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Battery, Battery Materials

<2024> Li-S Battery Technology Development Status and Outlook

 

 

Lithium-Sulfur (Li-S) batteries are lithium-ion secondary batteries (LIBs) that use sulfur or sulfur compounds as cathode active materials, and often use metallic lithium or its alloys for anode materials. Since sulfur can attract two lithium atoms or release two electrons with one atom, it can theoretically achieve a gravimetric energy density of 1675 mAh/g, which is about 10 times that of existing LIBs, but in reality, development is underway aimed at realizing gravimetric energy of about twice that.

 

Since Li-S batteries do not use expensive metal materials such as cobalt or nickel, their carbon footprint is 60% lower than that of general LIBs and 40% lower than that of all-solid-state batteries, making them more eco-friendly to produce. This has the potential to significantly improve battery performance, making them a strong candidate for next-generation batteries that can simultaneously provide low cost and improved performance.

 

Until now, the cycle life of charging-discharging processes has often been as short as around 200 cycles. This is primarily because sulfur from the cathode dissolves into the electrolyte or forms polysulfides (Li2Sx), which do not revert to the original sulfur, leading to rapid degradation of the original electrode structure. Additionally, since sulfur itself is an insulator, a large amount of conductive additives is needed for its use as a cathode, which has prevented the energy density from reaching theoretical levels. Researchers have been tackling these issues through extensive trial and error.

 

However, in 2022, researchers from Drexel University in the U.S. reported achieving a cycle life of 4,000 times. Development cases by battery manufacturers are also increasing. For instance, the US company Lyten reported over 1,400 cycles for a cell designed for electric vehicles in 2021. Additionally, Japanese company ADEKA announced in November 2022 that they had achieved over 5,000 cycles at an energy density of 100 Wh/kg and over 200 cycles at 450 Wh/kg. Furthermore, in November 2023, ADEKA revealed a prototype cell with an impressive weight energy density of 803 Wh/kg, the highest level ever achieved for lithium-ion batteries.

 

 

Recently, there has been an active movement to provide samples to car makers. Lyten received investment from European car maker Stellantis in 2023, and began shipping pilot-produced cells to Stellantis in May 2024, and announced that it would be shipping samples to more than 20 companies in late 2024. Currently, it is a pouch-type cell, but it is said that cylindrical cells will also be manufactured in late 2024. These can be manufactured at half the material cost of existing LIBs, and the manufacturing yield is also said to be high at over 90%.

 

Li-S Energy (Australia) started operating a pilot production line with a capacity of 2MWh/year in 2024. They are now planning to build a large-scale production facility with a capacity of GWh per year.

 

In 2023, Gelion (UK) acquired the intellectual property of OXIS Energy, which went bankrupt in May 2021. Using this technology, they announced a cell with an energy density of 395 Wh/kg in April 2024 and plan to start sample shipments in 2026.

 

In China, Zhongke Paisi Energy Storage Technology has been producing 35 Ah, 609 Wh/kg battery cells at a pilot scale since 2017 and is expanding production for advanced solar drones, EVs, and power storage applications.

 

LG Energy Solution, a global battery manufacturer, has also been researching Li-S as one of next-generation batteries since 2015. By applying the pouch outer material, introducing a new combination of electrolytes, and effectively controlling the volume with the know-how accumulated over many years, the lifespan has been increased, and it is intended for use in urban air mobility (UAM) and high-altitude unmanned aerial vehicles (UAVs), and the goal is commercialization in 2027. Meanwhile, in the case of high-altitude UAVs, it can be used for 6 months with 200 times of charges, and it is said that the condition required by the OEM is 400-500Wh/kg and used more than 200 times.

 

This report provides a comprehensive overview of the development of Li-S secondary batteries, including major technological advances, related technological obstacles, and component/material developments. It also focuses on the latest emergence of cell configurations that promise a leap forward in Li-S secondary battery research. It also introduces advanced characterization techniques that can help understanding the mechanisms involved in the chemistry of Li-S secondary batteries, and provides an introduction to research programs in various countries, covering the academic and practical applications of research results to date.

