Vertical Heterophase for Electrical, Electrochemical, and Mechanical Manipulations of Layered MoTe2

Phase engineering is a breakthrough for various electronic and energy device applications with transition metal dichalcogenides (TMDs). Chemical methods, such as lithium intercalation, are mostly used for phase engineering, which achieves atomically thin flakes and high catalytic performances in several group 6 TMDs including MoS2. However, chemical methods cannot be applied to MoTe2, a widely investigated group 6 TMD with intriguing semiconducting, topological, and catalytic properties. The lack of modifying MoTe2 by chemical methods remains a puzzling issue considering the small energy difference between the polymorphs of MoTe2. Here, a convection‐assisted lithium ion intercalation and phase transition is reported to achieve a vertical heterophase in a MoTe2 crystal. The vertical heterophase in MoTe2 reduces the Schottky barrier with metal electrodes down to 66 meV, enhancing the overall ion conductance for electrochemical hydrogen production. Moreover, the weakened adhesion of the 1T' phase layers on the top and bottom surfaces in the vertical heterophase, formed by the intercalation, enables a unique surface tension‐driven exfoliation of MoTe2 flakes. The heterophase chemical engineering suggests a new platform for hybrid catalysts and next‐generation electronic devices based on 2D materials. Convection‐assisted chemical intercalation is introduced to realize uniform and dual‐face phase transition in layered MoTe2 that provides a functional vertical heterophase structure. The vertical heterophase MoTe2 is demonstrated as a new platform for three distinct applications, hybrid catalysis, automatic exfoliation and next‐generation electronic devices based on 2D materials.