Metals in biology: applications of high-resolution EPR to metalloenzymes (New York, 2010). - ОГЛАВЛЕНИЕ / CONTENTS
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ОбложкаMetals in biology: applications of high-resolution EPR to metalloenzymes / eds.: G.Hanson, L.Berliner. - New York: Springer, 2010. - XIX,419 p.: ill. - (Biological magnetic resonance; vol.29). - Bibliogr. at the end of the chapters. - Ind.: p.411-419. - ISBN 978-1-4419-1138-4; ISSN 0192-6020
Шифр: (И/Е0-М61) 02
 

Место хранения: 02 | Отделение ГПНТБ СО РАН | Новосибирск

Оглавление / Contents
 
Preface ........................................................ ix
List of Color Figures and Website Materials ................... xix

Chapter 1. Introduction
   John R. Pilbrow
1  Iron-Sulfur Cluster-Containing Proteins ...................... 2
2  Molybdenum Enzymes ........................................... 3
3  Manganese-Containing Enzymes ................................. 5
4  Novel Melalloenzymes and Metalloproteins ..................... 5
5  Conclusions .................................................. 6

                  IRON-SULFUR-CONTAINING PROTEINS

Chapter 2. Electron Magnetic Resonance of Iron-Sulfur Proteins
in Electron-Transfer Chains: Resolving Complexity
   Richard Cammack and Fraser MacMillan
1  Introduction ................................................ 12
   1.1  Problems of Complex Electron-Transfer Systems .......... 13
2  Iron-Sulfur Proteins ........................................ 14
   2.1  Types of Clusters ...................................... 16
3  Information from Advanced EMR ............................... 17
   3.1  Relaxation Rates ....................................... 18
   3.2  Identification of Cluster Ligands ...................... 18
   3.3  Interactions with Protons and Paramagnets .............. 18
   3.4  Further Structural Information ......................... 19
   3.5  Orientation-Selective ENDOR and ESEEM .................. 19
   3.6  Studies of Intact Membrane-Bound Complexes ............. 20
   3.7  Methods of Isolating Spectra of Individual Components .. 21
   3.8  Results from l4N ESEEM ................................. 23
4  Selected Examples from Electron-Transport Chains ............ 27
   4.1  Xanthine Dehydrogenase/Oxidase as a Model .............. 27
   4.2  Mitochondria and Aerobic Bacteria ...................... 29
   4.3  Complex I (NADH:Ubiquinone Reductase) .................. 29
   4.4  Complex II (Succinate:Quinone Reductase) and
        Quinol:Fumarate Reductase .............................. 30
   4.5  Complex III ............................................ 32
   4.6  Microbial Anaerobic Respiration ........................ 33
5  Conclusions ................................................. 35

Chapter 3. Catalysis and Gene Regulation
   Helmut Beinert .............................................. 45


Chapter 4. Iron-Sulfur Clusters in "Radical SAM" Enzymes:
Spectroscopy and Coordination
   Serge Gambarelli1, Etienne Mulliez2, and Marc Fontecave
1  Introduction ................................................ 53
2  "Radical SAM" Iron-Sulfur Enzymes: An Example of
   a Low-Molecular-Weight Ligand to a [4Fe-4S] Cluster ......... 54
   2.1  The Pyruvate Formate Lyase System ...................... 57
   2.2  Lysine 2,3-Aminomutase ................................. 58
   2.3  Anaerobic Ribonucleotide Reductase ..................... 58
3  Detection of Hyperfine Coupling Interactions
   in Metalloproteins .......................................... 60
   3.1  ENDOR: Principles and General Considerations ........... 62
   3.2  ESEEM and HYSCORE ...................................... 64
4  Analysis of Ligand Hyperfine Coupling Interactions .......... 66
5  Applications to Metalloproteins ............................. 69
   5.1  Pyruvate Formate Lyase-Activating Enzyme (PFL-AE) ...... 69
   5.2  Lysine 2,3-Aminomutase (LAM) ........................... 72
   5.3  Anaerobic Ribonucleotide Reductase Activating Enzyme
        (aRNR-AE) .............................................. 73
6  Conclusion .................................................. 75

