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 COMPUTATIONAL AND
EXPERIMENTAL ANALYSIS OF
FUNCTIONAL MATERIALS
 AAP Research Notes on Polymer Engineering
Science and Technology

COMPUTATIONAL AND
EXPERIMENTAL ANALYSIS OF
FUNCTIONAL MATERIALS

Edited by
Oleksandr V. Reshetnyak, DSc
Gennady E. Zaikov, DSc
Apple Academic Press Inc. Apple Academic Press Inc.
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International Standard Book Number-13: 978-1-77188-342-9 (Hardcover)
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Library and Archives Canada Cataloguing in Publication

Computational and experimental analysis of functional materials / edited by Oleksandr Reshetnyak, DSc, Gennady E.
Zaikov, DSc.
(AAP research notes on polymer engineering science and technology series)
Includes bibliographical references and index.
Issued in print and electronic formats.
ISBN 978-1-77188-342-9 (hardcover).--ISBN978-1-315-36635-7 (PDF)
1. Polyanilines--Synthesis. 2. Polymeric composites. I. Zaikov, G. E. (Gennadii Efremovich), 1935-, editor
II. Reshetnyak, Oleksandr, author, editor III. Series: AAP research notes on polymer engineering science and
technology series
TP1180.P552C64 2017 668.9 C2016-907864-7 C2016-907865-5

Library of Congress Cataloging-in-Publication Data

Names: Reshetnyak, Oleksandr, editor. | Zaikov, G. E. (Gennadiæi Efremovich), 1935- editor.

Title: Computational and experimental analysis of functional materials / editors, Oleksandr Reshetnyak, DSc,
Gennady E. Zaikov, DSc.
Description: Toronto : Apple Academic Press, [2017] | Includes bibliographical references and index.
Identifiers: LCCN 2016054503 (print) | LCCN 2016057620 (ebook) | ISBN 9781771883429 (hardcover : alk. paper)
| ISBN 9781315366357 (ebook)
Subjects: LCSH: Polyanilines. | Conducting polymers. | Materials science.
Classification: LCC TP1180.P552 C66 2017 (print) | LCC TP1180.P552 (ebook) | DDC 620.1/9204297--dc23
LC record available at https://lccn.loc.gov/2016054503

Apple Academic Press also publishes its books in a variety of electronic formats. Some content that appears
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This book is dedicated to the memory of
Professor Eugen P. Koval’chuk, DSc
(1939–2012)
ABOUT THE EDITORS

Oleksandr V. Reshetnyak, DSc

Oleksandr Reshetnyak, DSc, is Head of the Department of Physical and
Colloid Chemistry of Ivan Franko National University of Lviv (Lviv,
Ukraine). He is the author of two monographs and more than 150 publica-
tions in various journals and conference proceedings. His scientific activity
is in the fields of physical chemistry of nanosystems, conductive polymers
and its composites, electrochemistry of organic compounds, and chemi- and
electrochemiluminescence. He is a member of the Editorial Board of the
Visnyk Lviv University Journal (Series: Chemistry) (Lviv, Ukraine) as well
as a member of the Editorial Board of the bimonthly scientific and technical
international journal Materials Science. He is also an active member of the
Taras Shevchenko Scientific Society (Lviv, Ukraine).
Contact address:
6 Kyryla & Mefodiya Str., Lviv, 79005, Ukraine
Tel: (+38) (032) 2600–397
Fax: (+38) (032) 2600–397
E-mail: reshetniak@franko.lviv.ua; Olexandr.Reshetnyak@gmail.com.

Gennady E. Zaikov, DSc

Gennady Zaikov, DSc, is Head of the Department of the Kinetics of Chem-
ical & Biological Processes at the N. M. Emanuel Institute of Biochemical
Physics at the Russian Academy of Sciences (Moscow, Russia) and Professor
at Moscow State Academy of Fine Chemical Technology (Russia) as well
as Professor at Kazan National Research Technological University (Kazan,
Russia). He is also a prolific author, researcher, and lecturer.
Contact address:
4 Kosygin Str., Moscow, 119991, Russia
Tel: 7 (495) 1374–101
Fax: 7 (495) 9397–320
E-mail: chembio@sky.chph.ras.ru
CONTENTS

List of Contributors ....................................................................................... xi

List of Abbreviations ...................................................................................xiii
Supporting Institutions ................................................................................ xix
Preface ........................................................................................................ xxi

