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,

THE ORGANIZATION OF RUSSIAN ACADEMY


OF SCIENCES INSTITUTE OF GEOLOGY OF ORE DEPOSITS,
PETROGRAPHY, MINERALOGY AND GEOCHEMISTRY
RUSSIAN ACADEMY OF SCIENCES
PRESIDIUM OF RAS, PROGRAMME N 16

CHANGES OF NATURAL
ENVIRONMENT AND CLIMATE
natural and possible consequent human-induced catastrophes
In 8 volumes

Volume V

IGEM RAS
Moscow
2008

16



2008
621.039.7
26.0
37

37 :
: 8 . / . . .: .. . . .: , 2008.
ISBN 978-5-916-82001-0

.., .., .., ., .., ..


. 2: : .
.: ; , 2008. 280 .: .
ISBN 9785889-180104


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621.039.7
26.0

In a monograph geological and geochemical aspects of the problem of spent nuclear fuel (SNF) and highlevel radioactive
wastes (HLW) safe underground isolation are analyzed. Based on the data on conditions for preservation and deterioration of
uranium ore deposits, a principal possibility for safe longterm storage and disposal of SNF and HLW in underground reposito-
ries was confirmed; protective features of geological environments are characterized; requirements and methods for selection of
sites appropriate for safe isolation of SNF and HLW are considered; processes of interaction of SNF and HLW with geological
environment and their affect upon safety of repositories are examined; influence of geochemical properties of radionuclides on
conditions of their migration and localization in geological medium are characterized.
A considerable attention is given to analysis of actinides migration in underground waters and to securing conditions for mini-
mization of their leakage from buried SNF and HLW. Engineered barriers conservation matrices and low permeable bentonite
buffers with high sorption capacity are described. Investigation methods for studies in underground research laboratories are
characterized.
The technique of liquid radioactive waste injection into aquifer horizons, employed in Russia, is described and problem of
sites selection for underground disposal of solidified HLW and SNF at regions adjacent to the PA Mayak and Mining and
Chemical Combine radiochemical plants is examined. The last chapter of the monograph is devoted to a problem of reducing
of HLW radiotoxicity by separation and transmutation technologies.

ISBN 9785889-180104
, 2008
ISBN 978-5-916-82001-0 , 2008
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, -
(, ).
- .
. , , -
, , . -
. - -
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. () -
- [Krauskopf, 19881; Krauskopf, 19882].
, , , -
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.
, -

. . -
, .
. -
- , ,
[The scientific, 1995] [, 1992].
. -
, , , -
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. - . -
,
. -
. - 76 600 .
, 1982 . , -
- -
. , - (Waste isolation pilot plant, WIPP). WIPP -
,
, 35

. -
, -
300000 2, .
75 . - . -
600
, , ,
, . 1999. - .
-
WIPP - in situ.
,
(TRU), - ,
. TRU c 19671978 . -
, - .
, - 125000 -
. , , , 1300 [The Gorleben ,
. TRU 1994]. -
3.7106 / [Neill, Lee, 1995]. - -
178000 3 490800 . 1979 .
(3.31017 ) 7100 3 - , -
1.851017 . 655 -
, .
, ,
70 .
. - -
, . -
, -
. - ,
, 200.
. 60Co -
- 1.31013 .
,
[Brookins, 1984]. .
WIPP . -
, . 1997 .
-
, ,
-
. . 506 , -
, - 150
30 . 4 .
-
506 . -
. .
, , - 40 %.
, -
.
200 , 1.7 /. WIPP, -
,
. . -
- 1979 1998 .
250 [The Gorleben, 1994]. ,
, - 40000 3 .
, - (BfS)
, , . 150000 3 . 1995 . -
20000 3 -
,
(. 6.1). . 95 %
. 1981 1991 .
14500 3 6200 .
36 6

. 6.1. () [The Gorleben, 1994].


: q ; t ; kro ; kru ; jo ; jm
; ju ; k ; m ; so ; sm
; su ; z .
, 37

1.810 14 . -
2900 . 2000 . - ,
150000 3 ,
1998 . - . ,
40000 3. - ( 0.01 0.02 /) -
, , 1 ,
. 1020 .

1979 . 44 30 4
. - 2000. -
- , -
1021 . ,
. - , .
14 4
260 3.5 -
(. 6.2 . ). - .
- -
1985 . . -
. , .
- , -
. -
. - ,

. ,
960 2 , - ,
840 . , -
. (500000300000 ) -
8401200 . - -
(
)
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2008 .
- 90130 .

. 140170 .

, .
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300 2. -
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150 . , -
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38 6

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- .
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in situ , . -
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[1992]. , , ,
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.
, 39

- , -
3.5 ,
() 1974 . -
. -
, -
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. 1984 . 223 - (h = 250 I400 mV) ( = 8.08.5)
. ,
100 , (13 %).
- (12.5 mM NaHCO3). -
.
, - . ,
- (15 %) -
. h. -
35 3.5 . 1988 .
60 , - .
. - -
- -
(200250 2/). 60 %
. , , ,
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) ; - 15 %. -
- (13 %)
; (~100 ppm). -
; , -
-
, ,
, , , ,
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, . ,
, - , in situ
(1.571012 /), 1012 /
. - . -
. , -
600 10 - .
1.0 / 0.2 /. 1010 /, -
, , - . (100 )
, ,
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, . -

. ,
40 6

. , - -
, . -
3107 / , -
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129I. = 7.24; h = 0.167 V; t = 25 C; log pCO2 = 2.2.

. 3 250 /.
1993 .
- .
( ). : ; -
, ; ;
- (
. 1994 . ),
- -
;
, - .
. - (~12 %)
. (125 ) -
, . in situ
- 1013 /
. 1014 / .
1000 3 ,
50 2. .
, 100 ,
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, .
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1750 /3. -
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38 . , 800 (. 6.3).
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(5 2); (20 5); (16 10);
+ (1 0.4); (4 2.4); ( 129I, 14C, 36Cl, 79Se)
(3 1.3); (1.1 1); - . -
(0.6 0.3). .
, 41

. 6.3. [Nagra, 2002].

- .
8.

[Safety, 2004]. .

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.
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-
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, - (, )
. . in situ
.
,
. 1.
-
, , ,
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20 [Smell, Rosholt, 1984].
. in situ ,
, 43

1 /,
2 % . -
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.
. - ,

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, -
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.
- .
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.
45

,

. - 137
s (1+)
- 137
Ba (2+)
20 %, 90Sr (2+) 90Zr (4+)
. 29 %;
. -
, -
. ;

5 50 . , -
- ;
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/, -
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, -
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-
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, NaPO 3 [ ., 1994]. ,
; , -
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;
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200 1000 .
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, -
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.

- . -
- -
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, K11.5Al4[Si76.5Al11.5O20](OH)4.
, , - -
,
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47

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10.
[Hodgkinson, , 10 -
1977; Deane, Hollis, 1979]. 100 , 100 -
250 . -
, - 1000
, 170 , 10000 60 . ,
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1977; Krauskopf, 1988 2; Chapman, McKinley, 1988]. , 500 -
50
: 10000 .
;

; 7.2.2.

.

,
7.2.1. -

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() -
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.
48 7

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., 1994]. -
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) -

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:
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[, 1970].
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. .

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49

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10 610 3 [, 1989]. , - 20
, , 180 .
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- 500600 -
. . 1.53 .
[Brace, 1980], - . -
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-
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-
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,
. ( = ) 50800
, -
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. [, , 1982].
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.
, , -
- -
[, , 1982; . 50 200 -
., 1989; Omelianenko et al., 1993]. - 103
, - 250300 ,
, = 500800
103 > 500
. - (. 7.2). -
,
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. - (~200 ).
,
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). . 400
500600 -
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.
50 7

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300
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-
[, 1972]. -
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[1948] -
:
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.

,
, - , .
. , -
- ,
- . -
, ,
, - :
. ..
- 2Mg2SiO4 + 3H2O = Mg(OH)2 + Mg3Si2O5(OH)4.
-

. 1.5
51

. - -
: .
-
Mg2SiO4 + 2O2 = 2MgO3 + Si2.
. -
1.7 - -
. , , , ,
,
. ( 50) - . -
() : ,
,
2NaCaAl3Si5O16 + 8H2O = . -
= Na2Ca2[Al2Si3O10]38H2O + SiO2. -

-
2.5 .
,
,

. -
,
:

5CaMgSi2O6 + H2O + 3CO2 =


= Ca2Mg5Si8O22(OH)2 + 2SiO2 + 3CaCO3.

30 %
.

(, .)

, . -

37 %:

CaAl2Si2O8 + 2H2O + CO2 = Al2Si2O5(OH)4 + CaCO3.

50 % -
-
18 %. , -

.
,
47 %,
3 % [ ., 1994]. -
, -



.

-
.
.
, . 7.3.
.
-

; ,
- ; .
, , . 50.
52 7


.
-

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-


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. 7.4. () (),
[Padovani et al., 1982]. ,
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[ ., 1983]. -
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7.4. [Blair et al., 1996].
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. -
, , -
- H2O2, O2, H2, OH, HNO3.
.
, .
8

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,
. 70
- .
[Site selection, 1977]. ,
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[ ., 1994;
Kochkin et al, 1997; , 1996; , 1998; 1 / 5 , 1 2 /
, 2002]. - 4, 2 3/ 3, 3 4/
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57

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[Kochin et al., 1997]

,
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1 5 4 4 5
2 5 3 2 4
3 5 2 2 4
4 5 5 4 5
5 5 3 3 2
1- 25 17 15 20
6 4 3 4 4
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2- 12 10 9 11
9 3 - - 2
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91

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12

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94
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( 1000 )
Eh
[Nordstrom et al., 19891]. -
, , - Fe2+/Fe3+
[, , .
1992]. - -
. - -
( , , . -
- , ,
) 28/
. Fe2+. , , -
, , - , -
200250 , .
400 . -
600800 , ,
700900 .
. Eh,
-
.
-
, - -
. , ,
, - -
,
in situ [Solodov, Zotov,
. , 1995]. ,
, .
-
, . 40 60 , -
. . -
- -
, - , .
pH -
[Degueldre et al., 1996]. 6.4 8.5, Eh +500 +50 mV.
1 4 . ,
, , 200
. - -
240 +350 mV. .
Eh < 180 mV -
430 . - -
Eh, 210 mV, , -
1680 .
95

.. (1996, 1997). ,
12.2.
Fe(II)Fe(III). -
-
,
- -
Fe(II)Fe(III). , , , , . -
, -
- ,
.
, - ,
, . -
pH Eh [, 1975]. -
0.25
.
. ,
pH Eh.
, , 12.2.1.
, ,
, Eh -
, . n(10 510 3) . %, -
pH. - . -
, pH Eh ,
. -
. , - , -
, , -
pH 9 Eh 160 mV [ ., [ .,
1996]. - 1983]. , -
, -
-
. - .
- -
, .
pH Eh
. -
(. 7.3).
, -
, ,
, -
. ,
. -
, - -
, ,
: , -
- .
-
;
- .
-

;
-
- .
- , .
500 ; ,
- ,
500 -
,
. .
96 12

-

:

U+4 + 4H2O = U(OH)4 + 4H+.

U(OH)4
n1052 [, , 1992].
-
-
[Redkin et al., 1990].
,
-
,
. -


108 /. -
, -
.
-
-
(. 12.2).
.
-
,

.
, -
.
, - . 12.2. EhpH UCOH
FeSOH [Brookins, 1988].
: U= 106, 108, 1010, C= 103,
.
Fe= 106, S= 103. EhpH
, .
.
, -
, , ),
. -
- . , -
-
. .
-
. - .
-
10 3 /. -
, ,
, .
106107 /. - 102 / -
, .

. - 10 4 /. -
- 10 6 /. [,
, , - 1975]. , -
, , ., .

. - .
-
- , -
(
97

, -
, -
. .
, -
, ,
, - .
- , -
: ,
-
U4+ + 2H2O = UO22+ + 4H+ + 2e. ,
.
UO2(OH)2 - , -
1022, 30 U(OH)4 -
[, , 1992]. , .
UO22+
. - -
- , -
, ,
- . -

, CO32, HCO3, SO42 [ - -
, 1980]. ,
. - (. 12.1).
UO2(CO3)34, -
UO2(CO3)22, UO2(CO3)0, UO2(SO4)22 [, . , -
, 1989]. , , 500
- , -

. [ ., 20011].
, ,
95 % .
, -
, - .
- -
.
, 108 / (. 12.2).

, .
-
,
- . -
. 7.9 . %,
. %.
1.1 .
12.2.2. 400 ,
,
. -

.
- , -
. -
. U
, - 40 % U ,
. 108 /.
- :

. , , , -

. , - 23 , ?
,
98 12

,

. -
-
, ,
, . -

[Johnson, Shoesmith,
1988]. , -

. -


,
10 , [Loida et al.,
2001].
- . 12.3. I ,
. [Natural fission
reactors, 1978].
. , - 1 ; : 2 , 3
20 . ; 4 ; : 5 ,
6 ; 7 ;

8 .
,
-
. -
, - GauthierLafaye, 1998]. -
-
. , ,
- ,
, . , Am,
Pu Np , -
( ). 209Bi
- 207Pb, , -
, ,
-
. -
235U, - . , Rb, Cs,
Sr, Mo, Cd, Xe I,
, . , Ru Sn .
-
2 , - , -
, 33.5 .
(. 12.3). , -
235U 3.25 . %, ,
- ,
. . ,
, , -
500 -
- .
, [Natural
fission, 1978]. -
, - . -
, -
-
- .
, , 100 , -
. , , -
250 , - -
[Pourcelot, [Pourcelot, GauthierLafaye,
99

1998]. ,
, 10 - ,
, ; 4 -
. ,
, , -
, ; 5 -
- .
. , ,
. - .
, - , , -
, .
, -
. , ,
, -
, - . , -
,
. , , -
.

12.2.3.
.
- (1 /),
(1 /), (2.2 /), -
(1.82.8 /),
(1031 /) -
, , (1015 /). ,
. ,
-
. - .
- 24
813 /, 24 , . , , 13 -
- .
(0.0040.08 /) - -
, - . Th -
(2543 /), (1030 /), Zr, Hf, U, TR, Ca.
(3050 /).
, , .
, ,
,
+IV
. - (. 12.4).
Th -
, , - pH < 4 (106 /) pH > 9 (105 /).
, pH 3.5
. - Th(OH)4 . -
, Th(OH)4 3.21045.
. -
, :
.
Th(OH)4 ThO2 + 2H2O.
. %,
. -
. , -
: 1 ,
, - .
, -
; 2 , . ,
, -
; 3 , .
100 12

.


. -
-
, , -
.
-
,
-
. -
, , , , ,
, . -
-
,
, , , -
, .. -

,

. -
,
. -

. -

20 . %, %.
( 16 %), -
( 8 %) . -
.
. 12.4. I , -
[Natural
-
fission reactors, 1978]. .
1 ; : 2 , 3 , -
; 4 ; : 5 , ,
6 ; 7 ; ,
8 .
,
.
,
, . [,
, 1987].
, - -
. .
, , , , , ,
, , . - , -
(, - . -
, , .) -
, ,
.
.
- -
(ThO2) (ThSiO4). , .
, . -
- -
. ,
(ThO2) (UO2) - .
, -
- ,
Th:U = 1. (Ce,La,Nd,Y,..Th,U,..)PO4.
101

2.528 . %. -
-
, ,
, - . -
, , ,
. -
- .
, ,
, . -
, , - 20250 ,
(>5),
, -
- -
. .
-
Th - .
109 /.
- .
.
( n107/) , -
, -

.
, -
, -
- .
.

.
. , , -
,
- . , -
- ,
. - , -
. , , . ,
- ()
- -
- , -
U(OH)4Th(OH)4. , ,
- .
-
. , , -

, , , -
, ,
. - -
,
(>250 C), - .
, -
.
, -
, 12.3.
,
,
[ ., 1980]. -
.
. - -
U4+ U6+, - , -
UO22+. ,
102 12

, - .

, -
. -
. - -
, Ce,
. Gd
, - .
-
-
-
. - , , ,
() , , -
. .
- -
Eh pH . -
( Pu)
. -
, ,
- Fe, Ti, Mn, Al,
- (, ,
, - .).
. , -

, -
12.3.1. ,
.
- -
, - ,
PuO2, ThO2 UO2, -
238
U. Pu/U . -
(0.415)10 12. -
- -
[, 1992]. 239Pu , [Brookins, 1984]. -
-
, ,
. . ,
. , -
, - ,
.

[Allen, 1978]. -
,
- , -
Pu+3(. 12.5). -
239
Pu [Kastenberg et al., 1996; Oversby,
1998]. -
, , ( ) -
. -
.
, .
, , , -
,
. - .
, , -
, , (8 1.5).
[Frejacques et al., ,
1976 .]. = 8 -
, Th, Pa, U, Np,
Am, Cm, Zr, Nb, Sn, Pb , (III),
103

-
1200 3/ 1800 3/ [ , 1999].

Kd -
.
2 [Baston et al.,
2000], [Berry et al., 2002]
.
, -
0.25 /
5:1. , Kd -
1000 3/, -


. , -
, -

( , , , -
.). -
, -
.
, 60 %
, -
1 % [Vaniman et al., 1996].
, -
,
,
-

. 12.5. EhpH PuCOH = 25
= 1 [Krauskopf, 1986]. . , -
Eh pH, ,
Pu 1017.
, , -
. .

PuCO3+ (. 12.6);
Eh 100 +150
(IV); ,
,
(V) (VI) [Berry et al., 2002]. -
-
Eh , -
Pu (IV),
-
.
Pu(OH)4.
, ,
, -
.

-
.
(Kd) -
, , Eh,
. 12.6. EhpH PuO 2CO 2H 2O
. Kd = 25 = 1 .
100 3/ Puaq = 108M,
- = 102 M [Traexler,
3/. Kd 550 3/, Eving, 2002].
104 12

in situ , -

2

[Neretnieks, 1993]. ,
( -
, -
)
,
,


.

-
-
, ,
. ,

-
.

-
(. 12.7). -
,
[ ., 1999].


-
[Vandergraaf,
Abry, 1982].
, ~51014 / -
, 19.5 % 237Pu
(1/2 = 45.3 ).
Kd
1 2 1 3 -
(/2:/3),
. -
9.5 2,
10 3, 28 . Kd -

1.470.0 14 .
, -

. . 12.7.
- .
, () ; ()
. , ( ., 1999).

, -
. -
- [Neretnieks, 1993].
. , - , Cs, Sr,
, Eu, Nd, Th, U,
, 510 -
. .
-
, - -

105


-
. - . [Lelous et al.,1998]
, -
. ,
, -
. -
. 90 ,
40 .
50250 . -
.
PuO2H2O Pu(OH)4, , - 3 % 300 ppm .
- 11 ,
, , . -
Eh 310 , 8.35, -
. - 160 7.95.
, - -
(). .

1.31011 / 1.81011 /. -
. - , , -
, - . -
, ,
, ,
. -
1.3 - ,
[Kersting et al., 1999]. ,
, - ,
-
1402 1968 . - .
1014 /, ?
99 % .
.
- , -
.

- , -
- . -
. , ,
, , -
- . , -
, , -
, , ,
. ,
.
410 11
2.8106 / [Keum et al., 2003]. ,
- . -
. [Loida et al., 2001]
, - -
. . 545
,
, 1 % .
. 34
- .
, - ,
. ,
- , . -
, -
. <3.
106 12

, , - ( = 7.6, h = 0.77).

