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BIOMASS, BIOFUELS, BIOCHEMICALS
MICROBIAL
ELECTROCHEMICAL
TECHNOLOGY
SUSTAINABLE PLATFORM FOR FUELS,
CHEMICALS AND REMEDIATION
Edited by
S. VENKATA MOHAN
SUNITA VARJANI
ASHOK PANDEY
Series: Biomass, Biofuels, Biochemicals
This book and the individual contributions contained in it are protected under copyright by the
Publisher (other than as may be noted herein).
Notices
Knowledge and best practice in this field are constantly changing. As new research and experience
broaden our understanding, changes in research methods, professional practices, or medical
treatment may become necessary.
Practitioners and researchers must always rely on their own experience and knowledge in evaluating
and using any information, methods, compounds, or experiments described herein. In using such
information or methods they should be mindful of their own safety and the safety of others,
including parties for whom they have a professional responsibility.
To the fullest extent of the law, neither the Publisher nor the authors, contributors, or editors,
assume any liability for any injury and/or damage to persons or property as a matter of products
liability, negligence or otherwise, or from any use or operation of any methods, products,
instructions, or ideas contained in the material herein.
Library of Congress Cataloging-in-Publication Data
A catalog record for this book is available from the Library of Congress
xv
xvi CONTRIBUTORS
Gunda Mohanakrishna Energy and Environ- Education and Research (IISER) Mohali, Pun-
ment Lab, Department of Chemical Engineer- jab, India
ing, Qatar University, Doha, Qatar R.S. Prakasham Medicinal Chemistry and Bio-
Antonio Moran Chemical and Environmental technology, CSIR-Indian Institute of Chemical
Bioprocess Engineering Group, Natural Technology, Hyderabad, India
Resources Institute (IRENA) - University of Navanietha K. Rathinam BuG ReMeDEE con-
Leon, León, Spain sortium, Department of Chemical and Bio-
Y.V. Nancharaiah Biofouling and Biofilm Pro- logical Engineering, South Dakota School of
cesses Section of Water and Steam Chemistry Mines and Technology, Rapid City, SD, United
Division, Bhabha Atomic Research Centre, States; Department of Chemistry and Applied
Kalpakkam, India; Homi Bhabha National Biological Sciences, South Dakota School of
Institute, Mumbai, India Mines and Technology, Rapid City, SD, United
G.N. Nikhil Department of Biotechnology, Dr. States
B.R. Ambedkar National Institute of Technol- Rohit Rathour P. D. Patel Institute of Applied
ogy Jalandhar, Jalandhar, Punjab, India Sciences, Charotar University of Science and
Emre Oguz Koroglu Department of Environ- Technology (CHARUSAT), Changa, India
mental Engineering, Yildiz Technical Uni- C. Nagendranatha Reddy Department of Envi-
versity, Davutpasa Campus, Istanbul, Turkey ronmental Science and Engineering, Kyung
Bestami Ozkaya Department of Environmental Hee University, Yongin-si, Republic of Korea
Engineering, Yildiz Technical University, M. Venkateswar Reddy Institut für Molekulare
Davutpasa Campus, Istanbul, Turkey Mikrobiologie und Biotechnologie, West-
Ashok Pandey CSIR-Indian Institute of Tox- fälische Wilhelms Universität Munster, Mun-
icology Research, Lucknow, India ster, Germany
Soumya Pandit Department of Biotechnology, Isaac Rivera Institute of Environmental and
Indian Institute of Technology Kharagpur, Sustainable Chemistry, TU-Braunschweig,
Kharagpur, India; Amity Institute of Bio- Braunschweig, Germany
technology, Mumbai, India Shantonu Roy Department of Biotechnology,
Deepak Pant Separation and Conversion Tech- National Institute of Technology Arunachal
nologies, Flemish Institute for Technological Pradesh, Arunachal Pradesh, India
Research (VITO), Boeretang, Mol, Belgium David R. Salem BuG ReMeDEE consortium,
Catarina M. Paquete Instituto de Tecnologia Department of Chemical and Biological
