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Full download Electrocatalysis for Membrane Fuel Cells: Methods, Modeling, and Applications Nicolas Alonso-Vante file pdf all chapter on 2024
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Electrocatalysis for Membrane Fuel Cells
Electrocatalysis for Membrane Fuel Cells
Contents
Preface xv
3 Electrochemical Fundamentals 71
Vito Di Noto, Gioele Pagot, Keti Vezzù, Enrico Negro, and Paolo Sgarbossa
3.1 Principles of Electrochemistry 71
3.2 The Role of the First Faraday Law 71
3.3 Electric Double Layer and the Formation of a Potential Difference at the
Interface 73
3.4 The Cell 74
3.5 The Spontaneous Processes and the Nernst Equation 75
3.6 Representation of an Electrochemical Cell and the Nernst
Equation 77
3.7 The Electrochemical Series 79
3.8 Dependence of the Ecell on Temperature and Pressure 82
3.9 Thermodynamic Efficiencies 83
3.10 Case Study – The Impact of Thermodynamics on the Corrosion of Low-T
FC Electrodes 85
3.11 Reaction Kinetics and Fuel Cells 88
3.11.1 Correlation Between Current and Reaction Kinetics 88
3.11.2 The Concept of Exchange Current 89
3.12 Charge Transfer Theory Based on Distribution of Energy States 89
3.12.1 The Butler–Volmer Equation 96
3.12.2 The Tafel Equation 100
3.12.3 Interplay Between Exchange Current and Electrocatalyst Activity 101
3.13 Conclusions 103
Acronyms 104
Symbols 104
References 107
15.3.3.5
. Supervisory Control 531
15.4 Fuel Cell Powertrains for Mobility Use 532
15.4.1 Transport Application Scenarios 532
15.4.2 Tools for the Codesign of Transport Fuel Cell Systems and Energy
Management Strategies 534
15.4.2.1 Automotive Case Study: Optimal Codesign of an LDV FCHV
Powertrain 535
Acronyms 540
Symbols 541
References 541
Index 545
xv
Preface
as supports. Moreover, in Chapter 5, the author discusses some means for protecting
catalytic sites in order to maintain high performance in the light of recent data
from the literature. Chapter 6, furthermore, puts into relevance the state-of-the-art
of platinum group metal (PGM)-free ORR catalysts. Herein, the authors provide
an overview of important parameters that influence the catalysis of ORR with
well-defined ORR catalysts. In Chapter 7, recent development in electrocatalysts
for the hydrogen oxidation reaction (HOR) is put on the floor, emphasizing the
state-of-the-art PGM- and non-PGM-based electrocatalysts for the HOR in alkaline
conditions. An important ingredient in the proton exchange membrane fuel cell
(PEMFC) system is the polymeric electrolyte. In this context, Chapter 8 describes the
features that a membrane must exhibit to be implemented in a fuel cell. This chapter
ends with a comprehensive overview of the mechanisms of ion conduction proposed
for fuel cell membranes, followed by a brief summary outlining the perspectives
of the research in this field. The characteristics of ORR electrocatalyst support
(carbon-based and oxide-based) have been analyzed in Chapter 9. Of importance, in
all interface research, is the in operando technique, and/or probing under real fuel
cell operating conditions is offered in Chapter 10 with the use of X-ray absorption
spectroscopy (XAS). Theoretical modeling and computation to unravel the local
reaction environment are given in Chapter 11. This chapter addresses this complex
issue by introducing some basic concepts of electrochemical interfaces, especially
the surface charging relation. The authors highlight the electrocatalytic interfaces
pertaining to the role of chemisorption-induced surface dipoles that could cause
nonmonotonicity in the surface charging behavior. The electrocatalytic materials
research protocols for investigating fuel cell reactions are deployed in Chapters 12
and 13. In sum, the correct evaluation of fuel cell reactions, selection of reference
electrodes, durability tests of PGM-free materials, and fuel cell testing procedures
are put forward in the light of the most advanced literature data research. The
last section of the book presents Chapters 14 and 15. These chapters analyze the
fundamentals of fuel cell simulation by means of a mono-dimensional analytical
model considering multiphase water transport affecting the electrical conductivity
properties of the cell membrane, whereas Chapter 15 analyzes the optimization of
the operative conditions and the prediction of the system durability that back the
design of the PEMFC stack and components of the balance of the plant.
The editors appreciate the contributing authors of this book, who maintained high
scientific standards.
N. Alonso-Vante acknowledges financial support from the European Union
(ERDF) and “Région Nouvelle Aquitaine.”
V. Di Noto thanks the financial support of EIT Raw Materials, project Alpe, and
Graphene Flagship, Core 3, of the European Union.
Nicolas Alonso-Vante
University of Poitiers, IC2MP-UMR CNRS 7285
Poitiers, France
Vito Di Noto
University of Padova, Department of Industrial Engineering
Padova, Italy
1
Part I
Overview of Systems
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necessary to cover it with some well-warmed and non-conducting
material and to have the room well warmed. If bed-sores are already
formed, they are to be treated according to ordinary surgical
principles. Antiseptic means should be in the foreground in the case
of the malignant bed-sore. It is to be remembered that the latter is a
gangrenous process, and, in so far as the formation of a line of
demarcation between the necrotic and the conserved tissue is
concerned, the ordinary expectant rules of surgery govern the case:
the water-bath appears to yield the best results. Ordinary bed-sores
yield readily to mechanical protection and stimulating ointments or
the balsam of Peru. Iodoform is recommended, but it produces
granulations of an indolent character as compared with those
obtained through the use of resinous ointments.
BY E. C. SPITZKA, M.D.
As the symptoms of the regular affections of the cord are by far the
most readily recognizable, and a preliminary knowledge of them will
facilitate the better understanding of the irregular forms, we shall
consider the former first. They may be subdivided into two groups.
The largest, longest known, and best studied consists of acquired,
the other, containing less numerous cases and varieties, and
rendered familiar to the profession only within the last decade,
comprises the spinal disorders due to defective development of the
cerebro-spinal and spinal-fibro systems.
Tabes Dorsalis.
While some patients escape these pains almost entirely,2 others are
tormented with them at intervals for years, their intensity usually
diminishing when the ataxic period is reached. There is little question
among those who have watched patients in this condition that their
pains are probably the most agonizing which the human frame is
ever compelled to endure. That some of the greatest sufferers
survive their martyrdom appears almost miraculous to themselves.
Thus, in one case the patient, who had experienced initial symptoms
for a year, woke up at night with a fulminating pain in the heels which
recurred with the intensity of a hot spear-thrust and the rapidity of a
flash every seven minutes; then it jumped to other spots, none of
which seemed larger than a pin's head, till the patient, driven to the
verge of despair and utterly beside himself with agony, was in one
continued convulsion of pain, and repeatedly—against his conviction
—felt for the heated needles that were piercing him. In another case
the patient, with the pathetic picturesqueness of invalid misery,
compared his fulminating pains to strokes of lightning, “but not,” he
added, “as they used to appear, like lightning out of a clear sky, but
with the background of a general electrical storm flashing and
playing through the limbs.”
2 I have at present under observation two intelligent patients (one of whom had been
hypochondriacally observant of himself for years) who experienced not a single pain,
as far as they could remember, and who have developed none while under
observation. Seguin mentioned a case at a meeting of the Neurological Society with a
record of but a single paroxysm of the fulgurating variety. Bramwell (Brit. Med. Journ.,
Jan. 2, 1886) relates another in which the pains were entirely absent.
Either while the pains are first noticed or somewhat later other signs
of disturbed sensation are noted. Certain parts of the extremities feel
numb or are the site of perverted feelings. The soles of the feet, the
extremities of the toes, the region about the knee-pan, and the
peroneal distribution, and, more rarely, the perineum and gluteal
region, are the localities usually affected.3 In a considerable
percentage of cases the numbness and tingling are noted in the little
finger and the ulnar side of the ring finger; that is, in the digital
distribution of the ulnar nerve. The early appearance of this symptom
indicates an early involvement of the cord at a high level. Some
parallelism is usually observable between the distribution of the
lightning-like pains when present and the anæsthesia and
paræsthesia if they follow them. With these signs there is almost
invariably found a form of illusive sensation known as the belt
sensation. The patient feels as if a tight band were drawn around his
body or as if a pressure were exerted on it at a definite point. This
sensation is found in various situations, according as the level of the
diseased part of the cord be a low or high one. Thus, when the lower
limbs are exclusively affected or nearly so the belt will be in the
hypogastric or umbilical region; if the upper limbs be much involved,
in the thoracic region; and if occipital pain, anæsthesia of the
trigeminus, and laryngeal crises are present, it may even be in the
neck. Correspondingly, it is found in the history of one and the same
patient: if there be a marked ascent—that is, a successive
involvement of higher levels in the cord—the belt will move up with
the progressing disease. This occurrence, however, is less
frequently witnessed than described. In the majority of cases of
tabes disturbances of the bladder function occur very early in the
disease. Hammond indeed claims that in the shape of incontinence it
may be the only prodromal symptom for a long period.4
3 In the exceptional cases where the initial sensory disturbance is marked in the
perineal and scrotal region I have found that the antecedent fulminating pains had
been attributed to the penis, rectum, and anal region; and in one case the subjective
sense of a large body being forcibly pressed through the rectum was a marked early
sign.
