Electrochemical Nitrate Reduction Catalyzed by Two-Dimensional Transition Metal Borides.

We investigated 2D transition metal borides (MBenes) for the efficient conversion of nitrate to ammonia. MBenes have been previously shown to bind oxygen with extraordinary strength, which should translate toward selective adsorption of nitrate in aqueous media. Using Density Functional Theory, we screened MBenes by computing their nitrate and water adsorption energies, seeking materials with strong nitrate binding and weak water binding. We identified MnB, CrB, and VB as the best materials for selective nitrate adsorption and proceeded by computing their free energies for generating ammonia. Of the three candidates, CrB requires the lowest overpotential, making it the best candidate. To further decrease the overpotential, we doped the CrB MBene with secondary transition metals and found the addition of Mn to the active site further reduced the overpotential. We then computed the reaction mechanism grand canonically to observe the effect of applied potential on the free energy landscape.