(illustrative examples)
(English versions of the papers given in Russian are available at the
British Library Board or "NAUKA/INTERPERIODICA" Publ. Co.)
Fundamental problems of
catalysis and adsorption
V.E. Ostrovskii, "Paradox of
heterogeneous catalysis": paradox or regularity, Ind. Eng. Chem.
Res., 43 (2004) 3113-3126. Abstract: "The paradox of
heterogeneous
catalysis" reflects an opinion that no data file on stationary rates of
a heterogeneous catalytic reaction can clarify whether the surface
heterogeneity is of principal importance for the catalysis and that the
surface heterogeneity is an open question. On the other hand, followers
of notions on principal importance of surface heterogeneity consider
the power-law kinetic equations for catalytic processes and also
logarithmic isotherms and exponential rate-coverage dependences for
middle-coverage chemisorption equilibriums and rates, respectively, as
the manifestations and proofs of surface heterogeneity. In this paper,
it is shown that the available power-law kinetic equations and the
relations translated by the logarithmic isotherms and exponential
rate-coverage dependences can be deduced on the basis of the notion on
surface uniformity. In addition, about 40 available metal-gas systems
demonstrating the constancy of the molar heats of chemisorption over
wide ranges of coverages are listed and the temporal tendency of the
measured molar heats of chemisorption to approach to constant levels,
as the techniques and procedures are improved, is demonstrated. It is
concluded that no surface heterogeneity reveals itself in catalysis and
chemisorption at metals and the paradox arose from algebraic
peculiarities.
V.E. Ostrovskii, Mechanisms of
methanol synthesis from hydrogen and carbon oxides at Cu-Zn-containing
catalysts in the context of some fundamental problems of heterogeneous
catalysis, Catal. Today, 77 (2002) 141-160. Abstract: It is stated
that, for deduction of the kinetic equation of a heterogeneous
catalytic process proceeding with a rate-determining step (RDS), it is
necessary and sufficient to reveal the chemical nature of the RDS,
composition of the surface intermediates, and stoichiometric number
(SN) of the RDS. On the basis of calorimetric and adsorption methods
applied to the Cu-Zn-containing catalyst reduced to a state identical
to that occurring during the steady-state methanol synthesis from
hydrogen and carbon oxides, three catalytic surfaces (S1, S2,
and S3) are specified and the individual steps of the
steady-state process are studied. It is stated that CH3OH is
produced at S2 (the ZnO-component) from H2 and CO2
by two routes N1 and N2 with RDSs of interaction
between gaseous H2 or CO2 and adsorbed CO2
or H2, respectively, SN = 2 for each RDS, and the adsorbed
intermediates are H2, CO2, HCOH, HCOOH, and O2;
CO2 is produced at S1 (the Cu-component
approximated by Cu4∙OH2) through the
shift-reaction; S1 and S2 are homogeneous in
their
adsorption properties. The causes of the absence of manifestation of
the
structural heterogeneity of catalysts in their adsorption and catalytic
properties are considered.
V.E.Ostrovskii, Mechanisms of
heterogeneous catalytic processes, Dokl. AN SSSR, 313 (1990)
645-650.
V.E.Ostrovskii, On the essence
of the logarithmic isotherm in adsorption and electrochemical studies,
Dokl. AN SSSR, 307 (1989) 1165-1169.
V.E.Ostrovskii, Progress in the
methods of describing of adsorption in the context of general
postulates of the Langmuir theory, Uspechi chimii (Rus. Chem.
Rev.), 45 (1976) 849-876.
Application of
calorimetric and adsorption techniques and theoretical approaches
(a) redox
heterogeneous catalytic reactions and chemisorption.
V .E. Ostrovskii, Mechanisms of
methanol synthesis from hydrogen and carbon oxides at
copper-zinc-containing catalysts, Khim.tverdogo topl. (Chemistry
of solid fuel), no.1 (2002) 59-79 (volumes are not numerated).
V.E.Ostrovskii, On the
mechanisms of the ammonia synthesis on iron catalysts and on the
kinetic equation of the process, Zh. Phys. Khim.(Rus. J. Phys.
