Ab Initio Simulation of Raman Fingerprints of Sulfur/Carbon Copolymer Cathodes During Discharge of Li-S Batteries.

Sulfur/carbon copolymers have emerged as promising alternatives for conventional crystalline sulfur cathodes for lithium-sulfur batteries. Among these, sulfur-n-1,3-diisopropenylbenzene (S/DIB) copolymers, which present a 3D network of DIB molecules interconnected via sulfur chains, have particularly shown a good performance and, therefore, have been under intensive experimental and theoretical investigations. However, their structural complexity and flexibility have hindered a clear understanding of their structural evolution during redox reactions at an atomistic level.

Characterization of sulfur/carbon copolymer cathodes for Li-S batteries: a combined experimental and Raman spectroscopy study.

Optimization of lithium-sulfur batteries highly depends on exploring and characterizing new cathode materials. Sulfur/carbon copolymers have recently attracted much attention as an alternative class of cathodes to replace crystalline sulfur. In particular, poly(sulfur--1,3-diisopropenylbenzene) (S/DIB) has been under considerable experimental and theoretical investigations, promising a good performance in mitigating the so-called shuttle effect.

On the Structure of Sulfur/1,3-Diisopropenylbenzene Co-Polymer Cathodes for Li-S Batteries: Insights from Density-Functional Theory Calculations.

Sulfur co-polymers have recently drawn considerable attention as alternative cathode materials for lithium-sulfur batteries, thanks to their flexible atomic structure and the ability to provide high reversible capacity. Here, we report on the atomic structure of sulfur/1,3-diisopropenylbenzene co-polymers (poly(S-co-DIB)) based on the insights obtained from density-functional theory calculations. The focus is set on studying the local structural properties, namely the favorable sulfur chain length (S with ) connecting two DIBs.