 

 

 

Strong Points of this report

 

     Summary of the concept of Li-S batteries and historical development trends

 

     Understanding of Li-S battery technical obstacles and the status of component/material development

 

     Latest trends in Li-S battery cell development material composition

 

     Presentation of Li-S battery application cases by major companies

 

     Introduction to the status of Li-S battery-related patent applications and future development directions

 

 

 


 
<Recent advances in shuttle effect inhibition for Li-S batteries>




 

 

 

 

< Overview of Li-S battery development from concept proposal to present & Roadmap for Li-S batteries >

 

 

 

 



< A brief timeline and key events in the development of Li-S batteries >


 

 


 

 

 

 

 

 

< Support projects for next-generation batteries_Li-S batteries >

 

 

 

 

 

 

 

 

 

 Table of Contents



1. Overview of Lithium-Sulfur Secondary Batteries  9 

1-1. Need for Lithium-Sulfur Secondary Batteries  9 

1-2. History of Lithium-Sulfur Secondary Batteries  12 

1-3. Principles of Lithium-Sulfur Secondary Batteries  16 

1-4. Technical Issues of Lithium-Sulfur Secondary Batteries  21 

1-4-1. Insulation of Sulfur  21 

1-4-2. Formation of Dissolved Substances and Shuttle Effect  21 

1-4-3. Formation of Insoluble Substances (Li2S)  25 

1-4-4. Self-Discharge Phenomenon  25 

1-4-5. Use of Lithium Anodes  28 

1-4-6. Use of Thick Sulfur Electrodes  29 

1-5. Commercialization of Lithium-Sulfur Secondary Batteries  30 

1-5-1. Important Parameters for High-Energy-Density Lithium-Sulfur Batteries  32 

1-5-2. Industrialization of Lithium-Sulfur Batteries  35

 

2. Development Status of Sulfur Cathode Technology for Lithium-Sulfur Secondary Batteries  37 

2-1. Traditional Sulfur Composite Electrode  37 

2-2. Sulfur-Porous Carbon Composite Materials  38 

2-2-1. Sulfur-Porous Carbon Composite Materials  38 

2-2-1-1. Carbon Materials  39 

2-2-1-2. Sulfur-Carbon Composite  39 

2-2-1-3. Synthesis Methods  47 

2-2-2. Sulfur-Graphene Composite Materials  50 

2-2-2-1. Graphene and Graphene Oxide  50 

2-2-2-2. Sulfur-Graphene/Graphene Oxide Composite  50 

2-2-3. Binder-Free Sulfur-Carbon Composite Electrode  52 

2-3. Sulfur-Graphene Composite Materials  55 

2-3-1. Sulfur-Polyacrylonitrile Composite  55 

2-3-2. Sulfur-Polypyrrole Composite  56 

2-3-3. Sulfur-Polyaniline Composite  57 

2-3-4. Other Sulfur-Conductive Polymer Composites  59 

2-4. Binder-Free Sulfur-Carbon Composite Electrode  61 

2-4-1. Metal Oxide Additives  61 

2-4-2. Metal Oxide Coatings  62

 

 

2-4-3. Metal Sulfide Complexes 63 

2-4-4. Intercalation Compounds 63 

2-5. Catalyst Materials for Sulfur Cathodes 63 

2-5-1. Metal Sulfide Catalysts 64 

2-5-2. Metal Oxide Catalysts 66 

2-5-3. Single-Atom Catalysts 68 

2-5-4. Defect Site Catalysts 69 

2-5-5. Quantum Dot Catalysts 71 

2-5-6. Heterostructure Catalysts 72 

2-5-7. Other Catalyst Materials 74

 

3. Development Status of Lithium Sulfide (Li2S) Cathode Technology for Lithium-Sulfur Secondary Batteries 76 

 

3-1. Activation of Micronized Li2S Particles 76 
3-2. Li2S-Carbon Composite 77 
3-3. Chemical Synthesis of Li2S Cathode Materials 78 
3-4. All-Solid-State Secondary Batteries Using Li2S Cathodes 80

 

 

4. Development Status of Anode Technology for Lithium-Sulfur Secondary Batteries 81 

 

4-1. Lithium Metal Anode 82 
4-2. Silicon Anode 82 
4-3. Carbon Anode 84 
4-4. Li-Free Anode 85 
4-5. Anode Protection Technology 85 
4-6. Anode Compound (Composite) Technology 85 
4-7. Prelithiated Graphene 86 
4-7-1. Summary of Prelithiated Graphene 86 
4-7-2. Results of Prelithiated Graphene 88 
4-7-3. Conclusion 96

 

 

5. Current Status of Electrolyte, Separator, and Binder Technology Development for Lithium-Sulfur Secondary Batteries 97

 

5-1. Liquid Electrolyte 98
5-2. Carbonate-based Electrolyte 101
5-3. Polymer/Solid Electrolyte 103
5-3-1. Solid Polymer Electrolyte 106

 

 

5-3-2. Inorganic Solid Electrolyte 109
5-3-2-1. Oxide-based Electrolyte 109
5-3-2-2. Sulfide-based Electrolyte 111
5-3-3. Composite Solid Electrolyte 116
5-4. Separator 119
5-4-1. Surface-coated Separator 120
5-4-2. Innovative Battery Separator 121
5-5. Current Status of Binder Technology Development for Lithium-Sulfur Secondary Batteries 122

