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Transition metal-doped Ni-rich layered cathode materials for durable Li-ion batteries.

ABSTRACT: Doping is a well-known strategy to enhance the electrochemical energy storage performance of layered cathode materials. Many studies on various dopants have been reported; however, a general relationship between the dopants and their effect on the stability of the positive electrode upon prolonged cell cycling has yet to be established. Here, we explore the impact of the oxidation states of various dopants (i.e., Mg²⁺, Al³⁺, Ti⁴⁺, Ta⁵⁺, and Mo⁶⁺) on the electrochemical, morphological, and structural properties of a Ni-rich cathode material (i.e., Li[Ni_0.91Co_0.09]O₂). Galvanostatic cycling measurements in pouch-type Li-ion full cells show that cathodes featuring dopants with high oxidation states significantly outperform their undoped counterparts and the dopants with low oxidation states. In particular, Li-ion pouch cells with Ta⁵⁺- and Mo⁶⁺-doped Li[Ni_0.91Co_0.09]O₂ cathodes retain about 81.5% of their initial specific capacity after 3000 cycles at 200 mA g^-1. Furthermore, physicochemical measurements and analyses suggest substantial differences in the grain geometries and crystal lattice structures of the various cathode materials, which contribute to their widely different battery performances and correlate with the oxidation states of their dopants.

SUBMITTER: Sun HH

PROVIDER: S-EPMC8589951 | biostudies-literature | 2021 Nov

REPOSITORIES: biostudies-literature

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Transition metal-doped Ni-rich layered cathode materials for durable Li-ion batteries.

Sun H Hohyun HH Kim Un-Hyuck UH Park Jeong-Hyeon JH Park Sang-Wook SW Seo Dong-Hwa DH Heller Adam A Mullins C Buddie CB Yoon Chong S CS Sun Yang-Kook YK

Nature communications 20211112 1

Doping is a well-known strategy to enhance the electrochemical energy storage performance of layered cathode materials. Many studies on various dopants have been reported; however, a general relationship between the dopants and their effect on the stability of the positive electrode upon prolonged cell cycling has yet to be established. Here, we explore the impact of the oxidation states of various dopants (i.e., Mg2+, Al3+, Ti4+, Ta5+, and Mo6+</ ...[more]

PMID: 34772958

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Project description:The chemical and electrochemical reactions at the positive electrode-electrolyte interface in Li-ion batteries are hugely influential on cycle life and safety. Ni-rich layered transition metal oxides exhibit higher interfacial reactivity than their lower Ni-content analogues, reacting via mechanisms that are poorly understood. Here, we study the pivotal role of the electrolyte solvent, specifically cyclic ethylene carbonate (EC) and linear ethyl methyl carbonate (EMC), in determining the interfacial reactivity at charged LiNi0.33Mn0.33Co0.33O2 (NMC111) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes by using both single-solvent model electrolytes and the mixed solvents used in commercial cells. While NMC111 exhibits similar parasitic currents with EC-containing and EC-free electrolytes during high voltage holds in NMC/Li4Ti5O12 (LTO) cells, this is not the case for NMC811. Online gas analysis reveals that the solvent-dependent reactivity for Ni-rich cathodes is related to the extent of lattice oxygen release and accompanying electrolyte decomposition, which is higher for EC-containing than EC-free electrolytes. Combined findings from electrochemical impedance spectroscopy (EIS), TEM, solution NMR, ICP, and XPS reveal that the electrolyte solvent has a profound impact on the degradation of the Ni-rich cathode and the electrolyte. Higher lattice oxygen release with EC-containing electrolytes is coupled with higher cathode interfacial impedance, a thicker oxygen-deficient rock-salt surface reconstruction layer, more electrolyte solvent and salt breakdown, and higher amounts of transition metal dissolution. These processes are suppressed in the EC-free electrolyte, highlighting the incompatibility between Ni-rich cathodes and conventional electrolyte solvents. Finally, new mechanistic insights into the chemical oxidation pathways of electrolyte solvents and, critically, the knock-on chemical and electrochemical reactions that further degrade the electrolyte and electrodes curtailing battery lifetime are provided.

Dataset Information

Transition metal-doped Ni-rich layered cathode materials for durable Li-ion batteries.

Publications

Transition metal-doped Ni-rich layered cathode materials for durable Li-ion batteries.

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