Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems
The influence of polyacrlic acid (PAA) adsorption on fumed silica (SiO2) surface on suspension stability has been studied. Сhanges in the suspension stability were monitored using a Turbiscan LabExpert with a TLAb Cooler cooling module at 25oC. PAA is an anionic polymer containing carboxyl groups; t...
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| Опубліковано в: : | Хімія, фізика та технологія поверхні |
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| Дата: | 2010 |
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| Формат: | Стаття |
| Мова: | Англійська |
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Інститут хімії поверхні ім. О.О. Чуйка НАН України
2010
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| Назва журналу: | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| Цитувати: | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems / M. Wiśniewska, K. Terpiłowski, V.I. Zarko, S. Chibowski, E. Chibowski, T. Urban, V.M. Gun’ko // Хімія, фізика та технологія поверхні. — 2010. — Т. 1, № 3. — С. 269-273. — Бібліогр.: 6 назв. — англ. |
Репозитарії
Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1859649049524699136 |
|---|---|
| author | Wiśniewska, M. Terpiłowski, K. Zarko, V.I. Chibowski, S. Chibowski, E. Urban, T. Gun’ko, V.M. |
| author_facet | Wiśniewska, M. Terpiłowski, K. Zarko, V.I. Chibowski, S. Chibowski, E. Urban, T. Gun’ko, V.M. |
| citation_txt | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems / M. Wiśniewska, K. Terpiłowski, V.I. Zarko, S. Chibowski, E. Chibowski, T. Urban, V.M. Gun’ko // Хімія, фізика та технологія поверхні. — 2010. — Т. 1, № 3. — С. 269-273. — Бібліогр.: 6 назв. — англ. |
| collection | DSpace DC |
| container_title | Хімія, фізика та технологія поверхні |
| description | The influence of polyacrlic acid (PAA) adsorption on fumed silica (SiO2) surface on suspension stability has been studied. Сhanges in the suspension stability were monitored using a Turbiscan LabExpert with a TLAb Cooler cooling module at 25oC. PAA is an anionic polymer containing carboxyl groups; therefore all the measurements were carried out at different pH 3, 6 and 9. Analysis of obtained transmission and backscattering curves and Turbiscan Stability Indexes (TSI) allowed determination of the most probable mechanism of the system stability.
Вивчено вплив адсорбції поліакрилової кислоти (ПAК) на поверхні високодисперсного кремнезему (SiO2) на стабільність суспензії. Зміни стабільності суспензії спостерігались за допомогою приладу Turbiscan LabExpert із охолоджуючим модулем TLAb Cooler при 25oC. ПAК є аніонним полімером, що містить карбоксильні групи, тому всі вимірювання проводились при різних рН (3, 6 та 9). Аналіз одержаних кривих перенесення та зворотнього розсіяння, а також індексів стабільності (Turbiscan Stability Indexes (TSI)) дозволив визначити найбільш вірогідний механізм стабілізації вивчених систем.
Изучено влияние адсорбции полиакриловой кислоты (ПAA) на поверхности высокодисперсного кремнезема (SiO2) на стабильность суспензии. Изменения стабильности суспензии наблюдались с помощью прибора Turbiscan LabExpert с охлаждающим модулем TLAb Cooler при 25oC. PAA является анионным полимером, содержащим карбоксильные группы, поэтому все измерения проводились при различных рН (3, 6 и 9). Анализ полученных кривых переноса и обратного рассеяния, а также индексов стабильности (Turbiscan Stability Indexes (TSI)) позволил определить наиболее вероятный механизм стабилизации изученных систем.