 

 

6. Configuration of Lithium-Sulfur Secondary Battery Cell  125 

6-1. Intermediate Layer  125 
6-1-1. Polysulfide Barrier Mechanism  126 
6-1-2. Materials for the Intermediate Layer  127 
6-2. Porous Current Collector  128 
6-2-1. Sulfur Impregnation Strategy  129 
6-2-2. Materials for Porous Current Collector  130 
6-3. Sandwich Electrode  130 
6-4. Dissolved Polysulfide Anolyte  131 
6-5. Voltage Window of Lithium-Sulfur Secondary Battery  132  
6-5-1. Upper Voltage Plateau  133   

             6-5-2. Lower Voltage Plateau  133 

 

7. Analysis Techniques and Mechanistic Understanding of Lithium-Sulfur Secondary Battery  133 

7-1. In-Situ Analysis  134 

7-2. Polysulfide Dissolution  135 

7-3. Formation of Protective Layer  136 

7-4. Kinetics  138

 

8. Development of All-Solid Lithium-Sulfur Batteries 140

8-1. Summary 140

8-2. Current Status of LIBs 141

8-3. Necessity of All-Solid Lithium-Sulfur Batteries 143

8-3-1. Safety Issues of LIBs 143

8-3-2. Increasing Demand for High-Energy-Density Batteries 146

8-3-3. Raw Material Supply and Sustainability Issues 148                                                                                                                              

8-4. Basics of All-Solid Lithium-Sulfur Batteries 149

8-4-1. Sulfide-Based Solid Electrolytes 151

8-4-1-1. Glass Solid Electrolytes 151

8-4-1-2. Crystalline Materials 152

8-5. Sulfide-Based Cathodes 156

8-5-1. Sulfur 156

8-5-2. Metal Sulfides 158

8-5-3. Organic Sulfur 158

8-5-4. Li2S 159

8-6. Anode Materials for All-Solid Lithium-Sulfur Batteries 160

8-6-1. Lithium Metal Anodes 160

8-6-2. Lithium Alloy Anode Materials 161

8-6-3. Silicon Anode Materials 162

8-7. Redefining Four Challenges of All-Solid Lithium-Sulfur Batteries 162

8-7-1. Interface Stability 162

8-7-2. Lithium Dendrites 164

8-7-3. Volume Expansion and Electrochemical Instability 166

8-7-4. Processing Issues 167

8-7-5. Regulatory Approval and Standardization 167

8-8. Five Strategies for Accelerating Commercialization of All-Solid Lithium-Sulfur Batteries 168

8-8-1. Performance Enhancement 168

8-8-2. Cell Design Improvements for Enhanced Efficiency 170

8-8-3. Strategies for Large-Scale Fabrication 172

8-8-4. Wet Coating Process 173

8-8-5. Dry Coating Process 174

8-8-6. Infiltration Process 175

8-9. Summary and Outlook 176

 

9. Energy Density Formula for Practical Li-S Battery Design  177 

 

9-1. Research Overview  177 
9-2. Formulation for High-Energy Density Li-S Batteries  178 
9-3. Ah-Class High-Energy Density Li-S Batteries  182 
9-3-1. Goals for Achieving Practical Li-S Batteries  184 
9-4. Calculations for Li-S Full Cells  187

 

 

10. Current Status of Lithium-Sulfur Battery Development Companies  188

10-1. LGES. 189

10-2. Sion Power 193

10-3. Zeta Energy. 198

10-4. Li-S Energy(Australia) 206

10-5. Polyplus. 211

10-6. TheION(Germany) 215

10-7. NexTech Batteries(US) 221

10-8. Lyten(US) 225

10-9. ADEKA (Japan) 237

10-10. Gelion plc(Australia) 252

10-11. GS Yuasa. 259

10-12. Zhongke Paisi Energy Storage Technology Co., Ltd. 265

10-13. Shaanxi Guoneng New Materials Co., Ltd(西能新材料有限公司) 267

 

11. Current Status of Major Patent Applications and Future Directions in Technology Development  268

 

12. Recent Developments in Lithium-Sulfur Batteries  276 

 

12-1. Recent Developments by Global Companies and Research Institutions  276 
12-2. Results of the DOE Li-S Battery Program  286  
12-2-1. Penn State University  286 
12-2-2. University of Pittsburgh  288 
12-2-3. PNNL (Pacific Northwest National Laboratory)  291 
12-3. Results of the European Li-S Battery Program  293 
12-4. South Korea National Project Program  296

 

 

13. References 303