Spatial Structure Engineering of Interactive Single Platinum Sites toward Enhanced Electrocatalytic Hydrogen Evolution

Regulating site-to-site interactions between active sites can effectively tailor the electrocatalytic behavior of single-atom catalysts (SACs). The conventional SACs suffer from low density of single atoms and lack of site-to-site interactions between them. Herein, a series of interactive Pt SACs with controllable Pt–Pt spatial correlation degree and local coordination environment is developed by integrating densely populated Pt single atoms in the sub-lattice of a Co₃O₄ matrix. The obtained interactive Pt-Co₃O₄ catalysts demonstrate remarkable electrocatalytic performance toward hydrogen production, outperforming those of isolated single atom- and nanoparticle-based catalysts. The intrinsic catalytic activity of interactive Pt-Co₃O₄ catalysts is closely dependent on the spatial structure of Pt sites with the adjusted d-band center by regulating contents and atomic configuration of Pt sites. This work provides fundamental insights for the structure-property relationship on interactive single active sites, which is expected to direct the rational design of highly efficient SACs. © 2023 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH.