initial water supply state of the rock column reaches a balance state;
fifthly, injecting an adsorbent and a tracer: according to experimentsThe method has different requirements, the adsorbent and the tracer can be selected independently, and the principle is followed that the adsorbent can be adsorbed with the sample rock mass column and the concentration change before and after the reaction can be detected by a measuring instrument; the tracer hardly reacts with the sample rock mass column, and does not belong to the components in the synthetic underground water solution, and the measuring mode is simple. Here, the adsorbent is exemplified by radionuclide U, and the concentration is selected according to a laboratory setting standard that the initial concentration is generally 10 to 100 times higher than the concentration of the component in the natural underground aqueous solution, and the initial concentration of uranium is set to 2.0 x 10-5mol/L; the tracer is exemplified by bromide ion, and the concentration is set to 1.0 x 10-2mol/L; preparing two types of synthetic underground water solutions, namely SGW1 type and SGW2 type, wherein SGW1 type is synthetic underground water only containing bromine tracers; SGW2 type is synthetic groundwater containing radionuclide adsorbent and bromine tracer; after the operation according to the fourth step, replacing the synthetic underground water solution introduced in the fourth step with SGW1 type; the process continues until the tracer bromide concentration collected in the sample collection tube is consistent with the initial bromide concentration, then the SGW1 model is replaced with the SGW2 model, and the process continues until the sorbent uranium concentration collected in the sample collection tube reaches 90% of the initial uranium concentration;
sixthly, observing, recording and determining experimental data: when the three-way air is finished in the step, the peristaltic pump starts to observe and record the experimental data, the experimental data of the pressure sensor and the temperature sensor are recorded at regular time, and each sample collecting test tube is set at regular time to collect 5ml of effluent liquid and then automatically transfers to the next test tube; the time setting of the automatic fraction collector can be determined by the percolation rate, which can be calculated from the flow of the effluent, and if the flow rate is higher, the set interval time is relatively smaller, and vice versa. The time for replacing the SGW1 type and the SGW2 type of the synthetic groundwater solution in the step five is based on the measured concentrations of the tracer and the adsorbent in the effluent liquid, so the concentrations of the tracer and the adsorbent are monitored in real time; the concentration of the radionuclide is determined by an ICP-OES instrument; the concentration of the tracer is determined by anion chromatography; by observing the concentration penetration curves of the adsorbent and the tracer at different times, the adsorption migration change rule of the adsorbent on the sample rock mass column can be visually observed; for the same sample rock mass column, the whole device needs to repeat the same group of experiments for 3 times in order to ensure the feasibility of the experimental result.
Compared with the prior art, the invention has the beneficial effects that:
1. because the research on the adsorption migration of nuclides on powdery minerals is too ideal, the migration of the nuclides in the real situation mainly occurs in cracks or broken zones of rocks. The research object that the device designed is to the original state contains the fissure rock pillar, and not rock mineral powder to make the experimental data of research nuclide absorption migration in the country rock, the law of detaining more laminate reality.
2. Through the design of the adjustable rock pillar volume, the limitation of the design of a general fixed-volume rock pillar is broken, the economic cost problem is considered, and rock pillars with different volumes can be flexibly used for researching the adsorption migration rule.
3. In order to prevent liquid from overflowing from the side surface of the sample rock mass column, 3 steps of sealing treatment measures carried out on the sample rock mass column are carried out in place, and the rock mass column is sequentially coated with a layer of epoxy resin on the surface of the rock mass column, sleeved with a layer of transparent emulsion film on the outer layer, and filled with gas to seal the rock mass column by utilizing air pressure.
4. The flow rate and the components of the liquid can be changed according to needs in the simulation process, and condition experiments and parallel tests under different influence conditions can be simultaneously carried out.
5. The experimental method is simple, convenient to operate, automatic in data collection, labor cost-saving, capable of repeating the experimental process, and high in reliability, and results can be contrastively analyzed.
Drawings
Fig. 1 is a schematic structural diagram of an experimental device for simulating the adsorption and migration of radioactive nuclides in a rock mass fracture.
