Complexation reactions in aquatic systems: an analyt. approach
Gespeichert in:
| 1. Verfasser: | |
|---|---|
| Format: | Buch |
| Sprache: | Undetermined |
| Veröffentlicht: |
Chichester u. a.
Horwodd u. a.
1988
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| Ausgabe: | 1. publ. |
| Schriftenreihe: | Elis Horwood series in analytical chemistry
|
| Schlagworte: | |
| Online-Zugang: | Inhaltsverzeichnis |
| Beschreibung: | XXI, 692 S. Ill., graph. Darst. |
| ISBN: | 0853125570 0470208309 |
Internformat
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| 100 | 1 | |a Buffle, Jacques |e Verfasser |4 aut | |
| 245 | 1 | 0 | |a Complexation reactions in aquatic systems |b an analyt. approach |c J. Buffle |
| 250 | |a 1. publ. | ||
| 264 | 1 | |a Chichester u. a. |b Horwodd u. a. |c 1988 | |
| 300 | |a XXI, 692 S. |b Ill., graph. Darst. | ||
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Datensatz im Suchindex
| _version_ | 1804120278392897536 |
|---|---|
| adam_text | Titel: Complexation reactions in aquatic systems
Autor: Buffle, Jacques
Jahr: 1988
Table of Contents
Preface xi
Foreword xv
List of Symbols xvii
1 INTRODUCTION 1
1.1 Definitions 6
1.1.1 Chemical reactivity and speciation 6
1.1.2 Measurement of different forms of M in natural
media (labile and inert complexes) 7
1.1.3 Determination of complexing agent properties
and concentrations 9
1.2 Limitations of Current Models and Methods 10
1.3 Measuring the Reactivity of Environmental Components:
A New Perspective of Analytical Chemistry 11
2 THE COMPONENTS OF AQUATIC SYSTEMS AND THEIR
REACTIVITY 16
2.1 Classification of Water Components 16
2.1.1 Well-characterized compounds and homologous
compound groups 18
Contents
2.1.2 Complexing compounds 18
2.1.3 Dissolved components and suspended particles 22
2.1.4 Characterization of complicated mixtures by
distribution spectra 23
2.1.4.1 Size distributions 24
2.1.4.2 Analytical windows and average measured
parameters 31
2.1.4.3 Distribution of chemical properties at
equilibrium 32
2.1.4.4 Distribution of kinetic properties 35
2.2 Concentration of Organic and Inorganic Compounds 37
2.2.1 Organic compounds 37
2.2.2 Inorganic compounds 41
2.3 Basic Principles of Metal Reactivity in Water 47
2.3.1 Reactivity with suspended solid surfaces 48
2.3.2 Reactivity with dissolved inorganic ligands 52
2.3.2.1 Distribution of complexed forms in model water
systems 52
2.3.2.2 Distribution of elements between their various
oxidation states 57
2.3.2.3 Trace metal classification 59
2.3.3 Reactivity with polyfunctional complexing agents 60
2.3.3.1 Softness and hardness of metals and ligands 64
2.3.3.2 Stereochemical factors , 65
2.3.3.3 Hydration properties of macromolecules and
colloids 65
233.4 Polyelectrolyte properties 69
2.3.3.5 Mixed complexes and intramolecular bonds 69
2.3.3.6 Micellization and aggregate formation 71
2.4 Relation Between Reactivity and Availability of Metals in
Aquatic Systems 72
2.4.1 Reactivities of the different metal groups 72
2.4.2 Ecochemical role of the various groups of aquatic
complexing agents 75
2.4.3 Overall complexing ability of an aquatic system 77
2.4.4 Importance of kinetic factors 81
COMPOSITION AND ORIGIN OF NATURAL ORGANIC MATTER 90
3.1 Definitions and Classification 91
3.1.1 Principal types of NOM 91
3.1.2 The NOM of different aquatic systems 95
3.2 Oceanic Organic Matter 96
3.2.1 Production of NOM in pelagic zones 96
3.2.2 Spatial distribution of particulate and dissolved NOM 97
3.2.3 Evolution of marine NOM 100
Contents iii
3.2.4 Composition of marine NOM 103
3.2.4.1 Composition of living organisms 103
3.2.4.2 Particulate organic matter 105
3.2.4.3 Dissolved organic matter 107
3.3 Pedogenic Organic Matter 110
3.3.1 Origin and fractionation of soil organic matter (SOM) l Þ
3.3.2 Relationship between soil NOM (SOM) and aquatic
pedogenic NOM (POM) 112