|
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Хімія, фізика та технологія поверхні. 2010. Т. 1. № 3. С. 269–273
_____________________________________________________________________________________________
* Corresponding author wisniewska@hektor.umcs.lublin.pl
ХФТП 2010. Т. 1. № 3 269
UDC 544.723
INFLUENCE OF SOLUTION pH ON STABILITY
OF FUMED SILICA–POLYACRYLIC ACID SYSTEMS
M. Wiśniewska1*, K. Terpiłowski2, V.I. Zarko3, S. Chibowski1, E. Chibowski2,
T. Urban1, V.M. Gun’ko3
1Maria Curie-Skłodowska University, Department of Radiochemistry and Colloid Chemistry
2Department of Physical Chemistry-Interfacial Phenomena, Faculty of Chemistry
3 Maria Curie-Skłodowka Square, Lublin 20-031, Poland
3Chuiko Institute of Surface Chemistry of National Academy of Sciences of Ukraine
17 General Naumov Street, Kyiv 03164, Ukraine
The influence of polyacrlic acid (PAA) adsorption on fumed silica (SiO2) surface on suspension stabi-
lity has been studied. Сhanges in the suspension stability were monitored using a Turbiscan LabExpert with
a TLAb Cooler cooling module at 25oC. PAA is an anionic polymer containing carboxyl groups; therefore
all the measurements were carried out at different pH 3, 6 and 9. Analysis of obtained transmission and
backscattering curves and Turbiscan Stability Indexes (TSI) allowed determination of the most probable
mechanism of the system stability.
INTRODUCTION
The conformation of macromolecules ad-
sorbed at a solid-liquid interface influences struc-
ture of a polymer adsorption layer on a metal ox-
ide surface. This structure determines the stabili-
zation-flocculation properties of colloidal systems
which are very important to control many techno-
logical and ecological processes. The interfacial
behavior of metal oxide-polymer solution systems
is substantial for mineral flotation, dispersion-
flocculation of cosmetics, paints, pharmaceuti-
cals, foods, oil recovery, regulation of plough-
lands erosion, purification of the industrial and
drinking water, etc. [1–3]. Polyelectrolytes, in-
cluding a polyacrylic acid classified as an anionic
polymer, are especially appropriate for these pur-
poses, because the suspension stability in the
presence of PAA can be regulated by both steric
and electrostatic forces.
The most important factor influencing the ad-
sorption process of polyacrylic acid on a silica sur-
face is the pH value of the solution. An increase in
pH causes an increase in the dissociation degree of
the carboxyl groups in the PAA chains that leads
to changes in the interactions between adsorbent
active sites and polymer functional groups. Taking
this fact into consideration, the aim of this paper
was to determine the pH influence on the silica
suspension stability.
Silica was chosen for the study because it is a
very popular adsorbent with well defined solid-liquid
interface [4]. Silica gels were widely used as a sta-
tionary phases in chromatography and as a drying
agent, catalyst and catalyst carrier. Moreover, SiO2
finds a great application in production of glass, ce-
ment, and ceramics. Nanosilica (or fumed silica) is
widely used in industry and medicine as powder ma-
terials or compact solids, polymer fillers, cores in
core-polymer shell particles, etc. Nanosilica is a
powder material (bulk density ρb=0.04–0.13 g/cm3
depending on the specific surface area between 300
and 50 m2/g) composed of aggregates (<1 µm in size,
mass fractal dimension Dmf=2.5–2.6) and agglomer-
ates of aggregates (>1 µm in size, Dmf=2.2–2.4).
MATERIALS AND METHODS
Fumed silica (pilot plant of Chuiko Institute
of Surface Chemistry, Kalush, Ukraine) studied
has the BET surface area of 57 m2 g-1 determined
from low-temperature nitrogen adsorption-
desorption isotherm measured using a Micro-
metritics ASAP 2405N analyzer.
Polyacrylic acid (PAA, Fluka) was used at the
average molecular weights of 2, 100, and 240 kDa.
All measurements were carried out in the
presence of NaCl solution (0.01 mol dm-3) which
was used as the supporting electrolyte. Moreover,
the stability experiments were performed at solu-
tion pH=3, 6 and 9 at 25oC.
