Abstract

The performances of rechargeable batteries are strongly affected by the operating environmental temperature. In particular, low temperatures (e.g., ≤0 °C) are detrimental to efficient cell cycling. To circumvent this issue, we propose a few-layer Bi2Se3 (a topological insulator) as cathode material for Zn metal batteries. When the few-layer Bi2Se3 is used in combination with an anti-freeze hydrogel electrolyte, the capacity delivered by the cell at −20 °C and 1 A g−1 is 1.3 larger than the capacity at 25 °C for the same specific current. Also, at 0 °C the Zn | |few-layer Bi2Se3 cell shows capacity retention of 94.6% after 2000 cycles at 1 A g−1. This behaviour is related to the fact that the Zn-ion uptake in the few-layer Bi2Se3 is higher at low temperatures, e.g., almost four Zn2+ at 25 °C and six Zn2+ at −20 °C. We demonstrate that the unusual performance improvements at low temperatures are only achievable with the few-layer Bi2Se3 rather than bulk Bi2Se3. We also show that the favourable low-temperature conductivity and ion diffusion capability of few-layer Bi2Se3 are linked with the presence of topological surface states and weaker lattice vibrations, respectively.

Highlights

  • The performances of rechargeable batteries are strongly affected by the operating environmental temperature

  • The transmission electron microscopy (TEM) analysis of P-Bi2Se3 presented in Supplementary Fig. 4a indicates irregular granules ranging in size from 200 nm to 1 μm

  • The high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) image of E-Bi2Se3 recorded along the [010] zone axis (Fig. 1e) is a magnified view from the A region of Supplementary Fig. 5a, where 1 QL is well assigned to the layered structure

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Summary

Introduction

The performances of rechargeable batteries are strongly affected by the operating environmental temperature. Fading electrochemical performance at low temperatures can be mitigated by introducing electrolyte additives[6], coating surfaces with some material that is highly electronically conductive[7,8], and heteroatom doping[9,10], but the attenuation is inevitable, and to date the highest retention of 86% at −25 °C for a sodium ion cell is achieved by Goodenough’s group using an organic electrolyte[5] This progress is valuable, for a cell required to operate over a long period in a cold climate, performance degradation remains unavoidable[5]. Bi2Se3, a topological insulator with a 0.3-eV nontrivial bulk gap and superficial single Dirac cone, is formed by periodic layers composed of five atomic planes (Se-Bi-Se-Bi-Se; namely, a quintuple layer denoted QL) connected through van der Waals forces; numerous unoccupied tetrahedral and octahedral exist between the Se atomic planes and result in the material’s potential as an intercalating cathode in batteries[14,15]

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