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

作者：Liru Cao, Fenfei Wei, Yang Chen, Xiaoli Pan, Hongchen Cao, Yang Su, Yang Zhao, Dali Chen, Yicong Chai, Lulu Chen, