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Building Model Systems To Understand Proton Coupled Electron Transfer In Heme
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Book Synopsis Building Model Systems to Understand Proton-Coupled Electron Transfer in Heme by : Christina J. Hanson
Download or read book Building Model Systems to Understand Proton-Coupled Electron Transfer in Heme written by Christina J. Hanson and published by . This book was released on 2013 with total page 111 pages. Available in PDF, EPUB and Kindle. Book excerpt: Proton-Coupled Electron Transfer (PCET) is an important mechanistic motif in chemistry, which allows for efficient charge transport in many biological systems. We seek to understand how the proton and electron motions are coupled in a bidirectional system allowing for individual turning of the kinetics and thermodynamics. The target of interest is a biomimedic heme system allowing for a detailed mechanistic study of the formation of the oxidation states of heme, of particular interest the highly reactive Fe(IV)=O species. The bidirectional model is prepared using a hangman porphyrin with an axially coordinated to the metal center, and the electron transfer event is triggered by excitation of the porphyrin. The synthesis of this motif is discussed as well as initial studies into the binding of a coordinated electron acceptor to the metal center. In the future, the excited state of the acceptor will be used to trigger the electron transfer portion of the PCET event. To understand the signatures of different electron acceptors and binding to the metal center, a redox inactive zinc porphyrin is used as a model to allow for longer excited state lifetimes and well known transient signatures. Three diimide acceptors have been coordinated through a pyridine ring to the metal center of the porphyrin, and electron transfer was triggered both by excitation of the porphyrin and the acceptor. Lifetimes of the charge separated state were determined using picoseconds and nanosecond transient absorption. The acceptors are then coordinated to a symmetrical iron porphyrin in an attempt to understand the behavior of charge separation in the more complicated open d shell system. Spectroscopic data of both systems is shown.
Book Synopsis Unraveling the Mechanistic Details of Proton Coupled Electron Transfer (PCET) Using Model Systems by : Afua Nti
Download or read book Unraveling the Mechanistic Details of Proton Coupled Electron Transfer (PCET) Using Model Systems written by Afua Nti and published by . This book was released on 2012 with total page 210 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Cytochrome Oxidase by : Mårten Wikström
Download or read book Cytochrome Oxidase written by Mårten Wikström and published by . This book was released on 1981 with total page 216 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Proton-coupled Electron Transfer (PCET) Model Systems by : Ewuradjoa Gadzanku
Download or read book Proton-coupled Electron Transfer (PCET) Model Systems written by Ewuradjoa Gadzanku and published by . This book was released on 2013 with total page 84 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Proton-Coupled Electron Transfer by : Sebastiao Formosinho
Download or read book Proton-Coupled Electron Transfer written by Sebastiao Formosinho and published by Royal Society of Chemistry. This book was released on 2011-12-07 with total page 169 pages. Available in PDF, EPUB and Kindle. Book excerpt: Proton-coupled electron transfer (PCET) is emerging as an important new class of reactions and, over the past decade, great strides have been made in our understanding of them. PCET reactions are studied in many branches of chemistry and are omnipresent in biological processes. This book covers recent developments from both the theoretical and experimental points of view. It concentrates on the importance of PCET in biological systems and for bioenergetic conversion. The oxidation of water in Photosystem II to produce oxygen, and the reduction of protons to hydrogen by hydrogenase, for energy storage gets particular emphasis. Chemical reactivity is currently explained in terms of several scientific principles. One of them is the bond-breaking-bond-forming process and is conceptually based on potential energy surfaces. Another incorporates the role of Franck-Condon factors resulting from the overlap of vibrational wavefunctions. A third, the so-called solvent reorganization, involves solvent configuration around a charged species. PCET brings together such concepts and links them to quantum mechanical tunnelling of the electron particle. This book uses personal accounts of experimental examples to provide additional insight on this important topic. It starts by presenting a general overview of the main theoretical approaches and experimental applications. The chapters then go on to cover topics including: the application of the Marcus Cross Relation; the solvation of ionic systems; experimental approaches in biological redox systems; metal ion-coupled electron transfer, and electrochemical concerted proton-electron transfers.
