Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence
Combining nuclear microanalytical, mineralogical, crystallochemical and geochemical approaches, the authors analyze a possibility of natural occurrence of enriched or even pure and superpure rare isotopes that can be extracted from ores. Methods of and results from the investigations of these isot...
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irk-123456789-812222015-05-14T03:01:52Z Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence Valter, A.A. Storizhko, V.E. Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Berlizov, A.N. Применение ядерных методов Combining nuclear microanalytical, mineralogical, crystallochemical and geochemical approaches, the authors analyze a possibility of natural occurrence of enriched or even pure and superpure rare isotopes that can be extracted from ores. Methods of and results from the investigations of these isotope anomalies are presented. На основі поєднання ядерно-фізичних, мінералогічних, кристалохімічних і геохімічних підходів проаналізовано можливість накопичення в природі в суттєво збагаченому і навіть в чистому та надчистому стані деяких звичайно рідкісних ізотопів, що можуть бути відокремлені з руд. Розглянуто методи і результати вивчення таких ізотопних аномалій. Путём сочетания ядерно-физических, минералогических, кристаллохимических и геохимических подхо- дов проанализирована возможность накопления в природе в существенно обогащённом или даже в чистом и сверхчистом виде некоторых обычно редких изотопов, которые могут быть выделены из руд. Рассмотрены методы и результаты исследования подобных изотопных аномалий. 2005 Article Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence / A.A. Valter, V.E. Storizhko, N.P. Dikiy, A.N. Dovbnya, Yu.V. Lyashko, A.N. Berlizov // Вопросы атомной науки и техники. — 2005. — № 6. — С. 142-145. — Бібліогр.: 5 назв. — англ. 1562-6016 PACS: 28.60.+s, 82.80.Jp28. http://dspace.nbuv.gov.ua/handle/123456789/81222 en Вопросы атомной науки и техники Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
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Применение ядерных методов Применение ядерных методов |
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Применение ядерных методов Применение ядерных методов Valter, A.A. Storizhko, V.E. Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Berlizov, A.N. Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence Вопросы атомной науки и техники |
| description |
Combining nuclear microanalytical, mineralogical, crystallochemical and geochemical approaches, the authors
analyze a possibility of natural occurrence of enriched or even pure and superpure rare isotopes that can be extracted
from ores. Methods of and results from the investigations of these isotope anomalies are presented. |
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Article |
| author |
Valter, A.A. Storizhko, V.E. Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Berlizov, A.N. |
| author_facet |
Valter, A.A. Storizhko, V.E. Dikiy, N.P. Dovbnya, A.N. Lyashko, Yu.V. Berlizov, A.N. |
| author_sort |
Valter, A.A. |
| title |
Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence |
| title_short |
Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence |
| title_full |
Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence |
| title_fullStr |
Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence |
| title_full_unstemmed |
Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence |
| title_sort |
nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence |
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
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2005 |
| topic_facet |
Применение ядерных методов |
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http://dspace.nbuv.gov.ua/handle/123456789/81222 |
| citation_txt |
Nuclear-analytical and mineralogical principles and techniques for prediction and investigation of the native-pure rare isotope occurrence / A.A. Valter, V.E. Storizhko, N.P. Dikiy, A.N. Dovbnya, Yu.V. Lyashko, A.N. Berlizov // Вопросы атомной науки и техники. — 2005. — № 6. — С. 142-145. — Бібліогр.: 5 назв. — англ. |
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Вопросы атомной науки и техники |
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NUCLEAR-ANALYTICAL AND MINERALOGICAL PRINCIPLES AND
TECHNIQUES FOR PREDICTION AND INVESTIGATION OF THE NA-
TIVE-PURE RARE ISOTOPE OCCURRENCE
A.A. Valter1, V.E. Storizhko1, N.P. Dikiy2, A.N. Dovbnya2, Yu.V. Lyashko2, A.N. Berlizov3
1Institute of Applied Physics, National Academy of Sciences of Ukraine, Sumy, Ukraine
e-mail: avalter@iop.kiev.ua
2National Science Center “Kharkov Institute of Physics and Technology”, Kharkov, Ukraine
3Institute for Nuclear Research, National Academy of Sciences of Ukraine, Kiev, Ukraine
Combining nuclear microanalytical, mineralogical, crystallochemical and geochemical approaches, the authors
analyze a possibility of natural occurrence of enriched or even pure and superpure rare isotopes that can be extracted
from ores. Methods of and results from the investigations of these isotope anomalies are presented.
