CN112505078B - Method for researching evolution of water chemistry environment in multiple barrier system - Google Patents
Method for researching evolution of water chemistry environment in multiple barrier system Download PDFInfo
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- G01N23/207—Diffractometry using detectors, e.g. using a probe in a central position and one or more displaceable detectors in circumferential positions
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Abstract
The invention discloses a method for researching evolution of a water chemistry environment in a multiple barrier system, which comprises the following steps: s1, collecting rock and mineral samples related to a multiple barrier system, and determining relevant parameters such as mineral composition of the samples; s2, collecting underground water, and determining all chemical parameters of the initial underground water; s3, carrying out rock-soil material physical property parameter test research on a mineral sample, and determining related parameters such as a saturation permeability coefficient, a porosity, a cation exchange capacity and the like; s4, carrying out a corrosion simulation experiment on the packaging container to determine the average corrosion rate of the container in the barrier system; s5, carrying out long-term numerical simulation research. The method provided by the invention is not limited, can be suitable for various different disposal warehouse structures, and can determine multi-component and multi-variable chemical reactions occurring in the water-rock interaction and container corrosion processes in a multi-barrier system on the basis of a series of physical parameter test researches and simulation experiments.
Description
Technical Field
The invention belongs to the technical fields of environmental science and geochemistry, and relates to a method for researching evolution of a water chemistry environment in a multilayer barrier system, which can be applied to site selection of disposal libraries and safety evaluation of waste disposal.
Background
With the rapid development of nuclear power, china will accumulate a considerable amount of high level waste, and safe and effective treatment and disposal of the high level waste is of great importance for the wide application of nuclear technology. The strategy of high-level waste disposal in China is to carry out deep geological disposal after solidification of the waste, and effectively isolate the waste from the human living environment by utilizing multiple protections such as packaging containers, engineering barriers, natural barriers and the like.
Because of the large total activity and specific activity of high level waste, high toxicity, and the long half-life of many species, disposal bins are typically designed for safety years of 10 to 100 tens of thousands of years. During this period, multiple barriers of the treatment library may be damaged due to rainfall, weathering, corrosion, earth crust activities and the like, so that radionuclides in the treatment library are released, wherein the dissolution and retardation of the radionuclides by the water chemical environment and the geological medium are key factors for controlling the diffusion and migration of the radionuclides for a long time, and the interaction of water and the medium material further changes the water chemical environment within a treatment time of up to ten thousands years, so that in order to accurately predict the migration behavior of the nuclides, the long-term safety of the treatment library is evaluated, and the water chemical evolution rule under the multiple barrier environment is the most important one, however, in the process of researching the evolution of the water chemical environment, the experimental means of light is insufficient, and a corresponding model must be established to obtain the predicted distribution of nuclides on the time and space scales.
At present, the research of the high-level waste disposal warehouse in China is mainly focused on the interaction between granite and underground water, the research on the change of the near-field water chemistry environment of the disposal warehouse along with time and space is less, and the following problems exist:
(1) In the research of the evolution of the water chemistry environment, reverse simulation is mostly adopted, namely, the principle of mass conservation is taken as a basic theory, an initial aqueous solution component, a reactant=an end aqueous solution component and a product are adopted, wherein the reactant and the product refer to substances entering or leaving a solution in the reaction process, and the substances can be gas, solid or ion exchange, and are a set of fuzzy phases. In a given hydrogeologic system, in general, there are multiple "possible reactant-product" combinations that satisfy the above formula, where the most likely "reactant" and "product" under the condition need to be determined according to factors such as lithology, geology, hydrogeologic conditions of the research area, and component distribution calculation results, thermodynamic parameters, and isotope data, so that the formation and evolution rules of the water chemistry under the condition cannot be accurately obtained only through starting points and ending points, and especially for the water chemistry evolution under a specific path, the reverse simulation cannot satisfy the requirements;
(2) At present, the water chemistry environment evolution scene is mostly the interaction between natural granite barriers and groundwater, and the complex problems faced by multiple barrier structures in a near-field environment, such as container corrosion, chemical reactions among various barrier layers and the like, are not involved.