Química e Biológica António Xavier, Uni- Engineering, South Dakota School of Mines
versidade NOVA de Lisboa, Oeiras, Portugal and Technology, Rapid City, SD, United
States; Department of Materials and Metal-
Alka Pareek Bioengineering and Environmental
lurgical Engineering, South Dakota School of
Science Lab, CEEFF CSIR-Indian Institute of
Mines and Technology, Rapid City, SD, United
Chemical Technology, Hyderabad, India
States; Composite and Nanocomposite
Piyush Parkhey Amity Institute of Bio- Advanced Manufacturing e Biomaterials Cen-
technology, Amity University, Raipur, India ter (CNAM-Bio Center), Rapid City, SD, United
Roberto Parra-Saldívar Tecnologico de Mon- States
terrey, School of Engineering and Science, Rajesh K. Sani BuG ReMeDEE consortium,
Campus Monterrey, Monterrey, Mexico Department of Chemical and Biological
Sunil A. Patil Department of Earth and Envi- Engineering, South Dakota School of Mines
ronmental Sciences, Indian Institute of Science and Technology, Rapid City, SD, United
CONTRIBUTORS xix
States; Composite and Nanocomposite Pier-Luc Tremblay School of Chemistry,
Advanced Manufacturing e Biomaterials Chemical Engineering and Life Science, Wuhan
Center (CNAM-Bio Center), Rapid City, SD, University of Technology, Wuhan, People’s
United States; Department of Chemistry and Republic of China
Applied Biological Sciences, South Dakota Inês B. Trindade Instituto de Tecnologia Quí-
School of Mines and Technology, Rapid City, mica e Biológica António Xavier, Universidade
SD, United States NOVA de Lisboa, Oeiras, Portugal
Sambhu Saptoka Civil and Environmental Karolien Vanbroekhoven Separation and Con-
Engineering, South Dakota School of Mines version Technologies, Flemish Institute for
and Technology, Rapid City, SD, United States Technological Research (VITO), Boeretang,
Omprakash Sarkar Bioengineering and Envi- Mol, Belgium
ronmental Sciences Lab, CEEFF, CSIR-Indian Jhansi L. Varanasi Department of Bio-
Institute of Chemical Technology, Hyderabad, technology, Indian Institute of Technology
India Kharagpur, Kharagpur, India
Uwe Schröder Institute of Environmental and Sunita Varjani Gujarat Pollution Control Board,
Sustainable Chemistry, TU-Braunschweig, Gandhinagar, Gujarat, India
Braunschweig, Germany
Ramya Veerubhotla Department of Bio-
Namita Shrestha Civil and Environmental technology, Indian Institute of Technology
Engineering, South Dakota School of Mines Kharagpur, Kharagpur, India
and Technology, Rapid City, SD, United States
G. Velvizhi Bioengineering and Environmental
Ana V. Silva Instituto de Tecnologia Química e Science Lab, CEEFF, CSIR-Indian Institute of
Biológica António Xavier, Universidade NOVA Chemical Technology, Hyderabad, India
de Lisboa, Oeiras, Portugal
Bhuvan Vemuri Civil and Environmental
J. Shanthi Sravan Bioengineering and Environ- Engineering, South Dakota School of Mines
mental Sciences Lab, CEEFF, CSIR-Indian and Technology, Rapid City, SD, United States
Institute of Chemical Technology, Hyderabad,
Anil Verma Sustainable Environergy Research
India
Lab (SERL), Department of Chemical Engi-
Pratiksha Srivastava Australian Maritime Col- neering, Indian Institute of Technology Delhi,
lege (AMC), University of Tasmania, Launces- New Delhi, India
ton, TAS, Australia
Ling Wang State Key Laboratory of Urban
Moogambigai Sugumar Department of Water Resource and Environment, Harbin
Mechanical Engineering, Anna University, Institute of Technology, Harbin, China
Chennai, India
Xin Wang MOE Key Laboratory of Pollution
Xiaohang Sun Department of Applied Sciences, Processes and Environmental Criteria, Tianjin
College of Environmental Technology, Mur- Key Laboratory of Environmental Remediation
oran Institute of Technology, 050-8585 Hok- and Pollution Control, College of Environ-
kaido, Muroran, Japan mental Science and Engineering, Nankai Uni-
Kuchi Swathi Bioengineering and Environ- versity, Tianjin, China
