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Hemicelluloses and Lignin
in Biorefineries
GREEN CHEMISTRY AND CHEMICAL ENGINEERING
Series Editor: Sunggyu Lee
Ohio University, Athens, Ohio, USA
by
Jean-Luc Wertz
Magali Deleu
Séverine Coppée
Aurore Richel
CRC Press
Taylor & Francis Group
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Boca Raton, FL 33487-2742
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vii
viii Contents
xv
xvi Foreword
Addressing issues that are crucial to achieving these important goals, centre
around ensuring the steady and sustainable supply of lignocellulosic biomass and
innovating new technologies for second generation biorefineries to enable the
transformation of the nonedible part of biomass. This book gives an overview of
the current science and technology contributing to this ongoing biobased revolution,
which is all about preparing Europe for the post-petroleum era.
In my role as an executive director of the Bio-Based Industries Joint Undertaking,
which is the ambitious €3.7 billion joint initiative between biobased industry and
the EU, I am delighted to see Jean-Luc and his coauthors to bring together their
extensive knowledge and share it with the new generation of engineers and scientists,
entrepreneurs, and innovators.
As its first reader I really welcome the initiative of Jean-Luc Wertz and his coau-
thors and recommend this book to you as a fascinating review of the current state of
the art for biomass valorization.
Philippe Mengal
Bio-Based Industries Joint Undertaking
Brussels, Belgium
Preface
The bioeconomy is a response to key environmental challenges that the world
is facing already today. Bioeconomy aims to reduce the dependence on natural
resources, transform manufacturing, promote sustainable production of renewable
resources from land, fisheries and aquaculture and their conversion into food, feed,
fiber, biobased products, and bioenergy, while developing new jobs and industries.
This book, titled Hemicelluloses and Lignin in Biorefineries, has been written to
demonstrate why the bioeconomy is crucial for future generations and why hemicel-
luloses and lignins are the molecules of the future.
At the heart of this bioeconomy are biorefineries. These processing facilities
transform biomass into energy and into a range of products in a sustainable way
by combining plant chemistry and biotechnology. They will gradually replace oil
refineries by using renewable resources in place of fossil fuels. A common goal for
biorefineries is to use all parts of the biomass raw material as efficiently as possible,
that is, maximizing the economic added value, whereas minimizing the environ-
mental footprint. These biorefinery concepts include the application of advanced
separation and conversion processes, which are the current hot topics in the research
and development sector.
Our book deals with lignocellulosic biomass, the three main components of which
are cellulose, hemicelluloses, and lignin, which form the cell wall of the plant. It not
only presents new knowledge about the biosynthesis of these molecules but also
about their enzymatic degradation by focusing particularly on hemicelluloses and
lignin. Conversion of the latter is a topic of particular interest in recent years. Indeed,
by taking an interest in its valorization, lignin is no longer considered as a waste, but
a key product, which will be at the origin of most aromatic compounds.
This book is intended to serve as a comprehensive reference for any chemical
company, research center, and university involved in or interested in the bioeconomy.
xvii
Acknowledgments
We express our gratitude to the FRS–FNRS (Fonds national de la Recherche
Scientifique, Belgium) who helped to get funding for this book.
We also thank Philippe Mengal, executive director of the Bio-Based Industries
(BBI) Joint Undertaking, for accepting to write a foreword.
Jean-Luc Wertz dedicates this book to his family and, in particular, to the still
unborn child of his daughter, and to Mathilda, Nicolas, and Carolina, the three
children of his son.
Magali Deleu thanks the FRS–FNRS for her position as a senior research
associate and dedicates this book to her family, particularly her husband and three
children, Justine, Batiste, and Léane.
Aurore Richel acknowledges the University of Liege for supporting her research in
the field of biomass and waste valorization, and development of green technologies.
She also thanks the Walloon Region (Belgium).
Finally, we thank Teresita and Allison from the CRC Press for the huge support
and assistance during the publication of this book.
xix
About the Authors
Jean-Luc Wertz holds degrees in chemical and civil engineering and in economic
science from Catholic University of Louvain, Louvain-la-Neuve, Belgium, as well
as a PhD from the same university in applied science, specializing in polymer
chemistry. He has held various international positions in R&D, including Spontex,
where he was the worldwide director of R&D. He holds several patents related to
various products. Jean-Luc Wertz is now a project manager in biomass valorization
at ValBiom and has worked for more than 8 years on lignocellulosic biorefineries and
biobased products. He also wrote two books: Cellulose Science and Technology in
2010 and Lignocellulosic Biorefineries in 2013.