3.3.3 Nature of soil NOM 113
3.3.4 NOM of rivers 118
3.4 Lake Organic Matter 120
3.4.1 Production of aquagenic NOM in freshwater 122
3.4.2 Distinctions between aquagenic (AOM) and pedogenic
(POM) NOM 122
3.4.2.1 C/N, C/O, C/H and C/S ratios 123
3.4.2.2 POC/TOC ratio 124
3.4.2.3 UV-absorption/DOC ratio 124
3.4.2.4 Isotopie ratios 126
3.4.3 Evolution of POM and AOM in lakes 127
3.4.4 Composition of lake NOM 132
3.5 Importance of Local Environments and Transition Zones 136
3.5.1 Coastal zones 137
3.5.2 Estuaries 139
3.5.3 Sediments 142
3.5.3.1 Sedimentation of undegraded cellular debris 142
3.5.3.2 Adsorption of NOM on inorganic particles 142
3.5.3.3 Benthic decomposition 143
3.5.3.4 Composition of sediment NOM 144
CHARACTERISTICS OF AQUATIC ORGANIC COMPOUNDS 146
4.1 Characterization and Fractionation of Major NOM Components 147
4.1.1 Characterization and determination methods 147
4.1.2 Fractionation of NOM 149
4.1.2.1 Separation by size 149
4.1.2.2 Separation on hydrophobic resins 151
4.1.2.3 Separation by ion-exchange 151
4.2 Nature of Aquatic Proteins and Peptides 152
4.3 Aquatic Polysaccharides 154
4.3.1 Origin 154
4.3.2 Composition 158
4.3.3 Properties 161
4.3.3.1 Size 161
4.3.3.2 Hydration 161
4.3.3.3 Viscosity 163
4.3.3.4 Charge 163
iv Contents
4.4 Composition of Refractory Organic Matter (ROM)
Originating from Soil 163
4.4.1 Overall composition 164
4.4.2 Specific Compounds 165
4.4.2.1 Carbohydrates 168
4.4.2.2 Fatty acids 168
4.4.2.3 Hydrocarbons 169
4.4.2.4 Nitrogen-containing compounds 170
4.4.2.5 Sulphur-containing compounds 171
4.4.2.6 Phosphorus-containing compounds 171
4.4.2.7 Aromatic compounds 172
4.5 Properties of Soil Refractory Organic Matter (ROM) 173
4.5.1 Structure 173
4.5.2 Size and molecular weight 177
4.5.2.1 Interpretation of data 177
4.5.2.2 Molecular weight 178
4.5.2.3 Size 178
4.5.2.4 Relationships between molecular weight and
composition 179
4.5.3 Hydration 183
4.5.4 Aggregation 184
4.6 Aquagenic Refractory Organic Matter 187
4.6.1 Properties of AROM 187
4.6.2 Structure and synthesis of marine LAROM 190
4.7 Sedimentary Humic and Fulvic Fractions 192
5 INTERPRETATION OF COMPLEXATION EQUILIBRIA 195
5.1 Introduction 195
5.1.1 Principal properties of natural complexants 195
5.1.2 Level of interpretation of complexation reactions 198
5.1.3 Symbols 200
5.2 Complexation by Simple Ligands 200
5.2.1 Principles and definitions 200
5.2.1.1 Equilibrium constants of complexes 200
5.2.1.2 Balance equations 201
5.2.1.3 Activity coefficients 202
5.2.2 Experimental determination of equilibrium constants 203
5.2.2.1 Definitions 203
5.2.2.2 General principle of determination 205
5.2.2.3 Cases where the ionic strength is constant 206
5.2.2.4 Example I, 1:1 complexes between major ions 207
5.2.2.5 Example II, formation of l.w complexes
between a minor cation and a major ligand 207
Contents
5.2.3 Theoretical calculation of complex distribution 209
5.2.3.1 Principles 209
5.2.3.2 Graphical representations 211
5.2.3.3 Limitations of thermodynamic modelling 216
5.3 Specific Reactions of a Single Ion or Compound with
Homologous Complexants 216
5.3.1 Principles and definitions 216
5.3.1.1 Internal and external variables 217
5.3.1.2 General formulation of the complexation
reaction 218
5.3.1.3 Influence of pH 219
5.3.1.4 Degree of site occupation; affinity spectra 220
5.3.2 Each site affinity is independent of è 224
5.3.2.1 Formation of 1:1 and 1:2 complexes with a
single type of site 225
5.3.2.2 Formation of 1:1 complexes with/ 1 228
5.3.3 Site affinity varies with è ; interpretation using a priori
theoretical models 236
5.3.3.1 General considerations 236
5.3.3.2 Purely electrostatic secondary interactions 238
— Principles 238
— Acid—base properties of metal oxides 245
— Acid—base properties of macromolecules 248
— Metal complexation by macromolecules 251
5.3.3.3 The complexant considered as a permeable