- -
. -
, ( = 7.68.1) - .
( = 7.5). - -
( = 78) ,
5.4105 /, 1.5106 /. ,
.
. - . -
1.8 , 96 %
99 % - 25 2108 /,
. - Pu(OH)4 -
108 /. , 25
6108 / [Kulyako et al., 2001]. 85 -
.
3050 , - (21011 /), -
, .
,
1 % [Neretnieks, 1997].
-
. -
, - :
, ,
, , , -
. -
41011/, 1011 /,

[Lelous et al.,1998], - 239
Pu ;
. -
- -
,
[Albinsson et al.,
2003]). ,
;
10.1 . - -
1825 , 10 ,
200 . , , -
, 8.05. -
106 /, ;
. - ,

108109 /. , , -
-
- -
, 106 /,
. 99 % ;
1091010 /, -

21011 /. , 108 /, -
, Pu(OH)4;
-
.
- , -
, - ,
, .
, - -
,
[Waste form, -
1998]. .
107

,
1.310 9 /,
7.71011 /. -
, - -
.
. [Tsuka- .
moto et al., 1995] , - , -
,
71160 , 0.22 . % 238Pu -
(1/2=88). , -
90 , 208 375 - ( -
. )
8.18.3, h 91 102 . .
-
10 810 7 /. ,
- 400 , ,

. , -
, ,
(h = 0.55) , ,
. [Inagaki et al.,
1999]. 238PuO 2 .
0.12 . %, 75150 . -
Ar + 4 % H2 pH ( )
99.5 90 . - .
100 . Pu ,
- , , -
106 /, , - . ,
1.8 109 /.
Pu - .
108 /, 109 /. -
- -
-

, 109108/,
. - 107106 /, -
, .
Pu -
Pu(OH)4. , -
, ,
. , -
109/. - . , , ,
, -
, .
- .
-
,
. 12.3.2.

-
90 , -
- ,
. ( 1000 )
[Chambers et al., 1998]. , 50 % (. 2.1), -
0.5 . % PuO2, 65 % (. 12.8).
, -
170 .
.
(, , , 241Am,
). 243Am.
108 12

-

, , .

. -
, -
. -
,
-
,

, REE, ,
, , .
-
-
.
.
-
. -
,
100 -
2, -
(0.427.55)1010 /
(0.0260.82)1010 / [Michard et al., 1987]. -
-
, -
( 9.0, T = 75 ),
. 12.8. 450
7.110 9 / 3.510 11 /,
PWR 10
5 , , [Michard et al., 1991].
0.1 % U Pu.
lg TBq, 1GW
.
[Flowers et al., 1986].


- (7107 /) (2108 /) -
, 100 ,
. - ( 1.33, = 43 C) -
[Michard, 1989]. -
, -
n103 % . , -
n104 %. - ,
REE - -
1025 % 0.52 % - . , -
. -
. REE [Sturchio et al., 1986].
-
. , REE
, . , -
REE -
.
. REE - , -
-
, , , . n109 M/ n1010 /,
REE , .
- -
. REE REE
.
Nd2O3 0.39 . %. .
109

- , Am(OH)3,
. REE Am(OH)(CO3) (. 12.9).
-
, -
. . -
-
REE (pH = 8.6) Am(OH)(CO3),
Am(OH) 3() Am(OH) 3() c -
- 1.7108 /, 3.7105 / 6.5104 /
, - [Waste form,1998].
.

REE, - .
. -
, -
. - ,
. . -
, Am(OH)3
, () -
- 106.3 / [Geochemistry of long, 1992]. -
.
[ ,1999]. -
,
, - 1
. 1010 /, . . -
. -
-
Am(OH)3, -
- .
, ( ) . -
Am(OH)3 (21012 /).
. ,
CO 32, SO 42, -
Am(OH)3
. -

,

.
,
.
-
, , -
,
Am(OH)3 . -

-
.
= 8,
.. (2001), -
( %): AmCO+3 43.2, Am(OH)2+ 22.4,
Am(OH) 2+ 15.0, Am(CO 3) 2 12.0, Am 3+ 4.1,
AmCl2+ 1.5, Am(CO3)33 1.1, AmSO4+ 0.8. -
-
, -
,
, , . 12.9. Am (III)
- 6 10.5
, 2 [Chemical thermodynamics of americium, 2004].
110 12

- -

- , ,
, Am(OH)CO3 Am(OH)3.
. , ,
UO2, , -
- , , -
. - . ,

, -
, ,

. , . 85 -
,
, , , 25, -
, -
. .
- Am
109 / -
, , . ,
. - -
, .
, (pH = 78) , -
545 , -
, - -
(2.53.6)10 8 / .
[Loida et al., 2001].
1.8 99 % Am . . -
- -
1.8 . .

,
.
, [Waste form, (, pH, Eh, -
1998]. , ,
(23 ) - .), -
(pH = 7.6). (Kd) -
25 85 3/, -
, -
. [Baston et al., 1995].
-
- 2000 /,
, UO2, 98 % [Geochemistry of long,
1992]. 70 Kd
, - (15 %) (85 %) 7.5104,
. - 0.46104 7.5104 3/ [Baston et al.,
, 1995]. Kd
, - , -
, ,
. . (Rf) -

, ,
,
. .
, ,
400 ,
~1.51010 M/. - -
1.8 , ,
5 , . -
.
111

. - . -
, . Np 3 ,
-
, -
, , .
-
. .
, - -
[ ,1999]. ,
, .
, , Np 3
, . .
- Np (III) , Pu (III),
. Np (V) ,
Pu (V). , -
. , -
Eh pH.
Np (V) ,
12.3.3. Np (IV), -
Np
.
- -

-
. .
Np2.
, - . Np2
,
- . -
, - -
. , , - ,
, , -
25 1.7109 /,
. 85 610 9 / [Waste form, 1998].
- ,
. -
- ,
237Np 2.1106 . NpO22H2O().
. -
1 /,
. 25 pH = 9.5 -
239Np, -
243Am, 10 /. 4108 /,
- Np(OH)40 [Inagaki et al.,
, 1998].
2.4 . -
239Np 239Pu, -
239Np Np(OH)3CO3 (. 12.10).
. - -
- , -
237Np.
3, 4, 5, 6 . [Pirlet et al., 1999] -
7 ,
- PAMELA SM539,
Np (IV), (0.034 . % 237Np 0.34 . % 237Np) -
Np (V). - . -
Np , - .
Eh, h
, 4 3 26 122 B 62 ,
112 12

-
. -

NpO2OH(am) NpO2+ + OH.
Np (V) Np (IV)
Np -
.
, -
,

-
106 /,
237Np
.
,
, ,
,
, -
, -
. 12.10. EhpH NpO2FSO4CO2H2O ,
= 25 = 1 . -
Npaq = 108M, , -
F= 104M, SO42 = 102M, .
= 102 M [Traexler, Eving, 2002]. Np (V)
NpO2OH().
9.6. - -
NpO2+ NpO2CO3 [, 2001].
. 6 , -
40 90
25 , pH = 9.5 h = +0.3 V
5107 /. 2106 /. Np
(2.910 6 /) , - , -
[Inagaki et al., 1998], 106 /,
(S/V = 1000 m1), 0.34 . % .
90 . Np -
2 , 80 % - J13, -
2 . , 4106 / [Waste form
, 20 % - 1998]. -
- Np (V)
2 , . 104 /,
- -
(R7T7), [Geochemistry, 1992].
( 0.22 . %), Np (
(90 C, S/V = 2600 m 1) - Tc U) ,
, -
. [Inagaki et al., 1998]. -
(Ar+5% H2) ,
90 - -
5106 / .
1.8. , -
, - .
<5 - K d
1.8 107 /. Np
, - . Kd -
Np (IV) ,
(4108 /), , 10 7 /, 8.5 -
, - 2.710 4 / [Nagasaki et al., 1998]. -
. , - Kd -
, . K d ,
113

-
.
(/): 4.1100, 5.510 2 2.010 3; ,
2.5101, 1.2103 9.9103; () ,
5.5101, 4.9103 8.1103 [ , 1999]. ,
= 56 Kd - -
, - -
(/): 1030, 200014000 10004000. . , -

, - .
1106 7107 / Np (V), Kd -
2 5 / [Traexler, Ewing, 2002]. -
Kd -
, .
h.
, - -
- [Kozai et al., 2001].
, -
. - , ,
,

, , , -
-
[Brookins, 1984]. . -
- , , ,
- , , , .
,
.
4 -
12.4.
. 209Bi, -
237 Np, -

. ,
, , ,
, -
- . -
, -
400 .

. - .
,
, -
. . -
, (O2, H2O2) (H2)
- , -
, -
. - -
, , , .
, :
-
. UO2 + H2O2 UO22+ + 2OH.
,
, - 9598 % , -
[Pourcelot, , -
GauthiesLafaye, 1998]. - .
5 , ,
. -
, - , Pu, Am, Cm, Th, REE, Nb, Zr, Sr, -
- ; Cs, I, C, Kr
114 12

, 12 -
,

; Mo, Tc, Pd - , -
.
[Johnson, Shoesmith, 1988].
, -
. - -
, - , -
, -
. .
, - [Rondinella et al., 2001] -
. - ,
0.1 % 10 % 238Pu, -
. - . -
, , 238Pu,
2.71106 2.71108 /2,
,
. , - 500
.
. 25 ,
- . Eh, -
60 , -
(Brookins, 1984; Chapman, McKinley, 1988; Krauskopf, 238Pu 0.1 % 10 %, ,
19882 .). - , 180, 380 570 .
, , Eh -
.
- , 238Pu
. - 0.1%, 108 /,
10 % 238Pu 2 . -
- 0.1% 238Pu
41012 /, 10 % 238Pu
- . :
(performance assessment).
- -
- ;
, - ,
5001000 , ,
, , -
. ;
-
, -
-
(.. 1000), ;

, , , -
c . 5 6
3050 , .

, - ,
1 % [Neretnieks, ,
1997]. . , -
, - 70
. - ,
, [Spahiu, Sellin, 2001].
- ,
, , -
. -
[Forsyth, Werme, 1986].
115

-
: .

3Fe + 4H2O Fe3O4 + 4H2. 2 .
, ,
, , -
- ,
, . , -
-
. - 2 -

- ,
, - .
[Loida et al., 2001]. , , -
- . , -
, - ,
. , ,
5.4105 /, 1.5106 /. - . , , -
.
20 , ,
U 2 , Pu, Am,
Eu, Np Sb , 3 , - , [Liu, Neretnieks,
. 1995]. -
, , -
805 , , - . , ,
, 4
, (FeOOH). , . -
2 ,
. [Oversby, 2000].
- -
UO2, ,
, , 500 -
, -
.

[Smith, Johnson, 2000]. -
, - . -
, , -
.
13

13.1. . 20041]. -
-
1000 ,

, , .
-
, -
. , -
, ,

. .
, -
: ,
;
, - . -
-
; .
-
; . -
-
; .
- 60 %, -
; , , -
- [, 1984].
; -
-
. -
- .
- -
,
, .
(), - -
. :
, -
, - (Ca0.5,Na)0.7(Al,Mg,Fe)4(Si,Al)8O20(OH)4nH2O.
,
-
[Brookins, 1984; Chapman, McKinley, 1988; , ,
117

( , -
.), , , , - ( )
, , , .
Fe, Mn, Ti. -
, ,
. .
e 80, , -
, ,
. 75 % - -
, 15 % , 58 % , .
1.4 % , 0.3 % 0.4 % ..-
.
.
- .
(, ,
FEBEX , ) -
-
(), 92 % - . Na2O
c : 2 . %.

(Ca0.49Na0.07K0.11)(Al2.77Fe3+0.33Fe2+0.01MgO0.80) . -
(Si7.82Al0.17)O20(OH)4.
,
(.%): .
92; 2; 2; 2; 90 /100. 80 %
0.35; -0.60; .
0.14; 0.02; 0.13. ,
, 7.37.5. 137Cs 90Sr,

- .
. -
, . -
-
. , -
, - -
, - [ ., 1983].
, -
10131014 /, , , , , -
, ,
, - , (,
1016 / [Conca et al., 1993]. , .).
, , -
,
. . -
-
. -

- .
.
1001001 - , -
. - .
, -
,
, - ,
-
, , -
. .

. :
118 13


;

;

;

;
-
;
,

.
-
FEBEX (Fullscale . 13.1.
Engineered Barrier Experiment), - [ ., 19982].
in situ - 1 ; 2
CIEMAT ; 3
. ; 4 ; 5 .
2.28 -
70 53 (70 ) -

1.7 /3 115.7 .
14 %. -
4.54
0.90 .
1.02 . , -
,
69 . ,
620 ,
,
, . -

, ,
.
. 13.2.
- [ ., 20031].
, - 1 ; 2 ;
, 3 ; 4 ; 5
- ; 6 .
.
-
.
-
,
.

13.2.


,
,

. . 13.3.
, - ,
(. 13.1, 13.2, 13.3). [NAGRA, 1994].
119

, -
, ,
- .
. , ,
, . , -
, . -
, ,
, .

. , , , -
, ( ,
. - .) , -
, , -
1000 [Andrews et al.,
1986]. .
. - , -
- 80,
-
,
, , -
. , - [NAGRA, 1994]. . 13.1 -
, -
. ,
15 . % 85 . % - .
- ,
51011 /, - .

[Esaki et al., 1997]. ,
Na+, SO24 , CO3 , F
2

, Ca .
2+

pH -
107 /. - 810 [The scientific..,
1995]. Eh -
. , - -
, ,
. -
- Eh.
0.3 1.3 , - -
. .

13.1. , 80 [NAGRA, 1994]

, M/ , M/
T C 50 50
8.97 8.49
Eh, mV 396 367
Na+ 78 240
K+ 0.17 0.57
Ca2+ 0.011 0.055
Mg2+ 0.067 0.48
HCO3 52 18
Cl 3 187
F- 0.70 0.19
SO42 4.5 16
Al3+ 0.1 0.036
Si 0.26 0.19
120 13

13.3.

-

-
. -
,
-

.
,
.
-
. 13.4.
, 50 %
.
- [Kurosawa et al., 1997].
. - 1.8 /3. ,
. . ,
,
- .
-
.
, - . -
[Kurosawa et al., ,
1997].
. -
. - , -
30, 40 50 . %, 0.921.18 .
50 .
5 .
1000 1800 /3. Pu, Am Np -
-
0.5 NaCl, 10 8106 /,
. - Tc 10 710 5 /.
1550 . ,
135
Cs, 14 129I, .
,
. -
- .

0.5 NaCl. . -
135 . - , -
NaCl - ,
. - ,
, -
. (Kd) -
, 1000 /, Cs, Tc
50 . % 1000 /3 /. , -
. -
, 40 . % [NAGRA,
, . 1994], -
, , -
, - ,
(. 13.4).
, (Kd, /): Pu 5000, Am 5000, Np 5000, Tc 100,
Cs 10.
121

- 10000
,
- .
. 79Se, 135Cs. 99Tc
- 300000
, [NAGRA, 1994].
, -
. 238Pu 135Cs,
, 1 /3, 103 ,
90 , - .
, -
10 7 / Pu, -
375 3 (14C, 36Cl, 129I),
1010 / [Tsukamoto et al., 1995]. - .
, -
1012/ 15 . -
- -
1000 , 55 10000 . : 14C,
, 135
Cs, 129I, 36CI, 79Se [Luhmann et al., 2000]. -
- ,
, . ,
, 10000 .
-
,
1 229Th, 241, 243Am 239, 240Pu - ()
, 30 - .
[Torstenfelt et al., ,
1982]. K d 2000 /,
. [Nowak, 1980] , , - .
237Np -
30 : , -
10000100000 , -
. . - ; , -
[Nilsson et al., 1993]
- . -
, , -
, - .
. , - -
239Pu 243Am, ,
, , - ,
. .
- .

.
-
Kd 13.4.
, -
, h,
. .
, , -
, , ,
- -
- 1000 .
-
. , -
, - .
, , -
- , . -
, ,
122 13

,
, - :
. ,
, ;
- ;
(. 13.5). -
3050 ;
. -
-
. - .
, , -
.
- .
. -

, 13.4.1.
-
. -
- -
90100 , ,
130 . . -
- .
250 . ,
-
. , - , .
, , -
-
. .
250 , -
[- ,
., 20011]. , .
, - 2000 -
110 [Selvadurai,
. Onofrei, 1993]. -

2 /3.
70 ,
-
90 62 . -
30 %,
10 %.
3.2 %. -
.
,
-
1.83 /3 [Pusch,
Karnland, 1993]. 10
-
80 , 32 . -
7.5% 19 %.
-
,
-
, . ,

. 13.5.
1.5, 9 40

[NAGRA, 1994]. .
1 ; 2 ; 3 -
; 4 . .
123

20 130
,

1.78 /3 1.96 /3 - 300 ,
1012 1011.8/ 1012.8 1012.0/ 300
[Nilsson et al., 1993]. , - [Hemley et al., 1961]. -
, , -
20 80 .
[Cho et al., 1998]. - , -
, - , , -
- 200 .
.
-
, -
13.4.2. , .
-
-
- .

. - . -
. - -
-
, , .
. ,

200 , 13.4.3.
-
[Deer et al., 1962]. ,
- . -
,
, , .
370 340 , : ,
[Allen et al., 1984]. , -
440 - . -
. ,
, - . -
250 ,
- . -
. - :
K11.5Al4[Si76.5Al11.5O20](OH)4. -
. - ,
Na , -
Ca Mg, , -
[Chapman, Savage, 1984]. .
53 , ,
,
100 . 140 - , . -
- -
,
[FuentesCantillana et al.,
1998]. , . , -
- ,
. -
. .
, pH, -
, -
[Allen, Wood, 1988]. ,
, - -
. -
. . ,
124 13

,
300500 (,
) -
,
. ,
-
-
.
-
.
-
,

.

. - . 13.6. ,

[Eberl, 1978]. 270 [Pytte, 1982].
350 , Na, CaMg +, ,
- , -
27 /.
1:10:30 [Roberson, Lahann, 1981]. -
,

(, - .
) , -
. -
- NAGRA [1994]
. - .
, 16501750 /3. -
- , -
300 341, - , 1016 /. ,
[Allen, Wood, -
1988]. , 150 ,
379 , 50 100 (. 13.5). -
, -
, -
65 % . - .
, , -
300 -
, , . , ,
, ,
, -
- (4.28.5 /)
. .
, - -
K+/Na+ -
,
1 .
[Pytte, 1982]. -
90 10 . - , -
10 % , 10 90 %.
150 , -
10 100 . , 210 30 . -
1000 (. 13.6).
, . , -
50
, -
, -
. [Perry, Hower, 1970].
125

, -
, .
,
200 . ,
. , -
- , , (). -

, ,
. [, 19782]. -
-
. ,
- .
. - -

, , 110
, -
- .
[ ., 1982; -
., 1984]. - 110 -
, - . ,
, - , -
, (, ),
. , .
, , -
, -
- .
.
- .
-
- 150
, [Pusch, Karnland,
. , 1988].
110 . 0.3
500 .
: - 110120 ,
,
55 % , , 25 % . -
7080 % , - ,
. , -
110130 , - (. 13.6). ,
230 .
,
- . -
-
. ,
, - .
, - -
, -
, - [Brusewitz, 1986].
- 100 -
.
- 10 , 5070 %.
, 2
, - , -
.
. , -
-
5070 % - ,
. .
126 13


,
- , -
. 36 , - :
,
1 . - 2Fe + 3H2O Fe2O3 + 3H2.

, , , -
, 250 :

4Fe + 3H2O2 2Fe2O3 + 3H2.
. -
-
100 - ,
100200 . - 2 , , -
, , , .
, -
. , -
, - .
-
- .
, - , -
. ,
, -
. ,
-
13.5. , , pH -
.

120 20 , 70
[ ., 1996]. ,
- -
,
.
() [ ., ,
20011 ].
- , -
. .
- -
- -
. - [Fe3(P2O8)8H2O],
.
, ,
- .
. - -
,
. -
, -
, (Np, Tc, Se).
-
, -
. ,
- .
, - , -
,
[ ., . , -
2003 1]. -
- -
( ) . -
, .
127

, ,
Na2B4O7.4H2O. .
- , -
- ,
, - . -
. , -
, ,
, .
. , , -
1 % -
, .
. -
,
. - , , , -
, . -
, . -
. ,
, -
. .
,
.
,
. - .
- ,
-
- ,
,
[Omelianenko et al., 1995]. . -
, ,
- , -
- -
. .
- /. -
,
, , . -
. , . . . -
,
,
-
. . -
,
- . ,
-
. , ,
.
,
, -
13.6. .

,
() . -
, - , -

- , ,
, -
. , .