Figure 2 is a right side view of the adsorptive mobility rock pillar apparatus.
Fig. 3 is a schematic diagram of a three-dimensional columnar structure of the adsorption and migration rock pillar device.
In the figure: a-variable rate liquid supply adjusting device, B-automatic effluent liquid collecting device and C-adsorption migrating rock pillar device; 1-a liquid supply bottle, 2-a synthetic underground water solution, 3-a liquid supply pipe, 4-a peristaltic pump, 5-a pressure sensor, 6-a temperature sensor, 7-a first hexagonal nut, 8-a pressure chamber bottom cover, 9-an organic glass cover, 10-a transparent emulsion film, 11-a water permeable plate, 12-an upright post, 13-a gas pressure meter, 14-a first quick connector, 15-a gas outlet pipe, 16-a gas valve, 17-a gas inlet pipe, 18-a gas cylinder, 19-an upright post, 20-an adjustable telescopic rod, 21-a second quick connector, 22-an adjusting rod, 23-a second hexagonal nut, 24-a liquid outlet pipe, 25-an effluent liquid, 26-a sample collection test tube, 27-an automatic partial collector and 28-a sample piece lower seat, 29-sample top cover, 30-sample rock pillar, 31-support, 32-plexiglass, 33-pressure chamber top cover.
Detailed Description
As shown in fig. 1, 2 and 3, an experimental device for simulating radionuclide adsorption migration in a rock mass fracture comprises a variable rate liquid supply adjusting device A, an adsorption migration rock pillar device C, an automatic collection and effluent device B, a pressure sensor 5, a temperature sensor 6, a barometer 13 and a gas bottle 18;
the variable-rate liquid supply adjusting device A consists of a liquid supply bottle 1, a synthetic underground water solution 2, a liquid supply pipe 3 and a peristaltic pump 4, wherein the synthetic underground water solution 2 is filled in the liquid supply bottle 1, and the synthetic underground water solution 2 enters the adsorption migration rock pillar device C through the liquid supply pipe 3. The synthetic underground water solution 2 is prepared by referring to the actual underground water ion composition of a field sampling area and is divided into an SGW1 type and an SGW2 type, and the SGW1 is synthetic underground water only containing a bromide ion tracer; SGW2 is a synthetic groundwater containing a radionuclide adsorbent and a bromide tracer. The peristaltic pump 4 adopts a BT100L model, the pump head adopts a DG10-4 model, the flow rate can be controlled between 0.21 mu L/min and 48mL/min, and the driving force is provided for the whole system. The flow rate of the peristaltic pump is adjustable, so that variable speed conditions are provided in the whole experiment process, and the influence of different flow rate changes on the adsorption and migration of the radioactive nuclide on the rock pillar can be observed.
The rock pillar adsorbing and migrating device C is a core area of the whole device and comprises a pressure chamber top cover 33, a pressure chamber bottom cover 8, a sample piece top cover 29, a sample piece lower seat 28, a water permeable plate 11, a first quick-plug connector 14, a second quick-plug connector 21, a sample rock pillar 30, a transparent emulsion film 10, an organic glass cover 9, organic glass 32, a support 31, a first upright post 12, a second upright post 19, a first hexagon nut 7, a second hexagon nut 23, a gas inlet pipe 17, a gas outlet pipe 15, an adjustable telescopic rod 20 and an adjusting rod 22; the pressure chamber bottom cover 8 is connected with the sample lower seat 28, the first quick-plug connector 14 is embedded into the sample lower seat 28, the adjustable telescopic rod 20 is externally connected with the sample top cover 29, the pressure chamber top cover 33 and the second upright post 19, the second upright post 19 is fixed with the adjustable telescopic rod 20 through the second hexagon nut 23, the adjustable telescopic rod 20 is internally connected with the adjusting rod 22 and the second quick-plug connector 21, the first upright post 12 and the organic glass cover 9 are connected between the pressure chamber top cover 33 and the pressure chamber bottom cover 8 and fixed through the first hexagon nut 7, the gas inlet pipe 17 and the gas outlet pipe 15 are embedded into the pressure chamber top cover 33 and the pressure chamber bottom cover 8, the gas inlet pipe 17 is externally connected with the barometer 13 and the gas bottle 18, the gas valve 16 is used for controlling the conveying of gas, and the gas outlet pipe 15 is externally connected with the gas valve for controlling the output of the gas; the liquid supply pipe 3 is externally connected with a pressure sensor 5 and a temperature sensor 6 to convey the synthetic groundwater solution 2 into a sample rock mass column 30 through a first quick-connection-peg 14, a sample lower seat 28 and a water permeable plate 11, and then flows into an automatic collection and effluent device B after flowing through an adjusting rod 22 and a second quick-connection-peg 21; the sample rock mass column 30 contains a single fracture;
