Predicting the Electrochemical Synthesis of 2D Materials from First Principles

We show that Pourbaix diagrams generated by combining first principles and tabulated experimental data can determine the electrochemical conditions needed to synthesize metastable phases in solution. As an example, we investigate the synthesis of two-dimensional transition-metal carbides and nitrides (M₂Xenes) from their M₂AX phase precursors and observe good agreement between the predicted synthesis conditions and those used for existing M₂Xenes. In addition, we prescribe synthesis conditions to increase the yields of certain M₂Xenes and possibly even enable the synthesis of new M₂Xenes. Our results show that the general stability of nitride M₂Xenes is not dramatically different from their carbide counterparts, but that most of their experimentally available precursors are more difficult to etch initially because of their more inert A elements.