, - , -
.
128 13

, -
. , -
,
- .
. -

. -
, - , -
. -

-
,
. .
14

- -
() , -
,
- . -
(). (U),
- ( Np, Pu, Am, Cm), -
. ,
( ) - ( ),
- . -
30 . 3 - 25 -
500 [, 2003]. , . -
, - ,
, 380 . 3 - , -
1 [Ewing, (Pu) -
2001]. , .
, , - (),
- ,
, [- -
, 1996]. . [Polyakov et al,
() 2000; Pyrochemical separations, 2004]. -
,
- ,
. - -
waste [ ., 1996; .,
form . 2003; Actinide and, 2001]. -
, - -
, -
, - .
()
. . -
-
,
. (), ( ),
50 ,
- . [Vance, Agraval, 1982; Fielding, White, 1987;
Lutze, Ewing, 1995; Burakov et al., 1999; Vance et al.,
U Pu ( ). 2000; ., 2002; , 2003].
130 14

,
- 14.1.
[Ebbinghaus et al., 1998 1; 1998 2; Ewing et al.,
2004; Strachan et al., 2005].

[Hench et al., 1984; Fielding,
White, 1987; Sombret, 1987; Stefanovsky et al.,
2004 .], [Hench et al., 1984; Radioactive Waste, 1988; Lutze,
. Ewing, 1995; ., 19982; Strachan et al.,
(Materials 1998; Stefanovsky et al., 2004; .]. -
Research Society) 30 - (),
- (), (),
. - / -
(/) -
. (),
() .
1988 . Radioactive Waste . 14.1.
Forms for the Future.
, .
( -
) . , ,
- -
, . -
. 16001700 ,
, 2500 .
- , ( ,
- ) , -
- , ,
(Review of Excess .
Weapons Plutonium Disposition. LLNL Contract Work , -
in Russia), . [ ., 2000].
19992003 .
() .
10 . - -
- , -
. , -
.
. .
-
. -
.
600800
, () -
- SiO2
, ( ) . -
( ). - ( 30 -
) 535 . %
.

14.1.


, , ,
, (
( , ), / ,
), , , -,
, , ,
,
. .
131

3050 . % -
[Radioactive Waste, 1988; Gong, Lutze, [, 1994]. -
2003]. 750780 1 .
10 % [Yamazaki, Inoue, 1995], (Cs)
[Russo et al., 1997], - [ ., 2005]. -
(Hayward, 1988). -
900 , , , -
750 - (CsAlSi2O6).
.
, -
, - .
(Ru, Mo, Cs, Tc), -
.
, , - .
,
, . .
-
-
. 14.1.1.
.
- -
. -

( ) (8501150 ). -
, -
( ). - [Hench et al, 1984]. -
- ,
[Ringwood, 1985; .
Ringwood et al., 1988]. - , , -
- , -
10 , -
- [Sombret,
. 1987; ., 20022]. -
100
. 500
, . -
. , -
6 3 . -
300400 , 14.4.
50 100
[Ebbinghaus et al., 19981].
- 14.1.2.
. /
, -
() - -
.
.
, - . -
,
-
. ( - [Sombret, 1987; Jouan et al., 1991],
. -
),
. , -
, -
. 13001400 .

() -
[Komarneni, Roy, 1981]. ( ,
132 14

) - [ ., 2002].

18002500 [ ., 1973]. -
- 23 . -

, Pu [Kushnikov et al., 700 . -
1997; ., 1997; Matyunin, 2000; -
, , 2002]. . .
, - -
. 30 950
, - 1200 -
. . ,
. - ,
, - 34.
. 80 %
. 300 -
. 350 -
, 30 45
2500. - .

, , -
. -
[ ., ,
1987; Sobolev et al., 1995; ., 1996], 0.05 . % Pu [Molokhov et al., 2000].
[ ., 1998],
-
[ ., 2001; 14.1.4.
Demine et al., 2001; Stefanovsky et al., 2001].

, -
60160 .
- [Ringwood, 1985]. -
, , Ti, Zr Al, Ca Ba.
SiC. ,
258070 20 . %.
- -
. 330 - 650750
75 - (3.5 % H2/N2). 2 %
. : -
- ( ) -
2025 . %, - 12 11501200
1421 .
, 40 60 -
. 60 .
- 45 .
[Jouan et al., 1999]. ,
, 98 % -
. 3
14.1.3.
.
10
- .
,
(2375 MHz). , - 400 .
515 ,
8501100 [ ., 2002]. -
, - 14.1.5.

. - , -
.
133

-
, - -


. . -
, - . -
, , - -
, 1020 , , ,
13001400 46 . [ ., 2004].
,
. 2,
Ca, Zr Ti
, .
. - REE 2(Zr,U) 2O 7, CaZr 0.25U 0.75Ti 2O 7 CaUTi 2O 7, -
. 10001550 . -
, 10 . % -
[Ebbinghaus et al., 1998 1; 1998 2]. 10001100 , 100200
300400 , -
( 6 2.5 ) - [Stefanovsky et al., 2002]. -
50 . 20 (1550 )
8 50 . 36
28 2040
60 3 . .
,
-
. 14.1.6.
.
1700
50 .
- -
, . -
-
.
.
(CaZrTi 2O 7), (Gd 2Ti Zr 2O 7, CaCeTi 2O 7) (3 Fe2O3), -
(Ca1,5GdCe0,5ZrFe4O12, Ca2,5Ce0,5Zr2Fe3O12). (TiO 2, ZrO 2, REE 2O 3)
2030 . (Ti, Zr, Al .). -
8001600 - ,
0.550 . - .
-
. ,
- 17002500 .
- .
. -
, , -
[ ., , ,
2002 1 ; ., 2002 2 ; Ioudintseva, Chae, .
2004]. , ,
, , : -
(Ca,Gd,U,Pu) 2 (Hf,Ti) 2 O 7 , ; -
. - ; -

. .
, ()
CsAlSi2O6 [ ., 2005], -
. - (Y,Gd,Zr,U)O2x,
, - Y 2(Ti,Mo) 2O 7 [ ., 2001]
, (REE)3(Al,Ga)5O12, REE = Gd, Sm Nd
. [Yudintsev et al., 20041 .].
134 14

(Materials Characterization Center)


14.2.
[Nuclear, 1983]. 1
,
.
5 100 1,
- 10 1.
. 1 12 , -
1820.
-
. ( 728 ) 7090 .
. - 1, 3, 7, 14, 28, 56 91 . -
-
, (). -
, - 2 12 .
, . 2 150200
- -
, . 3
,
. - , -
, .
, <45 75100 .
. - 1020 . -
, - , -
. (S/V)
- 300 20000 1, -
1 .
, - 90 7,
, . - 15 28 . , -
(, , 7
, , .). 25 6 8 [Characterisation of, 1997].
-
.
14.2.1. -
.

. (product consistency test, PCT),
, [Chamberlain et al., 1998].
7 -
.
90 S/V = 2000 1. -
-
. [Strachan et al., 1998].
-
75150 ( 100 200 .) -
( ) - 100 800
. - , S/V 10000200001.

( ) . -
. -
- , -
- ,
[Hench, Clark, 1984]. [Strachan et al., 1998; Bakel et al., 2000].
10 [Van Iseghem et al., 1996] -
. - 125250 ,
( - S/V = 100, 1000 100001, -
) 3, 14, 28, 60110. -
. , -
, .
135


.
[Strachan et
al., 1998; Haworth et al., 2003]. -
, -
70260 , (SPFT, single pass flow test).
(S/V = 106 1) 4. -
3, 7, 35 .
, - [Strachan et al,
(Pu Gd) 2005; Icenhower et al, 2000; Icenhower et al, 2006].
-
- 4060 -
. . ,
- (90 2) .
. ()
250 -
[ 521262003]. - 2 12. -
,
, . ,
2590 , - .
100 ( ) - -
1, 3, 7, 10, 14, 21, 28 , ,
, . .
1 3 -
10100 2. (NLi) : NLi = (Ci Co)/[fi(S/V)t],
. (Ci Co) -
( /3), fi
137Cs 90Sr - ( 1),
102 /(2), Pu S (2), V (3),
103 /(2) [ 5092696]. t .

- .
: 300700 , -
( 50 ) , - : Ri = ai/(Ai Stn), ai
[Ringwood, 1985; Malmstrom et al., 1999, 2000; , ; Ai -
Giere et al., 2001]. ; S -
, - tn
. [ 521262003]. -

- .
. 4 - -
0.110 , [Wicks,
3864 , S/V = 10 1, 2000]. -
2590 [McGlinn et al., 1995; , -
Icenhower et al., 2000]. - .
. ( ) -
, . .
- -
.
, -
. (drip) , -
, - [Ojovan et al., 2004].
[Fortner,
Bates, 1996].
() - 14.2.2.
J13 90 , -
0.025 , -
. -
, .
136 14

[Weber,
1500
1991; Ewing et al., 1995; Weber et al., 1986; Weber et al., , D
1997; Lumpkin, 2001; Weber, Ewing, 2002]. - , M
(U,Th) - , Nf , N
. [Lumpkin, Ewing, 1988]. -
,
[Ziegler et al., 1985].
, - -
.
, , , .
. U Th -
.%, -
-
. - 238U 232Th, -
- 238Pu,
. , .
, , , ,
,
. - [Ewing et al., 1995].
- -
, . - -
.
(. 14.2).
- , , , -
238Pu, 241Am, 244Cm 242Cm , ,
88, 433, 18 163
[ 500892003]. - [Radioactive Waste, 1988; 5092696].

, -
-
. , 14.3.

(Ne, Ar, Kr, Xe) Cs, Pb, Au.
, . -
: , - -
.
in situ -
, - . -
,
. ,
- , ,
, , .

. 1 ./
, 14.3.1.
.
SiO4
4 PO4 ,
3

: 1500(DM)/(NfNA),

14.2.

1. U-Th , , , , ,
, .
2. (ZrO2), (* ),
, (Zr- ) .
3. ... ,
.
* NaZr2(PO4)3.
137

. - P2O5,
B3+, Al3+ Fe3+, : Na 2O, Al 2O 3,
, , Fe2O3, PbO, B2O3 . -
. - ,
.
AlSi - (. 14.3).
1950 [Radioactive Waste, , -
1988]. 6585 . % P2O5V2O3Sb2O3 -
3515 . % (). ,
AgIAg2OP2O5 ,
1000. 129I [Fujihara et al., 1999].
-
(1350 ),
(Cs, Ru) - 1987 . NaAlP -
. .
- -
. , -
, - -
, [ ,
. 1997; ., 20021]. -
(9001100 )
- -
. 1960 , ,
25 . 2427.% Na2O,
. 2024 . % Al2O3 5052 . % P2O5.
-
, , 10 % -
. 45 . %.
, .
, , , .%:
, - 21.426.8 Na 2O; 12.519.8 Al 2O 3; 49.856.6 P 2O 5;
. 0.52.7 Fe 2 O 3 ; 0.12.0 NiO; 0.050.8 Cr 2 O 3 ;
0.13.0 ; 0.0030.04 PuO2 [ ., 2003].
500 -
11500 3
[Sombret, 1987; Radioactive Waste, 1988; 2000 284 [,
, 1997]. - , 2002]. -
(900950 ), - 3000 -
360 [, 2005].
, -
.
- . 10 . %
. 0.30.8 . % [,

14.3.

, - - - -
. %

Na2O 2427 2227
PbO 3253 3760
Al2O3 2024 0.13 - - 12
Fe2O3 13 0.58 2540 620 710*
P 2O 5 5052 4452 4050 3242 3343
B 2O 3 612
45 10 35 67 1520
* , .
138 14

2000]. NaAlP , 150 -


, ( . %) Na Cs 3 ,
1.51.7 % La; 2.02.2 % Ce; 2.52.7 % Sr 100
Nd 3.53.7 % Sm. [, ,
, 1987; ., 1990; , 2001].
-
. - [-
, 1997].
. , ,
. NaCaCl
[ ., , -
1994; Kushnikov et al, 1997]. ( )
, , 2 -
(Cr,Fe)2O3, - [Gupalo et al., 2001].
. NaAlP
- (Cs, Sr)
( ) - [ ., 1996; ., 1997].
. Ru, Rh, Pd ( . %): P2O5 49.3, Al2O3 21.2,
- Na 2O 21.0, Cs 2O 2.6, K 2O 1.8, SrO 1.5,
[ , 1997; , 2003]. FeO 1.3, CaO 0.7, SiO2 0.4, MgO 0.1 -
.. (). -
PdRh , RuO 2, Rh 2O 3 (Rh,Cr) 2O 3, 70250
- .
. , - 24 1 ( -
, 25 ).
,
. . 1 -
-
500, 2050.% . 2 -
[, 2001; ,
, 2002]. (Sr,Ca)(Al,Fe)3(PO4)2(OH)5H2O ()
NaAlP lCa lPFeSr (. 14.1). -
10 10 Sr -
- . -
21024 ./3. .
, , 112
10000 [ , 1997]. 70 , (120 ) -
- 170 . 16 120
, 20 , 4
, . 2535 ,
, .
. - 2
[Sun et al., 2004] , 4 250 ,
100 45 .
, -
. - .
s, Sr, -
. . -
Na, Cs, Sr Pu -
20 (0.53)102 /(2) : Na > Cs > Al > Sr.
- Cs
21 [ , 1997]. 12 .
, Sr , -
Na Cs -
.
, Fe Al.
Cr, Ti, Ce, Ni, Ca, 90250 20 [, 2001].
Mn, Co Mo 13 . % -
. Na Cs, Sr
139

. 14.1. NaAlP () NaBSi () ;


[ ., 1996]; [Glass as, 1996].

, , -
. ,
- Na3Al2(PO4)3.
, - -
. - -
. , ,
. Na3Al2(PO4)3 AlPO4 -
[ , ,
1997]. -
Na2OSrOCs2OAl2O3P2O5 30 [ , 1997].
(Na,Cs) 3PO 4, (Na,Cs)PO 3, AlPO 4 Sr 3(PO 4) 2 -
[ . 1994; , 2001]. - .
500 ,
.
, 500, .

. 14.2. NaAlP (), ().


; (), .
.
140 14

14.4. , ( /)

, . %
Na2O 24.0 25.5
Al2O3 17.2 19.3
P 2O 5 47.8 51.3 27.9
Cr2O3 0.4 0.2
Fe2O3 0.3 0.5
SrO 0.8 0.5
ZrO2 2.9
MoO3 1.4 0.4
Cs2O 0.5 0.5 0.6
BaO 0.8 0.7 0.4
La2O3 5.6
Ce2O3 2.0 0.4 56.3
Nd2O3 0.5 0.2 10.2
. .

(Na,K)3(Al,Fe)2(PO4)3, 70100 . -
-
(. 14.2). - , -
. - -
150 450 .
: Na3Al2(PO4)3, Na3PO4, AlPO4 NaPO3, NaAlP
(Fe,Cr)2O3 (Al,Cr)2O3 [, 2003]. . -
400 [-
, 1997]. 102 /(2),
, [, 1997],
, - [Demin et al., 1995] 24 .
. -
, , , , [Radioactive
, . Waste, 1988]. -
(. 14.3 . NaAlP
), . ,
- , . -
,
(. 14.4). ( ) ,
, NaAlP - . -
400450 . -
-
. , -
, .
100 - -
, - , .
.
. .
, ( . %): 24.0 Na2O; 18.3 Al2O3; 3.9 B2O3;
- 50.0 P2O5; 1.4 Fe2O3; 0.3 NiO; 0.1 Cr2O3; 0.5 La2O3;
. , 0.3 Nd2O3; 0.5 CeO2; 0.5 CaO; 0.3 MnO.
- 30 630
- , -
. .
, Na3(Al,Fe)2(PO4)3, NaAl -
(Ce,La,Nd)PO4 [ ., 2003]. -
. , -
( . %): 2227 Na2O;
141

3 Al 2O 3; 812 B 2O 3; 4452 P 2O 5; 8 Fe 2O 3; . FeP


1.5 NiO; 0.8 Cr 2O 3; 5 MnO 2; 3 SiO 2; 35 . % (. . 14.3).
1.5 CaO; 10 UO2; 0.5 PuO2 [Borisov et al., -
2001; ., 20021; , , 2002]. , , -

100500, [Marasinghe et al., 2000].
. ( PCT)
1030 , BSi
. SRL131.
(Ce, Nd) 10 4 /2 -
365 [Haworth et al., 2003].
PbFeP [MogusMilankovich et al., 2001]
( FeP 90 ,
) -
( ). - .
- -
, .
[Radioactive
Waste, 1988]. [Aloy et al., 2004],
POP POFe. , . -
-
. , 40 % -
, - () -
( , - .
) , .
BSi . Na, K, Al P
PbFeP 0.61.8 /(2) (, 90 , 7 ), -
5 9 90 1001000 , - -
. .
102103 /(2)
( 1). -
150 : - -
0.1 (150 ) 5 (190 ) /( 2). [Borisov et al., 2001]. -
PbFeP : 450 - ( -
500 - , )
. .%: 2225 Na 2O;
4748 P2O5; 5.7 Fe2O3; 1.0 Al2O3; 4.5 MnO2; 6.8 UO3;
, 1.0 NiO; 0.8 Cr 2O 3; 710 PbO; 0.3 CaO; 0.3 SiO 2;
- 0.5 PuO2. Pu
. 25
(58)102 /(2), 2
6 . 1530 ,
[ 5092696].
,
-
. , - Si,
, B Na, Li2, iO2, CaO, MgO,
Al2O3, K2O, ZnO, ZrO2 . (. 14.5).
. -
,
, . -
Si, Al Zr -
-
NaAlP . - .
, , , -
- .
. - . Li
, Fe2O3, F, SO3, -
NiO. , Ca, Mg, Ti Zn
142 14

14.5. BSi [Radioactive Waste, 1988]

, ()
. %
AVM SON68 SRL131 SRL165 PNL76-68 GP98/12 SM513 SM539

SiO2 56.1 54.9 58.7 68.0 59.4 58.5 58.6 45.5
B 2O 3 25.3 16.9 14.9 10.0 14.3 11.0 14.7 33.0
Li2O 2.4 5.8 7.0 4.7 4.5
Na2O 18.6 11.9 18.0 13.0 11.3 17.5 6.5 10.5
K 2O
TiO2 1.0 4.5 3.6 5.1
CaO 4.9 2.9 4.5 5.1 6.5
MgO 2.1 1.0 3.3 2.3
Al2O3 5.9 1.6 3.0
ZnO 3.0 7.6
ZrO2 0.5 1.0
La2O3 0.5

Kushnikov et al., 1997; Bart et al., 2001]. -


[Radioactive Waste, 1988; (Ni,Ru)S, PdTe,
Chamberlain et al., 1997]. PdRhTey, (Pd,Rh)O2, TcO2, RuO2 -
- .
,
. - [Demonie, Cuyvers, 1996; , 2003].

. -
- . -
1030 . % (. 14.6). . ,
(), -
- 859 1310 [Hrma et al,
2000].
. : Cr2O3 -
, 1 . % 260 . -
, - NiO 85 ,
, - MgO 33, Al2O3 18.
, - 1 . % 23 (Na2O, Li2O,
, Fe2+/Fe3+ K2O) 829 . -
, BSi -
[Vinjamuri et al., 1999].
( 1 .%).
- , -
. ,
, ,
BSi . ()
. La,
Nd Sm 10 . %, .
Ce , - .
4+.
- , -
, .
.
.
, - [Hench et al., 1984] -
, .%: 5153 % SiO2; 2428 % (Na2O + B2O3);
[Cheron et al., 1995; 2125 % (Al2O3 + Fe2O3 + ).
143

14.6. [Sombret, 1987], . %

,

SiO2 40.0 44.5 48.0 41.8 43.0 40.4 38.1 50.9 38.4
Na2O 13.0 9.9 13.0 22.3 10.2 16.5 17.9 8.3 17.1
K 2O 2.0
B 2O 3 9.6 14.0 18.0 10.5 2.0 7.2 16.4 11.1 17.3
Al2O3 4.9 1.2 3.5 3.1 12.3 5.1 11.0
Fe2O3 10.4 2.9 6.0 0.7 1.0 12.1 4.2 2.7 3.2
MgO 0.4 4.1 6.3 5.1
CaO 2.0 4.0 2.3 2.0 4.5
NiO+Cr2O3 0.6 0.8 0.5 0.5 0.3 1.5 1.0 0.9 0.8
TiO2 3,5 7,2
Li2O 2.0 3.0 2.9 4.0
MnO2 3.4
F 2.0 1.4
BaO 1.0
ZnO 5.0 2.5 2.0 0.4
ZrO2 1.0
0.5 1.3 0.3
(+)* 15.9 12.2 13.5 16.8 19.0 1.2 4.0 9.6 5.6
*

Fe, Mn, Al, Ca, Ni - , -


. ,
- (, ). , -
0.2 /( 2 ) (1, ,
S/V = 10 1 , 90 , 28 ). 10000
(14 ) [Radioactive Waste,
(S/V = 1000 1) - 1988; Gin, Frugier, 2003].
(14)10 3 /( 2 ). -
13 /(2) +, -
(50 /). .
- -
- ( -
10 [Ebert et al., 2000]. )
Tc, B, . -
Na, Li, Mo Si, Ca, Zn, Sr, Mn, Ni, -
Fe, Al, Zr, REE, . - .
10 1 (237Np, 241Am) , -
103 /(2) (Pu). - . -
25 75 , 0.82 /3, 2.5 /3.
3103 /(2) [Marples, 1996]. -
, -
, -
[Grambow et al., Al, Si, REE, Zr [Radioactive Waste, 1988;
1995]. Abdelouas et al., 1995]. ,
4 10.
, , (, ),
. = 2 - .
38 . - .

