Abstract

Graphite, the dominant anode in rechargeable lithium batteries, operates at ∼0.1 V versus Li+/Li and can result in lithium plating on the graphite surface, raising safety concerns. Titanates, for example, Li4Ti5O12, intercalate lithium at∼1.6 V versus Li+/Li, avoiding problematic lithium plating at the expense of reduced cell voltage. There is interest in 1 V anodes, as this voltage is sufficiently high to avoid lithium plating while not significantly reducing cell potential. The sulfides, LiVS2 and LiTiS2, have been investigated as possible 1 V intercalation electrodes but suffer from capacity fading, large 1st cycle irreversible capacity or polarization. Here we report that the 50/50 solid solution, Li1+x(V0.5Ti0.5)S2, delivers a reversible capacity to store charge of 220 mAhg−1 (at 0.9 V), 99% of theoretical, at a rate of C/2, retaining 205 mAhg−1 at C-rate (92% of theoretical). Rate capability is excellent with 200 mAhg−1 at 3C. C-rate is discharge in 1 h. Polarization is low, 100 mV at C/2. To the best of our knowledge, the properties/performances of Li(V0.5Ti0.5)S2 exceed all previous 1 V electrodes.

Highlights

  • Graphite, the dominant anode in rechargeable lithium batteries, operates at B0.1 V versus Li þ /Li and can result in lithium plating on the graphite surface, raising safety concerns

  • In order to avoid the potential danger of Li plating[1,2] on the widely used graphite anodes[3,4,5] in Li-ion batteries, which intercalate Li at 0.1 V versus Li þ /Li, important efforts have been made to identify anodes operating at 1 V, including organic intercalation compounds[10] and conversion reactions[11,12]

  • Inorganic intercalation electrodes operate by a well-established mechanism, without the drastic changes that accompany conversion reactions, without involving nanoparticles and with higher densities than organic intercalation compounds

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Summary

Introduction

The dominant anode in rechargeable lithium batteries, operates at B0.1 V versus Li þ /Li and can result in lithium plating on the graphite surface, raising safety concerns. The sulfides, LiVS2 and LiTiS2, have been investigated as possible 1 V intercalation electrodes but suffer from capacity fading, large 1st cycle irreversible capacity or polarization. LiTiS2 exhibits a massive 1st cycle irreversible loss of capacity of over 180 mAhg À 1

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