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Hollow-core optical fibre sensors for operando Raman spectroscopy investigation of Li-ion battery liquid electrolytes

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Miele, Ermanno 
Dose, Wesley 
Manyakin, Ilya 
Frosz, Michael 
Ruff, Zachary 


Improved analytical tools are urgently required to identify degradation and failure mechanisms in Li-ion batteries. However, understanding and ultimately avoiding these detrimental mechanisms requires continuous tracking of complex electrochemical processes in different battery components. Here, we report an operando spectroscopy method that enables monitoring the chemistry of a carbonate-based liquid electrolyte during electrochemical cycling in Li-ion batteries with a graphite anode and a LiNi0.8Mn0.1Co0.1O2 cathode. By embedding a hollow-core optical fibre probe inside a lab-scale pouch cell, we demonstrate the effective evolution of the liquid electrolyte species by background-free Raman spectroscopy. The analysis of the spectroscopy measurements reveals changes in the ratio of carbonate solvents and electrolyte additives as a function of the cell voltage and show the potential to track the lithium-ion solvation dynamics. The proposed operando methodology contributes to understanding better the current Li-ion battery limitations and paves the way for studies of the degradation mechanisms in different electrochemical energy storage systems.


Funder: Faraday Institution, grant reference: FIRG001

Funder: Faraday Institution, grant reference: FIRG001 Winton Programme for the Physics of Sustainability (Cambridge University)


Article, /639/624/1107/527/1821, /639/4077/4079/891, /639/624/1075/187, /639/301/930, /639/4077/4079, /140/133, /120, /128, article

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Nature Communications

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Nature Research
This work is supported by the Faraday Institution under grant no. FIRG001 (EM, WMD, ZR, MDV, CPG, JJB, TGE) and the Winton Programme for the Physics of Sustainability (EM, TGE).