One-Dimensional, Titania Lepidocrocite-Based Nanofilaments and Their Polysulfide Anchoring Capabilities in Lithium–Sulfur Batteries

The high theoretical energy density of metal–sulfur batteries compared to their lithium-ion counter parts renders sulfur-based electrode chemistries attractive. Additionally, sulfur is relatively abundant and environmentally benign. Yet, issues like the low conductivity of sulfur, polysulfide (PS) formation, and shuttling have hindered the development of sulfur chemistries. Here, we react titanium carbide powders with tetramethylammonium hydroxide ammonium salts at 50 °C for 5 days and convert them into one dimensional, titania-based lepidocrocite (1DL) nanofilaments (NFs) using our facile bottom-up approach. This simple and scalable approach led to better electrode functionalization, facile tunability, and a higher density of active sites. The 1DL NFs self-assembled into a variety of microstructures─from individual 1DL NFs with minimal cross sections ≈5 × 7 Å2 to 2D flakes to mesoscopic particles. A composite was made with a 1:1 weight ratio of sulfur and 1DL NFs, which were hand-ground, mixed with carbon black and binder in a weight ratio of 70:20:10, respectively. We obtained a specific capacity of 750 mA h g–1 at 0.5C for 300 cycles. The 1DL NFs that, in this case assembled into 2D layers, trapped the polysulfides, PSs, by forming thiosulfate species and Lewis acid–base interactions with the Ti, as confirmed by post-mortem X-ray photoelectron spectroscopy. These interactions were also confirmed by PS adsorption via UV–vis spectroscopy and shuttle current measurements that showed lower PS shuttling in the 1DL NFs cells.