1. Polyanilines: The Role of Particles of Radical Nature in Obtaining

of Polymers/Copolymers with a System of Conjugated π-Bonds ...............1
O. V. Reshetnyak, M. M. Yatsyshyn, and L. I. Bazylyak

2. Morphology of Polyaniline’s Films Electrochemically Deposited

on the Surface of Al-Based Amorphous Metal Alloys ................................61
М. М. Yatsyshyn, L. М. Boichyshyn, I. I. Demchyna, and Yu. A. Hnizdiukh

3. Electrooptic Phenomena in Conjugated Polymeric Systems Based

on Polyaniline and Its Derivatives ...............................................................91
О. I. Aksimentyeva, О. I. Konopelnyk, and D. О. Poliovyi

4. An Investigation of Monomolecular Films of Polyanilines .....................151

I. Ye. Opaynych, О. I. Aksimentyeva, and Yu. Yu. Horbenko

5. Epoxy–Polyaniline Composites: Synthesis, Structure, Properties .........179

V. P. Zakordonskiy, О. I. Aksimentyeva, and A. I. Krupak

6. Thermochromic Effect in the Films of Conjugated Polyaminoarenes ...219

О. I. Konopelnyk and О. I. Aksimentyeva

7. Polyaniline in Chemo-and Biosensorics: Overview .................................243

Ya. S. Kovalyshyn and O. V. Reshetnyak

8. Corrosion Protection of Aluminum and Al-Based Alloys by

Polyaniline and Its Composites ..................................................................287
О. V. Reshetnyak and М. M. Yatsyshyn

9. Synthesis and Physico–Chemical Properties of Composites of

Conjugated Polyaminoarenes with Dielectric Polymeric Matrices ........331
О. I. Aksimentyeva, О. I. Konopelnyk, G. V. Martyniuk, and O. M. Yevchuk

10. Polyanilines: Generation of Electrochemiluminescence..........................371

О. V. Reshetnyak
x Contents

11. Synthesis and Properties of Composites Based on Polyaniline and

Poly(Aniline-cо-Nitroaniline) with Xerogel of Vanadium (V) Oxide .....397
B. B. Ostapovych, O. V. Reshetnyak, and M. V. Buzhans’ka

12. Surface Modification of Polymeric Materials by Polyaniline

and Application of Polyaniline/Polymeric Composites............................423
Yu. A. Hnizdiukh, M. M. Yatsyshyn, and O. V. Reshetnyak

13. Hybrid Nanosystems Based on Conjugated Polyaminoarenes

Doped by Ferrum–Containing Compounds .............................................473
О. I. Aksimentyeva, Yu. Yu. Horbenko, and О. I. Konopelnyk

14. Structure and Thermal Stability of Silica–Glauconi-

Te / Polyaniline Composite .........................................................................497
M. M. Yatsyshyn, V. M. Makogon, O. V. Reshetnyak, and J. Błażejowski

Index .....................................................................................................................521
LIST OF CONTRIBUTORS

Olena I. Aksimentyeva
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Doctor of Science in Chemical Sciences, Chief Scientific Officer. E-mail: aksimen@
ukr.net

Liliya I. Bazylyak
Department of Physical Chemistry of Fossil Fuels, Institute of Physical–Organic Chemistry and Coal
Chemistry named after L. M. Lytvynenko, National Academy of Sciences of Ukraine; Candidate of
Science (Ph.D.) in Chemical Sciences, Senior Researcher. E-mail: bazyljak.l.i@nas.gov.ua

Jerzy Błażejowski
Department of Physical Chemistry, Faculty of Chemistry of the University of Gdańsk; Doctor of Science
in Chemical Sciences, Professor, Head of the Department. E-mail: jerzy.blazejowski@ug.edu.pl

Lidiya M. Boichyshyn
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Candidate of Science (Ph.D.) in Chemical Sciences, Docent (Associate Professor).
E-mail: lboichyshyn@yahoo.com

Mar’yana V. Buzhans’ka
Department of Chemistry and Physics, Lviv Aсademy of Commerce; Candidate of Science (Ph.D.) in
Chemical Sciences, Docent (Associate Professor)

Іvanna І. Demchyna
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Master in Chemistry, Postgraduate Student

Yuliia A. Hnizdiukh
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Master in Chemistry, Postgraduate Student. E-mail: yulya_hnisdyuch@ukr.net

Yulia Yu. Horbenko

Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Master in Biology and Biochemistry, Junior Researcher. E-mail: y-bilka@ukr.net

