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The Coordination Chemistry of Metalloenzymes : The Role of Metals in Reactions Involving Water, Dioxygen and Related Species Proceedings of the NATO Advanced Study Institute held at San Miniato, Pisa, Italy, May 28 - June 8, 1982

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概要 Assembling a program in bioinorganic chemistry that is scientifi cally relevant, well defined, and self-consistent is not an easy task. In this attempt we decided to consider zinc enzymes, copper oxid...ases, cytochromes and cytochrome oxidase. The choice is in part due to the great attention that the current specialized literature devotes to these topics, which are now debated among chemists, biochemists, biophysicists, etc .. We believe that hydration reactions, hydrolytic and oxidative processes have much in common from the point of view of the reaction mechanisms, the comprehension of which represents a frontier of science. For these reasons these topics have been the subject of the NATO-ASI held at San Miniato, Pisa, Italy, from May 28 to June 8, 1982. We hope we can transfer here the main conclusions of what (we believe) was a very stimulating scientific meeting. We would like to thank the local saving bank, Cassa di Risparmio di San Miniato, for helping in many ways. The financial contribution from the European Research Office of the US Army, and from the Bruker Spectrospin s.r.l., Italy, is also acknowledged. The National Science Foundation of the United States has provided a travel grant to one of the participants from the U.S.A. We are grateful to the NATO Scientific Affairs Division which provided a grant to finance this Institute.続きを見る
目次 I: The Coordination Properties of the Active Site of Zinc Enzymes
1. Introduction
2. The Residues Coordinated at the Zinc Ion
3. The Acid-Base Properties of Coordinated Water
4. The Electronic Spectra of Cobalt (II) Derivatives
5. The Water 1H NMR Studies
6. The Implications on the Catalytic Mechanism
II: Coordinated Solvent Molecules in Metalloenzymes and Proteins Studied Using NMRD
1. Introduction
2. The 'Fluoromet' Mechanism
3. Fe3+ - Transferrin
4. Cu2+ - and V02+ - Transferrin
5. Co2+ - Carbonic Anhydrase
6. Alcohol Dehydrogenase
7. Mn2+ - Carboxypeptidase A
8. Conclusions
III: 113Cd Nuclear Magnetic Resonance Studies of Zinc Metalloproteins
1. Introduction
2. Chemical Shifts
3. Sensitivity
4. Information Content
5. Concluding Remarks
IV: Carbonic Anhydrase: Structure, Kinetics, and Mechanism
1. Introduction
2. Structure
3. Kinetics
4. Mechanism
V: Metal Ion Promoted Hydrolysis of Nucleoside 5'-Triphosphates
1. Introduction
2. Results and Discussion
VI: Models of Metalloenzymes: Carboxypeptidase A
1. Introduction
2. Metal Ion Catalyzed Hydrolysis of Amides and Esters
3. Results and Discussion
4. Cu2+ Mediated Amide Hydrolysis
5. Conclusions
VII: Spectroscopic Studies on Cobalt(II) Carboxypeptidase A
VIII: Coordination Properties and Mechanistic Aspects of Liver Alcohol Dehydrogenase
1. Introduction
2. Coordination Chemistry of Metallo Alcohol Dehydrogenases
3. Mechanistic Aspects
IX: Metal-Directed Affinity Labelling and Promoted Alkylation of a Thiol Liganded to the Catalytic Metal Ion in Liver Alcohol Dehydrogenase
1. Introduction
2. Experimental
3. Results and Discussion
X: Ligand Sphere Transitions: A New Concept in Zinc-Enzyme Catalysis
1. Introduction
2. Experimental Background
3. The Proposed Model Concept
XI: Molecular Mechamisms of the Superoxide Dismutase Activity of the Cuprozinc Protein of Eucaryotic Cells (CuZn Superoxide Dismutase)
1. Molecular Properties of the Protein
2. General Mechanism of the Superoxide Dismutation by the Copper of the Protein
