High‐Temperature Superconductivity in Li‐Removed Icosahedral B 13 C 2

ABSTRACT The B 12 icosahedron serves as the fundamental building block in boron‐rich compounds, where the combination of strong multi‐center covalent bonding and low atomic mass favors high‐frequency phonons and robust electron‐phonon coupling, rendering them as promising candidates for high‐temperature superconductivity. However, these materials are typically insulating due to the electron‐counting rule. Here, we propose a viable strategy to achieve superconductivity in LiB 13 C 2 by degassing Li and leading to the formation of icosahedron‐based B 13 C 2 superconductor. First‐principles calculations demonstrate that the removal of Li alters density of states at the Fermi level () while retains its 3D covalent framework. Strikingly, after the complete removal of Li, the resulting B 13 C 2 is predicted to be an anisotropic single‐gap superconductor with a critical temperature ( T c ) of 53 K, primarily driven by strong coupling between B 12 icosahedral vibrational modes and conduction electrons. This work illustrates a potential route toward achieving high‐temperature superconductivity in icosahedron‐based boron‐rich frameworks.