the whole rock pillar adsorbing and migrating device C has two main characteristics:
the characteristics are as follows: the volume of the sample rock pillar 30 has a certain variable space, wherein the length of the rock pillar can be designed to be 5-12cm, and the variable space can be realized through the second upright post 19, the adjustable telescopic rod 20 and the adjusting rod 22; the corresponding diameter of the sample rock mass column 30 can be designed within the range of 5-7cm, and the height of the support 31 can be adjusted and controlled, and the matched sample lower seat 28, sample top cover 29 and water permeable plate 11 can be replaced. This kind of design that can regulate and control the rock pillar volume in certain within range has broken the limitation of general fixed volume rock pillar design, because the sample rock pillar volume 30 that different places or the different drilling in same place were taken may have certain difference, later stage can cause certain puzzlement to whole absorption migration rock pillar device B because of sample rock pillar volume is nonuniform when handling, the improper phenomenon that can cause sample rock pillar 30 breakage or sealed improper weeping of processing, thereby cause the unable used repeatedly's of rock specimen loss or experimental apparatus problem. In view of economic cost, the design of the adjustable rock pillar volume is necessary.
And (2) the characteristics: the whole device takes sealing treatment measures for the sample rock mass column 30 in place, and the purpose of preventing the sample rock mass column from leaking liquid is achieved through 3 steps. Firstly, coating a layer of epoxy resin with the thickness of 1-3mm on the side surface of a single-fracture rock mass column 30 to prevent liquid from laterally flowing out of the rock mass column; secondly, a transparent emulsion film with the thickness of 1mm is sleeved on the outer layer, and the effect of water resistance in the second step is achieved; finally, in order to make the sealing effect better, a gas bottle 18 is connected with a gas inlet pipe 17 through a control gas valve 16, so that the gas is conveyed into the whole adsorption migration column device C, and the gas pressure of the whole device is up to 2MPa through the reading of a barometer 13. The sealing effect of the single-crack sample rock mass column 30 is optimized through the 3 steps, and the error of the experimental result is reduced.
The automatic collection and effluent device B comprises an effluent pipe 24, an effluent liquid 25, a sample collection test tube 26 and an automatic part collector 27; the automatic partial collector 27 is of SBS-100 type, and can be used for sampling and collecting at regular time in the range of 1s-200h, or in the range of 1 drop-9999 drops in fixed drop sampling, and the sample collecting test tubes 26 are 100, and each tube has a maximum capacity of 12 ml. The automatic effluent collecting device B automatically collects the liquid flowing out from the adsorption and migration rock pillar device C into the sample collecting test tube 26 at regular time, and the test tube is controlled to be automatically replaced after every 5ml of effluent is collected.
The pressure sensor 5 and the temperature sensor 6 can monitor the temperature and the pressure of the synthesized underground water solution 2 in the liquid supply pipe 3 in real time before flowing into the adsorption migration rock pillar device C, and can provide data of the synthesized underground water solution and the pressure through real-time recording, so that certain theoretical basis and basic data support are provided for subsequently observed experimental data processing and analysis of radionuclide concentration or simulation of the adsorption migration rule of nuclides in the single-crack rock pillar by using a related model.