3. Inactivation of the Enzyme
4. Inhibition of the Enzyme
5. Role of the Zinc
XII: A Comment on Anion Binding to Superoxide Dismutase
XIII: Kinetic and Magnetic Resonance Studies on Amine Oxidases
1. Introduction
2. Studies on the Copper Cofactor
3. Mechanistic Studies
XIV: Metal Coordination and Mechanism of Blue Copper Containing Oxidases
1. Introduction
2. Chemical Composition and Reactions Catalyzed
3. Spectroscopic Data
4. Oxidation-Reduction Properties
5. The Catalytic Mechanism
XV: Metal Replacement Studies of Chinese Laccase
1. Introduction
2. Metal-Replacement Studies of Small Blue Proteins
3. The Removal and Replacement of Copper from Chinese Laccase
4. The Preparation of a Mixed-Metal Hybrid of Laccase
XVI: Reactions of Rhus Vernicifera Laccase with Azide and Fluoride, Formation of a 'Half-Met-N3 -Type' Binding
1. Reactions with N3- as Studied by EPR
2. Reactions with N3- in the Presence of Redox Reagents
3. Half-Met-N3-Type Binding in Laccase
4. Reactions with Fluoride
5. Temperature Effects
XVII: Structural Magnetic Correlations in Exchange Coupled Systems
1. Spin Hamiltonian Approach to Exchange Coupling
2. Molecular Orbital Approach to Exchange Coupling
XVIII: Structural and Magnetic Investigations on Model CU4O4 Cubane-Like Clusters
1. Introduction
2. Structural Description
3. Magnetic Properties and Structural Data
4. Extension of the Correlations Between Magnetism and Structures
5. Example
XIX: Neurospora Tyrosinase: Intrinsic and Extrinsic Fluorescence
1. Introduction
2. Intrinsic Fluorescence
3. Extrinsic Fluorescence
XX: Comparison of Two Fungal Tyrosinases
1. Introduction
2. Molecular Properties
3. Properties of the Copper Site
4. Identification of Endogenous Ligands
5. Inhibition by Anions
XXI: Activation of Molecular Oxygen
1. Introduction
2. Autoxidation Reactions
3. Wacker Oxidations
4. Oxidations by Metal Bound 02
5. Oxidations by Products Derived from Metal-O2 Species
6. Oxygen Atom Transfer Reactions
7. Conclusion
XXII: Mössbauer Studies on Putidamonooxin - A New Type of [2Fe-2S] Containing Oxygenase Component with a Mononuclear Non-Heme Iron Ion as Cofactor
1. Introduction
2. Mössbauer Spectroscopic Investigation
3. Conclusion
XXIII: The Enzyme-Substrate Interaction in the Catechol Dioxygenases
XXIV: Ferric Nitrilotriacetate: An Active Center Analogue of Pyrocatechase
XXV: Stereoselective Peroxidatic Activity of Iron(III) Complex Ions Supported on Polypeptides
XXVI: NMR Studies of Cytochromes
1. Introduction
2. Class II Cytochromes c
3. Low Spin Cytochromes
4. Electron Transfer Mechanisms
XXVII: The Structure of the Metal Centers in Cytochrome c Oxidase
1. Introduction
2. The Metal Centers
3. Summary
XXVIII: Models of Metalloenzymes: Peroxidase and Cytochrome P-450
1. Introduction
2. Model Systems
XXIX: Coordination Chemistry of Cytochrome P-450 and Herne Models
1. Introduction: Occurrence and Function of Cytochrome P450-Dependent Monooxygenases
2. The Catalytic Cycle of Cytochrome P450
3. Cytochrome P450-Iron Comlexes Formed by Direct Interaction with Organic Compounds
4. Cytochrome P450-Iron-Metabolite Complexes
5. Conclusion: The Unique Richness of Cytochrome P450 Coordination Chemistry
XXX: Mössbauer Studies of Synthetic Analogues for the Active Site in Cytochromes P450
1. Introduction
2. Preparation of the Compounds
3. X-ray Structures
4. Mössbauer Studies
5. Molecular Orbital Calculations and ?EQ- Interpretation
XXXI: Magnetic Circular Dichroism Spectroscopy as a Probe of Ferric Cytochrome P-450 and its Ligand Complexes
1. Introduction
2. Materials and Methods
3. Results and Discussion
4. Conclusion.
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登録日 2020.06.27
更新日 2020.06.28