New Insights into Structural Evolution of LiNiO2 Revealed by Operando Neutron Diffraction

Chien, Po‐Hsiu; Wu, Xianyang; Song, Bohang; Yang, Zhijie; Waters, Crystal K.; Everett, Michelle S.; Lin, Feng; Du, Zhijia; Liu, Jue

doi:10.1002/batt.202100135

New Insights into Structural Evolution of LiNiO₂ Revealed by Operando Neutron Diffraction

Journal Article · Wed Sep 08 00:00:00 EDT 2021 · Batteries & Supercaps

DOI:https://doi.org/10.1002/batt.202100135· OSTI ID:1831659

^[1]; Wu, Xianyang ^[2]; ^[1]; Yang, Zhijie ^[3]; Waters, Crystal K. ^[3]; Everett, Michelle S. ^[1]; Lin, Feng ^[3]; ^[1]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Purdue Univ., West Lafayette, IN (United States)
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)

LiNiO₂ (LNO) represents the end member in the compositional space of the LiNi_1-x-yMn_xCo_yO₂ (as x and y approach zero) cathode system. Despite its high theoretical specific capacity (275 mAh/g), LNO suffers from phase transitions with large volume change and unfavorable reactions upon electrochemical cycling, which restricts its practical use in the application of lithium-ion batteries. While the contributing factor to the structural instability is commonly linked to the undesired volume collapse associated with the H2-H3 phase transition, detailed analysis of structural evolution following the entire route of phase transitions (H1-M-H2-H3) in real time under battery operating conditions remains a challenging task. In this work, we employ operando neutron diffraction to study the structural changes (crystal lattice, Li/Ni–O bond length, O–Ni–O bond angles, and LiO₂/NiO₂ layer thickness) of LNO cathode in a home-built Li_xNiO₂ || graphite full cell during Li⁺ de-/intercalation. In particular, the anomalous increase(decrease) of Ni–O(Li–O) bond length at high SOC (>~85 %) in the H3 phase is discussed in the context of O^2- (2p)→Ni⁴⁺(3d) negative charge transfer.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC05-00OR22725; EE0008444

OSTI ID:: 1831659

Alternate ID(s):: OSTI ID: 1829365

Journal Information:: Batteries & Supercaps, Journal Name: Batteries & Supercaps Journal Issue: 11 Vol. 4; ISSN 2566-6223

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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