Oksana I. Konopelnyk
Department of General Physics, Faculty of Physics of the Ivan Franko National University of Lviv;
Candidate of Science (Ph.D.) in Physico–Mathematical Sciences, Docent (Associate Professor)

Yaroslav S. Kovalyshyn
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Candidate of Science (Ph.D.) in Chemical Sciences, Docent (Associate Professor).
E-mail: kovalyshyn@yahoo.com

Andriy I. Krupak
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Master in Chemistry, Junior Researcher

Viktoria M. Makogon
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Master in Chemistry, Postgraduate Student
xii List of Contributors

Galyna V. Martynyuk
Department of Methodology of Teaching of Physics and Chemistry, State Humanitarian University
of Rivne; Candidate of Science (Ph.D.) in Chemical Sciences, Docent (Associate Professor). E-mail:
galmart@ukr.net

Іryna Ye. Opaynych

Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Candidate of Science (Ph.D.) in Chemical Sciences, Senior Researcher

Bogdan B. Ostapovych
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Candidate of Science (Ph.D.) in Chemical Sciences, Docent (Associate Professor).
E-mail: bohdanostapovych@ukr.net

Dmytro О. Poliovyi
Department of Biology and General Ecology, Natural and Engineering Faculty of Kremenetski Regional
Humanitarian Pedagogical Institute named after Taras Shevchenko; Candidate of Science (Ph.D.) in
Chemical Sciences, Docent (Associate Professor)

Oleksandr V. Reshetnyak
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Doctor of Science in Chemical Sciences, Professor, Head of the Department. E-mail:
reshetniak@franko.lviv.ua

Mykhaylo M. Yatsyshyn
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Candidate of Science (Ph.D.) in Chemical Sciences, Docent (Associate Professor).
E-mail: m_yatsyshyn@franko.lviv.ua

Oksana M. Yevchuk
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Bachelor in Chemistry, Ph.D. getter

Gennady E. Zaikov
Kinetics of Chemical & Biological Processes Department of Institute of Biochemical Physics named
after N. N. Emanuel, Russian Academy of Sciences D.Sc. in Chemical Sciences, Head of the Department

Viktor P. Zakordonskiy
Department of Physical and Colloid Chemistry, Faculty of Chemistry of the Ivan Franko National
University of Lviv; Candidate of Science (Ph.D.) in Chemical Sciences, Senior Researcher. E-mail:
zakordonskiy@franko.lviv.ua
LIST OF ABBREVIATIONS

AA Al–alloys
AAc acrylic acid
AAr aminoarenes
AcN acetonitrile
ABS acrylonitrile–butadiene–styrene
AFM atomic force microscopy
AMA amorphous metal alloys
An aniline
An–BF3 aniline doped by tetrafluorborate acid
AnSi N–(3–trimethoxysilylpropyl)aniline
ANSA aminonaphthylsulphoacid
AO atomic orbitals
APS ammonium persulphate
ASA acetyl salicylic acid
Au–NPs nanoparticles functionalized by gold
BP benzoyl peroxide
BSA bovine serum albumin
CF Faraday capacitance
CCC cerium conversion coatings
CcFs coconut fibers
CeAFs cellulose acetate nanofibers
CFs curauá fiber
CL сhemiluminescence
CNT carbon nanotubes
CR contrast
CSA camphorosulfonic acid
Cu–NPs nanoparticles functionalized by copper
CVA cyclic voltammetry
DBSA dodecylbenzenesulfonic acid
DCA dichloric–acetic acid
Deff effective diffusion coefficient
DEL double electric layer
DMFA dimethylformamide
DN donor number
xiv List of Abbreviations

DNNSA dinonylnaphthalenesulfonic acid

DMI 1,3–dimethyl–2–imidazolidinone
DMSO dimethylsulfoxide
DSC differential scanning calorimetry
DTA differential thermal analysis
DTG differential mass loss curves
E emeraldine
EB emeraldine base
ECe ethyl cellulose
EChM electrochromic materials
EChP electrochromic polymers
ECL electrochemiluminescence
ECP electroconductive polymers
EDOT 3,4–ethylenedioxythiophene
EES electrochemical energy storage
EPD electrophoretic monochrome display
ER epoxy resin
ES emeraldine salt
EPD electrophoretic monochrome display
EPO/PAn epoxy–polyaniline composites
FEP fluorinated ethylene propylene copolymer
FSA ferrocenesulfonic acid
FTIR Fourier transform infrared spectroscopy
HDPE high-density polyethylene
HOMO high occupied molecular orbital
HRP horseradish peroxidase
ICPs intrinsically conducting polymers
IDPD integral procedural decomposition temperature
IPN interpenetrating polymer networks
ІТО indium–tin–oxide
IR infrared (spectrum, spectroscopy)
JFs jute fibers
ks heterogeneous constant of a charge transport
L leucoemeraldine
LB leucoemeraldine base
LB films Langmuir‒Blodgett films
LC liquid crystals
LDPE low-density polyethylene
LECs light-emitting electrochemical cells
LEDs light-emitting diodes
List of Abbreviations xv

