IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE
The review is devoted to the use of impregnated activated carbon materials as chemisorbents of sulfur (IV) oxide. General methods for obtaining ordinary activated carbon, preparation of raw materials, their chemical activation with alkalis and acids followed by heat treatment (carbonization) in an i...
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| Дата: | 2023 |
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| Автори: | , , |
| Формат: | Стаття |
| Мова: | Англійська |
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V.I.Vernadsky Institute of General and Inorganic Chemistry
2023
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| Назва журналу: | Ukrainian Chemistry Journal |
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Репозитарії
Ukrainian Chemistry Journal| _version_ | 1871466000259481600 |
|---|---|
| author | Khoma, Ruslan Vodzinskii, Sergey Klimov, Danyil |
| author_facet | Khoma, Ruslan Vodzinskii, Sergey Klimov, Danyil |
| author_institution_txt_mv | [
{
"author": "Ruslan Khoma",
"institution": "Одесский национальный университет имени И.И. Мечникова"
},
{
"author": "Sergey Vodzinskii",
"institution": "Одесский национальный университет имени И.И. Мечникова"
},
{
"author": "Danyil Klimov",
"institution": "Dnipro University of Technology"
}
] |
| author_sort | Khoma, Ruslan |
| baseUrl_str | https://ucj.org.ua/index.php/journal/oai |
| collection | OJS |
| datestamp_date | 2026-07-22T08:23:52Z |
| description | The review is devoted to the use of impregnated activated carbon materials as chemisorbents of sulfur (IV) oxide. General methods for obtaining ordinary activated carbon, preparation of raw materials, their chemical activation with alkalis and acids followed by heat treatment (carbonization) in an inert environment or in the presence of a gaseous oxidizer, the role of acid-base and redox catalysts in this process are considered. The influence of the chemical composition of the  activated carbon surface, the presence of functional groups, and their acid-base properties, as well as the products of surface reactions on the peculiarities of sulfur (IV) oxide  adsorption is analyzed from the point of view of SO2 removal efficiency and the possibility of SO2 regeneration. An important role in these processes is played by the  pore size, the possibility of co-adsorption of water, and the presence of an oxidant. The nature of adsorbent-adsorbate interactions on the surface of activated carbon, their energy, in particular, the contribution of so-called "physical" adsorption, van der Waals forces, hydrogen bonding, and the influence of surface functional groups are discussed. The activation of carbon raw materials with nitrogen-containing compounds leads to the N-doping of the surface, which increases the efficiency of SO2 adsorption, facilitating not only van der Waals and electrostatic interactions, but also S←N binding. The influence of oxygen and oxygen-containing functional groups on SO2 adsorption is also discussed.
To obtain impregnated activated carbon for SO2 absorption, the original activated carbon of the required quality is impregnated with solutions of inorganic and organic compounds that remain on the inner surface of the activated carbon after drying. Impregnation blocks partly  the porosity of activated carbon, but makes it more capable of chemical adsorption. Chemisorption, in which certain chemical bonds are formed between the surface of the activated carbon and the compound being adsorbed, is more selective than physical adsorption, where the size of  molecules is critical for an effective capture process. It can be noted that unlike inorganic alkalis, which spoil the porous structure of activated carbon, treatment with a solution of ammonia or organic N-containing bases promotes SO2 absorption. A special place in gas purification is occupied by activated carbon impregnated with ionic liquids, non-aqueous solvents being used for impregnation. A separate issue of the chemisorption of sulfur (IV) oxide by samples of impregnated activated carbon based on d-metals will be discussed in detail below. |
| doi_str_mv | 10.33609/2708-129X.89.10.2023.124-144 |
| first_indexed | 2025-09-24T17:43:54Z |
| format | Article |
| fulltext |
124 ISSN 2708-129X. Укр. хім. журн., 2023
UDC 541.183:661.183.2 doi: 10.33609/2708-129X.89.10.2023.124-144
IMPREGNATED ACTIVATED CARBON MATERIALS
FOR RESPIRATORY PURPOSE.
CHEMISORPTION OF SULFUR DIOXIDE.
R. E. Khoma1,2*, S. V. Vodzinskii1,2, D. G. Klimov1,3
1Physico-Chemical Institute of Environmental and Human Protection of the MES of Ukraine
and NAS of Ukraine, 3 vul. Preobrazhenska, 65082 Odesa, Ukraine;
2 I.I. Mechnikov National University of Odesa, 2 vul. Dvoryanska, 65082 Odesa, Ukraine;
3Dnipro University of Technology, 18 ave Dmytra Yavornytskoho, 49005 Dnipro, Ukraine
*e-mail: rek@onu.edu.ua
The review is devoted to the use of impregnated activated carbon materials as chemisorbents of
sulfur (IV) oxide. General methods for obtaining ordinary activated carbon, preparation of raw ma-
terials, their chemical activation with alkalis and acids followed by heat treatment (carbonization) in
an inert environment or in the presence of a gaseous oxidizer, the role of acid-base and redox catalysts
in this process are considered. The influence of the chemical composition of the activated carbon
surface, the presence of functional groups, and their acid-base properties, as well as the products of
surface reactions on the peculiarities of sulfur (IV) oxide adsorption is analyzed from the point of
view of SO2 removal efficiency and the possibility of SO2 regeneration. An important role in these
processes is played by the pore size, the possibility of co-adsorption of water, and the presence of an
oxidant. The nature of adsorbent-adsorbate interactions on the surface of activated carbon, their ener
gy, in particular, the contribution of so-called "physical" adsorption, van der Waals forces, hydrogen
bonding, and the influence of surface functional groups are discussed. The activation of carbon raw
materials with nitrogen-containing compounds leads to the N-doping of the surface, which increases
the efficiency of SO2 adsorption, facilitating not only van der Waals and electrostatic interactions, but
also S←N binding. The influence of oxygen and oxygen-containing functional groups on SO2 adsorp-
tion is also discussed.
