Danli Zeng

High rate lithium-sulfur battery enabled by sandwiched single ion conducting polymer electrolyte

Lithium-sulfur batteries are highly promising for electric energy storage with high energy density, abundant resources and low cost. However, the battery technologies have often suffered from a short cycle life and poor rate stability arising from the well-known “polysulfide shuttle” effect. Here, we report a novel cell design by sandwiching a sp3 boron based single ion conducting polymer electrolyte film between two carbon films to fabricate a composite separator for lithium-sulfur batteries. The dense negative charges uniformly distributed in the electrolyte membrane inherently prohibit transport of polysulfide anions formed in the cathode inside the polymer matrix and effectively blocks polysulfide shuttling. A battery assembled with the composite separator exhibits a remarkably long cycle life at high charge/discharge rates.

Single ion conducting lithium sulfur polymer batteries with improved safety and stability

Li–S secondary batteries use lithium metal as the anode. The safety hazard arising from the Li dendrite formation on the metal surface presents a formidable challenge that has hindered the technology from practical applications for many years. It has been confirmed that tiny and random lithium deposition takes place at the ion depletion layer on the surface of lithium metal. The time required to reach the ion depletion layer can be quantified using Sands equation, in which the time is inversely proportional to the transference number of anions (t−). Therefore, restricting the mobility of anions enables avoidance of ion depletion. In this study, lithium 4-aminophenylsulfonyl(trifluoromethylsulfonyl)imide (LiATFSI) is grafted with poly(ethylene-alt-maleic anhydride) (PEMA, Mw = 100 000–500 000) using a cyclic imide to form a single ion conducting polymer electrolyte (PEMA-graft-LiATFSI). The polymer electrolyte membrane made of PEMA-graft-LiATFSI is capable of withstanding a high current density of ±50 mA cm−2 (normalized to the surface area of the lithium disk) in a lithium symmetric cell. More remarkably, the metallic luster of the lithium foil remains essentially intact even after a galvanostatic cycling test with a current density of ±10 mA cm−2 for over 1600 hours, suggesting that the membrane can effectively suppress Li dendrite formation and thus pave a way to use lithium metal directly as the anode material with sufficient energy capacity and good safety. The lithium–sulfur battery assembled with the membrane as the electrolyte as well as the separator delivered a stable capacity of 780.8 mA h g−1 after 1000 cycles at 1C. This work demonstrates the necessity and fundamental importance of single ion conducting electrolyte membranes for achieving safe and stable performance with high energy density lithium metal secondary batteries.