M. Wiśniewska, K. Terpiłowski, V.I. Zarko et al.
_____________________________________________________________________________________________
270 ХФТП 2010. Т. 1. № 3
The stability measurements of the fumed silica
suspensions without and with PAA were carried
out using a Turbiscan LabExpert with a TLAb Cooler
cooling module. This apparatus possesses an elec-
troluminescence diode which emits collimated
light beam (λ=880 nm) passing through the sus-
pension. The apparatus has two synchronized de-
tectors. A transmission detector recorded light
passing through a probe under angle of 0o in rela-
tion to the incident light direction. The second one
is a backscattering detector registering the light
scattered under angle of 135o. The obtained data
are stored and converted by a computer program.
The results are presented in the form of curves,
which show the intensities of transmission and
scattering as a function of time.
The analyzed suspension in a glass vial (7 cm
in length) was placed in a thermostated measure-
ment chamber. The suspension with 0.02 g of
oxide in 20 cm3 of NaCl solution (solid content
0.1%) was sonicated for 1 min. Then the required
pH of the solution was adjusted. The suspension
was shaken in a water bath for 30 min and the pH
was checked. The changes in the suspension sta-
bility were monitored for 15 h (single scans were
obtained in every 15 min). The probes of the sil-
ica suspension with polyacrylic acid were pre-
pared in the similar way. An appropriate volume
of the PAA solution, desired the surface coverage
θ=1 (CPAA≈500 ppm), was added to the suspen-
sion after sonification.
The Turbiscan Stability Indices (TSI) were
calculated from the experimental results. The TSI
values were obtained using a special computer
program from the following equation
( )
1
1
2
−
−
=
∑
=
n
xx
TSI
n
i
BSi
, (1)
where xi is the mean backscattering for each min-
ute of measurement, xBS is the mean xi, and n is the
number of scans. The TSI is a parameter which
allows the estimation of the suspension stability.
High TSI value indicates that the system is unstable.
RESULTS AND DISCUSSION
The obtained transmission and backscattering
curves for invesigated systems are presented in
Figures 1–3. Calculated values of TSI were
shown in Table 1 and Fig. 4. The analysis of
these data suggests that samples are the most un-
stable at pH 3. The addition of PAA improves
insignificantly the SiO2 suspension stability.
a
b
c
d
Fig. 1. Transmission and backscattering at pH 3 for the
systems: a) SiO2 - NaCl,
b) SiO2 – NaCl - PAA 2 kDa,
c) SiO2 – NaCl - PAA 100 kDa,
d) SiO2 – NaCl – PAA 240 kDa
Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems
_____________________________________________________________________________________________
ХФТП 2010. Т. 1. № 3 271
a
b
c
d
Fig. 2. Transmission and backscattering at pH 6 for the
systems: a) SiO2 - NaCl,
b) SiO2 - NaCl - PAA 2 kDa,
c) SiO2 – NaCl - PAA 100 kDa,
d) SiO2 – NaCl – PAA 240 kDa
a
b
c
d
Fig. 3. Transmission and backscattering at pH 9 for the
systems: a) SiO2 - NaCl,
b) SiO2 - NaCl - PAA 2 kDa,
c) SiO2 – NaCl - PAA 100 kDa,
d) SiO2 – NaCl – PAA 240 kDa
M. Wiśniewska, K. Terpiłowski, V.I. Zarko et al.
_____________________________________________________________________________________________
272 ХФТП 2010. Т. 1. № 3
Table 1. TSI values for SiO2 - PAA systems at different
pH values
TSI System
pH 3 pH 6 pH 9
SiO2 57.75 4.00 3.17
SiO2–PAA
2 000
54.95 5.79 3.17
SiO2–PAA
100 000
43.94 1.56 3.00
SiO2–PAA
240 000
48.62 2.14 2.79
0
5
40
45
50
55
pH = 3
pH = 6
pH = 9
T
ur
bi
sc
an
S
ta
bi
lit
y
In
de
x
a) b) c) d) a) b) c) d) a) b) c) d)
Fig. 4. TSI values at different pH for the systems:
a) SiO2 - NaCl,
b) SiO2 - NaCl - PAA 2 kDa,
c) SiO2 – NaCl - PAA 100 kDa,
d) SiO2 – NaCl – PAA 240 kDa
Completely different situation takes place at
pH 6 and 9 where the suspensions are succes-
sively stable and addition of polymer minimally
influences their stability.
