Record-Breaking Elemental Superconductivity in Tetralayer Kagome Borophene

Abstract Superconductivity above the liquid-nitrogen temperature remains rare in two-dimensional elemental crystals, where strong covalent bonding often yields high phonon frequencies but insufficient electron–phonon coupling. Here, using first-principles calculations and fully anisotropic Migdal–Eliashberg theory, we predict tetralayer kagome borophene (TKB) stabilized by ABAB covalent stacking, as a liquid-nitrogen-temperature elemental superconductor. With a predicted critical temperature of ∼100–113 K, TKB sets a record-high value among previously reported elemental superconductors. Unlike known high-Tc boron-based superconductors dominated by in-plane σ-bonding states and high-frequency in-plane B–B stretching modes, TKB realizes an out-of-plane s–pz-bonding-mediated pairing mechanism, in which interlayer s–pz bonding states at the Fermi level are strongly coupled to low-frequency out-of-plane vibrations of boron atoms. These results reveal a distinct out-of-plane pairing channel in multilayer borophene and establish covalent stacking engineering as a potential route for high-Tc superconductivity in two-dimensional materials.