LGS lignosulfonate
Lum luminol
LUMO low unoccupied molecular orbital
λmax maximum absorption/transmission
LS leucoemeraldine salt
MDTIR multiply disturbed total internal reflection
MMT montmorrilonite
MPD N–methylpyrrolidone
MS mass spectrometry
MWCNT multiwalled carbon nanotubes
NAn nitroaniline
NASA naphthylaminosulfonic acid
NaSS Na salt of styrene sulfonic acid
ND nanodiamond
NM natural minerals
NMP N–methylpyrrolidinone
NSA 2–naphthalenesulfonic acid
P pernigraniline
PA polyacetylene
PAA polyacrylic acid
PACC protective anticorrosive coating
PAn polyaniline
PAn–BF3 polyaniline doped by tetrafluorborate acid
PAn/CeFs polyaniline–cellulose fibers
PAn/SF polyaniline/silk fibroin composite fibers
PAr polyarenes
PAAr polyaminoarene
PAN polyacrylonitrile
PAPh polyaminophenols
PAT polyaminothiazole
PBMA polybuthylmethacrylate
Pd–NPs nanoparticles functionalized by palladium
PnB pernigraniline base
PnS pernigraniline salt
PEDOT poly–3,4–ethylenedioxythiophene
PES polyester
PET polyethylene terephtalate
PI polyimide
PLm polyluminol
PmAPh poly–m–aminophenol
xvi List of Abbreviations

PMA polymetacrylic acid

PMMA polymethyl methacrylate
PoAPh poly–o–aminophenol
PoA poly–o–anisidine
PoEA poly‒o‒ethoxyaniline
PoMA poly–o–methoxyaniline
PoT poly–o–toluidine
PT polythiophene
PPh polyphenylene
PpPh poly–p–phenylene
PpPhV poly–p–phenylene–vinylene
PP polypropylene
PPy polypyrrol
PS polystyrene
PSF polysulfone film
PSS poly(sodium styrenesulfonate)
PSSA polystyrenesulfonic acid
PSSMA copolymer of styrenesulfonate and maleic acid
PTFE poly(tetrafluoroethylene)
PU polyurethane
PVA polyvinyl alcohol
PVC polyvinylcarbazole
PVDF polyvinylidenefluoride
PVN polyvinylnaphthalene
REM rare-earth metals
RF radio frequency
Re electronic resistance
Ri ionic resistance
Rs resistance of electrolyte solution
SAW surface acoustic waves
SCE saturated calomel electrode
Si–Gl/PAn silica–glauconite/polyaniline composite
SPSF sulfonated polysulfones
SSA sulfosalicylic acid
StMA copolymer of styrene with maleic anhydride
TG integrated mass loss curves
TGA differential thermal gravimetric analysis
TMA thermal mechanical analysis
TSA toluene sulfonic acid
TMSPA N–(3–(trimethoxysylil)–propyl)aniline
List of Abbreviations xvii

p–TSA p–toluene sulfonic acid

τD diffusion time
UV ultraviolet (spectrum, spectroscopy)
WE working electrodes
XRD X-ray diffraction analysis
SUPPORTING INSTITUTIONS

• Department of Physical and Colloid Chemistry, Faculty of Chemistry

of the Ivan Franko National University of Lviv (Kyryla i Mefodiya
Str. 6, 79005 Lviv, Ukraine);
• Department of General Physics, Faculty of Physics of the Ivan Franko
National University of Lviv (Kyryla I Mefodiya Str. 8, 79005 Lviv,
Ukraine);
• Kinetics of Chemical and Biological Processes Department, Insti-
tute of Biochemical Physics named after N. N. Emanuel, Russian
Academy of Sciences (Kosygin Str. 4, 119991 Moscow, Russian
Ferderation);
• Department of Physical Chemistry, Faculty of Chemistry, University
of Gdańsk (J. Sobieskiego Str., 18, 80-952 Gdańsk, Poland);
• Kremenetskyi Regional Humanitarian Pedagogical Institute named
after Taras Shevchenkо (Lyceum Str. 1, 47003 Kremenets, Ternopil
region, Ukraine);
• Lviv Aсademy of Commerce (Samchuka Str. 9, 79011 Lviv, Ukraine);
• Department of Physical Chemistry of Fossil Fuels, Institute of
Physical–Organic Chemistry and Coal Chemistry named after L. M.
Lytvynenko, National Academy of Sciences of Ukraine (Naukova Str.
3a, 79053 Lviv, Ukraine);
• Department of Methodology of Teaching of Physics and Chemistry,
State Humanitarian University of Rivne (Stepan Bandera Str. 12,
33000 Rivne, Ukraine).
PREFACE

The main attention in this presented collection of the scientific papers is paid
to the recent theoretical and practical advances in conductive polymers and
nanocomposites. It also coveres the different branches of knowledge: from
the obtaining of nanoparticles with the use of new synthetic techniques to
application of the obtained nanomaterials and nanocomposites in different
fields of industry.
During the last two decades, conductive polymers were the object of
intensive research and development in the academic world and also in the
chemicals and electronics industry worldwide. In the 2003–2013 period
only, over 5000 articles and more than 35 chapters of books were dedicated
to the polyaniline and to the composites on its basis and were published
in the scientific journals of the American Chemical Society, Elsevier, and
John Wiley & Sons Publishing. However, the books dedicated solely to the
polyaniline and its composites are practically absent, which makes this Book
unique among the modern scientific books.
This book of scientific papers represents by itself the result of the perma-
systematical and methodical investigations and also scientific accumulations
of the scientific team of the Department of Physical and Colloid Chemistry
(Chemical Faculty) of Ivan Franko National University of Lviv in the field
of the synthesis, investigation of the properties and practical application of
the electroactive polymers and composites on their basis, which have been
performed within the scientific school “Physical chemistry of polymers”
initiated by Professor Eugen P. Koval’chuk over 25 years ago. Under his
guidance two theses for a Doctor’s as well as over 10 Ph.D. theses were
defended, and the results of the investigations were published in more than
200 articles in scientific journals. The research in this area are still continuing.
This book comprehends the questions both of the synthesis of polyani-
line by different methods, under different conditions, for various applica-
tions, and also the studies of its properties by a wide range of the modern
physical–chemical methods. The advantages of this book are comprehensive
analysis of experimental results from the point of view of the correlations in
the triad “Synthesis Conditions−Structure−Physical and Chemical Proper-
ties”. Some chapters contain the integrated results, which will be very valu-
able for the potential purchaser as a referenced data.
xxii Preface

The mechanism of the initial stages of oxidative polymerization of

aniline and its derivatives with the formation of conductive polymers with
the system of conjugated π-bonds are analyzed in Chapter 1. It is shown
that both during chemical and electrochemical polymerization the process is
initiated by the cation-radicals of the initial monomer, which then recombine
in accordance with the type “head to tail”. The obtained dimers represent by
themselves the structural units of the future polymeric chain, and then they
can take part in similar chain of the transformations. In the process of poly-
meric chain propagation, the molecules with varying polymerization degree
can participate, because their reactivity is determined by the presence of
the end amino-groups, and, therefore the oxidative polymerization is typical
polyaddition process. On example of nitro- and oxymethyl- derivatives it
was evaluated an impact and position of the substituent in the aromatic ring
on the reactivity of the aniline derivatives in the reaction of oxidative polym-
erization. On the basis of spectral studies and elemental analysis it was deter-
mined the most likely structures of the obtained polymeric anilines, including
the polyluminol. It was shown that in the case of polyanilines obtaining by
chemical method regardless of the nature of the initial monomer the final
product represents by itself a form of emeraldine salt.
Chapter 2 is dedicated to the research of the morphology of polyaniline’s
films electrochemically deposited on the surface of Al-based amorphous
metal alloys. The films of polyaniline have been synthesized by potentio-
dynamic oxidation of aniline at the electrodes of amorphous metal alloys of
the composition Al87Ni8(REM)5, where REM ≡ Y, Ce, Gd and Dy, as well
as polycristalline aluminum. The process of electrochemical oxidation of
aniline on amorphous metal alloys-electrodes was analyzed and compared
with the process of aniline’s oxidation on the polycrystalline Al-electrode. It
was established, that the difference in the form of cyclic voltammogramms
is conditioned by the presence of amorphic components in the amorphous
metal alloys composition, which cause of different resistance of surface
oxide films on the working electrodes. With the use of X-ray and IR-spec-
tral analysis it was showed, that the structure of polyaniline’s films on the
surface of the Al-electrode and the Al87Ni8(REM)5 electrodes is amorphous-
crystalline. At this, the polyaniline deposited on Al87Ni8(REM)5 electrodes
has a higher degree of crystallinity. An analysis of the images of scanning
electron microscopy showed, that on the surface of the working electrodes
of amorphous alloys Al87Ni8(REM)5 the polyaniline’s films have spongy and
porous branched morphology.
Polymers of polyvinyl series (namely, polyaminoarenes) are considered
as the perspective materials for electrochromic devices from the point of
Preface xxiii

view of physical chemistry of electrooptic phenomena in Chapter 3. The

main regularities of polyaminoarenes films formation on transparent semi-
conducting surfaces have been studied based on the results of electrochem-
ical, optical and spectroelectrochemical investigations. The relationship
between the electrochemical and also electrooptical characteristics and the
structure of polymers was established. On a basis of determined diffusion
coefficients and heterogeneous constants of a charge transport in different
electrolytic media it was shown, that the structure of a polymeric chain has
the decisive effect on the electrochromic material efficiency. Some possible
methods of electrochromic characteristics improvement for polyaniline and
its derivatives have been proposed.
The properties of Langmuir films of polyaniline and also its derivatives
(namely, poly-o-methoxyani-line, poly-o-toluidine), as well as compositions
of these polymers with polymethyl methacrylate and copolymer of styrene
and maleic anhydride have been investigated and described in Chapter 4.
Monomo-lecular Langmuir films were obtained on water surface by their
application both from the individual and from the mixed solutions of poly-
mers in organic solvents (tetrahydrofuran, chloroform). It is shown, that the
initial surface concentration of the substance and the nature of a solvent
used for the deposition of a monolayer has an impact on the magnitude of
the surface pressure of polyaniline monolayers. Dependence of the effective
area of monomer link (Seff.) on the composition of binary mixture has been
studied on a basis of isotherms of surface pressure of binary compositions. It
was discovered both of Seff. magnitude increasing and decreasing compared
to the total values of the areas for individual components. Such behavior
of Langmuir films can be conditioned due to the conformational changes
undergone by macromolecules into composite monolayers. During an inves-
tigation of monomolecular films under conditions of compression–expan-
sion it was determined that the polyanilines can form both equilibrium and
non-equilibrium monolayers. The polymer “memory” effect is developed
in a case when the monolayers of polyanilines are applied on water surface.
The mechanism of formation and physical chemical properties of epoxy-
polyanilines composites obtained using both the curing agent and also the
electroconductive filler of polyaniline doped by tetra-fluorborate acid has
been studied in Chapter 5. The factors having an impact on curing mecha-
nism and properties of composites were analyzed. It was shown that the
combination of properties both of curing agent and electroconductive
component into one complex polyaniline– tetrafluorborate acid gives the
possibility essentially to simplify the conductive epoxy polymer obtaining,
to receive the polymer–polymeric composites characterizing by electric
xxiv Preface

conductivity 10–6–10–4 S/cm at relatively low content of complex polyani-

line– tetrafluorborate acid; at the same time, such composites are character-
ized by high thermal and physical mechanical properties which makes it
possible to use them for producing of antistatic coatings, electroconductive
adhesives, electrodes, etc.
The temperature dependences of optical absorption (transmittance)
spectra of the conducting polymer films—polyaniline, poly-o-toluidine,
poly-o-anisidine, poly-o-aminophenol doped by sulfuric acid, potassium
ferricyanide and silver nanoparticles have been represented in Chapter 6. It
has shown that temperature increasing causes a change in optical transmit-
tance (absorption) spectra of polymers in all temperature range. However,
characteristics of thermo-optical changes or thermochromic effects depend
on polymer nature and doping conditions. Changes in parameters of the
optical spectra were connected with conformation of polymer chain and
modification of electron properties of conducting polymers under tempera-
ture action.
The basic aspects of the electroactive polymers using in general as well
as the polyaniline as classical representative of these polymers in partic-
ular under design of chemo- and biosensors are considered in Chapter 7.
On example of typical experimental and industrial samples it was analyzed
the architecture and performance properties of chemosensors by resistive,
amperometric, potentiometric, voltamametriс, optical and gravimetric types,
their advantages and disadvantages at the analysis of various inorganic and
organic substrates. It’s shown the prospects of application of nanostructured
polyaniline and composites on its basis with nano-dispersed metallic, oxide
and mineral fillers at the design of sensor devices. An application of poly-
aniline in biosensorics is considered in a separate way; in particular, the
methods of biological components immobilization on the polymer-modified
substrates have been analyzed.
The main aspects of aluminum and aluminum alloys protection by
corrosion coatings based on various forms of polyaniline were considered
in Chapter 8. The advantages and disadvantages of modern chemical and
electrochemical methods of application of polyaniline protective coatings
on aluminum-containing substrates were analyzed as well as the relation-
ship between the conditions of application of protective layers and their
protective properties was shown. The modern approaches to the use of poly-
aniline in protective corrosion coatings, such as doping by polymeric acids,
the formation of double-strand polyaniline complexes, the use of polyani-
line as the pigment filler in paint coating, as well as a major component of
Preface xxv

various polymer–polymer or polymer–inorganic hybrid composites were

considered. Proposed today mechanisms of protective action of protonated
and deprotonated forms of polyaniline were in detail analyzed concerning
to the corrosion of aluminum-containing substrates by forming of the
protective oxide or salt passivation layers, as well as the inhibition of redox
processes by polyaniline doping anions was considered. Special attention
has been paid into the negative role of the intermetallic surface inclusions
concerning to the initiation of corrosion and to the use of conversion cerium
coatings to eliminate of this problem.
The synthesis conditions and physico–chemical properties of conductive
composites of conjugated po-lyaminoarenes (polyaniline, polyorthotolu-
idine, polyorthomethoxy–aniline in polymer matrixes of polyme-thylmeth-
acrylate, polyvinyl alcohol, polybuthylmethacrylate, polyacrylic acid and
polymetacrylic acid are described in Chapter 9. It was found that the depen-
dence of specific conductivity on the conducting polymer content has a
percolation character with extremely low “threshold”. It was established a
connection between electrical, mechanical and thermomechanical proper-
ties of polymer–polymer composites studied. On the basis of study optical
changes in film composites under gas action the method of obtaining the
flexible color indicators for express control of ammonia content in gas envi-
ronment has been developed.
Chapter 10 is dedicated to the investigation and analysis of the sources
of the electrochemi-luminescence during the electrochemical synthesis of
polyaniline and copolymers of aniline and luminol by different composition
at high electrode potentials. It was proposed that the generation of low inten-
sity of luminosity in acidic aqueous solutions at the high electrode potentials
is related with irreversible destruction of the polyanilines in the form of
pernigraniline as a result of their interaction with free radical intermediates of
oxidation of solvent (water) and anions of the base electrolyte. It was shown,
that the obtained copolymers exhibit the electrochemiluminescent activity
in aqueous alkaline solutions. The feature of electrochemiluminescence of
copolymers is the presence of two waves of the appearance of luminosity;
that’s why it was suggested, that the source of the electrochemiluminescence
is a direct electrochemical oxidation (the first wave) and chemical oxidation
by free radicals of electrochemically generated intermediates (the so-called
second wave) of luminolic fragments of copolymeric chain.
The structure and physical chemical properties of the synthesized
polymer–inorganic composites by intercalation type based on polyaniline/
copolymers of aniline and nitroaniline with xerogel of vanadium pentaoxide
are described in Chapter 11. The electrical conductivity of synthesized
xxvi Preface

