Rational regulation on polysulfide behaviors is of great significance in pursuit of reliable solution-based lithium–sulfur (Li–S) battery chemistry. Herein, we develop a unique polymeric zwitterion (PZI) to establish a smart polysulfide regulation in Li–S batteries. The zwitterionic nature of PZI integrates sulfophilicity and lithiophilicity in the matrix, fostering an ionic environment for selective ion transfer through the chemical interactions with lithium polysulfides (LiPS). When implemented as a functional interlayer in the cell configuration, PZI empowers strong obstruction against polysulfide permeation but simultaneously allows fast Li+ conduction, thus contributing to significant shuttle inhibition as well as the resultant facile and stable sulfur electrochemistry. The PZI-based cells realize excellent cyclability over 1000 cycles with a minimum capacity fading rate of 0.012% per cycle and favorable rate capability up to 5 C. Moreover, a high areal capacity retention of 5.3 mAh cm–2 after 300 cycles can be also obtained under raised sulfur loading and limited electrolyte, demonstrating great promise in developing high-efficiency and long-lasting Li–S batteries.

A noncovalent and phase-transfer-assisted method is developed for the fabrication of polymer-functionalized graphene, in which a series of cluster-cored star polymers (CSPs) containing a polyoxometalate core and polystyrene (PS) arms are used as modifiers. Through the electron transfer interaction between polyoxometalate and graphene, the CSPs can strongly adsorb on graphene nanosheets and transfer them from aqueous media to organic solvents like chloroform, forming individually dispersed graphene. Moreover, the CSP-functionalized graphene is well compatible with additional polymer matrices and can serve as a reinforcing nanofiller for polymer composites. A 0.2 wt% loading of them in PS coating achieves a 98.9% high enhancement in Young's modulus.

Hierarchical zinc–hexamethylenetetramine complex microflowers were developed to establish a multifunctional interlayer towards high-capacity and durable lithium–sulfur batteries.

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