Catalysts for Alcohol-Fuelled Direct Oxidation Fuel Cells: RSC (Energy and Environment Series)

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Energy and environment issues are of paramount importance to achieve the sustainable development of our society. Alcohol-fuelled direct oxidation fuel cells (DOFCs), as a clean and highly-efficient energy harvesting engine, have attracted intensive research activity over recent decades. Electrocatalysts are the material at the very heart of the cell that determines the performance of DOFCs. The rapid advances in electrocatalysts, particularly nano-sized ones, have left current information only available in scattered journals. To be truly useful to both present and future researchers, a new book is needed to present an insightful review of the reaction nature of this research and to systematically summarize recent advances in nanocatalysts, and convey a more global perspective. Catalysts for Alcohol-fuelled Direct Oxidation Fuel Cells will present a state-of-the-art review on recent advances in nanocatalysts and electrocatalysis in DOFCs, including both proton and hydroxide ion exchange membrane fuel cells. The main topics covered include a molecular-level understanding of electrocatalysis, the design principles of electrocatalysts, recent advances in nanocatalysts and future perspectives for DOFCs. The book presents a cutting-edge collection on nanocatalysts for alcohol-fuelled direct oxidation fuel cells and brings together the most authoritative researchers in the field from both industry and academia, filling the gap between both sides. Finally, the book will provide an insightful review on electrocatalysis at the molecular- level, which will be useful for postgraduate students and junior researchers in this field. It will be an essential resource for postgraduates, researchers and policy-makers globally in academia, industry, and government institutions.

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About the Author:

As a full professor of Mechanical Engineering and director of the Center for Sustainable Energy Technology at The Hong Kong University of Science and Technology (HKUST), Tim S. Zhao has been working on fuel cells for more than a decade. Zhen-Xiang Liang is full professor at the School of Chemistry and Chemical Engineering, South China University of Technlogy, Guangzhou, China. He has been working on direct alcohol fuel cells for almost a decade and has a proven track record in electrochemistry, particularly in the area of electrocatalyst developments.

Review:

“Catalysts for Alcohol-Fuelled Direct Oxidation Fuel
Cells” is aimed at a general audience with an interest
in low power fuel cells, as well as experts in the area.
The book is edited by Zhen-Xing Liang, Lecturer at
the South China University of Technology, and Tim
S. Zhao, Professor of Mechanical Engineering at the
Hong Kong University of Science and Technology
(HKUST) and director of the HKUST Energy Institute.
The book contains seven chapters in 264 pages and
reviews the catalysis of alcohol electrooxidation
in low-temperature fuel cells. The reader will fi nd
a general overview of the catalysis involved in the
oxidation of alcohols such as methanol and ethanol.
More unusually the oxidation of ethylene glycol and
glycerol are also described in detail. Although the
title for this book is specifi c to alcohol fuel cells it
also contains individual chapters describing the
oxidation of other fuels of interest such as formic acid,
borohydride and sugars. The book concludes with a
chapter on the challenges that alcohol fuel cells need
to overcome.
Role of the Platinum Group Metals
Many of the book’s chapters are easy to read even for
people with little experience in the area. Chapter 1,
‘Electrocatalysis of Alcohol Oxidation Reactions at
Platinum Group Metals’, by Claude Lamy (University
of Montpellier, France) and Christophe Coutanceau
(Université de Poitiers, France), starts with a good if
simplistic overview about what constitutes fuel cell
effi ciency. This is an important subject and the authors’
general description can easily be followed by students
in chemistry or related subjects. The authors highlight
that the theoretical effi ciencies for methanol/air
and ethanol/air fuel cells are actually higher than
hydrogen/oxygen fuel cells. This is a great foundation
for the book because it really justifi es the need for
research in this area. The chapter continues with a
very simplistic description of the methods used for
the synthesis and characterisation of fuel cell catalysts,
from well-known chemical and electrochemical
approaches to more exotic methods such as plasmaenhanced
techniques. The content fl ows in a logical
order with this introduction followed by dedicated
sections describing in detail the oxidation of different
fuels. The oxidation of methanol or ethanol is
described in acidic environments, mainly for the wellknown
platinum-based binary catalysts PtM/C (M =
ruthenium or tin), at different atomic ratios.
The authors describe the differences in reactivity
when using different atomic ratios such as Pt0.5Ru0.5,
Pt0.8Ru0.2, Pt3Sn and Pt9Sn. These binaries are known
to be active because of the effi cient removal of
adsorbed carbon monoxide (via the bifunctional
mechanism), a common intermediate in the oxidation
of primary alcohols. In contrast, the oxidation of
ethylene glycol and glycerol is described mainly in
alkaline media with the authors focusing on the use
of carbon supported platinum, platinum-palladium
and platinum-palladium-bismuth for the oxidation
of ethylene glycol and platinum, palladium and gold
catalysts and their binaries and ternaries such as
PtPd, PtBi, PdBi and PtPdBi for the oxidation of glycerol.
The chapter offers a good introduction, although it
lacks references to the use of commercial catalysts for
methanol oxidation (1, 2).
Catalyst Preparation
Chapter 2, ‘Nanoalloy Electrocatalysts for Alcohol
Oxidation Reactions’, by Jun Yin (Cornell University,
New York, USA) et al. describes the use of PtAu
catalysts for alcohol oxidation. The synthesis of PtAu
catalysts is a very interesting topic with challenging
nanoscale catalyst preparation. Nanoscale gold has
been shown to produce surface oxygenated species
such as gold(III) oxide, adsorbed gold hydroxide or
gold(III) hydroxide which are highly active for the
M1
M2
Precursors
Capping
agent
Reduction or
decomposition
Wet chemical
synthesis
Assembly
on support
Thermal
treatment
Supported
catalyst
Assembly
Activation
(a)
(b)
30 nm
(c)
30 nm
M1mM2100–m
+
Fig. 1. (a) A general scheme showing the molecularly engineered synthesis of bimetallic nanoparticles capped
with a monolayer shell of oleic acid/oleylamine and the preparation of bimetallic nanoparticles supported on
carbon powders or carbon nanotubes by assembly and activation. Transmission electron microscopy images
showing: (b) Au22Pt78 nanoparticles supported on carbon black; and (c) Au nanoparticles supported on carbon
nanotubes (Reproduced by permission of The Royal Society of Chemistry)
removal of adsorbed CO, especially in alkaline media.
Traditional methods for PtAu catalyst preparation are
mentioned such as co-precipitation, impregnation
with subsequent reduction, and calcination. More
interestingly, the synthesis of Au and PtAu supported
nanoparticles via the molecular encapsulation
synthesis is described (Figure 1). This approach
involves three steps: (a) chemical synthesis of metal
nanocrystal cores with molecular encapsulation;
(b) assembly of the encapsulated nanoparticles
on support materials; and (c) thermal treatment
of the supported nanoparticles. A brief mention of
core–shell type PtAu nanoparticles is also included
although no characterisation data is shown. PtAu
nanoparticles with different atomic compositions are
presented for the oxidation of methanol in alkaline
and acidic media. An iron(II,III) oxide Fe3O4@Au@Pt
ternary is presented as a more active catalyst than Pt
in acidic media. The chapter fi nishes with a section
dedicated to the characterisation of PtAu particles and
includes experimental data from different techniques
such as X-ray diffraction (XRD), Fourier transform
infrared (FTIR) spectroscopy and X-ray photoelectron
spectroscopy (XPS) which adds detailed information
to help understand the catalysis.
Quantum Mechanical Modelling
Chapter 3, ‘Theoretical Studies of Formic Acid
Oxidation’, by Wang Gao and Timo Jacob (Universität
Ulm, Germany), is the only chapter dedicated to
the use of quantum mechanical modelling for the
understanding of chemical reactions at the molecular
level. Although formic acid is not an alcohol, it is of
interest in terms of fuel cell effi ciency for low power
electronics. The authors cover the oxidation of formic
acid in ultra-high vacuum conditions and also with
increasing water coverage. Importantly, they pay
attention to the effect of the electrochemical potential
on the formic acid dehydrogenation and include a
detailed discussion of the adsorbed products that
are formed. A detailed and informative discussion of
the different reaction pathways, direct and indirect, is
presented. Readers with some experience in the fi eld
will fi nd the content extremely interesting. It is slightly
disappointing that the editors did not include more
content towards the use of theoretical modelling for
the oxidation of alcohols.
Catalysis by Gold
Chapter 4, ‘Gold Leaf Based Electrocatalysts’, by
Rongyue Wang and Yi Ding (Shandong University,
China) is dedicated to the use of nanoporous gold leaf
(NPG-leaf) as an alternative catalyst for the oxidation
of formic acid and alcohols in alkaline media. The
chapter describes the formation of NPG by chemical
dissolution also known as dealloying. This is a wellknown