To obtain impregnated activated carbon for SO2 absorption, the original activated carbon of the
required quality is impregnated with solutions of inorganic and organic compounds that remain on
the inner surface of the activated carbon after drying. Impregnation blocks partly the porosity of ac-
tivated carbon, but makes it more capable of chemical adsorption. Chemisorption, in which certain
chemical bonds are formed between the surface of the activated carbon and the compound being ad-
sorbed, is more selective than physical adsorption, where the size of molecules is critical for an effec-
tive capture process. It can be noted that unlike inorganic alkalis, which spoil the porous structure of
activated carbon, treatment with a solution of ammonia or organic N-containing bases promotes SO2
absorption. A special place in gas purification is occupied by activated carbon impregnated with ionic
liquids, non-aqueous solvents being used for impregnation. A separate issue of the chemisorption of
sulfur (IV) oxide by samples of impregnated activated carbon based on d-metals will be discussed in
detail below.
Key words: impregnated activated carbon materials, sulfur dioxide, physical adsorption, chemi
sorption.
125https://ucj.org.ua
R. E. Khoma, S. V. Vodzinskyi, D. G. Klimov UCJ № 10 / Vol. 89
INTRODUCTION. The increase in the level
of environmental danger in the conditions of
war is associated with the destruction or da
mage, as a result of hostilities, of enterprises
that are the largest (real or potential) polluters
of the environment in peacetime [1]. Sulfur
(IV) oxide, ammonia and aromatic hydrocar-
bons are among the main emergency emissions
into the atmosphere by coke and by-product
production enterprises [2–4]. One of the tasks
of occupational health and safety departments
at the enterprises of by-product coke indust
ry is to provide workers and engineering and
technical personnel with means of personal
respiratory protection (MPRP) equipped with
gas filter cartridges (GFCs), which are capa-
ble of absorbing toxic acid (in particular, SO2)
or/and basic (in particular, NH3) gases, as well
as vapors of organic compounds (in particular,
C6H6 and C6H12), etc. [3].
In addition, to ensure the protection of the
respiratory organs of workers and engineer-
ing and technical personnel of enterprises,
civilians and military personnel in emergen-
cy situations, when the nature of the toxicant
present in the air is unknown, it is desirable to
have a gas filter of wide range of action.
The high porosity, large inner surface area,
non-polarity, cheapness, chemical stability
compared to other porous materials (zeolite,
silica, alumina, etc.) of activated carbon (AC)
make it suitable for removing toxic and irritat-
ing gases and vapors from the air [1–4]. The
impregnation of a porous medium (in par-
ticular, AC) with carefully selected chemical
compounds can significantly increase its ab-
sorption capacity for certain gases/vapors, as
well as provide absorption capacity for gases/
vapors that cannot be captured (detoxified) by
non-impregnated AC [5–12]. This method has
been used for many years in the production of
gas filters and respiratory cartridges [13]. AC is
widely used for the production of impreg-
nated activated carbon materials (IACMs) –
chemisorbents of chemically hazardous sub-
stances of inhalation action and acidic (SO2,
HCl, HF, Cl2, F2, H2S, CO2, HCN, etc.), basic
(NH3, organic amines, etc.) and neutral (Hg,
etc.) nature, as well as for the decontamination
of volatile warfare agents from the air flow in
the case of radioactive, biological and chemical
contamination [5–9, 11, 14].
Methods of carbon activation.
To obtain ACs, which are used as adsor-
bents and catalyst carriers, methods of physi-
cal or chemical activation are usually used [5,
15–22]. Obtaining AC using physical activa-
tion includes the following stages: preparation
of raw materials (separation, crushing, drying,
etc.); pyrolysis (heat treatment in absence of
oxidant at a temperature of 550–1000 °C; ac-
tivation (heat treatment in the presence of an
oxidant, CO2 or water vapor at 700–1000 °C).
The production of AC by the method of ther-
mochemical activation is based on the intro-
duction of chemical additives into the starting
material followed by carbonization in an inert
environment or in the presence of a gaseous
oxidant. The transformation of raw materials
into AC is carried out under the action of ac-
id-base or redox catalysts (ZnCl2, FeCl3, Al2O3;
HNO3, H2SO4, H3PO4, (NH4)2HPO4; carbonates,
acetates or hydroxides of alkali metals, etc.) [5,
15–22]. Catalysts activate the transformation of
aliphatic fragments, practically without touch-
ing aryl C-C bonds, remove oxygen, hydrogen
and other heteroatoms with simultaneous car-
bonization and activation at temperatures gen-
erally below 700 °C. As a result, ACs with a de-
veloped porous structure are obtained.
126 ISSN 2708-129X. Укр. хім. журн., 2023
IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE.
CHEMISORPTION OF SULFUR DIOXIDE.PHISICAL CHEMISTRY
According to the results of the physico-
chemical study of the products of alkaline ac-
tivation of various raw materials, the specific
surface area, the pore volume and size, the size
distribution of pores depend on the nature
of the raw material itself and the alkali used
(LiOH, NaOH and KOH), as well as its content
in the original mixture; the activating ability
of hydroxides decreases in the order KOH >
NaOH > LiOH [18]. Phosphoric acid leads to
the expansion of micro- and mesopores in ac-
tivated carbon [19, 20, 21, 23].
