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

DOI: 10.1016/j.xcrp.2021.100647 DOI Help

Authors: Chun Tan (University College London) , Andrew S. Leach (University College London; The Faraday Institution) , Thomas M. M. Heenan (University College London; The Faraday Institution) , Huw Parks (University College London; The Faraday Institution) , Rhodri Jervis (University College London; The Faraday Institution) , Johanna Nelson Weker (Stanford Synchrotron Radiation Lightsource) , Daniel J. I. Brett (University College London; The Faraday Institution) , Paul R. Shearing (University College London; The Faraday Institution)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Cell Reports Physical Science , VOL 3

State: Published (Approved)
Published: November 2021
Diamond Proposal Number(s): 24178

Open Access Open Access

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.

Journal Keywords: lithium-ion batteries; transmission X-ray microscopy; XANES-CT; X-ray absorption spectroscopy; X-ray tomography

Diamond Keywords: Batteries; Lithium-ion

Subject Areas: Materials, Chemistry, Energy

Instruments: B18-Core EXAFS

Other Facilities: 6-2c at Stanford Synchrotron Radiation Lightsource

Added On: 16/11/2021 19:26


Discipline Tags:

Energy Storage Energy Physical Chemistry Energy Materials Chemistry Materials Science

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) X-ray Absorption Near Edge Structure (XANES)