Density functional theory (DFT) calculations were carried out to gain insights into the electronic properties of the synthesized molecules (Figures 2c and S23-S26); estimate the thermodynamic hydricity (𝜟𝑮 𝑯 -) of potential active species (Table ); and gain mechanistic insights of the electrocatalytic activity of BT-DCAF towards the H2 evolution reaction (Figures ).