Book Synopsis Towards New Model Systems for the Study of Proton-coupled Electron Transfer by : Jay Lee Yang
Download or read book Towards New Model Systems for the Study of Proton-coupled Electron Transfer written by Jay Lee Yang and published by . This book was released on 2009 with total page 46 pages. Available in PDF, EPUB and Kindle. Book excerpt: Two new model systems for the study of orthogonal proton-coupled electron transfer (PCET) have been developed. The first model system is based on Ru"(HzO)(tpy)(bpy) (tpy = 2,2';6',2"terpyridine, bpy = 2,2'-bipyridine) where methyl viologen (MV2 ) electron acceptors were appended to the ruthenium aqua complex through the bpy. Picosecond transient absorption measurements show that electron transfer from the excited state of the ruthenium complex to MV2+ occurs with [tau] -200 ps. Experiments performed in water and buffered solution at pH = 7 show no evidence of the loss of proton from the aqua ligand to the bulk solvent or to the phosphate buffer. A minor kinetic isotope effect for the rate of charge separation was found with kH/kD = 1.8 + 0.1 ps. Preliminary synthetic attempts of coupling the ET event to the PT event was accomplished by appending xanthene "Hangman" scaffolds to the 4' position of the tpy. The feasibility of modifying the xanthene scaffold to accommodate various hanging groups has been demonstrated. The second model system is based on Re'(CO)3(phen)(pyr) (phen = 1,10phenanthroline, pyr = pyridine) where tyrosine was appended to the rhenium complex through the axial pyr ligand. Unlike previous Re'(CO)3(bpy)(CN) (CN = cyanide) systems, substitution to the more rigid phen extended the lifetime of the excited state of the rhenium complex to 3.0 ls, which allowed PCET to occur from the tyrosine to the rhenium metal center and hydrogenbonded base in dichloromethane. This was inferred from substantial emission quenching of the rhenium-tyrosine complex through the titration of base (base = pyridine, imidazole, 2,4,6trimethylpyridine). Equilibrium constants measuring the extent of formation of the [rheniumtyrosine---base]+ species were found to correlate with the strength of the base based on aqueous pKa values.
Book Synopsis Spectroscopic Investigation of Photo-induced Proton-coupled Electron Transfer and Dexter Energy Transfer in Model Systems by : Elizabeth Renee Young
Download or read book Spectroscopic Investigation of Photo-induced Proton-coupled Electron Transfer and Dexter Energy Transfer in Model Systems written by Elizabeth Renee Young and published by . This book was released on 2009 with total page 266 pages. Available in PDF, EPUB and Kindle. Book excerpt: Spectroscopic investigations of systems designed to advance the mechanistic interrogation of photo-induced proton coupled electron transfer (PCET) and proton-coupled (through-bond) energy transfer (PCEnT) are presented. PCET is ubiquitous in Nature, where it is at the heart of bioenergy conversion and catalysis (Chapter I). Systems of relevance to mechanistic studies of PCET and PCEnT are the central tenet of this work. In uni-directional PCET, electron transfer (ET) occurs from an electron donor (De) to an electron acceptor (Ae) through a hydrogen bonded proton interface. The proton interface plays a vital role in mediating ET. Thus, the exact ionization configuration of the interface must be uncovered to fuIIy realize the influence of the interface. SpecificaIIy, does the interface exists in the non-ionized (i.e. amidine-carboxylic acid) or ionized (i.e. amidinium-carboxylate) form. Strategies to spectraIIy monitor the interface ionization state by extending electronic communication from a porphyrinic chromophore to its pendant amidinium functionality are pursued through examination of an alkynylamidinium Ni(II) porphyrin (Chapter II) and an amidinium appended Zn(II) purpurin (Chapter III). With the ionization state of the interface resolved, mechanistic studies of photo-induced PCET between an identical De and Ae pair juxtaposed by a non-ionized (amidine-carboxylic acid) and an ionized (amidinium-sulfonate) interface are undertaken to reveal that PCET occurring through an ionized interface is more strongly coupled to the surrounding solvent environment (Chapter IV). Work on this system is extended to a second solvent of similar dielectric constant to establish that molecular variation of the solvent environment impacts PCET, likely through its interaction with the proton interface (Chapter V). Two water-soluble amidinium-appended ferrocene moieties are presented as building blocks for aqueous bi-directional PCET in which PT occurs to the bulk and ET occurs along a covalently bound coordinate (Chapter VI). ET and through-bond EnT are described by the semiclassical nonradiative decay formalism, meaning both processes should be sensitive to an intervening proton network. For the first time, PCEnT is established using ferrocenyl-amidine moieties bound through an amidinecarboxylic acid interface to Ru(II) polypyridyl complexes (Chapter VII).