The working process of the invention is as follows:
the peristaltic pump 4 is electrified to rotate, the synthetic underground water solution 2 in the liquid supply pipe 3 is brought into the adsorption and migration rock pillar device C through the air pressure sensor 5 and the temperature sensor 6, the air bottle 18 provides an air pressure environment for the whole adsorption and migration rock pillar device C, the liquid flows through the quick first plug 14, the sample lower seat 28 and the water permeable plate 11 to enter the sample rock pillar 30 and then flows into the automatic collection effluent device B after flowing through the adjusting rod 22 and the second quick plug 21, after the liquid collected by the automatic part collector 27 reaches a preset concentration range, the peristaltic pump 4 and the automatic part collector 27 are powered off, and the whole process is ended.
In the invention, according to different types of surrounding rocks selected when deep geological processing banks are established in different countries to process radioactive nuclides, the single-crack sample rock body column 30 can be granite (China, Sweden and Canada), tuff (America), salt rock (Germany) and the like, and is selected according to the experiment requirement. The whole device for adsorbing and migrating the rock pillar is a cylinder, the length of the cylinder is 21cm, and the diameter of the cylinder is 14 cm; the shell is made of stainless steel and comprises a pressure chamber top cover 33, a pressure chamber bottom cover 8, a sample piece top cover 29, a sample piece lower seat 28, a first upright post 12, 4 upright posts 19, a first hexagonal nut 7, a second hexagonal nut 23, an adjustable telescopic rod 20, a first quick-plug connector 14 and a second quick-plug connector 21. The thicknesses of the pressure chamber top, the pressure chamber bottom cover, the sample piece top cover and the lower seat are all 2cm, the length of the first upright post 12 is 21cm, and the inner diameter is 1 cm; the length of the second upright post 19 is 9cm, and the inner diameter is 0.5 cm; the outer diameter of each hexagonal nut 7 is 1cm, and the inner diameter and the thickness of each hexagonal nut are 0.5 cm; the adjustable telescopic rod 20 is 13cm long and 2cm in inner diameter; the quick connector 14 or 21 has a length and an outer diameter of 1cm and an inner diameter of 0.25 cm. The inner layer structure of the device comprises organic glass 32, a bracket 31, an adjusting rod 22, a water permeable plate 11 and gas inlet and outlet pipes 17 and 15. The outer diameter of the organic glass 32 is 9cm, the inner diameter is 7cm, and the thickness is 1 cm; the support 31 is made of organic glass and is 12.5cm long, and the height of the support is reduced along with the increase of the diameter of the sample rock mass column 30 and ranges from 0cm to 1 cm; the thickness of the permeable plate 11 is 0.3 cm; the length of the adjusting rod 22 is 11cm, and the inner diameter is 0.25 cm. The inner diameters of a liquid supply pipe 3 and a liquid outflow pipe 24 of the whole experimental device are 0.1 cm; in order to bring the radionuclide into sufficient contact with the single-crack interface of the sample rock column 30, the flow rate of the peristaltic pump 4 may be set to 0.3 ml/h; the autoscore collector 27 automatically transfers to the next tube each time the sample tube 26 is collected to a capacity of 5 ml.