PACS: 28.60.+s, 82.80.Jp28.
INTRODUCTION
By the middle of the XXth century the importance of
the isotope enrichment and pure and superpure isotope
production to the further development of civilization has
been generally recognized. At present isotope starting
materials are employed in atomic industry; from stable
isotopes a wide spectrum of tracer atoms are obtained,
e.g. to produce various radioactive isotopes for thera-
peutic and diagnostic purposes in medicine. Isotope
shifts exhibited by different properties of materials can
be used for providing security of bank notes, documen-
tation, all sorts of information, for controlling laser sys-
tems, etc. Pure isotopes have use in nuclear and other
fields of research, suggesting that in the XXIst century,
most of them if not all stable and long-lived isotopes
now numbering 288 [1], will find applications.
Isotope separation is an expensive process, so pure
isotopes, especially rare ones cost from ten to hundred
thousand times more than a corresponding mixture of
natural isotopes of similar purity. Thus, a search for and
utilization of anomalously enriched natural isotopes
might be very promising.
The ratio of radioactive isotopes and derived thereof
radiogenic isotopes conserved in hard minerals and nat-
ural glasses is extensively applied to dating geologic
formations.
SPECIFYING THE RANGE OF SEARCH
FOR NATIVE PURE RARE RADIOGENIC
ISOTOPES
Pure stable radiogenic isotopes can be formed in the
course of natural radioactive transformations in which
radiogenic nuclides produce atoms with chemical prop-
erties differing from those of atoms whose nuclei under-
go the transformations. If the event takes place in miner-
als, the newly formed atoms may be "conserved" in the
mineral structure. The newly formed atoms may belong
to an abundant or trace element present in the crystal or
to an element that cannot be detected with most sensi-
tive detection techniques. In the latter case to be dis-
cussed here, a new element formed in the crystal as a re-
sult of a radioactive decay is accumulated as a pure iso-
tope. In this situation the crystal structure and geochem-
ical history of the mineral formation should be favorable
for accumulation of a radioactive element, but unfavor-
able for occurrence of an element to which a radiogenic
isotope belongs.
For example, three-layer packets in the mica struc-
ture (Fig. 1) are joined by large univalent cations, K+1. If
a mineral-forming medium includes rare alkalis whose
atoms also constitute large cations (Rb+1, Cs+1), they can
substitute potassium isomorphically. At the same time,
in the mica structure there is no position to be occupied
by a large divalent ion of strontium whose original con-
tent in mica is very low. 87Sr produced via a beta-decay
of 87Rb is probably held in the structure due to the defect
formation with the local substitution of (OH)- for O2.
Radioactive decays favoring the accumulation of
rare stable isotopes depend on the concentration of the
original radioactive nuclide (Cpa) and the ratio of its half
period (T1/2) and the host mineral age (t):
Cpr=Cpa·[exp(tn2·t/T1/2)-1], where Cpr is the radiogenic
isotope content in the mineral matrix.
To identify possible rare isotopes that can be pre-
served in pure form in mineral matrices certain bound-
ary conditions for their accumulation were considered.
MINIMAL RADIOACTIVE ATOM HALF-PE-
RIOD REQUIRED FOR RADIOGENIC ISO-
TOPE ACCUMULATION
Even the age of oldest earth minerals is far smaller
than that of their constituent atoms. The Solar System
age and the minimum age of its matter is approximately
4.8 billion years. Planets including our Earth are 4.5 bil-
lion years old. The first half-billion years of Earth's life
have recently been termed the "Hades era" from the old-
Greek word "Hades" which in ancient mythology was
the name of a place where souls went after death, i.e.
hell of a kind.
This term reflects a modern idea of the conditions on
Earth at that time: heavy meteorite "bombing", with
catastrophes of planetary scale following one after an-
other and the whole Earth mass to the depth of tens of
kilometers from the surface being many times shifted,
mixed and melted.
142 PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2005, № 6.
Series: Nuclear Physics Investigations (45), p. 142-145.
Fig. 1. A diagram of radiogenic strontium location in
the Rb bearing biotite structure (K,Rb)(Mg,Fe)3[(Al-
Si3)O10](OH,F)2
Thus, on early Earth long-lived radioactive nuclei
could not be found in more or less long-lived crystals
and their decay products could not be accumulated in a
hard matrix. The onset of a more quiet period in Earth's
history is displayed in the age of the oldest rocks that by
modern estimates approaches 3.7…4.0 billion years.
