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E-raamat: Bioelectrochemistry: Fundamentals, Applications and Recent Developments

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Bioelectrochemistry: Fundamentals, Applications and Recent DevelopmentsSuurem pilt
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Chemists review recent developments in methodology and new applications in analytical detection, medicine, and energy conversion. They cover amperometric biosensors, imaging of single biomolecules by scanning tunneling microscopy, applications in reflectivity in bioelectrochemistry, model lipid bilayers at electrode surfaces, enzymatic fuel cells, Raman spectroscopy of biomolecules at electrode surfaces, membrane electroporation in high electric fields, and electroporation for medical use in drug and gene electrotransfer. Annotation ©2012 Book News, Inc., Portland, OR (booknews.com)

Here, the expert editors have carefully selected contributions to best reflect the latest developments in this hot and rapidly developing interdisciplinary topic at the interface of electrochemistry, biochemistry, analytical and medicinal chemistry. The resulting excellent and timely overview of this multifaceted field covers recent methodological developments, as well as a range of new applications for analytical detection, drug screening, tumor therapy, and for energy conversion in biofuel cells.
Preface xi
List of Contributors
xiii
1 Amperometric Biosensors
1(84)
Sabine Borgmann
Albert Schulte
Sebastian Neugebauer
Wolfgang Schuhmann
1.1 Introduction
1(22)
1.1.1 Definition of the Term "Biosensor"
3(4)
1.1.2 Milestones and Achievements Relevant to Biosensor Research and Development
7(1)
1.1.3 "First-Generation" Biosensors
7(1)
1.1.4 "Second-Generation" Biosensors
7(6)
1.1.5 "Third-Generation" Biosensors
13(2)
1.1.6 Reagentless Biosensor Architectures
15(3)
1.1.7 Parameters with a Major Impact on Overall Biosensor Response
18(4)
1.1.8 Application Areas of Biosensors
22(1)
1.2 Criteria for "Good" Biosensor Research
23(2)
1.3 Defining a Standard for Characterizing Biosensor Performances
25(3)
1.4 Success Stories in Biosensor Research
28(27)
1.4.1 Direct ET Employed for Biosensors and Biofuel Cells
29(3)
1.4.2 Direct ET with Glucose Oxidase
32(4)
1.4.3 Mediated ET Employed for Biosensors and Biofuel Cells
36(2)
1.4.4 Nanomaterials and Biosensors
38(1)
1.4.4.1 Modification of Macroscopic Transducers with Nanomaterials
39(2)
1.4.4.2 Nanometric Transducers
41(1)
1.4.4.3 Modification of Biomolecules with Nanomaterials
42(1)
1.4.5 Implanted Biosensors for Medical Research and Health Check Applications
42(6)
1.4.6 Nucleic Acid-Based Biosensors: Nucleic Acid Chips, Arrays, and Microarrays
48(4)
1.4.7 Immunosensors
52(1)
1.4.7.1 Labeled Approaches
53(1)
1.4.7.2 Nonlabeled Approaches
54(1)
1.5 Conclusion
55(30)
Acknowledgments
56(1)
Abbreviations
57(1)
Glossary
57(4)
References