. .
144 14

- 1020 (70
- 70 ).
, -

. -
-
- . ,
. - , -
.. [Sombret, 1987; Radioactive Waste, 1988;
: 10 2110 22 2/ B, Ewing et al., 1995; Abdelouas et al., 1995].
Na, Li 90 40 -
[Aertsens et al., 2003]. . 3
( ) SON68,
. : Na (0.1 . %),
, B(0.038%) Si (0.013%),
- 1 ,
. (. 14.7).
, , , BSi (
- WV6) 182 -
- 90
[Buck et al., 2000]. -
.
200
- West Valley, .
SON68, [Glass as, (20100 ) ,
1996; Gong et al., 1996]. - . 100200
. - ,
0.5 22 26 . -
(1013 ), 6 .
1 (- .
, , ), ,
. BSi -
CaSi
1030 (. . 14.1). 2 - [Radioactive Waste, 1988).
(Na), -
, 3 (, ), , ,
. 4 5 (). -
, 5 -
, . . -
- 0.1 -
. 35 , , 1000 ,
Zr, Fe, Zn, Cr Ni, Ag2TeO3 (Ca,Sr) ,
Mo3O9(OH)2. 6 - -
. .
1.5 /2 , 3
3104 /(2) - 100 .
600 [Gin, 2001]. -
, [Hench et al., 1984].
, . BSi
, Np, Pu, Am Cm, , ,
80 % , - . -
, (Cu, Sn, Ti), (Al, Pb)
, - (Fe) -
10 % [Fortner et al., 1997; Inagaki et al., .
1997]. - , , ,

0.10.3 mm. SON68 , .
SRL131 SRL202U,
,
145

14.7. , Na, B Si. = 4.8, = 90 ,


V = 0.6 [Ferrand et al., 2004], . %.

Si Al Na Ca Fe Zn Zr Mo La Nd
49.0 6.0 16.8 6.7 4.7 4.6 4.5 2.6 1.8 3.1
52.6 2.3 6.8 1.0 1.2 0.6 1.7 0.2 3.0 0.2 17.0 4.0 6.9 1.1 5.6 0.9 2.7 0.3 2.6 0.3

25 , 350

0. - -
. . 150
30100 , 300 102105 ,
. , - 50 [Sombret, 1987; Radioactive Waste, 1988].
137Cs 90Sr - 100 600
Ba2+ 20 %, - ,
Y 3+ Zr4+ 0.024
29 % , Sr2+. (125 ) 6.4 (200 )
137Cs 67
. 25 [Ebert et al., 2003].
- 25 % 43
, - 10 250 [Marples,
1996]. -
200300 . 90250 [Hench, Clark,
. 1984].
400 , 100 80
0.85 . % 100, . -
1000 10000 0.7, 27 45 . -

BSi .
12 % [Weber,
1991; Weber et al., 1997]. - -
, - .

. ,
, -
300 / ( 80130) , . -
() (13)10 18 ./.
7 100 . -
90 % -
, . NaSrREE (); Ce2; ZnFeNiMnCr
, (); (), . [Ra-
, - dioactive Waste, 1988; Glass as, 1996; Bart et al.,
. 238Pu 2001; Rose et al., 2004]. 8
244Cm 600650 -
25 % 30 % [Weber, 1991]. 20 . % [Vienna et al., 1997], 570
31018 ./, , 550
( ) ( ) .
, ,
24 , , -
, 450 . SON68 21
[Matzke, van Geel, 1996; Weber et al., 2003; Peuget et 761 6 . % -
al., 2004]. , 586
71 [Radioactive Waste, 1988].
, ,
46 . ,
- PdTe (Ru,Rh)O2 [Cheron et al., 1995].
, 30 510
. , 780 4
146 14

3 6 . % CaMoO4,
, CeO2 (Ni,Fe)(Cr,Fe)2O4. Ca, Na, Cr Fe
, Si Mg . -
- 40
. 5 400 .
-
300 4 [Ringwood, 1985]. , Np, Pu Am,
, BSi - RALUS [Glass as,
- 1996; Van Iseghem et al., 1998; Valcke et al., 2004;
NaAlP . 2005]. 0.85 % 237NpO2,
, 35 238242
PuO2 241Am2O3
[Kawamura, Ohuchi, 1995]. () -
223 1.3 10.
- () 4 0.3
50 ,
. - SON68 . R7T7 -
- -
, . -
. ,
30 90 ,
- 60Co.
[Wicks, 2000]. - ,
- 2 MPa. :
. ( A), Ca -
1950 60 % 35 % 5 % (B),
, - 95 % Ca 5 %
[Radioactive SON68 (C). () ()
Waste, 1988]. (. %): 50.7 SiO2; -
19.9 Al2O3; 15.5 CaO; 8.9 Na2O; 3.9 K2O; 0.6 Fe2O3; , () .
0.2 UO2; 0.1 Cr2O3; 0.1 NiO; 0.1 MgO - ,
(137Cs, 90Sr, 144Ce, 106Ru). . -
, 2004 .,
. - 2009 2014 .
- , 90
60 . (
( - ) ,
), 7.512.5 ( ).
, 6 . 68 5595 0.30.8
1.3 . 30 :
106 /(2), 15 - 1 , 0.3
5107 /(2). 34 .
-
4 . -
25 . 30 (0.81/) -
20 , ,
.
- 90 (3058 /).
Ca, Na K -
.

14.8. / ( H, B O)

Na Mg Al Si K Ca Fe
. 1 10.3 1.0 2.9 25.5 0.9 13.5 3.5 57.6
. 2 1.3 1.0 7.8 29.4 0.3 6.6 7.3 53.7
. 3 0.9 1.0 7.9 29.5 0.3 6.0 8.0 53.6

. . 14.4.
147

. 14.4. , .
, (. 14.8); .
. 100 () 10 ().


-

[Ojovan et al., 2004]. -
( ): Si, Ca, Na, B, Fe,
Al, Mg. - , .
.
1015 . % , , .
. ,
10
. ()
. 14.8. -
(. 14.4) , - , ATS [Bates et al., 1996;
( 1) Chamberlain et al., 1997] ,
30 , LaBS [Bibler et al., 1996; Mesko et al., 1997]
. , , (. 14.9). 7 . %
, PuO 2 , -
5 - -
. .
. 2 3 - ATS ,
, (1100 ), LaBS 300 .
,
, , -
, . , [Gould et al., 1998; Marshall et al., 1998]
, . - [Matyunin et al., 2000] . -
, , Pu, , -
, 40 % 60 %
[Matyunin, 2000; 2001].
, - ATS ,
, , [Lutze, 1988; Abdelouas et al.,
1995; Buck et al., 2000; Aertsens et al., 2003; Gin, 103/2( , , 398).
Frugier, 2003]. LaBS -
, 50 -
AlP BSi BSi .
, -

. Ln2SiO5 [Fortner et al., 2000]. -
-
. ,
- , -
[Matyunin et al., 1995; Kushnikov et al., 1997], . -
. %. (Sr, Cs)
148 14

14.9. Pu , . %

ATS1 LaBS2 LaBS3 LaBS4 BBS ()5 BBS ()6


SiO2 41.4 34.6 17.4 24.3 29.0 33.7
B 2O 3 12.0 5.1 9.9 9.7 28.0 22.2
Al2O3 2.3 9.0 17.8 17.9 8.1 9.6
ZrO2 5.3 0.1 0.8 5.5 (HfO2)
La2O3 9.3 6.8 Fe2O3 5.7 Fe2O3 5.7
Ce2O3
Nd2O3 Ln2O3 = 30.0 6.9 MgO 4.7 MgO 2.9
Sm2O3 18.4
Gd2O3 3.2 10.8 CaO 16.6 CaO 14.4
SrO/BaO /3.8 3.6/ 2.1/
AnO2 11.4 (Pu) 6.9 (Pu) 20.0 (Th) 10.0 (Pu) 5.0 (Pu) 4.0 (Pu)
PbO 13.0
Li2O 4.0
Na2O 9.2 1.9 5.7
K 2O 5.2 0.5 0.9
Cs2O 0.7
TiO2 2.0 0.5 0.9
SnO2 2.5
UO3 3.0
3.0
99.2 100.2 99.5 100.0 99.5 99.5
. 1 Bates et al., 1996; 2 Bibler et al., 1996; 3 Mesko et al., 1997; 4 Strachan et al., 1998; 56





, -

[Matyunin, 2000; 2001].

Pu , -

. 5 . % 239Pu ,
35 , -
. , , -
, - , . [Radioactive Waste, 1988;
. Vance, Day et al., 1996; ., 1997; -
(Am,Cm) - ., 2002].

-
, , .
. -
25SrABS
(33.7 % SiO2, 25 % La2O3, 24.9 % Al2O3, 13.5 % B2O3, 14.3.2.
2.9 % SrO) 20 50 % -
. -
1153 1405 , -
( - ,
<43 . %) ().
[Riley et al., 2000]. , , -
, ATS LaBS , , , , , , ,
, BSi , (. 14.10).
[Peeler et al, , -
1998]. , -
, - , , , -
. [Sombret, 1987; Radioactive Waste, 1988].
[Strachan et al., 1998].
, - .
. (-
). 10
149

50 . %. - 13001400 ,
- 0.51 700 48
. - 900950 . -
. (Ca,Mg,Fe)2Si2O6, (Ca,Sr)
MoO4, (Ni,Fe,Mn)(Fe,Al,Cr)2O4.
( 1, 28 )
0.1 ( Na) 4102 (Si, Cs, Sr, Ba)
[Radioactive Waste, 2103 /(2) (Al). -
1988].
20% 11751250, - .
3 600650 - 3050 % 7050 % Si, Al, Fe, Ca, Mg,
1015 800850 Ti, Na K 14001500 -
. BaAl2Si2O8, - 10001100
(REE2Ti2O7), 1624 . ,
(BaMoO4) - , , , , -
(CsAlSi2O6), 50% , .
(. 14.10). - ZrO2
BSi , - CaZrTi2O7. 1 1500
. , 137Cs
1/(2) Mo, B, 0.3.%. (
Li 0.2 /(2) Si Ba (1). 1) 102 /(2), ,
2018 ./ 2.5 . % 238Pu .
. (CaMgSi2O6) -
1300 . 1 1100
(Ba2TiSi2O8), (BaFe2Ti6O16), -
. - , Fe3O4, CaMoO4 -
12 , . Cs Sr (1)
[Hayward, 1988]. 4101 /(2).


- (CaTiSiO 5) -

[Conley et al., 1984; Radioactive Waste, CANDU ()
1988]. 20 % [Radioactive Waste, 1988].

14.10. . [Sombret, 1987; Hayward, 1988]

, .% ( - ( . )
)
SiO2 47.5 30.0 40.0 2838 2228 4160
Al2O3 6.8 10.0 6.5 1013 02 1424
B 2O 3 5.0 3.5 27 03 411
Fe2O3 9.5 03 (PbO)
TiO2 2.7 10.0 10.0 34 1423 58
CaO 6.8 25.0 10.0 06 04 29
BaO 6.8 (MgO) 1316 2836 05
ZnO 35 06 413
Li2O 13 510
Na2O 02 03
20.0 20.0 30.0 20.0 20.0 20.0


(CaMoO4) 4
(CaMoO4) (CaMoO4) 4
Zn-Li-

150 14

-
. CaMoO 4,
.
.
, , , - , BSi ,
. -
.
- (Na, Cs, Sr, Ba, Mo)
. 101102 /(2) (1, 91 , , 100 ).
- -
, , , .
Na2OAl2O3CaOSiO2TiO2
, 10 . %
, -
[Hayward, 1988; Hawthorne et al., [Radioactive Waste, 1988].
1991; ., 1998].
.
(. %):
4.69.5 Na 2 O; 3.17.1 Al 2 O 3 ; 10.720.5 CaO;
10.722.1 TiO2; 49.663.9 SiO2. - -
()
(. %): 6.6 Na2O; 5.1 Al2O3; 16.5 CaO; 14.8 TiO2; (Na,Ca,REE) 10 (SiO 4 ) 6 O 2 .
57.0 SiO 2 . 13001400 , -
. - -
- . -
. (.14.5),
2050 . %. -
. -
9501050 - [Zhao et al., 2001] -
40 % , -
(. 14.5). [ ., 2000].
(Pd, Rh, Ru) - ,
.
REE Ni (
2 10), Cs () , -
, Sr . ,
. ( 30 . %) -
15 %. (Nd, Ce, La, Pr, Sm)
Ca(REE,Na)4Ti4(Si,Al)2O22, . -
(Ca,Na,REE,U)TiO 3 ,
(Ca,U,REE)2Ti2O7, Ca2REE8(SiO4)6O2,
REEO 2x . .

. 14.5. () ().
. .
151

NaPbP NaBSi , 24
33 . % . -
4075 . %
[Knecht et al., 1998], 2550 . % -
(Ca,REE,An)(Zr,An)(Ti,Al,Fe) 2O 7 - , 1525.% PuO2
- [OHolleran et al., 1997]. ,
, PuO 2 , (70.3 . % SiO 2 , 12.8 % Na 2 O,
. - 6.2 % Li2O, 8.5 % B2O3, 2.1 % CuO), Sm
- Ti 4 10501450 (
, . %: 40.249.7 SiO2; 5.611.0 Al2O3; , ). -
24.325.8CaO; 10.817.5TiO2; 08.2ZrO2; 04.9HfO2; 550700
1.21.3Ln2O3 (Ln = Nd, Ce, Eu, Gd, Yb) 0.91.1Na2O .
[Loiseau et al., 2003]. 10 , -
15501650 . - . -
: 2 810
2 10501200 1.2103 /(2).
. -
1020 % () ,
, -
Al2O3 (CaO+ZrO2+TiO2). - , -
, ,
, [Vance et al., 19962]. ,
, , .
. Na 2 O (25.3 . %),
U3O8(14.3%), Al2O3(13%), Fe2O3(11%), SiO2(10%)
ZrO2 (7.1 %). Ca, Ni, P, Bi, Ce, Mn
25 . %, (F, La, Nd,
- Mo, S, W, B, Cd, Cr, Mg, Cs, K, Pb, Sr, Th) -
1 %.
(. 14.11), - 1350 ,
. . %: 53 % ; 6 % CaO; 9 % Al2O3; 22 %
- SiO 2; 10 % TiO 2
. 19631982 . - ~5 C [Vance et al., 1997]. -
(), - ,
28600 3 3830 3. Sr, (Na Cs)
,

14.11. ( .%) (12), (3) (4), [Sombret,


1987; Radioactive Waste, 1988; Vance et al., 19962] (5) , [Kudinov et al., 2001].

(. %) 1 2 3 4 5
Al2O3 8295 1317 910 1345 4.4
Fe2O3 4450 1133 18.5
SiO2 16 010 4.7
Na2O 13 78 225 28.6
MnO2 1214 02 14.8
NiO 56 23 4.4
Cr2O 13 2.6
ZrO2 2127 27
CaF2 5056
CaO 24 34 02
NO3 25 0.52
B2O3 0.52 34
+ 0.21 0.22 67 1018 22.0 (UO3)
0.52 0.52 02 35
.
152 14

. -
.
0.1 /(2) ( ). - [Actinide and, 2001].
, -
. . , -

(. . 14.11)
,
[Kudinov et al., 2001]. 50% -
(. %): . ,
12.0 UO3; 10.1 Fe2O3; 8.1 MnO2; 2.1 Al2O3; 1.6 NiO; () -
14.6 Na2O; 1.4 Cr2O3; 36.1 SiO2; 7.0 Li2O; 7.0 B2O3. -
90 (Zr,Y,An)O2x, (Am,Pu)2Zr2O7
7 0.1 /(2) (Y,An) 3Al 5O 12,
Na B 0.001 /(2) U Fe [Aloy et al., 2000]. . [, 2000; Raison,
, 3040 . %, Haire, 2001; Fuels and, 2004]. -
Fe(Fe,Cr)2O4,
50 . % , -
UO2 U(Fe,Cr)O4. ( , ,
)
.
[ ., 1987; Kushnikov et al.,
1997; Demine et al., 2001; , , 2002],
. 14.3.3.
( -
) 90 %.
,
,
, - .
, , , . ,
, , - , (Th,U)
,
. .
, -
-
, tailored ceramics,
.
, , 1970 .
-
. [Mc Carthy, 1977; Radioactive
- Waste, 1988], 77 % -
, , , . - 23 % ( ,
, ).
1100 , -
, , , Sr, Zr REE, ,
. , - , .
-
1500 , ,
(Cs, Tc, Ru) [Sombret, 1987]. -
. - ,
, . . -
- , ,
- -
() . -
< 1000 ( . -
) .
, ,
- .
( ) , -
153

10 5 /( 2) ( 1). - 86.%,
, . -
- (),
(, , (. . 14.11), -
). , , -
, ,
1980 . , [Radioactive
- Waste, 1988]. 60.%,
-
, , , . -
. - 70 1040 . -
-
. , ,
.
, - , , , , .
(. 14.12). - ,
,
, SiO2, -
(, , .
).
-
. -
- -
(FeAl2O4), (UO2) .
(Ca,Sr,Cs,REE)(Al,Fe)12O19, -
. - 1970 [Radioactive
, . Waste, 1988]. ,
140 (, ,
1200 . ).

14.12. [Radioactive Waste, 1988]


(An) (Ln) (Zr,Th,U,Ln)O2-x
* CaZrTi2O7
* Ln2Ti2O7
* CaTiO3
(Ca,Mn,Ln,U)2Zr(Fe,Al)4Ti3O16
LnPO4
ZrSiO4
()* (Ca,Sr)(Al,Fe)12O19
* (Ca,Sr)TiO3
* BaAl2Ti6O16
* (Na,Cs)AlSiO4
* (Na0.5Ln0.5TiO3
()* (Na,Cs)0.5Ln0.5Al12O19
* (Na,Cs,Ba)Al2Ti6O16
()* SiO2 > Al2O3, CaO, Na2O, Cs2O
* Mo-Ru-Tc-Pd-Ag-Rh-Ni-Tc
* (Mg,Ni,Fe)(Al,Fe,Cr)2O4
Al2O3
* TiO2
Fe2TiO5
. , .
154 14

. [Ringwood, , Tc, Mo, Ru, Rh, Pd, Te, -


1978; Ringwood et al., 1981] - .
, (Synroc ,
synthetic rock).

