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The rational design of hydrogen evolution reaction (HER) electrocatalystswhich are competitive with platinum is an outstanding challenge to makepower-to-gas technologies economically viable. Here, we introduce thedelafossites PdCrO$_2$, PdCoO$_2$ and PtCoO$_2$ as a new family ofelectrocatalysts for the HER in acidic media. We show that in PdCoO$_2$ theinherently strained Pd metal sublattice acts as a pseudomorphic template forthe growth of a strained (by +2.3%) Pd rich capping layer under reductiveconditions. The surface modification continuously improves the electrocatalyticactivity by simultaneously increasing the exchange current density j$_0$ from 2to 5 mA/cm$^2_{geo}$ and by reducing the Tafel slope down to 38 mV/decade,leading to overpotentials $\eta_{10}$ < 15 mV for 10 mA/cm$^2_{geo}$, superiorto bulk platinum. The greatly improved activity is attributed to the in-situstabilization of a $\beta$-palladium hydride phase with drastically enhancedsurface catalytic properties with respect to pure or nanostructured palladium.These findings illustrate how operando induced electrodissolution can be usedas a top-down design concept for rational surface and property engineeringthrough the strain-stabilized formation of catalytically active phases.

Rational Strain Engineering in Delafossite Oxides for Highly Efficient Hydrogen Evolution Catalysis in Acidic Media