CN109060642A - A kind of quick aging method of geological disposal Engineering Barrier Materials - Google Patents

A kind of quick aging method of geological disposal Engineering Barrier Materials Download PDF

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Publication number
CN109060642A
CN109060642A CN201810634414.8A CN201810634414A CN109060642A CN 109060642 A CN109060642 A CN 109060642A CN 201810634414 A CN201810634414 A CN 201810634414A CN 109060642 A CN109060642 A CN 109060642A
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barrier materials
aging
engineering barrier
irradiation
aging method
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刘伟
叶盾毅
杨仲田
梁栋
李洪辉
贾梅兰
赵帅维
毛亮
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China Institute for Radiation Protection
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China Institute for Radiation Protection
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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01NINVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N17/00Investigating resistance of materials to the weather, to corrosion, or to light

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Abstract

The invention belongs to technical field of nuclear radiation protection, are related to a kind of quick aging method of geological disposal Engineering Barrier Materials.The quick aging method includes the following steps: that (1) successively carries out simple γ radiation aging, simple heat ageing and irradiation-heated succession aging to the Engineering Barrier Materials;(2) it after the irradiation-heated succession aging, determines and tests sensibility characteristic index;(3) test result of the sensibility characteristic index is compared and analyzed, provide the relative extent of sensibility characteristic index deterioration described after three kinds of accelerated ageings act on, to provide reaction mechanism and establish kinetics equation, the deduction of conservative is carried out to the performance of the Engineering Barrier Materials on this basis.Using the quick aging method of geological disposal Engineering Barrier Materials of the invention, the accurate conclusion or too conservative conclusion of Engineering Barrier Materials property evolution can be provided under long time scale.