process and has been applied for many years
in the manufacturing of high surface area catalysts.
The authors present as an example the formation of
NPG from a gold-silver alloy. Selective dissolution of Ag
leads to the formation of a porous structure (Figure 2)
(3). The authors describe the excellent research done
by John Newman (University of California, Berkeley,
USA) et al. (4) and Jonah Erlebacher (Johns Hopkins
University, USA) et al. (5) and the reader is advised
to follow up these references for further, detailed
information. Overall NPG-Pt catalysts give very low
benefi t compared to Pt/C.
In fact, the area of dealloying is currently an ongoing
research topic aimed at the design of highly
active catalysts for the oxygen reduction reaction in
H2/O2 fuel cells. Experts in the area such as Professor
Doctor Peter Strasser, now at Technische Universität
Berlin, Germany, have documented very interesting
results with the study of dealloyed particles and their
use as catalysts for the oxygen reduction reaction
(6, 7). However, the use of dealloyed catalysts has not
been well documented for alcohol oxidation.
(a)
120 nm
(b)
500 nm
Fig. 2. Scanning
electron microscopy
images of a
nanoporous gold
leaf (Reproduced by
permission of The Royal
Society of Chemistry
and Alkali Metal Borohydrides
Chapter 5, ‘Nanocatalysts for Direct Borohydride
Oxidation in Alkaline Media’ by Christophe
Coutanceau et al. considers the use of alkali metal
borohydrides as fuels. Sodium borohydride is
preferred because it offers a compromise between
specifi c energy density and relative abundance. The
authors clearly explain the anodic and cathodic
reactions that occur in a direct borohydride fuel
cell (DBFC) and the theoretical effi ciency of a
system capable of achieving the 8 electron reaction.
Due to the alkaline environment used the catalysts
considered are the usual binaries and ternaries,
such as PdAu, PdNi and PdPtBi. The authors
describe a very interesting study of the kinetics
of the electrode reaction but most importantly
they present a discussion of what makes a catalyst
selective towards complete oxidation and also to
the inhibition of hydrogen oxidation. The use of
Pt0.9Bi0.1/C is presented as the most selective catalyst
that leads to the 8e-- pathway without signifi cant
hydrogen evolution. Although this anode catalyst led
to lower performance compared to Pt/C, in terms of
current density, it is of interest for a DBFC because
of increased fuel effi ciency, a prime parameter for
the use of the fuel. It is important to highlight that a
system with high cell effi ciency is more attractive for
many practical applications than a system with low
effi ciency and high current density. The authors have
written a very interesting chapter and this reader
gained useful knowledge about the technology.
The Use of Enzymes
Chapter 6, ‘Bioelectrocatalysis in Direct Alcohol Fuel
Cells’, by Holly Reeve and Kylie Vincent (University
of Oxford, UK), is dedicated to the use of enzymes
for the oxidation of sugars such as fructose, lactose
and glucose. The use of sugars for fuel cells is a
very interesting area for research since it is based
on the generation of electricity by the oxidation of
natural products. Actually, the full oxidation of a
primary alcohol to carbon dioxide is also possible
when using a chain of enzymes via a sequence of
chemical reactions. This is a key characteristic that
differentiates enzymes from metal nanoparticles.
For instance, there are very few metal catalysts
capable of achieving the full oxidation of dilute
ethanol to CO2 without the formation of incomplete
products such as acetaldehyde and acetic acid
(8). The authors give a fair and realistic view of
the practical problems of enzymes as catalysts
due to their relatively large size, which leads to
low volumetric density and their limited stability
when varying conditions such as pH, temperature,
pressure and solvent type. The authors highlight
that biofuel cells could have their main application
as bioimplantable fuel cells for pacemakers and for
the purifi cation of waste water. Although research
in this area is in its infancy, the authors give an
excellent overview of the use of biofuel cells and the
reader with an interest in biocatalysis will fi nd this
chapter extremely interesting.
Problems in Alcohol Oxidation
The book closes with Chapter 7, ‘Challenges and
Perspectives of Nanocatalysts in Alcohol-Fuelled
Direct Oxidation Fuel Cells’, by Eileen Hao Yu
(Newcastle University, UK) et al. This chapter covers
some of the main problems in alcohol oxidation
focusing on the factors affecting activity and stability,
including the need for more active catalysts capable of
oxidising adsorbed CO. The authors report on the use
of binary and ternary catalysts in alkaline and acid
media, such as PtRu, PtSn and PtRuM (M = tungsten,
molybdenum, nickel) and PtSnM (M = Ni or Ru), PtAu,
PdNi and PdIrNi. The use of metal oxides such as
cerium(IV) oxide, nickel(II) oxide, cobalt(II,III) oxide
and manganese(II,III) oxide as promoters capable of
introducing oxygenated species to remove adsorbed
CO is also described. A brief mention of the benefi ts
and disadvantages of the use of core–shell catalysts
is presented with a special emphasis on PtAu core–
shell catalysts. In terms of stability, some interesting
approaches are mentioned such as the use of
alternative carbon supports (graphene and N-doped
carbon nanotubes) and supports such as titanium
dioxide and tungsten carbide. The authors, however, do
not mention the main problems of anode stability, such
as base metal dissolution, membrane contamination
and the impact on cathode performance or relate
these issues to real fuel cell data.
Conclusion
The authors describe in a detailed manner the
electrocatalytic oxidation of primary alcohols and
other relevant fuels of interest for low power fuel
cells in both acid and alkaline media. The reader
gains a useful introduction to the catalysis involved
in the oxidation of different fuels, such as methanol,
ethanol, ethylene glycol, glycerol, borohydride and
sugars. While enzymes and gold catalysts have been
introduced, platinum group metal catalysts, especially
those based on Pt and Pd, are the state of the art for
these technologies. The book only disappoints in
some areas such as the lack of real fuel cell data and,
for this reviewer’s taste, an overemphasis on alcohol
oxidation in alkaline media. Overall, this book can
be a good starting point for students and researchers
with an interest in low power fuel cells.
References
1 N. Cabello-Moreno, E. Crabb, J. Fisher, A. E. Russell and
D. Thompsett, ECS Trans., 2008, 16, (2), 483
2 J. M. Fisher, N. Cabello-Moreno, E. Christian and D.
Thompsett, Electrochem. Solid-State Lett., 2009, 12, (5),
B77
3 J. Erlebacher, M. J. Aziz, A. Karma, N. Dimitrov and K.
Sieradzki, Nature, 2001, 410, (6827), 450
4 R. C. Newman and K. Sieradzki, Science, 1994, 263,
(5 154), 1708
5 R. Zeis, A. Mathur, G. Fritz, J. Lee and J. Erlebacher, J.
Power Sources, 2007, 165, (1), 65
6 P. Mani, R. Srivastava and P. Strasser, J. Phys. Chem. C,
2008, 112, (7), 2770
7 L. Gan, M. Heggen, R. O’Malley, B. Theobald and P.
Strasser, Nano Lett., 2013, 13, ...