As a rule, acid treatment leads to an increase
in the number of acid groups, removes mineral
elements and improves the hydrophilicity of
the surface, which will have greater access to
the aqueous phase [24, 25].
Adsorption of SO2 on the surface of activated
carbon.
When studying SO2 adsorption by AC, the
researchers took into account such parameters
as porosity, chemical composition of the sur-
face, acid-base properties and ash content; the
products of surface reactions were analyzed
from the point of view of removal efficiency
and the possibility of regeneration [26–31].
There is an optimal pore size (approxima
tely 7 A) at which the adsorption of SO2 [32]
and its oxidation to SO3 [33] are favorable.
Although in such pores, the absorption po-
tential is not maximal (σSO2 = 4.29 E [34]),
a high capacity is achieved due to the ad-
sorption of SO2 and SO3 with the subsequent
formation of H2SO4 [31]. In such pores, SO2
together with H2O can statistically cover the
walls of pores, forming a monolayer. This
makes oxidation and reaction with co-ad-
sorbed water molecules possible. It should be
noted that H2SO4 at 25 °C has a higher density
(ρH2SO4 = 1.83 g/cm3) than liquid SO2 (ρSO2 =
1.27 g/cm3), but a lower density than that of
SO3 (ρSO3 = 1, 93 g/cm3). In addition, its boil-
ing point is about 330 °C, which is much high-
er than that of SO2 (-10 °C) and SO3 (45 °C)
[35]. Given the above, the amount of H2SO4
physically adsorbed from the vapor phase
should be greater than the amount of SO2 and/
or SO3 under the same conditions (pressure
and temperature). It follows that the order
of decreasing physical adsorption "capacity"
should be as follows: H2SO4 > SO3 > SO2. If the
pore size is too small, water molecules cannot
be co-adsorbed near SO2, preventing the for-
mation of sulfuric acid. Apparently, as in the
case of hydrogen sulfide adsorption [36], the
uniform distribution of micropores affects the
dispersion of active sites, where SO2 can be
oxidized to SO3, which is then converted to
H2SO4, which is adsorbed until all pores are
filled. Increasing the pore size decreases the
degree of SO2 → SO3 conversion and thus the
total amount of SO2 retained by the AC sam-
ple. According to [37], the adsorption capacity
of AC fibers for SO2 is inversely proportional to
the size and volume of pores.
Adsorbent-adsorbate interactions on the
AC surface are very complex, as they include
a wide range of physical and chemical prop-
erties of the adsorbent, and sometimes there
are significant uncertainties regarding individ-
ual adsorption mechanisms [38]. Sulfur (IV)
oxide is absorbed by AC with two adsorption
energies: ~50 kJ/mol, ~80 kJ/mol; according
to [27, 33, 39–43], the first is associated with
the interaction of SO2 and free sites on the sur-
face due to "van der Waals forces" and corre-
sponds to weak "physical" adsorption, and the
second corresponds to chemisorption, which
is enhanced in the presence of oxygen. How-
ever, the energy of formation of van der Waals
127https://ucj.org.ua
R. E. Khoma, S. V. Vodzinskyi, D. G. Klimov UCJ № 10 / Vol. 89
complexes is 20–40 kJ/mol [44]. The first ener
gy can also correspond to the energy of for-
mation of an "average" hydrogen bond (∆H =
17–63 kJ/mol [45, 46]); directionality, not
energy, is the defining feature of a hydrogen
bond, which is one type of chemical interac-
tion [47]. In addition to porosity, the acid-base
properties of the surface are also an important
factor that increases SO2 adsorption [26–28,
30, 39, 40]. Surface functional groups play the
role of active centers and predominate in SO2
chemisorption [26, 27, 43]. Functional groups
have a great influence on SO2 adsorption and
oxidation [40, 48, 49]. Currently, the experi-
mental study of this effect was carried out by
impregnating AC or raw materials for its pro-
duction with aqueous solutions of HNO3 [27,
29, 50–53], H3PO4 [53, 54], KOH [29, 33, 54–
57], NaOH [39, 51, 58]); modification or acti-
vation by high-temperature gas or steam: CO2
[33, 54], H2O [33], etc.
Effect of chemical activator on AC proper-
ties.
Surface groups of pyrone and pyrone-like
nature or centers having Lewis basicity are
responsible for the adsorption of sulfur (IV)
oxide with an energy of ~50 kJ/mol [39, 48].
Increasing the basic nature of carbon through
the inclusion of basic forms of nitrogen turned
out to be a positive factor affecting the absorp-
tion of SO2 and its oxidation to sulfuric acid
[31, 59–64]. Obviously, the above-mentioned
first adsorption energy (~50 kJ/mol) in this
case is determined not only by van der Waals
interactions (dipole-dipole interactions and
dispersion forces), but also by π-dative S←N
or S←O bonding (∆HS←N = 20–90kJ/mol;
∆HS←O = 10–55 kJ/mol [65]) with the forma-
tion of charge transfer complexes with Lewis
bases and H-bonding, similarly to [65].
In the process of obtaining AC, the authors
of [62, 66] carried out N-doping of various
carbon raw materials (sub-bituminous coal,
lignite; AC fabric based on viscose) by activa-
tion with steam enriched with ammonia or its
derivatives ((NH4)2CO3, H2NNH2, NH2OH,
H2NC (O)NH2; this leads to the formation of
various N-containing groups (amides, imides,
lactams, nitriles, pyrroles, pyridines, etc.) –
Lewis basic centers, which favors S←O and
S←N bonding, similarly to [65]. AC with a
high N content was obtained [31] by the car-
bonization of macroporous vinyl pyridine po
lymers, which are themselves chemisorbents of
acid gases, in particular SO2 [67].
