Journal Article

FZJ-2024-03206

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Insights into Electrolytic Pre‐Lithiation: A Thorough Analysis Using Silicon Thin Film Anodes

Haneke, L. ; Pfeiffer, F.FZJ* ; Bärmann, P. ; Wrogemann, J. ; Peschel, C. ; Neumann, J. ; Kux, F. ; Nowak, S. ; Winter, M.FZJ* ; Placke, T. (Corresponding author)

2023
Wiley-VCH Weinheim

This record in other databases:      

Please use a persistent id in citations: doi:10.1002/smll.202206092  doi:10.34734/FZJ-2024-03206

Abstract: 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 CO2 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 (CEff) of 95–96% for optimized electrolytes comparable to 1 m LiPF6/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 Cl2 dissolve in the electrolyte leading to a self-discharge Cl2/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.

Note: Unterstützt durch BMBF Projekt “PräLi” (03XP0238X).

---

Contributing Institute(s):

1. Helmholtz-Institut Münster Ionenleiter für Energiespeicher (IEK-12)

Research Program(s):

1. 1221 - Fundamentals and Materials (POF4-122) (POF4-122)

Appears in the scientific report 2024

---

Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; DEAL Wiley ; Essential Science Indicators ; IF >= 10 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

---