Ultra‐Stable Topological Telluride Monolayers for Next‐Generation Battery Anodes and Sulfur Hosts

Rechargeable batteries are approaching the energy density ceiling set by conventional intercalation electrodes, while still suffering from the polysulfide shuttle and dendrite growth. Here, 2D ternary metal tellurides (HfTiTe₄, ZrTiTe₄, and HfZrTe₄) are computationally designed, exhibiting a unique electronic environment with topological band structures and serving as multifunctional materials for ultrafast ion transport and strong catalytic anchoring in battery applications. Adsorption strengths demonstrate robust Li⁺/Na⁺ ion binding with considerable charge transfer, ensuring persistent chemisorption without affecting conductivity. Low ion-diffusion barriers of 0.206 eV for Li⁺ and 0.046 eV for Na⁺, and ultrahigh theoretical capacities up to 1600 mAh g^‒1 for Li⁺ and 1350 mAh g^‒1 for Na⁺, high open-circuit voltages in the range of 0.47-0.54 V for Li⁺ and 0.34-0.42 V for Na⁺ nominate them high-energy anode materials. Additionally, these monolayers mitigate the shuttle effect by exhibiting high reactivity and charge redistribution for polysulfide anchoring. Thermodynamic and kinetic calculations for the sulfur reduction process show that HfZrTe₄ possesses the lowest overpotential and activation barriers, while ZrTiTe₄ and HfTiTe₄ exhibit balanced binding and redox stability. This research on topological tellurides not only suggests them for next-generation anodic applications but also for appealing anchoring materials for lithium‒sulfur cathodes.