V. COMPUTATIONAL DETAILS DFT calculations were performed with the JDFTx code using an 60 Ryd planewave cutoff, SG15 ONCV norm-conserving pseudopotentials, and the Perdew-Burke-Ernzerhof (PBE) generalized gradient approxima-FIG. . DFT and G0W0 density of states of (3×3) 1T-MoS2 H adsorbed at the atop S site. tion (GGA) functional. All calculations for the metallic systems used 1st order Methfessel-Paxton 1 st order broadening with a broadening width of 0.2 eV while the 2D layered materials like FeN 4 @G and MoS 2 used a broadening width of 0.002 eV. A 8×8×8, 8×8×8, 12×12×12, and 6×6×1 k-point grid was used for the Si, MgO, bulk primitive fcc Pt cell, and (2×2) 1T-MoS 2 lattice relaxations, respectively. After cleaving each surface, the aperiodic grid direction was reduced to 1. At least 15 Å of vacuum space was added so that the slab width was less than half the length of each z lattice vector. The molecule calculations were performed in a 10.0 × 10.1 × 10.2 Å box at the Γ point.