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

Abstract

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 molC3H6 molIr-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 in situ 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.