Hexa‐atom Pt Catalyst Fabricated by a Ligand Engineering Strategy for Efficient Hydrogen Oxidation Reaction

Abstract Atomically precise supported nanocluster catalysts (APSNCs), which feature exact atomic composition, well‐defined structures, and unique catalytic properties, offer an exceptional platform for understanding the structure‐performance relationship at the atomic level. However, fabricating APSNCs with precisely controlled and uniform metal atom numbers, as well as maintaining a stable structure, remains a significant challenge due to uncontrollable dispersion and easy aggregation during synthetic and catalytic processes. Herein, we developed an effective ligand engineering strategy to construct a Pt 6 nanocluster catalyst stabilized on oxidized carbon nanotubes (Pt 6 /OCNT). The structural analysis revealed that Pt 6 nanoclusters in Pt 6 /OCNT were fully exposed and exhibited a planar structure. Furthermore, the obtained Pt 6 /OCNT exhibited outstanding acidic HOR performances with a high mass activity of 18.37 A ⋅ mg pt −1 along with excellent stability during a 24 h constant operation and good CO tolerance, surpassing those of the commercial Pt/C. Density functional theory (DFT) calculations demonstrated that the unique geometric and electronic structures of Pt 6 nanoclusters on OCNT altered the hydrogen adsorption energies on catalytic sites and thus lowered the HOR theoretical overpotential. This work presents a new prospect for designing and synthesizing advanced APSNCs for efficient energy electrocatalysis.