In summary, on the basis of the water-rock interaction reaction mechanism, a water chemical environment evolution model is established, and a more accurate and systematic method for researching the water chemical environment evolution under a multiple barrier system is one of key factors for evaluating whether a disposal warehouse can reliably block the migration of radioactive wastes, so that the site selection of the disposal warehouse in China, the safety evaluation of the radioactive wastes and the sustainable development of nuclear technology are determined.
Disclosure of Invention
Aiming at the problem that the existing research method can not meet the requirement of the evolution of the water chemistry environment in the multi-barrier system, the invention provides a forward simulation research method of the multi-barrier system in a large scale time range, and determines multi-component and multi-variable chemical reactions occurring in the water-rock interaction and container corrosion process in the multi-barrier system on the basis of a series of physical property parameter test researches and simulation experiments.
In order to achieve the above object, the present invention provides the following solutions:
the method for researching the water chemistry evolution in the multiple barrier system is characterized by comprising the following steps of:
S1, collecting rock and mineral samples related to a multiple barrier system, and determining related parameters of mineral composition of the rock and mineral samples;
S2, collecting underground water, and determining all chemical parameters of the initial underground water;
S3, carrying out rock-soil material physical property parameter test research on the rock-mineral sample, and determining parameters related to saturation permeability coefficient, porosity and cation exchange capacity;
S4, carrying out a corrosion simulation experiment on the packaging container, and determining the average corrosion rate of the packaging container in the barrier;
S5, carrying out long-term numerical simulation research.
Preferably, the specific steps of determining the parameters related to the mineral composition of the rock sample in the step S1 are:
s1.1, crushing and grinding the collected rock-ore sample to prepare powder with the particle size of 200 meshes;
S1.2, identifying rock sample powder through X-ray diffraction, and determining rock type, mineral composition and content.
Preferably, the specific steps of determining each chemical parameter of the initial groundwater in the step S2 are:
s2.1, storing the collected groundwater sample in an inert gas atmosphere;
S2.2, measuring the contents of carbonate ions and bicarbonate ions in the groundwater sample by a potentiometric titration method;
S2.3, obtaining the content of anions and cations in the groundwater sample through an ion chromatography and an atomic emission spectrometry, and measuring the dissolved oxygen content, the pH value and the Eh value of the water sample through a dissolved oxygen meter, a pH meter and an Eh meter.
Preferably, the specific steps for determining the parameters related to the permeability coefficient, the porosity and the cation exchange capacity in the step S3 are as follows:
s3.1, carrying out saturation permeability coefficient test through a flexible wall permeameter, and calculating to obtain a saturation permeability coefficient;
S3.2, measuring the porosity of minerals;
s3.3, measuring the cation exchange content of minerals.
Preferably, the specific steps for simulating the corrosion test of the packaging container in the step S4 are as follows:
The 16MnR bare steel sheet is buried in a buried layer with a certain thickness for 4 years, the buried layer is continuously soaked by field groundwater during the period, sampling is carried out in different time periods, and the average corrosion rate of the steel sheet is calculated by adopting a weightlessness method.
Preferably, the specific steps of developing the long-term numerical simulation study in the step S5 are:
S5.1, dividing the whole multi-barrier system into a plurality of tiny units by using geochemistry simulation software, wherein each tiny unit represents a complete water-rock interaction system;
S5.2, completely and independently simulating water flow by using a random walking method, and determining the direction and speed of the water flow field, boundary conditions of inflow and outflow and diffusion coefficients and diffusion distances of components in the water to obtain a calculated water flow field;
s5.3, performing improved characteristic method simulation on the basis of the calculated water flow field.