mental Science (BEES) Lab, CEEFF Centre, Ai-Jie Wang State Key Laboratory of Urban
CSIR-Indian Institute of Chemical Technology, Water Resource and Environment, Harbin
Hyderabad, India Institute of Technology, Harbin, China
Ekant Tamboli Department of Biotechnology, Huanting Wang Department of Chemical
National Institute of Technology (NITRR), Engineering, Monash University, Clayton, VIC,
Raipur, India Australia
xx CONTRIBUTORS
Jonathan W.C. Wong Sino-Forest Applied Dileep Kumar Yeruva Bioengineering and
Research Centre for Pearl River Delta Environmental Sciences Lab, EEFF Center,
Environment, Department of Biology, Hong CSIR-Indian Institute of Chemical Technology
Kong Baptist University, Hong Kong, P. R. (CSIR-IICT), Hyderabad, India
China Tian Zhang School of Chemistry, Chemical
Lichao Xia Civil and Environmental Engineer- Engineering and Life Science, Wuhan Uni-
ing, Rensselaer Polytechnic Institute, Troy, NY, versity of Technology, Wuhan, People’s
United States Republic of China
Asheesh Kumar Yadav CSIR-Institute of Min-
erals and Materials Technology, Bhubaneswar,
India
Preface
xxi
xxii PREFACE
1.1
Microbial Electrochemical
Technology: Emerging and
Sustainable Platform
S. Venkata Mohan1, J. Shanthi Sravan1, Sai Kishore Butti1,
K. Vamshi Krishna1, 2, J. Annie Modestra1, G. Velvizhi1,
A. Naresh Kumar1, 2, Sunita Varjani3, Ashok Pandey4
1
Bioengineering and Environmental Science Lab, CEEFF, CSIR-Indian Institute of Chemical
Technology, Hyderabad, India; 2Academy of Scientific and Innovative Research, Hyderabad,
India; 3Gujarat Pollution Control Board, Gandhinagar, Gujarat, India; 4CSIR-Indian Institute
of Toxicology Research, Lucknow, India
1.1.1 INTRODUCTION
Power
Nutrient/Chemical
Domestic Effluent MFC Recovery
Platform Chemicals/
Biogenic Waste BET Precursor molecules
Enhanced Product
Carbon/Nutrient MET Recovery
Source
Biobased
Electro-Product
FIGURE 1.1.1 Applications of diverse METs for bio-based product recovery from various waste feedstocks. BES,
bioelectrochemical system; BET, bioelectrochemical treatment; EF, electrofermentation; MDC, microbial desalination
cell; MEC, microbial electrolysis cell; MET, microbial electrochemical technology; MFC, microbial fuel cell.
The origin of electrical effects through biological catalyzed reactions was reported by Gal-
vani in 1789 when he observed that frog muscles twitched with copper-zinc couples [20],
which is probably the earliest observation on “physiological processes accompanied by chem-
ical changes associated with electrical changes.” Fig. 1.1.2 depicts an overview of the origin
and history of MET. After a considerable gap, in 1911 M.C. Potter reported microbial-
induced electrode reduction, which has led to the development of biofuel cells, later termed
as “microbial fuel cell (MFC)” [21]. The chemical energy stored in the bonds of organic
substrate is catalyzed by the action of bacterial metabolism producing electrical energy,
through a cascade of redox reactions in a defined fuel cell setup. Contrary to the fuel cell,
MFC uses biological organisms to catalyze the electrochemical reactions which are analogous
to an inorganic catalyst. This bioenergy obtained from MFC is recognized as an alternative to
MET’s
Microbial Fuel Cell (MFC)
Bioelectrochemical System (BES)
Microbial Electrolysis Cell (MEC)
Bio-Electrochemical Treatment (BET)
Microbial Desalination Cell (MDC)
Microbial Electrofermentation (MEF)
the conventional fuels that reduces the global carbon footprint if applied. Potter had experi-
mented with a special type of galvanic cells using platinum electrodes to determine the elec-
tromotive force (EMF) developed due to the disintegration of organic compounds by
microorganisms through fermentative activity. The study inferred a maximum potential
difference of 0.3e0.5 V when the experiments were performed with microorganisms [21].
