Grantová agentura České republiky. Grantová přihláška standardního projektu

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Grantová agentura České republiky

Část A

Grantová přihláška standardního projektu Datum podání: 31.03.2005

Číslo podoboru(ů) 104, 205

Registrační číslo: 104/06/1583

UCHAZEČ a NAVRHOVATEL Uchazeč: Ústav jaderného výzkumu Řež, a.s.

IČO: 46356088

Sídlo:

Husinec - Řež, č.p. 130, Řež, 25068

Navrhovatel:

Ing. Štefan Palágyi, DrSc.

Pracoviště navrhovatele:

Ústav jaderného výzkumu Řež, a.s., Husinec-Řež, č.p. 130

Rodné číslo: 391219072

Telefon: +420 266 172 073

Fax: +420 266 172 086

E-mail: [email protected]

Název projektu česky: Vertikální a horizontální migrace transuranů a dlouho žijících štěpných produktů v půdách a sedimentech z okolí úložišť radioaktivních odpadů Název projektu anglicky: Vertical and horizontal migration of transuranics and long-lived fission products in soils and sediments in the environment of radioactive waste repos Klíčová slova česky: migrace, transurany, štěpné produkty, modelování, půda, sedimenty, úložiště Klíč. slova anglicky: migration, tranuranics, fission products, modeling, soil, sediments, repository Datum podání *): Datum zahájení: 31/03/2005 01/01/2006 Doba řešení (roky): 3 DL,Jaderné odpady, radioaktivní znečištění a kontrola Zařazení do číselníku CEP: DK,Kontaminace a dekontaminace půdy včetně pesticidů DJ,Znečištění a kontrola vody

20050404105055.1.4.0.1

Odborní spolupracovníci, kteří se budou podílet na řešení výše uvedeného projektu. (V seznamu se neuvádí navrhovatel a spolunavrhovatelé.) Jméno a příjmení Aleš Laciok Václava Havlová r. Buňatová Jiří Landa

Instituce Ústav jaderného výzkumu Řež a.s. Ústav jaderného výzkumu Řež a.s. Ústav jaderného výzkumu Řež a.s.

Uchazeč a navrhovatel svými podpisy na grantové přihlášce stvrzují, že: - se před podpisem grantové přihlášky seznámili s obsahem zadávací dokumentace a s pravidly Grantového systému GA ČR 2005 a zavazují se dodržovat jejich ustanovení; - všechny údaje uvedené v grantové přihlášce jsou pravdivé, úplné a nezkreslené a grantová přihláška byla vypracována v souladu se zadávací dokumentací a s pravidly Grantového systému GA ČR 2005; - všichni spolunavrhovatelé a spolupracovníci uvedení v grantové přihlášce byli seznámeni s věcným obsahem grantové přihlášky, jakož i s finančními požadavky uvedenými v grantové přihlášce a dále i s obsahem zadávací dokumentace a s Pravidly Grantového systému GA ČR 2005; - před podáním grantové přihlášky zajistili souhlas výše uvedených osob s účastí na řešení grantového projektu uvedeného v grantové přihlášce; - souhlasí, aby údaje uvedené v této grantové přihlášce byly použity pro vnitřní informační systém GA ČR a dále souhlasí s uveřejněním údajů v rozsahu stanoveném v zadávací dokumentaci.

.................................................. Podpis navrhovatele (Palágyi)

.................................................................................................... Podpis a razítko uchazeče 1) (Ing. František Pazdera, CSc, generální ředitel)

.................................................. Datum

1) U uchazeče právnické osoby nebo organizační složky se uvádí rovněž jméno, příjmení a funkci jednající osoby (jednajících osob). Jednající osobou u uchazeče - právnické osoby může být pouze: - statutární orgán, nebo - člen statutárního orgánu oprávněný za uchazeče jednat, nebo - prokurista. Jednající osobou u uchazeče - organizační složky může být pouze: - vedoucí této organizační složky.

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Část Abstrakt

Navrhovatel: Registrační číslo: Ing. Štefan Palágyi, DrSc. 104/06/1583 Název projektu: Vertikální a horizontální migrace transuranů a dlouho žijících štěpných produktů v půdách a sedimentech z okolí úložišť radioaktivních odpadů

Podstata navrhovaného projektu (max. 15 řádek) - česky

Projekt se zaměřuje na studium migrace radionuklidů s dlouhým poločasem přeměny - transuranů o vysoké radiotoxitě (241Am) a některých štěpných produktů (129I a 135Cs). Projekt se zabývá experimentální hodnocením vzestupných vertikálních a horizontálních migračních procesů výše uvedených radionuklidů v saturovaném prostředí půd a sedimentů a na jejich modelování. V rámci projektu jsou navrhovány výzkumné práce v několika nových směrech, např. na laboratorní migrační experimenty v různém uspořádání se současným hodnocením kinetických a termodynamických aspektů procesů s cílem jejich kvantifikace. Pro tyto účely budou porovnány dvě třídy modelů (advektivně-disperzní a kompartmentový) z hlediska jejich vhodnosti pro dané účely a parametrické náročnosti. Bude provedena korelace hlavních parametrů půd a sedimentů s migračními rychlostmi a bude ověřena predikativní schopnost modelů pro různé podmínky. Pro migrační experimenty budou využity půdy a sedimenty z reálných lokalit. Očekávané výsledky použitelné v praxi spočívají v předpovědi možného pohybu radionuklidů z úložiště do okolního prostředí. Sestavené transportní modely pak mohou být použity jako součást hodnocení radiační bezpečnosti úložiště. Podstata navrhovaného projektu (max. 15 řádek) - anglicky

The project is aimed at the migration of long-lived radionuclides - transuranics of with high radiotoxicity (241Am) and some fission products (129I and 135Cs). The project is dealing with the experimental assessment of upward vertical and horizontal migration processes of the mentioned radionuclides in saturated conditions of soils and sediments and their modelling. Research activities in innovative ways are proposed as a part of this project, i.e., laboratory migration experiments of various designs with simultaneous evaluation of kinetic and thermodynamic aspects of processes with the aim of their quantification. Two classes of models (advectiondispersion and compartment) will be evaluated for this purpose from the point of view of their suitability and parametrical demand. The correlation of main parameters of soils and sediments with migration rates will be carried out and predictability of established models for different conditions will be assessed. Real soil and sediment samples will be used. The expected results applicable in the practice consist in the prediction of the possible radionuclide movement from the repository to the environment. The composed transport models would be used as a part of radiation safety analysis of radioactive waste repository.