S5.4, calculating the time required by the pore water flowing through the barrier according to the seepage rate of the rock and ore, and obtaining the evolution of the water chemistry environment in large scale time by setting the flushing times of the pore water.
Compared with the prior art, the invention has the following advantages:
the method provided by the invention is not limited, can be suitable for various different disposal warehouse structures, can obtain the evolution of the water chemistry environment in a large-scale time range, and can obtain the evolution rule of the water chemistry environment and the change rule of mineral composition along the water flow path.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions of the prior art, the drawings that are needed in the embodiments will be briefly described below, it being obvious that the drawings in the following description are only some embodiments of the present invention, and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a flow chart of the method of the present invention;
FIG. 2 is a schematic diagram of a multiple barrier system according to the present invention;
FIG. 3 is a schematic diagram showing the sequential reaction of groundwater and a barrier according to the invention.
Detailed Description
The following description of the embodiments of the present invention will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
In order that the above-recited objects, features and advantages of the present invention will become more readily apparent, a more particular description of the invention will be rendered by reference to the appended drawings and appended detailed description.
The process flow is shown in fig. 1.
S1, collecting rock and mineral samples related to a multiple barrier system, and determining relevant parameters such as mineral composition of the samples, wherein the specific steps are as follows: (1) Crushing and grinding the collected minerals to prepare powder with the particle size of 200 meshes; (2) And determining the rock type, mineral composition and content through X-ray diffraction identification. The mineral composition is shown in Table 1:
TABLE 1
S2, collecting underground water, and determining various chemical parameters of the initial underground water, wherein the specific steps are as follows:
(1) The collected water sample is stored in an inert gas atmosphere as soon as possible; (2) Obtaining the carbonate and bicarbonate ion content in the water sample by a potentiometric titration method; obtaining the content of anions and cations in a water sample by an ion chromatography and an atomic emission spectrometry; (3) The dissolved oxygen content, pH and Eh values of the water sample are measured by a dissolved oxygen meter, a pH meter and an Eh meter. The groundwater chemistry parameters are shown in Table 2:
TABLE 2
S3, carrying out rock-soil material property parameter test research on the mineral sample, and determining parameters related to permeability coefficient, porosity and cation exchange capacity. The method comprises the following specific steps:
(1) The saturation permeability coefficient is tested, the experimental instrument is a TK-2000 type flexible wall permeameter, and the method is as follows:
① Sample preparation
Adding distilled water into bentonite soil sample according to preset water content by spraying method to uniformly wet the sample, and placing into a humidifier for curing for 60h. And (3) adopting a JDS-2 standard compaction instrument to carry out compaction and prepare a sample for later use.
② Sample saturation
Because the sample has lower permeability and greater expansibility, it is difficult to achieve saturation using typical saturation methods. The experiment adopts a step-by-step back pressure saturation method, namely, gradient confining pressure and osmotic pressure are applied to the sample, so that the sample is saturated rapidly. Distilled water is used as a seepage medium in the experimental process, and the experimental process is saturated for 27 days.
③ Permeation experiments
Variable head permeation experiments were performed at room temperature of 25℃using distilled water as the pore liquid according to ASTM (D5084-03) test specification. The experimental permeation period lasts for 17 days, and the permeation coefficient finally tends to be stable.
④ Saturation osmotic coefficient calculation
By monitoring the water level change of the seepage variable head pipe, the saturated hydraulic conductivity (permeability coefficient) k of the sample is calculated by using the following formula (1):
Wherein: k-permeability coefficient, cm/s; a in、aout -cross-sectional areas of the permeate and permeate tubes, cm 2; l-permeate length through the sample, cm; a, cross-sectional area of a sample, cm 2;t0、ts, start and stop time of a reading head, s; h in、hout -the head of the infiltration and exudation tubes, cm; p in、pout -gas pressure applied to the infiltration head and the infiltration head, kPa; gamma w -the severity of the permeate at the temperature conditions tested, kN/m 3.