Barnett Cohen in 1931 stacked six cells using yeast as a biocatalyst and glucose as substrate
and developed a battery with an output of 35 V (2 mA) [22]. He also used potassium ferri-
cyanide/benzoquinone as artificial electron mediators. In 1962, Davis and Yarbrough stud-
ied microbes function in utilizing hydrocarbon [23]. Electrical output was not detected
when ethane was used as the sole substrate.
Duca and Fuscoe in 1964 explained the thermodynamics pertaining to bioelectrochemical
energy conversion along with the changes in electrode potential during the biochemical
reactions [24]. The report also suggested MET to have application in four general areas,
viz., as power sources, detectors of specific contaminants in low concentrations, sensors for
generation of control signals, and catalysts for the generation of electrochemical reactions
[24]. In 1977, Karube and co-workers studied anodic reactions of a biochemical cell by using
Number of Papers
Number of Citations
Number of Citations
800 6000
240
24000
600 200 4500
160
16000
400 120 3000
80
200 8000 1500
40
0
0 0 0
1985 1988 1991 1994 1997 2000 2003 2006 2009 2012 2012 2018* 1985 1988 1991 1994 1997 2000 2003 2006 2009 2012 2012 2018*
Publishing Year
Publishing Year
Microbial Electrolysis Cell Bioelectrochemical Treatment System
Number of Papers Number of Citations Number of Papers Number of Citations
6000 3600
210 180
5400
3200
180
4800 150
2800
Number of Papers
Number of Papers
Number of Citations
Number of Citations
150 4200
120 2400
3600
120 2000
3000 90
90 1600
2400
60 1200
60 1800
1200 800
30 30
600 400
0 0 0 0
1985 1988 1991 1994 1997 2000 2003 2006 2009 2012 2012 2018* 1985 1988 1991 1994 1997 2000 2003 2006 2009 2012 2012 2018*
Publishing Year Publishing Year
Microbial Desalination System
Number of Papers Number of Citations 2100
90
1800
75
Number of Papers
Number of Citations
1500
60
1200
45
900
30
600
15
300
0 0
1985 1988 1991 1994 1997 2000 2003 2006 2009 2012 2012 2018*
Publishing Year
the observation of light stimulus being absorbed as electrical energy in photosynthesis has
driven towards conception of an idea that a result of dissociation/association generates
current. To confirm this idea of electrical energy generation, preliminary experiments
were carried out to determine if any EMF or potential difference was developed by
10000 250000
Number of Citations
Number of Papers
8000 200000
6000 150000
4000 100000
2000 50000
0 0
*MFC: Microbial Fuel Cell, BES: Bioelectrochemical System, MEC: Microbial Electrolysis Cell,
BET: Bioelectrochemical Treatment, MDC: Microbial Desalination Cell,
MES: Microbial Electrochemical System
FIGURE 1.1.4 Year-wise published papers and citation indices of different microbial electrochemical technolo-
gies. Clarivate Analytics Web of Science report (5th March-2018).
fermentative activity of yeast or bacteria [23]. A simple yeast glucose experiment was
designed and carried out in a galvanic cell, which generated EMF by glucose metabolism
and has given promising leads for investigating this concept further [22]. The voltage/
EMF registered in yeast glucose cells was recognized to be the effect of charge collected
in the fermenting liquid. It was also observed that some enzymes partly contribute to po-
tential difference/voltage generation. Consecutively, few experiments were carried out us-
ing bacterial species, specifically Bacillus as biocatalyst in the galvanic cell containing
nutrient medium which depicted considerable growth along with current and EMF. It
was observed that biochemical systems such as whole-cell organism/crystallized
enzyme/cell-free extracts can generate ammonia, hydrogen or methanol from complex
organic raw materials such as starch, protein, fats, sugars, urea, etc. as substrate [32]. These
studies concluded that electrode materials can effect potential difference, and the electrical
energy generation is dependent on the activity of microorganism, nutrient availability, tem-
perature, etc. [25].