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Grantová agentura České republiky Uchazeč:

Ústav jaderného výzkumu Řež, a.s. - Ústav jaderného výzkumu Řež, a.s. Ing. Štefan Palágyi, DrSc.

Navrhovatel:

Část B-sumy Registrační číslo:

104/06/1583

1) Celkové předpokládané náklady na řešení projektu ze všech zdrojů financování na jednotlivé roky jeho řešení (finanční údaje se uvádějí jako celočíselné hodnoty v tis. Kč) 1.rok Náklady ze všech zdrojů financování

2.rok

3.rok

2034

2034

Celkem

2034

6102

2) Celkové předpokládané náklady na řešení projektu z jednotlivých zdrojů za celou dobu jeho řešení (finanční údaje se uvádějí jako celočíselné hodnoty v tis. Kč) Jednotlivé zdroje finančních prostředků na řešení projektu

tis. Kč

Celkové grantové prostředky požadované z GA ČR

3051

Ostatní veřejné prostředky nepatřící do státního rozpočtu (např. z rozpočtů krajů nebo obcí)

0

Ostatní neveřejné prostředky (např. vlastní prostředky uchazeče u soukromých subjektů)

3051

Celkem

6102

3) Celkové náklady na řešení projektu požadované od GA ČR (finanční údaje se uvádějí jako celočíselné hodnoty v tis. Kč) 1.rok Věcné prostředky celkem

2.rok

3.rok

530

530

530

0

0

0

Mzdové prostředky celkem

487

487

487

Celkem na řešení projektu

1017

1017

1017

Investiční prostředky celkem

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Část B-rozpis

Finanční prostředky požadované od GA ČR pro uchazeče (finanční údaje se uvádějí jako celočíselné hodnoty v tis. Kč) Uchazeč: Navrhovatel:


Registrační číslo:

104/06/1583

1.rok

2.rok

3.rok

Věcné prostředky Provozní náklady 1)

110

110

110

Služby 2)

130

130

130

Doplňkové (režijní) náklady 3)

80

80

80

Cestovní náklady 4)

30

30

30

Sociální a zdravotní pojištění a FKSP 5)

180

180

180

Věcné prostředky celkem

530

530

530

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

0

4

367

367

367

0

0

0

0

120

120

120

Odměny technického personálu 11)

0

0

0

Ostatní osobní náklady (celkem) 12)

0

0

0

487

487

487

1017

1017

1017

Investiční prostředky na hmotný a nehmotný majetek 6)

Celková cena 7)

Investiční prostředky celkem Mzdové náklady (detaily jsou uvedeny v části B-mzdy) Mzdy navrhovatele a spolupracovníků 8) Odměny navrhovatele a spolupracovníků 9)

Počet

Mzdy technického personálu 10)

Mzdové prostředky celkem Celkové prostředky z GA ČR 1) Část IV oddíl 7 odst. 7.1 písm. a) Grantového systému GA ČR 2005 2) Část IV oddíl 7 odst. 7.1 písm. b) Grantového systému GA ČR 2005 3) Část IV oddíl 7 odst. 7.1 písm. f) Grantového systému GA ČR 2005 4) Část IV oddíl 7 odst. 7.1 písm. c) Grantového systému GA ČR 2005 5) Část IV oddíl 7 odst. 7.1 písm. d) a e) Grantového systému GA ČR 2005 6) Část IV oddíl 9 Grantového systému GA ČR 2005 . Každou položku uveďte na zvláštní řádek. 7) Uvádí se celková pořizovací cena. 8) Část IV oddíl 8 odst. 8.3 písm. a) a b) Grantového systému GA ČR 2005 9) Část IV oddíl 8 odst. 8.3 písm. c) Grantového systému GA ČR 2005 10) Část IV oddíl 8 odst. 8.3 písm. a) a b) Grantového systému GA ČR 2005 11) Část IV oddíl 8 odst. 8.3 písm. c) Grantového systému GA ČR 2005 12) Část IV oddíl 8 odst. 8.7 Grantového systému GA ČR 2005

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Příloha k B-rozpis

Zdůvodnění a rozpis finančních prostředků Uchazeč: Navrhovatel:



104/06/1583

Příloha k B-rozpis je nedílnou součástí grantové přihlášky a údaje v ní se musí shodovat s údaji v příslušné části B-rozpis. V této části musí být každý požadavek jasně specifikován, zdůvodněn a uvedeny informace o konkrétním využití požadované účelové podpory v souladu s ustanovením části V oddíl 11 Grantového systému GA ČR 2005 . Údaje v části Příloha k B-rozpis se uvádějí pro první rok řešení, pro další léta se údaje upřesní v příslušné dílčí zprávě.

