Precise Atomic Structure Regulation of Single‐Atom Platinum Catalysts toward Highly Efficient Hydrogen Evolution Reaction

Abstract Noble metal single‐atom‐catalysts (SACs) have demonstrated significant potential to improve atom utilization efficiency and catalytic activity for hydrogen evolution reaction (HER). However, challenges still remain in rationally modulating active sites and catalytic activities of SACs, which often results in sluggish kinetics and poor stability, especially in neutral/alkaline media. Herein, precise construction of Pt single atoms anchored on edge of 2D layered Ni(OH) 2 (Pt‐Ni(OH) 2 ‐E) is achieved utilizing in situ electrodeposition. Compared to the single‐atom Pt catalysts anchored on the basal plane of Ni(OH) 2 (Pt‐Ni(OH) 2 ‐BP), the Pt‐Ni(OH) 2 ‐E possesses superior electron affinity and high intrinsic catalytic activity, which favors the strong adsorption and rapid dissociation toward water molecules. As a result, the Pt‐Ni(OH) 2 ‐E catalyst requires low overpotentials of 21 and 34 mV at 10 mA cm −2 in alkaline and neutral conditions, respectively. Specifically, it shows the high mass activity of 23.6 A mg −1 for Pt at the overpotential of 100 mV, outperforming the reported catalysts and commercial Pt/C. This work provides new insights into the rational design of active sites for preparing high‐performance SACs.