Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type
Plasma-catalytic system for generation of carbon nanomaterials based on tornado-type discharge (using reverse-vortex gas flow) in a mixture of ethanol aerosol and inert gas was studied. Current-voltage characteristics of the discharge for different modes of the system were investigated. Efficiency o...
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Національний науковий центр «Харківський фізико-технічний інститут» НАН України
2014
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| Cite this: | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type / Iu.P. Veremii, K.V. Iukhymenko, M.M. Kasumov, T.E. Lisitchenko // Вопросы атомной науки и техники. — 2014. — № 6. — С. 215-218. — Бібліогр.: 8 назв. — англ. |
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Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1859584285722279936 |
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| author | Veremii, Iu.P. Iukhymenko, K.V. Kasumov, M.M. Lisitchenko, T.E. |
| author_facet | Veremii, Iu.P. Iukhymenko, K.V. Kasumov, M.M. Lisitchenko, T.E. |
| citation_txt | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type / Iu.P. Veremii, K.V. Iukhymenko, M.M. Kasumov, T.E. Lisitchenko // Вопросы атомной науки и техники. — 2014. — № 6. — С. 215-218. — Бібліогр.: 8 назв. — англ. |
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| description | Plasma-catalytic system for generation of carbon nanomaterials based on tornado-type discharge (using reverse-vortex gas flow) in a mixture of ethanol aerosol and inert gas was studied. Current-voltage characteristics of the discharge for different modes of the system were investigated. Efficiency of the systems with metal and graphite electrodes was compared. The possibility of continuous operation of such plasma-liquid reactor combined with pyrolytic chamber was demonstrated. It was shown that different morphology of carbon structures (nanorods and nanotubes) generated in such plasma system depends on the temperature of pyrolytic chamber and electrode materials.
Представлены плазменно-каталитические системы для генерации углеродных наноматериалов на основе разряда типа "торнадо" (с использованием обратно-вихревого потока газа) в смеси аэрозоля этанола и инертного газа. Рассмотрены вольт-амперные характеристики такого разряда для различных режимов работы системы. Проведено сравнение эффективности системы с металлическими и графитовыми электродами. Показана возможность непрерывной работы такого плазменно-жидкостного реактора в сочетании с пиролитической камерой. Показана возможность образования в такой системе углеродных структур различной морфологии (наностержней и нанотрубок) в зависимости от температуры пиролитической камеры и материала электродов.
Представлено плазмово-каталітичні системи для генерації вуглецевих наноматеріалів на основі розряду типу "торнадо" (з використанням обернено-вихрового потоку газу) в суміші аерозолю етанолу та інертного газу. Розглянуто вольт-амперні характеристики такого розряду для різних режимів роботи системи. Проведено порівняння ефективності системи з металевими та графітовими електродами. Показана можливість безперервної роботи такого плазмово-рідинного реактора в поєднанні з піролітичною камерою. Показана можливість утворення в такій системі вуглецевих структур різної морфології (нанострижнів і нанотрубок) в залежності від температури піролітичної камери та матеріалу електродів.
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ISSN 1562-6016. ВАНТ. 2014. №6(94)
PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2014, №6. Series: Plasma Physics (20), p. 215-218. 215
CONTINUOUS PROCESS OF CARBON NANOPARTICLES
GENERATION BY THE PLASMA-LIQUID SYSTEM "TORNADO" TYPE
Iu.P. Veremii
1
, K.V. Iukhymenko
1
, M.M. Kasumov
2
, T.E. Lisitchenko
1
1
Taras Shevchenko National University of Kyiv, Ukraine;
2
Vernadsky Institute of general and inorganic chemistry of the NASU, Kyiv, Ukraine;
E-mail: veremii@i.ua
Plasma-catalytic system for generation of carbon nanomaterials based on tornado-type discharge (using reverse-
vortex gas flow) in a mixture of ethanol aerosol and inert gas was studied. Current-voltage characteristics of the
discharge for different modes of the system were investigated. Efficiency of the systems with metal and graphite
electrodes was compared. The possibility of continuous operation of such plasma-liquid reactor combined with
pyrolytic chamber was demonstrated. It was shown that different morphology of carbon structures (nanorods and
nanotubes) generated in such plasma system depends on the temperature of pyrolytic chamber and electrode
materials.
