Understanding the Solid-Electrolyte-Interface (SEI) Formation in Glyme Electrolyte Using Time-Of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS)

Chinmayee Padwal; Hong Duc Pham; Linh Thi My Hoang; Sagadevan Mundree; Ashok Kumar Nanjundan; Syam G Krishnan; Deepak Dubal

doi:10.1002/cssc.202301866

Understanding the Solid-Electrolyte-Interface (SEI) Formation in Glyme Electrolyte Using Time-Of-Flight Secondary Ion Mass Spectrometry (ToF-SIMS)

ChemSusChem. 2024 Apr 3:e202301866. doi: 10.1002/cssc.202301866. Online ahead of print.

Authors

Chinmayee Padwal^{1

2}, Hong Duc Pham³, Linh Thi My Hoang¹, Sagadevan Mundree⁴, Ashok Kumar Nanjundan⁵, Syam G Krishnan⁶, Deepak Dubal^{1

2}

Affiliations

¹ Centre for Agriculture and the Bioeconomy, Queensland University of Technology, Brisbane, QLD 4000, Australia.
² Centre for Materials Science, School of Chemistry and Physics, Queensland University of Technology, Brisbane, QLD 4000, Australia.
³ Centre for Future Materials, University of Southern Queensland, Toowoomba, QLD 4350, Australia.
⁴ School of Agriculture and Food Sustainability, The University of Queensland, Brisbane, QLD 4072, Australia.
⁵ School of Engineering, University of Southern Queensland, Springfield, QLD 4300, Australia.
⁶ Faculty of Engineering and Information Technology, The University of Melbourne, Victoria, 3010, Australia.

PMID: 38568784
DOI: 10.1002/cssc.202301866

Abstract

Lithium-ion batteries are commonly used for energy storage due to their long lifespan and high energy density, but the use of unsafe electrolytes poses significant health and safety concerns. An alternative source is necessary to maintain electrochemical efficacy. This research demonstrates new safe glyme-based electrolytes for silica/carbon (SiO_x/C) nanocomposite derived from Australian rice husk (RH). The quality of SiO_x/C was preserved by using deep eutectic solvent-based pre-treatment and single-step carbonization, which was confirmed through the X-ray analysis of the crystalline phase of silica. The electrochemical assessment of SiO_x/C anode using various glyme-based electrolytes for LIBs was carried out. Among them, the resultant half cells based on diglyme electrolyte is superior to others with the first discharge capacity at 1274 mAh/g and a reversible discharge capacity of 759.7 mAh/g. Ex-situ SEM and Time-of-Flight Secondary Ion Mass Spectrometry (ToF- SIMS) analysis of the electrode indicated that diglyme not only improves the capacity but also sustains the electrode architecture for longer cycle life with more LiF-based components and also showed the absence of HF components. Importantly, the addition of fluoroethylene carbonate (FEC) additive enhanced the cycling stability. These results provide a new perspective on developing advanced SiOx/C anode using glyme electrolytes for Li-ion batteries.

Keywords: Time-of-Flight Secondary Ion Mass Spectrometry; electrolyte; glyme; lithium-ion batteries; silicon-based anode.

Abstract

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