, - (. 14.6). -
, (U, Th). -
- .
(, , ) - , . -
( ).
1300 - 10 , 70 . % Ni
1100 30 . % Fe.
2 [Ringwood, 1978].
, . -
,
BSi . 10 .
-
. , - Ti ( -
71.4 % TiO2; 11.0 % CaO; 6.6 % ZrO2; ),
5.6 % BaO 5.4 % Al2O3. FeNi MoSeTePdRuTc .
1200 80 % 20 % - 100 ( 1300 ) -
(. 14.7), -
, 30 % , 30 % - -
, 20 % , 15 % , .
5 % . - -
- , -
, , -
( . %): Fe2O3 3.7, Cr2O3 0.8, NiO 0.3, (. 14.13).
P 2O 5 1.6, U 3O 8 3.3, NpO 2 2.1, PuO 2 0.02, ,
Am2O3+ Cm2O3 0.5, Rb2O 0.9, Cs2O 7.1, SrO 2.6, , Ba Al,
BaO 3.8, Y 2O 3 1.5, La 2O 3 3.6, Ce 2O 3 7.7, [Ringwood,
Pr6O11 + Nd2O3 + Pm2O3 15.0, Eu2O3 + Gd2O3 0.8, 1985]. -
Sm2O3 2.3, ZrO2 12.1, MoO2 12.7, TeO2 1.8, , 57 . %.
Tc 2O 7 3.2, RuO 2 7.3, Rh 2O 3 1.3, PdO 3.6, (80 %), ,
Ag2O 0.2, CdO 0.2. (BaAl2Ti6O16) 20 %.
; (Cs,Ba)(Ti3+,Ti4+)8O16 ,
(CaZrTi 2O 7) , Ti3+. -
; (CaTiO3) , -
, , .

. 14.6. , 1200 .
, , 150 ( , -
, ). ( ,
, , ).
155

defence ()
.
(Fe, Al, Mn,
Ni, Si, Na), : 36.1 % Fe2O3; 28.3 %
Al2O3; 9.9% MnO2; 3.3% U3O8; 2.7% CaO; 4.5% NiO;
0.9 % SiO2; 5.1 % Na2O; 0.9 % Na2SO4 8.9 % -
[Ryerson, 1983].
(16 %), (11 %), (55 %) -
(11 %), 6070 . %
( 1 /3 250 /
). -
-
BSi . -
10501100
1530 .
. 14.7. , , [Vance et al., 19961].
1300 . (2535 %), (1018 %), -
[Stefanovsky et al., 1996]. (510 %), (35 %) (54 %),
, , -
70 . %.
, , -
.

[Ringwood,
1985]. -
: 90 % CaUTi2O7, 5 %
, - Ba(Al,Ti)2Ti6O16, 5% TiO2,
50.%. -
. ,
- -
[Radioactive Waste, 1988]. - . -
, 88 % .
12 % . -
1100 20 (CANDU), -
. ,
5 [Solomah et al., 1986].
60 , 200
- .
1 . CaUTi2O7,
- (Ba,Cs)(Al,Ti)2Ti6O16,
() (Ca,U)(Ti3+,Ti4+)O3 UO2. -
[Hench et al., 1984]. d

14.13. [Ryerson, 1983; Ringwood, 1985; Vance et al., 1995; Buck et al., 1997;
Ebbinghaus et al., 199812; Strachan et al., 2004, 2005]

, - - - -
. %
TiO2 57.0 87.6 18.8 40.6 38.648.4 35.836.8
ZrO2 5.4 3.0 6.6 - 14.419.6 9.610.6 (HfO2)
Al2O3 4.3 - 6.6 (SiO2) 0.9 2.610.9
CaO 8.9 2.2 5.3 9.5 6.510.0 10.0
BaO 4.4 1.1 2.43.4 8.0 (Gd2O3)
20.0 7.0 62.7 50 % 10.419.3 (Pu) 11.9 (PuO2)
6.612.9 (Gd) 23.7 (UO2)
,

()



156 14

14.14. BSi [Radioactive Waste, 1988]

PNL 7678 -
, 11501200 1150 C/1040 Ma
, . % 33 % 10 %
, / 3
2.6 4.3
, /() 1.1 2.1
, , 10
1 6
8.1 10.5
, /() 0.9 0.55
, 100 110
, <100 574
, 82 134
0.22 0.30
, 7.2 8.4
, 1/2
0.97 1.83
, 0.42 0.005
/(2); B/Zr 1.12 (B) <6104 (Zr)
( -1, , 28 , 90 )
Ca 0.068 0.0065
Ba 0.036
Cs 1.03 0.033
Mo 1.40 0.12
Na 1.32 <0.2
Sr 0.075 0.010
Si/Ti 0.73 (Si) <5105 (Ti)

(11 . % UO2) 10000 . -


. 7.5
- 21.5 . % (. 14.15).
2 . % Fe2O3
, ,
[Radioactive Waste, 1988]. - 1% -
( - ,
) . 2 . %
( ) - ,
Cs/Sr, Tc [Vance et al., -
1995; 1998; ., 2003]. , 1020 [Vance, Hartman, 1999].
1 . % SiO2 3 . % Na2O
, 722 ,
, 34 .
, (. 14.13). -
, ,
. , .

(. 14.12). ( 1, 90 , 28 ).
-
. BSi , ,
, (. 14.16). -
(. 14.14). , -
( 30 ) , ( > 8) (pH < 4) -
- ,
(Cs, Sr, Ba, Ca) 95 ,
5001000 , .
[Ringwood, 1985]. - -
(Nd, U, Zr, Ti) ,
157

14.15. . 1,
90 , , 7

(.%)
7.5 13.0 16.3 18.3 21.5
Al <<0.04 <<0.04 <<0.04 <<0.04 <<0.04
Ba 0.091 0.067 0.087 0.018 0.068
Ca 0.030 0.014 0.046 0.053 0.017
Cs 0.105 0.072 0.087 0.093 0.067
Sr 0.030 0.036 0.084 0.037 0.021
Ti <<0.0002 <<0.0002 <<0.0002 <<0.0002 <<0.0002
Zr <<0.002 <<0.002 <<0.002 <<0.002 <<0.002
. /( ).
2

[Van Iseghem et al., 1996]. - , -


. 150
, -
. , 0.2 , -
, 80 %
. 50 % [Smith et al., 1997 1].
- -
. - . 835
10 . %
(1, 90 ) , - (25 , = 4) -
515 ,
0.11 /(2), 1000 [Xu et al., 2003].
84 105 /(2) 2000 . -
-
410 95200 , .
[Ringwood et al., 1988]. - -
, Ca, Cs, Mo, Ba, Sr,
200365 7103104 /(2) , -
[Smith et al., 19971], - [Ringwood et al., 1988].
0.04 . ,
104 . -
103 21055104 /(2), 24 (
, BSi PNL7678. , S/V)
.
. , S/V = 103 104 1 ,
. - (Ba, Sr, Ca, Mo),
, 28 90 ,
, . .
, - S/V. -
(Ti, Zr) -
, -
(SiB NaP). .

14.16. 10 %


0.036 0.016 0.028
0.007 0.007 0.015
Cs 0.022 0.018 0.007
Mo 0.080 0.077 0.040
Sr 0.010 0.006 0.009
. /(2).
158 14

-
(1, 70 , ), -
1.141.3 % 237 Np; 0.620.76 % 239 Pu;
0.0050.007 % 241 Am; 0.00040.91 % 244 Cm
[Ringwood et al., 1988; Mitamura et al., 1994;
Hart et al., 1995; Hart et al., 1999; Jostsons et al.,
1995; Jostsons et al., 1996 2; Matzke, van Geel, 1996;
Smith et al., 1996; Smith et al, 1997 2 ].
239 Pu, 241 Am 244 Cm
310 5510 6 /( 2), 237Np 10
2 -
. 28
70
( /(2)): 105 (Pu), 104 (Gd, Np) 3104 (Ce).
(7 ) -
-
(58)10 6 /( 2), -
Ti, Zr Hf . 14.8. (222)
(12) (34)
[Jostsons et al., 1996 2]. -
,
[Weber et al., 1986; Lumpkin, Ewing, 1988;
0.45 . Lukinykh et al., 2003; ., 20032].

,
. - ( ) -
, . -
. ,
- ( )
. - .
( 90 Sr, 137 Cs) ,
. - -
. 50 250
[Lumpkin et al., 1996; Weber, Ewing, 2002].
. , [Wald, Weber, 1984; Ewing et al.,
1995; Matzke, van Geel, 1996; Burakov et al., 2001;
, 200400 [Weber et al., Weber, Ewing, 2002] , -
1997], -
. 1050 .
() -
(). - ,
-
. -
, ,
, .

(. 14.8).
, ,
, -
, ,
[Lumpkin, Ewing,
1988; Lumpkin et al., 1998 2; ., 2003 2;
Yudintseva, 2005]. -
-
.

. -

. 14.9.
(), - ( ./) .
(. 14.17). 56 88 ; 1MeV Kr2+, 1.5MeV Xe2+
, (. 14.9). . [Utsunomiya et al., 2003].
159

14.17. [Ewing et al., 1995; 2004; Weber,


Ewing, 2002; ., 20032]

, ./ , , ,
( ) ( 25 ) . % /
CaTiO3 () >0.7 250(1)/420(2) >8
CaZrTi2O7 () 0.30.5 >300(1)/640(2) 56 50130
Gd2Ti2O7 () 0.20.4 600 /1000
(1) (2)
5 50130
CaPuTi2O7 () 0.2 600(1) 56 5060
CaUTi2O7 () 0.2 600 (1)
56 5060
(Ca,Gd,U)5(Ti,Mn,Zr,Fe,Al)10O27-x 0.2 (8001000)(2) >> >>
() ( )
UTi2O6 () 0.1 510 >35
Gd2Zr2O7 () >10 <20(2)
REEPO4 () >1 <300(1) >30
ZrSiO4 () 0.40.6 600(1)/900(2) 1618 320
CaTiSiO5 () 0.30.4
Ca2REE8(SiO4)6O2 () 0.30.6 300(1)/950(2) 5 130
(Ca,Gd,U,Th)3(Zr,Fe)2(Si,Fe,Al)3O12 0.2 (9001100) (2)
>> >>
( ) ( )
. (1) ; (2) .

( 620 %) - -
, : W = kexp(Ea/RT), Ea .
.
170 Pu 70 U ( 1, 1530 / 4080 / -
3 ) [Lukinykh et al., [Radioactive Waste, 1988].
2003] , 45 300
238Pu. - -
25 , BSi
, (36) .
7 12 . % 238PuO 2 [Strachan et al., 2004;
2005]. , 100200 , -
( SPFT, 90 ) [Ringwood,
, - 1985]. -
, 238Pu. , -
, , - ,
.
- -
- .
. - -
BSi
1000 , BSi . [Hench et al., 1984]. -
, - ( 1, 90 , )
, (. 14.18).
[Mitamura et al., 1994; Lukinykh
et al., 2003; Strachan et al., 2004; 2005]. 1 (Cs)102 (Ca) /(2)
- 103104 /(2) 100
. [Ringwood, 1985]. ,
- [Solomah et al.,
, 1986],
, - ,
. - (. 14.19). -
10
250300 , 60 -
100 . . ,
160 14

- -

. - , .
(-
. 10 )
.
:
; -
; , [-
[Radioactive Waste, 1988]. ., 1996].
- , -
. - .
12501300 ,
. ,
, -
, - -
-
10501200 20 [Ringwood et al, 1988; . 20 %
Stewart et al., 1996]. , 80 % : 5.4 % Al2O3, 5.6 % BaO,

14.18.
1 2 [Hench et al., 1984]

-1 (90 ) -2 (150 )
.. (3 ) .. (28 ) .. (28 ) (28 ) .. (28 ) .. (28 ) (28 )
Al 0.81 0.18 710 2
510 3
0.48 0.19 1103
Ni 0.04 7103 0.04 0.27 1.89
Si 2.5 0.67 0,24 0,28 2.87 0.95 2.68
Sr 1.4 0.38 0.01 <0.1 1.82 0.49 1.53
Ca 1.05 0.21 8102 0.63 0.19 0.52
Na 2.97 0.62 0.33 1.99 0.08
Cs 3.67 0.79 0.54 0.45 2.53 0.74 1.96
Ti <8104 <8105 <8105 <2103 <8105 <8105 2103
Zr <3103 <4104 <4104 <8103 <4104 <4104 8103
U 110 4
910 4
<1710 2

Nd <8102 <8103
. /(2). .. , .. , .

14.19.

4 7
Ba 0.25 0.13 0.05 0.025 0.013 0.004 Ba
U 1.6103 6.3104 3.2104 2104 8105 5105 U
Ti 10 3
410 4
2.510 4
1.310 4
510 5
210 5
Ti
4 7 14 28 56 120
Ba 0.25 0.13 0.05 0.025 0.013 0.004 Ba
U 1.6103 6.3104 3.2104 2104 8105 5105 U
Ti 10 3
410 4
2.510 4
1.310 4
510 5
210 5
Ti
4 7 14 28 56 120
Ba 0.25 0.13 0.05 0.025 0.013 0.004 Ba
U 1.6103 6.3104 3.2104 2104 8105 5105 U
Ti 10 3
410 4
2.510 4
1.310 4
510 5
210 5
Ti
4 7 14 28 56 120
. /(2).
161

. 14.10. , .
() .
. .

11.0 % CaO, 71.4 % TiO2 6.6 % ZrO2. - + . -


3.5 % H2/N2 750C -
2 % Ti ,
2 1200C 20 . - (. 14.10). -
(. . 14.6), Ca 0.77 Sr 0.15 Ba 0.09 MoO 4 ;
. - Ca0.15Sr0.14Ba0.81Mo0.97O4 Cs1.51Na0.52MoO4
: .
, , , - , -
. 1300 .
, ,
(. . 14.5).
- . ,
14001500 . ,
, .
[ ., 1987; Sobolev et al.,
1995; ., 1996]. ( 0.100.15 )
, 25, 100, 200 350 [Sobolev et al.,
1.76 U - 1997].
1100 3. . -
1:10, -
.
, - 1000 1. ,
- , -
. ( ) s , -
5 . 4050 % . -
s
, - 20 40160 /, -
.
0.48 /. 100 Cs
. - 5 /2, -
:

14.20. / [Sobolev et al., 1997]

4 7 14 28 56 120
Ba 0.25 0.13 0.05 0.025 0.013 0.004
U 1.6103 6.3104 3.2104 2104 8105 5105
Ti 103 4104 2.5104 1.3104 5105 2105
162 14

(. 14.20). - Ca, Mn, Zr, U, Ce Al.


, Sr UO2 ( 11.9 0.8 . %),
(Ca,Sr,Ba)MoO4. 100 - ZrO2(5.73.8%), Ce2O3(6.02.7%) CaO (15.613.0%),
Sr TiO2 (54.865.9 . %),
, , Ti, MnO (3.65.7 %) Al2O3 (0.83.7 %). -
Zr, Ce . 5 %, -
, - .
(, - /,
, ), . -
. ,
, 1015.% (, , -
, , )
. - . -
Sr, s Mo.
, .
, - .
.

,
(, , , ). - . -
, -
, . -
, .
. -
,
- [Mazzi, Munno, 1983]. TiO
Sr Cs, -
[, 2005]. (. .), 8,
(. . = 7). TiO
[ ., 1997]. (2),
20 . % , (3) (3) -
U, Cr, n, [Bayliss et al., 1989]. -
Ni, Fe, Zr. (. %): TiO2 56.5, ZrO2
14.7, CaO 8.2, BaO 5.7, Al2O3 4.0, SiO2 2.7,
MnO 2.3, K2O 1.5, Ce2O3 1.3, UO2 1.1, NiO 0.9, ,
Cr2O3 0.6, Na2O 0.3, Fe2O3 0.1, MgO 0.1. [Kesson et al., 1983; Vance et al., 1995; .,
, 1996; Lumpkin et al., 19981; Giere et al., 1998].
(8085 %) -
(. 14.11 . 27 . % UO2, 24 % PuO2 NpO2, 20 % ThO2,
). 29% , 14% Nb2O5, 7% Al2O3, 5% MnO,
0.10.5 . 4 % FeO, 5 % MgO, 1 % SrO Na2O. -
-
1 . - Zr4+ (Ce4+, U4+, Pu4+) Ca2+ (Pu4+,
, Np4+, REE3+, Pu3+).
. - ,
. (10 %) - , Al3+ Fe3+/2+.
, ( Ti4+
0.10.3 . (5 %) Al3+ Fe3+)
0.1 . . -
5 % REEZrTiAlO7, REE = Y, Gd, Tb [
, Si, Al Ti. ., 20032].
- . , 0.2
, , 0.3
, . [Kesson et
- al., 1983; Vance et al., 1994; Xu et al., 2003]. -
. -
. , [Vance et al.,
- 1995; Begg et al., 1997; 1998],
. Ti, . 4+ Pu4+
163

c 70100 % Strachan et al., 2004]. 21018 ./ -


0 - -
(2/N2, ). Np Pu -
, Np4+. .
Pu 510 18 ./, 0.5 ./.
, , , -
[Strachan et al., 2004]. 16 ./ [Sinclair,
, - Ringwood, 1981; Lumpkin, 2001].
: 1250
20 [Lumpkin et al.,
14001500 . - 19982].
(. 14.12). - , -
, . %: 2.6 Al2O3, 2.4 BaO, 10.0 CaO, 6.6 Nd2O3, 1050 .
48.4 TiO2, 10.4 UO2, 19.6 ZrO2 , - -
(80%), , 238Pu [Strachan et al., 2004].
. -
( /(2. )): Ca = 101102, Ba= 102103, . , -
Nd = 103104, U = 104105, Al = 102, Ti = 106, (70 %),
Zr= 107 [Vance et al., 1995]. 15 % [Vance et al., 19962].
104105/(2) [Hart et al., 1998; 2000]. -
,
[Lumpkin et. al., 1995; McGlinn et. al., 1995]. -
150 - -
17 .
( ),
. .
250 50 Ma, 12 -
- , .
[Malmstrom et al., 1999]. -
[Zhang et al., 1500 .
2004] 250 [Giere et al., 2001], - -
Ca2Zr5Ti2O16 [ .,
CaTiO3 ( 50 ) , - 1997]. :
ZrO2 (200 ).
(REE, Zr, Hf Ti) - (Ca1xGdx)Zr(Ti2xAlx)O7,
, , ,
(Al Ca) . Gd 3+ , Al 3+
- .
, 244Cm 238Pu (. %): Gd 2O 3 30.0, TiO 2 26.3, ZrO 2 25.4,
[Radioactive Waste, 1988; Matzke, van Geel, 1996; Al 2 O 3 7.5, CaO 4.9, SiO 2 5.6, FeO 0.1,

. 14.12. , 1500 , (1 ,
2 , ), , (1 , 2 Zr,Gd,
3 + ).
164 14

Na2O 0.1, K2O 0.1. - -


, .
, - ,
. . . ,
, X.
80 % , 10 % 10 % -
. , -
. 1 - . [Raison et al., 1999],
( 1 ) (A 3+) 2(B 4+) 2O 7 ,
(. 14.12). ( 5) RA:RB 1.461.80 (RA
2 1. - RB ). -
4:1.
1 . . = 8 (
20 . , ), -
. - .
1 Zr, Ti ,
Gd ,
. - . -
35 . %. - , [
[Jostsons et al., 19961] - ., 20012; Ewing et al., 2004].
,
18 36 . % PuO 2. [Kesson et al., [Ebbinghaus et al.,
1983; Vance et al., 1995], 19981; Ebbinghaus et al., 19982; Strachan et al., 2004;
30 . %. Strachan et al., 2005]. 30 %
, , ,
, , , (Hf, Gd),
. . -

(, , ) (. 14.21).
(70%), -
- (. 14.13). Pu -
(Pu, Np, U) , , .%: 10.0CaO, 35.8TiO2, 10.6HfO2,
- 23.7UO2, 8.0Gd2O3, 11.9PuO2 -
. , UPu (. 14.22).
(. Fd3m, Z = 8) - ,
, , , Ce Pu.