PACS: 52, 52.77.-j
INTRODUCTION
The urgent task to ensure demands for industrial
synthesis of carbon nanomaterials (CNM) is continuous
process of its production.
Plasma-liquid systems (PLS) can operate in
continuous mode k and considerably facilitate a scaling
process, in comparison with traditional methods of
nanomaterials generation, provide selectivity of target
products, safety and profitability [1-5].
Plasma-liquid system of inverse gas flow type vortex
tornado with liquid electrode was previously developed
by our research group [6, 7]. To generate carbon
nanoparticles inert gas - argon and liquid – ethanol (as a
carbon source) were used.
However, the alcohol significantly alters its
properties in the combustion chamber volume during
the discharge burning that leads to the instability of the
system. To keep the possibility of plasma in heterophase
system with all its benefits, a system with continuous
injection of aerosol into the plasma chamber was
developed. Besides it is believed that water-cooling
metal electrodes in contact with the spray is coated of
liquid film and therefore avoids erosion of electrodes.
During the study of the substrate temperature
influence on the synthesis process, it was found that
CNM production has a peak of effectiveness which
corresponds to the specific temperature [8]. This effect
is caused by a competition between diffusion and
adsorption of carbon atoms, rates of both these
processes are determined by the surface temperature.
This result is in a good agreement with the most recent
theories of CNM synthesis that is based on the
investigation of surface models.
Since it have been conclusively proved a decisive
influence of the substrate temperature on size and
morphology of the final product, formation and removal
of produced CNM should be carried out by particles
with controlled surface temperature. So the main task of
the presented work was to ensure process with
continuous formation and removal of the formed carbon
material from the reaction volume on the particles with
controlled surface temperature.
1. EXPERIMENT
To solve the task mentioned above chemically
passive particles used to create carbon nanomaterials
growth centres were injected into the pyrolytic reaction
chamber. Usage of such particles makes possible to
synthesize resulting products outside the system and
greatly simplify the process of the purification.
This feature was implemented in an experimental
setup consisted of "tornado" type PLS combined with
pyrolytic chamber with dust feeding (Fig. 1). A chamber
temperature is considered to be the same as a substrate
temperature and was maintained by the heating coil.
Spray of ethanol, argon as plasmaforming and carrier
gas, stainless steel or graphite electrodes were used
during the experiment.
Ethanol aerosol was created by the piezocrystal
emitter and carry out by the argon stream (feed rate was
3.3 l/min) to the area of raw activation. Alcohol feed
rate was 1.7 ml/min. The ethanol aerosol flow was
injected with argon into the vessel through the orifice in
the upper flange tangentially to the cylinder wall and
created a reverse vortex flow of tornado type.
Fig. 1. Plasma-liquid system “Tornado” combined
with the reaction pyrolytic chamber
216 ISSN 1562-6016. ВАНТ. 2014. №6(94)
a
b
Fig. 2. Current-voltage characteristics of the discharge,
the inter-electrode gap of 3 mm: a – in pure argon and
mixture argon/aerosol alcohol, b – for the two polarities
of discharge in mixture argon/aerosol alcohol, for
different flows of working substance
The electrical discharge burned between the bottom
and the upper electrode. The both electrodes were made
from stainless steel or graphite (EG-2), which was
attached to the holder from stainless steel and have
water cooling. The interelectrode gap e was 3 mm.
Plasma torch was blown by stream of argon through the
outlet in the top electrode ( 3.4 mm) in the pyrolytic
chamber. The formation of carbon nanomaterials was
occurred on the surface of chemical passive
microparticles (so-called dust) in the the pyrolytic
chamber. The flow rate of argon for filing dust was 10-
15 L/min. The temperature of pyrolytic chamber was
controlled by the system of thermocouples.
With aerosol injection into the discharge chamber
the voltage significantly increased (Fig. 2,a). Such
peculiarity of the current-voltage characteristics of the
discharge in the presence of alcohol aerosol can be
explained by appearance of negative ions O
-
and CO
-
,
leading to a significant increase of the recombination
rates, and hence to maintain the discharge the voltage
increase the is needed. Besides, voltage increase on the
discharge may be connected with cooling of electrodes
by aerosol.
