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The Physics of Polymer Interactions: a New Approach.
Application to Rheology and Processing
by Jean Pierre Ibar
8 Chapters, 431 pages, 182 Figs, HANSER (published October 2019 ISBN: 978-1-56990-710-8)
E-book ISBN: 978-1-56990-711-5
REVIEW of the book by Dr. T.J. Hutley, PhD, MBA, June 2022
THE PHYSICS OF POLYMER INTERACTIONS
A NOVEL APPROACH. APPLICATION TO RHEOLOGY AND PROCESSING
Jean Pierre IBAR
2019, HANSER ISBN 978-1-56990-710-8
This book is not for the faint-hearted. It is both a complex, difficult read, and yet at the
same time, exciting - brimming over with new concepts and ideas, almost mind-bending !
Both industrial polymer scientists and academics will find this a text that requires intense
concentration, continued focus, great and careful attention to detail, along with plenty of
imagination. But for the determined reader, a new vista is available.
The contents and core concepts of this book have been under consideration and
development by the author Prof Dr Jean Pierre IBAR for almost 50 years (since 1973).
This book provides an answer to the question that he posed 25 years ago:
“Do We Need a New Theory in Polymer Physics?” (1)
This 430-page book is the first in an expected set of volumes on what Dr Ibar calls
“New School Polymer Physics”, which will describe qualitatively, quantitatively and
practically the new approach (paradigm) to polymer physics introduced here in this
volume, which is only concerned with (already the vast field of) polymer viscoelasticity.
Other topics that may also be upturned by this ‘new school of polymer physics’ will
include polymer crystallisation (which we will see in a future volume “Dual-phase
crystallisation”).
This book consists of several interwoven threads. In one sense, it is the history of the life
and thinking of the author, which has been focussed on the impact of vibration on
polymer melts. In another sense, it is the explanation of how his experimental work in
polymer physics, and his own careful and detailed analysis of the work of others, has
highlighted the limitations of classical polymer physics theories, and his development of a
new theory that fits all the experimental data. A further thread of this book is the practical
implementation - as an entrepreneur and polymer engineer - of his knowledge of how
vibration can interact with polymer melts and affect their rheology, behaviour and
properties. A final thread is that this book is a compilation of articles previously published
in the Journal of Macromolecular Science 2009-2015 on this topic.
The focus of this book is on disentangling polymer chains in the melt. This itself is a true
paradigm shift.
Dr Ibar explains how the mutual entanglement of polymer molecules in
the melt state can be controlled, and substantially kinetically altered, by temperature,
shear and vibration. He hints at how this is actually done practically (and which will be the
subject of another related volume); and how these disentangled, lower viscosity polymer
melts behave, such as processing at temperatures 50 - 100°C below their normal level.
Furthermore, he explains that this disentangled state - which is actually a new state for
industrial polymer melts - can be maintained in the extruded pellets (we can think ‘frozen-
in disentanglement’), such that their viscosity during subsequent processing - typically
injection moulding - is significantly lower.
These ideas are already implemented in the polymer industry, albeit somewhat covertly.
So what Dr Ibar is talking about in this book is not just an idea or a theory, but of an
implemented innovative technology. This book chiefly explores how his new model of
polymer physics and rheology can explain, and help us understand, this disentanglement
process (which he names “rheo-fluidification”).
Those readers involved with polymer materials will understand that polymer processing is
essentially "man's struggle to make incredibly viscous materials flow in to the desired
shape" [Reviewer’s definition]. The typical high viscosity of these industrial polymers is
because above a critical molecular weight Mc (typically 4-10 kg/mole), the melt viscosity is
no longer proportional to the molecular weight, but abruptly becomes proportional to the
3.4th power of the molecular weight weight η ∝ M3.4. So, in order to process these
viscous polymer melts, machines with huge electric motors (extruders) or massive
hydraulic pressure plants (injection moulding machines), both of which operate at high
temperatures, have been developed. This changes completely (a paradigm shift) if we
can disentangle the polymer melts, and enjoy a significantly lower melt viscosity.
The new model: in essence, what Dr Ibar has done is to change the way we scrutinise
polymer molecules: instead of looking at a single polymer molecule in a tube and how it
is influenced by its environment (the Reptation model), he considers a more “system”
approach, looking at the entire population of polymer molecules: how the conformers
(3-bond / 4-atom segments) of all the polymer molecules are categorised by their
conformation (c, g, t - cis, trans, gauche) and the amount of intermolecular coupling
(b, intermolecularly bonded, or F, free from intermolecular bonding). This he calls the
dual-phase. Above the critical molecular weight for entanglement, his model shows that
two co-existing and interactive populations are formed, described as the cross-dual-
phase. Best described qualitatively as the entanglement network (phase) and core phase,
respectively, and shown in summary, mathematically, by:
[b/F <—> (c, g, t)]1 ⇌ [b/F <—> (c, g, t)]2
Note that the detailed mathematical and statistical treatment of this model will be
provided in a further volume “The Grain Field Statistics of Polymer Interactions”,
and is not covered in this book).
With this new cross dual phase model, Dr Ibar is able to explain the physics of polymer
molecules, and particularly their rheology, and entanglement and disentanglement
behaviours.
Within this new model, we also see some very different perspectives on free volume.
Free volume arises from the F (free from bonding) conformers, and is no longer seen as a
function of two independent variables, Temperature and Molecular Weight. Almost
hidden away, passed over in a sentence or two, the author explains that when we
consider constant free volume, the classical exponent of molecular weight determining
melt viscosity of 3.4 becomes 5.3. That alone is a step-change in understanding!
