Probing Depth-Dependent Transition-Metal Redox of Lithium Nickel, Manganese, and Cobalt Oxides in Li-Ion Batteries

Yu, Yang; Karayaylali, Pinar; Giordano, Livia; Corchado-García, Juan; Hwang, Jonathan; Sokaras, Dimosthenis; Maglia, Filippo; Jung, Roland; Gittleson, Forrest S.; Shao-Horn, Yang

doi:10.1021/acsami.0c16285

Title: Probing Depth-Dependent Transition-Metal Redox of Lithium Nickel, Manganese, and Cobalt Oxides in Li-Ion Batteries

Journal Article · Mon Dec 07 00:00:00 EST 2020 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.0c16285· OSTI ID:1768263

Yu, Yang ^[1]; Karayaylali, Pinar ^[1];

^[1]; Corchado-García, Juan ^[2]; Hwang, Jonathan ^[1]; Sokaras, Dimosthenis ^[3]; Maglia, Filippo ^[4];

^[4]; Gittleson, Forrest S. ^[5];

^[2]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Research Lab. of Electronics
SLAC National Accelerator Lab., Menlo Park, CA (United States)
BMW Group, München (Germany)
BMW Group Technology Office, Mountain View, CA (United States)

Layered lithium nickel, manganese, and cobalt oxides (NMC) are among the most promising commercial positive electrodes in the past decades. Understanding the detailed surface and bulk redox processes of Ni-rich NMC can provide useful insights into material design options to boost reversible capacity and cycle life. Both hard X-ray absorption (XAS) of metal K-edges and soft XAS of metal L-edges collected from charged LiNi_0.6Mn_0.2Co_0.2O₂ (NMC622) and LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) showed that the charge capacity up to removing ~0.7 Li/f.u. was accompanied with Ni oxidation in bulk and near the surface (up to 100 nm). Of significance to note is that nickel oxidation is primarily responsible for the charge capacity of NMC622 and 811 up to similar lithium removal (~0.7 Li/f.u.) albeit charged to different potentials, beyond which was followed by Ni reduction near the surface (up to 100 nm) due to oxygen release and electrolyte parasitic reactions. Overall, this observation points toward several new strategies to enhance reversible redox capacities of Ni-rich and/or Co-free electrodes for high-energy Li-ion batteries.

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Research Organization:: SLAC National Accelerator Lab., Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Renewable Power Office. Solar Energy Technologies Office

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; ACI-1548562

OSTI ID:: 1768263

Journal Information:: ACS Applied Materials and Interfaces, Vol. 12, Issue 50; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Probing Depth-Dependent Transition-Metal Redox of Lithium Nickel, Manganese, and Cobalt Oxides in Li-Ion Batteries

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