Coupling Interaction between Precisely Located Pt Single‐Atoms/Clusters and NiCo‐Layered Double Oxide to Boost Hydrogen Evolution Reaction

Catalysts based on Pt single atom (SA) on metal oxides have shown tremendous potentials for alkaline hydrogen evolution reaction (HER), but they are severely limited by insufficient electron interactions of Pt sites and supports. Herein, a new methodology is developed to precisely locate Pt SAs and Pt clusters into NiCo layered double oxide (LDO) nanosheets, achieved using a dual‐ion etching process with subsequent phase transformation method. Uniquely, the Pt SAs are inserted into LDO layers to form Pt─Co bonds by occupying partial Ni positions, significantly strengthening electron interactions with NiCo LDO and promoting activity of HER. Results from density functional theory calculations indicate that the H* species are preferentially absorbed onto O sites on top of these Pt SAs, which are coupled with their adjacent Pt clusters to accelerate water dissociation in the Volmer step. As‐obtained Pt─NiCo LDO exhibits a low overpotential of 92 mV at 10 mA cm−2 and a Tafel slope of 73 mV dec−1, an excellent stability over 105 hours at 60 mA cm−2, and its mass activity is 6 times higher than commercial 20% Pt/C. This study highlights essential functions of coupling interactions between Pt SAs/clusters and LDOs to boost HER for hydrogen energy production.