In the book itself, six pages of Preface provide a historical perspective, and an overview of
the new theory of polymer physics. This is followed by 9 pages of Chapter Abstracts,
which enable the reader to get an overview and broad perspective of the book. The
book proper consists of eight chapters, of very unequal length: chapter 4 at 163 pages,
Chapter 5 is 125 pages, whereas Chapter 2 is just 9 pages, chapter 7 just 10 pages. What
is helpful, bearing in mind how complex this topic is, and how many new ideas are being
introduced, is that almost every Chapter has a summary and conclusions section. Some
are short, some are long (in Chapter 6 it is 1 page, in chapter 5 it is 17 pages). What the
reader might find troubling is that new ideas and concepts are sometimes introduced in
these summaries ! The final Chapter 8 is a Summary of the previous Chapters.
In Appendix A - which might have been developed further, as it is just 1 page - is a list of
potential applications of the rheo-fluidification technology.
The broader and more extensive industrial implementation of disentanglement
technology might be hindered by the complete paradigm shift introduced here. It
requires a re-boot of the thinking of polymer engineering and the design of polymer
processing equipment, which have all developed based upon an earlier rigid paradigm
that polymers are necessarily high viscosity fluids.
The reviewer believes that achieving disentangled polymer melts is a new disruptive
technology that could reconfigure the polymer industry value chain, and bring brand new
economic and environmental (lower energy consumption) benefits. Bold engineers who
can imagine the potential of what is described in this book will be on a path, along which
few have travelled.....
References
(1) Ibar, J.P., Do we need a new theory in polymer physics? J. Macromol. Sci., Polym. Rev. (1997) 37, pp. 389–458
Dr Trevor J. Hutley MBA
Global Polymer Industry Consultant
Arrabon Technologies Limited
Hapton NR15 1AD, Norfolk UK
TrevorHutley@consultant.com
m: +44 789 501 2902
www.linkedin.com/in/trevorhutley
www.pcn.org/Hutley.htm
version 1.7 @ 16 June 2022
BOOK ABSTRACT
Understanding of polymer interactions is important for effective processing of plastics and their blends, mixing with nanoparticles, and understanding of their mechanical and physical (e.g., electrical) properties. This book describes a new physics of interactions in polymers that challenges existing theories, and explains the concept of entanglement in a very different way.
Rheology is formulated with different parameters defining the physics of Dual-Phase and Cross-Dual-Phase. The rubbery behavior of thermoplastics is explained quite differently to conventional theory.
Rheo-fluidification experiments ("disentanglement smart processing" ) which are applicable to industry (injection molding, extrusion, sheet forming, etc.) are described and analyzed, including molding under conditions of reduced viscosity (up to several hundred percent). The application of this theory to industry has already been proven by a number of successful derived inventions.
The physics of Dual-Phase and Cross-Dual-Phase (which can also be formulated to simulate crystallization from the molten state) is dedicated in this book to the description of the flow properties of melts under linear and far from linear conditions, not only for the case of classical experiments performed to determine the viscosity and the elasticity of polymeric melts (linear rheology) but also for the fast rate melt deformation encountered in industrial processes. It is suggested in this work that the classical concepts of rheology (relaxation time, Me, GoN, Newtonian viscosity) may be useful parameters at low rates only, becoming deficient and responsible for the difficulty to describe non-linear effects (shear-thinning, strain softening, swelling) as the strain rate or the strain increases to the level of the industrial needs.
Table of Content
Preface : 40 YEARS OF PAINTING ON THE SAME CANVAS.
Chapter 1: PREAMBLE:INTRODUCTION TO THE DUAL-PHASE MODEL OF POLYMER INTERACTIONS AND TO THE CROSS-DUAL-PHASE MODEL OF ENTANGLEMENTS.
Chapter 2: TROUBLE WITH POLYMER PHYSICS: “SUSTAINED-ORIENTATION”
Chapter 3: THE GREAT MYTHS OF POLYMER RHEOLOGY, PART 1: COMPARING THEORY WITH EXPERIMENTAL DATA.
Chapter 4: THE GREAT MYTHS OF POLYMER RHEOLOGY, PART 2: TRANSIENT AND STEADY STATE. STABILITY OF THE NETWORK OF ENTANGLEMENT
Chapter 5: THE GREAT MYTHS OF POLYMER RHEOLOGY, PART 3: ELASTICITY OF THE NETWORK OF ENTANGLEMENTS
Chapter 6: THE ELASTIC DISSIPATIVE STATE OF POLYMERIC MELTS. SOLID-LIKE BEHAVIOR IN THE MOLTEN STATE
Chapter 7: SHEAR-THINNING OF POLYMERIC MELTS: THE FAILURE OF THE REPTATION MODEL
Chapter 8: ENTANGLEMENTS: A NEW INTERPRETATION AND ITS PERSPECTIVES IN SCIENCE AND TECHNOLOGY
ABOUT THE AUTHOR
Prof. Dr. J.P. Ibar, educated at ENSCP and MIT, has spent his entire career studying, characterizing
and processing the amorphous state of matter, both at an academic level (Professor of the Universities) and through 3 start-ups that he co-founded and directed as Director of Research. He is the
recipient of numerous awards (Chaudron’s medal, Fulbright, Sigma-Xi Society (MIT Chapter), Marie-
Curie, Ikerbasque Fellowship etc.), has been granted over 300 patents worldwide (35 seminal ones)
and has authored more than 15 hundred peer-reviewed papers and 3 books. He has lectured as a
keynote speaker at numerous international conferences (APS, ACS, ANTEC, Gordon Conferences, ICR,
SOR, SER, PPS, Cambridge University, Russian Academy of Science, Sichuan University, etc.). He is
currently writing a series of books on the Duality and Cross-Duality of the interactions in polymer
science and engineering, and, more generally, to describe the physics of dissipative systems.
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