The discharge weakly depends on the gas flow at
interelectrode gap of 3...5 mm (Fig 2,b).
The carbon deposit with the graphitized outer wall
was formed on anode in aerosol plasma system with
metal electrodes (Fig. 3). When the anode was lower
electrode, carbon deposit was fairly stable, in the case
when the anode was upper electrode - carbon deposit
was easily destroyed and taken out by the gas flow in
the process. The deposit formation in the interelectrode
space leads to a breach of the discharge and continuous
system operation. We supposed that it can be avoided
by the using of graphite electrodes.
CVCs, discharge character, and physical phenomena
in the discharge chamber (aerosol extinction in the
discharge volume) were significantly changed when
metal electrodes were replaced by graphite ones. This
phenomenon can be explained by high absorptive
capacity sprayed graphite electrodes.
Fig. 3. Carbon deposit on the anode, appearance and
internal structure
Significantly increased voltage on the discharge, and
decreased difference discharges with different polarity,
compared with metal electrodes (Fig. 4). Uneven
heating of the cooled electrodes has the main influence
on the current-voltage characteristics.
In the case of graphite electrodes carbon deposit did
not formed that allows to increase the life of continuous
discharge significantly. Despite the presence a liquid
aerosol in the reactor graphite electrodes were sputtered
significantly. Concentric nature of the sputtering areas
in the electrodes is due to the presence of the vortex gas
flow.
ISSN 1562-6016. ВАНТ. 2014. №6(94) 217
a
b
Fig. 4. Current-voltage characteristics of the discharge
with graphite electrodes: a – for different polarities;
b – between metal electrodes (1), between graphite
electrodes (2)
It was shown that effectiveness of the nanomaterials
formation f is much higher in the case of graphite
electrodes using. But the increasing of productivity is
likely due to the included scattered electrode material
into the final product. This conclusion was made by
comparing emission plasma spectra of discharges with
different electrodes. The intensity of atomic carbon
emission line significantly increases in the case of
graphite electrodes using. It indicates the increasing of
the concentration of activated carbon in the bulk at the
same temperatures of excited levels population of the
carbon molecule (C2).
2. METHODS AND RESULTS
The outlet material was collected by decantation
method, when chemically passive particles removed by
acid derived. CNM sample was washed in distilled
water several times. Then the material annealed in a
muffle oven at 500
0
C (0.5 h) to remove amorphous
carbon component, and sonicated in the ultrasonic bath
with frequency 42 kHz and power 50 W (0.5 h in
ethanol, which is then evaporated) to avoid clumping of
particles.
Formation of carbon structures with different
morphology was found in samples obtained at high
temperatures (600°C and higher). Accumulation of
carbon rods with a diameter of 70...100 nm and a length
of 10 mm placed randomly was observed in the samples
at the pyrolytic chamber temperature of 600°C.
(Fig. 5). A small number of carbon nanotubes with a
diameter of 10...50 nm were presented in samples at
temperatures over 650°C. Mixture of carbon structures
in samples may be caused by the specifics of the
formation as well as the influence of cleaning
procedures.
Purified samples obtained in the system with
graphite electrodes are almost entirely composed of
entangled carbon nanotubes of different diameters
10...80 nm (Fig. 6).
This difference in the products of synthesis can be
explained by better atomization of carbon in the
discharge zone possibly due to the sputtering of graphite
electrodes. Іt promotes to the formation of
nanostructures with smaller dimension.
Thus it can be concluded that working with graphite
electrodes are more productive, but requires constant
control of the electrodes. The procedure of the samples
purification is the same.
Fig. 5. Photo purified sample СNM obtained in the
system with metal electrodes
Fig. 6. Photo purified sample СNM obtained in the
system with graphite electrodes
218 ISSN 1562-6016. ВАНТ. 2014. №6(94)
CONCLUSIONS
It was found that samples obtained at "Tornado"-
type PLS mainly consist of nanostructured carbon. The
possibility of carbon nanomaterials removal from
plasma by chemically passive dust particles was shown.