To explain observed features of the sys-
tems stability, it is necessary to analyze the
ionization degree of PAA carboxylic groups and
the SiO2 surface charge density with increasing
pH value. The increase in pH causes dissociation
of the polyacrylic acidic groups. Their dissocia-
tion degree (αd) at pH 3 equals to 0.03. At pH 4.5
(pKPAA=4.5 [5]) αd=0.5 and at pH 7.5 practically
all the PAA macromolecules are fully ionized
(αd=0.999).
Previous investigations indicated that
pHpzc of silica is equal to approximately 3 [6].
It means that the SiO2 surface is negatively
charged in the whole pH range studied from 3
to 9; however, the surface charge density (σ0)
is small at pH < 7. In such a situation, the
electrostatic repulsion between the solid sur-
face and PAA chains appears. Its strength in-
creases with increasing pH. This results in
more and more stretched conformation of the
negatively charged macromolecules on the ne-
gatively charged adsorbent surface. For this
reason the pH increase causes a decrease in
the polymer adsorption [6]. However, the PAA
adsorption on the silica surface occurs in the
whole range of pH, even at the highest values
of pH. It proved that different non-
electrostatic forces had to be responsible of
the PAA adsorption on the SiO2 surface. Other-
wise, the adsorption of negatively charged
polymer chains on the negatively charged sol-
id surface should not take place. The energy of
these interactions [6] corresponds to the en-
ergy of strong hydrogen bonds (40-50 kJ/mol).
These bonds can be formed between both neu-
tral (≡SiOH) or charged (≡SiO−, ≡SiOH2
+) si-
lanol groups of adsorbent and dissociated or
neutral groups of the polymer.
At pH 3 without the polymer, the silica sus-
pension is characterized by much lower stability
(TSI=57.75) as compared to that at pH 6 and 9
(TSI=4.00 and 3.17, respectively). This is caused
by lowering σ0 value, as well as diffusion layer
charges, with decreasing pH close to the point of
zero charge [6]. The repulsive interactions be-
tween solid particles are weak and not able to
provide the system stability; therefore, the coagu-
lation takes place. The addition of PAA insignifi-
cantly improves the dispersion stability. At such
pH, the PAA chains are practically non-
dissociated. The adsorbed macromolecules form
more coiled structures at the silica surface. Such
coils adsorbed on a particle can interact with the
macromolecules adsorbed on other particles or
with bare particles. As a result, large floccules
composed of solid particles covered with a dense-
ly packed polymer layer are formed in the sus-
pension. Thus, a decrease in the silica suspension
stability in the presence of PAA can be due to
bridging interactions PAA-silica and PAA-PAA
leading to flocculation of the system.
Completely different situation is observed
at pH 6 and 9. The systems both in the absence
and in the presence of polymer are stable. The
high stability of silica suspension without
PAA is caused by electrostatic interactions
between negatively charged solid particles.
Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems
_____________________________________________________________________________________________
ХФТП 2010. Т. 1. № 3 273
The adsorption of polyacrylic acid weakly af-
fects the SiO2 suspension stability. Under
these conditions, the polymer chains are com-
pletely dissociated that results in strong elec-
trostatic repulsion between polymer-coated
particles. This effect is additionally strength-
ened by intermolecular repulsive interactions
of dissociated carboxylic groups in non-
adsorbed polymer chains in the solution. As a
result, both steric and electrostatic effects are
responsible of high suspension stability in the
presence of the polymer. Thus, at pH 6 and 9
electrosteric stabilization of the SiO2 – PAA
suspension occurs.
ACKNOWLEDGEMENT
The research leading to these results has re-
ceived funding from the European Community’s
Seven Framework Programme (FP7/2007 – 2013)
under a Maria Curie International Research Staff
Exchange Scheme, Grant Agreement No. PIRSES –
GA – 2008 – 230790.