Provozní náklady: Běžný provozní materiál potřebný v chemické a radiochemické laboratoři. Nákup radionuklidů a pořízení materiálu pro sestavení zařízení pro výzkum migrace (kolony atd.). Služby: Tvoří část nákladů na dozimetrii, likvidaci RAO, připojení k počítačové síti, služby knihovny, provoz laboratoře. Významnou část budou tvořit chemické analýzy. Cestovné: Účast na konferenci ARCEBS 06 nebo ERA 10. Mzdové náklady Náklady na mzdy pro navrhovatele a jeho spolupracovníky odpovídají pracovním kapacitám uvedených v tabulce Část B - mzdy

20050404105055.1.4.0.1


Část B-mzdy

Mzdové náklady pro uchazeče pro 1. rok řešení (finanční údaje se uvádějí jako celočíselné hodnoty v tis. Kč) Uchazeč:


Navrhovatel:


104/06/1583

Náklady na mzdy nebo odměny odborných zaměstnanců: Navrhovatel a spolupracovníci: Jméno Štefan Aleš Václava Jiří

Příjmení Palágyi Laciok Havlová r. Buňatová Landa

Požadované prostředky od GA Pracovní ČR kapacita na řešení projektu Odměna za rok Roční mzda 2) 1) 3) 60 180 0 12 50 0 25 65 0 28 72 0

Mzdy a odměny technického a administrativního personálu Požadované prostředky od GA ČR Roční mzda 2) Odměna za rok 3) Celkový počet technických a administrativních zaměstnanců:

2

120

0

Ostatní osobní náklady (dohodu o provedení práce nebo dohody o pracovní činnosti) - uveďte typ pracovní činnosti, uvádějí se rovněž jména studentů přijatých na dohody: 4) Typ činnosti

Celkem požadované

1) Uvádí se v procentech odpovídajících rozsahu úvazku zaměstnanců na řešení grantového projektu. 2) Uvádí se celková výše hrubé mzdy nebo hrubého platu, resp. jejich poměrná část požadovaná z prostředků GA ČR na první rok řešení grantového projektu. Nevyplňuje se, pokud je požadována odměna. 3) Uvádí se odměna (tj.zvýšení pohyblivé částky mzdy nebo platu) požadovaná z prostředků GA ČR. 4) Pokud se budou práce na projektu účastnit studenti, uvádí se jméno a příjmení s označením „(s)“. V případě, že studenti budou odměňování z položky OON uvádí se tyto údaje do pole "typ pracovní činnosti".

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Část E

Finanční podpory, které navrhovatel získal z jiných zdrojů Neúplnost údajů bude mít za následek vyřazení ze soutěže Uchazeč: Navrhovatel:



104/06/1583

Projekty v současné době podporované Poskytovatel MPO ČR Doba řešení od-do (roky) 01/05/2004 31/12/2008

Reg. č. a zkrácený název projektu 1H-PK/25 - Výzkum bariér úložišť radioaktivních odpadů Pracovní kapacita 2) 2%

Řešitelské pracoviště Ústav jaderného výzkumu Řež a.s.

1) Jde o výši podpory na celou dobu řešení projektu v tisících Kč. 2) Rozsah úvazku na řešení jednotlivých projektů (v %) a to i když podpora nezahrnuje mzdy.

Podpora 1) Kč 17575

Grantová agentura České republiky - Část C Zdůvodnění návrhu Jméno navrhovatele: Štefan Palágyi Název projektu: Vertikální a horizontální migrace transuranů a dlouho žijících štěpných produktů v půdách a sedimentech z okolí úložišť radioaktivních odpadů

a) Literature survey of the project and identification of problems to be solved The evaluation of the radiation dose to the public from the ingested radionuclides through food chain and the transport of these radionuclides in soil system are extensively studied. The analysis of critical transport pathways and mechanisms of the release of radionuclides from the repository of radioactive waste into the repository surroundings are an essential part of the risk & safety analyses and performance assessment (PA) of any disposal facility, e.g. in the form of environmental impact assessment (EIA). Environmental impact assessment is a basic element of each initial, preliminary and preoperational safety report, required by law, for the issue of a respective license for siting, construction and commissioning of a repository [1,2]. The important role of the soil or sediments in radioecology is caused by the fact that these sediments may function as a sink or as a temporary reservoir for radionuclides. The migration of radionuclides in soil system considerably influences the contamination of groundwater as a source of drinking water [3-5]. Migration processes in soil are rather complex and are strongly influenced by interactions with their environment. They involve different mechanisms (advection, diffusion, movement driven by the capillary forces and various interaction mechanisms like adsorption, ion-exchange, complexation, colloid formation and their interactions, dissolution, precipitation and crystallization) and are dependent on various factors (speciation of radionuclides, soil properties, hydro-geochemical and microclimatic conditions, or microbiological activity, etc.). They proceed in many directions, simultaneously vertically and horizontally. In the comparison with water, the migration of radionuclides in soil profiles is rather slow, therefore, they represent a source of contamination. It is well-known that the vertical and horizontal distributions of radionuclides in soil is uneven and time dependent [6-8]. For the radionuclide migration different mathematical (analytical, numerical) models, some of them implemented also into computer software, have been worked out including also the soil-vegetation pathway [see 9,10 and Refs. therein]. Models for the description of the vertical migration in soils can roughly be divided into two groups [see 9,11 and Refs. therein]. The firsts one, similarly as in the studies of contaminants transport processes, is based on the advection-dispersion (diffusion) approach [e.g., 12-17], the other one is based on a simple multilayer compartment (box) principle [e.g., 10,18-21]. The advection-dispersion approach of the contaminant transport through porous solid media is widely used in the PA of nuclear installations. The column experiments are usually modeled using the well-known onedimensional advection-dispersion equation (ADE), assuming that the initial concentration of a contaminant in the liquid phase is constant during the experiment on the top of the column (Co): R . ∂C/∂t = Dd . ∂2C/∂x2 – vp . ∂C/∂x – λ . R . C,

(1)

1

where: C [ML-3] – contaminant concentration (radionuclide activity) in the liquid phase, t [T] – time, Dd [L2T] coefficient of hydrodynamic dispersion, R [-] - retardation coefficient, vp [LT-1] - mean pore-water velocity, x [L] – is the distance along the column and λ [T-1] - radioactive decay constant. Depending on the ratio of the duration of experiments and the half-lives of applied radionuclides, the third term in Eq. 1 can be neglected. Then we can obtain the integrated form of Eq. 1 as CR = C/Co = 0,5 . erfc [(R – nVp) / 2 (R . nVp /Pe)0,5],

