Revealing the Role, Mechanism, and Impact of AlF<sub>3</sub> Coatings on the Interphase of Silicon Thin Film Anodes

Adhitama, Egy; Wickeren, Stefan van; Neuhaus, Kerstin; Frankenstein, Lars; Demelash, Feleke; Javed, Atif; Haneke, Lukas; Nowak, Sascha; Winter, Martin; Gómez-Martín, Aurora; Placke, Tobias

doi:10.1002/aenm.202201859

Cited by 20 publications

(15 citation statements)

References 74 publications

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“…The thickness of the products was adjusted by changing the deposition time. [64][65][66] Crystalline porous aluminium phosphonate material (AlPIm) was synthesized by using iminodi (methylphosphonic acid) as the organophosphorus source under simple hydrothermal reaction conditions followed by the synthesis of lithium doped aluminium phosphonate (LiAlPIm) through sonication of AlPIm in Li-salt taken in water. The AlPIm shows a flake-like morphology with a dimension of 100-130 nm.…”

Section: Other Al-based Materialsmentioning

confidence: 99%

“…Particularly after lithiation, AlF 3 also possesses relatively high ionic conductivity, resulting in enhanced reaction kinetics. 64 Al foil has also been propelled to the forefront in the investigations of LIBs as a multifunctional sub-unit. Kwon et al deposited layers of nanoporous graphene (NPG) on the top of the surface of Al thin films employed as an anode for LIBs.…”

Section: Al-based Electrodes For Libsmentioning

confidence: 99%

Section: Al-based Electrodes For Lmbsmentioning

confidence: 99%

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Al-based materials for advanced lithium rechargeable batteries: recent progress and prospects

Sun

Yin

Yang

et al. 2023

Mater. Chem. Front.

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Section: Other Al-based Materialsmentioning

confidence: 99%

Section: Al-based Electrodes For Libsmentioning

confidence: 99%

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Al-based materials for advanced lithium rechargeable batteries: recent progress and prospects

Sun

Yin

Yang

et al. 2023

Mater. Chem. Front.

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“…Lithium-free oxides 26−30 (e.g., Al 2 O 3 , ZnO, ZrO, and TiO 2 ) and fluorides 31,32 (e.g., MgF 2 and AlF 3 ) are two classes of materials that have been heavily investigated as coating materials for anodes and cathodes. Materials of both classes are relatively poor ionic conductors, even until they are fully lithiated, along with Li wastage.…”

Section: Introductionmentioning

confidence: 99%

Atomic/Molecular Layer-Deposited Laminated Li₂O–Lithicone Interfaces Enabling High-Performance Silicon Anodes

Fang¹,

Li²,

Qin³

et al. 2023

ACS Appl. Mater. Interfaces

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Silicon-based materials are of long-standing interest as the anodes for next-generation lithium-ion batteries, yet their low initial Coulombic efficiency and poor interfacial stability are lethal limitations. In this work, we used atomic layer deposition (ALD) and molecular layer deposition (MLD) techniques to fabricate a lithium-containing laminated Li 2 O−lithicone hybrid film (∼5 nm) on a silicon electrode. The laminated film provides an additional surface Li source around silicon cores, which can partially reimburse the Li loss during battery cycling. Characterization of interfacial components shows that such a laminated Li 2 O−lithicone interface undergoes gentle element changes and participates in a hybrid solid electrolyte interphase with Li 2 CO 3 , Li 2 O, Li x POF y , and LiF species. Finite element model analysis and morphology characterization demonstrate that the laminated structure design can help relieve the interfacial stress and thus retain the integrity and reactivity of the silicon composite anode during cycling. Moreover, the lithium-based laminated film leads to a fast Li + migration kinetics on the surface of the electrode as revealed by the galvanostatic intermittent titration technique and density functional theory calculation. Benefiting from the above merits, a silicon anode with a 91.2% initial Coulombic efficiency, a rate performance of 1460 mA h g −1 at 2 A g −1 , and a reversible capacity over 646 mA h g −1 after 850 cycles was achieved. This work exemplifies the advantages of lithium-based hybrid films precisely engineered by ALD/MLD techniques for improving performances of advanced silicon anode batteries and deepens understandings on the mechanism of interfacial stability and reaction kinetics.