A test method using the simulation device for radionuclide adsorption migration in a rock mass fracture comprises the following steps:
firstly, rock pillar pretreatment and sealing: the sample rock pillar 30 is selected according to the experimental requirements, and a standard granite rock pillar with the length of 10cm and the diameter of 5cm is taken as an example for explanation; in order to generate a single crack in the granite core, the single crack is pretreated by using a Brazilian splitting method, and after treatment, a sealing measure is taken for the granite core with the single crack, firstly, a layer of epoxy resin with the thickness of 1-3mm is coated on the side surface of a single crack rock body column 30, and then, a transparent emulsion film 10 with the thickness of 1mm is sleeved on the outer layer of the single crack rock body column;
secondly, assembling the rock pillar device: the whole adsorption and migration rock pillar device C is detachable and recombined; assembling the sample rock cylinder body 30 subjected to primary sealing treatment in the first step sequentially according to the pressure chamber bottom cover 8, the first quick-connection plug 14, the water permeable plate 11, the sample rock cylinder body 30, the organic glass 32, the support 31, the first upright post 12, the sample piece top cover 29, the pressure chamber top cover 33, the adjusting rod 22, the adjustable telescopic rod 20, the second upright post 19 and the second quick-connection plug 21; the outside is connected with a gas bottle 18 through a gas inlet pipe 17, gas is selected according to experiment requirements, and argon is selectively introduced at the position; the first quick-connection plug 14 is externally connected with a liquid supply pipe 3, the synthetic underground water solution 2 in the liquid supply bottle 1 is introduced into the first quick-connection plug 14 by a peristaltic pump 4, the flow rate is set according to the experimental requirements, the initial setting is 0.3ml/h, and a group of pressure sensors 5 and temperature sensors 6 are arranged on the liquid supply pipe 3 before introduction;
thirdly, ventilating the rock pillar: in order to prevent the phenomenon that liquid overflows from the side face of the rock pillar when the liquid is introduced into the single-fracture sample rock pillar 30, a gas bottle 18 is connected with a gas inlet pipe 17 through a control gas valve 16, and simultaneously, the gas valve of a gas outlet pipe 15 is opened, so that the gas is conveyed into the whole adsorption migration column device C, the gas valve of the gas outlet pipe 15 is closed after the gas is continuously introduced for a few minutes, the gas is continuously introduced, the gas pressure of the whole device is controlled to be about 2MPa through the reading of a gas pressure meter 13, the gas tightness is observed, and the gas valve 16 is closed if the reading of the gas pressure meter 13 is stabilized at 2 MPa;
fourthly, initially balancing the water supply of the rock pillar: the synthetic underground water solution 2 is selected according to the experimental requirements, and is prepared and synthesized according to the ion components of underground water in the depth of 600m of a certain drilled hole in certain northwest China; firstly, measuring the initial concentration and pH of each ion in the prepared and synthesized underground water solution 2; starting the whole device, setting the flow rate of the peristaltic pump 4 to be 0.3ml/h, wherein the flow rate in the whole process is very slow, further discharging bubbles sealed in the sample rock mass column 30, and observing the flow rate, the ion concentrations and the pH value of the effluent liquid 25 in the sample collection test tube 26 at intervals, so as to calculate the real flow rate and the stability of the synthetic underground water solution 2 flowing in the whole sample rock mass column 30, wherein the process is continued until the flow output of the effluent liquid 25 is stable and the ion concentrations and the pH values are consistent with the initial measurement result, which indicates that the initial water supply state of the rock mass column reaches a balance state;
fifthly, injecting an adsorbent and a tracer: the adsorbent and the tracer can be selected independently according to different experimental requirements, and the principle is that the adsorbent can be adsorbed with the sample rock mass column 30 and the concentration change before and after the reaction can be detected by a measuring instrument; the tracer hardly reacts chemically with the sample rock mass column 30 and does not belong to a component in the synthetic underground aqueous solution, and the measurement mode is simple. Here, the adsorbent is exemplified by radionuclide U, and the concentration is selected according to a laboratory setting standard that the initial concentration is generally 10 to 100 times higher than the concentration of the component in the natural underground aqueous solution, and the initial concentration of uranium is set to 2.0 x 10-5mol/L; the tracer is exemplified by bromide ion, and the concentration is set to 1.0 x 10-2mol/L; two types of synthetic underground water solutions 2 are prepared into SGW1 type and SGW2 type, and the SGW1 type is synthetic underground water only containing bromine tracer; SGW2 type is synthetic groundwater containing radionuclide adsorbent and bromine tracer; after the operation according to the fourth step, replacing the synthetic underground water solution 2 introduced in the fourth step with SGW1 type; this process continues until the tracer bromide concentration collected by the sample collection tube 26 is consistent with the initial bromide concentration, followed by replacement of the SGW1 version with the SGW2 version, until the sorbent uranium concentration collected by the sample collection tube 26 reaches 90% of the initial uranium concentration;
sixthly, observing, recording and determining experimental data: when the three-way air is finished in the step, the peristaltic pump 4 is started to start to observe and record the experimental data, the experimental data of the pressure sensor 5 and the temperature sensor 6 are recorded at regular time, and each sample collecting test tube 26 is set at regular time to collect 5ml effluent liquid 25 and then automatically transfers to the next test tube; the timing of the automatic fraction collector 27 can be determined by the percolation rate, which can be calculated from the flow of effluent 25, and by setting the interval times to relatively smaller values if the flow rate is higher, and vice versa. Since the time for the replacement of the synthetic groundwater solution SGW1 type and SGW2 type in step five depends on the measured concentrations of the tracer and the adsorbent in the effluent 25, the concentrations of the two need to be monitored in real time; the concentration of the radionuclide is determined by an ICP-OES instrument; the concentration of the tracer is determined by anion chromatography; by observing the concentration penetration curves of the adsorbent and the tracer at different times, the adsorption migration change rule of the adsorbent on the sample rock mass column 30 can be visually observed; the whole device needs to repeat the same set of experiments 3 times for the same sample rock pillar 30 to ensure the feasibility of the experimental results.
