Revealing solid electrolyte interphase formation through interface-sensitive Operando X-ray absorption spectroscopy.

Autor: Swallow JEN; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK.; Diamond Light Source, Didcot, Oxfordshire, OX11 0DE, UK.; The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot, OX11 0RA, UK., Fraser MW; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK.; The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot, OX11 0RA, UK., Kneusels NH; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK., Charlton JF; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK.; Diamond Light Source, Didcot, Oxfordshire, OX11 0DE, UK., Sole CG; Diamond Light Source, Didcot, Oxfordshire, OX11 0DE, UK.; The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot, OX11 0RA, UK., Phelan CME; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK., Björklund E; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK.; The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot, OX11 0RA, UK., Bencok P; Diamond Light Source, Didcot, Oxfordshire, OX11 0DE, UK., Escudero C; ALBA Synchrotron Light Source, Carrer de la Llum 2-26, 08290, Cerdanyola del Vallès, Barcelona, Spain., Pérez-Dieste V; ALBA Synchrotron Light Source, Carrer de la Llum 2-26, 08290, Cerdanyola del Vallès, Barcelona, Spain., Grey CP; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK., Nicholls RJ; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK., Weatherup RS; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK. robert.weatherup@materials.ox.ac.uk.; Diamond Light Source, Didcot, Oxfordshire, OX11 0DE, UK. robert.weatherup@materials.ox.ac.uk.; The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot, OX11 0RA, UK. robert.weatherup@materials.ox.ac.uk.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2022 Oct 14; Vol. 13 (1), pp. 6070. Date of Electronic Publication: 2022 Oct 14.
DOI: 10.1038/s41467-022-33691-1
Abstrakt: The solid electrolyte interphase (SEI) that forms on Li-ion battery anodes is critical to their long-term performance, however observing SEI formation processes at the buried electrode-electrolyte interface is a significant challenge. Here we show that operando soft X-ray absorption spectroscopy in total electron yield mode can resolve the chemical evolution of the SEI during electrochemical formation in a Li-ion cell, with nm-scale interface sensitivity. O, F, and Si K-edge spectra, acquired as a function of potential, reveal when key reactions occur on high-capacity amorphous Si anodes cycled with and without fluoroethylene carbonate (FEC). The sequential formation of inorganic (LiF) and organic (-(C=O)O-) components is thereby revealed, and results in layering of the SEI. The addition of FEC leads to SEI formation at higher potentials which is implicated in the rapid healing of SEI defects and the improved cycling performance observed. Operando TEY-XAS offers new insights into the formation mechanisms of electrode-electrolyte interphases and their stability for a wide variety of electrode materials and electrolyte formulations.
(© 2022. The Author(s).)
Databáze: MEDLINE