Description

A kind of quick aging method of geological disposal Engineering Barrier Materials
Technical field
The invention belongs to technical field of nuclear radiation protection, are related to a kind of accelerated ageing side of geological disposal Engineering Barrier Materials Method.
Background technique
High-level radioactive waste (HLW) has nucleic half-life period long (half-life period of part nucleic is hundreds of thousands year), releases Therefore the features such as heat is big, bio-toxicity is high is in the world at present deep geological disposal to its generally acknowledged disposal options, to reach To the purpose being isolated for a long time with the mankind.Deep geological disposal is based on multibarrier principle more and is designed, and wherein spentnuclear fuel/waste is solid Changing body itself is first barrier, and disposal container is second barrier, and buffering/backfilling material is third barrier, and disposes and be situated between The geological environment of matter (country rock) and surrounding is the 4th barrier.In above-mentioned four barrier, first three road barrier belongs to engineering barrier, It can make it suitable for specific condition by engineering design;And the 4th barrier is natural barrier, is mainly added by Site Selection With determination.
In addition, it is general again according to the position of barrier, function, by waste body effect, evolutionary process occurs wherein Deng disposal system being divided near field and far field, near field includes Engineering Barrier Materials and country rock disturbed belt.And for disposition For system near field, Engineering Barrier Materials will be for a long time by irradiation field, temperature field, flow of water field, stress field, chemical fields and micro- life The influence of the multi- scenarios methods such as object effect.Therefore, under many factors collective effect, the evolution of Engineering Barrier Materials long-term behaviour is ground One of the key problem being concerned about in matter disposition safety evaluation.
It but is essentially all at present approximate verifying extrapolation about the method for Engineering Barrier Materials long-term behaviour evolution research Method, i.e., in the approximate verifying for carrying out certain time (several months to several years) close at the temperature and other environmental conditions really disposed (main research is heat-water-power-chemistry (THMC) bench test and subterranean laboratory original place heat run), analysis presumption material Long-term behaviour.In general, this method is difficult to obtain the evolution mechanism and kinetics equation of material, therefore when can not establish long Between under scale when-temperature Evolvement;And if only going to infer under long time scale according to the property evolution under short-term time scale Property evolution, then it is concluded that confidence level is lower.Therefore, it is drilled to obtain Engineering Barrier Materials performance under long time scale The accurate conclusion or too conservative conclusion changed, need to establish new test method, quick aging method is one of them.
Summary of the invention
The object of the present invention is to provide a kind of quick aging method of geological disposal Engineering Barrier Materials, with can be when long Between the accurate conclusion or too conservative conclusion of Engineering Barrier Materials property evolution are provided under scale.
In order to achieve this, the present invention provides a kind of geological disposal Engineering Barrier Materials in the embodiment on basis Quick aging method, the quick aging method include the following steps:
(1) Engineering Barrier Materials are successively carried out with simple γ radiation aging, simple heat ageing and irradiation-heated succession Aging;
(2) it after the irradiation-heated succession aging, determines and tests sensibility characteristic index;
(3) test result of the sensibility characteristic index is compared and analyzed, provides three kinds of accelerated ageing effects The relative extent of sensibility characteristic index deterioration afterwards, to provide reaction mechanism and establish kinetics equation, in this base The deduction of conservative is carried out on plinth to the performance of the Engineering Barrier Materials.
The basic principle of quick aging method of the invention are as follows:
(1) service life of certain material under its use condition is predicted, since test simulation condition and test period etc. are more The limitation of aspect factor can not take full-scale condition to simulate under normal circumstances, and optimal method is using accelerated aging test;
(2) selectivity properties characteristic index is found, then determines radiation and heat effect to material according to these achievement datas The influence of performance is synergistic effect or superposition;
(3) it according to radiation and hot two factors on the relationship between the influence of accelerated aging test result, studies and grasps old Change reaction mechanism, establishes reaction kinetics equation, predict the service life of material;
(4) under the experimental condition of accelerated ageing, the reaction mechanism of material aging and it is anti-under true use condition Answer mechanism identical.
In a preferred embodiment, the present invention provides a kind of accelerated ageing side of geological disposal Engineering Barrier Materials Method, wherein in step (1), the simple γ radiation aging is in the period required by safety evaluation, with the engineering The practical cumulative maximum γ irradiation dose being subject to of barrier material is starting point, carries out irradiation using big cobalt source gamma-rays device and adds Speed.
In a kind of more preferred embodiment, the acceleration that the present invention provides a kind of geological disposal Engineering Barrier Materials is old Change method, wherein the time that the irradiation of big cobalt source gamma-rays device accelerates is 40 days to 3 months.