61(24)
2 Imaging of Single Biomolecules by Scanning Tunneling Microscopy
85(58)
Jingdong Zhang
Qijin Chi
Palle Skovhus Jensen
Jens Ulstrup
2.1 Introduction
85(2)
2.2 Interfacial Electron Transfer in Molecular and Protein Film Voltammetry
87(5)
2.2.1 Theoretical Notions of Interfacial Chemical and Bioelectrochemical Electron Transfer
88(2)
2.2.2 Nuclear Reorganization Free Energy
90(1)
2.2.3 Electronic Tunneling Factor in Long-Range Interfacial (Bio)electrochemical Electron Transfer
90(2)
2.3 Theoretical Notions in Bioelectrochemistry towards the Single-Molecule Level
92(5)
2.3.1 Biomolecules in Nanoscale Electrochemical Environment
92(1)
2.3.2 Theoretical Frameworks and Interfacial Electron Transfer Phenomena
92(1)
2.3.2.1 Redox (Bio)molecules in Electrochemical STM and Other Nanogap Configurations
93(2)
2.3.2.2 New Interfacial (Bio)electrochemical Electron Transfer Phenomena
95(2)
2.4 In Situ Imaging of Bio-related Molecules and Linker Molecules for Protein Voltammetry with Single-Molecule and Sub-molecular Resolution
97(10)
2.4.1 Imaging of Nucleobases and Electronic Conductivity of Short Oligonucleotides
97(1)
2.4.2 Functionalized Alkanethiols and the Amino Acids Cysteine and Homocysteine
98(2)
2.4.2.1 Functionalized Alkanethiols as Linkers in Metalloprotein Film Voltammetry
100(2)
2.4.2.2 In Situ STM of Cysteine and Homocysteine
102(2)
2.4.2.3 Theoretical Computations and STM Image Simulations
104(1)
2.4.3 Single-Molecule Imaging of Bio-related Small Redox Molecules
105(2)
2.5 Imaging of Intermediate-Size Biological Structures: Lipid Membranes and Insulin
107(5)
2.5.1 Biomimetic Mono- and Bilayer Membranes on Au(111) Electrode Surfaces
107(2)
2.5.2 Monolayers of Human Insulin on Different Low-Index Au Electrode Surfaces Mapped to Single-Molecule Resolution by In Situ STM
109(3)
2.6 Interfacial Electrochemistry and In Situ Imaging of Redox Metalloproteins and Metalloenzymes at the Single-Molecule Level
112(11)
2.6.1 Metalloprotein Voltammetry at Bare and Modified Electrodes
112(1)
2.6.2 Single-Molecule Imaging of Functional Electron Transfer Metalloproteins by In Situ STM
112(2)
2.6.2.1 Small Redox Metalloproteins: Blue Copper, Heme, and Iron-Sulfur Proteins
114(1)
2.6.2.2 Single-Molecule Tunneling Spectroscopy of Wild-Type and Cys Mutant Cytochrome b562
114(2)
2.6.2.3 Cytochrome c4: A Prototype for Microscopic Electronic Mapping of Multicenter Redox Metalloproteins
116(3)
2.6.2.4 Redox Metalloenzymes in Electrocatalytic Action Imaged at the Single-Molecule Level: Multicopper and Multiheme Nitrite Reductases
119(1)
2.6.2.5 Au-Nanoparticle Hybrids of Horse Heart Cytochrome c and P. aeruginosa Azurin
120(3)
2.7 Some Concluding Observations and Outlooks
123(20)
Acknowledgments
126(1)
References
126(17)
3 Applications of Neutron Reflectivity in Bioelectrochemistry
143(46)
Ian J. Burgess
3.1 Introduction
143(1)
3.2 Theoretical Aspects of Neutron Scattering
144(10)
