Reviews in mineralogy and geochemistry; vol.73 (Chantilly; Saint Louis, 2011). - ОГЛАВЛЕНИЕ / CONTENTS
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ОбложкаSulfur in magmas and melts: its importance for natural and technical processes / ed. by H.Behrens, J.D.Webster. - Chantilly: Mineralogical Society of America; Saint Louis: Geochemical Society, 2011. - xiii, 578 p.: ill., map. - (Reviews in mineralogy and geochemistry; vol.73). - Incl. bibl. ref. - ISBN 978-0-939950-87-4; ISSN 1529-6466
 

Оглавление / Contents
 
1  Studies of Sulfur in Melts - Motivations and Overview
   Harald Behrens, James D. Webster
   INTRODUCTION ................................................. 1
      Background ................................................ 1
      The behavior and importance of sulfur in melts ............ 2
   REVIEW CHAPTERS IN THIS VOLUME ............................... 2
   REMAINING ISSUES AND CONSIDERATIONS FOR FUTURE RESEARCH ...... 6
   ACKNOWLEDGMENTS .............................................. 7
   REFERENCES ................................................... 8
   
2  Analytical Methods for Sulfur Determination in Glasses,
   Rocks, Minerals and Fluid Inclusions
      Edward M. Ripley, Chusi Li, Craig H. Moore Erika 
      R. Elswick, J. Barry Maynard, Rick L. Paul Paul 
      Sylvester, Jun Hun Seo, Nobomichi Shimizu
   INTRODUCTION ................................................. 9
   ANALYTICAL TECHNIQUES ....................................... 10
      Total sulfur concentration in minerals, rocks and
      glasses using elemental analyzer - infrared absorption
      technology ............................................... 10
      Total sulfur concentration in minerals, rocks and 
      glasses using elemental analyzer - mass spectrometer
      technology ............................................... 11
      Total sulfur concentration of minerals, rocks and
      glasses using X-ray fluorescence ......................... 13
      "Kiba" method for the determination of sulfur
      concentration in whole rocks and glasses ................. 15
      Nuclear methods (activation analysis) for the
      determination of sulfur concentration in minerals, 
      rocks and glasses ........................................ 16
      Sulfur analysis of minerals and glasses using the
      electron microprobe ...................................... 19
      Analyses of the sulfur concentration of minerals and
      glasses by secondary ion mass spectrometry (SIMS) ........ 20
      Analyses of the sulfur concentration of minerals and
      glasses by laser ablation inductively coupled plasma
      mass spectrometry (LA-ICP-MS) ............................ 22
      Determination of the sulfur concentration in fluid
      inclusions by LA-ICP-MS .................................. 31
   SUMMARY ..................................................... 32
   ACKNOWLEDGMENTS ............................................. 35
   REFERENCES .................................................. 35
   
3  Spectroscopic Studies on Sulfur Speciation in Synthetic
   and Natural Glasses
      Max Wilke, Kevin Klimm, Simon C. Kohn
   INTRODUCTION ................................................ 41
   X-RAY EMISSION AND ABSORPTION SPECTROSCOPY .................. 42
      S Kα X-ray emission ...................................... 42
      Determination of the S oxidation state using EPMA ........ 45
      X-ray excited high-resolution X-ray emission
      spectroscopy ............................................. 46
      X-ray absorption spectroscopy ............................ 46
      Determination of S oxidation state from XANES ............ 54
      Beam damage during Analysis by EPMA and XANES ............ 55
      Sulfur redox equilibrium determined in glasses by 
      λ(S Kα) and XANES ........................................ 57
   NUCLEAR MAGNETIC RESONANCE .................................. 60
      33S NMR of solid model compounds ......................... 61
      33S NMR of glasses ....................................... 64
   RAMAN AND IR SPECTROSCOPY ................................... 66
      Raman spectroscopy of sulfur model compounds ............. 66
      Experimental details for Raman spectroscopy on glasses ... 67
      Raman spectroscopy on sulfur in glasses .................. 69
      Beam damage by Raman Spectroscopy ........................ 71
      Determination of the oxidation state using Raman
      spectroscopy ............................................. 71
   SUMMARY AND OUTLOOK ......................................... 72
   ACKNOWLEDGEMENTS ............................................ 73
   REFERENCES .................................................. 73
   