The cleaning process of material obtained in this work
is much simpler than clearing CNM synthesized by
conventional methods. It was concluded that working
with graphite electrodes is more productive.
The main advantages of the investigated PLS are: a
long service time; ability to maintain uninterrupted
working cycle; ability to control chemical composition
of produced nanoparticles by using aerosols of different
hydrocarbon liquids or by changing material of
electrodes and microparticles injected into pyrolytic
chamber. It was shown that the temperature of the
pyrolytic chamber significantly affects on the
morphology of final products of and its value can vary
in wide range.
ACKNOWLEDGEMENTS
This work was partially supported by the State fund
for fundamental researches, Ministry of Education and
Science of Ukraine, National Academy of Sciences of
Ukraine, Taras Shevchenko Kyiv National University.
REFERENCES
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Article received 26.10.2014
НЕПРЕРЫВНЫЙ ПРОЦЕСС ГЕНЕРАЦИИ УГЛЕРОДНЫХ НАНОЧАСТИЦ
В ПЛАЗМЕННО-ЖИДКОСТНОЙ СИСТЕМЕ ТИПА "ТОРНАДО"
Ю.П. Веремий, К.В. Юхименко, М.М. Касумов, Т.Е. Лиситченко
Представлены плазменно-каталитические системы для генерации углеродных наноматериалов на основе
разряда типа "торнадо" (с использованием обратно-вихревого потока газа) в смеси аэрозоля этанола и
инертного газа. Рассмотрены вольт-амперные характеристики такого разряда для различных режимов
работы системы. Проведено сравнение эффективности системы с металлическими и графитовыми
электродами. Показана возможность непрерывной работы такого плазменно-жидкостного реактора в
сочетании с пиролитической камерой. Показана возможность образования в такой системе углеродных
структур различной морфологии (наностержней и нанотрубок) в зависимости от температуры
пиролитической камеры и материала электродов.
НЕПЕРЕРВНИЙ ПРОЦЕС ГЕНЕРАЦІЇ ВУГЛЕЦЕВИХ НАНОЧАСТИНОК
У ПЛАЗМОВО-РІДИННІЙ СИСТЕМІ ТИПУ "ТОРНАДО"
Ю.П. Веремій, К.В. Юхименко, М.М. Касумов, Т.Є. Лиситченко
Представлено плазмово-каталітичні системи для генерації вуглецевих наноматеріалів на основі розряду
типу "торнадо" (з використанням обернено-вихрового потоку газу) в суміші аерозолю етанолу та інертного
газу. Розглянуто вольт-амперні характеристики такого розряду для різних режимів роботи системи.
Проведено порівняння ефективності системи з металевими та графітовими електродами. Показана
можливість безперервної роботи такого плазмово-рідинного реактора в поєднанні з піролітичною камерою.
Показана можливість утворення в такій системі вуглецевих структур різної морфології (нанострижнів і
нанотрубок) в залежності від температури піролітичної камери та матеріалу електродів.
|
| id | nasplib_isofts_kiev_ua-123456789-81955 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-11-27T09:13:23Z |
| publishDate | 2014 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Veremii, Iu.P. Iukhymenko, K.V. Kasumov, M.M. Lisitchenko, T.E. 2015-05-22T18:19:10Z 2015-05-22T18:19:10Z 2014 Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type / Iu.P. Veremii, K.V. Iukhymenko, M.M. Kasumov, T.E. Lisitchenko // Вопросы атомной науки и техники. — 2014. — № 6. — С. 215-218. — Бібліогр.: 8 назв. — англ. 1562-6016 PACS: 52, 52.77.-j https://nasplib.isofts.kiev.ua/handle/123456789/81955 Plasma-catalytic system for generation of carbon nanomaterials based on tornado-type discharge (using reverse-vortex gas flow) in a mixture of ethanol aerosol and inert gas was studied. Current-voltage characteristics of the discharge for different modes of the system were investigated. Efficiency of the systems with metal and graphite electrodes was compared. The possibility of continuous operation of such plasma-liquid reactor combined with pyrolytic chamber was demonstrated. It was shown that different morphology of carbon structures (nanorods and nanotubes) generated in such plasma system depends on the temperature of pyrolytic chamber and electrode materials. Представлены плазменно-каталитические системы для генерации углеродных наноматериалов на основе разряда типа "торнадо" (с использованием обратно-вихревого потока газа) в