3.2.1 Why Use Neutrons?
144(1)
3.2.2 Scattering from a Single Nucleus
145(2)
3.2.2.1 The Fermi Pseudo Potential
147(1)
3.2.3 Scattering from a Collection of Nuclei
147(1)
3.2.3.1 Neutron Scattering Cross Sections
147(1)
3.2.3.2 Coherent and Incoherent Scattering
148(1)
3.2.3.3 Effective Potential and Scattering Length Density
148(1)
3.2.4 Theoretical Expressions for Specular Reflectivity
149(1)
3.2.4.1 The Continuum Limit
149(2)
3.2.4.2 The Kinematic Approach
151(3)
3.3 Experimental Aspects
154(14)
3.3.1 Experimental Aspects of Reflectometer Operation
154(3)
3.3.2 Substrate Preparation and Characterization
157(3)
3.3.3 Cell Design and Assembly
160(2)
3.3.4 Data Acquisition and Analysis
162(6)
3.4 Selected Examples
168(14)
3.4.1 Supported Proteins, Peptides, and Membranes without Potential Control
168(1)
3.4.1.1 Quartz- and Silicon-Supported Bilayers
168(2)
3.4.1.2 Hybrid Bilayers on Solid Supports
170(3)
3.4.1.3 Protein Adsorption and DNA Monolayers
173(2)
3.4.2 Electric Field-Driven Transformations in Supported Model Membranes
175(7)
3.5 Summary and Future Aspects
182(7)
Acknowledgments
184(1)
References
185(4)
4 Model Lipid Bilayers at Electrode Surfaces
189(40)
Rolando Guidelli
Lucia Becucci
4.1 Introduction
189(1)
4.2 Biomimetic Membranes: Scope and Requirements
189(3)
4.3 Electrochemical Impedance Spectroscopy
192(2)
4.4 Formation of Lipid Films in Biomimetic Membranes
194(7)
4.4.1 Vesicle Fusion
196(2)
4.4.2 Langmuir-Blodgett and Langmuir-Schaefer Transfer
198(2)
4.4.3 Rapid Solvent Exchange
200(1)
4.4.4 Fluidity in Biomimetic Membranes
201(1)
4.5 Various Types of Biomimetic Membranes
201(21)
4.5.1 Solid-Supported Bilayer Lipid Membranes
201(2)
4.5.2 Tethered Bilayer Lipid Membranes
203(1)
4.5.2.1 Spacer-Based tBLMs
204(1)
4.5.2.2 Thiolipid-Based tBLMs
205(10)
4.5.2.3 Thiolipid-Spacer-Based tBLMs
215(1)
4.5.3 Polymer-Cushioned Bilayer Lipid Membranes
216(2)
4.5.4 S-Layer Stabilized Bilayer Lipid Membranes
218(2)
4.5.5 Protein-Tethered Bilayer Lipid Membranes
220(2)
4.6 Conclusions
222(7)
Acknowledgments
223(1)
References
223(6)
5 Enzymatic Fuel Cells
229(40)
Paul Kavanagh
Donal Leech
5.1 Introduction
229(6)
5.1.1 Enzymatic Fuel Cell Design
231(1)
5.1.2 Enzyme Electron Transfer
231(4)
5.2 Bioanodes for Glucose Oxidation
235(8)
5.3 Biocathodes
243(12)
5.4 Assembled Biofuel Cells
255(4)
5.5 Conclusions and Future Outlook
259(10)
Acknowledgments
261(1)
References
262(7)
6 Raman Spectroscopy of Biomolecules at Electrode Surfaces
269(66)
Philip Bartlett
Sumeet Mahajan
6.1 Introduction
269(1)
6.2 Raman Spectroscopy
270(2)
6.3 SERS and Surface-Enhanced Resonant Raman Spectroscopy
272(4)
6.4 Comparison of SE(R)RS and Fluorescence for Biological Studies
276(2)
6.5 Surfaces for SERS
278(2)
6.6 Plasmonic Surfaces
280(1)
6.7 SERS Surfaces for Electrochemistry
281(10)
6.8 Tip-Enhanced Raman Spectroscopy
291(1)
6.9 SE(R)RS of Biomolecules
292(23)
6.9.1 DNA Bases, Nucleotides, and Their Derivatives
292(4)
6.9.2 DNA and Nucleic Acids
296(3)
6.9.3 Amino Acids and Peptides
299(4)
6.9.4 Proteins and Enzymes
303(1)
6.9.4.1 Redox Proteins
303(4)
6.9.4.2 Other Proteins
307(1)
6.9.4.3 Enzymes
308(2)
6.9.5 Membranes, Lipids, and Fatty Acids
310(1)
6.9.6 Metabolites and Other Small Molecules
311(1)
6.9.6.1 Neurotransmitters
311(1)
6.9.6.2 Nicotinamide Adenine Dinucleotide
312(1)
6.9.6.3 Flavin Adenine Dinucleotide
313(2)
6.9.6.4 Bilirubin
315(1)
6.9.6.5 Glucose
315(1)
6.10 Conclusion
315(20)
References
316(19)
7 Membrane Electroporation in High Electric Fields
335(34)
