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Table of contents
Chapter I: Literature review
I.1 Introduction
I.2 Management of harbor sediments
I.2.1 Defining dredging operations
I.2.2 European management of sediments. Legislation
I.2.3 Existing projects and hierarchy for DM management
I.2.3.1 Projects for DM in France and Ireland
I.2.3.2 Hierarchy of dredged materials
I.3 Origin and composition of sediments
I.3.1 Geological origin of sediments
I.3.2 Composition of sediments
I.3.2.1 Inorganic phase
I.3.2.1.1 Clays
I.3.2.1.2 Oxides, hydroxides, oxyhydroxides
I.3.2.1.3 Carbonates
I.3.2.1.4 Sulfurs
I.3.2.2 Organic phase
I.4 Contaminants in sediments and their sources
I.4.1 Organic contaminants
I.4.2 Inorganic contaminants
I.4.2.1 Zinc
I.4.2.2 Nickel
I.4.2.3 Cadmium
I.4.2.4 Copper
I.4.2.5 Arsenic
I.4.2.6 Chromium
I.5 Factors affecting HM availability
I.5.1 Influence of pH
I.5.2 Oxidation-Reduction Potential
I.5.3 Cation exchange capacity (CEC)
I.5.4 Organic matter
I.5.5 Salinity
I.6 Treatment technologies for dredged sediments
I.6.1 Pre-treatment
I.6.2 Physical separation
I.6.3 Washing
I.6.4 Electrokinetic remediation
I.6.5 In-situ Capping
I.6.6 Biological remediation
I.6.7 Thermal Extraction
I.6.8 Solidification/Stabilization (S/S)
I.6.8.1 Tests for the S/S evaluation
I.6.8.2 S/S main reactions mechanisms of HM fixation
I.6.8.3 Stability of the treated matrix
I.7 Considered binding agent properties
I.7.1 Ordinary Portland cement (OPC)
I.7.1.1 Composition of OPC
I.7.1.2 Hydration chemistry of OPC
I.7.2 Ground granulated blast-furnace slag (GGBS)
I.7.2.1 What is GGBS?
I.7.2.2 Chemical composition, mineralogy of GGBS
I.7.2.3 Hydration of GGBS-based binders
I.7.3 C-S-H structure
I.7.4 OPC and GGBS-based binders in S/S practice
I.7.4.1 OPC as a S/S agent
I.7.4.2 GGBS as a S/S agent
Chapter II: Materials and Methods
II.1 Introduction
II.2 Raw materials
II.2.1 Sediment
II.2.1.1 Origin of the considered sediments
II.2.1.2 Physical analysis of the sediments
II.2.1.2.1 Particle size distribution
II.2.1.2.2 Density
II.2.1.3 Mineralogy
II.2.1.3.1 XRD analysis
II.2.1.3.2 TGA (Thermogravimetric analysis), DTA (Differential thermal analysis)….
II.2.1.4 Chemical properties of the sediments
II.2.1.4.1 pH measurements
II.2.1.4.2 Total Organic Carbon (TOC) analysis
II.2.1.4.3 Cation Exchange Capacity (CEC) measurement
II.2.1.5 Operational fractionation of inorganic pollutants
II.2.1.5.1 Total Attack of the Dublin sediment and the main binding agents
II.2.1.5.1.1 Total attack procedure
II.2.1.5.1.2 Results of the total attack of the Dublin sediment
II.2.1.5.1.3 Enrichment factor
II.2.1.5.2 Sequential extraction of HM from the Dublin sediment
II.2.1.5.2.1 Sequential extraction fractions proposed by Tessier protocol
II.2.1.5.2.2 Procedure of sequential extraction applied in the study
II.2.1.5.2.3 Sequential Extraction results for the major elements
II.2.2 Binders and other materials
II.3 Sediment-Binder Systems
II.3.1 Samples’ preparation
II.3.1.1 Samples for the main case Dublin port sediment
II.3.1.2 Samples for the study of the impact of the nature of sediments
II.3.2 Samples’ characterization
II.3.2.1 Compressive Strength
II.3.2.2 Shrinkage Test
II.3.2.3 Leaching Test
II.3.2.4 XRD analysis
II.3.2.5 Zeta Potential
II.3.2.6 Rheology
II.3.2.7 Tomography
II.3.2.8 SEM analysis
II.3.2.9 Solid State Nuclear magnetic resonance
II.3.2.10 Pyrolysis GC/MS
II.3.2.11 XAS (X-ray Absorption Spectroscopy)
II.4 Simplified models
II.4.1 Clay-Binder system
II.4.1.1 Materials
II.4.1.2 Samples’ preparation
II.4.1.3 Samples’ characterization
II.4.1.3.1 Compressive strength
II.4.1.3.2 XRD analysis
II.4.1.3.3 27Al MAS NMR investigation
II.4.1.3.4 SEM analysis
II.4.1.3.5 Zeta Potential
II.4.1.3.6 Rheology
II.4.2 Heavy metals – binders’ system for the investigation of early hydration
II.4.2.1 Materials
II.4.2.2 Samples’ preparation
II.4.2.3 Samples’ characterization
II.4.2.3.1 XRD analysis
II.4.2.3.2 27Al and 29Si MAS NMR investigation
II.4.2.3.3 Isothermal calorimetry analysis
II.4.2.3.4 Zeta Potential measurements
II.4.3 Investigation of Ni and Cd in OPC and GGBS-based binders
II.4.3.1 Materials
II.4.3.2 Samples’ preparation
II.4.3.3 Samples’ characterization
II.4.3.3.1 Leaching test
