Ye, C.Shan, J.Zhu, C.Xu, W.Song, L.Zhu, Y.Zheng, Y.Qiao, S.Z.2023-12-122023-12-122023Advanced Energy Materials, 2023; 13(45):2302190-1-2302190-81614-68321614-6840https://hdl.handle.net/2440/140170Regulating 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.en© 2023 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.electrocatalysis; electronic structure; single atom catalysts; site-to-site interaction; spatial structureJournal article10.1002/aenm.2023021902023-12-12659987Shan, J. [0000-0003-4308-5027]Zheng, Y. [0000-0002-2411-8041]Qiao, S.Z. [0000-0002-1220-1761] [0000-0002-4568-8422]