                 MONONUCLEAR MOLYBDENUM ENZYMES

Chapter 5. EPR Studies of Xanthine Oxidoreductase and Other
Molybdenum-Containing Hydroxylases
   Russ Hille
1  Introduction ................................................ 91
2  Historical Context .......................................... 91
3  The Active Site Structure of Xanthine Oxidoreductase ........ 93
4  Isotopic Substitution Studies .............................. 106
5  Magnetic Interactions Between Centers in Xanthine
   Oxidoreductase ............................................. 111
6  Concluding Comments ........................................ 114

Chapter 6. High-Resolution EPR Spectroscopy of Mo Enzymes.
Sulfite Oxidases: Structural and Functional Implications
   John H. Enemark, A.V. Astashkin, and A.M. Raitsimring
1  Introduction and Structures from X-Ray Crystallography ..... 122
2  Earlier cw EPR Investigations .............................. 125
3  Frequencies Observed in Pulsed EPR for a System of
   Electron Spin S = 1/2 and Arbitrary Nuclear Spin
   in Weak Interaction Limit .................................. 127
4  Pulsed EPR Techniques Used in This Work .................... 133
   4.1  ENDOR ................................................. 133
   4.2  ESEEM Techniques ...................................... 134
5  General Problems in Extraction of Structural Parameters
   from Magnetic Resonance Parameters ......................... 138
6  Sample Preparation and Instrumentation ..................... 139
7  High-Resolution Pulsed EPR Spectra, Magnetic Resonance
   Parameters, and Structural Implications for Various
   Forms of SO ................................................ 140
   7.1  Exchangeable Protons: Similarities and Differences
   in SOs from Different Organisms ............................ 140
   7.2  Groups Blocking Water Access to Mo(V) ................. 148
   7.3  Nonexchangeable Protons ............................... 151
   7.4  Exchangeable Oxygen Ligands ........................... 154
8  Biological Implications .................................... 159
9  Conclusion ................................................. 162
   Note Added in Proof ........................................ 162

Chapter 7. Dimethylsulfoxide (DMSO) Reductase, a Member of
the DMSO Reductase Family of Molybdenum Enzymes
   Graeme R. Hanson and Ian Lane
1  Introduction ............................................... 169
2  EPR Studies of Mo(V) Species ............................... 171
3  EPR Studies of DMSO Reductase .............................. 172
   3.1  Respiratory DMSO Reductase ............................ 173
   3.2  Periplasmic DMSO Reductase ............................ 173
   3.3  Catalytic Mechanism ................................... 188
4  Conclusions ................................................ 193

                  MANGANESE-CONTAINING ENZYMES

Chapter 8. The Manganese-Calcium Cluster of the Oxygen-
Evolving System: Synthetic Models, EPR Studies, and
Electronic Structure Calculations
   Marcin Brynda and R. David Britt
1  Introduction ............................................... 203
2  Theoretical Background for the Polynuclear Manganese
   Clusters ................................................... 205
   2.1  Introduction to the Spin Physics of Exchange-
        Coupled Manganese Complexes ........................... 205
   2.2  EPR Theory for Exchange Coupled Systems ............... 209
   2.3  Computational Methods for Magnetically Coupled
        Homonuclear Metal Clusters ............................ 218
3  Synthetic Models for Manganese Cluster of the OEC .......... 222
   3.1  Current Structural Proposals for the Pentanuclear
        Mn4Ca Cluster of the OEC ............................. 222
   3.2  EPR Characteristics of the Manganese Cluster of
        the OEC ............................................... 225
   3.3  Synthetic Models ...................................... 228
4  Computational Studies of the OEC ........................... 248
   4.1  Calculations on the Mechanistic Aspects of the
        Water Oxidation with DFT .............................. 248
   4.2  Mixed Molecular Mechanics/Quantum Mechanics Studies
        of Water Oxidation .................................... 252
5  Conclusions and Prospectives ............................... 253
   Appendix ................................................... 255

