Spontaneous and reversible hollowing of alloy anode nanocrystals for stable battery cycling

Boebinger, Matthew G.; Yarema, Olesya; Yarema, Maksym; Unocic, Kinga A.; Unocic, Raymond R.; Wood, Vanessa; McDowell, Matthew T.

doi:10.1038/s41565-020-0690-9

Spontaneous and reversible hollowing of alloy anode nanocrystals for stable battery cycling

Journal Article · Mon Jun 01 00:00:00 EDT 2020 · Nature Nanotechnology

DOI:https://doi.org/10.1038/s41565-020-0690-9· OSTI ID:1775225

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Georgia Inst. of Technology, Atlanta, GA (United States)
Eidgenoessische Technische Hochschule, Zurich (Switzerland)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

High-capacity alloy anode materials for Li-ion batteries have long been held back by limited cyclability caused by the large volume changes during lithium insertion and removal. Hollow and yolk-shell nanostructures have been used to increase the cycling stability by providing an inner void space to accommodate volume changes and a mechanically and dimensionally stable outer surface. These materials, however, require complex synthesis procedures. Here, using in situ transmission electron microscopy, we show that sufficiently small antimony nanocrystals spontaneously form uniform voids on the removal of lithium, which are then reversibly filled and vacated during cycling. This behaviour is found to arise from a resilient native oxide layer that allows for an initial expansion during lithiation but mechanically prevents shrinkage as antimony forms voids during delithiation. In this work, we developed a chemomechanical model that explains these observations, and we demonstrate that this behaviour is size dependent. Thus, antimony naturally evolves to form optimal nanostructures for alloy anodes, as we show through electrochemical experiments in a half-cell configuration in which 15-nm antimony nanocrystals have a consistently higher Coulombic efficiency than larger nanoparticles.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

Sponsoring Organization:: Alfred P. Sloan Foundation; National Science Foundation (NSF); Swiss National Science Foundation (SNF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1775225

Journal Information:: Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 6 Vol. 15; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Tin Domain Growth on Quasi-Two-Dimensional CdTe and CdSe Nanoparticles Lazareva, E. P.; Kozlovskii, V. F.; Vasiliev, R. B. Russian Journal of Inorganic Chemistry, Vol. 63, Issue 5 https://doi.org/10.1134/s0036023618050133	journal	May 2018
In-Situ Arc Discharge-Derived FeSn2/Onion-Like Carbon Nanocapsules as Improved Stannide-Based Electrocatalytic Anode Materials for Lithium-Ion Batteries Han, Dandan; Chatterjee, Amrita; Man, Long Hin Catalysts, Vol. 9, Issue 11 https://doi.org/10.3390/catal9110950	journal	November 2019
Sub-wavelength waveguide properties of 1D and surface-functionalized SnO ₂ nanostructures of various morphologies Bonu, Venkataramana; Sahu, Binaya Kumar; Das, Arindam Beilstein Journal of Nanotechnology, Vol. 10 https://doi.org/10.3762/bjnano.10.37	journal	January 2019
Inexpensive Antimony Nanocrystals and Their Composites with Red Phosphorus as High-Performance Anode Materials for Na-ion Batteries Walter, Marc; Erni, Rolf; Kovalenko, Maksym V. ETH Zurich https://doi.org/10.3929/ethz-b-000099378	text	January 2015
Monodisperse CoSn2 and FeSn2 nanocrystals as high-performance anode materials for lithium-ion batteries Wang, Shutao; He, Meng; Walter, Marc ETH Zurich https://doi.org/10.3929/ethz-b-000261753	text	January 2018
Building better all-solid-state batteries with Li-garnet solid electrolytes and metalloid anodes Afyon, Semih; Kravchyk, Kostiantyn V.; Wang, Shutao ETH Zurich https://doi.org/10.3929/ethz-b-000372251	text	January 2019

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