Beyond Conventional Catalysts: Monoelemental Tellurium as a Game Changer for Piezo‐Driven Hydrogen Evolution

Abstract The increasing demand for clean hydrogen production over fossil fuels necessitates the development of sustainable piezoelectrochemical methods that can overcome the limitations of conventional electrocatalytic and photocatalytic approaches. In this regard, existing piezocatalysts face challenges related to their low piezoelectricity or active site coverage for hydrogen evolution reaction (HER). Driven by global environmental concerns, there is a compelling push to engineer practical materials for highly efficient HER. Herein, monoelemental 2D tellurium (Te) is presented as a class of layered chalcogenide with a non‐centrosymmetric crystal structure (P3 1 21 space group). The refined Te nanosheets demonstrate an unprecedented highly efficient H 2 production rate ≈9000 µmol g −1 h −1 under ultrasonic mechanical vibration due to built‐in piezo‐potential in the system. The remarkable piezocatalytic performance of Te nanosheets arises from a synergistic interplay between their semi‐metallic nature, favorable free energy landscape, enhanced electrical conductivity and outstanding piezoelectricity. As a proof of concept, the theoretical approach based on Density Functional Theory (DFT) validates the findings due to the gradual exposure of active sites on the Te nanosheets leading to a self‐optimized catalytic performance for hydrogen generation. Therefore, mechanically driven Te emerges as a promising piezocatalyst with the potential to revolutionize highly efficient and sustainable technology for futuristic applications.