Séverine Coppée after completing her master’s degree in chemical sciences earned
her PhD degree in material sciences at the University of Mons, Mons, Belgium. She
then worked as a postdoctoral fellow in the field of organic photovoltaics first in
the United States and then for Materia Nova research center, Mons, Belgium. Since
2014, Dr. Coppée has been a project manager for GreenWin competitiveness cluster
in Wallonia, Belgium and is supporting the cluster members with building up the
biobased chemistry research projects through various funding opportunities, par-
ticularly in the framework of the Bio-based Industries Consortium (BIC) of which
GreenWin is an effective member. She is also an life cycle assessment (LCA) advisor
involved in the Life Cycle in Practice (LCiP), a European project (cofunded by the
LIFE + Environmental Policy and Governance Programme of the EU) of which
GreenWin is a partner. The LCiP project helps small and medium-sized enter-
prises (SMEs) in France, Belgium, Portugal, and Spain to reduce the environmental
impacts of their products and services across the entire life cycle.
Aurore Richel holds a degree in chemical sciences and PhD in chemistry from
the University of Liege, Liège, Belgium. Prof. Richel is currently professor and
xxi
xxii About the Authors
1
2 Hemicelluloses and Lignin in Biorefineries
Reuse
le
yc
ec
R
P ro d ucts
e lo ops
NPK
2
CO
Wa
g th
als
M
te re
te
ic
ts
ria m en
a
ner
in
ls a n d che g y n utri
Cl
os
ycle
Biorefinery
Rec
Bu s
il d i n g b l o c k Bio m a ss
FIGURE 1.1 Bioeconomy as part of the circular economy. (Courtesy of Patrick van
Leeuwen; Reproduced from Bio-based Industries Consortium, Bioeconomy: Circular by
Nature, http://biconsortium.eu/news/bioeconomy-circular-nature, 2015. With permission.)
FIGURE 1.2 The left circle is the bioeconomy; the right circle is the technical economy.
(Courtesy of Loes Deutekom; Reproduced from Partners4Innovation, Towards a Biobased and
Circular Economy, https://www.youtube.com/watch?v=3ibJsOQdeoc, 2013. With permission.)
Introduction 3
Biological Technical
materials materials
Mining/materials
Farming/
manufacturing
collection*
Materials/parts manufacturer
Biochemical
feedstock Product manufacturer
Soil Recycle
Biosphere
restoration
Retail/service provider
Refurbish/
remanufacture
Biogas Cascades Reuse/
redistribute
Maintain
Consumer User
Anaerobic
digestion/ Collection Collection
composting†
Extraction of Energy recovery
biochemical
feedstock†
Leakage (to be minimized)
Landfill
FIGURE 1.3 Inspired by living systems, the circular economy concept is built around opti-
mizing an entire system of resource or material flows. Like biological materials, technical
materials can be part of a cycle built around reuse, remanufacture, and recycling. A circular
economy advocates a shift away from the consumption of products to services. (Reprinted
by permission from Macmillan Publishers Ltd. Nat. Clim. Change, Ellen MacArthur
Foundation, 3, 180, copyright 2013.)
In the core of this economy are the biorefineries that sustainably transform bio-
mass into food, feed, chemicals, materials, and bioenergy (fuels, heat, and power)
generally through combination of plant chemistry and biotechnologies.
Lignocellulosic biomass consists of three major components—cellulose, hemicel-
luloses, and lignin—which form the plant cell wall. Although the cell walls of plants
vary in both composition and organization, they are all constructed using a struc-
tural principle common to all fiber composites.5 How the cell wall is biosynthesized
is not yet completely understood today.
Historically, cellulose was investigated the first, about 20 years ago, which
resulted in bioethanol fuel. Research on hemicelluloses followed resulting in valori-
zation of 5 carbon (C5) sugars. Investigation on lignin is starting now, with the grow-
ing understanding that the whole plant should be valorized and not only its cellulose
and hemicelluloses fractions.