distinct (gel) phase 255
5.3.3.4 Interpretation by means of arbitrary isotherms
and affinity spectra 258
5.3.4 Direct determination of affinity spectra 266
5.3.4.1 Numerical resolution of Eq. (5.58) 266
5.3.4.2 Differential equilibrium functions 268
5.3.4.3 Relationships between theoretical representations
and experimentally measured variables for
heterogeneous complexants 272
5.4 Competition Reactions 277
5.4.1 Non-specific reactions; ion-exchange 279
5.4.1.1 Impenetrable colloidal particles 281
5.4.1.2 Flexible organic polyelectrolytes 282
5.4.2 Equilibrium quotients of competition reactions, and
retention capacity 284
5.4.3 Specific competition reactions on pure oxide surfaces 286
5.4.3.1 Principles 286
5.4.3.2 Cation complexation 288
5.4.3.3 Anion complexation 290
5.4.3.4 Formation of mixed surface complexes 292
vi Contents
5.4.4 Specific competition reactions with polyfunctional
complexants 292
5.4.4.1 Inorganic polyfunctional complexants 293
5.4.4.2 Multi-metal/multi-site competition in organic
polyfunctional gels 296
5.5 Choice of Interpretation Model 299
COMPLEXATION PROPERTIES OF HOMOLOGOUS
COMPLEXANTS AND CHOICE OF MEASURING METHODS 304
6.1 Organic Complexants 306
6.1.1 Fulvic and humic compounds 306
6.1.1.1 Physical properties 306
6.1.1.2 Acid—base properties 308
6.1.1.3 Complexing properties 314
6.1.2 Proteins and polysaccharides 322
6.1.3 Cell walls 326
6.1.3.1 Structure and physical properties 326
6.1.3.2 Complexing properties 329
6.2 Inorganic Complexants 330
6.2.1 Metal oxides and hydroxides 330
6.2.1.1 Structure and physical properties 330
6.2.1.2 Chemical properties 333
6.2.2 Other inorganic solids 338
6.3 Natural Solid-Solution Systems 340
6.3.1 NOM coating of particles 341
6.3.1.1 Adsorption energy 342
6.3.1.2 Influence of organic coating on particle
properties 346
6.3.2 Sediments 347
6.3.3 Soils 352
6.4 Kinetic Properties 354
6.4.1 Rate constants of chemical reactions 354
6.4.1.1 General principles 354
6.4.1.2 Metal complexation by fulvic compounds 356
6.4.1.3 Complexes with inorganic solids 358
6.4.1.4 Competitive reactions 358
6.4.2 Diffusion coefficients 359
6.4.3 Classification of complexants by kinetic properties 363
6.5 Complexation Measurements in Complete Aquatic Media:
Choice of Methods and Experimental Conditions 364
6.5.1 Strategy for complexation measurements 365
6.5.1.1 The various approaches 365
6.5.1.2 The various steps 367
Contents vii
6.5.2 Choice of reaction interpretation model (step V) 371
6.5.3 Choice of methods and experimental conditions 372
6.5.3.1 Equilibrium parameter measurements 373
6.5.3.2 Role of kinetic factors 380
7 EXPERIMENTAL DETERMINATION OF THE IN SITU
DISTRIBUTION OF CHEMICAL SPECIES 384
7.1 Sampling and Pretreatment 385
7.1.1 Contamination 385
7.1.2 Sample collection 387
7.1.3 Storage; adsorption on containers 391
7.1.4 Pretreatment 392
7.1.4.1 Preconcentration 392
7.1.4.2 Separation of particulate and dissolved
compounds 393
7.1.4.3 Separation of dissolved-compound groups 395
7.2 Distribution Schemes for Metals, based on Fractionation 395
7.2.1 Fractionation schemes for dissolved compounds 396
7.2.1.1 Single-criterion schemes based on size 396
7.2.1.2 Single-criterion schemes based on complex
lability 398
7.2.1.3 Chromatographie fractionation 402
7.2.1.4 Fractionation by decomposition 403
7.2.1.5 Multiple-criteria schemes 403
7.2.2 Fractionation scheme for non-living particles 405
7.2.2.1 Principles 405
7.2.2.2 Relationship between chemical fractionation
and thermodynamic models 407
7.2.2.3 Relationship between chemical fractionation
and biological uptake 411
7.2.3 Fractionation scheme for unicellular organisms 412
7.3 Distribution Schemes based on Combination of Direct
Measurements: Case of Fe and S in eu trophic lakes 415
7.3.1 Principles 415
7.3.2 Methodological scheme 418
7.3.2.1 Filtration (particle/colloid limit) 420