4  Diffusion and Redox Reactions of Sulfur in Silicate
   Melts
      Harald Behrens, Jan Stelling
   INTRODUCTION ................................................ 79
   SULFUR DIFFUSION STUDIES .................................... 80
      Silica glass ............................................. 82
      Simple silicate glasses .................................. 82
      Borosilicate glasses ..................................... 89
      Aluminosilicate melts relevant to magmatic systems ....... 90
   COMPARISON TO DIFFUSION OF OTHER VOLATILES .................. 92
   EFFECT OF REDOX STATE ON SULFUR DIFFUSION ................... 95
   SULFIDE/SULFATE INTERDIFFUSION AND REDOX REACTIONS OF 
   SULFUR ...................................................... 96
      Redox reactions in dry melts ............................. 96
      Redox reactions in hydrous melts ......................... 98
   SULFUR DIFFUSION VERSUS VISCOSITY ........................... 99
   SUMMARY AND OUTLOOK ........................................ 102
   ACKNOWLEDGMENTS ............................................ 103
   REFERENCES ................................................. 103
   
5  The Role of Sulfur Compounds in Coloring and Melting
   Kinetics of Industrial Glass
      Roberto Falcone, Stefano Ceola, Antonio Daneo,
      Stefano Maurina
   INTRODUCTION ............................................... 113
   SULFUR COMPOUNDS IN INDUSTRIAL GLASS PRODUCTION ............ 114
      Sodium sulfate .......................................... 114
      Slag .................................................... 114
      Glass cullet ............................................ 114
      Filter dust ............................................. 114
      Pyrite .................................................. 115
      Others .................................................. 115
   INDUSTRIAL GLASS PRODUCTION ................................ 115
      Batch preparation ....................................... 116
      Melting ................................................. 117
      Batch reactions ......................................... 117
      Fining .................................................. 121
      Forming and post-forming ................................ 123
   OPTICAL PROPERTIES AND COLORS OF INDUSTRIAL SLS CONTAINER
   GLASS ...................................................... 124
   COLOR GENERATION IN SLS GLASSES ............................ 126
   SULFUR SOLUBILITY, REDOX AND GLASS COLOR ................... 128
      The batch redox number .................................. 129
      Experimental melting .................................... 131
   CHEMICAL CHARACTERIZATION OF GLASS COLORS .................. 132
   BUBBLES IN SLS GLASSES ..................................... 134
      Incomplete fining ....................................... 135
      Redox ................................................... 135
      Reboil .................................................. 135
      Deposits ................................................ 136
   SUMMARY AND OUTLOOK ........................................ 138
   ACKNOWLEDGMENTS ............................................ 138
   REFERENCES ................................................. 139
   
6  О  Experimental Studies on Sulfur Solubility in Silicate
   Melts at Near-Atmospheric Pressure
   Linda Backnaes, Joachim Deubener
   INTRODUCTION ............................................... 143
   ANALYSIS METHODS FOR SULFUR CONTENT ........................ 144
   INDUSTRIAL MELTS ........................................... 144
      Effect of oxygen fugacity ............................... 144
      Effect of melt temperature .............................. 149
      Effect of melt composition .............................. 150
   SOLUBILITY OF SULFUR-BEARING WASTE IN MELTS ................ 155
   SOLUBILITY OF SULFUR IN NATURAL MELTS AND SYNTHETIC
   ANALOGS .................................................... 157
   SUMMARY AND OUTLOOK ........................................ 160
   ACKNOWLEDGMENTS ............................................ 161
   REFERENCES ................................................. 161
   
7  Modeling the Solubility of Sulfur in Magmas: A 50-Year
   Old Geochemical Challenge
      Don R. Baker, Roberto Moretti
   INTRODUCTION ............................................... 167
   THERMODYNAMICS AND MODELING SULFUR SOLUBILITY IN MAGMATIC
   SYSTEMS .................................................... 168
      A few necessary definitions and concepts ................ 168
      Modeling philosophies ................................... 169
      Thermodynamic basis for dissolution of sulfur in
      silicate melts .......................................... 171
   A BRIEF HISTORY OF EXPERIMENTS AND EMPIRICAL MODELS FOR
   SULFUR SOLUBILITY IN SILICATE MELTS ........................ 175
      Sulfur behavior in systems with only sulfur-rich gas 
      and silicate melts at 1 atm ............................. 175
   SULFIDE AND SULFATE SATURATION IN SILICATE MELTS ........... 178
      Sulfide saturation at 1 bar ............................. 178
      Sulfide and sulfate saturation at high-pressure with 
      or without the presence of a hydrous fluid .............. 182
   THERMODYNAMIC MODELS FOR THE BEHAVIOR OF SULFUR IN
   MAGMATIC SYSTEMS ........................................... 191
      Sulfur speciation in silicate melts ..................... 192
      The thermodynamic model of Moretti and Ottonello ........ 194
   GEOLOGICAL APPLICATIONS .................................... 203
   CONCLUSIONS ................................................ 208
   ACKNOWLEDGMENTS ............................................ 209
   REFERENCES ................................................. 209
   