In a preferred embodiment, the present invention provides a kind of accelerated ageing side of geological disposal Engineering Barrier Materials Method, wherein in step (1), the simple heat ageing be according to the practical maximum temperature being heated of the Engineering Barrier Materials, The simulation maximum duration of the period in conjunction with required by safety evaluation and accelerated aging test determines according to Arrhnius law and accelerates Thermal aging temperature afterwards, and heat ageing is carried out within the determining accelerated ageing time.
In a kind of more preferred embodiment, the acceleration that the present invention provides a kind of geological disposal Engineering Barrier Materials is old Change method, in which:
The practical maximum temperature being heated of Engineering Barrier Materials is 80-100 DEG C;
Period required by safety evaluation is 1000-10000;
The simulation maximum duration of accelerated aging test is 1000-10000.
In a preferred embodiment, the present invention provides a kind of accelerated ageing side of geological disposal Engineering Barrier Materials Method, wherein in step (1), the irradiation-heated succession aging is that first γ is irradiated to cumulative maximum dosage, then with simple heat Heat ageing is carried out in the identical aging temperature and ageing time of effect.
In a preferred embodiment, the present invention provides a kind of accelerated ageing side of geological disposal Engineering Barrier Materials Method, wherein in step (2), the sensibility characteristic index includes shear strength, elasticity modulus, expansive force, expansion rate, swelling The dissolubility of Si in native mineral structure.
In a kind of more preferred embodiment, the acceleration that the present invention provides a kind of geological disposal Engineering Barrier Materials is old Change method, in which:
The shear strength and elasticity modulus is cut according to three axis described in " earthwork test rule " (SL237-1999) Cut experimental test acquisition;
The expansion rate is tested using consolidation apparatus according to method described in " earthwork test rule " (SL237-1999) It obtains;
The expansive force is tested using consolidation apparatus according to method described in " earthwork test rule " (SL237-1999) It obtains.
In a kind of more preferred embodiment, the acceleration that the present invention provides a kind of geological disposal Engineering Barrier Materials is old Change method, wherein the dissolubility of Si tests acquisition using the infusion method of following steps in the bentonite mineral structure:
1) Engineering Barrier Materials before and after a certain amount of accelerated ageing, the aqueous solution being placed in test tube together are taken respectively In;
2) test tube is put into timing daily in oscillation shaking table to vibrate, to the Engineering Barrier Materials and the aqueous solution Interaction a period of time (such as 50 days) is centrifugated afterwards, and clear liquid is taken to carry out Si4+Ion concentration test.
In a kind of more preferred embodiment, the acceleration that the present invention provides a kind of geological disposal Engineering Barrier Materials is old Change method, wherein the Si4+The test of ion concentration is closely red using icp ms or UV, visible light Outer spectrophotometer (spectrophotometry test is carried out according to GB/T8538-2008 " the natural mineral water method of inspection ").
The beneficial effects of the present invention are, using the quick aging method of geological disposal Engineering Barrier Materials of the invention, The accurate conclusion or too conservative conclusion of Engineering Barrier Materials property evolution can be provided under long time scale.
Quick aging method provided by the present invention can realize that Engineering Barrier Materials property evolution under long time scale is pre- Survey and life appraisal, or relatively too conservative, high reliablity prediction conclusion is provided, to improve the credible of safety evaluation conclusion Degree.
Sensibility characteristic index provided in the present invention can provide Engineering Barrier Materials performance change after accelerated aging Significant index, and provide the characterizing method of these indexs.Quick aging method and its sensibility characteristic index of the invention with Crossed used in existing practical operation/method currently in use compares, it has the advantage that
(1) (one section i.e. after the closing of disposition library can be simulated the Hlw Geological Repository hot stage in a relatively short period of time Time) centuries can pass through sensibility index and answer radiation and heat to γ radiation effects and heat effect suffered by thousands of years Relationship between effect;
(2) when can provide under specific long time scale-temperature evolution quantitative relationship, or can obtain it is too conservative, can The qualitative forecasting of letter is as a result, this helps to improve the confidence level of safety evaluation conclusion.
Detailed description of the invention
Fig. 1 is the flow chart of the quick aging method of illustrative geological disposal Engineering Barrier Materials of the invention.
Specific embodiment
The process of the quick aging method of illustrative geological disposal Engineering Barrier Materials of the invention is as shown in Figure 1, packet Include following steps.
(1) γ irradiation-heated succession aging
Engineering Barrier Materials are mainly carried out 3 kinds of agings by the step.
It is simple γ radiation aging first, i.e., in the period required by safety evaluation, to dispose library near field engineering barrier The practical cumulative maximum γ irradiation dose being subject to of material is starting point, carries out irradiation acceleration, spoke using big cobalt source gamma-rays device It is generally 40 days to 3 months according to the time.Simple γ radiation aging Effect study experimental condition and result are as shown in table 1 below.
The simple γ radiation aging Effect study experimental condition of table 1 and result
Followed by simple heat ageing, i.e., according to the disposition practical maximum temperature (such as 90 being subject to of library near field Engineering Barrier Materials DEG C), the simulation maximum duration (such as 1000) of the period in conjunction with required by safety evaluation (such as 1000) and accelerated aging test, The thermal aging temperature after accelerating is determined according to Arrhnius law, and carries out heat ageing within the determining accelerated ageing time.It is single Pure heat ageing Effect study experimental condition and result are as shown in table 2 below.