7 .3.2.2 Differential pulse polarography (colloid/labile
compounds limit) 421
7.3.3 Results 423
STUDY OF COMPLEXATION PROPERTIES BY POTENTIO-
METRIC METHODS 427
8.1 General Characteristics of Electrochemical Methods 427
viii Contents
8.2 Membrane Electrodes (ISEs) 433
8.2.1 Principles 437
8.2.2 Optimum conditions for direct measurement of {M} 439
8.2.2.1 Constancy of Eo 439
8.2.2.2 Interfacial equilibrium 441
8.2.2.3 Response time 443
8.2.3 Direct measurement of the degree of complexation 445
8.2.3.1 Calibration in non-complexing media 446
8.2.3.2 Measurements in complexing media 447
8.2.3.3 Practical conditions for complexation
measurements 449
8.2.3.4 Optimal measurement conditions 455
8.3 Amalgam Electrodes 456
8.3.1 Preparation 456
8.3.2 Measurements in non-complexing media 457
8.3.2.1 Principles 457
8.3.2.2 Sensitivity limits 459
8.3.3 Application to complexation measurements 463
8.3.3.1 Examples 463
8.3.3.2 Influence of oxygen 465
STUDY OF COMPLEXATION PROPERTIES BY VOLTAM-
METRIC METHODS 467
9.1 Factors Influencing Sensitivity in Non-complexing Media 468
9.1.1 Principles 468
9.1.1.1 Faradaic current—potential—time relationships 469
9.1.1.2 Interpretation of current—potential curves in
terms of concentration gradients 475
9.1.2 Principal voltammetric methods 477
9.1.2.1 Electronic factors: conditioning and
measurement times 480
9.1.2.2 Mechanical and geometric factors 482
9.1.2.3 Chemical preconcentrati on on or into the
electrode 486
9.1.3 Applications to natural waters 489
9.2 General Phenomena Influencing Complexation Measurements 490
9.2.1 Nature of the reactions studied 490
9.2.2 Nature of secondary phenomena 492
9.2.2.1 Influence of electric field 493
9.2.2.2 Adsorption at the interface 495
9.2.2.3 Influence of compound fluxes at the interface 500
9.2.3 Simple systems and secondary phenomena: definitions 501
9.2.4 Reaction rates in simple systems 503
9.2.4.1 General principles 503
9.2.4.2 Signal measurement time 507
Contents ix
9.2.4.3 Reversibility and irreversibüity 508
9.2.4.4 Lability and inertness 515
9.3 Complexation Measurements in Simple Systems 519
9.3.1 Labile systems 519
9.3.1.1 Theoretical relationships 519
9.3.1.2 Discussion 521
9.3.1.3 Application of the DeFord and Hume method
withZ)M=Z ML 522
9.3.1.4 Labile slowly diffusing complexes 524
9.3.2 Chemically inert systems 527
9.3.2.1 Principles 527
9.3.2.2 Measurement of ? by variation in [L] 528
9.3.2.3 Measurement of complexation capacity, Cc 531
9.3.3 Slow systems 531
9.4 Quantitative Influence of Secondary Phenomena 535
9.4.1 Mixture effect 535
9.4.2 Surface pH and complexation buffer capacities 536
9.4.2.1 Reduction methods 537
9.4.2.2 Reoxidation methods 538
9.4.3 Ligand adsorption and adsorbed complex formation 542
9.4.3.1 General principles 542
9.4.3.2 Comparison of diffusion and adsorption rates 546
9.4.3.3 System (M-PROM) forming soluble and
adsorbed complexes, studied by direct
reduction methods 548
9.4.3.4 System (M-PROM) forming soluble and
adsorbed complexes, studied by ASV 555
9.5 Choice of Optimum Conditions 559
10 STUDY OF COMPLEXATION PROPERTIES BY NON-ELECTRO-
CHEMICAL METHODS 563
10.1 Choice of Method 564
10.2 Direct Methods Without Separation: Spectrometry 566
10.2.1 Electron spin resonance (ESR) 566
10.2.2 Fluorescence 567
10.2.2.1 Emission wavelength and intensity 567
10.2.2.2 Quenching effect 568
10.2.2.3 Fluorescence polarization 569
10.2.2.4 Fluorescence lifetime 569
10.2.2.5 Applications to aquatic complexants 569
10.3 Methods Based on Direct Physical Separation 570
10.3.1 Membrane separation principles 570
10.3.1.1 Different modes of separation 570
Contents
10.3.1.2 Ultrafiltration flux and retention coefficient 573
10.3.1.3 Experimental methods and membranes 576
10.3.2 Membrane separation: applications to equilibrium studies 578
10.3.2.1 Dialysis 578
