Lithium degradation in lithium–sulfur batteries: insights into inventory depletion and interphasial evolution with cycling

Nanda, Sanjay; Manthiram, Arumugam

doi:10.1039/d0ee01074j

Lithium degradation in lithium–sulfur batteries: insights into inventory depletion and interphasial evolution with cycling

Journal Article · Fri Jul 03 00:00:00 EDT 2020 · Energy & Environmental Science

DOI:https://doi.org/10.1039/d0ee01074j· OSTI ID:1799360

Nanda, Sanjay ^[1]; ^[2]

Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program. Texas Materials Inst.; OSTI
Univ. of Texas, Austin, TX (United States). Materials Science and Engineering Program. Texas Materials Inst.

The promise of high energy density lithium–sulfur batteries with long cycle life is currently tempered by the rapid degradation of lithium-metal anodes with cycling. An in-depth understanding of the dynamical behavior in liquid electrolytes, including the mechanisms underlying depletion of lithium inventory and evolution of lithium interphases, is crucial to make Li–S batteries a reality. We use here an anode-free full cell configuration, pairing a Li₂S cathode with a bare nickel current collector with no lithium metal on it, to quantitatively estimate the lithium inventory loss per cycle. Lithium inventory loss is shown to be the main factor limiting the overall cyclability of Li–S batteries. Time-of-flight secondary ion mass spectrometry measurements on the deposited lithium reveal the presence of substantial metallic lithium even after most of the active lithium inventory has been depleted. The trapped metallic lithium is rendered electrochemically inactive by the growth of a resistive electrolyte decomposition interphase on the lithium surface. The bulk of the deposited lithium is shown to be composed of various fully reduced interphasial components, including several hydrogen-containing species that show a substantial reduction in intensity with cycling. This indicates considerable gas evolution and is also correlated with the loss of lithium inventory. The use of an anode-free full cell configuration provides a framework for accurate assessment of the dynamics of lithium inventory depletion and characterization of the accompanying interphasial evolution with cycling. The insights gained will prove invaluable to the development of strategies for extending the cycle life of energy-dense Li–S batteries.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: EE0007762

OSTI ID:: 1799360

Alternate ID(s):: OSTI ID: 1637720
OSTI ID: 2217336

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 8 Vol. 13; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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