The authors of [43] indicate an increase
in SO2 adsorption efficiency as a result of the
N-doping of the carbon surface due to in-
creased physical adsorption. For a pristine
carbon surface after N-doping, SO2 physical
adsorption mainly occurs on the basal plane
through van der Waals (similarly to [68, 69])
or π-dative interactions (similarly to [65, 70]).
N-doping redistributes electrons on carbon
surfaces, thereby changing not only the in-
tensity but also the types of interactions in-
volved; quaternary N atoms contribute to SO2
adsorption, mainly due to the enhancement of
"van der Waals" interactions between the ba-
sal plane and SO2 [43]. The improvement of
SO2 adsorption by pyridine and pyrrole com-
pounds corresponds to enhanced electrostatic
interactions in the edge regions. These results
show that N-doping can increase SO2 adsorp-
tion efficiency by facilitating not only van der
Waals and electrostatic interactions [43], but
also mainly S←N bonding.
The oxygen-containing functional groups
on the AC surface include carboxyl, phenolic,
quinone, lactone, carboxyanhydride groups,
128 ISSN 2708-129X. Укр. хім. журн., 2023
IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE.
CHEMISORPTION OF SULFUR DIOXIDE.PHISICAL CHEMISTRY
cyclic peroxide, etc. [71]. According to the data
of X-ray photoelectron spectroscopy [72], when
sulfur (IV) oxide is absorbed, the relative con-
tent of the carbonyl (C=O) group, which exists
mainly in the form of quinone and chromene
on the AC surface [73], decreases, and that of
the C–O (hydroxyl and ether [74]) group in-
creases. The effect of ketone C=O groups on
desulfurization activity was confirmed by pas-
sivation with phenylhydrazide [75]; they are
the internal active centers of the desulfuriza-
tion reaction on carbon materials. The centers
of "physical" sorption can also be carboxyl or
hydroxyl groups [31]. A small part of SO2 can
also react with OH groups to form hydrosulfite
anions (as a chemisorption form) [42]; when
SO2 interacts with the C=C bond, 1,3,2-diox-
athiolane and/or 1,2-oxathiethene-2-oxide are
formed, which decompose with the formation
of CO2 and an intermediate episulfide [76].
There are data [30, 39] that oxygen present in
the system can negatively affect the amount of
adsorbed SO2. This is due to its ability to react
with the carbon matrix, its oxidation and, as
a result, the reduction of the surface area [37,
77]. On the other hand, during SO2 adsorp-
tion in the absence of water, oxygen functional
groups significantly improve adsorption char-
acteristics, which, according to [37], is due to
surface reactions of quinones with SO2 and wa-
ter with the formation of diol and sulfuric acid.
According to [33], removing oxygen from the
surface forms new high-energy SO2 adsorp-
tion/oxidation centers. Surface acid groups are
a catalyst for SO2 oxidation [27]; the adsorp-
tion capacity of AC for SO2 is inversely pro-
portional to the amount of O2 adsorbed on its
surface [29].
The reactivity of AC depends on the balance
between the content and type of oxygen func-
tional groups and the surface area [78]. The
authors of [31, 33] found that pyridine func-
tional groups, which are located at the edges
of graphene layers, significantly increase the
amount of SO2 adsorbed and converted into
sulfuric acid, especially when the groups are
located in pores with a size of 7–8 E. The only
negative point of this mechanism is a strong
adsorption of H2SO4 and, as a result, difficul-
ties in the regeneration of adsorbents [27].
The chemical nature of the activated car-
bon surface can be changed by oxidation treat-
ment. After treatment with nitric acid, the total
concentration of surface oxygen increases, the
concentration of basic surface groups decreas-
es significantly, and the content of acid groups
significantly increases, which improves both
the extraction of the formed sulfuric acid and
the adsorption capacity for SO2 and its oxida-
tion [27].
The oxidation of SO2 to H2SO4 (sulfates)
on catalysts takes place via the Eli-Riedil (ER)
[79–81], Langmuir-Hinshelwood (LH) [81,
82] or Mars-van Krevelen (MvK) [81] mecha
nisms: the LH and ER mechanisms account for
the oxidation of SO2 (adsorbed or from the gas
phase) through surface-activated molecular
oxygen, while the MvK mechanism is close-
ly related to surface O lattices that generate
atomic oxygen vacancies during the forma-
tion of SO3 and H2SO4. Since the co-adsorp-
tion of SO2 and O2 on carbon catalysts has a
large adsorption energy (-1.03 eV) compared
to the individual adsorption of SO2 (-0.45 eV)
or O2, then, according to [75], the oxidation
of SO2 on carbon materials is more likely to
occur by the LH mechanism, compared to the
ER mechanism. According to the data given in
the review [83], when SO2 is absorbed from a
gas mixture (SO2 : О2 = 2 : 1), the catalytic ac-
129https://ucj.org.ua
R. E. Khoma, S. V. Vodzinskyi, D. G. Klimov UCJ № 10 / Vol. 89
tivity of adsorbents decreases in the following
order:
АВ > V2О5 > графіт > Сr2О3 > Fe2O3.
The acidic and alkaline modifications of
AC (by impregnating it with 1 M solutions of
HNO3 and KOH, respectively, at 70 °С) affect
the concentration of functional groups on the
surface of AC: they reduce the relative content
of С–Н, but increase the share of the functional
groups С–О, С= О and О=С–О; and the for-
mer modification has a stronger effect than the
latter one [84]. The BET specific surface area
and the total pore volume of acid-modified AC
were decreased, and those of alkali-modified
AC were increased.