(2) The method for measuring the porosity of the minerals comprises the following steps:
① Specific gravity calibrating bottle
The pycnometer (100 ml) was washed, dried, placed in a desiccator, cooled, and weighed to an accuracy of 0.001g. Pouring the boiled and cooled pure water into a specific gravity bottle. The short-neck specific gravity bottle is filled with water, the bottle stopper is tightly plugged, the excessive water overflows from the capillary tube of the bottle stopper, and the specific gravity bottle is placed into a constant-temperature water tank until the water temperature in the bottle is stable. Taking out the specific gravity bottle, wiping the outer wall, weighing the total mass of the bottle and the water to 0.001g, and measuring the water temperature in the constant temperature water tank to 0.5 ℃. And (3) regulating the temperature in the constant-temperature water tanks, wherein the temperature difference is 5 ℃, and measuring the total mass of the bottle and the water at different temperatures. Two replicates were performed at each temperature, the difference between the two determinations being no greater than 0.002g, and the average of the two determinations was taken. And drawing a relation curve of temperature and the total mass of the bottle and the water.
② Experimental procedure
The specific gravity bottle was dried, the dried sample was weighed to about 15g, and the total mass of the sample and bottle was weighed to the nearest 0.001g. Injecting half bottle of pure water into the gravity bottle, shaking the gravity bottle, and boiling in sand bath for not less than 30min, and not less than 1 hr for clay and silt. The temperature should be regulated after boiling, and the suspension in the specific gravity bottle should not overflow.
Boiled and cooled pure water was injected into a specific gravity flask containing a sample suspension. When the bottle with short neck specific gravity is used, pure water is filled, the bottle stopper is tightly plugged, and the redundant water overflows from the capillary tube of the bottle stopper. The specific gravity bottle is placed in a constant temperature water tank, the temperature is stable, and suspension at the upper part in the bottle is clarified. Taking out the specific gravity bottle, wiping the outer wall of the bottle, weighing the total mass of the specific gravity bottle, water and a sample, and accurately obtaining 0.001g; and the temperature of water in the bottle should be measured to be accurate to 0.5 ℃. And (5) searching the total mass of the bottle and the water at each test temperature from the relation curve of the temperature and the total mass of the bottle and the water.
③ Total pore calculation
The rock pores determined in this experiment are total pores, including closed pores and open pores. Calculated according to the following formula (2):
n＝(1-ρd/Gs·ρw)*100 (2)
Wherein: n-porosity; ρ d -dry density of rock mass, g/cm 3;ρw -density of water under test conditions, g/cm 3;Gs -density of rock particles.
(3) The method for measuring the cation exchange content of minerals comprises the following steps:
① Determination of the content of exchangeable cations
1G of a sample was weighed, 15mL of an ammonium chloride-ammonia leaching solution was added, stirred on a magnetic stirrer, suction-filtered with a microporous filter membrane, and the filtrate was diluted to 100mL. Sucking 10.0mL of the test solution into a 100mL quartz beaker, adding 2-3 drops of hydrochloric acid, evaporating to dryness at low temperature, adding 2mL of hydrochloric acid and 10mL of water, heating to boil to dissolve salts, cooling, transferring into a 100mL plastic volumetric flask, diluting to scale with water, and uniformly mixing. The content of exchangeable cations K +、Na+、Ca2+、Mg2+ was determined on an atomic emission spectrometer.
② Total Cation Exchange Capacity (CEC)
The residue was added with 25mL of formaldehyde-calcium chloride solution, 4 drops of phenolphthalein indicator, and titrated to a pink color with 0.05mol/L sodium hydroxide standard solution. The cation exchange capacity was calculated as the volume of spent sodium hydroxide standard solution. The cation exchange capacity was calculated using the following formula (3):
CEC＝C(NaOH)*V/m (3)
Wherein: CEC-cation exchange capacity, mmol/g; c (NaOH) -NaOH standard solution concentration, mol/L; v-volume of NaOH standard solution consumed during titration, mL; m-sample mass, g.
