A Laser‐Triggered Self‐Decomposition Strategy for Engineering Boridene‐Supported Metal Nanoparticles With Electronic Metal‐Support Interactions

ABSTRACT 2D transition‐metal borides (MBenes), such as Boridene (Mo 4/3 B 2 T x ), exhibit excellent catalytic potential but suffer from instability, high resistivity, and loaded nanoparticle deactivation. Here, a laser‐triggered self‐decomposition strategy is developed to activate thermally unstable Boridene, cleaving Mo─B bonds and producing defective Mo nanoparticles (Mo V ) that form electronic metal‐support interactions (EMSIs) with the Boridene substrate (Mo V /Boridene). Analyses of Gibbs free energy and bond energetics confirm the intrinsic instability of Boridene, revealing that its negative Gibbs free energy and relatively weak Mo─B bonds drive a thermodynamic propensity for controlled decomposition. Driven by EMSIs that enhance interface durability and optimize the electronic structure for accelerated oxygen electrocatalysis, the Mo V /Boridene cathode achieves a low overpotential (0.32/0.40 V) and ultralong cyclability (550 cycles), surpassing most existing Mo‐based lithium‐oxygen batteries (LOBs) to date. This strategy is further demonstrated in another Mo 2 C MXene system with EMSI effects, establishing a versatile platform for activating MBenes/MXenes and expanding their potential applications in energy storage and conversion.