Claims (4)
1. An experimental device for simulating the adsorption and migration of radioactive nuclides in a rock mass fracture is characterized in that: comprises a variable rate liquid supply adjusting device (A), an adsorption and migration rock pillar device (C), an automatic effluent liquid collecting device (B), a pressure sensor (5), a temperature sensor (6), a barometer (13) and a gas bottle (18);
the variable-rate liquid supply adjusting device (A) consists of a liquid supply bottle (1), a synthetic underground aqueous solution (2), a liquid supply pipe (3) and a peristaltic pump (4), wherein the synthetic underground aqueous solution (2) is arranged in the liquid supply bottle (1), and the synthetic underground aqueous solution (2) enters the adsorption migration rock pillar device (C) through the liquid supply pipe (3);
the adsorption migration rock pillar device (C) is a core area of the whole device and comprises a pressure chamber top cover (33), a pressure chamber bottom cover (8), a sample top cover (29), a sample lower seat (28), a water permeable plate (11), a first quick-plug connector (14), a second quick-plug connector (21), a sample rock pillar (30), a transparent latex film (10), an organic glass cover (9), organic glass (32), a support (31), a first upright column (12), a second upright column (19), a first hexagon nut (7), a second hexagon nut (23), a gas inlet pipe (17), a gas outlet pipe (15), an adjustable telescopic rod (20) and an adjusting rod (22); the pressure chamber bottom cover (8) is connected with the sample lower seat (28), the first quick-plug connector (14) is embedded in the sample lower seat (28), the adjustable telescopic rod (20) is externally connected with the sample top cover (29), the pressure chamber top cover (33) and the second upright post (19), the second upright post (19) is fixed with the adjustable telescopic rod (20) through a second hexagon nut (23), the adjustable telescopic rod (20) is internally connected with an adjusting rod (22) and a second quick-plug connector (21), the first upright post (12) and the organic glass cover (9) are connected between the pressure chamber top cover (33) and the pressure chamber bottom cover (8) and fixed through a first hexagon nut (7), the gas inlet pipe (17) and the gas outlet pipe (15) are embedded in the pressure chamber top cover (33) and the pressure chamber bottom cover (8), the gas inlet pipe (17) is externally connected with a gas pressure gauge (13) and a gas bottle (18), the gas valve (16) is used for controlling the gas delivery, and the gas outlet pipe (15) is externally connected with the gas valve and used for controlling the gas output; the synthetic underground water solution (2) is conveyed into the sample rock mass column (30) by the pressure sensor (5) and the temperature sensor (6) which are externally connected with the liquid supply pipe (3) through the first quick-connection-peg (14), the sample lower seat (28) and the water permeable plate (11), and then flows into the automatic collection effluent device (B) after flowing through the adjusting rod (22) and the second quick-connection-peg (21);
the automatic collection effluent device (B) comprises an effluent liquid pipe (24), an effluent liquid (25), a sample collection test tube (26) and an automatic part collector (27); the automatic collection effluent device (B) automatically collects the liquid flowing out from the adsorption and migration rock column device (C) into a sample collection test tube (26) at regular time;
said sample rock mass column (30) containing a single fracture;
the pressure sensor (5) and the temperature sensor (6) monitor the temperature and the pressure of the synthesized underground water solution (2) in the liquid supply pipe (3) in real time before flowing into the adsorption and migration rock pillar device (C);
the peristaltic pump (4) is electrified and rotated, the synthetic underground water solution (2) in the liquid supply pipe (3) is brought into the adsorption migration rock pillar device (C) through the air pressure sensor (5) and the temperature sensor (6), the gas bottle (18) provides an air pressure environment for the whole adsorption migration rock pillar device (C), the liquid flows through the first quick plug (14), the sample lower seat (28) and the water permeable plate (11) to enter the sample rock pillar (30), then flows through the adjusting rod (22) and the second quick plug (21) to flow into the automatic collection effluent device (B), after the liquid collected by the automatic partial collector (27) reaches a preset concentration range, the peristaltic pump (4) and the automatic partial collector (27) are powered off, and the whole process is terminated.
