Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr
За допомогою малокутового розсiяння нейтронiв (МКРН) дослiджено структурнi переходи в потрiйнiй рiдиннiй системi тетрадецилтриметиламонiй бромiд–D2О–NaBr у широкому дiапазонi температур, тискiв i концентрацiй солi. Побудовано фазовi P–T дiаграми переходу колоїдної мiцелярної рiдинної системи в колої...
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Відділення фізики і астрономії НАН України
2010
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| Cite this: | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr / Л.А. Булавін, О.І. Іваньков, А.Х. Ісламов, А.І. Куклін // Укр. фіз. журн. — 2010. — Т. 55, № 4. — С. 412-416. — Бібліогр.: 13 назв. — укр. |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1859953681014718464 |
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| author | Булавін, Л.А. Іваньков, О.І. Ісламов, А.Х. Куклін, А.І. |
| author_facet | Булавін, Л.А. Іваньков, О.І. Ісламов, А.Х. Куклін, А.І. |
| citation_txt | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr / Л.А. Булавін, О.І. Іваньков, А.Х. Ісламов, А.І. Куклін // Укр. фіз. журн. — 2010. — Т. 55, № 4. — С. 412-416. — Бібліогр.: 13 назв. — укр. |
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| description | За допомогою малокутового розсiяння нейтронiв (МКРН) дослiджено структурнi переходи в потрiйнiй рiдиннiй системi тетрадецилтриметиламонiй бромiд–D2О–NaBr у широкому дiапазонi температур, тискiв i концентрацiй солi. Побудовано фазовi P–T дiаграми переходу колоїдної мiцелярної рiдинної системи в колоїдну систему типу суспензiя за рахунок структурного переходу мiцели–кристалiти (преципiтати). Показано, що додавання солi не веде до змiни нахилу лiнiї фазової рiвноваги мiцелярна колоїдна система–суспензiя з преципiтатами, який дорiвнює 53 бар/К. Показано, що пiдвищення концентрацiї солi викликає зсув вказаної лiнiї фазової рiвноваги в бiк бiльших температур та менших тискiв.
С помощью малоуглового рассеяния нейтронов (МУРН) исследованы структурные переходы в тройной жидкостной системе тетрадецилтриметиламмоний бромид–D2O–NaBr в широком диапазоне температур, давлений и концентраций соли. Построены фазовые P–T диаграммы перехода коллоидной мицеллярной системы в коллоидную систему типа суспензия за счет структурного перехода мицеллы–кристаллы (преципитаты). Показано, что добавление соли не ведет к изменению наклона линии фазового равновесия мицеллярная коллоидная система–суспензия с преципитатами, который равен 53 бар/К. Показано, что повышение концентрации соли вызывает смещение указанной линии фазового равновесия в сторону больших температур и меньших давлений.
Structure transitions in the triple liquid system tetradecyltrimethylammonium bromide–D2O–NaBr are studied by the method of small-angle neutron scattering (SANS) in wide ranges of the temperature, pressure, and salt concentration. The phase P–T diagrams of the transition of the colloidal micellar liquid system to a colloidal system of the suspension type through a structural micellae–crystals (precipitates) transition are constructed. It is shown that the addition of the salt does not result in a change of the slope of the line of phase equilibrium between a micellar colloidal system and a suspension with precipitates which is equal to 53 bar/K. It is shown that an increase in the salt concentration causes a shift of the line in the direction of higher temperatures and lower pressures.