REFERENCES
1. Sorbie K.S. Polymer-Improved Oil Recovery. –
Boca Raton FL: CRC Press, 1991. – 376 p.
2. Audibert A., Bailey F., Hall P.L et al. Physical
Chemistry of Colloids and Interfaces in Oil
Production / Eds. H. Toulhoat, J. Lecourtier. –
Paris: Editions Technip, 1992. – P. 203–210.
3. Amirtharajah A., O’Melia C.R. Water Quality
and Treatment. – New York: MCGraw-Hill,
1990. – 587 p.
4. Parida S.K., Dash S., Patel S., Mishra B.K.
Adsorption of organic molecules on silica sur-
face // Adv. Colloid Interf. Sci. – 2006. –
V. 121. – P. 77–110.
5. Gebhardt J.E., Furstenau D.W. Adsorption of
polyacrylic acid at oxide/water interfaces //
Colloids Surf. – 1983. – V. 7. – P. 221–231.
6. Wiśniewska M. Temperature effect on adsorp-
tion properties of silica–polyacrylic acid inter-
face // J. Therm. Anal. Cal. – 2010. – DOI
10.1007/s10973-010-0888-4.
Received 18.05.2010, accepted 17.08.2010
Вплив рН розчину на стабільність систем
високодисперсний кремнезем – поліакрилова кислота
M. Вішневська, K. Терпиловський, В. Зарко, С. Хібовський, E. Хібовський, T. Урбан, В. Гунько
Університет Марії Кюрі-Склодовської
пл. Марії Кюрі-Склодовської 3, Люблін 20-031, Польща, wisniewska@hektor.umcs.lublin.pl
Інститут хіміі поверхні ім. О.О. Чуйка Національної академії наук України
вул. Генерала Наумова 17, Київ 03164, Україна
Вивчено вплив адсорбції поліакрилової кислоти (ПAК) на поверхні високодисперсного кремнезему (SiO2)
на стабільність суспензії. Зміни стабільності суспензії спостерігались за допомогою приладу Turbiscan
LabExpert із охолоджуючим модулем TLAb Cooler при 25oC. ПAК є аніонним полімером, що містить карбокси-
льні групи, тому всі вимірювання проводились при різних рН (3, 6 та 9). Аналіз одержаних кривих перенесен-
ня та зворотнього розсіяння, а також індексів стабільності (Turbiscan Stability Indexes (TSI)) дозволив ви-
значити найбільш вірогідний механізм стабілізації вивчених систем.
Влияние рН раствора на стабильность систем
высокодисперсный кремнезем – полиакриловая кислота
M. Вишневска, K. Терпиловский, В. Зарко, С. Хибовский, Э. Хибовский, T. Урбан, В. Гунько
Университет Марии Кюри-Склодовской
пл. Марии Кюри-Склодовской 3, Люблин 20-031, Польша, wisniewska@hektor.umcs.lublin.pl
Институт химии поверхности им. А.А. Чуйко Национальной академии наук Украины
ул. Генерала Наумова 17, Киев 03164, Украина
Изучено влияние адсорбции полиакриловой кислоты (ПAA) на поверхности высокодисперсного кремне-
зема (SiO2) на стабильность суспензии. Изменения стабильности суспензии наблюдались с помощью прибо-
ра Turbiscan LabExpert с охлаждающим модулем TLAb Cooler при 25oC. PAA является анионным полимером,
содержащим карбоксильные группы, поэтому все измерения проводились при различных рН (3, 6 и 9). Анализ
полученных кривых переноса и обратного рассеяния, а также индексов стабильности (Turbiscan Stability
Indexes (TSI)) позволил определить наиболее вероятный механизм стабилизации изученных систем.