Chem.), 63 (1989) 2560-2570. Abstract: Basing on an
analysis of available data relating to the properties of catalytic
surfaces and to the individual steps of the process of ammonia
formation, we show that the basic assumptions on the mechanism of this
process postulated in the earlier works by Temkin are not fulfilled. We
propose a mechanism which is not inconsistent with the experimental
data on the reaction steps and leads to a kinetic equation which
describes the rates of the synthesis both under industrial conditions
(i.e. close to the equilibrium) and far from the equilibrium. The
mechanism does not stipulate heterogeneity of the surface with respect
to adsorption capacity and treats the reaction as taking place on a
surface almost entirely covered with nitrogen atoms or by species
containing one nitrogen atom and one or two hydrogen atoms.
V.E. Ostrovskii, Metal-oxygen-hydrogen
solid system of controlled composition: differential heat effects,
kinetics, and mechanism of the CuO --> Cu4∙OH2
grading, Intern. J. Modern Phys. B, 16 (1-2) (2002) 42-49. Abstract: The process of
fine-crystal CuO reduction by successive small portions of H2
was studied through isothermal calorimetric, kinetic,
adsorption-desorption, and stoichiometric measurements at 293-520 K and
H2 pressures up to 100 Pa under conditions when equilibrium
within the solid was achieved at any instant. The CuO studied was in
the form of the component of the CuO-ZnO-Al2O3
system. The stoichiometry of the copper component reduced corresponded
to Cu4∙OH2.
V.E. Ostrovskii, Heats of
oxygen chemisorption by cobalt and the influence of inert gases on the
rate of chemisorption, Zh. Fiz. Khim. (Rus. J. Phys. Chem.), 62
(1988) 674-681.
A.A. Dyatlov, V.E. Ostrovskii, Identification
of substances desorbing under vacuum from the surface of a
copper-zinc-aluminum catalyst of methanol synthesis after carbon
dioxide and hydrogen chemisorption by the catalyst, Kinet.
Katal., 26 (1985) 1154-1161.
A.A. Dyatlov, V.E. Ostrovskii, Chemisorption
of carbon dioxide, oxygen and hydrogen on the Cu-Zn-Al catalyst of the
methanol synthesis, Kinet. Katal., 25 (1984) 159-168.
V.E. Ostrovskii, E.A. Medvedkova, Calorimetric and adsorption study of
oxygen, hydrogen and water interaction with surface of silver catalyst,
Kinet. Katal., 20 (1979) 966-973.
V.E. Ostrovskii, A.A. Dyatlov, Calorimetric
study of the mechanisms of CO and hydrogen oxidation and of shift
reaction on an oxide Cu-Cr catalyst, Kinet. Katal., 20 (1979)
958-968.
V.E. Ostrovskii, Combined use
of calorimetric and adsorption kinetic methods for the study of the
mechanisms of catalytic processes, J. Therm Anal., 14 (1978)
27-43.
V.E. Ostrovskii, E.G. Igranova, Calorimetric
study of heats of nitrogen chemisorption at the catalyst of ammonia
synthesis, Kinet. Katal., 19 (1978) 681-689.
E.G. Igranova, V.E. Ostrovskii, M.I. Temkin, Calorimetric study of nitrogen incomplete
hydrogenation products adsorbed on iron catalyst, in the context of the
mechanisms of ammonia synthesis, Kinet. Katal., 17 (1976)
1257-1265.
V.E. Ostrovskii, A.A. Dyatlov, N.N. Dobrovol’skii, Mechanisms and kinetics of hydrogen
oxidation at black copper oxide, Kinet. Katal., 17 (1976)
405-412.
E.G. Igranova, V.E. Ostrovskii, Calorimetric
study of hydrogen sorption at an iron catalyst of ammonia synthesis,
Dokl. AN SSSR, 221 (1975) 1351-1356.
V.E. Ostrovskii, Differential
heats of hydrogen adsorption on surface of NiO and kinetics of the
process, Dokl. AN SSSR, 196 (1971) 1141-1149.
N.N. Dobrovol’skii, V.E. Ostrovskii, Kinetics and differential heats of
adsorption of oxygen on gold, Kinet. Katal., 12 (1971)
1495-1502.
