Graphene–Metal–Organic Framework Composite Sulfur Electrodes for Li–S Batteries with High Volumetric Capacity

In an age of rapid acceleration toward next-generation energy storage technologies, lithium–sulfur (Li–S) batteries offer the desirable combination of low weight and high specific energy. Metal–organic frameworks (MOFs) have been recently studied as functionalizable platforms to improve Li–S battery performance. However, many MOF-enabled Li–S technologies are hindered by low capacity retention and poor long-term performance due to low electronic conductivity. In this work, we combine the advantages of a Zr-based MOF-808 loaded with sulfur as the active material with a graphene/ethyl cellulose additive, leading to a high-density nanocomposite electrode requiring minimal carbon. Our electrochemical results indicate that the nanocomposites deliver enhanced specific capacity over conventionally used carbon/binder mixtures, and postsynthetic modification of the MOF with lithium thiophosphate results in further improvement. Furthermore, the dense form factor of the sulfur-loaded MOF–graphene nanocomposite electrodes provides high volumetric capacity compared to other works with significantly more carbon additives. Overall, we have demonstrated a proof-of-concept paradigm where graphene nanosheets facilitate improved charge transport because of enhanced interfacial contact with the active material. This materials engineering approach can likely be extended to other MOF systems, contributing to an emerging class of two-dimensional nanomaterial-enabled Li–S batteries.