Reversible Crosslinked Polymer Binder for Recyclable Lithium Sulfur Batteries with High Performance

Abstract

Owing to the negative impact of the extensive utilization of batteries on the environment, sustainability of the cells needs to be included in the systemic research of batteries. Herein, a dissolvable ionic crosslinked polymer (DICP) is exploited as a binder for lithium–sulfur batteries by crosslinking the polyacrylic acid and polyethyleneimine through carboxy‐amino ionic interaction. This interaction is pH‐controlled, and therefore, the crosslinked binder network can be readily dissociated under basic conditions, providing a facile strategy enabling valuable components recycled through a convenient washing method. The sulfur cathode prepared using the recycled carbon–sulfur composite can deliver comparable capacity as that of fresh electrode. In addition, evidence from cell performance and characterizations, such as in situ X‐ray absorption spectroscopy, in situ UV–visible spectroscopy, X‐ray photoelectron spectroscopy, and density functional theory calculation, confirms that DICP is a more effective binder than its commercial counterpart on suppressing polysulfide dissolution in the electrolyte. Exploiting reversible crosslinked polymer binder for recyclable Li–S batteries with ameliorated electrochemical performance, this study illuminates sustainable development for large‐scale energy storage systems.

Revealing the working mechanism of a multi-functional block copolymer binder for lithium-sulfur batteries

“…An alternative route is to use the chemical adsorption of the functional polymer binders in the sulfur cathode to immobilize polysulfides [20][21][22]. Various chemical bonding approaches have been employed to meet the required chemical, electrochemical, and mechanical stability in the cell [23][24][25][26]. Polyvinylidene fluoride (PVdF) is a conventional non-reactive polymer binder in Li-S batteries that acts as an effective adhesion agent to connect the active materials and conductive additives together, and then steadily adhere them to the current collectors.…”

Highly Ordered Carbon Coating Prepared with Polyvinylidene Chloride Precursor for High‐Performance Silicon Anodes in Lithium‐Ion Batteries

“…Lithium‐ion batteries (LIBs) have long cycling life, high energy density, and high power capability, thus dominating the current energy storage market [1,2] . Significant research efforts have been devoted to development of next‐generation rechargeable batteries to meet the demand of the rapidly growing energy storage market, [3–7] as the graphite anodes in current LIBs have a rather limited theoretical capacity of 372 mAh/g. Silicon materials, with a nearly 10‐fold higher theoretical capacity of 3579 mAh/g, relatively low discharge potential (<0.5 V vs. Li/Li + ), and abundant resource, have been considered as promising anode materials for LIBs [8–10] .…”

Nitrogen‐Doped Hollow Carbon Polyhedrons with Carbon Nanotubes Surface Layers as Effective Sulfur Hosts for High‐Rate, Long‐Lifespan Lithium–Sulfur Batteries

“…Li‐S batteries are generally considered as a potential alternative to the current widely used lithium‐ion batteries due to various advantages, such as low production cost, [1–3] several‐time higher theoretical capacity (1675 mAh g −1 ) and energy density (2600 Wh kg −1 ) as well as the abundant reserve of sulfur in earth crust and its environmental inertness [4–7] . Yet, the commercialization of Li‐S batteries encounters many challenges, including rapid capacity degradation derived from the dissolution of polysulfides into electrolyte as well as the large volume fluctuation of sulfur during charge‐discharge cycling, [8,9] low rate performance due to the extremely low electrical conductivity (5×10 −28 S cm −1 ) of sulfur [10–12] . Therefore, effectively confining lithium polysulfides in porous/hollow conductive nanomaterials represents a judicious way to mitigate the afore mentioned issues [13] .…”