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| first_indexed | 2025-12-07T16:18:16Z |
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SOFT MATTER
410 ISSN 2071-0194. Ukr. J. Phys. 2010. Vol. 55, No. 4
STRUCTURE TRANSFORMATIONS IN THE TRIPLE
LIQUID SYSTEM TETRADECYLTRIMETHYLAMMONIUM
BROMIDE–D2О–NaBr
L.A. BULAVIN,1 O.I. IVANKOV,1, 2 A.KH. ISLAMOV,2 A.I. KUKLIN2
1Taras Shevchenko National University of Kyiv, Faculty of Physics
(1 Build., 2, Academician Glushkov Ave., Kyiv 03022, Ukraine)
2Joint Institute of Nuclear Research, I.M. Frank Laboratory of Neutron Physics
(6, Joliot-Curie Str., Dubna 141980, Russia)
PACS 61.05.fg
c©2010
Structure transitions in the triple liquid system tetradecyltrimethy-
lammonium bromide–D2O–NaBr are studied by the method of
small-angle neutron scattering (SANS) in wide ranges of the tem-
perature, pressure, and salt concentration. The phase P–T di-
agrams of the transition of the colloidal micellar liquid system
to a colloidal system of the suspension type through a structural
micelles–crystals (precipitates) transition are constructed. It is
shown that the addition of the salt does not result in a change
of the slope of the line of phase equilibrium between a micellar
colloidal system and a suspension with precipitates which is equal
to 53 bar/K. It is shown that an increase in the salt concentration
causes a shift of the line in the direction of higher temperatures
and lower pressures.
1. Introduction
The necessity to study cationic surfactants is related,
to the first turn, to their wide use in industry and in
various branches of science. In biology, cationic surfac-
tants are widely applied in the separation of DNA (RNA)
[1], protection of DNA from enzymatic cleavage, extrac-
tion of membrane proteins from cells and plasmids, etc.
The important role is played by the possibility to sta-
bilize nanoparticles by cationic surfactants, which pre-
vents their agglutination and precipitation. In addition,
cationic surfactants are efficient anticeptics. We men-
tion also their catalytic action on the reactions with the
participation of polyamides and polycarbonates [2, 3].
The application of surfactants in industry is related, to
the first turn, to their use in the production of various
detergents [4].
Such wide field of the use of cationic surfactants
requires the detailed study of properties of systems
formed with the participation of surfactants under
various thermodynamic conditions on the molecular
level. It is known that cationic surfactants partici-
pate in the creation of crystalline structures, the so-
called precipitates, in liquid systems at certain val-
ues of the pressure, concentration of surfactants, and
temperature (lower than the Kraft temperature) [5–
7]. In work [7], the authors investigated the transition
micelles–precipitates with the participation of cationic
surfactants – tetradecyltrimethylammonium bromide
C14H29N(CH3)3Br (TTAB) within the method of small-
angle neutron scattering and the method of Raman spec-
troscopy. The dependence of the pressure on the temper-
ature on the line of phase equilibrium between a liquid
system with micelles and a liquid system with crystallites
for the micellar liquid system C14H29N(CH3)3Br–D2О
and the triple micellar liquid system C14H29N(CH3)3Br-
D2О–NaBr was studied. The purpose of the present
work is the study of the influence of the salt concen-
tration on the structural transition micelles–precipitates
in the above-mentioned liquid colloid system.
2. Method of Experiments
To realize the posed problem, we choose the diffraction
method, namely the method of small-angle scattering
of slow neutrons which allows one to trace a change in
the structure of a colloid micellar liquid system occurring
under the action of the pressure and the temperature. As
a micellar liquid system, we took the system TTAB-D2O
STRUCTURE TRANSFORMATIONS IN THE TRIPLE LIQUID SYSTEM
which was earlier studied in [7]. To this micellar system,
we add salt NaBr in order to trace the influence of the
salt concentration on the structural transition micelles-
precipitates.
For the experiments, we prepared the liquid sys-
tem TTAB-heavy water with a TTAB concentration of
50 mM. To this micellar system, we add the NaBr ad-
mixture. As a result, we obtained triple liquid systems
TTAB-heavy water-NaBr with NaBr concentrations of
25, 50, 100, 200, and 800 mM.
In order to prepare micellar liquid systems of surfac-
tants, we took dry TTAB of the Sigma-Aldrich Co. (a
content of TTAB equals 99%) and D2O of the Izotop
firm (Moscow) (a content of D2O equals 99.8%).