смеси аэрозоля этанола и инертного газа. Рассмотрены вольт-амперные характеристики такого разряда для различных режимов работы системы. Проведено сравнение эффективности системы с металлическими и графитовыми электродами. Показана возможность непрерывной работы такого плазменно-жидкостного реактора в сочетании с пиролитической камерой. Показана возможность образования в такой системе углеродных структур различной морфологии (наностержней и нанотрубок) в зависимости от температуры пиролитической камеры и материала электродов. Представлено плазмово-каталітичні системи для генерації вуглецевих наноматеріалів на основі розряду типу "торнадо" (з використанням обернено-вихрового потоку газу) в суміші аерозолю етанолу та інертного газу. Розглянуто вольт-амперні характеристики такого розряду для різних режимів роботи системи. Проведено порівняння ефективності системи з металевими та графітовими електродами. Показана можливість безперервної роботи такого плазмово-рідинного реактора в поєднанні з піролітичною камерою. Показана можливість утворення в такій системі вуглецевих структур різної морфології (нанострижнів і нанотрубок) в залежності від температури піролітичної камери та матеріалу електродів. This work was partially supported by the State fund for fundamental researches, Ministry of Education and Science of Ukraine, National Academy of Sciences of Ukraine, Taras Shevchenko Kyiv National University. en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Вопросы атомной науки и техники Низкотемпературная плазма и плазменные технологии Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type Непрерывный процесс генерации углеродных наночастиц в плазменно-жидкостной системе типа "торнадо" Неперервний процес генерації вуглецевих наночастинок у плазмово-рідинній системі типу "торнадо" Article published earlier |
| spellingShingle | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type Veremii, Iu.P. Iukhymenko, K.V. Kasumov, M.M. Lisitchenko, T.E. Низкотемпературная плазма и плазменные технологии |
| title | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type |
| title_alt | Непрерывный процесс генерации углеродных наночастиц в плазменно-жидкостной системе типа "торнадо" Неперервний процес генерації вуглецевих наночастинок у плазмово-рідинній системі типу "торнадо" |
| title_full | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type |
| title_fullStr | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type |
| title_full_unstemmed | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type |
| title_short | Continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type |
| title_sort | continuous process of carbon nanoparticles generation by the plasma-liquid system "tornado" type |
| topic | Низкотемпературная плазма и плазменные технологии |
| topic_facet | Низкотемпературная плазма и плазменные технологии |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/81955 |
| work_keys_str_mv | AT veremiiiup continuousprocessofcarbonnanoparticlesgenerationbytheplasmaliquidsystemtornadotype AT iukhymenkokv continuousprocessofcarbonnanoparticlesgenerationbytheplasmaliquidsystemtornadotype AT kasumovmm continuousprocessofcarbonnanoparticlesgenerationbytheplasmaliquidsystemtornadotype AT lisitchenkote continuousprocessofcarbonnanoparticlesgenerationbytheplasmaliquidsystemtornadotype AT veremiiiup nepreryvnyiprocessgeneraciiuglerodnyhnanočasticvplazmennožidkostnoisistemetipatornado AT iukhymenkokv nepreryvnyiprocessgeneraciiuglerodnyhnanočasticvplazmennožidkostnoisistemetipatornado AT kasumovmm nepreryvnyiprocessgeneraciiuglerodnyhnanočasticvplazmennožidkostnoisistemetipatornado AT lisitchenkote nepreryvnyiprocessgeneraciiuglerodnyhnanočasticvplazmennožidkostnoisistemetipatornado AT veremiiiup neperervniiprocesgeneracíívuglecevihnanočastinokuplazmovorídinníisistemítiputornado AT iukhymenkokv neperervniiprocesgeneracíívuglecevihnanočastinokuplazmovorídinníisistemítiputornado AT kasumovmm neperervniiprocesgeneracíívuglecevihnanočastinokuplazmovorídinníisistemítiputornado AT lisitchenkote neperervniiprocesgeneracíívuglecevihnanočastinokuplazmovorídinníisistemítiputornado |