Nanoscale state-of-charge heterogeneities within polycrystalline nickel-rich layered oxide cathode materials

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Nanoscale state-of-charge heterogeneities within polycrystalline nickel-rich layered oxide cathode materials

Tan, C; Leach, AS; Heenan, TMM; Parks, H; Jervis, R; Weker, JN; Brett, DJL; (2021) Nanoscale state-of-charge heterogeneities within polycrystalline nickel-rich layered oxide cathode materials. Cell Reports Physical Science , 2 (12) , Article 100647. 10.1016/j.xcrp.2021.100647. Green open access

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Abstract

Nickel-rich cathodes (LiNixMnyCo1-x-yO2, x > 0.6) permit higher energy in lithium-ion rechargeable batteries but suffer from accelerated degradation at potentials above 4.1 V versus Li/Li+. Here, we present a proof-of-concept in situ pouch cell and methodology for correlative 2D synchrotron transmission X-ray microscopy with 3D lab-based micro-CT. XANES analysis of the TXM data enables tracking of Ni edge energy within and between the polycrystalline NMC811 particles embedded in the operating electrode through its initial delithiation. By using edge energy as a proxy, state-of-charge heterogeneities can be tracked at the nanoscale, revealing the role of cracked particles as potential nucleation points for failure and highlighting the challenges in achieving uniform (de-)lithiation. We propose, in future work, to leverage the pouch cell design presented here for longitudinal TXM-XANES studies of nickel-rich cathodes across multiple cycles and operating variables and investigate the effect of dopants and microstructural optimization in mitigating degradation.

Type:	Article
Title:	Nanoscale state-of-charge heterogeneities within polycrystalline nickel-rich layered oxide cathode materials
Open access status:	An open access version is available from UCL Discovery
DOI:	10.1016/j.xcrp.2021.100647
Publisher version:	https://doi.org/10.1016/j.xcrp.2021.100647
Language:	English
Additional information:	This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
UCL classification:	UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering
URI:	https://discovery.ucl.ac.uk/id/eprint/10141276