8  The Sulfur Budget in Magmas: Evidence from Melt
   Inclusions, Submarine Glasses, and Volcanic Gas Emissions
      Paul J. Wallace, Marie Edmonds
   INTRODUCTION ............................................... 215
   SULFUR CONCENTRATIONS IN MAGMAS ............................ 216
   MAGMATIC DEGASSING OF SULFUR ............................... 221
      Degassing and vapor-melt partitioning ................... 221
      Degassing inferred from melt inclusions from mafic
      volcanoes ............................................... 223
      Magmatic vapor phase and volcanic gases ................. 226
      "Excess sulfur" or more accurately, "excess volatiles"
      problem ................................................. 229
      Magmatic sulfur and ore deposits ........................ 236
      Recycling of sulfur in subduction zones ................. 237
   ACKNOWLEDGMENTS ............................................ 239
   REFERENCES ................................................. 239
   
9  Distribution of Sulfur Between Melt and Fluid in 
   S-O-H-C-Cl-Bearing Magmatic Systems at Shallow Crustal
   Pressures and Temperatures
      James D. Webster, Roman E. Botcharnikov
   INTRODUCTION ............................................... 247
   BACKGROUND ................................................. 249
      Experimental background ................................. 250
   METHODS .................................................... 251
      Experimentation: advantages and challenges .............. 251
      Analytical: issues and challenges ....................... 256
   EXPERIMENTAL RESULTS ON SULFUR PARTITIONING BETWEEN FLUID
   AND SILICATE MELT .......................................... 258
      Felsic melts - S-H2O±CO2 ................................ 258
      Rhyodacitic melts - S-H2O-Cl ............................ 261
      Phonolitic melts - S-H2O-Cl ............................. 261
      Andesitic melts - S-H2O±CO2+B ........................... 265
      Basaltic melts - S-H2O±CO2-Cl ........................... 265
      Summary on S partitioning between fluids and rhyolitic
      to basaltic melts at crustal conditions ................. 269
   APPLICATION OF THE EXPERIMENTAL DATA TO PROCESSES OF
   FLUID EXSOLUTION AND THE EVOLUTION OF MAGMA AND MAGMATIC
   FLUIDS ..................................................... 271
      Magmatic gas composition as an indicator of magma and
      volcanic degassing activity ............................. 272
      Volatile mixing relationships and the influence of S 
      on CO2, H2O, and Cl solubility in melt and new
      insights on vapor (fluid) saturation infelsic magmas .... 274
   SUGGESTIONS FOR FUTURE RESEARCH ............................ 276
   ACKNOWLEDGMENTS ............................................ 276
   REFERENCES ................................................. 276
   
10 Sulfur-bearing Magmatic Accessory Minerals
   Fleurice Parat, François Holtz, Martin J. Streck
   INTRODUCTION: THE OCCURRENCE OF MAGMATIC SULFUR-BEARING
   MINERALS ................................................... 285
      Magmatic sulfides ....................................... 286
      Magmatic sulfates and sulfate-bearing minerals .......... 291
   MINERAL STABILITY, PARAGENESES AND MINERAL/MELT
   PARTITIONING OF SULFUR ..................................... 295
      Transition from sulfide to sulfate stability fields in
      silicate melts .......................................... 295
      Stability range of sulfide phases in magmatic systems ... 296
      Sulfates and sulfate-bearing minerals ................... 302
   THE IMPORTANCE OF S-BEARING ACCESSORY MINERALS FOR
   DECIPHERING MAGMA RESERVOIR PROCESSES ...................... 306
   IN SITU SULFUR ISOTOPE IN S-BEARING MINERALS ............... 308
   CONCLUDING REMARKS ......................................... 309
   ACKNOWLEDGMENTS ............................................ 309
   REFERENCES ................................................. 309
   