The simple heat ageing Effect study experimental condition of table 2 and result
It is finally irradiation-heated succession aging, i.e. elder generation γ is irradiated to cumulative maximum dosage, then identical as simple heat effect Aging temperature and ageing time in carry out heat ageing.Irradiation-heated succession aging action development test condition and result such as the following table 3 It is shown.
3 irradiation of table-heated succession aging action development test condition and result
(2) it determines and tests sensibility characteristic index
After irradiation/thermal acceleration aging, the index of sensibility mainly have soil mechanics performance indicator (shear strength, elasticity modulus, Expansive force, expansion rate) and chemical measurements of water (dissolubility of Si in bentonite mineral structure).
It, can be according to " earthwork test rule " for the shear strength and elasticity modulus in soil mechanics performance indicator (SL237-1999) test of triaxial shear test described in obtains.
For the expansive force in soil mechanics performance indicator, consolidation apparatus can be used according to " earthwork test rule " (SL237- 1999) method described in carries out test acquisition;Also lateral confinement swelling stress test device can be used to be tested, specific test side Method is referring to Chinese patent application 201610108913.4 (two-way swelling stress measurement tester) specification 11-23 row of page 5.
For the expansion rate in soil mechanics performance indicator, consolidation apparatus can be used according to " earthwork test rule " (SL237- 1999) test of method described in obtains.
For the dissolubility of Si in the bentonite mineral structure in chemical measurements of water, the main infusion method for using following steps Test obtains.
1) Engineering Barrier Materials before and after a certain amount of accelerated ageing, the aqueous solution being placed in test tube together are taken respectively In;
2) test tube is put into timing daily in oscillation shaking table to vibrate, to the Engineering Barrier Materials and the aqueous solution Interaction a period of time (such as 50 days) is centrifugated afterwards, and clear liquid is taken to carry out Si4+Ion concentration test.
Wherein Si4+The test of ion concentration is divided using icp ms or UV, visible light near-infrared Photometer (spectrophotometry test is carried out according to GB/T8538-2008 " the natural mineral water method of inspection ").
(3) assessment that irradiation-heated succession accelerated ageing influences Engineering Barrier Materials performance
The result that sensibility characteristic index is tested after acting on three kinds of accelerated ageings compares and analyzes, and provides three kinds of acceleration The relative extent that sensibility index deteriorates after aging action, thus provide reaction mechanism and establish kinetics equation, it is basic herein On the deduction of conservative is carried out to the performances of Engineering Barrier Materials.
According to the method for above-mentioned example, carry out Gaomiaozi bentonite (production of Inner Mongol Xinghe County) accelerated ageing research, The result shows that:
(1) tailored radiation aging, simple heat ageing and radiation-heated succession aging all cause the deliquescent increasing of bentonite Si Add, and increases with the increase of accumulation radioactive dose, thermal aging temperature and thermal aging time;Tailored radiation aging cumulative maximum The dissolubility of radioactive dose sample Si increases 8.4% than sample before aging, simple heat ageing maximum temperature maximum duration aging The dissolubility of sample Si increases 40.8% than sample before aging, radiation-heated succession aging maximum temperature maximum duration aging sample The dissolubility of product Si increases 57.7% than sample before aging;
(2) three kinds of aging actions cause the reduction of Gaomiaozi bentonite swelliong power, tailored radiation aged samples it is swollen Expansive force lowers with the increase of accumulation radioactive dose, its expansive force is reduced than sample before aging under cumulative maximum radioactive dose 55.0%;The expansive force of simple heat ageing sample is reduced with the increase of aging temperature, and minimum and highest aging temperature is most Its expansive force is than having respectively reduced 41.9% and 60.5% before aging under long ageing time;Radiation-heated succession aged samples are swollen Expansive force increases with the increase of aging temperature, and minimum and highest aging temperature its expansive force under longest ageing time compares aging Before respectively reduced 61.5% and 39.5%.
(3) under radiation/heat effect, the performance of Gaomiaozi bentonite is by serious deterioration after 1000.Bentonite structure Si Dissolubility greatly increase, swelliong power is very low, so after 1000 its chemical buffer ability and absorption nucleic ability will be very Weak, water conductivity function will increase.Namely after 1000, function (mechanics of the Gaomiaozi bentonite in high-level waste geology treatment Support function, chemical buffer function, retardance nucleic function and water stop function are incited somebody to action) it will greatly be weakened.
Obviously, various changes and modifications can be made to the invention without departing from essence of the invention by those skilled in the art Mind and range.If in this way, belonging to the model of the claims in the present invention and its equivalent technology to these modifications and changes of the present invention Within enclosing, then the present invention is also intended to include these modifications and variations.Above-described embodiment or embodiment are only to the present invention For example, the present invention can also be implemented with other ad hoc fashions or other particular form, without departing from of the invention Main idea or substantive characteristics.Therefore, the embodiment of description is regarded as illustrative and non-limiting in any way.This The range of invention should be illustrated that any variation equivalent with the intention and range of claim also should include by appended claims In the scope of the present invention.