Table 3 shows the saturation permeability of each barrier, table 4 shows the porosity of each mineral, table 5 shows the total cation exchange capacity of the mineral, and Table 6 shows the cation content of the exchangeable mineral of the second layer, for detecting how many ions can be exchanged out of the mineral;
TABLE 3 Table 3
| Mineral material | Saturation osmotic coefficient (m/s) |
| First layer | 4.99E-10 |
| Second layer | 3.81E-10 |
| Third layer | 2.54E-10 |
| Cured layer | 6.36E-10 |
TABLE 4 Table 4
| Mineral material | Dry Density (g/cm 3) | Porosity% |
| First layer (80 mesh) | 2.38 | 30.0 |
| Second layer (80 mesh) | 1.50 | 42.0 |
| Third layer (80 mesh) | 1.12 | 51.3 |
| Solidified layer (80 mesh) | 1.70 | 36.5 |
TABLE 5
| Mineral material | CEC(mmol/g) |
| Second layer (80 mesh) | 0.43 |
| Third layer (80 mesh) | 0.06 |
| Solidified layer (80 mesh) | 0.01 |
TABLE 6
S4, carrying out corrosion simulation experiments on the packaging container, and determining the average corrosion rate of the container in the barrier, wherein the method comprises the following specific steps: the 16MnR bare steel sheet is buried in a buried layer with a certain thickness for 4 years, the buried layer is continuously soaked by field groundwater during the period, sampling is carried out in different time periods, and the average corrosion rate of the steel sheet is calculated by adopting a weightlessness method.
Table 7 shows the corrosion weight gain data for the test pieces at various times.
TABLE 7
S5, carrying out numerical simulation research
(1) Determining reaction paths and various reaction types of water-rock interaction in a multiple barrier system by combining mineral composition, underground water chemical composition, water-rock interaction reaction equation and the like, wherein the reaction paths and various reaction types of the water-rock interaction in the multiple barrier system are shown in a table 8, and the sequential reaction schematic diagram of underground water and barriers is shown in fig. 3;
TABLE 8
(2) The reaction sites and reaction processes in the corrosion process of the container are reasonably simplified in the model, the container and the solidified waste are regarded as a whole, and the porosity and the initial pore water composition of the container are further considered to be consistent with the solidified minerals.
(3) In an actual multiple barrier environment, the simulation Time is Time year, and according to the sequence of the artificial barrier layers, the pore ratio, the seepage rate and other characteristics, the whole system is divided into a plurality of small units (figure 2) with the length of 0.1m on a one-dimensional level, and a numerical simulation model is established. 1kg of pore water is converted into corresponding initial mineral content according to the porosity, mineral density and the like. The specific calculation method is exemplified by quartz contained in the cured layer:
① The cured layer had a dry density of 1.7g/cm 3 and a porosity of 0.36 (Table 4)
② The total mass of the cured layer corresponding to a volume of 1L is m=ρ=v=1.7×1000=1700 g
③ The mass of the solidified layer corresponding to 1kg of pore water is as follows: m=1700/0.36= 4722.2g
④ The mass of quartz in the solidified layer is as follows: m (quartz) =m x w% =4722.2 x 0.037= 174.7g
⑤ The mole number of quartz in the cured layer is: n (quartz) =m (quartz)/M (molar mass) = 174.7/60=2.91 mol
(4) Simulating a groundwater long-term infiltration multiple barrier system. Based on a numerical model, under the constraint of different thermodynamic data and kinetic data of minerals, the geochemical simulation software is utilized to conduct long-term evolution research of the water chemistry environment, and the reactions involved in the simulation research are shown in Table 8.
(5) In the process of water-rock simulation research, various reactions are carried out simultaneously and are mutually coupled, and the water chemistry environment changes along with the change of time and space.