7 Not even the absence of the knee-jerk ranks as high as these two signs. Aside from
the fact that this is a negative symptom, it is not even a constant feature in advanced
tabes.
8 It does not seem as if the disturbance of static equilibrium were due merely to the
removal of the guide afforded by the eyes, for it is noted not alone in patients who are
able to carry out the average amount of locomotion in the dark, but also in those who
have complete amaurosis. Leyden (loc. cit., p. 334) and Westphal (Archiv für
Psychiatrie, xv. p. 733) describe such cases. The act of shutting the eyes alone,
whether through a psychical or some occult automatic influence, seems to be the
main factor.
In most cases of early tabes it is found that the pupil does not
respond to light; it may be contracted or dilated, but it does not
become wider in the dark nor narrower under the influence of light.
At the same time, it does contract under the influence of the
accommodative as well as the converging efforts controlled by the
third pair, and in these respects acts like the normal pupil. It is
paralyzed only in one sense—namely, in regard to the reflex to light;
just as the muscles which extend the leg upon the thigh may be as
powerful as in health, but fail to contract in response to the reflex
stimulus applied when the ligamentum patellæ is struck. For this
reason it is termed reflex iridoplegia.9 It is, when once established,
the most permanent and unvarying evidence of the disease, and is
of great differential diagnostic value, because it is found in
comparatively few other conditions.
9 It is also known as the Argyll-Robertson pupil. Most of the important symptoms of
tabes are known by the names of their discoverers and interpreters. Thus, the
swaying with the eyes closed is the Romberg or Brach-Romberg symptom; the
absence of the knee-phenomenon, Westphal's or the Westphal-Erb symptom; and the
arthropathies are collectively spoken of as Charcot's joint disease.
18 Loc. cit.
While the symptoms thus far considered as marking the origin and
progress of tabes dorsalis are more or less constant, and although
some of them show remarkable remissions and exacerbations, yet
may in their entity be regarded as a continuous condition slowly and
surely increasing in severity, there are others which constitute
episodes of the disease, appearing only to disappear after a brief
duration varying from a few hours to a few days: they have been
termed the crises of tabes dorsalis. These crises consist in
disturbances of the functions of one or several viscera, and are
undoubtedly due to an error in innervation provoked by the
progressing affection of the spinal marrow and oblongata. The most
frequent and important are the gastric crises. In the midst of
apparent somatic health, without any assignable cause, the patient is
seized with a terrible distress in the epigastric region, accompanied
by pain which may rival in severity the fulgurating pains of another
phase of the disease, and by uncontrollable vomiting. Usually, these
symptoms are accompanied by disturbances of some other of the
organs under the influence of the pneumogastric and sympathetic
nerves. The heart is agitated by violent palpitations, a cold sweat
breaks out, and a vertigo may accompany it, which, but for the fact
that it is not relieved by the vomiting and from its other associations,
might mislead the physician into regarding it as a reflex symptom. In
other cases the symptoms of disturbed cardiac innervation or those
of respiration are in the foreground, constituting respectively the
cardiac and bronchial crises. Laryngeal crises are marked by a
tickling and strangling sensation in the throat, and in their severer
form, which is associated with spasm of the glottis, a crowing cough
is added.22 Enteric crises, which sometimes coexist with gastric
crises, at others follow them, and occasionally occur independently,
consist in sudden diarrhœal movements, with or without pain, and
may continue for several days. Renal or nephritic crises are
described23 as resembling an attack of renal colic. The sudden