The Phase Evolution and Degradation Modes of $ R\overline{3}$m LixNi1-y-zCoyAlzO2 Electrodes Cycled Near Complete Delithiation

Faenza, Nicholas V.; Pereira, Nathalie; Halat, David M.; Vinckeviciute, Julija; Bruce, Lejandro; Radin, Maxwell D.; Mukherjee, Pinaki; Badway, Fadwa; Halajko, Anna; Cosandey, Frederic; Grey, Clare P.; Van der Ven, Anton; Amatucci, Glenn G.

doi:10.1021/acs.chemmater.8b02720

Title: The Phase Evolution and Degradation Modes of $$ R\overline{3}$$m Li_xNi_1-y-zCo_yAl_zO₂ Electrodes Cycled Near Complete Delithiation

Journal Article · Tue Oct 09 00:00:00 EDT 2018 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.8b02720· OSTI ID:1477223

^[1]; Pereira, Nathalie ^[1];

^[2];

^[3]; Bruce, Lejandro ^[1]; Radin, Maxwell D. ^[3];

^[4]; Badway, Fadwa ^[1]; Halajko, Anna ^[1]; Cosandey, Frederic ^[4];

^[2]; Van der Ven, Anton ^[3];

^[1]

Rutgers Univ., North Brunswick, NJ (United States)
Univ. of Cambridge (United Kingdom)
Univ. of California, Santa Barbara, CA (United States)
Rutgers Univ., Piscataway, NJ (United States)

We report that the practical utilization of energy densities near the theoretical limit for $$ R\overline{3}m$$ layered oxide positive electrode materials is dependent on the stability of the electrochemical performance of these materials at or near full delithiation. In order to develop new chemistries and novel approaches towards the improvement of the electrochemical performance of these materials at such high states of charge, a robust understanding of the failure mechanisms limiting current materials is necessary. Thorough analysis of Li_xCo_1-yAl_yO₂ and Li_xNi_1-yAl_yO₂ as well as Li_xNi_0.8Co_0.2O₂ and Li_xNi_0.8Co_0.15Al_0.05O₂ (1 ≥ x ≥ 0 and 0.2 ≥ y ≥ 0) enabled the identification of key relationships between the transition metal chemistry of the electrode, its structural stability, and cycling characteristics at or near complete delithiation (4.75 V). Extensive characterization of these materials was achieved by a multitude of physical and electrochemical techniques to investigate the relative importance of surface vs. bulk phenomena. Here, the resulting insights derived from these analyses highlight the importance of the intrinsic structural and mechanical stability of the electrode when highly delithiated and establish guidelines for identifying positive electrode materials with improved high state of charge performance. Lastly, particularly important is the contrasting electrochemical impact of Al substitution into LiCoO₂- and LiNiO₂-based materials, which is shown to likely arise from the enhanced propensity for Al ions to migrate to the tetrahedral site in Co-rich compounds at high states of delithiation.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES); Rutgers Univ., New Brunswick, NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012583

OSTI ID:: 1477223

Journal Information:: Chemistry of Materials, Vol. 30, Issue 21; Related Information: Supplemental information for The Phase Evolution and Degradation Modes of R3 ̅m LixNi1-y-zCoyAlzO2 Electrodes Cycled Near Complete Delithiation; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 22 works

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