Phase, Conductivity, and Surface Coordination Environment in Two-Dimensional Electrochemistry

The booming frontier of electrochemistry is radically transforming the landscape of global chemical and energy industry. Most recent advancements in electrocatalysts have been built on trial and error, lacking model experiments to illuminate the fundamental factors hidden behind, such as phase, conductivity, and surface coordination environment. Here, we use phase-controllable, highly oriented two-dimensional MoTe2 as the model catalysts. The 2H phase MoTe2’s conductivity can be engineered both extrinsically and intrinsically by single-layer graphene and lithiation, bringing down the sheet resistance from 0.95 MΩ/□ to 0.8 kΩ/□ and 0.6 kΩ/□. The corresponding electrocatalytic performance was unlocked from a silent state, catching up to its 1T′ counterpart, with a parallel Tafel slope of 141 mV/dec. A focused ion beam further exposed the edge atoms, which exhibited a hydrogen evolution turnover frequency 104 times superior to that of basal plane atoms.