In the presence of air moisture, sulfur (IV)
oxide on the AC surface forms a hydrate (reac-
tion 1), which subsequently dissociates (reac-
tion 2), which contributes to an increase in the
acidity of the AC surface:
SO2 + H2O →← SO2⋅H2O, (1)
SO2⋅H2O+ H2O →← HSO–
3 +H3O
+ (2)
Methods of obtaining IACM.
For the preparation of IACM, activated car-
bon of the required quality for a specific ap-
plication is impregnated with solutions of in-
organic and organic compounds (acids, bases,
salts, etc.; see the table ), which after drying or
other stages of further treatment remain on
the inner surface of activated carbon [3, 85,
86]. AC impregnation is carried out by soaking
[14, 87–90], spraying [6], sublimation using a
fluidized bed adsorption column [13, 14]. Im-
pregnation is carried out:
– with some volume of the impregnating
solution, which occupies a certain portion of the
total volume of AC pores (Vр-ну/Vпор) [91, 92];
– by the initial moisture content method
(capillary impregnation, dry impregnation) –
limiting the volume of the solution only to fill
the volume of pores (it is determined at what
volume of the solution for the impregnation of
a water-soluble compound, AC particles be-
gin to adhere to each other or to the walls of
the vessel for impregnation even after several
minutes of mixing after adding the solution)
[12–14, 87, 93–98];
– by the method of ultrasonic impregnation
[36, 55, 99, 100];
– by the method of mechanical mixing [87,
100];
– by the spraying method [5] (AC is sprayed
in a rotating chamber or in a fluidized bed un-
der certain conditions);
– by the high- pressure impregnation me
thod [100];
– by the hydrothermal sol-gel method [34].
In some cases, impregnated reagents are
present in the form of hydroxides, carbonates,
chromates or nitrates, which are subjected to
heat treatment at higher temperatures (150–
400 °C) to decompose the above anions. An
even impregnation distribution on the inner
surface of AC is important. Blocking of micro-
and mesopores (responsible for physical ad-
sorption) should be avoided in order that the
impregnating chemical reagent remains acces-
sible for adsorbates [5, 6].
AC impregnation partially blocks the po-
rosity, but in turn makes AC more capable of
chemisorption, which is necessary to captu
re some low-molecular-weight volatile pollu
tants [3]. Chemisorption is more selective than
physical adsorption, where the size of mole-
cules is critical for an efficient capture process.
During chemisorption, certain chemical bonds
are formed between the surface of activated
130 ISSN 2708-129X. Укр. хім. журн., 2023
IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE.
CHEMISORPTION OF SULFUR DIOXIDE.PHISICAL CHEMISTRY
carbon and the adsorbed compound, so the
choice of impregnating reagents depends on
the field of application. The main technological
requirement to the obtained fibrous IACMs for
respiratory purposes is that after drying they
remain elastic for the construction of filter ele
ments [101].
Adsorption of SO2 on the surface of im-
pregnated activated carbon.
According to the data given in the table,
chemisorbents of SO2 can be AC impregnated
with alkaline reagents (NaOH, KOH, K2CO3,
ammonia, organic amines, etc.); oxidants
(KMnO4, KClO3); ionic liquids (ILs); salts, oxi
des and hydroxides of transition metals (V,
Cr, Mn, Cu, Zn, Ag, Mo, etc.). The protective
properties against SO2, such as dynamic acti
vity (DA, mg of SO2/g), of IACM samples are
affected by the physicochemical characteristics
of the carrier (AC), the nature of the applied
reagents, impregnation and experimental con-
ditions.
Microporous AC obtained by mixing an-
thracite with KOH or NaOH was distinguished
by a large surface area, which makes it a pro
mising sorbent for SO2 capture [55]. In addi-
tion, the products of desulfurization are alkali
metal sulfates (K2SO4, Na2SO4, etc.) applied to
AC, which can be used as soil conditioners or
prolonged fertilizers, eliminating the need for
sorbent regeneration [32].
However, the impregnation of AC based
on coal dust with aqueous NaOH solutions
destroys the strength of the porous structure
and causes its collapse during the adsorption
process, thereby reducing the number of mic
romesopores and the specific surface area of
the carrier and does not contribute to the ad-
sorption of SO2 by AC-NaOH samples [49].
According to X-ray photoelectron spectro
scopy [40], pyridine and pyrrole fragments are
present on the surface of AC-NH3 samples ob-
tained by impregnating AC fibers with aque-
ous solutions of NH3 (for 40 hours) followed
by drying at 100 °C, which causes its increased
alkalinity and enhances catalytic sulfoxidation.
The authors of [102, 103] obtained chemisor-
bents of SO2 with prolonged action by impreg-
nating AC with aqueous solutions of potassi-
um iodide. According to the results of expe
rimental studies by the authors of this review,
the formation of molecular iodine (reaction 3)
was observed on the surface of AC-KI based
on the activated carbon fibers of the "Karbo-
pon- β-Aktiv" material, in contrast to lavsan
fibers [104, 105], which is obviously due to the
presence of acid groups on the surface of the
former:
4I− + 4H3O
+ + O2 → 2I2 + 6H2O. (3)
Thus, iodine formed on a carbon base has
a promoting effect due to hydrolytic oxidation
(reaction 4), improving protective characteris-
tics, similarly to [105].
