Prelithiated Carbon Nanotube‐Embedded Silicon‐based Negative Electrodes for High‐Energy Density Lithium‐Ion Batteries

Advanced Materials Interfaces, vol. 11

Abstract

Abstract Multi‐walled carbon Nanotubes (MWCNTs) are hailed as beneficial conductive agents in Silicon (Si)‐based negative electrodes due to their unique features enlisting high electronic conductivity and the ability to offer additional space for accommodating the massive volume expansion of Si during (de‐)lithiation. However, both MWCNTs and Siirreversibly consume an enormous amount of Li inventory to principally form a Solid Electrolyte Interphase (SEI) and due to other parasitic reactions, which results in lowering the Coulombic Efficiency (CE), rapid decrease in reversible capacity, and shorter battery life.To tackle these hurdles, electrochemical prelithiation is adopted as a taming strategy to mitigate the large capacity loss (nearly reducing the first irreversible capacity by ≈60%) of MWCNT‐Si/Graphite (Gr) negative electrode‐based full‐cells. In contrast, a yardstick negative electrode utilizing commercially used Super P (Super P‐Si/Gr) showed a reduction of ≈47% after in vitro pre‐doping with lithium, which is considerably smaller compared to that of MWCNTs‐based electrode design. Furthermore, the Initial CE, life cycle, and rate capability are enhanced by prelithiation. Interestingly, prelithiation brings more impact on MWCNTs ‐Si/Gr than with Super P‐Si/Gr design. An in‐depth analysis using X‐ray photoelectron spectroscopy (XPS), RAMAN Spectroscopy, Attenuated Total Reflection Fourier Transform Infrared Spectroscopy (ATR FTIR), laser microscopy, and Scanning Electron Microscopy (SEM) reveal deeper insights into the differences in SEI layer between prelithiated MWCNTs and their Super P‐based electrode counterparts.

Authors 7

1. Leyla Ünal corresponding

   Forschungszentrum Jülich · Helmholtz-Institute Münster

   Affiliation as printed

   Helmholtz Institute Münster (HI MS) IEK‐12 Forschungszentrum Jülich GmbH Campus Boulevard 89 52074 Aachen Germany

2. Viviane Maccio‐Figgemeier Aachen Center for Ageing Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL)

   RWTH Aachen University

   Affiliation as printed

   Center for Ageing Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL) RWTH Aachen University Campus Boulevard 89 52074 Aachen Germany

3. Lukas Haneke

   University of Münster

   Affiliation as printed

   Insitute of Physical Chemistry MEET Battery Research Center University of Münster 48149 Münster Germany

4. Gebrekidan Gebresilassie Eshetu corresponding Aachen Center for Ageing Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL)

   Mekelle University · RWTH Aachen University

   Affiliation as printed

   Center for Ageing Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL) RWTH Aachen University Campus Boulevard 89 52074 Aachen Germany

   Department of Material Science and Engineering Mekelle Institute of Technology, Mekelle University 1632, Tigray Ethiopia

5. Johannes Kasnatscheew

   University of Münster

   Affiliation as printed

   Insitute of Physical Chemistry MEET Battery Research Center University of Münster 48149 Münster Germany

6. Martin Winter

   University of Münster

   Affiliation as printed

   Insitute of Physical Chemistry MEET Battery Research Center University of Münster 48149 Münster Germany

7. Egbert Figgemeier corresponding Aachen Center for Ageing Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL)

   Forschungszentrum Jülich · Helmholtz-Institute Münster · RWTH Aachen University

   Affiliation as printed

   Center for Ageing Reliability and Lifetime Prediction of Electrochemical and Power Electronic Systems (CARL) RWTH Aachen University Campus Boulevard 89 52074 Aachen Germany

   Helmholtz Institute Münster (HI MS) IEK‐12 Forschungszentrum Jülich GmbH Campus Boulevard 89 52074 Aachen Germany