14.21. ( 100 . %)

, . % 1 2 3 4 5 6
CaO 9.2 9.5 11.7 10.7 11.3 10.0
UO2 46.6 47.8 17.5 23.7
PuO2 8.8 11.9
CeO2 26.3 27.9
Gd2O3 10.8 9.2 9.1 8.0
ZrO2 2.5 8.8 12.2
HfO2 11.8 10.6
TiO2 39.7 40.7 42.4 40.4 41.1 35.8
Al2O3 0.9 0.9
BaO 1.1 1.1
, . % 60 % , 90 % , 70 % , 98 % , 90 % , 80 % ,
30 % , 5 % , 20 % , 2 % 5 % , 10 % ,
10 % 5 % 10 % 5 % 10 %
. 1 , [ ., 2001]; 2 [Ringwood, 1985], 36
Ce Pu [Ebbinghaus et al., 19981; Ebbinghaus et al., 19981; Gould et al., 1998; Icenhower et al, 2006]. ,
, , , , .
165

. 14.13. , ()
().
20 . (111)
. : 1 , 2 . : 1 ,
2 , 3 .

Pu4+, 30 % O4 [Bakel et al., 1999; Stewart et al., 2002; Zhang et al.,


+3 [Fortner et al., 20001; 2002].
., 2004], - . -
[Xu et al., 2000]. , 104 -
, - 17 105 /(2) 112324
. [Hart et al., 2000].
, -
( , -
SPFT, 90 , = 2) (. 14.13).
( 6103 /(2) (. 14.21), UTi2O6
[Icenhower, 2006]. .
( 3, 95 , 7 ) -
- Ti, Zr U
[Chamberlain, et al. 1998]. (26)105 /(2) [ ., 2001].
-
( /( 2)): 10 2,
Gd 103, Pu 104 [Hart et al., 1998; Hart et al., ( 2 ) -
2000; Strachan et al., 1998].
Gd Pu ( SPFT, 90 , 612440 ( = Y, Na; = Ti; C = Fe; T = Zn;
= 2) (14)104 /(2), - X = O, F) : F 43m,
- a = 14.89 A, Z = 4 [Ercit, Hawthorne, 1995].
[Strachan et al., 2005]. 815 . % : [8] -
(F, Cl, Na, Mg, K, Na, 8, [6] ,
Si, Al, Ga, Mo, W) , [5] ( )
, Ca(Mo,Wo) [4] .

14.22. [Ebbinghaus et al., 19981; Ebbinghaus et al., 19982]

UPu
1 2 1 2 1 2 1 2 1 2
CaO/Ca 2+
10.5 0.91 8.9 0.73 1.0 0.07 1.9 0.08
UO2/U4+ 24.3 0.43 7.6 0.13 35.4 0.55 2.9 0.01 48.1 0.45
PuO2/Pu 4+
13.3 0.24 6.7 0.11 14.1 0.22 43.0 0.40
Gd2O3/Gd3+ 8.2 0.22 5.7 0.15 4.9 0.11 3.4 0.05
HfO2/Hf 4+
11.6 0.27 37.7 0.83 7.0 0.14 18.9 0.08 2.6 0.03
TiO2/Ti4+ 31.7 1.91 31.4 1.82 37.0 1.94 77.8 0.90 0.5 0.02
Al2O3/Al 3+
0.4 0.04 2.0 0.18 0.6 0.05 0.4 0.01 0.5 0.03
. 1 . %; 2 4 () 7 (), 6 ()
2 ( UPu ) . .
166 14

14.23. 10 . % Th2 U2

Th- U-
5M 8M 3 5M 8M 3M
Al2O3 2.7 4.3 7.9 0.6 3.7 1.2 4.1 7.0 3.7 0.5
CaO 11.2 10.9 9.5 21.9 4.2 10.7 11.2 10.9 0.4 0.9
TiO2 52.2 54.8 55.6 48.6 71.2 45.4 53.7 57.4 68.1 51.9
MnO 8.5 9.2 10.9 1.0 7.4 7.1 8.8 10.6 13.3 26.3
Fe2O3 3.0 3.6 7.2 0.6 8.4 2.1 3.5 5.7 16.1 19.7
ZrO2 9.7 6.5 2.1 .. 1.3 12.2 7.0 3.1 .. ..
AnO2 12.6 10.9 5.1 24.1 2.7 21.5 11.3 4.6 .. ..
. 5M, 8M, 3M , , , ,
. .. .

(Ca,Mn)2Zr(Fe,Al)4Ti3O16 - , -
,
[Morgan, Ryerson, 1982]. - ( ) 3 -
- [ ., 2005]. -
. -
20 . % , : 5 (2 + 3)
(. 14.11). 8 (3 + 2 + 3).
5 . %, 3 R 2M2X7x
50 % . - R3M16M22X20x, R Na,
. Ca, Mn, , M1 2 -
- Ti, Zr, Hf, Fe, Al. -
, ,
. - R 5M1 8M2 2X 27x ( 5) R 8M1 14M2 4X 47x (8).
, -
. , [
, ., 1999; ., 2002; .,
. - 2003; Kirjanova et al., 2003].
- 5
. 8 3, -
- , (. 14.23).
, ,
. ... - (. 14.11, 14.14).
. - , 5, -
- , -
(. %): 55 % TiO 2, 10 % MnO, .
10 % CaO, 5 % Al2O3, 5 % Fe2O3, 5 % ZrO2, 10 % (8),
. - (3).
(UO 2, ThO2, NpO2, PuO2), U, Th Zr
(La 2O 3, CeO 2, Nd 2O 3, Sm 2O 3, Eu 2O 3, Gd 2O 3, 312 . Ti, Al Fe -
Tb2O3, Yb2O3, Y2O3) , - ,
, -
. . , ,
. -
, - .
, , ,
. , 1 Kr +
- ( ) 1012 /(2). [ .,
, , 20032; Lian et al., 2004].
5 (5, 5) 8 (8, 8) , -
, [ ., .
19981; ., 1999]. - , -
(3, 3) - : 3 5 1,
(7, 7) . 5 8 2.
167

. 14.14. 10 % () ().
1 5; 2 8; 3 3; 4 ; 5 .
.

.
, - 650750 .
- -
. ,
. -
(. 14.15). , , -
- .
, . -
25 , -
~0.2 ./. , , .
600,
, , -
0.9 (8) 1.1 ./ (-5). .
- Ca2+ Mn2+, Ti4+,
. - Zr4+, Al3+, Fe3+. , -
, - : -
, 5 8 3.

. 14.15. 5
.
; 4.381013 (0.04); 9.391013 (0.08); 15.61013 Kr +/2 (0.13 ./).
168 14

14.24. ( 1)

, ,
, / , /(2)
Pu Am Pu Am Pu Am
3 22.2 3.39102
3.0210 6
4.62104
8.3710 3
5.48103
7 4.25 3.23102 5.79102 4.41104 6.88104 5.23103
14 7.19 3.12102 9.79102 4.26104 5.82104 2.39103
21 2.40 2.88102 3.27102 3.93104 1.30104 1.55103
28 0.47 4.25103 6.44103 5.78105 1.91105 2.34104
35 0.65 6.53103 8.87103 8.90105 2.11105 2.88104
42 0.61 7.28103 8.24103 9.92105 1.63105 2.68104
49 0.78 6,60103 1.06103 8.99105 1.79105 2.08104
56 0.50 9.42103 6.80103 12.8105 1.01105 1.9010-4
63 0.66 11.9103 9.04103 16.2105 1.19105 2.14104

3 . -
, , - XO 4 BO 6 ,
( ). -
. - A ,
, . U Th
-
105106/(2) ( 1, 90, .
, ). - -
-
.. . 14.24 -
, .
10.% 239Pu.
0.1 . % 241Am. -
, , .
,
104105 /(2) 63 . 46 . % [Burakov et al., 1999;
- ., 2000; Burakov, Anderson, 2000].
( , -
SPFT, , 95 ), -
. Fe3+, -
, Al3+ Ga3+ [, 2003].
30 . %, - (Ca 2 Th)(ZrFe)
300 . - Fe 3O 12 (Ca 2Ce)(ZrFe)Fe 3O 12 Th 4+ 4+
(. 14.25). -
. Pu4+ (0.96A), Np4+ (0.98A) U4+(1.0A)
, Th4+(1.05A) Ce4+(0.97A),
, - ,
Hf, , , -
. .
- -
, REE3Fe2Fe3O12.
- (Pu, Am, Cm) ,
. , .
-
, - :
[, 2003; , 2005].
[Cax(REE,An)33+2x(An,Ce)x4+]Fe5O12.

-
- . -
VIIIA 3 VI B 2 [XO 4 ] 3
169

14.25.

T C T,
Ca2ThZrFe4O12 1050 24 , 12.68 Ito, Frondel, 1967
Ca2ThZrFe4O12 1200 24 (12.68 ) > ThO2
Ca2.5Th0.5Zr2Fe3O12 1200 20 (12.74 )
Ca2.5Ce0.5Zr2Fe3O12 1200 3 (12.69 )
(Ca,Gd,Ce,Pu)3(Al,Ga)5O12 >> Burakov et al., 2000
Ca2.5Th0.5Zr2Fe3O12 1300 5 (12.75 ) > , 2003
Ca1.5GdTh0.5ZrFe4O12 1300 5 (12.62 )
Ca1.5GdPu0.5ZrFe4O12 1400 3 (12.57 ) > Ca-Fe
Ca1.5GdCe0.5ZrFe4O12 1300 5 (12.59 ) >> Ioudintseva, Chae, 2004
Ca2,5Ce0,5Zr2Fe3O12 1300 5 (12.69 ) >>
Ca2CeZrFeFe3O12 1200 5 (12.64 ) >>
Ca2ThZrFe4O12 1200 2 (12.67 ) > Shabalin et al., 2003
Ca2,5Th0,5Zr2Fe3O12 1200 2 (12.74 )
Ca2,5Ce0,5Zr2Fe3O12 1200 2 (12.73 )
Ca2Th0,5Ce0,5ZrFe4O12 1200 2 (12.62 ) >

[Sombret, 1987]

, .%: 47 % Fe2O3; 310 5 (Gd)10 6 (Ce, Th) /( 2 ).
30 % REE 2 O 3 + An 2 O 3 (Nd, Pr, Sm, La, Am); 10 3 /(2))
10 % CeO 2; 8 % AnO 2 (U, Pu, Np) 5 % CaO, Gd Th, (0.2/(2))
: Ce [Yudintsev et al., 20042]. -
-
[Ca0.75(REE,An)13+.5(Ce0.5An0.25)4+]Fe5O12. 3+ [Brookins, 1984].

,
. ,
: . -
-
(Ca2,5An04+.5)(Zr,Hf)Fe3O12 [Utsunomiya et al., 2002].
0.2 ./ 25 ,

(Ca1.5GdAn04+.5)(ZrFe)Fe3O12, , ,
(. . 14.17).
An4+ (Pu, Np), Gd Hf - -
, .
- . ,
16 . %. 1618 13 . % -
, - 0.5
(0.01 M HCl) (0.01 NaOH) [Yudintsev et al., 2002; , 2003; -
( 2 3, 95150 , S/V = 10 1). , 2005]. , , -
: (. 14.16),
.
Ca2,5Ce0,5Zr2Fe3O12, Ca1,5GdCe0,5ZrFeFe3O12 2 Fe3+ 2 -
Al 3+
Ca1.5GdTh0.5ZrFeFe3O12; .
12001400
, . [Yudintseva, 2005]. , -
- ,
, , -
(Fe 2O 3), .
. - , -
, , (,
170 14

. 14.16. , () ().
: Ca1.5GdTh0.5ZrFeFe3O12. : (Ca1.2Gd1.6Th0.2)(Zr0.5Fe1.5)(Si0.6Al1.3Fe1.1)O12, ,
ThO2. (111)* . = 50 .

, ).
( , -
), , , Pu.
, .
, - ( -
,
: , -
, - )
. -
, .

14.26.


VIII
(Zr,An 3+/4+
,REE )O2z
3+
Fm3m
VIII
(REE,An)23+/4+VIZr2O7 ( ) Fd3m
XII
(Ba,Ca,REE, An)VI(Zr,An)O3 ( ) Pm3m
VIII
An Ti2O6 (An = U, Th, Pu)
VI
C2/m
VIII
A2VIB2O7-x (A = Ca, REE, An; B = Ti, Nb, Zr) Fd3m ()
A BVI-VC2O7(A = Ca, REE, An; B = Zr, An, REE; C = Ti, Nb, Al, Fe)
VIII VII
C2/c
XII VI
A BO3(A = Na, Ca, Sr, REE, An; B = Zr, Ti, Nb, Al) Pnma, Pm3m ,
VIII
A3VIB6VC2O22-x(A = Ca, Mn, REE, An, Zr; B = Ti, Fe; C = Ti, Al, Mn, Fe) F 43m
XII
A2-1 VI-IV
B19-21O36-38(A = Na, Ca, REE, An; B = Zr, Ti, Fe, Al, Mg) R3 ,
VIII VI
A TiVIBO6(A = REE, An; B = Nb, Ti, Al, Fe) Pcan/bnm /
IX
(REECe,An,Ca)PO4 P21/n
VI
(Na,Ca,REE)VI(Zr,An) 2(PO4)3 R 3c
VIII
[Th4-x(U,Np,Pu)x](PO4)4P2O7 Pcam
VIII
(Zr,Hf,U,Pu)SiO4 I41/amd
VII-IX
(Ca,REE,An)10(SiO4)6O2 P63/m
VIII
(Ca,Y,REE)3VIB2(SiO4)3 (B = Fe, Al, Ga, Ti, Zr) Ia3d ()
VII
(Ca,REE,An)VI(Ti,Fe)IVSiO5 C2/c
X
A4 B3 Ti2 Si4O22 (A = a, Sr, REE, An; B = Mg, Fe, Al, Ga, Zr)
VI VI IV
P21/a ,
XII
(REE,An3+)VIAlO3 Pnma/R 3
VIII
(Ca,Y,REE,An)3 (Al,Ga) 2(AlO4)3
VI
Ia3d
XII
(Na,,REE,An)VIIV(Al,Ti) 12O19 P63/mmc
171

[Rovnyi et al., 2004].


,
.
- 7185% .
, - -
. (2000 ).
[Burakov et al., 2004] ,
-
14.3.4. 238Pu .
PuPO4 , ,
4.21024 ./3 (0.12 ./). ,
, - -
.
(. 14.26). , - . (La,Pu)PO4 ,
, , . 8.1 . % 238Pu,
(, ) - 11.91024 ./3 ( 0.3 ./).
. - NaZr 2(PO 4) 3
, . -
, ( , MA2(PO4)3
) , - (R 3cD36d, Z = 6). -
. M A ,
, P5+
. Si4+, As5+, V5+.
,
-
.
,
(NZP), -
. [Boatner, Sales, 1988; [Radioactive
Radioactive Waste, 1988; Dacheux et al., 1999]. - Waste, 1988]. 1030 % -
- 2056 % -
(LaEu). , - (8501100 )
REEO9 (1100 /100 )
4. [Hawkins et al., 1997; Zyryanov, Vance, 1997]. -
, NZP ,
.
. - [Seida et al., 2003]
1000 4 8 . % Cs, Sr Ba; A
1300. - 78 . % Cr Fe; 15 . %
104 /(2), 1 [Aloy et al., . , -
2002]. 90 - -
2103 /(2), 1000 , - . -
. LuPO4 (- , .
) 1 . % 244Cm NZP
18 [Liu et al., , (Mo,
1998]. 1.51019 ./, Te, Sr, Cs, Ba)
1.3 ./ 2300 12 .
10.% 239Pu. - Na 238Pu 2(PO 4) 3 9.31018 ./
, [Orlova et al., 2002], , -
. - . , -

. .
-
, - , -
. -
(Th,An) 4 (PO 4 ) 4 P 2 O 7 [Gent et al., 1999]. -
,
. , -
( ). 100200 ,
172 14

1100 +4 , -
1250 ( (Np, Pu)5+/6+ -
). ,
300800 . -
1030 1250 . ,
9599 % . - -
Th4(PO4)4P2O7 - .
U > Np > Pu , -
. 75 . % ( 48 . %) .
Th4+ U 4+, 52 . % (33 . %)
Th4+ Np4+ 41 . % (26 . %) -
Th4+ Pu4+ [Dacheux et al., 1999; Genet et al., , -
1999]. -
Zr4+ Th4+. - .
[ ., 1966] -
, 2+
0.1 . %. - 3+.
, (PO4)3 (SiO4)4.
- -
. : Ca2+ + P5+ REE3+ + Si4+. -
-
Th 4(PO 4) 4P 2O 7 : IXVII 10IV 6 24 2 (P6 3/m, Z = 1),
U, Np Pu, , REEPO 4, Ca, REE, Th, Al, Fe, Mn, Mg, Na, K; B Si, P,
Am Cm [Clavier et al., 2004]. - B, F, Al; X O, OH, F [Ito, 1968]. U4+
- Pu4+ Ca4x(REE,An)6+x(SiO4)6y(PO4)yO2
, , 0.5 0.05 , -
. Gd3+ Hf4+ -
, - 8 <0.1 (. 14.27).
, 2 -
25 . % ( . 25
2.610 16 ./) , - (1 Kr2+ 1.5 Xe+) -
- 0.20.4 ./
. - (. . 14.9),
10 6 10 8 /( 2 ) 244 Cm [Ewing et al., 1995].
( 1, 28 , 90 ), 23 ,
, - ,
, . 1 ./ [Gong et al., 1997;
Yudintseva, 2005].
105 /(2) 0.1 M HClO4 [Genet et al.,
1999]. , - , ZrSiO4(Burakov, 1993; Ewing, 1999;
(, - Ewing, 2001). 612.% -
) , -
[Anderson et al., 1993].
[Goffe et al., 2002]. - ( )
- 4.1104(250) 4.6105(90) /(2) [Ewing,
. 2001].

14.27. [Vance et al., 2000]

U4+ Pu4+ Pu3+ Hf4+ Gd3+


REEPO4 0.5 0.25 1 <0.01 1
ZrSiO4 1 1 0.1 1 <0.1
REE2Ti2O7 1 1 2 0.3 2
CaZrTi2O7 0.7 0.7 1 1.4
CaTiSiO5 0.020.05 0.02 0.05 0.5 0.3
Ca2REE8(SiO4)6O2 0.5 0.05 <0.1 8
CaTiO3 >0.1 0.10.13 1 1 1
173

14.28.

. , , d () a,
/, / (222)
M-24 /24 >> Zr > Nd 3.058 10.593
(4 6 )
A-1 -2, 5 /3 3.064 10.614
A-2 , 5 /6 3.062 10.607
A-3 , 10 /3 3.060 10.600
A-4 , 10 /6 3.062 10.607
-1 -0,5, 5 /3 >> 3.069 10.631
-2 , 5 /6 >> 3.073 10.645
-3 , 10 /3 3.060 10.600
-4 , 10 /6 3.062 10.607

6 10 . % [Nikolaeva, Burakov, 2003], ,


, , [Radioactive
Pu2. Pu (1, 90 , Waste, 1988].
1428) 71032101/(2) .
. .
1019 ./ ( 0.6 ./)
( 1820 %) .

.
[Wang et al., 1999;
[Vance et al., 2000], - Kinoshita et al., 2000; Burakov et al., 2002; Ewing et al.,
. 2004],
- . -
. (Zr,An3+/4+,REE)O2x
(CaTiSiO 5) (An3+,REE)2Zr2O7 [Raison et al., 1999;
. - Gong et al., 1999; Raison, Haire, 2001].
Na+, Ce3+, La3+, (Zr,Np,Y)O2x 2040.% NpO2
Y3+, Fe3+, Al3+, Nb5+; O2 OH F, 10 5 /( 2 )
Mn2+, Mg2+, (2, , 150 , 84 , ).
Cr3+, Sn4+, U4+, Th4+. - ,
51018 ./, , 4 , BSi -
8 %. [Kinoshita et al., 2000]. REEZr -
3 ,
, - : 2REE3+ = An4+ + Ca2+.
. - -
21.5 9.3 . % , -
[Stefanovsky et al., 2000]. , - . -
-
. [Stewart et al., 2002], -
: 2Ca2+ = Gd3+ + Na+; , . -
Ca2+ + Ti4+ = Gd3+ + Al3+; Ca2+ + 2Ti4+ = U4+ + 2Al3+.
Gd3+ U4+ , . -
0.250.07, [Vance et al., ,
2000]. U4+, Pu4+, Pu3+
( ) 0.020.05, ( 50 )
Hf4+ Gd3+ 0.5 0.3 (. . 14.26), 15001600 [ ., 20021;
- ., 20022].
. - -
, . -

. [ ., 2004].
, -
174 14

. 14.17. , (La0.26Ce0.51Pr0.24Nd0.79Sm0.14Eu0.04Gd0.03)
(U0.07Zr1.93)O7.
, . 4, 4 ( 14.28).
(110)* (211)* .