(2)

which is the so-called breakthrough curve (BTC) equation. The nVp is the number of pore volumes Vp and the Pe (= vp.L/Dd) is the Peclet number of the column length of L. This curve is valid for continuous input of a radionuclide. If a discontinuous, so-called pulse input is considered, Eq. (2) gains the following form: CR = C/Co = ( Lp/L). exp[-(R - nVp)2/(4R . nVp/Pe)] / (4π . R . nVp/Pe)0,5,

(3)

where Lp is the pulse length and the meaning of other symbols are the same as in Eq. 2. From the experimentally constructed BTC, i.e., the function of C/Co = f (nVp), the values of both main transport parameters of R and Dd can be calculated. As the distribution coefficient (Kd) is related to R through porosity (θ) and bulk density (ρ) of the porous solid medium: Kd = θ . (R-1). ρ,

(4)

its value can also be easily calculated from e.g., experimentally determined values of the mentioned parameters of the solid phase. Of course, the character of Kd is dependent on the character of the interaction of a contaminant on the solid-liquid interface and/or bulk mass of these (mechanism and kinetics of sorption-desorption reactions, acido-basic reactions, dissolution-precipitation, ion-exchange or complexation, cell microbial syntheses). Recently, pilot studies on the sorption of UO22+ (as 10-4 M nitrate solution in demineralised water) and several types of sand of various origins have been carried out in our laboratory [22]. For desorption 0,01M Na2CO3 solution was used. The results obtained with porous granular material with the simplest phase systems sea sand (98,2% of quartz and 1,8% of cristobalite), with grain (particle) size distribution of 0,50 mm - 0,125 mm up to of 96,7%, are presented in Fig. 1. Using the respective breakthrough curves from this figure and Eq. 2 it can be easy calculated that the value of R for sorption is about 2 and for desorption is somewhat higher than 1 (in this figure nVp = nPV).

1,0 0,9 0,8 0,7

CR

0,6 0,5 0,4 0,3 0,2 0,1 0,0 0

1

2

3

4

nPV

Fig. 1. Breakthrough curves of U(VI) on a 50 cm3 column of the sea sand (■ – sorption and □ – desorption)

2

In the compartment type of model, an exponential decrease of concentration (activity) of radionuclides with the depth of the vertical profile is supposed, frequently. It makes it possible to set, according to the number of compartments considered in the soil profile, a series of differential equations of the first order with a constant migration rate coefficients in respective compartments, which can easily be solved analytically [9,10]. For the sake of simplicity, it is supposed that the soil properties within a given layer are the same or very similar, and, therefore, the radionuclide migration rates are also constant and they change only when they pass through the compartments. It is admitted that in the various compartments the rate constants may be different, but in each separate compartment they are supposed to be uniform in relation with the migration rate. Under these conditions, we have devised a simple dynamic multilayer compartment model, which is illustrated in Fig. 2 [10]. Each layer has the same size, i.e. their profiles are equal (hi = const). In consequence of the irrigation, only downward migration of radionuclides is considered and the potential back-flow of water is neglected. Ao (e.g., in %) denote the radionuclide activity (concentration), deposited uniformly on the soil surface before the start of the migration at time t=0. Ai is the activity of the ith soil layer (compartment) at the end of the elapsed migration time (t), respectively, where i = 1, 2, 3,…, n, so that n

∑

Ai = A1 + A2 + A3 + … + An-2 + An-1 + An = Ao.

(5)

i =1

Ao, t=0 →

↓ A1

A3

k1

↓

A2

t

↓

k2

↓

k3

↓ Ai-1

↓

ki-1

Ai

↓

ki

Ai+1

↓

ki+1

↓ An-2

↓

kn-2

An-1

↓

kn-1

An

↓

kn

↓

Fig.2. Schematic diagram of the vertical soil profile with a downward water flow (vertical arrows; the horizontal arrow represents a uniformly spreading of radionuclides on the soil surface; for symbols see the explanation in the text) If the exponential decrease is supposed of the radionuclide activity in each layer due to its removal from the compartment to the next one, the change of activity Ai to Ai+1,t can be described by equation: Ai = [Ao - A1 - A2 - A3 - … - Ai-1] . exp (-ki.t),

(6)

or rearranged for An = Ai: An = [Ao.exp(-kn.t) ].{[1– exp(-k1.t)].[1– exp(k2.t)]. … .[1– exp(-kn-2.t)].[1– exp(-kn-1.t)]},

(7)

3

where kn = ki is the rate constant of the vertical migration of a radionuclide in the ith = nth soil compartment. The kn can be expressed by the equation: n-1

kn = {ln [(Ao - A1 - A2 - … - An-1) / An]} / t = {ln [(Ao -

∑ A ) /A ]} / t . i

(8)

n

i=1

Similarly as the relaxation depth in relation to the activity distribution in the vertical soil profile [9], the relaxation time of the migration of a radionuclide in the layer i (ti) can be introduced, which is a reciprocal value of the migration rate constant (ti = 1/ki ). The ti is equal to the time during which the activity or concentration of a radionuclide decreases to e-1, i.e., to 36,79%, of the initial activity in this layer. Thus, from the soil layer hi the vertical migration rate (vi) in this soil layer can be calculated (vi = hi / ti = hi). The total relaxation time of the vertical migration of a radionuclide (tT) is the sum of the individual ti (tT = n n ∑ ti = ∑ (1/ki) i=1 i=1

= 1/kT), which means that the total vertical migration rate constant of a radionuclide in a given soil

horizon hT (hT is the sum of hi) can be calculated by the harmonic sum of the individual vertical migration rate constants in the segmented soil profiles. Subsequently, as follows from Eqs (7) and (8), the vertical migration rate of a radionuclide in a given depth horizon is vT = hT . kT = hT / tT . The derived model was verified successfully in the studies of vertical migration of

