Atomic-Level Understanding of Surface Reconstruction Based on Li[NixMnyCo1–x–y]O2 Single-Crystal Studies

Zhu, Jian; Sharifi-Asl, Soroosh; Garcia, Juan C.; Iddir, Hakim H.; Croy, Jason R.; Shahbazian-Yassar, Reza; Chen, Guoying

doi:10.1021/acsaem.0c00411

Title: Atomic-Level Understanding of Surface Reconstruction Based on Li[Ni_xMn_yCo_1–x–y]O₂ Single-Crystal Studies

Journal Article · Thu Apr 30 00:00:00 EDT 2020 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.0c00411· OSTI ID:1660390

Zhu, Jian ^[1];

^[2];

^[3];

^[2];

^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of Illinois, Chicago, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

The stability of cathode particle surfaces that are directly exposed to the electrolyte is one of the most crucial and determining factors for cathode performance at high operating voltages. Theory has predicted a strong dependence of surface stability on chemical compositions as well as surface facets of layered oxides, yet conflicting results on the correlations exist as most experimental studies focus on cycled secondary particles recovered from composite electrodes. Here, we synthesize well-formed Li[Ni_xMn_yCo_1–x–y]O₂ (NMC) single-crystal samples, carefully define pristine surface properties, and then monitor their evolution with cycling. Atomic-resolution scanning transmission electron microscopy (STEM) imaging and electron energy loss spectroscopy (EELS) analysis show the formation of a surface reconstruction layer (SRL) as well as an extended surface reduction layer on pristine, Li-permeable non-(001) surfaces, even before cycling. We reveal a transition region with chemical gradient, in which the layered structure gradually densifies and eventually transforms into the SRL on the top surface. Contrary to these observations, no SRL is observed on pristine, Li-impermeable (001) surfaces, revealing the facet-dependent nature of surface reconstructions during particle synthesis. Upon electrochemical cycling, significant composition-and facet-dependent SRL growth is observed. The driving force and mechanism for surface reconstruction are further discussed. The present study provides insights into the origin as well as the nature of SRLs, highlighting the significance of surface engineering in cathode material optimization.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; AC02-05CH11231; CBET-1805938

OSTI ID:: 1660390

Journal Information:: ACS Applied Energy Materials, Vol. 3, Issue 5; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 31 works

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25 ENERGY STORAGE
Li-ion battery cathodes
Li[NixMnyCo1-x-y]O2 (NMC)
composition-dependent
single crystals
surface reconstruction
surface-face dependent

Title: Atomic-Level Understanding of Surface Reconstruction Based on Li[NixMnyCo1–x–y]O2 Single-Crystal Studies

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Title: Atomic-Level Understanding of Surface Reconstruction Based on Li[Ni_xMn_yCo_1–x–y]O₂ Single-Crystal Studies