() -

(). -
, .%: 7.1 La2O3, 14.0 Ce2O3, 6.8 Pr6O11, ,
22.2 Nd2O3, 4.1 Sm2O3, 2.0 EuO, 0.9 Gd2O3, 3.2 UO2, . -
39.7 ZrO2
, -
: .
,
(La0.26Ce0.51Pr0.24Nd0.79Sm0.14Eu0.04Gd0.03)(U0.07Zr1.93)O7.

25 .
1500. -
. ,
- , .
(. 14.28, . 14.17)
(. 14.29). .
( ),
.
14.3.5.
:

- (Th, U)4+ + (Mg, Fe)2+ = Ca2+ + Ti4+;


- REE3+ + Al3+ = Ca2+ + Ti4+;
, . -
REE3+ + Fe2+ + Nb5+ = Ca2+ + 2Ti4+;
. Hf4+ = Zr4+ [Giere et al., 1998; Giere, 2001].

14.29. [ ., 2004]

M-24 A-1 A-2 A-3 A-4 -1 -2 -3 -4


/ (% .)
3
4.68 4.92 4.95 4.93 4.98 5.58 5.63 5.60 5.72
(72) (76) (76) (76) (77) (86) (87) (86) (88)
, % 23.6 0.5 1.8 1.5 0.5 3.6 1.0 1.5 0.6
, /( )
2
La ~10 5

-1, 90 7 , Ce ~105 ~106 ~106 ~105 ~106


Pr ~10 5
~10 6

Nd, Sm ~10 6

U, Zr ~107
175

, , 1001000 , -

. 110 .
24 . %, -
22 . %, ,
30 . % [ ., 1996; Lumpkin, 2001]. , , [Ewing, 1999; 2001;
- Lumpkin, 2001; Yudinseva, 2005] .
32 . % ( , ,
).
, - .
U, Ti, Ca .
30 . %, 9 . %,
16 . %. -
, 14.4.
210 17 310 20 ./. -

21019 1020 ./ [Sinclair, Ringwood,
1981; Lumpkin, 2001].
1 6 ./, - -
20 ./ [ ., 20032]. NaBSi NaAlP
, .
[Lumpkin et al., (. 14.30). -
1998 1; Lumpkin et al., 1998 2]. -
1.11020 ./, , -
10 % 400 ()
,
[Sinclair, Ringwood, 1981]. 200 [Jouan et al., 1991]. -
1000 , BSi - (1.3 42
. ),
110 - 0.15 3 (412 ) .
() , , -
23 [Lumpkin et al., 1.4 . -
2001]. R7
590 .

14.30. 1990 [Sombret, 1987; Glass as, 1996;


Warnecke, 1997; ., 1997]

,
-1, -500/1,2 19871997 , 2200
("", ) ~300
PAMELA 19851991 , 493
(, ) 2201
PIVER 19691972 , 12 (164 ) 1- ;
(, ) 19781980 900 2-
UP1, AVM 19781995 , 860
(, ) (2412 360 )
UP2, UP3: R7-T7 R7 c 1989 , 2434 400
(, ) 7 1992 1275 400
( AVM) ( 1995 )
WVP 1991 , 1000 ,
(, ) 200
( AVM) ( 1995 )
TVF 1996 , 140 ,
(, ) 300
DWPF 1996 , 240 (DWPF) 120 (WVDP) ,
( , )
WVDP 1996 , 1700 1900
(, )
176 14

[Bart et al., 2001] , , -


. % ( ): .
42.451.7 SiO 2 (45.2); 12.416.5 B 2 O 3 (13.9); -
8 . 1 1 1 . 0 N a 2O ( 9 . 8 ) ; 3 . 6 6 . 6 A l 2O 3 ( 4 . 9 ) ; ()
3 . 5 4 . 8 C a O ( 4 . 0 ) ; 1 . 6 2 . 4 L i 2O ( 2 . 0 ) ; .
2.22.8 ZnO (2.2); 4.218.5 (12.0). -
1991 . 220 . -
. 25 . % ,
75 . % - -
. 8 .
200 , 19911997 . ( )
. 500/2
1999 . 35 %
4000 . 2200
3 [Jouan et al., 1999]. - 300 u.
, -
, 1000 , (500/3)
( 2500 ). 2001 . [, 2001].
2000 500
10000 20000 250300 / 100 /
[Lee et al., 2006]. [, 2005].
(, , , )
-
() , , ,
, - . 40
. - -
20 -
. [Sinkler et al., 2000;
, - Pyrochemical Separations, 2004].
, -
BSi [Sombret, 1987]. ,
, . -
3 .
- .
-
, [Petkus et al., 2003].
860
, 30 14.5.
. 19962001 .
2 . 3 ( 24 ) -
275 2000 BSi .
,
, 10 -
(LiClKCl) -
(. . 14.30).
1987 . - . -
NaAlP 500 - , -
500 . ,
[ ., 1997; .,
20022]. - , -
, -
9.64.23.2 (), [Lewis et al., 1997; Esh et al.,
1999; Sinkler et al., 2000].
. 8090 . % 4 1020 . %
, , 15 -
- 500 .
. () - BSi 3:1

. 750850 40170
177

16 915 -
. .
Na 8 [AlSiO 4 ] 6 Cl 2 (60 . %) (45 . %)
(25 . %), - (1030 %),
, , - ( 70 % ).
[Frank et al., 2000]. - -
(PCT 1) , , -
BSi 3 .
[Simpson, Wronkiewicz, 1997; Frank et al., 2000; , 500/1 -
Moschetti et al., 2000]. Li, . -
B Cl 0.10.3 /( 2), -
310 (Na, K, Cs, Rb, Ba, Sr, Si, Al) (5.5 ), 2001 .
70200 (Pu, U, REE). [, 2005].
-
[Frank et al., 1999; Lewis et al., 2003]. , -
, 70 90 (100),
- NaAlP , -
( = 10) ( = 5) -
- [Kushnikov et al, 1997;
, , 2002], -
310 [Morss et al., 2000]. -
- [, 2005]. -
,
[Pyrochemical separations, 2004]. 100 ,
- - - -
- [ ., 2002 1; ., 2002 2]
. , .

( .) . ,
-

(NZP). . -
-
NaAlPF . [Demine et al, 2001].
1536 %, -
580 , , -
-
28 10 2 /( 2 ) [Polyakov et al., 2000].
12 118 [Bychkov, 2003]. , -
- , -
- , -
. .
- -
,
. [Aloy et al., 2000].
, ,

-
14.6. 8001000 -
.
-
.

, -
, .
- (1020 %)
, . , -
-
.
178 14

. ,
, , (,
, , , ).
,

( 6070 . %). .
- 1020 . %,
-
(Cs, Sr) . 3050 . %.
- ,
- ,
99Tc, 129I 135Cs,
, . -
[Fuels and,
. 2004].
, - ,
, - [Actinide, 2001]. -
. -
, - . -
. (Np, Am, Cm)
- [Lopatkin et al., 2001]. -
(12501300 ), ,
- ,
(14501500 ). -
, , -
. .
15

, - -
, ,
, , -
, .
,
, - () ,
. .

. , -

15.1.
-

[ ., 1989; ., 19911; -
., 19912; , 1992; ,
, 1997; Gupalo, Beygul, 2001 .]. -
, - .

, .
-

(. 15.1).
- .
, -
. -
, ,
, ,
. . -
-
,
, - .
.
- :
- -
in situ .
,
. - , -

. ;
180 15

. 15.1. [Disposition of , 2001].

-
, -
;
.
.
, -
; .. [1991].

- 630 -
, ; 200400 /. -
, - 1 . 400 1000
- -
- . -
, . 0.5 ,
. -
- [, 1992]. -
: 400
- . .
- -
, ,
- 9001000 .
, - .
; 70
- 1.9
( ) - 1.4 .
, -
; ()
..
- [ ., 2000]. 4500 ,
. - 400 . -
, 10 250 .
, - ,
; 18 ,
.
, . ,
108 . -
.
181

1.5 . - ,
4500 1000. - ,
1 . .
. -
. , , 90 - -
7.5 , ,
0.31 . ,
. -
, - , -
, ,
- , -
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1996]. . -
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. 15.7. [ ., 19912].
1 ; 2 ; 3 ; 4, 5 ;
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186 16

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.
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I 355500 ,
5585 , 2535 .
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188 16

. 16.2. II (a) IIII () [ ., 2000].


1 ; 2 ; 3 ;
4 ; 5 ; 6 .

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(~12 ) -
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,
[ . 1994]. .
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1972 . 12
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23 . 3). I , ,
7 , 1992 . -
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189

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1999 . 5 3
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1995 . 850 ,
568.5
[ ., 1999]. -
.
1 1995 . 260
[ ., 1999]. -
, -
I, (/):
90
Sr 1.2,
137
Cs 0.08,
144
Ce + 95
Zr + 95
Nb + 103, 106
Ru 04,
241
Am 1.9107,
. 16.3. I [
239
Pu 2.2106,
.,1999]. 99
8106,
13 . . 16.1; 4
; 5 .
237
Np 1.5107.

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, -
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.

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190 16

. 16.4.
, . [ ., 1994].
191

. 16.5. 18 18 [ ., 1994].
1 ; 2 ; 3
; 4 ; 5 ; 6
.

, 170 -
, - .
0.0009. = 23,
18 18 II 349386 (1020 /), (90140 /),
314341 (. 16.5), ~2 / (Cr, Fe, Ni, Al), -
1324 1330, -
0.53.0 0.70.9 /. - , -
6 , (90Sr, 134+137Cs, 106Ru, 95Zr, 95Nb, 144),
0.51.2 /. ( 239Pu, 241Am, 237Np, U),
[ ., 2000; ., 2002]. -
- 220 /. -
. - 74000 3, -
1012 838.8 , 1.5 ,
. , , . -
.. (2000), - , -
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, . -
10 /, , 1 -
1 /; 1995 . (/): 90Sr 1.62, 137Cs 0.1,
, - 144
Ce + 95Zr + 95Nb + 103, 106Ru 055, 241Am 1.9107,
10 /. 239
Pu 2.2106, 237Np 1.5107.
1975 . ,
18. ,
13 -
12 . 3. - .
-
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, -
. , [ ., 2000; ., 2002].
192 16

,

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-
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in situ - ,
,
. [NAGRA, 1994; Luhmann, 2000; ,
- 2002]. -
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[ ., 2000; ., 2002].
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.
Cr, Fe, Ni, Al, , , -
- , -
.

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[ .,
1978]. c ,

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, - . , ,
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105 1 / [International Comission, 1985]. -

193


. K d
99
Tc (2.110 5 ), 129 I (1.610 7 ), 79 Se (6.510 4 ), (3/): 90Sr 3540, 137Cs 7080, 144Ce 2540,
237
Np (2.110 6 ). 106
Ru 1015, 241 Am 3040, 239 Pu 4550,
- 237
Np 1015.
Kd 144Ce, 241Am, 239Pu -
, ,
, .
, , -
, (, pH, Eh, ,
, ,
, - .),
, . (Kd) -
, - 3/, -
, -
[Baston et al., 1995].
[NAGRA, 1994; Luhmann, 2000; , -
2002]. , - 2000 /,
- [Geochemistry of long,
, - 1992]. 70 Kd
(15 %) (85 %) 7.5104,
, . 0.46104 7.5104 3/. Kd
-
- , -
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. , - (Rf)
-
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- -
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22.3 %. .
315 %, 225 %,
27 %, - , , -
12 %, 0.53 %. -
, 1 . , -
- -
, - . , ,
(Kd), [ .
1999], - , ,
(3/): 90Sr 1.2, 137Cs 2.7 -
2.8, 144Ce 1.01.6, 106Ru 1.31.6, 241Am 1.11.2, . -
239
Pu 1.46.0, 237Np 1.82.3. Kd
-
. - -
,
Kd . ,
(3/): 90Sr 1035, 137Cs 1020, 144Ce 2040, , :
106
Ru 715, 241Am 830, 239Pu 1050, 237Np 715.

.
, -
, - ;
.
- -
. - -
-
194 16

,

; (99Tc, 129I, 79Se, 237Np). -
- -
I
, .

. -
- .

-
, -
[ ., 1999] -
[ ., 2000].
-
, -
,

-
.
. -
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137Cs,
,
. -

:
.
, -
0.01 %,
,
-


[ ., 1999]. , -
-

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-
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). , -
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1.0. -
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1000 , -
: [ .,1999].
, 1 ; 2
. ; 3 ( :
(. 16.6, ). , 1000); 4
,
. 1500 . /.
195


- Kd,
, .
(. 16.7). - -
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)
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17

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[Site selection, 1977]. 20002006 ., -
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197

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1957 1967 . -
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199

200 - .

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; , - [, , 1972;
- ., 1997].
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. ). -
100150 . . -

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.
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(. . 17.5).
, ( [ , 1977].
) -
: (
1) ; ), -
2) ; ( )
3) ;
4) . ( ). -
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, -
, - 40 120.
. - , 1 ,
, -
, -
- [ ., 1980].
.
( )
( ) - 17.1.2. ,
,
,
-
.


[Velichkin et al., 1995]. ,
-
- : , -
(. 17.8 . [Sysoev et al., 1999]. -
).
, -
, -
: - .
, (v = 2 ~ 3)
.
-
,
200 17

- .
. - ,
.
-
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- -
, -
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[-
1 3 - ., 1977].
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300400
[, 1975]. - ,
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, [ ., ,
1997], -

1015 . . -
-
() - () -
, , -
, .
, [ ., 1988], . . -
10000 . - -
- , -
-
, -
100300 . , -
(1) . -
2040 , ()
(3) 1020 . , ,
[ .,
1969]. - , -
, , -
(- in situ (. 17.9 .
). ). ,
,
, 70 -
4 50 , (0.200.57)106,
201

- , ,
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, , - -
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10000
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n104 .
0.4 % , 200 -
-
~15 / (5107 )
~5105 /. , ~400 -

[ ., 1994].
, - , -
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, ,
[Petrov et al., 20051]. , , , -
,
,
- . -
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[Omelianenko et al., 1993]. .
, , [ .,
, - 1987], 25 100 -
-
.
- (. 17.1). -
: , , ,

17.1. 2 [ ., 1987]

, , . ,
/() /() 1
25 100 25 100 100
Min/Max Min/Max Min/Max Min/Max Min/Max
1.77/3.83 2.65 1.46/3.57 2.57 638/966 783 320/1065 883 0.52/1.06 0.78
202 17

-
, -
. ,
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-
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250400 - .

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203

- ,

, . . -
, 10 - 13- :
, -
: (Mg5.6.Fe3.7.Al2.4.Na0.1.Ca0.1.Mn0.1)12
[(Si5.9.Al2.1)8O20](OH)16.
(Ca0.89.Fe0.05.Mn0.01.Na0.05)(Mg0.81.Fe0.16.Al0.03)
(Si1.89.Ti0.02.Al0.09)O6.
. -
,
. , .
- 13-, -
, . -
: :

Na0.21.Ca2.07(Mg3.27.Mn0.03.Al0.03.Ti0.10.Fe1.43)4.86 Ca2.0.Fe0.9.Al2.1.O.OH[Si2O7][SiO4].
(Si7.72.Al0.28)O22(OH)2.
, , -
.
, -
, . - ,
CaO 1.5 . % - -
0.7 . %. . .
-
Ca. :
-
Na0.94.Ca0.03.Al1.01.Si2.99.O8. , -
. 17.2
,
, , - 8002 ( ~1200 ),
. 2.

17.2. 8002 ( )


920 800 930 840 820 123 875 909 880 860
SiO2 45.71 46.31 46.47 47.67 47.70 46.11 46.20 48.39 48.74 49.18
TiO2 0.59 0.70 0.72 0.67 0.67 0.73 0.74 0.67 0.71 0.69
Al2O3 12.05 12.54 16.13 12.06 11.54 14.58 14.32 13.18 12.80 12.58
Fe2O3 1.95 4.12 5.44 5.13 4.34 3.39 5.42 4.25 4.57 4.28
FeO 4.02 6.80 6.57 5.34 7.42 7.07 5.90 6.65 6.13 5.67
MnO 0.09 0.10 0.09 0.09 0.11 0.11 0.09 0.09 0.14 0.13
MgO 5.94 10.47 6.84 9.44 11.74 7.78 9.40 8.98 9.84 9.20
CaO 12.78 11.17 9.98 11.05 10.35 6.55 10.36 9.66 9.55 10.42
Na2O 3.55 1.85 2.36 3.44 2.58 2.39 2.84 3.01 3.33 3.46
K 2O 1.17 0.88 0.91 0.12 0.11 1.02 0.52 0.37 0.12 0.25
H 2O 0.35 0.47 0.37 0.40 0.23 0.80 0.55 0.28 0.38 0.19
H 2O 1.71 2.04 2.43 1.94 1.98 4.71 2.19 2.41 1.88 1.52
P 2O 5 0.46 0.10 0.08 0.06 0.06 0.10 0.08 0.08 0.10 0.08
S. 0.02 0.01 0.01 0.03 0.03 0.03 0.02
SrO 0.05
CO2 9.34 2.25 1.05 2.72 1.40 4.60 1.29 1.78 1.30 2.22
99.72 99.81 99.50 100.15 100.23 99.94 99.90 99.82 99.60 99.88
: 920, 800, 930, 840, 820 ; 123, 875, 909, 880, 860 .
204 17

17.3.


. %
1 2 3 4 5 6 7 8
SiO2 49.52 50.35 48.49 48.51 44.08 57.11 90.78 60.68
TiO2 0.87 0.94 0.77 0.82 0.69 0.65 0.58
Al2O3 13.84 14.39 13.17 13.30 12.96 15.30 0.63 14.84
Fe2O3 3.07 3.18 2.92 3.34 2.23 8.23 3.08
FeO 6.59 7.05 6.03 6.45 7.31 0.65 0.46 1.87
MnO 0.16 0.17 0.15 0.18 0.15 0.08 0.03 0.08
MgO 8.38 8.74 7.93 9.48 8.35 1.14 0.04 4.13
CaO 9.27 7.83 11.03 9.99 9.41 15.40 4.50 6.03
Na2O 3.33 3.15 3.56 3.04 0.08 0.26 0.03 5.79
K 2O 0.51 0.60 0.41 0.49 2.23 0.03 0.06 0.70
P 2O 5 0.10 0.16
CO2 1.36 0.16 2.83 1.31 7.15 0.10 3.35 0.54
H 2O 3.10 3.44 2.68 3.09 5.25 0.90 0.13 1.68
110 55 9 5 3 2 2 2
: 1 , 2 , 3 ,
4 , 5 , 6 , 7 , 8 .

17.3 -
, . -
110 . ,

.
- [, 1967; ., 1996],
, Si, Mg, Fe, pH , -
Ca CO2. ,
- ,
7.58.2. Eh ,
- , 80 400 , -
-
150 250 . [Krauskopf, 1986;
[, , 1977]. Krauskopf, 19881], , pHEh
[Dixon, Batiza, 1979] c -
Mg (FeO + Fe2O3) - ,
- -
. , -

[Asadulin et al., 1995], - .
ThHfTa LaTh [Wood,
1980; Gill, 1981]. -
. ,
4080 ,
17.1.4. () .
( 6.47.2), -
(Eh +200+480 ),
(512 /), ( 90200 /).
-
pHEh , , , -
, - , .
4080 . -
. .
205

(Eh < +120 I 120 ) - ,


( 88.5) ,
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500 ) , -
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-
90Sr, 137Cs - , -
- ,
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, -
[ ., 1996].
- 17.1.5.
, -
= 200
= 0.3 , ()
-
,
.
,
,
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206 17

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(, )

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207

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, -
-
, (. . 17.5).
, - , ,
, - -
1015 . - , -
, , -
- ,
, - -
, . , -
. , -

, - (. 17.13 . ).
- , -
. , .
, ,
, , ,
, , , , -
.
-
(. 17.13). -
( -
, ,
- , (1.01.5 )
) -
( - , -
) , 23
,
, .
. -
- (~2 ~4 2), , , -

, - .