At the normal pressure, we placed specimens in quartz
Hellma cuvettes with a neutron path length of 1 mm or
2 mm. To study of the influence of the pressure, tem-
perature, and concentration of electrolyte admixtures on
the structural state of the system under study, the speci-
mens were placed in a thermostatted chamber with high
hydrostatic pressure [8]. In this case, the temperature of
specimens was maintained with the help of a thermostat
of the Lauda firm to within ±0.1 ◦C.
The SANS experiments were carried out on a modern-
ized spectrometer YuMO [9] in a two-detector version
[10, 11]. The spectrometer is positioned at the IBR-2
pulse reactor of the Joint Institute of Nuclear Research
(Dubna, Russia). The available experimentally interval
of the wave vectors q was 7× 10−3Å−1–1.4×10−1Å−1.
We registered the curves of small-angle neutron scat-
tering at various pressures, temperatures, and concen-
trations of the NaBr admixture in the indicated system
with regard for its diagram of state. As is known [4],
one of the main characteristics of the diagrams of state
of liquid systems with surfactants is the Kraft line, on
which the structural transition in a colloid liquid system,
namely the transition of the colloids of micelles into the
colloids of crystallites, occurs.
To determine the influence of the salt admixture in
the liquid system with cationic surfactants on param-
eters of such structural transition, we investigated the
small-angle neutron scattering in the interval of thermo-
dynamical parameters which includes the Kraft line.
The experiment was performed as follows: a speci-
men was heated to a temperature higher than the Kraft
temperature, and then the temperature was decreased.
In this case, we registered the scattering pattern with
an exposure of 10 min. If no variations in the neutron
scattering curve happened during 20 min, then the tem-
perature was decreased further.
Fig. 1. Intensity of small-angle neutron scattering at the pressure
P = 320 bar when the temperature is higher than the Kraft one,
T = 16 ◦C. The concentration of TTAB is 50 mM. The concen-
tration of NaBr equals 50 mM
3. Results and Discussion
On the first stage, we studied inhomogeneities in the
liquid system with the help of SANS in the case where
the system is in the micellar state.
In Fig. 1, we present the curves of small-angle neutron
scattering for the liquid micellar system with cationic
surfactants and the NaBr admixture. As seen in Fig. 1,
we observe a peak at q ∼ 0.044 Å which corresponds to
the interaction between charged micelles.
Indeed, the neutron scattering intensity in the liquid
system under study can be written in the form
I = n〈|F 2(q)|〉S(q), (1)
where n is the the concentration of particles, and F (q) is
the form-factor corresponding to the intensity of neutron
scattering by a single micelle:
F 2(q) =
[∫
(ρ− ρs) exp(iqr)d3r
]2
, (2)
where ρ and ρs are, respectively, the scattering length
densities of micelles and the solution. In formula (1),
S(q) describes the interaction between micelles and cor-
responds to a certain distribution of the centers of masses
of micelles in space. Just this structural factor is the
cause for the formation of such a peak. The structural
factor S(q) can be given in the form [12]
S(q) = 1 + V −1
[∫
(g(r)− 1) exp(iqr)d3r
]
, (3)
ISSN 2071-0194. Ukr. J. Phys. 2010. Vol. 55, No. 4 411
L.A. BULAVIN, O.I. IVANKOV, A.KH. ISLAMOV et al.
Fig. 2. Intensity of small-angle neutron scattering reflecting the
kinetics of the structural transformation micelles-precipitates at
the steady pressure P=320 bar at the passage across the Kraft
line. T=14 ◦C. The concentration of TTAB is 50 mM, and the
concentration of NaBr is 50 mM
Fig. 3. Photos of the micelles–precipitates transition which are
obtained with a chamber with high hydrostatic pressure for visual
observations
where g(r) is the pair correlation function, and V is a
volume per micelle.
