Insights into Electrolytic Pre-Lithiation: A Thorough Analysis Using Silicon Thin Film Anodes.

Autor: Haneke L; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany., Pfeiffer F; Helmholtz Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149, Münster, Germany., Bärmann P; Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB), Albert-Einstein-Straße 15, 12489, Berlin, Germany., Wrogemann J; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany., Peschel C; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany., Neumann J; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany., Kux F; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany., Nowak S; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany., Winter M; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany.; Helmholtz Institute Münster, IEK-12, Forschungszentrum Jülich GmbH, Corrensstraße 46, 48149, Münster, Germany., Placke T; University of Münster, MEET Battery Research Center, Institute of Physical Chemistry, Corrensstraße 46, 48149, Münster, Germany.
Jazyk: angličtina
Zdroj: Small (Weinheim an der Bergstrasse, Germany) [Small] 2023 Feb; Vol. 19 (8), pp. e2206092. Date of Electronic Publication: 2022 Dec 11.
DOI: 10.1002/smll.202206092
Abstrakt: Pre-lithiation via electrolysis, herein defined as electrolytic pre-lithiation, using cost-efficient electrolytes based on lithium chloride (LiCl), is successfully demonstrated as a proof-of-concept for enabling lithium-ion battery full-cells with high silicon content negative electrodes. An electrolyte for pre-lithiation based on γ-butyrolactone and LiCl is optimized using boron-containing additives (lithium bis(oxalato)borate, lithium difluoro(oxalate)borate) and CO 2 with respect to the formation of a protective solid electrolyte interphase (SEI) on silicon thin films as model electrodes. Reversible lithiation in Si||Li metal cells is demonstrated with Coulombic efficiencies (C Eff ) of 95-96% for optimized electrolytes comparable to 1 m LiPF 6 /EC:EMC 3:7. Formation of an effective SEI is shown by cyclic voltammetry and X-ray photoelectron spectroscopy (XPS). electrolytic pre-lithiation experiments show that notable amounts of the gaseous product Cl 2 dissolve in the electrolyte leading to a self-discharge Cl 2 /Cl - shuttle mechanism between the electrodes lowering pre-lithiation efficiency and causing current collector corrosion. However, no significant degradation of the Si active material and the SEI due to contact with elemental chlorine is found by SEM, impedance, and XPS. In NCM111||Si full-cells, the capacity retention in the 100th cycle can be significantly increased from 54% to 78% by electrolytic pre-lithiation, compared to reference cells without pre-lithiation of Si.
(© 2022 The Authors. Small published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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