The above embodiments are only illustrative of the preferred embodiments of the present invention and are not intended to limit the scope of the present invention, and various modifications and improvements made by those skilled in the art to the technical solutions of the present invention should fall within the protection scope defined by the claims of the present invention without departing from the design spirit of the present invention.
Claims (4)
1. The method for researching the water chemistry evolution in the multiple barrier system is characterized by comprising the following steps of:
S1, collecting rock and mineral samples related to a multiple barrier system, and determining related parameters of mineral composition of the rock and mineral samples;
S2, collecting underground water, and determining various chemical parameters of the initial underground water:
s2.1, storing the collected groundwater sample in an inert gas atmosphere;
S2.2, measuring the contents of carbonate ions and bicarbonate ions in the groundwater sample by a potentiometric titration method;
S2.3, obtaining the content of anions and cations in the groundwater sample through an ion chromatography and an atomic emission spectrometry, and measuring the dissolved oxygen content, the pH value and the Eh value of the water sample through a dissolved oxygen meter, a pH meter and an Eh meter;
S3, carrying out rock-soil material physical property parameter test research on the rock-mineral sample, and determining parameters related to saturation permeability coefficient, porosity and cation exchange capacity;
S4, carrying out a corrosion simulation experiment on the packaging container, and determining the average corrosion rate of the packaging container in the barrier;
s5, carrying out long-term numerical simulation research, wherein the specific steps are as follows:
s5.1, determining a reaction path and various reaction types of water-rock interaction in a multi-barrier system by using a comprehensive mineral composition, a groundwater chemical composition and a water-rock interaction reaction equation, reasonably simplifying reaction sites and reaction processes in a container corrosion process in a model, integrating a container and solidified wastes, and further considering that the porosity and initial pore water composition of the container are consistent with those of the solidified minerals;
Under the actual multiple barrier environment, using geochemistry simulation software, wherein the simulation Time is Time, dividing the whole system into a plurality of small units with the length of 0.1m on a one-dimensional level according to the sequence of an artificial barrier layer, the pore proportion and the seepage rate characteristic, each small unit represents a complete water-rock interaction system, establishing a numerical simulation model, and converting the initial mineral content corresponding to 1kg of pore water according to the porosity and the mineral density;
S5.2, completely and independently simulating water flow by using a random walking method, and determining the direction and speed of the water flow field, boundary conditions of inflow and outflow and diffusion coefficients and diffusion distances of components in the water to obtain a calculated water flow field;
s5.3, performing improved feature method simulation on the basis of the calculated water flow field;
S5.4, calculating the time required by the pore water flowing through the barrier according to the seepage rate of the rock and ore, and obtaining the evolution of the water chemistry environment in large scale time by setting the flushing times of the pore water.
2. The method for studying the chemical evolution of water in a multiple barrier system according to claim 1, wherein the specific steps of determining the parameters related to the mineral composition of the rock and mineral sample in the step S1 are as follows:
s1.1, crushing and grinding the collected rock-ore sample to prepare powder with the particle size of 200 meshes;
S1.2, identifying rock sample powder through X-ray diffraction, and determining rock type, mineral composition and content.
3. The method for studying the chemical evolution of water in a multiple barrier system according to claim 1, wherein the specific steps for determining the parameters related to the permeability coefficient, the porosity and the cation exchange capacity in the step S3 are as follows:
s3.1, carrying out saturation permeability coefficient test through a flexible wall permeameter, and calculating to obtain a saturation permeability coefficient;
S3.2, measuring the porosity of minerals;
s3.3, measuring the cation exchange content of minerals.
4. The method for researching the evolution of the water chemistry in the multiple barrier system according to claim 1, wherein the specific steps of simulating the corrosion test of the packaging container in the step S4 are as follows:
The 16MnR bare steel sheet is buried in a buried layer with a certain thickness for 4 years, the buried layer is continuously soaked by field groundwater during the period, sampling is carried out in different time periods, and the average corrosion rate of the steel sheet is calculated by adopting a weightlessness method.
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