11 Sulfur in Extraterrestrial Bodies and the Deep Earth
   Denton S. Ebel
   COSMOCHEMISTRY OF SULFUR ................................... 315
      Silicate melts and sulfur in primitive source
      materials ............................................... 315
      Sulfur content of the terrestrial planets ............... 318
   EXPERIMENTAL CONSTRAINTS ................................... 318
      Element partitioning .................................... 318
      Liquid silicate - liquid metal-sulfide .................. 320
      Solid metal - liquid metal-sulfide ...................... 321
      Sulfide saturation and immiscibility .................... 323
      Rheology: wetting and deformation ....................... 324
   PLANETARY INTERIORS ........................................ 324
      Iron meteorites ......................................... 324
      Sulfur in core fractionation ............................ 325
      Earth core formation .................................... 326
      Sulfur and lithophile element partitioning .............. 328
   MAGMAS OF OTHER SOLAR SYSTEM BODIES ........................ 328
   CONCLUSIONS ................................................ 330
   ACKNOWLEDGMENTS ............................................ 330
   REFERENCES ................................................. 330
   
12 Fining of Glass Melts
      Hayo Müller-Simon
   INTRODUCTION ............................................... 337
   AGENTS USED FOR CHEMICAL FINING ............................ 339
   LABORATORY EXPERIMENTS ON SULFUR CHEMISTRY ................. 341
      Equilibrium experiments ................................. 341
      Melting experiments ..................................... 344
   MONITORING OF THE REACTION PARAMETERS ...................... 348
      Oxidation state of iron ................................. 348
      Oxygen sensors .......................................... 349
      Redox number concepts ................................... 350
      Interdependence of redox related measurements ........... 351
   MODELS OF INDUSTRIAL SULFUR FINING ......................... 352
      Solubility concept ...................................... 352
      Equilibrium concepts .................................... 352
      Dynamic equilibrium concepts ............................ 353
   INVESTIGATIONS UNDER INDUSTRIAL CONDITIONS ................. 355
   SUMMARY .................................................... 358
   ACKNOWLEDGMENT ............................................. 359
   REFERENCES ................................................. 359
   
13 Sulfur Degassing From Volcanoes: Source Conditions,
   Surveillance, Plume Chemistry and Earth System Impacts
      Clive Oppenheimer, Bruno Scaillet, Robert S. Martin
   INTRODUCTION ............................................... 363
      Geodynamics and the geochemical behavior of sulfur ...... 363
      Subduction zones ........................................ 364
      Ocean ridge environments ................................ 369
      Hot spots ............................................... 371
      Flood basalts and silicic parts of large igneous
      provinces ............................................... 372
   MEASURING VOLCANIC SULFUR EMISSIONS ........................ 373
      Direct sampling ......................................... 377
      In situ sensing ......................................... 377
      Ultraviolet spectroscopy ................................ 378
      Broad-band infrared spectroscopy ........................ 383
      Laser spectroscopy ...................................... 385
      Satellite remote sensing ................................ 385
   INTERPRETATION OF SULFUR-EMISSION DATA ..................... 386
      Proportions of sulfur species ........................... 386
      Sulfur fluxes ........................................... 387
      Sulfur isotopes ......................................... 388
   VOLCANIC SULFUR EMISSION TO THE ATMOSPHERE ................. 389
      Ice cores ............................................... 392
   ATMOSPHERIC AND CLIMATIC IMPACTS OF SULFUR DEGASSING ....... 394
      Chemical schemes relevant to volcanic sulfur
      emissions ............................................... 394
      Impacts of tropospheric sulfur emissions from
      volcanoes ............................................... 398
      The atmospheric and climatic impact of the 1991
      eruption of Mt. Pinatubo ................................ 399
      Requirements for a climate-forcing eruption ............. 404
   SUMMARY AND CONCLUSIONS .................................... 405
   ACKNOWLEDGMENTS ............................................ 406
   REFERENCES ................................................. 406
   