Relatively abundant are rocks (3.7…3.4)⋅109 years old.
Somewhat younger are the oldest ores, i.e. natural for-
mations of contrasting chemical composition enriched
by certain chemical and mineral components and thus
suitable for extractions. The oldest ores are (3.0…3.4)⋅
109 years of age. This is precisely the age of the oldest
rocks and ores of the Ukrainian Shield [2] that occupies
an area of about 200 thousand km2, i.e. one-third of the
Ukrainian territory (Fig. 2).
Fig. 2. Location of the Ukrainian Shield (shaded)
Thus, the age of nuclides, including radioactive one,
exceeds the age of the oldest minerals by at least (0.8…
1.1)⋅109 years for rocks and (1.4…1.8)⋅109 years for
ores.
To specify boundary conditions for the search for ra-
diogenic isotopes "conserved" in the ancient mineral
structure we assumed the minimum time interval be-
tween the production of a nucleus and its fixation in a
certain solid (crystalline) phase to be 109 years in a first
approximation. The fraction of the initial radioactive
atom preserved after the time, t, is determined by the
equation C=1/2(t/T) where C is the radioactive atom con-
centration in terms of the initial concentration after the
time, t, for the half-period, T1/2. So in the exponent we
have the number of half-periods within the time elapsed
since the nuclide production. In our case it is 109 years.
Hence, even with a 100% initial concentration after a
billion years the ppm or higher contents would be pre-
served only by radioactive nuclei with half-periods
longer than 100 million years.
Since the initial concentration of radioactive atoms
in minerals is invariably much lower than unity (most
frequently by as much as a factor of 10) this figure can
be taken to be the lower limit of the half-period value in
the investigation of possible cases of rare radiogenic
isotope accumulation in mineral matrices.
PREDICTIONS FOR ACTIVE NATURAL EN-
RICHMENT OF RARE ISOTOPES INCLUD-
ING POSSIBLE FORMATION OF PURE
AND SUPERPURE ISOTOPE
We have performed a search for natural nuclides that
via a radioactive decay can generate nuclides of new el-
ements, which in turn can produce in minerals suffi-
ciently high concentrations of radiogenic isotopes to be
reliably detected. The lower limit of the half-period is
assumed to be equal to 108 years as pointed out above.
The typical life time of the oldest minerals was as-
sumed to be 3⋅109 years.
Analyzing the data and bearing in mind that there
may be more than one decay channel, we found 30
preservations in minerals of 28 radiogenic stable iso-
topes in concentrations that in cases of favourable min-
eral compositions can be determined using modern tech-
niques. The examination of the present-day mineralogy
data permits us to predict certain abundant mineral for-
mations most advantageous for the radiogenic isotopes
to accumulate (Table).
From these, for 10 nuclides, with considerable iso-
tope enrichment, the pure isotope formation is not possi-
ble for cristallochemical and geochemical reasons.
Thus, due to the presence of invariably two uranium iso-
topes in minerals, two radiogenic lead isotopes (206Pb,
207Pb) cannot be present there in the pure form.
The accumulation of pure radiogenic isotopes of rare
earth produced via a decay of radiogenic nuclides of this
group, is impossible because of the chemical proximity
and permanent coexistence of elements belonging to
this group in the mineral crystals.
8 isotopes can be contained in mineral matrices in
the pure form in concentrations above the ppm range,
suggesting a possibility of their extraction as monoiso-
tope products by means of modern technologies. 6 iso-
topes can be present in mineral matrices in the pure
form in concentrations ranging from ppm to ppb. 4 iso-
topes can be found in concentrations from 10-9 to 10-11.
The table highlights occurrences of pure isotopes
that are easy to identify with modern analytical tech-
niques and amenable to extraction from ores by conven-
tional physicochemical and chemical enrichment proce-
143
dures. Presented separately are isotopes that can be ex-
tracted from the Ukrainian ores.