(9) 85

Sr,

137

Cs and

131

I in

various arable and undisturbed soil profiles from six Czech and Slovak localities in the environment of two nuclear power plants (NPP Dukovany and NPP Bohunice, respectively). Using the model, values of migration rate constants, migration rates and relaxation times were calculated both in individual layers and in the total bulk horizons of the studied soils. A modification of the model (simple exponential model [8]), it is also possible to calculate the relaxation depth and retardation factor (R) of the radionuclides in these soils under these dynamic conditions. The results presented here have confirmed the validity of the compartment model used to the quantification of the downward vertical migration of radionuclides in arable and undisturbed soil profiles. The compartment model used here, based on the exponential removal principle of radionuclides in individual soil profile segments, allows us to calculate simply the necessary migration parameters in soils, which can be used to elucidate the radionuclide transport processes in various food-chains, where soils are involved. The migration rate constants can be implemented in relations used to evaluate the extent of resuspension of radionuclides from ground surface following their deposition. The method can also be utilized in the characterization of the role of the natural barriers of near-surface repositories of radioactive waste. The drawback of this method lies in the fact that the rate constants are time dependent, which makes their use for not investigated time period somewhat difficult. Both models are aimed at the prediction of the concentration (activity) of the radionuclides at a distance, which the radionuclide could travel in the investigated time under specified circumstances. In the proposed project, we would like to further extend earlier works (focused exclusively on downward vertical migration mainly of Sr and Cs) on the study of migration radionuclides long-lived fission products and transuranics) and their modeling in several aspects, as follows: -

determination of some most important transport parameters, including hydraulic conductivity of the tested porous granular materials,

4

-

experimental investigation of migration of selected transuranics and long-lived fission product in downward/upward vertical and horizontal columns (filled with undisturbed cores and /or treated materials, e.g., granulometric fractions), under near natural hydraulic and hydrogeochemical conditions,

-

construction of experimental breakthrough curves obtained by continuous and pulse inputs of radionuclides and development of their new evaluation method based on ADE approach,

-

determination of rate constants and rates of migration of radionuclides in columns according to multicompartment model of migration,

-

construction of

an apparatus of medium (dm) scale for preliminary migration studies of soluble

radionuclides in order to start development of 2-D ADE model, -

set up and parameterization of both 1-D advection-dispersion model and multi-compartment model,

-

comparison of the column breakthrough data with migration rate constants in vertical and horizontal direction and with batch experimental data,

-

quantification of kinetic and thermodynamic aspects of the main transport process, including batch experiments,

-

correlation of major soil/sediment parameters with migration rates and geochemical speciation-solubility modeling,

-

comparative analysis of ADE and compartment models, verification of the ability of models to predict migration under different conditions.

b) Target of the proposed project and time schedule The project is dealing with long-lived radionuclides with potential high radiological consequences to human health and environment. This includes the long half-life and high radiotoxicity transuranics (in particular Np, Pu, Am, etc.) and some long-lived fission products (such as

135

Cs,

129

I and 99Tc). These radionuclides are important

critical nuclides mainly for deep geological disposal and represent a very different geochemical behaviour. Iodine is very mobile element migrating in the environment in various anionic forms usually without significant sorption; organic matter and microbial process may affect the redox reaction in soil. Cesium is medium to strongly sorbing element not forming any important complexes with ligands in the environment and usually interacting with soil surfaces via ion exchange. Americium is strongly sorbing redox sensitive element; strong complexation with humic substances is also reported – usually hydroxides and carbonates are solubility-limiting phases – migration of americium could be facilitated by colloids through its mobilization with them. The project is aimed at the experimental quantification and mathematical modeling of upward vertical and horizontal migration processes of radionuclides in the saturated soils and sediments. The issues described in the preceding subchapter will be investigated in the project. Time schedule and supposed results of the project: 2006: Modification of currently used and construction of new apparatus for the investigation of vertical migration in the selected materials. Detailed mineralogical, hydraulic and chemical characterization of studied materials (soil and sediment samples). Study of the migration of radionuclides representing the transuranics and mobile long-lived fission products (mainly

241

Am,

135

Cs and

129

I). Obtaining relevant data for modeling the upward

vertical migration of selected radionuclides in the soils and sediments. Batch experimental studies.

5

2007: Modification of currently used medium-scale migration apparatus and construction of new columns for the study of horizontal migration of selected radionuclides in the selected soils and sediments. Investigation of the radionuclide migration under horizontal conditions. Obtaining relevant data and modeling of horizontal migration of selected radionuclides in the studied materials. Performance of equilibrium batch experiments. 2008: Evaluation of the data acquired in the study and mathematical modeling of the 1-D vertical and horizontal migration of selected radionuclides in the investigated materials. Verification and validation of the onedimensional model in both directions. Correlation analysis for the assessment of the effect of major components of soils and sediments on the migration rate of studied radionuclides. Comparison of the results obtained with the advection-dispersion model (ADE) with multi-compartment model. Publishing all results of this project in a Technical Report and the relevant results in a well-known scientific international journal. c) Concept and methods The soil and sediment samples will be collected from the environment of the selected sites of radioactive waste repositories. The selected transuranic will be

Am (principal decay mode α of 5,6 MeV energy, with a

241

half-life of 433 y); this radionucilde can be detected via 60 keV γ-ray energy by a conventional NaI/Tl scintillaton detector. The selected long-term half-life fission product radionuclide will be 129I (principal decay mode β¯ of 0,15 MeV energy, with a half life of 1,57.107 y) and 135Cs (principal decay mode β¯ of 0,21 MeV energy, with a halflife of 2,95.106 y. For the sake of easy and simultaneous detection with

241

Am,

125

I (decay by EC accompanied

with emission of 27 keV X-ray and 35 keV γ-ray energies, with a half-life of 60,3 days) and 134Cs (decay mode β¯ of 0,658 MeV energy, accompanied by 605 keV gamma, with a half-life of 2,06 y) will be used instead of 129I and 135

Cs, respectively. In the selection of these radionuclides a cationic nature of americium and cesium, and anionic

nature of iodine, occurring in the studied system, has been also taken into account. The experimental arrangement of vertical column experiments will be similar to that of described in [9]. The real dimensions of the column fitting to the new conditions will be adapted suitably. In the vertical experimental arrangement the flow of the aqueous phase will be directed from bottom to the top of the column, in which the upward vertical migration processes will take place. The experiments will be performed in saturated conditions. For the investigation of migration processes in the horizontal direction columns with a special design will be used. In real samples, the directional anisotropy of soils and sediments will be taken into account, especially in horizontal core sampling, where mainly the stratification of the bulk material will be considered. Sorption of water soluble radionuclides will be done from synthetic and real liquid media. In a given time period, aliquots of the column outflow solution will be taken, in which the investigated radionuclides wil be determined.