On the second stage of execution of the experiment,
we changed the thermodynamical parameters P and T
so that the system passed the Kraft equilibrium line. We
observed how micelles in such colloid system are trans-
formed into crystallites.
In Fig. 2, we show the curves of small-angle neutron
scattering at once after a decrease in the temperature for
the following time intervals after the start of the decrease
in the temperature: (�) – t=30 min, (•) – t=60 min,
(◦) – t=90 min, (N) – t=120 min, (4) – t=150 min, (H) –
t=180 min, (O) – t=210 min, (?) – t=240 min. It is seen
from Fig. 2 that the kinetics of formation of the solid
phase is manifested in the change in the curves of small-
angle scattering. The peak at q ∼ 0.044 Å disappears
in the course of the time; but, in this case, the neutron
scattering intensity in the region of small q increases.
Fig. 4. Dependence of the pressure on the temperature on the
Kraft line of phase equilibrium for the triple liquid system TTAB–
D2О–NaBr for various contents CNaBr, mM: � – 0; � – 25; • –
50; ◦ – 100; N – 200; 4 – 800. The concentration of TTAB equals
50 mM
The process of structural transition in the liquid sys-
tem (in other words, the micelles-precipitates transition)
was also observed visually. For this purpose, we used a
high-pressure chamber for visual observations. In Fig. 3,
we give the photos showing the micelles-precipitates
transition. The chamber window diameter is about 1
cm, and the distance between windows equals 1 mm. At
the beginning of the process of crystallization, the pre-
cipitates sink on the chamber bottom, but their sizes
did not allow us to see them visually. In the course of
the time, the crystalline structures with significant sizes
are formed. They are shown in the photo (see Fig. 3).
Therefore, with the help of a chamber, we can obtain
the information only about the presence or absence of
the process of crystallization, rather than about its ki-
netics. For example, we see a formed crystal which oc-
cupies a half of the chamber window area in the left
photo. In the middle and right photos, the crystal is
already in contact with the whole surface of a chamber
window.
On the basis of the obtained data on small-angle neu-
tron scattering, we constructed the curves showing the
dependences of the pressure on the temperature on the
line of a phase equilibrium between the micellar system
and a suspension (Fig. 4). As seen from Fig. 4, the slopes
of the lines of phase equilibrium are the same and are
about 53 bar/K.
It follows from Fig. 4 that the addition of the salt
admixture into the micellar liquid system TTAB–D2О
412 ISSN 2071-0194. Ukr. J. Phys. 2010. Vol. 55, No. 4
STRUCTURE TRANSFORMATIONS IN THE TRIPLE LIQUID SYSTEM
Fig. 5. Dependence of the pressure of the phase transition at a
constant temperature on the NaBr admixture concentration in the
liquid system. The concentration of TTAB equals 50 mM. � – 25
◦C, • – 40 ◦C, N – 60 ◦C
causes a shift of the line of phase equilibrium between
the liquid system and the solid to the region of higher
temperatures and less pressures.
We now analyze the dependence of the pressure of
the phase transition on the concentration of NaBr
in the liquid system at various temperatures on the
Kraft line of phase equilibrium. To this end, we
approximated the experimental data on the tempera-
ture dependence of the pressure on the line of equi-
librium for five values of the NaBr concentration in
the liquid system in the studied temperature inter-
val by straight lines. Then, for temperatures of 25
◦C, 40 ◦C, and 60 ◦C, we constructed the depen-
dence of the pressure of the structural transition on
the salt concentration and give it in Fig. 5. It fol-
lows from the figure that, at low concentrations of
NaBr in the system, the realization of the phase transi-
tion requires much higher pressure than that at high
concentrations. For example, at a temperature of
25 ◦C, the ratio of such pressures is ∼1.5. This
is related, first of all, to the sizes of micelles: at
high concentrations of surfactants, the strongly elon-
gated cylindrical micelles are formed [13], and the cre-
ation of large aggregates requires a less energy. Fig-
ure 5 indicates that we can trace, on the phase equi-
librium line, the asymptotic behavior of the depen-
dence of the pressure on the NaBr admixture con-
centration in the system for the three given tempera-
tures.