I2 + HSO3
−+ 4H2O → 2I− + SO4
2− + 3H3O
+ (4)
According to [102], increasing the potassi-
um iodide content of AC-KI to 16% improves
its protective properties against SO2 (τpa (SO2))
according to equation (5); then when ωKI in-
creases to 22%, this characteristic approaches
an almost horizontal asymptote, after which it
sharply decreases. This indicates that at high
contents, KI (like K2CO3 [5], 1,8-diazobicy-
clooctane (DABCO) [106], triethanolammo-
nium citrate (1:3) [107]) aggregates and/or
blocks AC pores, which limits the accessibility
of I2 for SO2. Along with this, increasing the KI
content lowers the sorption capacity of KI with
respect to C6H6 according to equation (6):
131https://ucj.org.ua
R. E. Khoma, S. V. Vodzinskyi, D. G. Klimov UCJ № 10 / Vol. 89
C
ha
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9
[9
6]
132 ISSN 2708-129X. Укр. хім. журн., 2023
IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE.
CHEMISORPTION OF SULFUR DIOXIDE.PHISICAL CHEMISTRY
1
2
3
4
5
6
7
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BC
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pm
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C
Cu
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Ag
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* A
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P
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c
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bo
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po
w
de
r;
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C
Fs
–
a
ct
iv
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ar
bo
n
fib
er
s;
A
BC
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b
io
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n.
133https://ucj.org.ua
R. E. Khoma, S. V. Vodzinskyi, D. G. Klimov UCJ № 10 / Vol. 89
τpa(SO2) = -11,787 + 17,739⋅ωKI,
R2 = 0,9876; n = 12, (5)
τpa(C6H6) = 380,36 – 87,78⋅ωKI,
R2 = 0,9617; n = 12. (6)
where τpa(SO2) is the time of the protective ac-
tion against SO2 (min) at СSO2= 150 mg/m3,
a relative humidity of the GAM of 90-95%, a
flow rate of the GAM of 2.0 cm/s; τpa(C6H6)
is the time of protective action against C6H6
(min) at С6H6 = 500 mg/m3, a relative humi
dity of the GAM of 90–95%, a flow rate of the
GAM of 2.0 cm/s); ωKI is the mass fraction
of KI, %.
The addition of a water-repellent additive
(polytetrafluoroethylene) to AC-KI leads to
the fact that the formed H2SO4 is continuous-
ly released from the surface of AC-KI [102].
However, AC-KI has disadvantages due to the
carrying away of molecular I2 from the surface
with the air flow.
To remove acidic gaseous pollutants, IAC
materials based on impregnating solutions of
N-containing organic bases are used: mono
ethanolamine (MEA) [108-111], diethanola-
mine (DEA) [109, 110, 112], triethanolamine
(TEA) [113], DABCO [14, 106, 112, 114–116],
N-methyldiethanolamine (MDEA) [118], pi
perazine [111], etc., similarly to [119, 120].
IACs based on N-containing organic bases are
also widely used for the sanitary removal of
formaldehyde from the air [121]. As is known
[122], ethanolamines and aminoguanidine
are inhibitors of S(IV) → S(IV) sulfoxidation.
However, no information was found in the li
terature about the effect of AC impregnation
with the listed compounds on the course of the
above reaction on the AC surface.
During the chemisorption of sulfur (IV) oxi
de by carbamide-impregnated AC in the pre
sence of oxygen and water vapor, the following
reduction reactions are possible:
1,5SO2 + (NH2)2CO → 1,5S + N2 + CO2 + 2 H2O;
(7)
H2SO4 + (NH2)2CO → CO2 + N2 + S + 3H2O;
(8)
SO3 + (NH2)2CO → CO2 + N2 + S + 2H2O.
(9)
A special place in gas purification is occu-
pied by IACs based on ionic liquids; in this
case, impregnating solutions are prepared us-
ing nonaqueous solvents (methanol, ethanol)
[96, 107, 123].
Based on data from thermogravimet-
ric, IR and 1H NMR spectroscopic studi
es, it was established [96] that IAC based on
1-ethyl-3-methylimidazolium acetate ([C2mim]
[Ac]; EMA) absorbs SO2 through physical
and chemical sorption. AC-EMA has a bre
akthrough absorption capacity for SO2 that
is 26 times and more greater than that of
AC samples impregnated with other salts:
1-ethyl-3-methylimidazolium (lactate, methyl
sulfate and hydrosulfate), 1-butyl-3-methyli
midazolium (hydrosulfate and tetrafluorobo-
rate), 1-hexyl-3-methylimidazolium (bis(tri-
fluoromethylsulfonyl)imide and tris(penta
fluoroethyl)-trifluorophosphate) and 1-allyl-3-
methylimidazolium (chloride).
The chemisorption of SO2 by the ionic li
quid [C2mim][Ac] on the AC surface occurs
as a result of displacement of acetate anions
by sulfate and sulfite anions [123]. Since hyd
rosulfate (pKb = 17.0 [128]) and hydrosulfite
(pKb = 12.9 [128]) are weaker bases than the
acetate ion (pKb = 9.24 [128]), in the pre
sence of two acids (H2SO4 and SO2⋅H2O),
CH3COO− is protonated and replaced by
134 ISSN 2708-129X. Укр. хім. журн., 2023
IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE.
CHEMISORPTION OF SULFUR DIOXIDE.PHISICAL CHEMISTRY
HSO4− and HSO3− anions, which leads to the
formation of CH3COOH, [C2mim][HSO4] and
[C2mim][HSO3]. Chemisorbed forms of SO2
in the AC-[C2mim][Ac] sorbent can be AC-
[C2mim][HSO4], AC-[C2mim][HSO3], H2SO4
and SO2⋅H2O.
It should be noted that most researchers,
in contrast to [96, 105, 122, 129], do not pay
due attention to the influence of water on the
processes of SO2 capture by both AC and IAC.