14 Sulfur Isotopes in Magmatic-Hydrothermal Systems, Melts,
   and Magmas
      Luigi Marini, Roberto Moretti, Marina Accornero
   INTRODUCTION ............................................... 423
   BASIC PRINCIPLES ........................................... 424
      Terminology of sulfur isotope systematics ............... 424
      δ33S and δ36S values .................................... 425
      Equilibrium fractionation factors ....................... 426
      Isotope geothermometry .................................. 430
   SULFUR ISOTOPIC COMPOSITION OF NATURAL SAMPLES ............. 430
      Mantle-derived materials and igneous rocks .............. 430
      Sulfide and sulfate minerals from magmatic,
      magmatic-hydrothermal and related ore deposits .......... 431
      Sulfur isotopes in magmatic and magmatic-hydrothermal
      systems ................................................. 434
   SULFUR STABLE ISOTOPES AND THE POTENTIAL FOR PROBING
   DEGASSING AND CRYSTALLIZATION PROCESSES AND SULFUR 
   SOURCES IN MAGMAS .......................................... 452
      Magmatic degassing and sulfur isotope fractionation ..... 453
      Separation of S-bearing liquids and/or solid phases ..... 454
      Parametric assessment ................................... 454
      Comparison of analytical S and δ34SΣS data from
      selected volcanic systems and theoretical models of
      degassing and separation of sulfides and anhydrite ...... 465
      Conclusions and future research ......................... 481
   ACKNOWLEDGMENTS ............................................ 482
   REFERENCES ................................................. 482
   
15 Interactions Between Metal and Slag Melts: Steel 
   Desulfurization
      Jean Lehmann, Michele Nadif
   INTRODUCTION ............................................... 493
   PARTITIONING OF SULFUR BETWEEN SLAG AND METAL MELTS ........ 494
      Sulfide capacity ........................................ 494
      Modeling ................................................ 495
      Desulfurization during secondary metallurgy 
      operations .............................................. 496
   METHODS OF DESULFURIZATION ................................. 499
      Evolution of S-content during liquid steel refining ..... 499
      Desulfurization of steel by steel-slag stirring ......... 501
      Slag formers additions .................................. 503
      Slag composition ........................................ 503
      Stirring conditions ..................................... 503
      Desulfurization of steel by lime powder injection ....... 506
   SUMMARY AND FUTURE WORK .................................... 507
   LIST OF SYMBOLS ............................................ 509
   REFERENCES ................................................. 510
   
16 The Role of Magmatic Sulfur in the Formation of Ore
   Deposits
      Adam C. Simon, Edward M. Ripley
   INTRODUCTION ............................................... 513
   GEOCHEMISTRY OF SULFUR IN MAGMATIC-HYDROTHERMAL SYSTEMS .... 514
      Sulfur basics ........................................... 514
      Behavior of sulfur in silicate melts .................... 516
   THE PARTITIONING OF METALS AND SULFUR AMONG MAGMATIC
   PHASES ..................................................... 519
      The partitioning of sulfur between silicate melt and
      H-O-S-Cl fluid(s) ....................................... 519
      Controls on the partitioning of ore metals among
      silicate melt and crystalline sulfides .................. 519
      The partitioning of ore metals among silicate melt, 
      sulfide liquid and sulfide crystals ..................... 523
      The partitioning of ore metals among silicate melt and 
      S-bearing aqueous fluid(s) .............................. 527
      The transport of ore metals in magmatic-hydrothermal 
      fluid(s) ................................................ 530
      The partitioning of ore metals between vapor and brine
      at temperatures below the water-saturated granite
      solidus ................................................. 539
   PORPHYRY-TYPE ORE DEPOSITS ................................. 540
      Porphyry basics ......................................... 540
      Tectonic setting and associated magma composition of
      porphyry deposits ....................................... 540
      Source of sulfur in porphyry environments ............... 541
      Source of ore fluids in porphyry environments ........... 542
      Constraints on the composition of porphyry-ore forming
      fluids .................................................. 543
      Harmonizing fluid transport data from nature and
      experiments ............................................. 546
      Oxidation state of causative magmas: the role of
      sulfide vs. sulfate ..................................... 546
      Causative magma sources: normal or enriched? ............ 549
      Deposition of metal-sulfides in the porphyry
      environment ............................................. 551
   Ni-Cu-(PGE) DEPOSITS ....................................... 552
      Characteristics and classification of magmatic 
      Cu-Ni-(PGE) deposits .................................... 552
      Resource and grade characteristics ...................... 553
      A general model for magmatic Ni-Cu ore genesis .......... 554
      Source magmas for Ni-Cu deposits ........................ 556
      Transport of sulfide melt ............................... 556
   PGE DEPOSITS IN LAYERED INTRUSIONS ......................... 557
      Characteristics and classification of PGE deposits ...... 557
      Models for the genesis of PGE deposits in layered 
      mafic intrusions ........................................ 559
      Source magmas for PGE deposits .......................... 563
   FUTURE RESEARCH: WHAT DO WE NEED? .......................... 563
   ACKNOWLEDGMENTS ............................................ 564
   REFERENCES ................................................. 564


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