4. Conclusions
Within the method of small-angle neutron scattering,
we have studied the structural transformations micelles–
precipitates in the micellar liquid system TTAB-heavy
water in a wide interval of temperatures and pres-
sures at various concentrations of NaBr in the sys-
tem. We constructed the lines of phase equilibrium for
two colloid systems. In one of the systems, the col-
loid is micelles which are formed by molecules of sur-
factants. In the second system, the colloid consists
of crystallites (precipitates) which appeared in the liq-
uid system under the action of the pressure due to
the structural transition. It is shown that the ad-
dition of the NaBr admixture does not influence the
slope of the line of phase equilibrium which is equal
to 53 bar/K. We have found the asymptotic depen-
dence of the behavior of the pressure of the structural
transition on the salt concentration. It is shown that
the addition of the salt into the micellar liquid sys-
tem causes a shift of the line of the structural tran-
sition micelles–precipitates to higher temperatures and
less pressures.
1. M. Goto et al., J. of Chem. Eng. Japan 32, 123 (1999).
2. R. Bakeeva et al., Kinetics and Catalysis 49, 631 (2008).
3. E. Kosacheva et al., Colloid J. 68, 713 (2006).
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Surfactants and Polymers in Aqueous Solutions (Wiley,
New York, 2002).
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(1995).
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994 (2006).
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791 (2006).
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9. Yu.M. Ostanevich, Makromol. Chem., Macromol. Symp.
15, 91 (1988).
10. A.I. Kuklin et al., Poverkhn. 6, 74 (2006).
11. A.I. Kuklin et al., Neutron News 16, 16 (2005).
12. J. Teixeira, in Structure and Dynamics of Strongly Inter-
acting Colloids and Supramolecular Aggregates in Solu-
tion, edited by S.H. Chen, J.S. Huang, and P. Tartaglia
(Kluwer, Dordrecht, 1992), p. 635.
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Received 22.01.10.
Translated from Ukrainian by V.V. Kukhtin
ISSN 2071-0194. Ukr. J. Phys. 2010. Vol. 55, No. 4 413
L.A. BULAVIN, O.I. IVANKOV, A.KH. ISLAMOV et al.
СТРУКТУРНI ПЕРЕТВОРЕННЯ В ПОТРIЙНIЙ РIДИННIЙ
СИСТЕМI ТЕТРАДЕЦИЛТРИМЕТИЛАМОНIЙ
БРОМIД–D2О–NaBr
Л.А. Булавiн, О.I. Iваньков, А.Х. Iсламов, А.I. Куклiн
Р е з ю м е
За допомогою малокутового розсiяння нейтронiв (МКРН) до-
слiджено структурнi переходи в потрiйнiй рiдиннiй системi
тетрадецилтриметиламонiй бромiд–D2О–NaBr у широкому дi-
апазонi температур, тискiв i концентрацiй солi. Побудовано
фазовi P–T дiаграми переходу колоїдної мiцелярної рiдинної
системи в колоїдну систему типу суспензiя за рахунок стру-
ктурного переходу мiцели–кристалiти (преципiтати). Показа-
но, що додавання солi не веде до змiни нахилу лiнiї фазової
рiвноваги мiцелярна колоїдна система–суспензiя з преципiта-
тами, який дорiвнює 53 бар/К. Показано, що пiдвищення кон-
центрацiї солi викликає зсув вказаної лiнiї фазової рiвноваги в
бiк бiльших температур та менших тискiв.