Claims (10)

1. a kind of quick aging method of geological disposal Engineering Barrier Materials, which is characterized in that the quick aging method packet Include following steps:
(1) it is old that the Engineering Barrier Materials are successively carried out with simple γ radiation aging, simple heat ageing and irradiation-heated succession Change;
(2) it after the irradiation-heated succession aging, determines and tests sensibility characteristic index;
(3) test result of the sensibility characteristic index is compared and analyzed, provides institute after three kinds of accelerated ageing effects The relative extent for the sensibility characteristic index deterioration stated, to provide reaction mechanism and establish kinetics equation, on this basis The deduction of conservative is carried out to the performance of the Engineering Barrier Materials.
2. quick aging method according to claim 1, it is characterised in that: in step (1), the simple γ irradiation is old Change is in the period required by safety evaluation, with the practical cumulative maximum γ irradiation dose being subject to of the Engineering Barrier Materials For starting point, irradiation acceleration is carried out using big cobalt source gamma-rays device.
3. quick aging method according to claim 2, it is characterised in that: big cobalt source gamma-rays device irradiation accelerate when Between be 40 days to 3 months.
4. quick aging method according to claim 1, it is characterised in that: in step (1), the simple heat ageing is According to the practical maximum temperature being heated of the Engineering Barrier Materials, the period in conjunction with required by safety evaluation and accelerated ageing examination The simulation maximum duration tested determines the thermal aging temperature after accelerating according to Arrhnius law, and in determining accelerated ageing Interior carry out heat ageing.
5. quick aging method according to claim 4, it is characterised in that:
The practical maximum temperature being heated of Engineering Barrier Materials is 80-100 DEG C;
Period required by safety evaluation is 1000-10000;
The simulation maximum duration of accelerated aging test is 1000-10000.
6. quick aging method according to claim 1, it is characterised in that: in step (1), the irradiation-heated succession Aging is that first γ is irradiated to cumulative maximum dosage, is then carried out in aging temperature identical with simple heat effect and ageing time Heat ageing.
7. quick aging method according to claim 1, it is characterised in that: in step (2), the sensibility characterization refers to Dissolubility of the mark including Si in shear strength, elasticity modulus, expansive force, expansion rate, bentonite mineral structure.
8. quick aging method according to claim 7, it is characterised in that:
The shear strength and elasticity modulus is tested according to triaxial shear test described in SL237-1999 and is obtained;
The expansion rate is tested according to method described in SL237-1999 using consolidation apparatus and is obtained;
The expansive force is tested according to method described in SL237-1999 using consolidation apparatus and is obtained.
9. quick aging method according to claim 7, which is characterized in that Si's is molten in the bentonite mineral structure Solution property is tested using the infusion method of following steps and is obtained:
1) Engineering Barrier Materials before and after a certain amount of accelerated ageing are taken respectively, are placed in the aqueous solution in test tube together;
2) test tube timing daily in oscillation shaking table is put into vibrate, it is mutual to the Engineering Barrier Materials and the aqueous solution It is centrifugated after effect a period of time, clear liquid is taken to carry out Si4+Ion concentration test.
10. quick aging method according to claim 9, it is characterised in that: the Si4+The test of ion concentration utilizes Icp ms or UV, visible light near infrared spectrometer.
CN201810634414.8A 2018-06-20 2018-06-20 A kind of quick aging method of geological disposal Engineering Barrier Materials Pending CN109060642A (en)

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CN105043964A (en) * 2015-07-16 2015-11-11 哈尔滨工业大学 Test apparatus for ultraviolet aging acceleration of asphalt-based materials

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102539310A (en) * 2011-12-15 2012-07-04 广东工业大学 Method for atmospheric exposure test for photovoltaic cable
CN203941086U (en) * 2014-05-19 2014-11-12 国核电站运行服务技术有限公司 A kind of multifactor coupling cable accelerated deterioration system
CN105043964A (en) * 2015-07-16 2015-11-11 哈尔滨工业大学 Test apparatus for ultraviolet aging acceleration of asphalt-based materials

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