Book Synopsis The Development and Analysis of Model Systems to Probe Proton-Coupled Electron Transfer in Ribonucleotide Reductase Ia of E. Coli by : Bon Jun Koo
Download or read book The Development and Analysis of Model Systems to Probe Proton-Coupled Electron Transfer in Ribonucleotide Reductase Ia of E. Coli written by Bon Jun Koo and published by . This book was released on 2016 with total page pages. Available in PDF, EPUB and Kindle. Book excerpt: Proton-coupled electron transfer (PCET) combines proton transfer with electron transfer to bypass high-energy intermediates. The ribonucleotide reductase (RNR) family of enzymes catalyzes the conversion of ribonucleotides to deoxynucleotides using amino acid radicals. The enzyme contains an efficient PCET pathway that transfers an electron and proton over a 35 Å distance across two subunits, the longest PCET pathway known in biology. The enzyme func-tions with very high fidelity, performing >105 turnovers before radical loss.
Book Synopsis Modeling Proton-coupled Electron Transfer with Ferrocene Derivatives by : Claire Drolen
Download or read book Modeling Proton-coupled Electron Transfer with Ferrocene Derivatives written by Claire Drolen and published by . This book was released on 2015 with total page 124 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Regulation of Proton Coupled Electron Transfer from Amino Acids in Artificial Model Systems by : Martin Sjödin
Download or read book Regulation of Proton Coupled Electron Transfer from Amino Acids in Artificial Model Systems written by Martin Sjödin and published by . This book was released on 2004 with total page 65 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Atomistic Approaches in Modern Biology by : Markus Reiher
Download or read book Atomistic Approaches in Modern Biology written by Markus Reiher and published by Springer Science & Business Media. This book was released on 2007-01-08 with total page 368 pages. Available in PDF, EPUB and Kindle. Book excerpt: With contributions by numerous experts
Book Synopsis Atomic-Scale Modelling of Electrochemical Systems by : Marko M. Melander
Download or read book Atomic-Scale Modelling of Electrochemical Systems written by Marko M. Melander and published by John Wiley & Sons. This book was released on 2021-09-09 with total page 372 pages. Available in PDF, EPUB and Kindle. Book excerpt: Atomic-Scale Modelling of Electrochemical Systems A comprehensive overview of atomistic computational electrochemistry, discussing methods, implementation, and state-of-the-art applications in the field The first book to review state-of-the-art computational and theoretical methods for modelling, understanding, and predicting the properties of electrochemical interfaces. This book presents a detailed description of the current methods, their background, limitations, and use for addressing the electrochemical interface and reactions. It also highlights several applications in electrocatalysis and electrochemistry. Atomic-Scale Modelling of Electrochemical Systems discusses different ways of including the electrode potential in the computational setup and fixed potential calculations within the framework of grand canonical density functional theory. It examines classical and quantum mechanical models for the solid-liquid interface and formation of an electrochemical double-layer using molecular dynamics and/or continuum descriptions. A thermodynamic description of the interface and reactions taking place at the interface as a function of the electrode potential is provided, as are novel ways to describe rates of heterogeneous electron transfer, proton-coupled electron transfer, and other electrocatalytic reactions. The book also covers multiscale modelling, where atomic level information is used for predicting experimental observables to enable direct comparison with experiments, to rationalize experimental results, and to predict the following electrochemical performance. Uniquely explains how to understand, predict, and optimize the properties and reactivity of electrochemical interfaces starting from the atomic scale Uses an engaging “tutorial style” presentation, highlighting a solid physicochemical background, computational implementation, and applications for different methods, including merits and limitations Bridges the gap between experimental electrochemistry and computational atomistic modelling Written by a team of experts within the field of computational electrochemistry and the wider computational condensed matter community, this book serves as an introduction to the subject for readers entering the field of atom-level electrochemical modeling, while also serving as an invaluable reference for advanced practitioners already working in the field.