V.E. Ostrovskii, B.B. Chesnokov, M.I. Temkin, Adiabatic warming of coal as a result of
ethylene adsorption, Khim. prom. (Chemical industry), no. 12
(1968) 926-930 (volumes are not numerated).
V.E. Ostrovskii, Study of
oxygen and hydrogen adsorption on copper by a method of adsorption
calorimetry, Dokl. AN SSSR, 172 (1967) 892-897.
(b) catalytic
polymerization
V.E. Ostrovskii, V.A. Khodzhemirov, Catalytic polymerization of ethylene,
1,4-butadiene, and ethylene oxide with no solvent: heat effects,
kinetics, and mechanisms, Mol. Cryst. Liq. Cryst.,390 (2003)
67-78. Abstract: The processes of
solid polyethyleneoxide (PEO), polyethylene (PE), and
trans-1,4-polybutadiene (PB) formation at solid catalysts in gas-solid
systems with no solvent are studied. For a monomer pressure of 760
Torr, maximum rates of 1.5∙10-7, 1.2∙10-5, and
4∙10-7 (mol/s cm3) are fixed for C2H4O,
C2H4, and 1,4-C4H6
polymerization, respectively; therewith, potentialities of
intensification of the reactions are not exhausted. The DH0298
values
measured for the reaction (MON)(gas) = (1/n) (-MON-)n(solid)
(MON is a monomer molecule) are -107.5+/-2.5, -112.5+/-2.5, and
-140.5+/-3.8 (kJ/mol) for PE, PB, and PEO, respectively.
V.E. Ostrovskii, V.A. Khodzhemirov, Polyethyleneoxide: kinetics and
polymerization heat measurements for the process of catalytic
polymerization in a solid-gas system free of solvent, Int. J.
Modern Phys. B,16(1) (2002) 399-406. Abstract: The process of
polymerization of ethylene-oxide (EO) vapor to solid polyethyleneoxide
(PEO) at the dry KOH catalyst with no solvent is studied at 298 K and a
monomer pressure up to 400 Torr. The maximum rate observed is about
1.5∙10-7 mol/s per 1 cm3 of the catalyst at 760
Torr; therewith, potentialities of intensification of the process are
not exhausted. It is found that, at any fixed degree of polymerization,
the rate of the process is proportional to the monomer pressure. A
phenomenon of gradual increasing in the rate of polymerization with the
degree of polymerization is observed. The DH0298 value
measured for the reaction n(EO)(gas) = (-EO-)n(solid)
is equal to -140.5+/-3.8 kJ/mol; by using this value, DH(liq. EO P sol.. PEO) = -109.20
kJ/mol is computed. The calorimetric results and the nature of the
phenomenon revealed are discussed.
(c) physical adsorption
K.I.Sakodynsky, V.E.Ostrovskii, L.D.Glazunova, Study of some polymeric sorbents by
adsorption and calorimetric methods, J. Chromatogr., 156 (1978)
233-240.
V.E.Ostrovskii, L.D.Glazunova, Heats
of vapor adsorption and mechanisms of vapor adsorption on polymer
sorbents, Kinet. Katal., 18 (1977) 995-1004.
L.D. Glazunova, V.E. Ostrovskii, K.I. Sakodynskii, Use of the theory of polymolecular
adsorption on heterogeneous surfaces for description of adsorption of
hydrocarbons on polymer sorbents, Zh. Teor. Eksp. Khim. (J.
Theor. Exper. Chem.), 12 (1976) 482-490.
V.E. Ostrovskii, A.N. Abdrakhimova, K.I. Sakodynskii, Adsorption equilibrium and heats of butane
adsorption on polydivinylbenzene, Dokl. AN SSSR, 208 (1973)
654-659.
