LAUSR

Palladium hydrides (PdHx) have important applications in hydrogen storage, catalysis, and superconductivity. Because of the unique electron subshell structure of Pd, quenching PdHx materials with more than 0.706 hydrogen stoichiometry remains challenging. Here, the 1:1 stoichiometric PdH ( Fm3¯m)$Fm\bar{3}m)$ is successfully synthesized using Pd nano icosahedrons as a starting material via high‐pressure cold‐forging at 0.2 GPa. The synthetic initial pressure is reduced by at least one order of magnitude relative to the bulk Pd precursors. Furthermore, PdH is quenched at ambient conditions after being laser heated ≈2000 K under ≈30 GPa. Corresponding ab initio calculations demonstrate that the high potential barrier of the facets (111) restricts hydrogen atoms' diffusion, preventing hydrogen atoms from combining to generate H2. This study paves the way for the high‐pressure synthesis of metal hydrides with promising potential applications.