Download or read book Molecular Biology of the Cell written by and published by . This book was released on 2002 with total page 0 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Biophysical and Structural Aspects of Bioenergetics by : Mårten Wikström
Download or read book Biophysical and Structural Aspects of Bioenergetics written by Mårten Wikström and published by Royal Society of Chemistry. This book was released on 2005 with total page 416 pages. Available in PDF, EPUB and Kindle. Book excerpt: This book provides a representative snapshot of the very latest key developments in this multidisciplinary subject.
Author :José A. Martinho Simões Publisher :Springer Science & Business Media ISBN 13 :9400900996 Total Pages :313 pages Book Rating :4.4/5 (9 download)
Book Synopsis Energetics of Organic Free Radicals by : José A. Martinho Simões
Download or read book Energetics of Organic Free Radicals written by José A. Martinho Simões and published by Springer Science & Business Media. This book was released on 2012-12-06 with total page 313 pages. Available in PDF, EPUB and Kindle. Book excerpt:
Book Synopsis Expressed Protein Ligation by : Miquel Vila-Perelló
Download or read book Expressed Protein Ligation written by Miquel Vila-Perelló and published by Humana. This book was released on 2020-03-07 with total page 0 pages. Available in PDF, EPUB and Kindle. Book excerpt: This book provides a comprehensive overview of Expressed Protein Ligation (EPL), detailing methods and protocols to generate site-specifically modified proteins. Chapters include an overview of the protein semi-synthesis field, as well as related areas that have contributed to the development of EPL such as protein splicing and peptide synthesis. Following the introductory chapters, the rest of the book guides readers through protocols to perform EPL reactions, methods to synthesize peptide thioesters and to perform peptide and protein ligations, label proteins inside living cells, protocols for the semi-synthesis of phorphorylated, glycosylated and ubiquitylated proteins, synthesis and assembly of assymetrically modified nucleosomes, use of ligation auxiliaries and synthesis of cyclic proteins, as well as novel desulfurization strategies and use of selective Cys side chain protection to obtain precisely modified proteins.Written in the highly successful Methods in Molecular Biology series format, chapters include introductions to their respective topics, lists of the necessary materials and reagents, step-by-step, readily reproducible laboratory protocols, and tips on troubleshooting and avoiding known pitfalls. Authoritative and cutting-edge, Expressed Protein Ligation: Methods and Protocols will ensure successful implementation of protein semi-synthesis methods to further study the structure and function of proteins.
Book Synopsis Biomolecular EPR Spectroscopy by : Wilfred Raymond Hagen
Download or read book Biomolecular EPR Spectroscopy written by Wilfred Raymond Hagen and published by CRC Press. This book was released on 2008-12-22 with total page 264 pages. Available in PDF, EPUB and Kindle. Book excerpt: Comprehensive, Up-to-Date Coverage of Spectroscopy Theory and its Applications to Biological SystemsAlthough a multitude of books have been published about spectroscopy, most of them only occasionally refer to biological systems and the specific problems of biomolecular EPR (bioEPR). Biomolecular EPR Spectroscopy provides a practical introduction t