Rumiana Dimova
7.1 Introduction
335(3)
7.1.1 Giant Vesicles as Model Membrane Systems
335(2)
7.1.2 Mechanical and Rheological Properties of Lipid Bilayers
337(1)
7.2 Electrodeformation and Electroporation of Membranes in the Fluid Phase
338(4)
7.3 Response of Gel-Phase Membranes
342(3)
7.4 Effects of Membrane Inclusions and Media on the Response and Stability of Fluid Vesicles in Electric Fields
345(5)
7.4.1 Vesicles in Salt Solutions
345(2)
7.4.2 Vesicles with Cholesterol-Doped Membranes
347(2)
7.4.3 Membranes with Charged Lipids
349(1)
7.5 Application of Vesicle Electroporation
350(7)
7.5.1 Measuring Membrane Edge Tension from Vesicle Electroporation
350(3)
7.5.2 Vesicle Electrofusion
353(1)
7.5.2.1 Fusing Vesicles with Identical or Different Membrane Composition
353(2)
7.5.2.2 Vesicle Electrofusion: Employing Vesicles as Microreactors
355(2)
7.6 Conclusions and Outlook
357(12)
Acknowledgments
358(1)
References
358(11)
8 Electroporation for Medical Use in Drug and Gene Electrotransfer
369(20)
Julie Gehl
8.1 Introduction
369(1)
8.2 A List of Definitions
370(1)
8.3 How We Understand Permeabilization at the Cellular and Tissue Level
371(3)
8.4 Basic Aspects of Electroporation that are of Particular Importance for Medical Use
374(3)
8.4.1 Delivery of Drugs
374(1)
8.4.2 Delivery of DNA
375(1)
8.4.3 Delivery of Other Molecules
376(1)
8.4.4 Delivery of Electric Pulses
376(1)
8.4.5 End of the Permeabilized State
376(1)
8.4.6 The Vascular Lock
377(1)
8.5 How to Deliver Electric Pulses in Patient Treatment
377(1)
8.5.1 Pulse Generators and Electrodes
377(1)
8.5.2 Anesthesia
377(1)
8.6 Treatment and Post-treatment Management
378(1)
8.7 Clinical Results with Electrochemotherapy
378(2)
8.7.1 Tumors Up to Three Centimeters in Size
378(2)
8.7.2 Larger Tumors
380(1)
8.8 Use in Internal Organs
380(1)
8.8.1 Endoscopic Use
381(1)
8.8.2 Bone Metastases
381(1)
8.8.3 Brain Metastases, Brain Tumors, and Other Tumors in Soft Tissues
381(1)
8.8.4 Liver Metastases
381(1)
8.9 Gene Electrotransfer
381(5)
8.9.1 Gene Electrotransfer to Muscle
383(1)
8.9.2 Gene Electrotransfer to Skin
383(1)
8.9.3 Gene Electrotransfer to Tumors
384(1)
8.9.4 Gene Electrotransfer to Other Tissues
385(1)
8.10 Conclusions
386(3)
References
386(3)
Index 389
Richard C. Alkire is Professor Emeritus of Chemical & Biomolecular Engineering Charles and Dorothy Prizer Chair at the University of Illinois, Urbana, USA. He obtained his degrees at Lafayette College and University of California at Berkeley. He has received numerous prizes, including Vittorio de Nora Award and Lifetime National Associate award from National Academy.

Dieter M. Kolb is Professor of Electrochemistry at the University of Ulm, Germany. He received his undergraduate and PhD degrees at the Technical University of Munich. He was a Postdoctoral Fellow at Bell Laboratories, Murray Hill, NJ, USA. He worked as a Senior Scientist at the Fritz-Haber-Institute of the Max-Planck-Society, Berlin and completed his habilitation at the Free University of Berlin, where he also was Professor. Prof. Kolb has received many prizes and is a member of several societies.

Jacek Lipkowski is Professor at the Department of Chemistry and Biochemistry at the University of Guelph, Canada. His research interests focus on surface analysis and interfacial electrochemistry. He has authored over 120 publications and is a member of several societies, including a Fellow of the International Society of Electrochemistry.
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