144
Predicted radiogenic isotope enrichment of minerals (for ore age of 3 billion years)
Origi-
nal iso-
tope
Atom percent
abundance
Decay type* Half-peri-
od, years
Newly
formed
isotope
Predicted
content in
mineral,
mass %
Possible mineral matrix (Simplified
Formula)
40К 0.0117 B (89,28%) 1,27⋅109 40Са 0,0n Halides, Potassium Silicates
40 K 0,0117 EC(10,72%) 1,27⋅109 40Ar 0,0n As above
48Cа 0,187 2В 5⋅1019 48Ti 2⋅10-11 Calcite (CaCO3) and other carbonates
50V 0,25 B (17%) 1,4⋅1017 50Cr 5⋅10-11 Vanadium-oxides, Vanadium-bearing
аcmite (Na(Fe,V) Si2O6)
50V 0,25 EC (83%) 1,4⋅1017 50Ti 2,4⋅10-10 As above
50Cr 0,25 2EC 1,8⋅1017 50Ti 3,5⋅10-8 Chromite (Fe Cr2O4)
87Rb 27,835 B 4,88⋅1010 87Sr 0,0n Micas (see text), Pollucite
(Cs,Na,Rb)2 Al2Si4O12
96Zr 2,8 2B 3,9⋅1019 96Mo 1,5⋅10-10 Zircon (ZrSiO4)
100Мо 9,63 2B 2⋅1019 100Ru 10-9 Molybdenite (MoS2)
113Cd 12,22 B 9,3⋅1015 113In n⋅10-8 Sphalerite (ZnS)
115In 95,71 B 4,41⋅1014 115Sn 4,5⋅10-6 Rare minerals of In, cassiterite (SnO2)
123Те 0,908 EC >1013 123Sb <8⋅10-5 Tellurides
138La 0,0902 EC (66,4%) 1,05⋅1011 138Ba 7,5⋅10-4 Monazite1, Britholite2
138La 0,0902 В (33,6%) 1,05⋅1011 138Ce 5⋅10-4 As above
142Ce 11,08 2B >5⋅1016 142Nd 10-9 As above
144Nd 23,8 A 2,29⋅1015 140Ce 10-6 As above
147Sm 15 A !,06⋅1011 143Nd 10-3 As above
148Sm 11,3 A 7⋅1015 144Nd 10-6 As aboveе
149Sm 13,8 A >2⋅1015 145Nd 10-6 As above
152Gd 0,2 A 1,08⋅1014 148Sm 10-7 As above
174Hf 0,162 A 2⋅1015 170Yb 10-7 Zircon (ZrSiO4)
176Lu 2,59 B 3,7⋅1010 176Hf 10-3 Monazite1, Britholite2
184W 30,642 A >3⋅1017 180Hf 10-7 Wolframite (Fe,Mn)WO4
186Os 1,58 A 2⋅1015 182W 10-7 Osmiridum (Ir,Os)
187Re 62,6 B 4,12 1010 187Os 10-4 Molybdenite (MoS2)
187Re 62,6(<1⋅10−4%) A 3⋅1010 183W 10-9 As above
190Pt 0,01 А 6,5⋅1011 186Os 10-4 Platinum (Pt)
232Th ∼100 Decay chain 1,40⋅ 1010 208Pb 0,01 Thorianite (ThO2), Monazite1
235 U 0,72 As above 7,04 ⋅ 108 207Pb 1,7⋅10-3 Utaninite (UO2)
238U 99,275 As above 4,47⋅ 109 206Pb 0,037 As above
* Type of decay: (A) α-decay, (B) β-decay, (2B) double β-decay, (EC) electron capture, and (2EC) double electron capture.
• Bold Roman type: pure rare isotope occurrences easily identifiable with modern analytical techniques;
Bold italics: pure isotope occurrences in Ukrainian ores already found and those to be identified.
• Normal type: isotope enrichment with possible formation of pure isotopes in concentrations below the detection
limit of conventional modern techniques.
• Crossed type: active isotope enrichment, but without pure isotope production.