composites was studied and they were tested as cathode materials of lithium
chemical power sources. It was shown that the use of copolymers of aniline
with its nitro derivatives improves the electrical characteristics of lithium
chemical power sources based on hybrid polymer–xerogel composites by
introducing of the electroactive nitro groups into the structure of the polymer.
The subject of Chapter 12 is the modification of large-scale (films, sheets,
tapes, threads, fibers, etc.) non-conductive material-substrates of different
polymeric nature by polyaniline layer and also obtaining of homogeneous
polyaniline / polymeric composites. The methods of preparation of non-
conductive polymeric substrates, and also the basic techniques of applying
of the polyaniline layers or films on such substrates, namely the technique
from the solution in situ, from the gaseous phase, by polymerization method
in plasma, by forming of polyaniline’s films on the surface of polymeric
substrates from its solutions and suspensions, by preparation of polyaniline
/ polymeric composites using the methods of co-dissolving, by making of
melts as well as by combined methods are discussed. The basic stages of
the processes have been analyzed, the physico–chemical properties and
morphology of the obtained in each case composites were considered, the
examples of composite materials based on polyaniline and nonconducting
massive polymers of natural, artificial and synthetic origin are demonstrated.
It is shown that due to its physical and chemical properties such materials are
promising for applications as sensitive sensory materials, anticorrosive, anti-
static, electrostatic coating materials for shielding of electromagnetic waves,
elements of organic optoelectronic devices, diaphragms, artificial muscles,
electroconductive fabrics, biologically active substrates, etc.
One of the main tasks of modern physical and chemical investigations is
the development of scientific principles and new approaches to the creation
of polymeric and composite materials with given functional properties,
namely electrical, optical, magnetic, an ability to the charge storage and its
transfer, the catalysis of a number of reactions, sensorics and etc. The actual
problem of the science and technology at the present step is an investiga-
tion of the mechanism of formation and the development of new nanosized
composite materials based on polymers doped or filled by inorganic clusters,
in particular carbonic (graphene, fullerene, nanotubes), silicium (silicum
(IV) oxide, nanocrystals of silicon, porous silicon, silicum carbide) as well
as by the compounds of transition metals, in particular by ferrum-containing
ones, namely clusters of ferrum and its oxide, magnetite, the complexes of
ferrum and etc. Due to the nanostructures of such composites (the size of the
particles consists from some units to dozens nm) they have unique magnetic,
spectral and electrochemical properties. General scientific problem at the
Preface xxvii

development of high-dispersed and film composites of the polymers with

inorganic nanoparticles is understanding of the character of components
interaction. For this purpose, it is necessary to investigate the physical chem-
istry both of initial compounds and of the obtained composites; this gives
the possibility to control the parameters of the synthesized materials. This
knowledge can be obtained via the complex investigations of crystalline,
molecular, supramolecular, and electronic structure, the dispersion degree of
the particles, their distribution, determination of the relationship between the
structure and magnetic, electrical and optical properties of nanomaterials.
The investigations presented in Chapter 13 are dedicated to the solution of
the above-said tasks.
In recent decades, researchers actively developed the various hybrid
mineral–polymeric composites, among which special attention is given to
the materials based on polyaniline and natural minerals, which combine the
properties both of the polymer and natural minerals showing the synergism
effect. Сombination of properties of the polyaniline and inorganic substances
of micro-, and especially of nanosized dispersion degree leads to the forma-
tion of composites with physical and chemical properties that are much better
compared to individual properties both of polymer and inorganic mineral. In
many cases the thermal stability of polyaniline into obtained composites is
increased, and the composites acquire electromagnetic, magnetic, catalytic,
adsorptive and other properties. Chapter 14 is dedicated to the investiga-
tions of the structure and thermal stability of silica-glauconite / polyaniline
composite.
The results of the unique experimental investigations and original
methodology of the description of physical–chemical and electrochem-
ical phenomena at the interface surfaces are organically combined in the
presented book. It is shown an influence of such phenomena on the applied
aspects of the polyaniline and nanocomposites on its basis applications. The
last fact advantageously distinguishes the presented book of the scientific
papers among existent range of the works dedicated to such subject matter
at the present time.
This book will be useful first of all for scientists and post-graduate
students who are engaged in physical chemistry of conductive polymers in
the whole and polyaniline particularly. It will be helpful also for profes-
sors teaching courses dedicated to the materials science, chemistry of
high-molecular compounds, physical–chemical properties of conductive
polymers and its applications in electronics, power sources, sensors, anticor-
rosive coatings, etc.
xxviii Preface

This presented work has been performed under the partial financial
support of the scientific grants of the Ministry of Education and Science
of Ukraine (state registration numbers 0112U001283, 0112U001294,
0112U001295, 0113U003055, 0115U003262 and 0115U003263).
—Olexandr Reshetnyak
Lviv, July 2016
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Aug
7137 Sloan J M Cav 18 D
28
113 Aug
7141 Springer J
F 29
Aug
7262 Shriver B Cav 18 K
30
Aug
7302 Singer J Art 2A
30
Aug
7358 Scoleton J 53 F
31
Aug
7363 Sweeney D Cav 14 E
31
Aug
7379 Scott W B “ 4D
31
Sept
7631 Streetman J 7E
2
62 Sept
7638 Steele J
M 2
Sept
7648 Spencer Geo 20 C
3
183 Sept
7662 Snyder M S
A 3
Sept
7705 Swartz Geo Cav 5A
3
Stockhouse D, Sept
7770 “ 18 I
Cor 4
149 Sept
7905 Sellers H
G 5
Sept
7939 Shultz Jno Cav 4 I
5
7960 Smith A C 7F Sept