Atomic Coordination Editing Achieves Ultraproductive Single-Atom Catalysts with Ultralow Loadings

Fabrication of noble-metal-based catalysts combining ultralow loadings with industrial-grade performance remains a grand challenge. Here, we report a facile strategy to synthesize ppm-level loaded Ir₁ single-atom catalysts (SACs) that can break scaling-relation limitations, achieving exceptional propane dehydrogenation (PDH) performance. Simple H₂IrCl₆ impregnation on carbon followed by NH₃ pyrolysis yields a catalyst that achieves ∼33% propane conversion and ∼92% propylene selectivity. It demonstrates a remarkable propylene time-space yield of 14976 mol_C₃H₆ mol_Ir^-1 h^-1 with an ultralow deactivation constant (0.00191 h^-1), outperforming Ir nanoparticles and most reported noble-metal catalysts. Advanced characterizations and density functional theory calculations disclose that NH₃ pyrolysis induces <i>in situ</i> substitution of Cl by N species to generate an Ir-O₂N₂ active motif, where dual N/O coordination simultaneously drives the PDH reaction and prevents metal aggregation. This approach provides a blueprint for developing industrial-viable SACs that reconcile atom-economy with process-intensity demands, as validated across multiple noble-metal systems.