1Monazite (Ce,La, Nd…Lu, Th)PO4,, 2Britholite (Ca, Ce, La, …Lu)5 (SiO4, PO4)3 (OH,F)
IDENTIFIED PURE RADIOGENIC ISOTOPES
• Ancient rocks and ores are the most suitable objects
for investigations of the pure rare isotope produc-
tion from initial radioactive isotopes present in suf-
ficient concentrations. As mentioned above, a con-
venient testing ground for these studies is the
Ukrainian Shield where we work with minerals (2
…3)⋅109 years old. Since in most cases, especially
in those of practical interest, pure isotopes are pro-
duced via a β-decay or electron capture, direct
mass-spectrometry techniques are not applicable to
the search and identification of pure isotopes pro-
duced. Simple, (in this application) fast and nonde-
structive analytical methods are activation tech-
niques. Mostly the gamma-activation analysis was
employed performed with high-current linacs at the
KFTI NSC [3-5] and complemented by neutron-ac-
tivation techniques with chemically prepared sam-
ples and also by using experimental neutron activa-
tion methods at the research reactor WWR –M of
the INR. This combination permitted the concentra-
tions of the radiogenic and one of nonradiogenic
isotopes to be determined whereof the radiogenic
isotope purity was calculated.
In molybdenite from the Ukrainian Shield the un-
precedented osmium-187 purity (99.995%) was discov-
ered, natural abundance being 1.64%. The distribution
of this element in mineral was found to be consistent
with the solid solution model. A possible crystallochem-
ical mechanism underlying strong radiogenic osmium
retention in molibdenite was examined which consists
in that the recoil atom occupies a vacant octahedron in
the crystal structure (Fig. 3) slightly modifying it to pro-
duce a defect.
145
A high degree of purity (above 96%, with natural
abundance of 7%) was also determined for radiogenic
strontium-87 in rubidium-bearing biotites.
It is intended to use minerals of the Ukrainian Shield
to identify other naturally-pure isotopes formed in min-
eral matrices of foreign composition.
Fig. 3. Diagram of the impurity Re and Os atom loca-
tion in the molybdenite structure
CONCLUSIONS
1) The range of search for native pure rare ra-
diogenic isotopes which can be extracted as
monoisotope products by means of modern tech-
nologies has been specified.
2) The methods for investigation of such iso-
topic anomalies were proposed.
3) The existence of pure 187Os and 87Sr isotopes
in the Ukrainian ores was found.
ACKNOWLEDGEMENTS
The authors wish to thank Dr. M.F. Vlasov for use-
ful discussions, Dr. S. Yudina for translation of the
manuscript into English and A.I. Pisansky for prepara-
tion of the figures.
This work was done under the financial support of
the Fundamental Research Foundation of Ukraine
(Project № 02.07/199).
REFERENCES
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2. N.P. Tserbak, E.V. Bibikova, V.M. Skobelev,
D.N. Tserbak. Evolution in time and metallogenic
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ЯДЕРНО-ФИЗИЧЕСКИЕ И МИНЕРАЛОГИЧЕСКИЕ ПРИНЦИПЫ И МЕТОДЫ ПРОГНОЗИРОВА-
НИЯ И ИССЛЕДОВАНИЯ СЛУЧАЕВ СУЩЕСТВОВАНИЯ РЕДКИХ ИЗОТОПОВ В ПРИРОДНО-
ЧИСТОМ СОСТОЯНИИ
А.А. Вальтер, В.Е. Сторижко, Н.П. Дикий, А.Н. Довбня, Ю.В. Ляшко, А.Н. Берлизов
Путём сочетания ядерно-физических, минералогических, кристаллохимических и геохимических подхо-
дов проанализирована возможность накопления в природе в существенно обогащённом или даже в чистом и
сверхчистом виде некоторых обычно редких изотопов, которые могут быть выделены из руд. Рассмотрены
методы и результаты исследования подобных изотопных аномалий.
ЯДЕРНО-ФІЗИЧНІ І МІНЕРАЛОГІЧНІ ПРИНЦИПИ І МЕТОДИ ПРОГНОЗУВАННЯ І ВИВЧЕННЯ
ВИПАДКІВ ІСНУВАННЯ РІДКІСНИХ ІЗОТОПІВ У ПРИРОДНО-ЧИСТОМУ СТАНІ
А.А. Вальтер, В.Ю. Сторіжко, М.П. Дикий, А.М. Довбня, Ю.В. Ляшко, А.М. Берлізов
На основі поєднання ядерно-фізичних, мінералогічних, кристалохімічних і геохімічних підходів
проаналізовано можливість накопичення в природі в суттєво збагаченому і навіть в чистому та надчистому
стані деяких звичайно рідкісних ізотопів, що можуть бути відокремлені з руд. Розглянуто методи і
результати вивчення таких ізотопних аномалій.
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2National Science Center “Kharkov Institute of Physics and Technology”, Kharkov, Ukraine
INTRODUCTION
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