Hydrogenated two-dimensional (2D) materials have recently attracted significant attention for their potential to achieve high-temperature superconductivity via the conventional electron-phonon coupling. However, insufficient surface coordination often limits effective hydrogenation in traditional 2D systems. Here, we identify hexagonal MBenes as an ideal platform with the compact atomic stacking for constructing robust hydrogen-based networks. MBenes are boron-based analogs of MXenes, in which boron (B) atoms form the intermediate layer and transition metals (M) make up the outer layers. A comprehensive study of 53 MBene compounds, including pristine MB, monohydride MBH, and dihydride ${\mathrm{MBH}}_2$ phases, identifies 29 dynamically and mechanically stable structures. Hydrogen adsorption significantly enhances the superconducting critical temperature ($T_{\text{c}}$) in Sc-, Ti-, V-, Nb-, and Ta-based MBenes. Among them, ${\mathrm{VBH}}_2$ exhibits a record $T_{\text{c}}$ of 83 K for hydrogenated 2D superconductors. This enhancement is attributed to a Van Hove singularity (VHS) near the Fermi level, induced by strong hybridization between H $s$ and M $d$ orbitals. Biaxial strain calculations further confirm the decisive role of the VHS by showing a suppression of $T_{\text{c}}$ when the VHS shifts away from the Fermi level. Furthermore, except for ${\mathrm{TaBH}}_2, {\mathrm{MBH}}_2$ (M = Sc, Ti, V, Nb) exhibit three-gap superconductivity, with anisotropy stemming from the dispersive nature of M $d$ orbitals. This research constructs a robust theoretical basis to probe high-temperature superconductivity and its fundamental origin in hydrogenated MBenes.

Close

PrevNext

View figure in article

• Electron-phonon coupling
• Electronic structure
• Superconducting gap
• Superconductivity
• 2-dimensional systems
• First-principles calculations