2. The experimental device for simulating radionuclide adsorption migration in rock mass fractures according to claim 1, characterized in that: the synthetic underground water solution (2) is prepared by referring to the actual underground water ion composition of a field sampling area and is divided into an SGW1 type and an SGW2 type: SGW1 type synthetic groundwater containing only bromide ion tracer; SGW2 type is synthetic groundwater containing radionuclide adsorbent and bromide tracer; the peristaltic pump (4) adopts a BT100L model, the pump head adopts a DG10-4 model, and the flow rate is controlled to be 0.21 mu L/min-48 mL/min.
3. The experimental device for simulating radionuclide adsorption migration in rock mass fractures according to claim 1, characterized in that: the automatic partial collector (27) is of SBS-100 type, and the sampling and collecting range is 1s-200h at regular time, or the sampling range is 1 drop-9999 drops at regular drop; the sample collection tubes (26) are 100 tubes each having a maximum capacity of 12 ml.
4. An experimental method of the experimental device for simulating the adsorption and migration of the radionuclide in the rock mass fracture as claimed in claim 1, is characterized in that: the method comprises the following steps:
firstly, rock pillar pretreatment and sealing: the sample rock pillar (30) is selected according to experiment requirements, and a standard granite rock pillar with the length of 10cm and the diameter of 5cm is taken as an example for explanation; in order to generate a single crack in the granite core, the single crack is pretreated by using a Brazilian splitting method, and after treatment, a sealing measure is taken for the granite core with the single crack, firstly, a layer of epoxy resin with the thickness of 1-3mm is coated on the side surface of a single crack rock body column (30), and then, a transparent latex film (10) with the thickness of 1mm is sleeved on the outer layer of the single crack rock body column;
secondly, assembling the rock pillar device: the whole adsorption and migration rock pillar device (C) is detachable and recombined; assembling the sample rock pillar body (30) subjected to primary sealing treatment in the first step sequentially according to a pressure chamber bottom cover (8), a first quick-insertion connector (14), a water permeable plate (11), a sample rock pillar body (30), organic glass (32), a support (31), a first upright post (12), a sample piece top cover (29), a pressure chamber top cover (33), an adjusting rod (22), an adjustable telescopic rod (20), a second upright post (19) and a second quick-insertion connector (21); the outside is connected with a gas bottle (18) through a gas inlet pipe (17), gas is selected according to experiment requirements, and argon is selectively introduced at the position; the first quick-connection plug (14) is externally connected with a liquid supply pipe (3), the synthetic underground water solution (2) in the liquid supply bottle (1) is led into the first quick-connection plug (14) by a peristaltic pump (4), the flow rate is set according to the experimental requirement, the flow rate is preliminarily set to be 0.3ml/h, and a group of pressure sensors (5) and temperature sensors (6) are arranged on the liquid supply pipe (3) before leading;
thirdly, ventilating the rock pillar: in order to prevent the phenomenon that liquid overflows from the side face of a single-crack sample rock mass column (30) when the liquid is introduced into the rock mass column, a gas bottle (18) is connected with a gas inlet pipe (17) through a control gas valve (16), the gas valve of a gas outlet pipe (15) is opened at the same time, so that the gas is conveyed into the whole adsorption migration column device (C), the gas valve of the gas outlet pipe (15) is closed after the gas is continuously introduced for a few minutes, the gas is continuously introduced, the gas pressure of the whole device is controlled to be 2MPa through the reading of a barometer (13), the airtightness is observed, and the gas valve (16) is closed if the reading of the barometer (13) is stabilized to be 2 MPa;