4 Hemicelluloses and Lignin in Biorefineries
1.2 BIOECONOMY
1.2.1 Definition anD StakeS
Over the coming decades, the world will witness increased competition for limited
and finite natural resources. A growing global population will need a safe and secure
food supply. Climate change will have an impact on primary production systems
such as agriculture, forestry, fisheries, and aquaculture.6
A transition is needed toward an optimal use of renewable biological resources. We
must move toward sustainable primary production and processing systems that can
optimally produce food, fiber, and other biobased products with fewer inputs, less envi-
ronmental impact, and reduced greenhouse gas emissions. The optimal production
refers to modern concepts such as Functional Economy. The Functional Economy is a
concept that describes new economic dynamics based on providing solutions including
the use of equipment and services from a perspective that reduces the mobilization of
material resources while increasing the servicial value (the useful effects) of the solu-
tion.7 The model proposes to exchange the material goods by functional goods.
In 1989, the World Commission on Environment and Development—created
by the United Nations and chaired by the Norwegian Prime Minister Gro Harlem
Brundtland—has defined sustainable development as “development which meets the
needs of current generations without compromising the ability of future generations to
meet their own needs.”8 Sustainability includes three pillars: environment, social, and
economic. That definition explains without ambiguity that economic and social well-
being cannot coexist with measures that impact over the environment (Figure 1.4).
According to the EU definition, the bioeconomy encompasses the sustainable
production of renewable biological resources and their conversion into food, feed,
biobased products, and bioenergy.11 It includes agriculture, forestry, fisheries, food
and pulp, and paper production, as well as parts of chemical, biotechnological, and
energy industries. Its sectors and industries have a strong innovation potential due
to an increasing demand for its goods (food, energy, other biobased products) and to
SOCIAL
Bearable Equitable
Sustainable
FIGURE 1.4 The three pillars of sustainability. (Adapted from Green Planet Ethics, http://
greenplanetethics.com/wordpress/sustainable-development-can-we-balance-sustainable-
development-with-growth-to-help-protect-us-from-ourselves; http://en.wikipedia.org/wiki/
File:Sustainable_development.svg.)
Introduction 5
TABLE 1.1
The Bioeconomy in the European Union (2009)
Sector Annual Turnover (billion EUR) Employment (thousands)
Food 965 4400
Agriculture 381 12000
Paper/pulp 375 1800
Forestry/wood industries 269 3000
Fisheries and aquaculture 32 500
Biochemicals and plasticsa 50 150
Enzymesa 0.8 5
Biofuelsa 6 150
Total 2078 22005
Source: Commission Staff Working Document of COM, 60 final. Innovation for Sustainable Growth. A
Bioeconomy for Europe. http://ec.europa.eu/research/bioeconomy/pdf/bioeconomycommunication-
strategy_b5_brochure_web.pdf, 2012; https://biobs.jrc.ec.europa.eu/sites/default/files/generated/files/
policy/KBBE%20September%202010%20Report%20Achievements%20and%20Challenges.pdf
a Biobased industries.
their use of a wide range of sciences (from agronomy to process engineering or mate-
rials sciences) and industrial technologies, along with local and tacit knowledge.
Based on the available data from a wide range of sources, it is estimated that the
European bioeconomy has an annual turnover of about EUR 2 trillion and employs more
than 22 million people and approximately 9% of the total EU workforce (Table 1.1).11
The race problem is not one problem. It differs not only in time,
but in place. Therefore I always go to different groups of colored
people in this land with much of interest and curiosity, knowing that
each will present its peculiar phase of relationship between the white
and colored group.
I have just come back from such a journey, and its scenes and
lessons are filling my thought.
There was Toledo, with its colored group a little pushed aside and
half forgotten in the onward rush of the growing city till the group
gripped itself and awoke and said: “We are a part of Toledo—you
may not forget us.” So now slowly comes the push forward and
upward.