[ ., 1997], - -
- ( 600 )
, , .
-
. , .
,
208 17

. 17.15. ( ) ( ).
C (VP), (VS) (VR)
. VP VP c ( )
. a a .

,
17.2.
, -

. -
,
7260 3
,
. 130 , -
, - .
, 10 /. -
, . ( 1000)
- ,
-
- . -

. , -
, - . -
1992 . -
,
, -
. .
209


-
- [ ., 20023] , -
, ( 50 %) -
(. 17.14 . ). -
,
, - .
, -
3500 2. . -
- ,
. - , -
.
, , - -
, , - -
[, 1995]. 50 , -
, , , ,
, -
. . -
,
, , - -
. , , (,
.. (1999), ).
-
/.
23 1995 . 100 . ,
,
, ,
19962005 -
( 1030) .
-
, , , ,
2. , ,
,
. - , -
, -
, , ,
, -
(. 17.14). ,
2528 2 [ ., 1999] , ,
, , , -
, - [Petrov et al.,
[, 1999], 56 . 20052]. ,
- -
1 700 (1700) 1 (2.612.63 /3)
500 (1500). (2.742.79 /3).
- , -
: (2.652.75 /3).
-
,
; .
, , -
;

(. 17.15).
-
; (Vp = 4794 /) -
- (Vp = 5589 /).
/ (-
-
. )
210 17

, -
. , -

- (. 17.16 . ).
-
, ,
- -
. . N
.
0.14 0.95 %. - -
,
( 1.31 %) - -
(5.6 %). - -
, - , -
.
.
n1020 , , ,
n1016 2. , (,
, , - , ),
, -
. . -
-
, . ( -
) ( -
, - ) .

, () -
. ,

.
.
, , - ,
, - ,
- -
,
. . ,
-
,
- . -
.
-
, , -
-
. ,
. - -
.
18

, - , -
, ,
. - , -
, .
. -
- -
. - . -
( )
,
- , ,
-
. - -
-
100 , , . . 18.1 (. )
-
: (UO2)
, - 50 / . . [OECD/NUCLEAR, 1999].
. -
-
:
, . -
(>300 ) . 18.1,
,
;
, - , .. .
-
[International, 2004]:
; :
- .
. 130000 -
;
. ,
-
(99.5%
99% ). -
18.1. 500 .
, 1000 ;
, -

-
(99.5 % 95 %
). 1000 ;
212 18

: -
( -
99.5 %) - .
.

18.1.1.
-
90 %.
1500 . -
- , -
3000 . 129I, 137Cs, 135Cs, 79Se 126Sn,
- ,
, - ,
, . -
- 129I, ,
. - . 137Cs, -
, 10 .
, -
.
(. . ). 270 . (, 99Tc 107Pd)
- , -
- , -
137Cs 90Sr. . -
~250000 - 99Tc ( TO4)
. 250000 .
237Np , -
. , ,
, - -
,
. . 18.2 (. ) -
- . -
. - , -
. ,
. . 18.2, -
, , -
, - ,
. 200 - , -
4.3107 . . ,
, -
, , . -
0.994.
200
9.4106 (. . 40 ). -
, .
0.975. ,
. ,
, .
200 , ,
, .

, - 18.2.
.
105 200 5000 . - -
, -
,
, . -
. ,
-
[ ., 2002], , .
213

, - -
99.899.9 % ,
, (129I)
; - 99.9 %.
(99Tc 137,135Cs) -
. - 99.9% (..
, 1000 ).
(, 93Zr, 107Pd ,
97Se), , - PUREX -
. -
- -
, , - ,
.
.
- :
, , - PUREX
. PUREX ;
- -
, , ,
. , -
, , , . ,
, 1 PUREX;
( , ), , - -
Np CsSr ,
(. 18.3) - PUREX.
-
UP3 .

. 18.3. 1 [Korotkevich, Kudryavtsev, 2003].


214 18

(),
, PUREX:
SUPERPUREX;
100 . - PUREXTRUEX , -
= 3.2104
241Am. , -
.
,
= 1000. ( )
. 18.4.
( PUREX) , , -
- , -
1 [- PUREX.
., 20033]. , , -
Cs, Sr ,
1 - (>2M HNO 3) -
: ,
- , 20 -
, ; .
-
,
(CCD); -
- . -

. Ln

. 18.4. PUREX [Warin, 2002].


215

. Cm
. , -
- 99.9 %. -
. , 10 %
. (TcO4)
. 80 % , -
237
Np - . -
PUREX ( 1). (>99 %)
.
, -
, - ,
- , Cyanex 301, SANEX,
. ALINA BTR ( 1, 2, 4 )
237
Np - [International, 2004].
-
. ,
, -
. - , SANEX,
(Am + Cm >99.5 %) .
- -
. - [Warin,
: , , , , 2002] -
. Am Cm (. 18.5).
, - 2001 ., -
20 . 99.9 % Am Cm,
, ; .
TRUEX,
DIDPA, TRPO, TALSPEAK DIAMEX. -
TRUEX, DIDPA, TRPO
DIAMEX - ,
-
.
- ( ), -
DIAMEX TRPO. -
. 18.1. .
-
CRIEPI, [Inoue, Tanaka,
99.9 %. , - 1997]. -
- -
Np, Am Cm. , Am

18.1.
[International, 2004]

PUREX (.)
(.) (.)
99.9 % 99.9 % 99.9 % (.)
99.8 % 99.9 % 99.9 % (.)
95 % 99.9 % 99.9 %
- 99.9 % 99.9 %
- 99.3 % ?(>95 %)
- <5 % <10 %
-135,137 - 99.9 % (>99,9 %)
-99 - ~80 % (~99 %) -
-129 98 % 99.9 %
a
PUREX, DIAMEX SANEX; Calixarenes; [, , 2003; Bychkov et al., 1997].
216 18

. 18.5. , [Warin, 2002].

. -
UREX
, PYRO. UO 2
UPuZr -
. . 18.6. - , -
, UREX ( ) -
, [Laidler,
: 99.7 % Pu, 2002]. , -
99.8 % Np 99.4 % Am. (~6 % ),

. 18.6. CRIEPI
[OECD/NUCLEAR , 1999].
217

- 129
I
. - 9598 % ( = 2050).
129I
LiLiCl 650 C. . -
( )
- 129I -
. , - ~1000. -
(, .
. .) -
500 C. - , , -
- .
+ . (AgI, Pb(IO3)2, . .). -

. () .
, - (
) -
, -
. , , -
.
, - [Warin, 2002]. -
, , - -
- (),
[OECD/NUCLEAR.., 2004]. 10 -
,
.
[ ., 2003].
-
18.2.1. Pu U, -
Np, AmCm.
-
: , . -
,
(137,135,134Cs) , -
, ,
: ;
-
(); , .
[International, 2004].
90
Sr .
. - -
, -
.
99
Tc .
, TcO2, - -

.
(80%) (20%). .
PUREX -
(~1000)
()
4, - 99.9 % -
PUREX . 100
4 -
. ,
99Tc - 1000 .
, , , 100
. ,

. . ,
218 18

. 1999; Berthou, Magill, 2003].


- -
, . c .

0.1 % / - , -
.
- . -
- -
. ,
, , - ( ,
, - ) -
.
, ,
, ,
. -
. ,
. ,
, - 237Np 238Pu, -
, - -
, -
- (2106 87 ,
, ).
, - ,
. , ,
- ,
, .
- , , ,
. , , 244Cm, 18.1 -
, -
. . (180 )
99.9 % 240Pu -
, - 6560 .
, 244Cm 245Cm
- 8500 ,
. - ,
: 240
Pu. ,
, , -
, , - -
. .
;

, - , -
, . .
;

, . ,
, , -
. .
,

. 18.3.1.

, -
18.3. . ,
, -
, , (n,g), (n,2n) . . -
(1001000 ) -
() [Baetsle et al., , ,
219

- 1 %,
, -
, , , 99.8 %.
. ,
1 () -
. 1 .
238
Pu(n,g)239Pu , - , , -
, 235U(n,f) 3.2 ,
239Pu(n,f) . 100() 50./ ..
[Baetsle, 1997]. , , ,
( -
. - , ),
, 3 % , -
, -
( ).
. , -
, , ,
. , ,
1, , - ,
. - . -
, /ADS 6 ().
, 0.8 ( ,
) 0.2 ( ). ( ADS), -
-
, . (IMF)
. .
-
, , , -
. 18.3.2.
-
,
, PT.
- -
,
P ,
( ) T -
[Magill et al., 2003]:
. -
= 1 PT = R(1 P)/M (, 244Cm)
PT = JPT = JT/(1(1JT)JP),
(. 18.7 . ).
M ( ); -
R -
; , -
T ; 235U. -
P .
, ,
- ,
. ,
T = 1, - (16 ) -
1 (. . PT = 1). 235U [International, 2004].

P 0.98 0.999 (, -
) T 18.3.3.

0.15 0.20 (, 1520 % -
). -
8085 % , - , -
, (R) 57 . - (ADS).
220 18

- (), -
, , - -
ADS
. , .
, - , -
[OECD/NUCLEAR..,
, - 2002].
. , -
, ; -
, , -
.
,
. , . -
- -
[Berthou, Magill, 2003; De Raedt et al., 2002]
1 -
ADS [MYRRHA]. .
- , -
, ,
. . ,
- , -
. , .
, -
( ADS), , -
, , -
- . -
, - , -
- , ,
/, , .
.
200 ./, - . -

(150250 ./ ..) -
, 7585 % . -
. - , .
- ,
, - -
. . 18.8 (. ) .18.9 . ,
(. ) - .
.
, -
, 18.3.5.
ADS.
-
( ) -
. , -


18.3.4. . ,
-
- .
.. - -
1941 . 1990 . .
[Bowman, 1998] . [Rubbia et al., 1993] /

( ) (,
( ) )
LWR. -
, .
221

, - 2. -
, ,
- -
, 137Cs 90Sr. , , -
, .
2830 , -
, 238Pu -
300 . . 95 %
, - . -
- 237Np
, , .
, 129I, 99Tc, 135Cs,
93
Zr, 95Se 126Sn. ( 800 ) -
. - .
-
(, 14C 36Cl). ,

.
3.
18.4. , ,
238Pu, -
.
-
- , LWR, -
, ,
- . ,
- -
. -
.
( ), -
, - .
. - 4. -

/ , - . -
, -
. .
.
[International, ( )
2004] : . -

1. ,
LWR -
, - .
45 %, - 5.
238Pu LWR
.
(8002460 .), (30 % 238Pu 10 % ),
(<18 %) .
LWR 244
Cm (8 %) 243Am. 241Am
- : 80 % .
. -
, ,
(10310 4)
(238Pu) (8 %) - . -
, 239,240,241,242Pu.
LWR LWR 244Cm, -
UO 2. - 18 . -

.
222 18

. -
,
. - ,
-
, , , .
, - -
-
. . -
6. LWR
, (192455 / ..)
. - , ,
244Cm -
. - .
,
.
.
7. -

18.5.
. 98 %

(20 ).
, 80% 20%
( ). -
-
5 , 241Am -
( 432 ) :
239Pu ( 24400 ), -
243Am 244Cm. - . -
,
. , , -

241,242,243Am (2500 ) - ?
.
- ?
- -
. .
8. -
? , -
. . -
- , ?
,
, . - ?
18 . % - ,
, , , -
,
. -
. -
, - , ,
. , -
,
, . -
, , Pu,
. , -
9. .
, -
-
. - . -
. -
223

2006 . -
. / ,

( ) 800, -
. .
/- ,
- , -
[, , 2005]. [Uhlir et al., 2002].
- ,
. (U, PuTh) , -

( ). - . -

:
.
-
, , - (. 18.11).
, - , -
. .
- , -
. .
1960
. MSRE [OECD/NUCLEAR.., 2004] -
, - BRII [Stevenson, 1987].
1970
. - [OECD/NUCLEAR..,
2004], 19902000 . -
.
- 60 [Bychkov et al., 19971; Bychkov et al., 19972].
, -
,
.
, - 18.6.
,
-
DOVITA [Bychkov et al., 1997 1 ; :
Bychkov et al., 1997 2 ].
: 1.
e, , -
, - ,
.
, - . , -
. 18.10 (. )
, 1520 % , 100200 , ,
, , , -
. ( ),
- 100000 10005000 .
. U, Pu Np , -
( Am) . - -
Am, Cm , ()
34 - .
2.
. .
Am Cm -
-
, - .
. , -
,
DOVITA 1992
224 18

. 18.11. .

. -
,
.
, - ,
. -
3. , .
- -
- .
, . 7. , -
,
.
- -
.
, , , - , -
(IMF)
. , -
4. ,
- ,
- .
- 8. , -
. , -
.
. ,
5. -
, ,
, . -
- ,

. . -
, , -
. - , -
, - ,
, - . -
.
6. ,
. .

- ( ) -
- .

. ,
, -
- .
. -
, - .
- -
- .

.

,
-
-
.
-
. - ,
- .
,
, ,
. - ,
, ,
. .
-
, :
. ,
/; -
, - 95 % -
- ,
. ; ,
, ;
, -
90 % ,
, , - -
, ,
. . - ;
-
. ,
226

- ,
(); - . -
- -
;
, - .
, -
.
. -
- -
, -
, ,
. -
, ,
, - .

1000 , , 1000 -
. , - -
-
.
-
-
. , -
.
,
-
,
- 5001000 , -
137Cs,
- 90
Sr, 241Pu.
. ,
,
. .
-
, c -


. -
:
-
: -
-
;
, - ; -
. ; -
: -
, ;
.
, . -
- -
. , -
, -

,
, - ,
, , .
-
.
-
.
227

-
,
. ,
,
- ,
: ) , ) .
, ) .

, -
. - ,

, , -
, ,
,
, -
. - -
- .
, ,
() .
. -
- .

- .
- ,
,

. - (, -
, , ,
95 % (), .),
.
. -
- -
(, ) ,
-
. -
- ,
- ,
, -
, - .
.
( ) .
400500 -
,
. -
, -

, -
.
- -
- , ,
- -
, .
, - -
- .
, , - -
. ,
- ,
- -
.
228

-
,

, -
, .
. ,

, ,
.
, .
, -

, - . -
- ,
, .
,
, -
- . -
- -
. ,
. -
. ,
, ,
.
- -
. , -
,
. -
: 85Kr, 3H,
- 14
C, 36Cl, 129I. , -
, -
,
-

, - . ,
,
/. -
,
,
in situ
.
-
( , ) -
,

-
- . -
. - -
(4001000 )
.
( -
). -
. - , -

(-
), , -
, . :
, - , -
. , ,
- ,
,
229

. , -
- .
, ,
, . .
-
, . -
,

, , -
. ,
-


. , -
-
, 10000 .

.
- -
, . -
-
. . ,
, , -
, - ,
, -
, , - . -
. -
, ( ).
. -
,
. 1000
-
. -


(98 %)
: Am Pu,
Np.
-
- , ,
-
. - .

-
,
, -

.
, -
-
, -
.
, ,
.
, -
.
. - , -
- ,
,
230

, - ,

. .

,
.

-
400 ,
, -

, -
, - ,
, - -
.
. , -
,
U Pu.
,
,
,
, .
-
- : -
, -
,
, - , ,

- -
,
. .
-
,
, , - -
,
.
. 25
-
- , , -
.

, .
. -
, - ,
, -
. .
- ,
, -
, ,

- .
. -
-
- 12001300 , -
, -
- 15001600 .
. -
- ,
, , ,
231

. .



. - .
1020 . %, , -
- .
3050 . %. , -
95 % , -
- ,
. Pu, Am, Cm, -
Np, Th, REE, Nb, Zr - .
. - -
300 . -
. Tc, Se,
I, Cs, Sn, Sr
. .
- -
: -
. -
5001000 , - , ,
-
, 98 % - .
Pu Am.
-
, - .
-
- , -
400 , -
,
- . -
. , -
, 200500 300
. -
-
-
,
.
, -
- , -
() , -
, . ,

.
, ,
- , -
. -
, .
-
, -
- ,
. , -
. -
, ,
- -
(),
,
. .
, -
.
232

, -
-
, , -
: ( )
. -
, -
-
. - -
.

,
, ,
. .
-
-
.
.
, -

-
-
,
-
, -
( )
,
1967 ., - -
.
, - -
,
- -
. .
, - -
.
,
,
-
-
.

-
, -
, -
200 ,
, - .
, - ,
, ,
, . -
.
,
- , -
, .
, -
. , ,
, - -
. -
,
, . , -
. () , ,
233

- . -
. ,
,
.
-
/ - .
- -
, ,
.
- -
.
- (20072010 .).
-
, ,
, - ,
.
,
. .
-
,
-
-
.


. , -
, -
, , 100200 ,
, -
( ). ,
. 100000 10005000 .
- ,
- ,
- -
. ,
, - -
,
.

1. .., .., .. // . .: ,
1984. . 180189.
// -
10. . .: ,
.
1987. 312 .
. 1997. 1. C. 1830.
11. .., .., ..
2. .., .., .., ..

-
// -
// . 1977. 2. . 156159.
.
3. .., .., .. . - . 1998. 4. . 314.
//
12. .., .., .. -
. : ,

1988. . 106113.
// .
4. .., .., .., . 1997. 4.
.. . 6874.
// .
13. .., .. -
1973. 12. . 2939.

5. .., .., .., // .
.. . .: , 1982. . . . 69109.
. .: , 1966. 221 .
14. .., .. -
6. .. - -
// . 1987. . 63. . 4.
( - . 277279.
) // . 2002. 6. . 506516.
15. .., .., .. . -
7. .., .., .., .. .
-
-
// -
// . 3
. . . . 1998.
.: . .., 1999. . 1418 2002 . . . 20021.
. 1423. UCRLID149341. . 6568.
8. .., .., .. - 16. .., .., .. . -
- -
// . :
1982. 3. . 3138. //

9. .., .., ..
. 3 -

.
235

1418 2002 . . . 20022. UCRLID149341. // . . 4 . .


. 113123. 2003. 2025 2003 . , 20033.
C. 3132.
17. .., .., .. .
(Y,Gd,..)3(Al,Ga,..)5O12 31. .. -
(Y,Gd,..)(Al,Ga,..)O3 : -
// - // . ,
. . 2000. 1415 2003 . ,
1. . 1114. 2005. . 276290.
18. .., .. - 32. .. (IMF)
. // . // , 20001. 10. . 38.
-
. 33. .. (IMF)
1315 2005 . . // , 20002. 11. . 311.

19. .., .., .. . 34. .. (IMF)


- // . 20003. 12. . 311.
// . 35. 5092696. .
. 2002. 2. . .: , 1996. 5 .
. 2935.
36. 500892003. .
20. .. // . 2003. -
7. . 37. . .: . 2003. 6 .
21. .., .., .. . - 37. 521262003. .
-
// Vienna. 1987. JAEA . .:
M294/3. P. 109116. . 2003. 6 .
22. . . 38. .., .., .. .
. .: , 1990. 463 . . .:
23. - . 2000. 415 .
. . . 18 / . 39. .., .., .. //
.. . .: , 1994. 219 . . .: , 1980. . 201218.
24. / . .. - 40. ..
. .: , 1980. 270 . ( ). ,
25. .., .., .. . 1995. 123 .
, - 41. .., .., .., ..
// . -
2001. . 43. 6. . 557562. ()
26. .., .., .. . - //
- .
// . . 15 .
. 1996. 2. . 310. . 1994. . 1. . 9295.

27. .., .., .. . - 42. .. -


1: (Ru, Rh, Pd Ag)
, , // : . . . . . . 2003. 142 .
. . 43. .., .., .., -
1997. 2. . 312. ..
28. .., .., .. . // .
. . 1 (11). 1982. . 1224.
44. .. -
// // -
. . . .: , 1972. . 224257.
20031. 1. . 1419.
45. .., .., .. .
29. .., .., .., .. // -
.
// . 1996. 1. . 1119.
. .
20032. 1. . 513. 46. ..
// -
30. .., .. . .
. 1997. 4. . 38.
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