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Table of contents
General Introduction
1. Motivation
2. General Objective
3. Layout of the Manuscript
I. Literature Review on Solid Oxide Cells: Technology Fundamentals and Degradation Phenomena
I.1 Solid Oxide Cells: Basic Operating Mechanisms and Materials
I.1.1 SOCs Principle
I.1.2 SOCs Architecture
I.1.3 Materials Selection
I.1.4 Thermodynamic Description of SOCs and Nernst Equation
I.1.5 Losses at the Cell Level and Impact on Cell’s Performances
I.2 Literature Review on the Reaction Mechanisms for the Two Electrodes
I.2.1 Reaction Mechanism for the Hydrogen Electrode
I.2.2 Reaction Mechanism for the Oxygen Electrode
I.3 Durability of SOCs
I.3.1 Durability Results Reported in Literature
I.3.2 Main Degradation Mechanisms
I.3.3 Concluding Remarks
I.4 Conclusions of This Chapter: Objectives and Methodology of the Thesis
II. Durability Experiments and Post-Test Characterization Techniques
II.1 Long-term Tests in Electrolysis Mode at Different Operating Temperature
II.1.1 Cell Description
II.1.2 Description of the Test Benches
II.1.3 Experimental Techniques
II.1.4 Testing Protocols
II.1.5 Tests Results
II.2 Long-term Tests in Collaboration with External Partners
II.2.1 Cells Description
II.2.2 Durability Tests
II.3 Physico-Chemical Characterizations and 3D Reconstructions
II.3.1 Sample Selection
II.3.2 Sample Preparation
II.3.3 Characterization Techniques
II.4 Conclusion of This Chapter
III. Development and Validation of the Multi-Scale Modeling Tools
III.1 Micro-Scale Models for the Hydrogen Electrode
III.1.1 Models Description
III.1.2 Experimental Characterization
III.1.3 Models Validation and Discussion
III.1.4 Concluding Remarks and Model Adaptation for the Degradation Studies
III.2 Micro-Scale Model for the Oxygen Electrode
III.2.1 Experimental Characterization
III.2.2 Microstructural Reconstruction for Cell I
III.2.3 Description of the Modeling Tools
III.2.4 Model Validation and Discussion
III.2.5 LSCF-GDC Composite Electrodes
III.2.6 Concluding Remarks
III.3 Macro-Scale Model at the Cell level and Multi-Scale Integration
III.3.1 Macro-Scale Model Description
III.3.2 Multi-Scale Integration
III.3.3 Multi-Scale Model Validation
III.4 Conclusion of This Chapter
IV. Hydrogen Electrode Degradation: Impact of Polarization and Initial Microstructure on the Ni Evolution
IV.1 3D Reconstructions and Image Processing Techniques for Microstructural Computations
IV.1.1 Samples Extracted from Cell-A and Cell-B
IV.1.2 Methodology for the Determination of the Microstructural Parameters
IV.2 Results of the Microstructural Analysis
IV.2.1 Microstructural Properties of the Reference Cells
IV.2.2 Microstructural Evolution of the Aged Cells
IV.3 Impact of Ni Evolution on the Cell Performances
IV.3.1 Preliminary Remark: Adaptation of the H2 Electrode Model
IV.3.2 Role of Ni Agglomeration on Degradation
IV.3.3 Role of Ni Depletion on Degradation
IV.4 Suggested Mechanism of Ni Depletion
IV.5 Conclusion of This Chapter
V. Oxygen Electrode Degradation: LSCF Demixing and Interdiffusion at the GDC/8YSZ Interface
V.1 Characterization of the Pristine Cell
V.1.1 Detection of SrZrO3 After Sintering
V.1.2 Inter-Diffusional Layer Between the GDC and the YSZ
V.1.3 Crystalline Phases Distribution Across the Electrolyte and Barrier Layer
V.2 Characterization of the Aged Cells
V.2.1 Preliminary Remark: Proposed Mechanism for the LSCF Destabilization
V.2.2 LSCF Destabilization: Sr Release from the Material as a Function of Temperature and Polarization
V.2.3 Evolution of the IDL After Aging in Electrolysis Mode: Preliminary Characterizations and Discussion
V.3 Conclusion of This Chapter
VI. Conclusions and Perspectives
VI.1 General Conclusions
VI.2 Perspectives
Appendix A Cells Description and Experimental Conditions
Appendix B Development of the Micro-Kinetic Model for the Hydrogen Electrode Reaction Mechanism: Model I Based on the Oxygen Spillover Mechanism
Appendix C Development of the Micro-Kinetic Model for the Hydrogen Electrode Reaction Mechanism: Model II Based on the Hydrogen Spillover Mechanism
Bibliography



