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

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Abstract
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 Co 3 O 4 matrix. The obtained interactive Pt‐Co 3 O 4 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‐Co 3 O 4 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.
Funding Information
  • Australian Research Council (FL170100154)
  • Australian Research Council (DP220102596)
  • Australian Research Council (DP190103472)
  • Australian Research Council (LP210301397)
  • Australian Research Council (DE230101011)

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