Chapter 9. Manganese Metalloproteins
   Sarah J. Smith, Kieran S. Hadler, Gerhard Schenk,
   Graeme R. Hanson, and Nataša Mitić
1  Introduction ............................................... 273
2  Manganese Catalases ........................................ 276
   2.1  Biochemical and Structural Characterization ........... 276
   2.2  Spectroscopic Characterization ........................ 278
   2.3  Mechanistic Implications .............................. 284
3  Ribonucleotide Reductase ................................... 285
   3.1  Biochemical and Structural Characterization ........... 285
   3.2  Spectroscopic Characterization ........................ 287
   3.3  Mechanistic implications .............................. 294
4  Class lb Ribonucleotide Reductases ......................... 295
   4.1  Biochemical and Structural Characterization ........... 295
   4.2  Spectroscopic Characterization ........................ 296
   4.3  Mechanistic Implications .............................. 299
5  Manganese-Iron Oxygenases .................................. 299
   5.1  Biochemical and Structural Characterization ........... 299
   5.2  Spectroscopic Characterization ........................ 301
   5.3  Mechanistic Implications .............................. 303
6  SoxB ....................................................... 304
   6.1  Biochemical and Structural Characterization ........... 304
   6.2  Spectroscopic Characterization ........................ 305
   6.3  Mechanistic Implications .............................. 306
7  Bacteriophage λ Protein Phosphatase ........................ 306
   7.1  Biochemical and Structural Characterization ........... 306
   7.2  Spectroscopic Characterization ........................ 307
   7.3  Mechanistic Implications .............................. 309
8  Purple Acid Phosphatase .................................... 310
   8.1  Biochemical and Structural Characterization ........... 310
   8.2  Spectroscopic Characterization ........................ 310
   8.3  Mechanistic Implications .............................. 312
9  Phosphotricsterase ......................................... 312
   9.1  Biochemical and Structural Characterization ........... 312
   9.2  Spectroscopic Characterization ........................ 313
   9.3  Mechanistic Implications .............................. 314
10 Arginase ................................................... 317
   10.1 Biochemical and Structural Characterization ........... 317
   10.2 Spectroscopic Characterization ........................ 317
   10.3 Mechanistic Implications .............................. 322
11 Methionyl Aminopeptidase ................................... 324
   11.1 Biochemical and Structural Characterization ........... 324
   11.2 Spectroscopic Characterization ........................ 325
   11.3 Mechanistic Implications .............................. 327

            NOVEL METALLOENZYMES AND METALLOPROTEINS

Chapter 10. EPR of Cobalt-Substituted Zinc Enzymes
   Brian Bennett
1  Introduction ............................................... 345
2  Review of Cobalt-Substituted Enzymes ....................... 346
3  Methods of Co(II) Insertion ................................ 348
4  EPR Experimental Techniques and Considerations ............. 350
5  Spectral Interpretation .................................... 356
6  Spectral Interpretation: A Case Study ...................... 364
7  Complementary Techniques ................................... 365
8  Conclusions ................................................ 366

Chapter 11. Hyperfine and Quadrupolar Interactions in
Vanadyl Proteins and Model Complexes: Theory and Experiment
   Sarah С. Larsen and N. Dennis Chasteen
1  Introduction ............................................... 372
   1.1  Coordination Chemistry of VO2+ ........................ 372
   1.2  EPR Properties ........................................ 373
   1.3  The Additivity Relationship for Predicting Ligand
        Environments .......................................... 374
   1.4  The Ground State and Ligand Hyperfine Couplings ....... 374
2  ENDOR and ESEEM of Vanadyl Model Complexes ................. 376
   2.1  14N Hyperfine and Quadrupole Coupling Constants ....... 376
   2.2  1H and l7O Coupling Constants ......................... 379
   2.3  31P Hyperfine Coupling Constants ...................... 380
   2.4  51V Nuclear Quadrupole Coupling Constants ............. 380
3  Density Functional Theory Calculations of EPR
   Parameters in Vanadyl Model Complexes ...................... 381
   3.1  Overview of DFT Methods for Calculations of EPR
        Parameters ............................................ 381
   3.2  DFT Calculations of Vanadium EPR Parameters ........... 383
   3.3  DFT Calculations of Ligand Hyperfine and Quadrupole
        Coupling Constants .................................... 387
   3.4  Outlook ............................................... 390
4  Select Protein Studies ..................................... 391
   4.1  Pyruvate Kinase ....................................... 391
   4.2  S-Adcnosylmcthionine Synthetase ....................... 393
   4.3  Imidazole Glycerol Phosphate Dehydratase .............. 394
   4.4  ATP Synthase .......................................... 394
   4.5  D-Xylose Isomerase .................................... 395
   4.6  Transferrins .......................................... 397
   4.7  Ferritin .............................................. 398
5  Tissues .................................................... 399
   5.1  Kidney and Liver ...................................... 399
   5.2  Bone .................................................. 401
6  Conclusions ................................................ 402

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