Regulating Cation Interactions for Zero–Strain and High–Voltage P2–type Na2/3Li1/6Co1/6Mn2/3O2 Layered Oxide Cathodes of Sodium–Ion Batteries

Zou, Peichao; Yao, Libing; Wang, Chunyang; Lee, Sang Jun; Li, Tianyi; Xin, Huolin L.

doi:10.1002/anie.202304628

Regulating Cation Interactions for Zero–Strain and High–Voltage P2–type Na_2/3Li_1/6Co_1/6Mn_2/3O₂ Layered Oxide Cathodes of Sodium–Ion Batteries

Journal Article · Wed May 03 00:00:00 EDT 2023 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202304628· OSTI ID:1998180

Zou, Peichao ^[1]; Yao, Libing ^[2]; Wang, Chunyang ^[2]; Lee, Sang Jun ^[3]; Li, Tianyi ^[4]; ^[2]

Univ. of California, Irvine, CA (United States); SLAC
Univ. of California, Irvine, CA (United States)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Deep sodium extraction/insertion of sodium cathodes usually causes undesired Jahn–Teller distortion and phase transition, both of which will reduce structural stability and lead to poor long-cycle reliability. Here we report a zero-strain P2- Na_2/3Li1/6Co_1/6Mn_2/3O₂ cathode, in which the lithium/cobalt substitution contributes to reinforcing the host structure by reducing the Mn³⁺/Mn⁴⁺ redox, mitigating the Jahn–Teller distortion, and minimizing the lattice change. 94.5 % of Na⁺ in the unit structure can be reversibly cycled with a charge cut-off voltage of 4.5 V (vs. Na⁺/Na). Impressively, a solid-solution reaction without phase transitions is realized upon deep sodium (de)intercalation, which poses a minimal volume deviation of 0.53 %. Finally, it attains a high discharge capacity of 178 mAh g^–1, a high energy density of 534 Wh kg^–1, and excellent capacity retention of 95.8 % at 1 C after 250 cycles.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; SC0012704; SC0021204

OSTI ID:: 1998180

Alternate ID(s):: OSTI ID: 2404842

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 28 Vol. 62; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Regulating Cation Interactions for Zero–Strain and High–Voltage P2–type Na2/3Li1/6Co1/6Mn2/3O2 Layered Oxide Cathodes of Sodium–Ion Batteries

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Regulating Cation Interactions for Zero–Strain and High–Voltage P2–type Na_2/3Li_1/6Co_1/6Mn_2/3O₂ Layered Oxide Cathodes of Sodium–Ion Batteries