414 ISSN 2071-0194. Ukr. J. Phys. 2010. Vol. 55, No. 4
|
| id | nasplib_isofts_kiev_ua-123456789-13430 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 2071-0194 |
| language | Ukrainian |
| last_indexed | 2025-12-07T16:18:16Z |
| publishDate | 2010 |
| publisher | Відділення фізики і астрономії НАН України |
| record_format | dspace |
| spelling | Булавін, Л.А. Іваньков, О.І. Ісламов, А.Х. Куклін, А.І. 2010-11-08T17:13:41Z 2010-11-08T17:13:41Z 2010 Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr / Л.А. Булавін, О.І. Іваньков, А.Х. Ісламов, А.І. Куклін // Укр. фіз. журн. — 2010. — Т. 55, № 4. — С. 412-416. — Бібліогр.: 13 назв. — укр. 2071-0194 PACS 61.05.fg https://nasplib.isofts.kiev.ua/handle/123456789/13430 538,97 За допомогою малокутового розсiяння нейтронiв (МКРН) дослiджено структурнi переходи в потрiйнiй рiдиннiй системi тетрадецилтриметиламонiй бромiд–D2О–NaBr у широкому дiапазонi температур, тискiв i концентрацiй солi. Побудовано фазовi P–T дiаграми переходу колоїдної мiцелярної рiдинної системи в колоїдну систему типу суспензiя за рахунок структурного переходу мiцели–кристалiти (преципiтати). Показано, що додавання солi не веде до змiни нахилу лiнiї фазової рiвноваги мiцелярна колоїдна система–суспензiя з преципiтатами, який дорiвнює 53 бар/К. Показано, що пiдвищення концентрацiї солi викликає зсув вказаної лiнiї фазової рiвноваги в бiк бiльших температур та менших тискiв. С помощью малоуглового рассеяния нейтронов (МУРН) исследованы структурные переходы в тройной жидкостной системе тетрадецилтриметиламмоний бромид–D2O–NaBr в широком диапазоне температур, давлений и концентраций соли. Построены фазовые P–T диаграммы перехода коллоидной мицеллярной системы в коллоидную систему типа суспензия за счет структурного перехода мицеллы–кристаллы (преципитаты). Показано, что добавление соли не ведет к изменению наклона линии фазового равновесия мицеллярная коллоидная система–суспензия с преципитатами, который равен 53 бар/К. Показано, что повышение концентрации соли вызывает смещение указанной линии фазового равновесия в сторону больших температур и меньших давлений. Structure transitions in the triple liquid system tetradecyltrimethylammonium bromide–D2O–NaBr are studied by the method of small-angle neutron scattering (SANS) in wide ranges of the temperature, pressure, and salt concentration. The phase P–T diagrams of the transition of the colloidal micellar liquid system to a colloidal system of the suspension type through a structural micellae–crystals (precipitates) transition are constructed. It is shown that the addition of the salt does not result in a change of the slope of the line of phase equilibrium between a micellar colloidal system and a suspension with precipitates which is equal to 53 bar/K. It is shown that an increase in the salt concentration causes a shift of the line in the direction of higher temperatures and lower pressures. uk Відділення фізики і астрономії НАН України М'яка речовина Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr Структурные преобразования в тройной жидкостной системе тетрадецилтриметиламмоний бромид–D2O–NaBr Structure Transformations in the Triple Liquid System Tetradecyltrimethylammonium Bromide−D2O−NaBr Article published earlier |
| spellingShingle | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr Булавін, Л.А. Іваньков, О.І. Ісламов, А.Х. Куклін, А.І. М'яка речовина |
| title | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr |
| title_alt | Структурные преобразования в тройной жидкостной системе тетрадецилтриметиламмоний бромид–D2O–NaBr Structure Transformations in the Triple Liquid System Tetradecyltrimethylammonium Bromide−D2O−NaBr |
| title_full | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr |
| title_fullStr | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr |
| title_full_unstemmed | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr |
| title_short | Структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−D2O−NaBr |
| title_sort | структурні перетворення в потрійній рідинній системі тетрадецилтриметиламоній бромід−d2o−nabr |
| topic | М'яка речовина |
| topic_facet | М'яка речовина |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/13430 |
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