In Cleveland it is far different—it is not so much a matter of
gaining civic recognition as men and women—that battle was fought
by worthy men long years ago. It is the deeper problem of holding
the ground gained; of not letting theatres and restaurants and hotels
inaugurate a new discrimination which had once disappeared. This is
a difficult battle of the new economic rise of the Negro; when few
Negroes applied or had money to apply it was easy to say
theoretically, “Live where you will, go where you please.” But when a
group of black folk growing in power put a $75,000 church on your
corner—that is a phase of the race problem that hadn’t struck you
before.
Between these cities of past and present lies the mystic city of the
future, with its great cloud walls.
In Oberlin there are nearly two thousand young folk at study and
at play. Working and playing beside them are a hundred colored boys
and girls, and they all walk on sacred ground, on ground long since
consecrated to racial equality and hatred of caste and slavery. Yet
among these venerable ideals obtrudes the Present and it, with all its
odd corners, must be builded into the future city.
The present holds not only the problem of the treatment of ten
million black folk elsewhere, but of the hundred colored boys and
girls right there in Oberlin. It presents a tremendous moral dilemma
to frank young souls. When these children came from anti-slavery
homes they found it easy and natural to treat black men as men. But
coming now from a world that thinks God made a big mistake in ever
creating black folk—coming from such social teaching, they hesitate.
Once in a while a black student (or rather a yellow one) may be
elected a society, but usually no desert in character or scholarship
avails.
Yet this fact brings no mental peace or moral satisfaction. The
spirit of democracy is strong, the influence of the faculty is righteous,
and I came from five hours’ earnest conference with these young folk
with a sense of seeing a mighty battle for righteousness, and a belief
that somehow, sometime, justice would prevail.
But after all it was the men I met that meant most. Could I
introduce them? Let me see. There was the young lawyer who burned
to awaken a sleeping city to its duties and rights; there was the
brown physician who is one of the leading surgeons in the city, and
his knife finds no color line. Then the girl who ran a political
campaign last month had a father who was director in a white bank
and one of the solid business men of the town. In their parlor
gathered a brown father, a yellow mother, the white pastor and the
white girl chum—but why should we catalog the colors of their skins
and not those of their clothes? In Oberlin the chief book store is
“colored,” and the chief paperhanger and the chief building
contractor. Elsewhere I sat with the man who had just been elected a
member of a leading white city club and heard how the second
highest mechanic in the Peerless motor factory wore “the shadowed
livery of the sun.”
Therefore, all is well? Therefore, all is not well. Here are a climbing
people. The hardiest and most talented and the pushing are literally
forcing a way. But against them and against the ordinary black man
the bonds of medievalism are drawn and ghettos and sumptuary laws
are encompassed in the color line.
W. E. B. D.
EDITORIAL
ENVY.
It is unfortunate that in the recent newspaper discussion of an
Appeal to Europe sent out not by this Association but by a number of
colored men of influence and standing, reference was constantly
made to the lowest personal motives and seldom to the arguments
presented.
It is true that with all peoples, and especially with a race in the
throes of birth-pain, personal likes and jealousies play a wretchedly
large part. But it does not follow that they explain all the struggle and
difference of opinion. It is true that the rise of a man like Mr. Booker
T. Washington to a place of commanding influence has made him an
object of envy to many narrow souls. But it does not follow that the
thousands of intelligent people who differ with Mr. Washington are
all actuated by such motives, or are unable to distinguish great and
vital principles apart from personal feeling.
When, therefore, such differences of opinion arise, as it is natural
and healthy that they should arise, it is both wrong and unjust to
assume the motive to be necessarily low. Particularly is this true
when adequate causes of deep and compelling importance are openly
and honestly given as the cause of this difference.
Are such causes sufficient to sustain the complainers? That is a
matter of argument, not of innuendo or abuse. No man and no cause
are above the careful scrutiny and criticism of honest men, and
certainly to-day there is in the United States a very large field for
argument as to the proper attitude of colored leaders toward the race
problem.
THE TRUTH.