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“…Lithium-ion batteries (LIBs) have revolutionized human civilization as they have laid the foundation of portable electronic devices, electric vehicles, and renewable energy toward a electrolyte consumption making the practical application even more challenging. [13][14][15] The quest to achieve maximum use of Si in the anode is lengthy and despite various efforts that have been made in recent years, several challenges still remain. Strategies have been devoted to the modification of the Si particle morphology and size to prevent particle cracking during cycling.…”

Section: Introductionmentioning

confidence: 99%

On the Practical Applicability of the Li Metal‐Based Thermal Evaporation Prelithiation Technique on Si Anodes for Lithium Ion Batteries

Adhitama

Bela

Demelash

et al. 2022

Advanced Energy Materials

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fossil fuel-free society. [1,2] Further developments in the whole battery value chain and across all technology readiness levels are needed to fulfill the demand for batteries with increased energy density and fast charging capability, lower cost, and higher safety. [3,4] With regard to the negative electrode (anode), so-called "alloyingtype" materials such as tin and silicon have become promising candidates to replace state-of-the-art (SOTA) graphite in future LIBs because they can reversibly store nearly four lithium ions per host atom offering much higher energy densities. [5][6][7] Si has become more attractive than Sn most likely due to the lower cost, greater availability, and higher capacity. [8][9][10] In theory, the specific capacity that can be achieved with Si is up to 3579 mAh g −1 combined with a low average delithiation potential (≈0.4 V vs Li|Li + ) and low voltage hysteresis. [11] Despite all these advantageous characteristics, the practical use of Si-based anode materials in commercial LIB cells faces major challenges, i.e., enormous particle stress on the atomic scale which leads to particle fracture and detachment from the current collector on the electrode scale. [12] In addition, continuous (re-)formation of the solid electrolyte interphase (SEI) causes ongoing active lithium losses (ALL) and Lithium ion batteries (LIBs) using silicon as anode material are endowed with much higher energy density than state-of-the-art graphite-based LIBs. However, challenges of volume expansion and related dynamic surfaces lead to continuous (re-)formation of the solid electrolyte interphase, active lithium losses, and rapid capacity fading. Cell failure can be further accelerated when Si is paired with high-capacity, but also rather reactive Ni-rich cathodes, such as LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM-811). Here, the practical applicability of thermal evaporation of Li metal is evaluated as a prelithiation technique on micrometer-sized Si (µ-Si) electrodes in addressing such challenges. NCM-811 || "prelithiated µ-Si" full-cells (25% degree of prelithiation) can attain a higher initial discharge capacity of ≈192 mAh g NCM-811−1 than the cells without prelithiation with only ≈160 mAh g NCM-811−1. This study deeply discusses significant consequences of electrode capacity balancing (N:P ratio) with regard to prelithiation on the performance of full-cells. The trade-off between cell lifetime and energy density is also highlighted. It is essential to point out that the phenomena discussed here can further guide the direction of research in using the thermal evaporation of Li metal as a prelithiation technique toward its practical application on Si-based LIBs.

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Revealing the Role, Mechanism, and Impact of AlF₃ Coatings on the Interphase of Silicon Thin Film Anodes

Cited by 20 publications

References 74 publications

Al-based materials for advanced lithium rechargeable batteries: recent progress and prospects

Al-based materials for advanced lithium rechargeable batteries: recent progress and prospects

Atomic/Molecular Layer-Deposited Laminated Li₂O–Lithicone Interfaces Enabling High-Performance Silicon Anodes

On the Practical Applicability of the Li Metal‐Based Thermal Evaporation Prelithiation Technique on Si Anodes for Lithium Ion Batteries

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Revealing the Role, Mechanism, and Impact of AlF3 Coatings on the Interphase of Silicon Thin Film Anodes

Cited by 20 publications

References 74 publications

Al-based materials for advanced lithium rechargeable batteries: recent progress and prospects

Al-based materials for advanced lithium rechargeable batteries: recent progress and prospects

Atomic/Molecular Layer-Deposited Laminated Li2O–Lithicone Interfaces Enabling High-Performance Silicon Anodes

On the Practical Applicability of the Li Metal‐Based Thermal Evaporation Prelithiation Technique on Si Anodes for Lithium Ion Batteries

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Revealing the Role, Mechanism, and Impact of AlF₃ Coatings on the Interphase of Silicon Thin Film Anodes

Atomic/Molecular Layer-Deposited Laminated Li₂O–Lithicone Interfaces Enabling High-Performance Silicon Anodes