Following the sorption and desorption experiments will be carried out on the same filling of the

columns and in the batch experiments as well, using various reagents, including real groundwater. Both of the migrations will be followed by non-destructive technique using scanning gamma-ray spectrometry. At the end of the each run also destructive analyses will be made. The experimental data will be treated and used into mathematical models, which will be further compared with each other (including input data demand). The ADE model is based on a different approach in comparison with the compartment model. The construction of breakthrough curves (BTCs) will be the mostly used evaluation technique, along with the sorption and desorption studies. The compartment model will be applied besides the advection-dispersion equation (ADE) model, which will be also used for comparison of the obtained results.

6

In order to obtain some important geochemical parameters necessary into the migration models, selected kinetic and isothermal equilibrium (batch) experiments will be conducted in parallel. The batch method will be used as complementary method. Other parameters: physical, chemical and mineralogical characterization of sampled materials (granulometric analysis, phase analysis, specific surface area, exchange capacities, permeability, etc.) will be experimentally determined or taken from the literature. Throughout the experiments, laboratory conditions will be applied. In the experiments, home-made apparatuses and chemicals will be used with the exception of radionuclides. These will be supplied from the domestic (e.g., Lacomed) or foreign company (e.g., Amersham International Ltd). The conventional single-channel analyzer will be used for the evaluation of the gamma spectra. Statistical treatment of data and their tabular and graphical presentation will be performed in widely available software (MS Excel) and in advanced statistical package (Palisade Decision Tools Suite). d) Expected results, their use, and significance for practice The main goal of this project is a laboratory quantification of migration of typical long-lived fission products and transuranics in soils and sediments under near natural conditions. The expected important result will be onedimensional mathematical model(s), which can depict the migration of actinides and long-lived fission products based on the bench-top experiments, investigating horizontal and upward vertical direction. The experimentally determined breakthrough data, mainly retardation coefficients and hydrodynamic dispersion coefficients, migration rate constants and relaxation times, respectively, in both directions, will be used for description of spatial dispersion of radionuclides from a source of contamination. The results can also be used to calculate the migration rate and relaxation length of radionuclides in their environment in a given direction. Other results will comprise the acquired parameters of the sorption of radionuclides in selected soils and sediments, among others the distribution coefficients, retardation coefficients, constants of isotherms (Langmuir, Freundlich, etc.), which, along with the hydraulic conductivity data, may well complement the depiction of radionuclide migration into ground waters. The expected and assessed different simulation capability of the ADE and multi-compartment model will be tested in different areas of migration process in order to obtain more reliable evaluation of radionuclide migration. The model(s) will be used for the description of the radionuclides migration and interaction under far field conditions of repositories. The model(s) thus can form an integral part of the radiological risk & safety analyses and performance assessment of the repository. e) Applicant and co-workers, laboratory facilities The applicant, DSc. in nuclear chemistry, was a coordinator of the research work, which studied the migration of

90

Sr,

137

Cs and

131

I radionuclides in soil as an important compartment of the air-soil-vegetation-

animal-man food-chain, in the former Institute of Radioecology and Applied Nuclear Techniques in Košice, Slovakia, in years 1985-1992. This institute was founded by Czechoslovak Atomic Energy Commission, which operated, among some other Czechoslovak research institutions, also this institute. Later, the applicant left this institute and in 1993 started to work in the Department of Radiation Dosimetry, Institute of Nuclear Physics, Academy of Sciences of the Czech Republic, Prague, until 1994, where he finished theoretical works in modeling. Then he joined the State Office for Nuclear Safety in Prague, where he was active in the field of radioactive waste management and decommissioning of nuclear installations, until 2004. During these periods, he did not stop his

7

cooperation with his former co-workers, as it can be seen from the modest list of his publications from the solved issue (subchapter g) of this chapter C). The applicant also lectured on the research in this field on several domestic and one international conference (21th Annual Meeting of the European Society of Nuclear Methods in Agriculture (ESNA), Košice, 1990). The applicant has published more than 60 original papers in the scientific journals including two chapters in two monographs, mainly from column separation chemistry and radiochemical analysis, but most recently also in the field of the retention and migration of radionuclides and heavy metals in soil [23]. A. Laciok (born on 3 November 1967), co-worker, university graduated researcher of the Nuclear Research Institute Řež plc, head of the department, has an extensive experience in geochemistry, natural analogue studies, risk & safety analyses and performance assessment of radioactive waste disposal facilities, including deep geological repositories. V. Havlová (née Buňatová, born on 8 March 1970), co-worker, university graduated and post-graduated researcher of the Nuclear Research Institute Řež plc. She has specialization in environmental geochemistry, geochemical modeling, natural analogue studies and risk & safety analysis. She has experience with different nationally funded and international projects. J. Landa (born on 7 February 1966), co-worker, university graduated researcher in Nuclear Research Institute Řež plc, have substantial experiences in simulation modeling of transport processes, including radionuclides, and risk & safety analysis. Two technicians, with an excellent practice in the radiochemical work, will participate in this project. There is an assumption that this research group is able to fully perform the proposed project. The laboratory facilities of the Nuclear Research Institute Řež plc are equipped with the main devices necessary for work with radionuclides. The required services, including radioactive waste management, working place and personal dosimetry, and medical care, are available. The experimental part of the proposed project will be carried out in the radiochemical laboratories equipped with necessary facilities and apparatuses. The conventional one-channel spectrometer with a NaI/Tl gamma ray detector will be used for the activity measurement. f) Use of the financial support No capital expenditures are planned. The financial support will be used only for salaries and for purchase of radionuclides, chemicals and laboratory materials, to pay for the preparation of migration columns and laboratory services. A part of the support is planned to use for the active participation in an international conferences on radionuclides migration in a terrestrial environment. g) References 1. Postup při zpracování z předběžné bezpečnostní zprávy pro povolení výstavby úložiště radioaktivních odpadů – Doporučení (The method for elaboration of preliminary safety report for the construction of a radioactive waste repository – Recommendation), SÚJB, Prague, 2003. 2. Factors determining the long term back end nuclear fuel cycle strategy and future nuclear systems, IAEATECDOC, Vienna, May 2002. 3. M.J. Frissel, H. Noordijk, K.E. Van Bergeijk, The transfer of radionuclides in natural and semi-natural environments, Elsevier Applied Science, London, 1990. 4. Š. Palágyi, T. Szabová, A. Mitro, Retention of some important radionuclides in soils, Jad. energie (Czech Nucl. Energy), 37, 5 (1991) 177-180.

