Depth-Dependent Redox Behavior of LiNi 0.6 Mn 0.2 Co 0.2 O 2

Tian, Chixia; Nordlund, Dennis; Xin, Huolin L.; Xu, Yahong; Liu, Yijin; Sokaras, Dimosthenis; Lin, Feng; Doeff, Marca M.

doi:10.1149/2.1021803jes

Title: Depth-Dependent Redox Behavior of LiNi _0.6 Mn _0.2 Co _0.2 O ₂

Journal Article · Thu Feb 08 00:00:00 EST 2018 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/2.1021803jes· OSTI ID:1425689

Tian, Chixia; Nordlund, Dennis; Xin, Huolin L.; Xu, Yahong; Liu, Yijin; Sokaras, Dimosthenis;

;

Nickel-rich layered materials are emerging as cathodes of choice for next-generation high energy density lithium ion batteries intended for electric vehicles. This is because of their higher practical capacities compared to compositions with lower Ni content, as well as the potential for lower raw materials cost. The higher practical capacity of these materials comes at the expense of shorter cycle life, however, due to undesirable structure and chemical transformations, especially at particle surfaces. To understand these changes more fully, the charge compensation mechanism and bulk and surface structural changes of LiNi0.6Mn0.2Co0.2O2 were probed using synchrotron techniques and electron energy loss spectroscopy in this study. In the bulk, both the crystal and electronic structure changes are reversible upon cycling to high voltages, whereas particle surfaces undergo significant reduction and structural reconstruction. While Ni is the major contributor to charge compensation, Co and O (through transition metal-oxygen hybridization) are also redox active. An important finding from depth-dependent transition metal L-edge and O K-edge X-ray spectroscopy is that oxygen redox activity exhibits depth-dependent characteristics. This likely drives the structural and chemical transformations observed at particle surfaces in Ni-rich materials.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0012704; AC02-76SF00515

OSTI ID:: 1425689

Alternate ID(s):: OSTI ID: 1458538; OSTI ID: 1466615; OSTI ID: 1466712

Report Number(s):: BNL-207961-2018-JAAM; /jes/165/3/A696.atom

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Vol. 165 Journal Issue: 3; ISSN 0013-4651

Publisher:: IOP Publishing - The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 106 works

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