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Silicon-Doped Argyrodite Solid Electrolyte Li6PS5I with Improved Ionic Conductivity and Interfacial Compatibility for
Jun Zhang1, Lujie Li1, Chao Zheng1
1College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, P. R. China.
ACS Applied Materials & Interfaces
|August 22, 2020
Summary
Silicon doping enhances argyrodite solid electrolytes (SEs) for all-solid-state lithium batteries (ASSLBs). This research improves ionic conductivity in Li6+xP1-xSixS5I, boosting battery performance and efficiency.
Area of Science:
- Materials Science
- Electrochemistry
- Solid-State Chemistry
Background:
- Argyrodite-type sulfide solid electrolytes (SEs), specifically Li6PS5X (X = Cl, Br, I), are promising for all-solid-state lithium batteries (ASSLBs) due to their lithium-ion transport capabilities.
- Li6PS5I exhibits poor ionic conductivity (10^-7 S cm^-1) attributed to ordered I-/S2- site arrangements, hindering its application in ASSLBs.
- Enhancing ionic conductivity in sulfide SEs is crucial for advancing high-performance ASSLBs.
Purpose of the Study:
- To develop a silicon-doped solid electrolyte, Li6+xP1-xSixS5I, to overcome the conductivity limitations of Li6PS5I.
- To investigate the structural modifications induced by silicon doping and their impact on ionic conductivity and activation energy.
- To evaluate the electrochemical performance of the developed solid electrolyte in ASSLBs using a Li(Ni0.8Mn0.1Co0.1)O2 cathode and lithium metal anode.
Main Methods:
- Synthesis of silicon-doped Li6+xP1-xSixS5I solid electrolytes.
- Characterization of structural changes using techniques such as X-ray diffraction (XRD) and impedance spectroscopy.
- Fabrication and electrochemical testing of ASSLBs incorporating the synthesized solid electrolytes, including cycling performance and interfacial reaction analysis.
Main Results:
- Silicon doping significantly increased ionic conductivity to 1.1 × 10^-3 S cm^-1 and reduced activation energy to 0.19 eV.
- The structural unit within the argyrodite network was altered by silicon doping, leading to improved lithium-ion transport.
- ASSLBs utilizing Li6.55P0.45Si0.55S5I demonstrated an initial discharge capacity of 105 mA h g^-1 at 0.05C with high Coulombic efficiency.
Conclusions:
- Silicon doping is an effective strategy to enhance the ionic conductivity of Li6PS5I-based solid electrolytes.
- The improved Li6+xP1-xSixS5I solid electrolytes show great potential for high-performance ASSLBs.
- Further investigation into interfacial reactions is necessary for optimizing long-term cell performance and understanding degradation mechanisms.