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5. M. Hercík P. Lietava, M. Vidra, Experimentální validace matematického modelu transportu kapalin a kontaminantů (Experimental validation of the mathematical models for transport of liquids and contaminants), Dílčí výstup grantu (Progress report) GA ČR č. 103/98/0989, ÚJV Řež a.s., 2001. 6. Navarčík, A. Čipáková, Š. Palágyi, Study of physico-chemical forms of 85Sr, 137Cs and 109Cd occurrence in soils, J. Radioecol., 2 (1994) 19-24. 7. Š. Palágyi, J. Palágyiová, A. Mitro, Migration of radionuclides in undisturbed vertical soil profiles, Research Report No. 396/94 of the Department of Radiation Dosimetry, Institute of Nuclear Physics, Academy of Sciences of the Czech Republic, Prague, December 1994, 31 p. 8. Š. Palágyi, J. Palágyiová, A. Mitro, Caesium and strontium migration in column experiments, Subchapter 4.1 of Radionuclide distributions in undisturbed soil and related gamma dose rates in air, Chapter 4 of European Commission Final Report by J. Tschiersch et al.: Deposition of radionuclides, their subsequent relocation in the environment and resulting implications, EUR 16604 EN, Brussels- Luxembourg, 1995, 113 p. 9. Š. Palágyi, J. Palágyiová, Migration of 85Sr and 137Cs in vertical soil profiles, J. Radioanal. Nucl. Chem., 241, 3 (1999) 475-481. 10. Š. Palágyi, J. Palágyiová, Vertical migration of 85Sr, 137Cs and 131I in various arable and undisturbed soils, J. Radioanal. Nucl. Chem., 257, 2 (2003) 353-359. 11. Z. Hölgye, M. Malý, Sources, vertical distribution, and migration rates of 239,240Pu, 238Pu, and 137Cs in grassland soil in three localities of central Bohemia, J. Environ. Radioactivity, 47 (2000) 135-147. 12. M. G. McDonald, A. W. Harbaugh, A Modular Three-Dimensional Finite-Difference Ground-Water Flow Model, Techniques of Water-Resources Investigations of the U.S. Geological Survey, Book 6, Modeling Techniques, Chapter A1, 1988. 13. M. P. Anderson, W. W. Woessner, Applied Groundwater Modeling, Simulation of Flow and Advective Transport, Academic Press Inc., San Diego, California, 1992, 381 p. 14. C. Zheng, G. D. Bennett, Applied Contaminant Transport Modeling: Theory and Practice, VanNostrand Reinhold, NewYork, NY, 1995, 440 p. 15. K. Štamberg, Modelování migračních procesů v životním prostředí (Modeling of the migration processes in the environment), Vydavatelství ČVUT, Praha, 1995, 119 str. 16. Císlerová M., Vogel T., Transportní procesy (Transport processes), Vydavatelství ČVUT Praha, 1998, 182 p. 17. M. O. Barnett, P. M. Jardine, S. C. Brooks, H. M. Selim, Adsorption and transport of uranium(VI) in subsurface Media, Soil Sci. Soc. Am. J., 64 (2000) 908-917. 18. F. W. Boone, M. V. Kantelo, P. G. Mayer, J. M. Palmas, Residence half-times of 129I in undisturbed surface soils based on measured concentration profiles, Health Phys., 48 (1985) 401-413. 19. D. C. Kocher, A validation test of a long-term retention of 129I in surface soils, Health Phys., 60 (1991) 523531. 20. G. Kirchner, D. Baumgartner, Migration rates of radionuclides deposited after the Chernobyl accident in various North German soils, Analyst, 117 (1992) 475-479. 21. K. Bunzl, H. Förster, W. Kracke, W. Schimmack, Residence times of fallout 239,240Pu, 238Pu, 241Am, and 137Cs in the upper horizons of an undisturbed grassland soil, J. Environ. Radioact., 22 (1994) 11-27. 22. Š. Palágyi, A. Laciok, Teoretické a experimentální studium migrace ve vodě rozpustných látek v kolonách plněných přírodním zrnitým materiálem (Theoretical and experimental studies of migration of water-soluble substances in columns filled with natural granular materials) Internal Research Report, ÚJV Řež a.s., 2004. 23. Š. Palágyi, J. Rigas, Sorption of cadmium in some arable and forest soils, J. Radioanal. Nucl. Chem., 261 2 (2004) 255-261.

