Utilizing van der Waals Slippery Interfaces to Enhance the Electrochemical Stability of Silicon Film Anodes in Lithium-Ion Batteries

Swastik Basu, Shravan Suresh, Kamalika Ghatak, Stephen F. Bartolucci, Tushar Gupta, Prateek Hundekar, Rajesh Kumar, Toh Ming Lu, Dibakar Datta, Yunfeng Shi, Nikhil Koratkar

Research output: Contribution to journalArticlepeer-review

34 Scopus citations

Abstract

High specific capacity anode materials such as silicon (Si) are increasingly being explored for next-generation, high performance lithium (Li)-ion batteries. In this context, Si films are advantageous compared to Si nanoparticle based anodes since in films the free volume between nanoparticles is eliminated, resulting in very high volumetric energy density. However, Si undergoes volume expansion (contraction) under lithiation (delithiation) of up to 300%. This large volume expansion leads to stress build-up at the interface between the Si film and the current collector, leading to delamination of Si from the surface of the current collector. To prevent this, adhesion promotors (such as chromium interlayers) are often used to strengthen the interface between the Si and the current collector. Here, we show that such approaches are in fact counter-productive and that far better electrochemical stability can be obtained by engineering a van der Waals "slippery" interface between the Si film and the current collector. This can be accomplished by simply coating the current collector surface with graphene sheets. For such an interface, the Si film slips with respect to the current collector under lithiation/delithiation, while retaining electrical contact with the current collector. Molecular dynamics simulations indicate (i) less stress build-up and (ii) less stress "cycling" on a van der Waals slippery substrate as opposed to a fixed interface. Electrochemical testing confirms more stable performance and much higher Coulombic efficiency for Si films deposited on graphene-coated nickel (i.e., slippery interface) as compared to conventional nickel current collectors.

Original languageEnglish (US)
Pages (from-to)13442-13451
Number of pages10
JournalACS Applied Materials and Interfaces
Volume10
Issue number16
DOIs
StatePublished - Apr 25 2018

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

Keywords

  • interfacial slip
  • lithium-ion battery
  • silicon film anode
  • stable cycle life
  • van der Waals interface

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