We present sulfurized polyolefins, i.e. sulfurized polypropylene (S/PP), sulfurized poly(norbornadiene) (S/pNBD) and its analog, sulfurized poly(dicyclopentadiene) (S/pDCPD), all synthesized in one-step by reacting the corresponding polyolefin with sulfur as new polysulfide shuttle-free cathode materials for Li-S batteries. All materials have been fully characterized by time-of-flight secondary ion mass spectrometry (ToF-SIMS), X-ray photoelectron spectroscopy (XPS) measurements and cyclic voltammetry (CV). In all materials, the sulfur is covalently bound to the polymer matrix in the form of C-Sx-C units. S/PP exhibits a reversible capacity as high as 1000 mAh/gsulfur at 0.1 C and a sulfur loading of up to 68 wt.-%, which in turn allows for high sulfur loadings up to 47 % in the final cathode. Li-S cells based on an S/pNBD cathode exhibit a high discharge capacity up to 1050 mAh/gsulfur at 1 C with a good capacity retention of 62 % after 1900 cycles. The structurally similar analog S/pDCPD shows comparable electrochemical performance, again with excellent capacity retention. The high reversibility and ultra-long cycle life of all materials are attributed to the covalent binding of sulfur to the polymer backbone. The low-cost starting materials together with the simple synthetic procedure and the good electrochemical performance in combination with a commercially available electrolyte make them very promising cathode materials for Li-S batteries.

Sulfurized polyolefins as low-cost cathode materials for high-capacity lithium-sulfur batteries

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