Exploring two-dimensional (2D) ferromagnetic materials with a high transition temperature and large magnetic anisotropy is extremely essential for highly efficient spintronic applications. With the density functional theory method, we predicted planar hypercoordinate transition-metal borides, TMB (TM = Ti, V, Cr, Mn, Fe; B = boron), by the condensation of TM@B and B units. The results showed that these transition-metal borides possess superior thermal, dynamic and mechanical stabilities. Interestingly, the TMB monolayer with TM = (V, Cr) is confirmed as a robust ferromagnetic metal with a high Curie temperature of ∼335 K and ∼221 K, respectively. In addition, the system with TM = (Mn, Fe) is found to be an antiferromagnetic metal with a Néel temperature of ∼173 K and ∼91 K, respectively. In particular, large perpendicular magnetic anisotropy is identified for CrB, MnB, and FeB monolayers, around 198-623 μeV. Furthermore, four TMB (TM = Ti, V, Cr, Mn) systems are determined to be candidate catalysts for the hydrogen evolution reaction, with nearly zero free energy of hydrogen adsorption (Δ = -0.0003 to -0.03 eV). Our study highlighted potential 2D metal borides for spintronic devices and high efficiency electrochemical catalysts.
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