BOUCHET Renaud,? Professor, CNRS, Grenoble Alpes University.

DOLLE Mickaël, Associate Professor, Department of Chemistry, University of Montreal.

Introduction vii

Chapter 1. Anatomy of an All-Solid-State Battery 1

1.1. Constituents of an all-solid battery 3

1.1.1. Nature of solid electrolytes: required qualities 3

1.1.2. Positive electrode materials 4

1.1.3. Negative electrode materials 5

1.1.4. Conductive additive 7

1.1.5. Formulation of electrodes 7

1.2. Shaping methods of all-solid batteries 8

1.2.1. Assembly by cold pressing 8

1.2.2. Design by high temperature sintering 10

Chapter 2. Solid Ionic Conductors 13

2.1. Introduction 13

2.2. Solid lithium-ion conductors 15

2.2.1. The Garnets 15

2.2.2. The NASICON AxMM′(XO4)3 structure 17

2.2.3. The compounds LISICON and Thio-LISICON 18

2.2.4. Ion conductive glass and glass-ceramics 23

2.2.5. The Argyrodites 29

2.2.6. The complex hydrides . 34

2.2.7. Phosphorus and lithium oxynitride or LiPON 36

2.2.8. Anti-perovskite lithium-rich solid electrolytes 36

2.2.9. Solid polymer electrolytes 39

2.3. Solid sodium-ion conductors 40

2.3.1. NASICON compounds 41

2.3.2. Na3PS4 42

Chapter 3. All-Solid-State Battery Technology Using Solid Sulfide Electrolytes 47

3.1. Monolithic Li-ion “all-solid-state” batteries 47

3.1.1. The first “all-solid-state” batteries 47

3.1.2. Second generation “all-solid-state” batteries 48

3.1.3. Toward High Performance Batteries 53

3.1.4. Batteries using lithium argyrodite electrolytes 58

3.1.5. Li10XP2S12 (X = Ge, Si, Sn) phase in the structure LGPS 66

3.1.6. Understanding stability at the interfaces between the electrolyte and electrode materials 81

3.1.7. Summary 84

3.2. Sodium monolithic “all-solid-state” batteries 85

3.3. “All-solid-state” Li–S batteries 91

Chapter 4. Monolithic “All-Solid-State” Batteries Using Solid Oxide Electrolytes 97

4.1. Silver “all-solid-state” battery technology 97

4.2. Li-ion “solid-state” battery technology 100

4.3. Sodium “solid-state” battery technology 108

4.3.1. Sodium-ion “solid-state” battery technology 108

4.3.2. Sodium-sulfur “all-solid-state” battery technology 116

Chapter 5. LiBH4 Electrolyte and Polymer Battery Technology 119

5.1. “All-solid-state” battery technology: LiBH4 electrolyte 119

5.2. “Solid-state” polymer battery technology 120

Chapter 6. Markets 123

6.1. Solid electrolytes 123

6.1.1. Ohara 123

6.1.2. NEI 127

6.2. Solid-state batteries 127

6.3 Conclusion 137

Conclusion 139

Bibliography 145

Index 167

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