Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides

Enyue Zhao; Qinghao Li; Fanqi Meng; Jue Liu; Junyang Wang; Lunhua He; Zheng Jiang; Qinghua Zhang; Xiqian Yu; Lin Gu; Wanli Yang; Hong Li; Fangwei Wang; Xuejie Huang

doi:10.1002/anie.201900444

Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides

Enyue Zhao, Qinghao Li, Fanqi Meng, Jue Liu, Junyang Wang, Lunhua He, Zheng Jiang, Qinghua Zhang, Xiqian Yu, Lin Gu, Wanli Yang, Hong Li, Fangwei Wang, Xuejie Huang

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126 Scopus citations

Abstract

Lattice-oxygen redox (l-OR) has become an essential companion to the traditional transition-metal (TM) redox charge compensation to achieve high capacity in Li-rich cathode oxides. However, the understanding of l-OR chemistry remains elusive, and a critical question is the structural effect on the stability of l-OR reactions. Herein, the coupling between l-OR and structure dimensionality is studied. We reveal that the evolution of the oxygen-lattice structure upon l-OR in Li-rich TM oxides which have a three-dimensional (3D)-disordered cation framework is relatively stable, which is in direct contrast to the clearly distorted oxygen-lattice framework in Li-rich oxides which have a two-dimensional (2D)/3D-ordered cation structure. Our results highlight the role of structure dimensionality in stabilizing the oxygen lattice in reversible l-OR, which broadens the horizon for designing high-energy-density Li-rich cathode oxides with stable l-OR chemistry.

Original language	English
Pages (from-to)	4323-4327
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	58
Issue number	13
DOIs	https://doi.org/10.1002/anie.201900444
State	Published - Mar 22 2019

Funding

This work was supported by funding from National Key R&D Program of China (2016YFA0202500), Foundation for Innovative Research Groups of the NSFC (No. 51421002), NSFC (No. 11675255, 51502334, 51822211). This work used resources of the ALS, which is a US DOE Office of Science User Facility, W.Y. acknowledges support from EERE VTO under the Applied Battery Materials Program of the US DOE, both under Contract No. DE-AC02-05CH11231.

Keywords

cathodes
lattice oxygen redox
lithium-ion batteries
oxides
structural dimensionality

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10.1002/anie.201900444

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Zhao, E., Li, Q., Meng, F., Liu, J., Wang, J., He, L., Jiang, Z., Zhang, Q., Yu, X., Gu, L., Yang, W., Li, H., Wang, F., & Huang, X. (2019). Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides. Angewandte Chemie - International Edition, 58(13), 4323-4327. https://doi.org/10.1002/anie.201900444

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title = "Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides",

abstract = "Lattice-oxygen redox (l-OR) has become an essential companion to the traditional transition-metal (TM) redox charge compensation to achieve high capacity in Li-rich cathode oxides. However, the understanding of l-OR chemistry remains elusive, and a critical question is the structural effect on the stability of l-OR reactions. Herein, the coupling between l-OR and structure dimensionality is studied. We reveal that the evolution of the oxygen-lattice structure upon l-OR in Li-rich TM oxides which have a three-dimensional (3D)-disordered cation framework is relatively stable, which is in direct contrast to the clearly distorted oxygen-lattice framework in Li-rich oxides which have a two-dimensional (2D)/3D-ordered cation structure. Our results highlight the role of structure dimensionality in stabilizing the oxygen lattice in reversible l-OR, which broadens the horizon for designing high-energy-density Li-rich cathode oxides with stable l-OR chemistry.",

keywords = "cathodes, lattice oxygen redox, lithium-ion batteries, oxides, structural dimensionality",

author = "Enyue Zhao and Qinghao Li and Fanqi Meng and Jue Liu and Junyang Wang and Lunhua He and Zheng Jiang and Qinghua Zhang and Xiqian Yu and Lin Gu and Wanli Yang and Hong Li and Fangwei Wang and Xuejie Huang",

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Zhao, E, Li, Q, Meng, F, Liu, J, Wang, J, He, L, Jiang, Z, Zhang, Q, Yu, X, Gu, L, Yang, W, Li, H, Wang, F & Huang, X 2019, 'Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides', Angewandte Chemie - International Edition, vol. 58, no. 13, pp. 4323-4327. https://doi.org/10.1002/anie.201900444

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T1 - Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides

AU - Zhao, Enyue

AU - Li, Qinghao

AU - Meng, Fanqi

AU - Liu, Jue

AU - Wang, Junyang

AU - He, Lunhua

AU - Jiang, Zheng

AU - Zhang, Qinghua

AU - Yu, Xiqian

AU - Gu, Lin

AU - Yang, Wanli

AU - Li, Hong

AU - Wang, Fangwei

AU - Huang, Xuejie

PY - 2019/3/22

Y1 - 2019/3/22

N2 - Lattice-oxygen redox (l-OR) has become an essential companion to the traditional transition-metal (TM) redox charge compensation to achieve high capacity in Li-rich cathode oxides. However, the understanding of l-OR chemistry remains elusive, and a critical question is the structural effect on the stability of l-OR reactions. Herein, the coupling between l-OR and structure dimensionality is studied. We reveal that the evolution of the oxygen-lattice structure upon l-OR in Li-rich TM oxides which have a three-dimensional (3D)-disordered cation framework is relatively stable, which is in direct contrast to the clearly distorted oxygen-lattice framework in Li-rich oxides which have a two-dimensional (2D)/3D-ordered cation structure. Our results highlight the role of structure dimensionality in stabilizing the oxygen lattice in reversible l-OR, which broadens the horizon for designing high-energy-density Li-rich cathode oxides with stable l-OR chemistry.

AB - Lattice-oxygen redox (l-OR) has become an essential companion to the traditional transition-metal (TM) redox charge compensation to achieve high capacity in Li-rich cathode oxides. However, the understanding of l-OR chemistry remains elusive, and a critical question is the structural effect on the stability of l-OR reactions. Herein, the coupling between l-OR and structure dimensionality is studied. We reveal that the evolution of the oxygen-lattice structure upon l-OR in Li-rich TM oxides which have a three-dimensional (3D)-disordered cation framework is relatively stable, which is in direct contrast to the clearly distorted oxygen-lattice framework in Li-rich oxides which have a two-dimensional (2D)/3D-ordered cation structure. Our results highlight the role of structure dimensionality in stabilizing the oxygen lattice in reversible l-OR, which broadens the horizon for designing high-energy-density Li-rich cathode oxides with stable l-OR chemistry.

KW - cathodes

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KW - lithium-ion batteries

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Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides

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