Origins of Different Performances of the VSx (x = 2, 4) Materials in Electroreduction of Nitrogen

Abstract

The synthesis of a VS 4 -140 material and its high performance in electrocatalytic nitrogen reduction are reported. VS 4 -140 shows the highest NH 3 yield of 46.74 μg h −1 mg cat −1 with a faradaic efficiency (FE) of 8.5% at −0.59 V (vs RHE), superior to VS 2 . By using first-principles calculations, we identify the different behaviors of VS 2 and VS 4 -140 regarding both the reaction mechanism and the associated electronic origins. The reduction of nitrogen proceeds preferentially via the alternative pathway with VS 4 -140. This work points out the promising potential of vanadium tetrasulfide in nitrogen reduction and provides ideas for the design of more efficient catalysts.