II.4.3.3.2 X-ray Absorption Fine Structure (XAFS) of Ni and Cd in binders
Chapter III. Solidification of contaminated sediments using GGBS-based binders
III.1 Introduction
III.2 Main case – S/S treatment of the Dublin port sediment
III.2.1 Compressive strength evolution of the Dublin sediment mixed with binders at 150 kg/m3
III.2.2 pH of the mixtures
III.2.3 Mineralogical analysis
III.2.4 Shrinkage results
III.2.5 Microstructure investigation
III.2.5.1 X-Ray microtomography
III.2.5.2 SEM observations
III.2.6 Electrokinetic properties
III.2.6.1 Results
III.2.6.2 Discussion
III.2.7 Conclusions
III.3 Study of the various factors impacting the evolution of compressive strength during S/S treatment
III.3.1 Impact of the nature of sediments
III.3.1.1 Compressive strength results and pH measurements
III.3.1.2 XRD analysis of the Dublin and Gothenburg sediments mixed with the binders
III.3.1.3 Conclusions
III.3.2 Impact of the sediment pore water
III.3.3 Impact of the clay fraction. Clay-Binder system’s study
III.3.3.1 Compressive strength and pH of the clay-binder systems
III.3.3.2 XRD analysis of the clay-binder systems
III.3.3.3 27Al NMR analyses of the clay-binder systems
III.3.3.4 TGA
III.3.3.5 SEM observations
III.3.3.6 Impact of the binder’s ions on the rheology and zeta potential of the clay
III.3.3.6.1 Zeta Potential results of the clay-binder systems
III.3.3.6.2 Rheological measurements of the clay-binder systems
III.3.3.7 Discussion
III.3.4 Impact of dispersing agents. Dublin sediment – Binder system
III.3.4.1 Effect on the rheological behaviour
III.3.4.2 Compressive strength results
III.3.4.3 Zeta Potential measurements
III.3.4.4 Discussion
III.4 Interaction between the Dublin sediment’s organic matter and binders
III.4.1 Organic matter reconstruction before and after S/S treatment
III.4.2 13C – NMR investigation
III.4.3 Discussion
III.4.4 Effect of the organic matter on early age hydration of hydraulic binders
III.4.4.1 Heat flow results
III.5 Conclusions
Chapter IV: Impact of heavy metals pollutants contained in dredged sediments on the hydration of hydraulic binders
IV.1 Introduction
IV.2 Early age hydration of the binders with HM
IV.2.1 Impact of zinc
IV.2.1.1 100%OPC formulation
IV.2.1.2 85%GGBS/15%OPC formulation
IV.2.1.3 Supersulfated formulation
IV.2.1.4 Discussion
IV.2.2 Impact of copper
IV.2.2.1 100%OPC formulation
IV.2.2.2 85%GGBS/15%OPC formulation
IV.2.2.3 Supersulfated formulation
IV.2.2.4 Discussion
IV.2.3 Impact of nickel
IV.2.3.1 100%OPC formulation
IV.2.3.2 85%GGBS/15%OPC formulation
IV.2.3.3 Supersulfated formulation
IV.2.3.4 Discussion
IV.2.4 Impact of cadmium
IV.2.4.1 100%OPC formulation
IV.2.4.2 85%GGBS/15%OPC formulation
IV.2.4.3 Supersulfated formulation
IV.2.4.4 Discussion
IV.2.5 Zeta Potential of the binders in the presence of HM
IV.2.5.1 100%OPC formulation
IV.2.5.2 85%GGBS/15%OPC
IV.2.5.3 Discussion
IV.2.6 Conclusions
IV.3 27Al and 29Si NMR spectra of the ‘hydraulic binders-heavy metals’ system. Long term hydration
IV.3.1 Introduction
IV.3.2 Considered samples
IV.3.3 27Al NMR spectra of the OPC system in the presence of Cd and Zn
IV.3.4 27Al NMR spectra of the GGBS85 system in the presence of Cd and Zn
IV.3.5 27Al NMR spectra of the AAS system in the presence of Cd and Zn
IV.3.5.1 29Si NMR and 1H-29Si spectra of the AAS system in the presence of Zn
IV.3.5.2 Conclusions
Chapter V. Stabilization of heavy metals using GGBS-based hydraulic binders
V.1 Introduction
V.2 Batch leaching test
V.2.1 Leaching test Results
V.2.2 pH measurements
V.2.3 Impact of a strongly acidic and basic pH on the stability of HM in the Dublin sediment
V.2.4 Discussion
V.2.4.1 Oxyanions metals
V.2.4.2 Cationic heavy metals
V.3 XAS Investigations
V.3.1 Speciation of Zn and Cu in the raw Dublin sediment and the sediment mixed with the binders
V.3.1.1 Zinc speciation
V.3.1.2 Copper speciation
V.3.2 Speciation of Ni and Cd in the binders
V.3.2.1 Cadmium speciation
V.3.2.2 Cadmium Leaching
V.3.2.3 Nickel speciation and leaching results
V.4 Sequential Extractions of HM from the Dublin sediment with and without hydraulic binders’ addition
V.4.1 Untreated sediments samples
V.4.2 Impact of the addition of hydraulic binder on the fractionation of HM
V.4.3 Discussion
V.4.4 Conclusions
V.5 Conclusions