|
| id | nasplib_isofts_kiev_ua-123456789-28991 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 2079-1704 |
| language | English |
| last_indexed | 2025-12-07T13:31:56Z |
| publishDate | 2010 |
| publisher | Інститут хімії поверхні ім. О.О. Чуйка НАН України |
| record_format | dspace |
| spelling | Wiśniewska, M. Terpiłowski, K. Zarko, V.I. Chibowski, S. Chibowski, E. Urban, T. Gun’ko, V.M. 2011-11-27T16:49:31Z 2011-11-27T16:49:31Z 2010 Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems / M. Wiśniewska, K. Terpiłowski, V.I. Zarko, S. Chibowski, E. Chibowski, T. Urban, V.M. Gun’ko // Хімія, фізика та технологія поверхні. — 2010. — Т. 1, № 3. — С. 269-273. — Бібліогр.: 6 назв. — англ. 2079-1704 https://nasplib.isofts.kiev.ua/handle/123456789/28991 544.723 The influence of polyacrlic acid (PAA) adsorption on fumed silica (SiO2) surface on suspension stability has been studied. Сhanges in the suspension stability were monitored using a Turbiscan LabExpert with a TLAb Cooler cooling module at 25oC. PAA is an anionic polymer containing carboxyl groups; therefore all the measurements were carried out at different pH 3, 6 and 9. Analysis of obtained transmission and backscattering curves and Turbiscan Stability Indexes (TSI) allowed determination of the most probable mechanism of the system stability. Вивчено вплив адсорбції поліакрилової кислоти (ПAК) на поверхні високодисперсного кремнезему (SiO2) на стабільність суспензії. Зміни стабільності суспензії спостерігались за допомогою приладу Turbiscan LabExpert із охолоджуючим модулем TLAb Cooler при 25oC. ПAК є аніонним полімером, що містить карбоксильні групи, тому всі вимірювання проводились при різних рН (3, 6 та 9). Аналіз одержаних кривих перенесення та зворотнього розсіяння, а також індексів стабільності (Turbiscan Stability Indexes (TSI)) дозволив визначити найбільш вірогідний механізм стабілізації вивчених систем. Изучено влияние адсорбции полиакриловой кислоты (ПAA) на поверхности высокодисперсного кремнезема (SiO2) на стабильность суспензии. Изменения стабильности суспензии наблюдались с помощью прибора Turbiscan LabExpert с охлаждающим модулем TLAb Cooler при 25oC. PAA является анионным полимером, содержащим карбоксильные группы, поэтому все измерения проводились при различных рН (3, 6 и 9). Анализ полученных кривых переноса и обратного рассеяния, а также индексов стабильности (Turbiscan Stability Indexes (TSI)) позволил определить наиболее вероятный механизм стабилизации изученных систем. The research leading to these results has received funding from the European Community’s Seven Framework Programme (FP7/2007 – 2013) under a Maria Curie International Research Staff Exchange Scheme, Grant Agreement No. PIRSES – GA – 2008 – 230790. en Інститут хімії поверхні ім. О.О. Чуйка НАН України Хімія, фізика та технологія поверхні Функціоналізовані матеріали, одержані золь-гель і темплатним методами Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems Вплив рН розчину на стабільність систем високодисперсний кремнезем – поліакрилова кислота Влияние рН раствора на стабильность систем высокодисперсный кремнезем – полиакриловая кислота Article published earlier |
| spellingShingle | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems Wiśniewska, M. Terpiłowski, K. Zarko, V.I. Chibowski, S. Chibowski, E. Urban, T. Gun’ko, V.M. Функціоналізовані матеріали, одержані золь-гель і темплатним методами |
| title | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems |
| title_alt | Вплив рН розчину на стабільність систем високодисперсний кремнезем – поліакрилова кислота Влияние рН раствора на стабильность систем высокодисперсный кремнезем – полиакриловая кислота |
| title_full | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems |
| title_fullStr | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems |
| title_full_unstemmed | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems |
| title_short | Influence of Solution pH on Stability of Fumed Silica–Polyacrylic Acid Systems |
| title_sort | influence of solution ph on stability of fumed silica–polyacrylic acid systems |
| topic | Функціоналізовані матеріали, одержані золь-гель і темплатним методами |
| topic_facet | Функціоналізовані матеріали, одержані золь-гель і темплатним методами |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/28991 |
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