The authors of [96] found that increasing the
moisture content (from 50 to 80%) of purified
air increases the protective characteristics of
AC-EMA samples against SO2, which indicates
the predominance of chemical sorption over
physical sorption in this case. Impregnation of
the AC surface with IL: with ammonium cit-
rate and triethanolamine lactate (3TEA⋅H3Cit
and TEA⋅HLact, respectively) leads to an in-
crease in their SO2 absorption capacity from
3.34 and 1.29 mol SO2/mol IL (for [TEAH]3[ Cit]
and [TEAH][Lact]) to 6.60 and 1.95 mol
SO2/mol IL (for samples of AC-[TEAH]3[Cit]
and AC-[TEAH][Lact]) [107]. When impreg
nating with IL, thin films are formed on the AC
surface, and the functional centers of AC are
thereby exposed, which increases their reactiv-
ity towards SO2. The issue of the chemisorp-
tion of sulfur (IV) oxide with IAC samples
based on d-metals has been discussed in detail
in research papers [6, 114, 130] and reviews
[131, 132], which deserves special attention.
CONCLUSIONS. ACs are used as adsor-
bents and catalyst carriers to remove toxic and
irritating gases and vapors from the air. In order
to increase the chemisorption capacity of AC
for chemically hazardous substances of inha-
lation action and acidic and basic nature, their
impregnation with various reagents should be
carried out. Chemisorbents of SO2 can be ACs
impregnated with alkaline reagents, oxidants,
ILs, as well as salts, oxides and hydroxides of
transition metals. The protective properties of
IACM samples against SO2 are influenced by
the physical and chemical characteristics of
the carrier (AC), the chemical nature of the
applied reagents, the impregnation and ex-
perimental conditions. In this regard, IACMs
based on impregnating solutions of N-contain-
ing organic bases are promising, however, due
attention to this issue has not been given by re-
searchers. No data on SO2 sulfoxidation on the
surface of the above chemisorbents were found
in the literature. In our opinion, the influence
of moisture on the chemisorption of SO2 by
IACM samples has been little investigated.
ACKNOWLEDGMENT. The work
was carried out within the framework
of the state budget topic "Scientific
principles of the design and bringing
to a commercial level of the pilot-scale
production of light dual-purpose res-
pirators", state registration number:
0122U000864.
135https://ucj.org.ua
R. E. Khoma, S. V. Vodzinskyi, D. G. Klimov UCJ № 10 / Vol. 89
ІМПРЕГНОВАНІ АКТИВОВАНІ ВУГІЛЬНІ
МАТЕРІАЛИ РЕСПІРАТОРНОГО ПРИЗНАЧЕННЯ
I ХЕМОСОРБЦІЯ ДІОКСИДУ СІРКИ
Р. Е. Хома1,2*, С. В. Водзінський1,2,
Д. Г. Клімов1,3
1Фізико-хімічний інститут захисту нав
колишнього середовища і людини,
вул. Преображенська, 3, Одеса 65082, Україна;
2Одеський національний університет імені
І. І. Мечникова, вул. Дворянська, 2, Одеса
65082, Україна; 3Дніпровський технологіч-
ний університет, просп. Дмитра Яворниць-
кого, 19, Дніпро 49005, Україна
*e-mail: rek@onu.edu.ua
Огляд присвячено використанню ім-
прегнованих активованих вугільних мате-
ріалів як хемосорбентів оксиду сірки (IV).
Розглянуто загальні способи отримання
звичайного активованого вугілля, підго-
товки сировини, її хімічної активації луга-
ми та кислотами з наступним термооброб
ленням (карбонізацією) в інертному серед-
овищі або за присутності газоподібного
окислювача, роль у цьому процесі кислот-
но-основних та окисно-відновних каталіза-
торів.
Вплив на особливості адсорбції оксиду
сірки (IV) хімічного складу поверхні акти-
вованого вугілля, присутності функціональ-
них груп, їхніх кислотно-основних власти-
востей, а також продуктів поверхневих ре-
акцій проаналізовано з точки зору ефектив-
ності видалення та можливості регенерації
SO2. Важливу роль у цих процесах відігра-
ють розмір пор, можливість співадсорбції
води, присутність окислювача. Обговорено
природу взаємодій адсорбент – адсорбат на
поверхні активованого вугілля, їхню енер-
гію, зокрема внесок так званої «фізичної»
адсорбції, ван-дер-ваальсових сил, водне-
вого зв’язку, вплив поверхневих функціо-
нальних груп. Активація вугільної сирови-
ни азотовмісними сполуками призводить
до N-легування поверхні, що підвищує
ефективність адсорбції SO2, полегшуючи не
лише ван-дер-ваальсові та електростатичні
взаємодії, а й S←N зв’язування. Обговорено
також вплив на адсорбцію SO2 кисню та ки-
сеньвмісних функціональних груп.
Для отримання імпрегнованого активо-
ваного вугілля для поглинання SO2 вихідне
активоване вугілля потрібної якості просо-
чують розчинами неорганічних та органіч-
них сполук, які після сушіння залишаються
на внутрішній поверхні активованого ву-
гілля. Імпрегнування блокує частину по-
ристості активованого вугілля, але робить
його більш здатним до хімічної адсорбції.
Хемосорбція, за якої утворюються певні
хімічні зв’язки між поверхнею активовано-
го вугілля і сполукою, що адсорбується, є
більш селективною, ніж фізична адсорбція,
де розмір молекул має вирішальне значен-
ня для ефективного процесу вловлювання.