Biological systems are associated with energy transfer reactions of oxidation/reduction
reactions. The relation between free energy change and standard redox potential of biological
reactions can be determined through the second law of thermodynamics, which will provide
a holistic view of bioenergetics [33]. In general, from a thermodynamic perspective, a reaction
is defined as “spontaneous” or “non-spontaneous” based on the free energy change and the
redox potential. Electron transfer from one compound to the other is in turn dependent on
redox potentials between electron donor and acceptor. The tendency of a redox reaction to
-0.3
Flavoprotein CO2/Acetate [-0.28]
Acetaldehyde/Ethanol [-0.2]
-0.2
Fe-S proteins Pyruvate/Lactate [-0.18]
Quinone -0.1 Oxaloacetate/Malate [-0.16]
Cytochrome C 0.3
0.4
Cytochrome
aa3 0.5
0.6
0.7
NO3-/N2 [0.74]
O2 Fe3+/Fe2+ [0.76]
0.8
O2/H2O [0.82]
FIGURE 1.1.5 Standard redox potentials reported with standard hydrogen electrode (SHE) in volts (V) for
several biological redox mediators.
FIGURE 1.1.6 Various biocatalysts used in METs and their modes of extracellular electron transport.
Like many of the owners of that time Murray lived directly opposite
his works and he installed in his house a steam heating apparatus
which excited much wonder and which must have been one of the
first in use. He built the first locomotive which was put to successful
commercial use. Trevithick had invented a steam road-engine with a
single steam cylinder and a large flywheel, which had attracted
considerable attention, but was wholly impracticable. It was
important, however, as it had one of the first high-pressure engines,
working above atmospheric pressure. In 1811 Blenkinsop of Leeds,
taking his idea from Trevithick, had a number of locomotives built to
operate a railway from the Middletown collieries to Leeds, a distance
of 3¹⁄₂ miles. Blenkinsop was not a mechanic and the work was
designed and executed by Matthew Murray. Murray used two steam
cylinders instead of one, driving onto the same shaft with cranks set
at right angles, and therefore introduced one of the most important
features of modern locomotive design. These engines were in daily
use for many years and were inspected by George Stephenson
when he began his development of the locomotive. Murray’s design
formed the basis from which he started. The engines, however, were
operated by a cog-wheel driving onto a continuous rack laid along
the road bed. It was not until a number of years later that Hedley and
Stephenson established the fact that the wheel friction of smooth
drivers would furnish adequate tractive power. The old Blenkinsop
engines, as they were called, hauled about thirty coal wagons at a
speed of 3¹⁄₄ miles an hour.
Murray’s most important inventions were connected with the flax
industry and for these he obtained a gold medal from the Society of
Arts. At the time they were developed, the flax trade was dying. Their
effect was to establish the British linen trade on a permanent and
secure foundation. All the machine tools used in his establishment
were designed and built by himself and among these was the planer
which was unquestionably one of the earliest built. He made similar
articles for other firms and started a branch of engineering for which
Leeds became famous. He was a frank, open-hearted man, and one
who contributed greatly to the industrial supremacy of England.
Joseph Clement was born in Westmoreland in 1779.[56] His father
was a weaver, a man of little education but of mental ability, a great
lover of nature and something of a mechanic. Joseph Clement
himself had only the merest elements of reading and writing. He
started in life as a thatcher and slater, but picked up the rudiments of
mechanics at the village blacksmith shop. Being grateful to the
blacksmith, he repaid him by making for him a lathe which was a
pretty creditable machine. On this he himself made flutes and fifes
for sale and also a microscope for his father to use in his nature
studies. As early as 1804 he began to work on screw cutting and
made a set of die-stocks, although he had never seen any. He
worked in several small country shops, then in Carlisle and in
Glasgow, where he took lessons in drawing from a Peter Nicholson
and became one of the most skillful draftsmen in England. Later he
went to Aberdeen and was earning three guineas ($15) a week
designing and fitting up power looms. By the end of 1813 he had
saved £100. With this he went to London, meaning sooner or later to
set up for himself. He first worked for an Alexander Galloway, a ward
politician and tradesman who owned a small shop. Galloway was a
slovenly manager and left things to run themselves. When Clement
started in he found the tools so poor that he could not do good work
with them, and immediately set to work truing them up, to the
surprise of his shopmates who had settled down to the slipshod
standards of the shop. Seeing that Clement was capable of the
highest grade work, one of his shopmates told him to go to Bramah’s
where such workmanship would be appreciated.
