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Instruments / Technical Area	Publication Details	Published	Actions
B07-B1-Versatile Soft X-ray beamline: High Throughput ES1 I10-Beamline for Advanced Dichroism - scattering I20-Scanning-X-ray spectroscopy (XAS/XES)	Distinguishing bulk redox from near-surface degradation in lithium nickel oxide cathodes Lijin An , Ruomu Zhang , Prvanin N. Didwal , Michael W. Fraser , Leanne A. H. Jones , Conor M. E. Phelan , Namrata Ramesh , Grant Harris , Robert S. Weatherup , Jack E. N. Swallow , Peixi Cong , Andrey Poletayev , Erik Bjorklund , Christophe J. Sahle , Pilar Ferrer , David C. Grinter , Peter Bencok , Shusaku Hayama , Saiful Islam , Robert House , Peter D. Nellist , Robert J. Green , Rebecca J. Nicholls Energy & Environmental Science DOI: 10.1039/D4EE02398F Diamond Proposal Number(s): [33283, 33062, 32010] Open Access Show Abstract ▼ Abstract: Ni-rich layered oxide cathodes can deliver higher energy density batteries, but uncertainties remain over their charge compensation mechanisms and the degradation processes that limit cycle life. Trapped molecular O2 has been identified within LiNiO2 at high states of charge, as seen for Li-rich cathodes where excess capacity is associated with reversible O-redox. Here we show that bulk redox in LiNiO2 occurs by Ni-O rehybridization, lowering the electron density on O sites, but importantly without the involvement of molecular O2. Instead, trapped O2 is related to degradation at surfaces in contact with the electrolyte, and is accompanied by Ni reduction. O2 is removed on discharge, but excess Ni2+ persists forming a reduced surface layer, associated with impeded Li transport. This implicates the instability of delithiated LiNiO2 in contact with the electrolyte in surface degradation through O2 formation and Ni reduction, highlighting the importance of surface stabilisation strategies in suppressing LNO degradation.	Sep 2024

Instruments / Technical Area

Publication Details

Published

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B07-B1-Versatile Soft X-ray beamline: High Throughput ES1
I10-Beamline for Advanced Dichroism - scattering
I20-Scanning-X-ray spectroscopy (XAS/XES)

Distinguishing bulk redox from near-surface degradation in lithium nickel oxide cathodes