Dislocation‐Strained IrNi Alloy Nanoparticles Driven by Thermal Shock for the Hydrogen Evolution Reaction

Abstract Designing high‐performance and low‐cost electrocatalysts is crucial for the electrochemical production of hydrogen. Dislocation‐strained IrNi nanoparticles loaded on a carbon nanotube sponge (DSIrNi@CNTS) driven by unsteady thermal shock in an extreme environment are reported here as a highly efficient hydrogen evolution reaction (HER) catalyst. Experimental results demonstrate that numerous dislocations are kinetically trapped in self‐assembled IrNi nanoparticles due to the ultrafast quenching and different atomic radii, which can induce strain effects into the IrNi nanoparticles. Such strain‐induced high‐energy surface structures arising from bulk defects (dislocations), are more likely to be resistant to surface restructuring during catalysis. The catalyst exhibits outstanding HER activity with only 17 mV overpotential to achieve 10 mA cm −2 in an alkaline electrolyte with fabulous stability, exceeding state‐of‐the‐art Pt/C catalysts. These density functional theory results demonstrate that the electronic structure of as‐synthesized IrNi nanostructure can be optimized by the strain effects induced by the dislocations, and the free energy of HER can be tuned toward the optimal region.