Можна відмітити, що на відміну від неорга-
нічних лугів, які псують пористу структуру
активованого вугілля, оброблення розчи-
ном аміаку або органічних N-вмісних основ
сприяє поглинанню SO2. Особливе місце у
газоочищенні займає активоване вугілля,
імпрегноване іонними рідинами, при про-
сочуванні якими використовують неводні
розчинники. Окреме питання хемосорбції
оксиду сірки (IV) зразками імпрегнованого
активованого вугілля на основі d-металів
буде детально розглянуто далі.
Ключові слова: імпрегновані активова-
ні вугільні матеріали, діоксид сірки, фізич-
на адсорбція, хемосорбція.
136 ISSN 2708-129X. Укр. хім. журн., 2023
IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE.
CHEMISORPTION OF SULFUR DIOXIDE.PHISICAL CHEMISTRY
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Стаття надійшла 01.11.2023.
|
| id | oai:ojs2.1444248.nisspano.web.hosting-test.net:article-594 |
| institution | Ukrainian Chemistry Journal |
| keywords_txt_mv | keywords |
| language | English |
| last_indexed | 2026-07-23T01:10:58Z |
| publishDate | 2023 |
| publisher | V.I.Vernadsky Institute of General and Inorganic Chemistry |
| record_format | ojs |
| resource_txt_mv | ucjorgua/a6/cdc384fe7c1973f34d7e0573eceaaca6.pdf |
| spelling | oai:ojs2.1444248.nisspano.web.hosting-test.net:article-5942026-07-22T08:23:52Z IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE Khoma, Ruslan Vodzinskii, Sergey Klimov, Danyil impregnated activated carbon materials, sulfur dioxide, physical adsorption, chemisorption. The review is devoted to the use of impregnated activated carbon materials as chemisorbents of sulfur (IV) oxide. General methods for obtaining ordinary activated carbon, preparation of raw materials, their chemical activation with alkalis and acids followed by heat treatment (carbonization) in an inert environment or in the presence of a gaseous oxidizer, the role of acid-base and redox catalysts in this process are considered. The influence of the chemical composition of the  activated carbon surface, the presence of functional groups, and their acid-base properties, as well as the products of surface reactions on the peculiarities of sulfur (IV) oxide  adsorption is analyzed from the point of view of SO2 removal efficiency and the possibility of SO2 regeneration. An important role in these processes is played by the  pore size, the possibility of co-adsorption of water, and the presence of an oxidant. The nature of adsorbent-adsorbate interactions on the surface of activated carbon, their energy, in particular, the contribution of so-called "physical" adsorption, van der Waals forces, hydrogen bonding, and the influence of surface functional groups are discussed. The activation of carbon raw materials with nitrogen-containing compounds leads to the N-doping of the surface, which increases the efficiency of SO2 adsorption, facilitating not only van der Waals and electrostatic interactions, but also S←N binding. The influence of oxygen and oxygen-containing functional groups on SO2 adsorption is also discussed. To obtain impregnated activated carbon for SO2 absorption, the original activated carbon of the required quality is impregnated with solutions of inorganic and organic compounds that remain on the inner surface of the activated carbon after drying. Impregnation blocks partly  the porosity of activated carbon, but makes it more capable of chemical adsorption. Chemisorption, in which certain chemical bonds are formed between the surface of the activated carbon and the compound being adsorbed, is more selective than physical adsorption, where the size of  molecules is critical for an effective capture process. It can be noted that unlike inorganic alkalis, which spoil the porous structure of activated carbon, treatment with a solution of ammonia or organic N-containing bases promotes SO2 absorption. A special place in gas purification is occupied by activated carbon impregnated with ionic liquids, non-aqueous solvents being used for impregnation. A separate issue of the chemisorption of sulfur (IV) oxide by samples of impregnated activated carbon based on d-metals will be discussed in detail below. V.I.Vernadsky Institute of General and Inorganic Chemistry 2023-11-24 Article Article Physical chemistry Физическая xимия Фізична xімія application/pdf https://ucj.org.ua/index.php/journal/article/view/594 10.33609/2708-129X.89.10.2023.124-144 Ukrainian Chemistry Journal; Vol. 89 No. 10 (2023): Ukrainian Chemistry Journal; 124-144 Украинский химический журнал; ##issue.vol## 89 ##issue.no## 10 (2023): Ukrainian Chemistry Journal; 124-144 Український хімічний журнал; Том 89 № 10 (2023): Український хімічний журнал; 124-144 2708-129X 2708-1281 en https://ucj.org.ua/index.php/journal/article/view/594/305 Copyright (c) 2023 Ruslan Khoma, Sergey Vodzinskii, Danyil Klimov https://creativecommons.org/licenses/by-nc/4.0 |
| spellingShingle | Khoma, Ruslan Vodzinskii, Sergey Klimov, Danyil IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE |
| title | IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE |
| title_full | IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE |
| title_fullStr | IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE |
| title_full_unstemmed | IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE |
| title_short | IMPREGNATED ACTIVATED CARBON MATERIALS FOR RESPIRATORY PURPOSE. CHEMISORPTION OF SULFUR DIOXIDE |
| title_sort | impregnated activated carbon materials for respiratory purpose. chemisorption of sulfur dioxide |
| topic_facet | impregnated activated carbon materials sulfur dioxide physical adsorption chemisorption. |
| url | https://ucj.org.ua/index.php/journal/article/view/594 |
| work_keys_str_mv | AT khomaruslan impregnatedactivatedcarbonmaterialsforrespiratorypurposechemisorptionofsulfurdioxide AT vodzinskiisergey impregnatedactivatedcarbonmaterialsforrespiratorypurposechemisorptionofsulfurdioxide AT klimovdanyil impregnatedactivatedcarbonmaterialsforrespiratorypurposechemisorptionofsulfurdioxide |