LAUSR

Hydride metallenes show great potential for hydrogen-related catalytic applications due to favorable electronic structures modulated by interstitial hydrogen atoms and large active surface areas of metallenes. Metallene nanostructures generally have compressive strain relative to bulk, which can affect both the stability and the catalytic behavior of hydride metallenes but in general cannot be controlled. Here, we demonstrate highly stable PdHx metallenes with a tensile strained Ru surface layer and reveal the spatial confinement effect of the Ru skin by multiple spectroscopic characterizations and molecular dynamics simulations. These PdHx@Ru metallenes with a 4.5% expanded Ru outer layer exhibit outstanding alkaline hydrogen evolution reaction activity with a low overpotential of 30 mV at 10 mA cm-2 and robust stability with negligible activity decay after 10,000 cycles, which are superior to commercial Pt/C and most reported Ru-based electrocatalysts. Control experiments and first-principles calculations reveal that the tensile strained Ru outer layer lowers the energy barrier of H2O dissociation and provides a moderate hydrogen adsorption energy.