Dataset Information

Prolonged lifespan of initial-anode-free lithium-metal battery by pre-lithiation in Li-rich Li₂Ni_0.5Mn_1.5O₄ spinel cathode.

ABSTRACT: Anode-free lithium metal batteries (AF-LMBs) can deliver the maximum energy density. However, achieving AF-LMBs with a long lifespan remains challenging because of the poor reversibility of Li⁺ plating/stripping on the anode. Here, coupled with a fluorine-containing electrolyte, we introduce a cathode pre-lithiation strategy to extend the lifespan of AF-LMBs. The AF-LMB is constructed with Li-rich Li₂Ni_0.5Mn_1.5O₄ cathodes as a Li-ion extender; the Li₂Ni_0.5Mn_1.5O₄ can deliver a large amount of Li⁺ in the initial charging process to offset the continuous Li⁺ consumption, which benefits the cycling performance without sacrificing energy density. Moreover, the cathode pre-lithiation design has been practically and precisely regulated using engineering methods (Li-metal contact and pre-lithiation Li-biphenyl immersion). Benefiting from the highly reversible Li metal on the Cu anode and Li₂Ni_0.5Mn_1.5O₄ cathode, the further fabricated anode-free pouch cells achieve 350 W h kg^-1 energy density and 97% capacity retention after 50 cycles.

SUBMITTER: Chen L

PROVIDER: S-EPMC9944687 | biostudies-literature | 2023 Feb

REPOSITORIES: biostudies-literature

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Prolonged lifespan of initial-anode-free lithium-metal battery by pre-lithiation in Li-rich Li2Ni0.5Mn1.5O4 spinel cathode.

Chen Leiyu L Chiang Chao-Lung CL Wu Xiaohong X Tang Yonglin Y Zeng Guifan G Zhou Shiyuan S Zhang Baodan B Zhang Haitang H Yan Yawen Y Liu Tingting T Liao Hong-Gang HG Kuai Xiaoxiao X Lin Yan-Gu YG Qiao Yu Y Sun Shi-Gang SG

Chemical science 20230125 8

Anode-free lithium metal batteries (AF-LMBs) can deliver the maximum energy density. However, achieving AF-LMBs with a long lifespan remains challenging because of the poor reversibility of Li+ plating/stripping on the anode. Here, coupled with a fluorine-containing electrolyte, we introduce a cathode pre-lithiation strategy to extend the lifespan of AF-LMBs. The AF-LMB is constructed with Li-rich Li2Ni0.5Mn1.5O4 cathodes as a Li-ion extende ...[more]

PMID: 36845937

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Project description:The high-voltage LiNi0.5Mn1.5O4 (LNMO) spinel cathode material offers high energy density storage capabilities without the use of costly Co that is prevalent in other Li-ion battery chemistries (e.g., LiNixMnyCozO2 (NMC)). Unfortunately, LNMO-containing batteries suffer from poor cycling performance because of the intrinsically coupled processes of electrolyte oxidation and transition metal dissolution that occurs at high voltage. In this work, we use operando electron paramagnetic resonance (EPR) and nuclear magnetic resonance (NMR) spectroscopies to demonstrate that transition metal dissolution in LNMO is tightly coupled to HF formation (and thus, electrolyte oxidation reactions as detected with operando and in situ solution NMR), indicative of an acid-driven disproportionation reaction that occurs during delithiation (i.e., battery charging). Leveraging the temporal resolution (s-min) of magnetic resonance, we find that the LNMO particles accelerate the rate of LiPF6 decomposition and subsequent Mn2+ dissolution, possibly due to the acidic nature of terminal Mn-OH groups. X-ray photoemission electron microscopy (XPEEM) provides surface-sensitive and localized X-ray absorption spectroscopy (XAS) measurements, in addition to X-ray photoelectron spectroscopy (XPS), that indicate disproportionation is enabled by surface reconstruction upon charging, which leads to surface Mn3+ sites on the LNMO particle surface that can disproportionate into Mn2+(dissolved) and Mn4+(s). During discharge of the battery, we observe high quantities of metal fluorides (in particular, MnF2) in the cathode electrolyte interphase (CEI) on LNMO as well as the conductive carbon additives in the composite. Electronic conductivity measurements indicate that the MnF2 decreases film conductivity by threefold compared to LiF, suggesting that this CEI component may impede both the ionic and electronic properties of the cathode. Ultimately, to prevent transition metal dissolution and the associated side reactions in spinel-type cathodes (particularly those that operate at high voltages like LNMO), the use of electrolytes that offer improved anodic stability and prevent acid byproducts will likely be necessary.

Dataset Information

Prolonged lifespan of initial-anode-free lithium-metal battery by pre-lithiation in Li-rich Li₂Ni_0.5Mn_1.5O₄ spinel cathode.

Publications

Prolonged lifespan of initial-anode-free lithium-metal battery by pre-lithiation in Li-rich Li<sub>2</sub>Ni<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub> spinel cathode.

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