fourthly, initially balancing the water supply of the rock pillar: selecting the synthetic underground water solution (2) according to experimental requirements, and firstly measuring the initial concentration and pH of each ion in the prepared synthetic underground water solution (2); starting the whole device, setting the flow rate of the peristaltic pump (4) to be 0.3ml/h, wherein the flow rate in the whole process is very slow, further discharging bubbles sealed in the sample rock mass column (30), observing the flow rate, the concentration of each ion and the pH of the effluent (25) in the sample collection test tube (26) at intervals, and calculating the real flow rate and the stability of the synthetic underground water solution (2) flowing in the whole sample rock mass column (30), wherein the process is continued until the flow output of the effluent (25) is stable and the concentration of each ion and the pH value are consistent with the initial measurement result, so that the initial balance state of the water supply of the rock mass column is achieved;
fifthly, injecting an adsorbent and a tracer: the adsorbent and the tracer can be selected independently according to different experimental requirements, and the principle is followed that the adsorbent can be adsorbed with the sample rock mass column (30) and can be detected by a measuring instrumentThe change in concentration before and after the reaction; the tracer hardly reacts with the sample rock mass column (30) chemically, and does not belong to the components in the synthetic underground water solution, and the measuring mode is simple; here, the adsorbent is exemplified by radionuclide U, and the concentration is selected according to a laboratory setting standard that the initial concentration is generally 10 to 100 times higher than the concentration of the component in the natural underground aqueous solution, and the initial concentration of uranium is set to 2.0 x 10-5mol/L; the tracer is exemplified by bromide ion, and the concentration is set to 1.0 x 10-2mol/L; preparing two types of synthetic underground water solutions (2) of SGW1 type and SGW2 type, wherein the SGW1 type is synthetic underground water only containing a bromine tracer; SGW2 type is synthetic groundwater containing radionuclide adsorbent and bromine tracer; after the operation according to the fourth step, replacing the synthetic underground water solution (2) introduced in the fourth step with SGW1 type; the process continues until the tracer bromide concentration collected by the sample collection tube (26) is consistent with the initial bromide concentration, and then the SGW1 model is replaced with the SGW2 model, and the process continues until the adsorbent uranium concentration collected by the sample collection tube (26) reaches 90% of the initial uranium concentration;
sixthly, observing, recording and determining experimental data: when the three-way air is finished in the step, the peristaltic pump (4) is started to start to observe and record the experimental data, the experimental data of the pressure sensor (5) and the temperature sensor (6) are recorded at regular time, and each sample collecting test tube (26) is set at regular time to collect 5ml of effluent liquid (25) and then automatically transfer to the next test tube; the time setting of the automatic fraction collector (27) can be determined by the percolation rate, which can be calculated from the flow of the effluent (25), and if the flow rate is higher, the set interval time is relatively smaller, and vice versa; since the time for the replacement of the synthetic groundwater solution SGW1 type and SGW2 type in step five depends on the measured concentrations of the tracer and the adsorbent in the effluent (25), the concentrations of both need to be monitored in real time; the concentration of the radionuclide is determined by an ICP-OES instrument; the concentration of the tracer is determined by anion chromatography; by observing concentration penetration curves of the adsorbent and the tracer at different times, the adsorption migration change rule of the adsorbent on the sample rock mass column (30) can be visually observed; the whole device needs to repeat the same group of experiments 3 times for the same sample rock pillar (30) in order to ensure the feasibility of the experimental result.
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