Operando Characterization of Lithium-Ion Batteries using Lab-Scale X-ray Emission/Absorption Spectroscopy

Tracking changes in the electronic structure of target elements is crucial to investigate the nature of redox reactions occurring in battery electrodes. Core-hole characterization techniques such as X-ray Emission Spectroscopy (XES) and X-ray Absorption Fine Structure (XAFS) perform this role well through the generation/quenching of core holes in the sample. Laboratory-based core hole x-ray spectroscopy techniques have recently gained popularity as they are more accessible and provide energy resolution close to that of a synchrotron source. In this study, the use of a lab-scale XAFS/XES to investigate the change in the electronic structure around transition elements present in electrode materials for lithium-ion storage is explored under operando conditions. This enables real-time monitoring of chemical shifts resulting from changing electrode potential. The relationship between energy shifts and oxidation/spin state is obtained using K-edge XANES and Kβ1,3 XES measurements of transition metals present using reference compounds. This relationship is utilized to predict the change in chemical environment during the cycling of cathode/anode materials for energy storage. Additionally, the spin sensitivity of Kα and Kβ fluorescence is utilized to explore the magnetic behavior of LCO cathodes in the first 10% of lithium removal along with K-edge XAFS for oxygen and cobalt to investigate local and electronic structure changes.

Level thesis:degree_level

Masters

Department dc:contributor.department

Materials Science and Engineering

Grantor dc:publisher

Georgia Institute of Technology

Year dc:date.issued

2023

Author dc:creator

• Krishnan, Abiram

Advisor dc:contributor.advisor

• Alamgir, Faisal M.

Committee members dc:contributor.committeemember

• Yushin, Gleb
• Srinivasarao, Mohan
• Toor, Anju

• XES
• XAFS
• Spin structure
• Li-Ion Batteries
• operando
• electronic structure

Language dc:language.iso

en_US

Handle dc:identifier.uri

https://hdl.handle.net/1853/75083

OAI identifier oai:identifier

oai:repository.gatech.edu:1853/75083