4.8 Article

Elucidating the Mechanism of Li Insertion into Fe1-xS/Carbon via In Operando Synchrotron Studies

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 47, Pages 52691-52700

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c15500

Keywords

in operando synchrotron X-ray diffraction; lithium storage mechanism; conversion reaction; X-ray absorption spectroscopy; phase transition

Funding

  1. China Scholarship Council (CSC) [201707030004]

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The detailed understanding of kinetic and phase dynamics taking place in lithium-ion batteries (LIBs) is crucial for optimizing their properties. It was previously reported that Fe1-xS/C nanocomposites display a superior performance as anode materials in LIBs. However, the underlying lithium storage mechanism was not entirely understood during the 1st cycle. In this work, in operando synchrotron techniques are used to track lithium storage mechanisms during the 1st (de)-lithiation process in the Fe1-xS/C nanocomposite. The combination of in operando techniques enables the uncovering of the phase fraction alternations and crystal structural variations on different length-scales. Additionally, the investigation of kinetic processes, morphological changes, and internal resistance dynamics is discussed. These results reveal that the phase transition of Fe1-xS -> Li2Fe1-xS2 -> Fe-0 + Li2S occurs during the 1st lithiation process. The redox reaction of Fe2+ + 2e(-) (sic) Fe-0 and the Fe K-edge X-ray absorption spectroscopy (XAS) transformation process are confirmed by in operando XAS. During the 1st de-lithiation process, Fe-0 and Li2S convert to Li2-yFe1-xS2 and Li+ is extracted from Li2S to form Li2-yS. The phase transition from Li2S to Li2-yS is not detected in previous reports. After the 1st de-lithiation process, amorphous lithiated iron sulfide nanoparticles are embedded within the remaining Li2S matrix.

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