Revisiting the charge compensation mechanisms in LiNi0.8Co0.2−yAlyO2 systems

Zachary W Lebens-Higgins; Nicholas V Faenza; Maxwell D Radin; Hao Liu; Shawn Sallis; Jatinkumar Rana; Julija Vinckeviciute; Philip J Reeves; Mateusz J Zuba; Fadwa Badway; Nathalie Pereira; Karena W Chapman; Tien-Lin Lee; Tianpin Wu; Clare P Grey; Brent C Melot; Anton Van Der Ven; Glenn G Amatucci; Wanli Yang; Louis F. J Piper; Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES)

doi:10.1039/C9MH00765B

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Revisiting the charge compensation mechanisms in LiNi0.8Co0.2−yAlyO2 systems

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Revisiting the charge compensation mechanisms in LiNi0.8Co0.2−yAlyO2 systems

Zachary W Lebens-Higgins, Nicholas V Faenza, Maxwell D Radin, Hao Liu, Shawn Sallis, Jatinkumar Rana, Julija Vinckeviciute, Philip J Reeves, Mateusz J Zuba, Fadwa Badway, …

Materials horizons, Vol.6(10), pp.2112-2123

11/18/2019

DOI: https://doi.org/10.1039/C9MH00765B

Abstract

Oxygen participation, arising from increased transition metal–oxygen covalency during delithiation, is considered essential for the description of charge compensation in conventional layered oxides. The advent of high-resolution mapping of the O K-edge resonant inelastic X-ray scattering (RIXS) provides an opportunity to revisit the onset and extent of oxygen participation. Combining RIXS with an array of structural and electronic probes for the family of Ni-rich LiNi0.8Co0.2−yAlyO2 cathodes, we identify common charge compensation regimes that are assigned to formal transition metal redox (<4.25 V) and oxygen participation through covalency (>4.25 V). From O K-edge RIXS maps, we find the emergence of a sharp RIXS feature in these systems when approaching full delithiation, which has previously been associated with lattice oxidized oxygen in alkali-rich systems. The lack of transition metal redox signatures and strong covalency at these high degrees of delithiation suggest this RIXS feature is similarly attributed to lattice oxygen charge compensation as in the alkali-rich systems. The RIXS feature's evolution with state of charge in conventional layered oxides is evidence that this feature reflects the depopulation of occupied O 2p states associated with oxygen participation.

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Title: Revisiting the charge compensation mechanisms in LiNi0.8Co0.2−yAlyO2 systems
Creators: Zachary W Lebens-Higgins - Department of Physics, Applied Physics, and Astronomy, Binghamton University, New York 13902, USA
Nicholas V Faenza - Energy Storage Research Group, Department of Materials Science and Engineering, Rutgers University, North Brunswick, New Jersey 08902
Maxwell D Radin - Materials Department, University of California Santa Barbara, Santa Barbara, USA
Hao Liu - Department of Chemistry, Binghamton University, New York 13902, USA
Shawn Sallis - Materials Science & Engineering, Binghamton University, Binghamton, USA, Advanced Light Source
Jatinkumar Rana - Department of Physics, Applied Physics, and Astronomy, Binghamton University, New York 13902, USA
Julija Vinckeviciute - Materials Department, University of California Santa Barbara, Santa Barbara, USA
Philip J Reeves - Department of Chemistry, University of Cambridge, Cambridge, UK
Mateusz J Zuba - Materials Science & Engineering, Binghamton University, Binghamton, USA
Fadwa Badway - Energy Storage Research Group, Department of Materials Science and Engineering, Rutgers University, North Brunswick, New Jersey 08902
Nathalie Pereira - Energy Storage Research Group, Department of Materials Science and Engineering, Rutgers University, North Brunswick, New Jersey 08902
Karena W Chapman - Department of Chemistry, Stony Brook University, Stony Brook, USA
Tien-Lin Lee - Diamond Light Source Ltd., Diamond House, Harwell Science and Innovation Campus, Didcot, UK
Tianpin Wu - X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, USA
Clare P Grey - Department of Chemistry, University of Cambridge, Cambridge, UK
Brent C Melot - Department of Chemistry, University of Southern California, Los Angeles, USA
Anton Van Der Ven - Materials Department, University of California Santa Barbara, Santa Barbara, USA
Glenn G Amatucci - Energy Storage Research Group, Department of Materials Science and Engineering, Rutgers University, North Brunswick, New Jersey 08902
Wanli Yang - Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, USA
Louis F. J Piper - Department of Physics, Applied Physics, and Astronomy, Binghamton University, New York 13902, USA
Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES)
Publication Details: Materials horizons, Vol.6(10), pp.2112-2123
Date published: 11/18/2019
Academic Unit: Materials Science and Engineering (SOE)
Language: English
Resource Type: Journal article
Identifiers: 991031654799504646