Nano-vault architecture mitigates stress in silicon-based anodes for lithium-ion batteries

Marta Haro*, Pawan Kumar, Junlei Zhao, Panagiotis Koutsogiannis, Alexander James Porkovich, Zakaria Ziadi, Theodoros Bouloumis, Vidyadhar Singh, Emilio J. Juarez-Perez, Evropi Toulkeridou, Kai Nordlund, Flyura Djurabekova, Mukhles Sowwan, Panagiotis Grammatikopoulos*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

7 Scopus citations

Abstract

Nanomaterials undergoing cyclic swelling-deswelling benefit from inner void spaces that help accommodate significant volumetric changes. Such flexibility, however, typically comes at a price of reduced mechanical stability, which leads to component deterioration and, eventually, failure. Here, we identify an optimised building block for silicon-based lithium-ion battery (LIB) anodes, fabricate it with a ligand- and effluent-free cluster beam deposition method, and investigate its robustness by atomistic computer simulations. A columnar amorphous-silicon film was grown on a tantalum-nanoparticle scaffold due to its shadowing effect. PeakForce quantitative nanomechanical mapping revealed a critical change in mechanical behaviour when columns touched forming a vaulted structure. The resulting maximisation of measured elastic modulus (~120 GPa) is ascribed to arch action, a well-known civil engineering concept. The vaulted nanostructure displays a sealed surface resistant to deformation that results in reduced electrode-electrolyte interface and increased Coulombic efficiency. More importantly, its vertical repetition in a double-layered aqueduct-like structure improves both the capacity retention and Coulombic efficiency of the LIB.

Original languageEnglish
Article number16
JournalCommunications Materials
Volume2
Issue number1
DOIs
StatePublished - Dec 2021
Externally publishedYes

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