10.3.2.2 Ultrafiltration with continuous reagent addition 578
10.3.2.3 Ultrafiltration by the concentration method 579
10.3.2.4 Influence of complex dissociation kinetics 580
10.3.3 Membrane separation: factors influencing the retention
coefficient 585
10.3.3.1 Electrostatic and hydration effects 586
10.3.3.2 Steric effects 589
10.3.3.3 Concentration polarization 589
10.3.3.4 Other surface effects 591
10.3.4 Size exclusion chromatography 591
10.3.4.1 Separation principles 591
10.3.4.2 Applications to complexation measurements 595
10.4 Chemical Competition Methods 597
10.4.1 Chemical competition in solution 598
10.4.1.1 Methods without separation (spectrometric
detection) 598
10.4.1.2 Methods with separation 599
10.4.2 Chemical competition with a solid phase 600
10.4.2.1 Principles 600
10.4.2.2 Solid phase characteristics and determination
of [M] 602
10.4.2.3 Operating conditions and limitations 604
10.5 Biological Methods 606
10.5.1 Measurements of complexation capacity 606
10.5.2 Measurement of free ion activity 607
10.5.3 Discussion 608
Appendix 611
References 636
Index 673
|
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| id | DE-604.BV006060556 |
| illustrated | Illustrated |
| indexdate | 2024-07-09T16:39:33Z |
| institution | BVB |
| isbn | 0853125570 0470208309 |
| language | Undetermined |
| oai_aleph_id | oai:aleph.bib-bvb.de:BVB01-003821452 |
| oclc_num | 630343877 |
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| physical | XXI, 692 S. Ill., graph. Darst. |
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| publishDateSearch | 1988 |
| publishDateSort | 1988 |
| publisher | Horwodd u. a. |
| record_format | marc |
| series2 | Elis Horwood series in analytical chemistry |
| spelling | Buffle, Jacques Verfasser aut Complexation reactions in aquatic systems an analyt. approach J. Buffle 1. publ. Chichester u. a. Horwodd u. a. 1988 XXI, 692 S. Ill., graph. Darst. txt rdacontent n rdamedia nc rdacarrier Elis Horwood series in analytical chemistry Metallanalyse (DE-588)4169566-5 gnd rswk-swf Komplexbildungsreaktion (DE-588)4164887-0 gnd rswk-swf Wasserverschmutzung (DE-588)4189299-9 gnd rswk-swf Metallanalyse (DE-588)4169566-5 s Wasserverschmutzung (DE-588)4189299-9 s Komplexbildungsreaktion (DE-588)4164887-0 s DE-604 HBZ Datenaustausch application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=003821452&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis |
| spellingShingle | Buffle, Jacques Complexation reactions in aquatic systems an analyt. approach Metallanalyse (DE-588)4169566-5 gnd Komplexbildungsreaktion (DE-588)4164887-0 gnd Wasserverschmutzung (DE-588)4189299-9 gnd |
| subject_GND | (DE-588)4169566-5 (DE-588)4164887-0 (DE-588)4189299-9 |
| title | Complexation reactions in aquatic systems an analyt. approach |
| title_auth | Complexation reactions in aquatic systems an analyt. approach |
| title_exact_search | Complexation reactions in aquatic systems an analyt. approach |
| title_full | Complexation reactions in aquatic systems an analyt. approach J. Buffle |
| title_fullStr | Complexation reactions in aquatic systems an analyt. approach J. Buffle |
| title_full_unstemmed | Complexation reactions in aquatic systems an analyt. approach J. Buffle |
| title_short | Complexation reactions in aquatic systems |
| title_sort | complexation reactions in aquatic systems an analyt approach |
| title_sub | an analyt. approach |
| topic | Metallanalyse (DE-588)4169566-5 gnd Komplexbildungsreaktion (DE-588)4164887-0 gnd Wasserverschmutzung (DE-588)4189299-9 gnd |
| topic_facet | Metallanalyse Komplexbildungsreaktion Wasserverschmutzung |
| url | http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=003821452&sequence=000002&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
| work_keys_str_mv | AT bufflejacques complexationreactionsinaquaticsystemsananalytapproach |