Abstract

To obtain soft electronics, it is essential to develop high-performance and mechanically flexible energy storage at the industry level. Herein, we report flexible high-energy-density lithium-sulfur (Li–S) batteries based on all-fibrous sulfur cathodes and separators. To implement free-standing and flexible sulfur cathodes, electrically conductive single-walled carbon nanotubes (CNTs) are impregnated with cellulose nanofibers. This fibrous structure forms a 3D porous electrode with a large surface area to improve redox kinetics and achieve a high sulfur loading content without the use of a metal collector, which can then be applied in high-energy-density batteries. These flexible sulfur cathodes are combined with a commercial glass fiber separator coated with a CNT layer through a cost-effective solution process to suppress the shuttle effects of lithium–polysulfide, thereby exhibiting robust cycling stability. The prepared Li–S batteries exhibit high capacities of 940 mAh g−1 at a charge current density of 1.57 mA cm−2 and at 25 °C, and the Coulombic efficiency exceeds 90% even after 50 charge/discharge cycles. Moreover, Li-S batteries with a high gravimetric energy density of 443 Wh kg−1 per cell is achieved, and these batteries demonstrate excellent reliability in regard to electrochemical performance even under severe mechanical stress conditions for over 100 cycles.

Highlights

  • Some pioneering companies have launched innovative mobile smart devices, such as the Samsung Galaxy Z Flip and Huawei Mate X, which are foldable 5 G smartphones

  • We propose flexible Li–S batteries based on the fibrous composition of sulfur cathodes that consist of a cellulose nanofiber (CNF) framework and electronically conductive carbon nanotubes (CNTs) additives

  • A sulfur layer with a nanoscale thickness conformably formed on the surface of the one-dimensional structure of the multiwalled carbon nanotubes (MWCNTs)

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Summary

Introduction

Some pioneering companies have launched innovative mobile smart devices, such as the Samsung Galaxy Z Flip and Huawei Mate X, which are foldable 5 G smartphones. These foldable phones are not mainstream devices, this technological trend will be maintained further and is expected to be accelerated by the development of new materials and components. Lithium-ion batteries (LIBs) have been widely used for portable electronic devices and electric vehicles owing to their high energy density (~300 Wh kg−1), high operating voltage, and long cycling lifetime. The high capacity and charge/discharge cycling performance of these materials results from their two-electron system during the electrochemical reaction. Li-S batteries can exhibit a specific energy density of ~ 2500 Wh kg−1, which is five- to tenfold higher than that of LIBs7,13–16

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