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Book Description Royal Society Of Chemistry, United Kingdom, 2012. Hardback. Condition: New. Language: English. Brand new Book. Energy and environment issues are of paramount importance to achieve the sustainable development of our society. Alcohol-fuelled direct oxidation fuel cells (DOFCs), as a clean and highly-efficient energy harvesting engine, have attracted intensive research activity over recent decades. Electrocatalysts are the material at the very heart of the cell that determines the performance of DOFCs. The rapid advances in electrocatalysts, particularly nano-sized ones, have left current information only available in scattered journals. To be truly useful to both present and future researchers, a new book is needed to present an insightful review of the reaction nature of this research and to systematically summarize recent advances in nanocatalysts, and convey a more global perspective. Catalysts for Alcohol-fuelled Direct Oxidation Fuel Cells will present a state-of-the-art review on recent advances in nanocatalysts and electrocatalysis in DOFCs, including both proton and hydroxide ion exchange membrane fuel cells. The main topics covered include a molecular-level understanding of electrocatalysis, the design principles of electrocatalysts, recent advances in nanocatalysts and future perspectives for DOFCs. The book presents a cutting-edge collection on nanocatalysts for alcohol-fuelled direct oxidation fuel cells and brings together the most authoritative researchers in the field from both industry and academia, filling the gap between both sides. Finally, the book will provide an insightful review on electrocatalysis at the molecular- level, which will be useful for postgraduate students and junior researchers in this field. It will be an essential resource for postgraduates, researchers and policy-makers globally in academia, industry, and government institutions. Seller Inventory # AAC9781849734059

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