To the honest seeker for light the puzzling thing about the Southern
situation is the absolutely contradictory statements that are often
made concerning conditions. For instance, the New York Evening
Post is taken to task by the Norfolk (Va.) Landmark for assuming
that Southern colored men are largely disfranchised. The Virginia
paper says “No Negro in Virginia can be kept from voting, provided
he measures up to the same requirements for the exercising of that
right that the white man must. The laws of the State will protect him
in the right should election officials deny it him. That Negroes in this
State may freely qualify to vote is fully attested by the fact that
thousands of them do vote.” Again, the New Orleans Picayune
declares with regard to the complaint of disfranchisement, “The
arrant and absolute falsity of the specification in regard to the ballot
is seen in the fact that every legal bar to the exercise of the ballot
applies to whites and Negroes alike. Every elector (voter) must either
be able to read and write or, in case of illiteracy, he must pay taxes on
ordinary assessable property of the minimum value of $300. These
laws are strictly in accordance with the requirements of the
Constitution of the United States, and have been so pronounced by
the courts.”
Just so in earlier days before legal disfranchisement, paper after
paper and orator after orator declared that the Negro could and did
vote without let or hindrance.
Despite this, every intelligent person in the United States knows
that these statements are false. The Southern testimony to this is
itself open and convincing. Not only have we Mr. Tillman’s frank and
picturesque testimony on the past, but to-day the Richmond (Va.)
Leader says that all is well in Virginia “since we disfranchised the
Negro”; Congressman Underwood of Alabama says the Alabama
Negro “does not count for anything politically” in that State; a
prominent judge on the Mississippi bench says “The Negroes in
Mississippi do not vote and should not,” and it is a matter of plain
official record in Louisiana that of over 150,000 Negro males 21
years of age and over (of whom nearly 70,000 could read and write)
there were in 1908 only 1,743 registered as voters, and these were
disfranchised by the “White Primary” system. In the face of these
facts, does it pay deliberately to misrepresent the truth?
OPPORTUNITY.
A friend of our Association writes: “While I heartily approve of the
colored people being given an opportunity to improve their
condition, I feel that after doing what I can to help them to earn a
living honorably, they must depend on their own resources to
advance themselves.” This is the attitude of many excellent friends of
humanity, but it assumes that if a man is fairly equipped for earning
a living to-day he will have the opportunity to do so, and that the
paths before him will be open so as to make the rise of the deserving
possible.
It is precisely because the opportunity to earn a living, even for
those equipped to do so, is not given to-day to thousands of colored
people in the United States, that the National Association for the
Advancement of Colored People exists. It is wrong and wasteful to do
for people what they can and ought to do for themselves, but when
the doors of opportunity are so shut in their faces so as to discourage
and keep back the hard-working and deserving, then action is called
for.
To-day Negroes may work freely as menials at low wages; they may
work freely as farm laborers under conditions of semi-slavery; higher
than that they meet unusual difficulties—the difficulty of saving
capital from low wages to farm or go into business; the difficulty of
securing admission to the trades even when competent; the difficulty
of securing protection under the law and of rearing a family in
decency; the difficulty of educating their children; the difficulty of
protecting their rights by the ballot. To be sure, if they are unusually
gifted and pushing they may push higher at the risk of insult and
bitter opposition. Thus the fact remains that the mass of the willing,
eager workers of the race are held back and forced down by a deep
and growing race prejudice, and these, pressing down on the lower
strata, encourage in them laziness and vagrancy and crime. The
National Association for the Advancement of Colored People is an
organization for giving the colored race a reasonable opportunity to
help itself.
SCHOOLS.
The philanthropist of a city like New York is bewildered and often
exasperated by the demands and begging of colored schools in the
South.
To some extent this is inevitable, and is due to the fact that the
United States is undertaking to give elementary education to a race
of ten million people very largely by private philanthropy instead of
making this a State and even a national charge, and leaving to
voluntary effort the college work and work of social uplift.
But beyond this the philanthropic world is to some extent itself to
blame because of the encouragement it gives to unknown and
unvouched-for enterprises and to unwise and unjustifiable attempts
to duplicate existing foundations.
The representative of a great fund once called on the writer and
expressed great sorrow that an alleged school in the South to which
one of the most prominent New York philanthropists had given
$5,000 was found on investigation to be no school at all. This was
unfortunate, but there are hundreds of good and deserving schools
starving for help which this philanthropist did not give to because
their representatives did not appear so glib or plausible. It is not the
smoothest talker who necessarily is doing the best work.
THE NATIONAL PASTIME.
Seventy-five per cent. of the Negroes lynched have not even been
accused of rape.