(d) H2O
sorption by monomers and polymers (including DNA), wetting and drying
V.E. Ostrovskii, E.A. Kadyshevich, Hydrate model of the equilibrium DNA-water
systems, Intern. J. of Nanoscience, 1 (2002) 101-121. Abstract: A hydrate model
for the DNA-H2O system is proposed. For the notions developed,
available data on a tendency of H2O molecules to form
structured hydrates containing atomic groups, molecules, or atoms
housed
within the structural cavities formed by H-bonded H2O
molecules are used. It is shown that the large and small cavities of
the hydrate structure II are in close geometric agreement with N-bases
and deoxyribose and with other atomic groups of DNA molecules,
respectively. On the basis of the model proposed and with the
Watson-Crick base-pairing scheme, the number of pairs of N-bases per
helix turn (11.25), the density (1.161 g/cm3), and the helix
step (0.567 nm) for the quasi-equilibrium DNA (RNA)-water system are
computed, the last value nearly coinciding with the well-known
alpha-helix step in the protein secondary structure (5.44 nm). It is
found that the density computed by us for Wilkins-Franklin's DNA-H2O
samples assumed to be non-equilibrium (1.351 g/cm3) is in
accordance with their earlier data. (1.34-1.39 g/cm3).
Assumptions on the phenomenology of some stages of mitosis are
presented.
V.E. Ostrovskii, B.V. Tsurkova, E.A. Kadyshevich, B.V. Gostev, Comparison study of the acrylamide-water
and polyacrylamide-water systems: differential heat effects, kinetics,
and mechanisms of drying and water-vapor wetting, J. Phys.
Chem. B, 105 (2001) 12680-12687. Abstract: Heat effects and
kinetics of wetting by water vapor and of vacuum drying in the
acrylamide (AA)-water system at 0 < n < 74 (n is the number of
sorbed water molecules per one AA molecule) are studied. The water
sorption by AA from air of 100% humidity appears to be limitless. It is
shown that the differential heats of water sorption are about 25 kJ/mol
at dry AA, pass a maximum of 42 kJ/mol in the vicinity of n = 1 and a
minimum of 24 kJ/mol in the vicinity of n = 2, and then approach the
level of the heat of water condensation on the pure water surface;
probability of vacuum desorption of water molecules is totally
increasing with n, and against this background, minima at n = 5-6 and n
= 15-17 are observed. The results are compared with the corresponding
data for the polyacrylamide (PAA)-water system; the mechanisms of
wetting and drying of these two systems are developed on the basis of
the new results, available literature and our previous pattern.
V.E.Ostrovskii, E.A. Kadyshevich, Use of data on the polyacrylamide–water
system for clarification of the equilibrium DNA–water system structure,
Rus. J. Phys. Chem., 74 (2000) 1114-1124.
V.E. Ostrovskii, B.V. Tsurkova, The
polyacrylamide-water system: application of differential calorimetry to
study the mechanisms of dissolution, Thermochem. Acta, 316
(1998) 111-122. Abstract: Differential
heat
effects and rates of water sorption and desorption are investigated in
the polyacrylamide (PAA)-water system at 0 < n < 25 (n = (H2O)sorb
/(-C(O)NH2)). It is stated that, at 292 K in air of 100%
humidity, the equilibrium corresponds to n ~ 18 (n (eq)); the heats of
water vapor sorption decrease from 56 kJ/mol (initial heat) to the
heat of water vaporization (QL) at n ~ 0.5, and then
they pass (up to n (eq)) through several maxima and minima
in the vicinity of QL; at n > n (eq) they are equal
to QL. It is concluded that sorption of water by dry PAA
leads to linearization of PAA molecules, to the space between the amido
groups of each PAA molecule being filled with water, and to neighboring
order at which each PAA molecule is surrounded (at the section normal
to the main carbon chain) by six nearest ones. At equilibrium, the PAA
molecules are separated from each other by a water layer of
three-molecule thickness.
V.E. Ostrovskii, B.V. Tsurkova, Differential
heat effects and mechanisms of interaction of polyacrylamide with water,
Zh. Fiz. Khim.(Russ. J. Phys. Chem), 71 (1997) 967-973.
V.E. Ostrovskii, B.V.Gostev, Heat
effects and rates and molecular mechanisms of water sorption by
pefluorinated polymer materials bearing functional groups, J.
Therm. Anal., 46 (1996) 397-416. Abstract: The heat effects
and the rates and equilibrium quantities of H2O vapour sorbed and
desorbed on polymeric perfluorinated materials (functional groups -SO3H,
-SO3Na, -SO3K) and on material treated with FeCl3
solution as sorbent were investigated. Sorbed H2O may be
completely desorbed in vacuum at 443 K. The material bearing -SO3H
has maximum sorption affinity: the molar heat of -SO3H
wetting is close to that of H2SO4 wetting. The
differential heat of sorption decreases from 68 kJ/mol at n~0 (n = H2O/-SO3H)
to 45 kJ/mol at n~5, but not below the heat of H2O
condensation. The -SO3H samples sorb H2O vapour
in the presence of liquid H2O at 293 K up to n~17. The -SO3K
material has minimum affinity for H2O: the equilibrium
quantity sorbed in room air is less by a factor of 4 than that for the
-SO3H material. The spatial arrangement of H2O
molecules near the sulpho groups is considered.
B.V. Gostev, V.E. Ostrovskii, Water
sorption by perfluorinated membrane materials treated by ferric
chloride water solution, Zh. Fiz. Khim. (Russ. J. Phys. Chem),
68 (1994) 668-675.
V.E. Ostrovskii, S.A. Artamonov, G.P. Korneeva, et al., Heats of acrylamide dissolution in water,
Izv. AN Kaz. SSR (Proc. Kazakh. Acad. Sci.), B, no. 4 (1974) 84-88.
Scientific
Instrumentation and Methodology
V.E. Ostrovskii, Some problems
in adsorption and calorimetric studies of the steps of catalytic
processes, J. Natural Gas Chem., 13 (2004) 123-147. Abstract: Principal side
factors as well as technical and procedural peculiarities capable of
distorting the results of measurements of adsorbed and desorbed
amounts, of falsifying the nature of the processes proceeding in the
systems under study, and of promoting artifacts in calorimetric and
other studies of gas chemisorption on powders are considered. Modified
techniques and procedures allowing the elimination of sources of side
phenomena and artifacts and freeing traditional glass static adsorption
apparatuses and experimental procedures from undesirable factors and
peculiarities are proposed. Some available chemisorption and
calorimetric data representing artifacts and also some data that are
not artifacts but, due to imperfections of chemisorption techniques,
show up as artifacts are presented and discussed. Several applications
of the improved techniques and procedures to calorimetric and
adsorption studies of the steps of catalytic processes proceeding on
the basis of natural gas and of products of its processing are
presented and iscussed.
Microcalorimeter
"FOSKA"
- calorimetric vessel,
- calorimetric ampoule,
- Pt thermoresistors,
- insulating rings,
- insulating tubes,
- whatnot devices,
- canisters,
- metal block,
- heater,
- detent,
- insulating material.
V.E. Ostrovskii, Differential
microcalorimeter for isothermal measurements of heat effects in
two-phase systems and examples of its application, Rev. Sci.
Instr., 73 (2002) 1304-12. Abstract: A differential
heat-conducting double microcalorimeter intended for heat measurements
at 300-700 K is described. Platinum resistance thermometers are applied
as the heat-flux sensors. The calorimeter is a low-noise instrument
with the baseline fluctuations ranging up to 0.02∙10-6 V
(5∙10-6
W); it allows measurements of the heat effects with an error of 1-1.5%
at a recorder scale of about 1∙10-2 J/cm2. The
design features and the method of the heat flux transformation to the
electric signals, the calorimetric ampoules for measurements and for
calibration and the calibrating device, the heat-balance equation and
the equation for the temperature dependence of the calorimetric
sensitivity, the results of the calibration and the verification of the
calorimeter, and a number of illustrative examples of calorimetric
measurements are presented. The calorimeters are applicable for
studying solid-gas, solid-liquid, and liquid-gas interactions and
thermophysical characteristics of solids and liquids.
V.E. Ostrovskii, N.V. Kul’kova, M.S. Kharson, M.I. Temkin, Kinetics of ethylene oxidation,
Kinet. Katal., 5 (1964) 469-476.
V.E. Ostrovskii, N.V. Kul’kova, V.L. Lopatin, M.I. Temkin, Influence of electronegative elements on
catalytic properties of silver catalysts in the process of ethylene
oxidation, Kinet. Katal., 3 (1962) 189-195.