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Grantová agentura České republiky - Část D Navrhovatel a spolunavrhovatelé Jméno navrhovatele: Štefan Palágyi (born on 19 December 1939) After moving to the Czech Republic in 1993, he joined the Department of Radiation Dosimetry, Institute of Nuclear Physics, Academy of Sciences of Czech Republic in Prague, where he was active as a senior research scientist in the field of environmental radioactivity, until 1994. During his stay in this department he received D.Sc. degree in nuclear chemistry for his work “Analytical concentration-separation methods for determination of radionuclides and trace elements in the environment”, which was adjudicated at the Slovak Technical University Bratislava in 1995. From 1994 he worked for ten years at the State Office for Nuclear Safety in Prague, where he was responsible for supervision of the radioactive waste management and decommissioning of nuclear installations as a nuclear safety and radiation protection inspector. He performed several professional and scientific visits in many countries (Austria, Belgium, France, Hungary, Italy, Japan, Slovakia, Slovenia, Spain, USA) where he had lectures on these issues as a member of IAEA or NEA OECD technical committees, advisory and consultants groups. By the beginning of March 2004 he joined the Nuclear Research Institute Řež plc, where he is a staff member of the Waste and Environmental Management Department. In his past professional career, the applicant worked in a broad range of various areas in radiochemical analysis, radioanalytical methods and preconcentration and separation chemistry. The present research activity of the applicant comprises the study of the theoretical and practical aspect of migration of ecologically important long-lived radionuclides in the environmental systems, where soil is involved. Formerly his interest included the soil-vegetation system, presently his scientific interest has focused on to the soil-groundwater systems from the view-point of the radiological safety & risk/environmental impact assessment studies of the radioactive waste repository. He published more than 60 articles mostly in international scientific journals and was the coauthor of 2 books at CRC Press from the radiochemistry and radioanalytical chemistry. At present he is a member of the Czech Chemical Society, committee member of the Czech Radioecological Society, International Public Body of the Hungarian Academy of Science, Associate Editor of the Journal of Radioanalytical and Nuclear Chemistry, member of the committee for Adjudication of DSc. in nuclear chemistry at the Slovak Technical University (STU) Bratislava and member of a committee for the Appointment of associated professors and professors at the Charles University in Prague and STU in Bratislava. Selected publications and reports from the last 7 years: 1. Š. Palágyi: Separation and preconcentration of ionic solutes by transport extraction based on solvent sublation, Chemical Papers, 52, 5 (1998) 671-681. 2. Š. Palágyi with a collective of authors: Approaches to decommissioning of nuclear facilities, PDRP-2, IAEA, Vienna, 1998, 14 pp. 3. Š. Palágyi: Separation of radioiodine from water by transport extraction based on solvent sublation, OECD Nuclear Science Committee, Proceedings of the Workshop on Long-Lived Radionuclide Chemistry in Nuclear Waste Treatment, Villeneuve-les-Avignon, France, 18-20 June 1997, Nuclear Energy Agency, OECD, Paris, 1998, pp. 209-220. 4. Š. Palágyi: Kinetics of transport extraction based on solvent sublation, Czechoslovak Journal of Physics, 49 (1999) 739-745, Supplement S1, Part II. 5. Š. Palágyi, J. Palágyiová: Migration of 85Sr and 137Cs in vertical profiles of soils, Bezpečnost jaderné energie (The Safety of Nuclear Energy) , 7 (45) 5/6 (1999) 159-164.

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6. Š. Palágyi, J. Palágyiová: Migration of 85Sr and 137Cs in vertical soil profiles, Journal of Radioanalytical and Nuclear Chemistry, 241, 3 (1999) 475-481. 7. Š. Palágyi: Application of the proportional mapping technique to the representation of some nuclear energy and radioactive waste generation related indicators, Bezpečnost jaderné energie (The Safety of Nuclear Energy), 9 (47) 5/6 (2001) 188-193. 8. R. Alejandro, J. Burclová, A. Colquhon, V.M. Efremenkov, P. Hartwig, M.S. Kimura, J. Mišák, Š. Palágyi, L. Teuckens, A. Thomas , L. Valencia, P. Vankerckhoven: Methods for the minimization of radioactive waste from decontamination and decommissioning of nuclear facilities, IAEA TRS No. 401, Vienna 2001, 157 pp. 9. Š. Palágyi, V. Fajman: The strategy of the long-term back-end nuclear fuel cycle in the Czech Republic, in Factors determining the long term back end nuclear fuel cycle strategy and future nuclear systems, IAEATECDOC-1286, Vienna, May 2002, p. 49-56. 10. Š. Palágyi, in a collective of authors: Decommissioning of Nuclear Power Plants: Policies, Strategies and Costs, NEA OECD, Paris, 2003, 105 pp. 11. Š. Palágyi, J. Palágyiová: Vertical migration of 85Sr, 137Cs and 131I in various arable and undisturbed soils, Journal of Radioanalytical and Nuclear Chemistry, 257, 2 (2003) 353-359. 12. Š. Palágyi, Representation of some nuclear energy and radioactive waste generation related indicators using the proportional mapping technique, Proceedings of the 23rd International Symposium “Industrial Toxicology `03”, Bratislava, June 18-20, 2003, p. 95-103. 13. Š. Palágyi, J. Rigas: Sorption of cadmium in some arable and forest soils, Journal of Radioanalytical and Nuclear Chemistry, 261, 2 (2004) 255-261. 14. Laciok, Š. Palágyi, P. Rajlich, Anthropogenic analogues in the Czech Republic – studies on glass and concrete materials, IAEA Final Report: Anthropogenic Analogues for Geological Disposal of High Level and Long Lived Radioactive Waste (1999-2003), IAEA Vienna, 2004, 54 pp. 15. Š. Palágyi, Sorpce kadmia na orné a lesní hnědé půdě (Sorption of cadmium in arable and forest brown soils), Sborník semináře “Radioanalytické metody – IAA `04”, Praha, 30. června 2004, 4 str. 16. Š. Palágyi, A. Laciok, Teoretické a experimentální studium migrace ve vodě rozpustných látek v kolonách plněných přírodním zrnitým materiálem (Theoretical and experimental studies of migration of water-soluble substances in columns filled with natural granular materials), Internal Research Report, ÚJV Řež a.s., 2004, 30 p.

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Grantová agentura České republiky. Grantová přihláška standardního projektu

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