[56] The best information on Clement comes from Smiles’ “Industrial
Biography,” Chap. XIII.
He saw Bramah and engaged to work for him for a month on trial.
The result was so satisfactory that he signed an agreement for five
years, dated April 1, 1814, under which he became chief draftsman
and superintendent of the Pimlico works. Clement threw himself
eagerly into the new work and took great satisfaction in the high
quality of work which was the standard in Bramah’s establishment.
Bramah was greatly pleased with him and told him, “If I had secured
your services five years since I would now have been a richer man
by many thousands of pounds.” Bramah died, however, within a year
and his two sons returning from college took charge of the business.
They soon became jealous of Clement’s influence and by mutual
consent the agreement signed with their father was terminated.
Clement immediately went to Maudslay & Field’s as chief draftsman
and assisted in the development of the early marine engines which
they were building at that time. In 1817 he started in for himself in a
small shop in Newington, with a capital of £500 and his work there
until his death in 1844 is of great importance.
Figure 18. Matthew Murray
Figure 19. Richard Roberts
Since M. Camus has treated of no other curve than the epicycloid, it would
appear that he considered it to supersede all others for the figure of the teeth of
wheels and pinions. And the editor must candidly acknowledge that he entertained
the same opinion until after the greater part of the foregoing sheets were printed
off; but on critically examining the properties of the involute with a view to the
better explaining of its application to the formation of the teeth of wheels and
pinions, the editor has discovered advantages which had before escaped his
notice, owing, perhaps, to his prejudice in favor of the epicycloid, from having,
during a long life, heard it extolled above all other curves; a prejudice strengthened
too by the supremacy given to it by De la Hire, Doctor Robison, Sir David
Brewster, Dr. Thomas Young, Mr. Thomas Reid, Mr. Buchannan, and many others,
who have, indeed, described the involute as a curve by which equable motion
might be communicated from wheel to wheel, but scarce any of whom have held it
up as equally eligible with the epicycloid; and owing also to his perfect conviction,
resulting from strict research, that a wheel and pinion, or two wheels, accurately
formed according to the epicycloidal curve, would work with the least possible
degree of friction, and with the greatest durability.
But the editor had not sufficiently adverted to the case where one wheel or
pinion drives, at the same time, two or more wheels or pinions of different
diameters, for which purpose the epicycloid is not perfectly applicable, because
the form of the tooth of the driving wheel cannot be generated by a circle equal to
the radius of more than one of the driven wheels or pinions. In considering this
case, he found that the involute satisfies all the conditions of perfect figure, for
wheels of any sizes, to work smoothly in wheels of any other sizes; although,
perhaps, not equal to the epicycloid for pinions of few leaves.
So far as the writer knows this is the first real appreciation of the
value of the involute curve for tooth outlines, and Hawkins should be
given a credit which he has not received,[64] especially as he points
the way, for the first time, to the possibility of a set of gears any one
of which will gear correctly with any other of the set. It was thought at
that time that there should be two diameters of describing circles
used in each pair of gears, each equal to the pitch radius of the
opposite wheel or pinion. This gave radial flanks for all teeth, but
made the faces different for each pair. The use of a single size of
describing circle throughout an entire set of cycloidal gears, whereby
they could be made to gear together in any combination, was not
known until a little later.
[64] John Isaac Hawkins was a member of the Institution of Civil
Engineers. He was the son of a watch and clock maker and was born at
Taunton, Somersetshire, in 1772. At an early age he went to the United
States and “entered college at Jersey, Pennsylvania, as a student of
medicine,” but did not follow it up. He was a fine musician and had a
marked aptitude for mechanics. He returned to England, traveled a great
deal on the Continent, and acquired a wide experience. He was consulted
frequently on all kinds of engineering activities, one of them being the
attempt, in 1808, to drive a tunnel under the Thames. For many years he
practiced in London as a patent agent and consulting engineer. He went to
the United States again in the prosecution of some of his inventions, and
died in Elizabeth, N. J., in 1865. From a Memoir in the “Transactions of the
Institution of Civil Engineers,” Vol. XXV, p. 512. 1865.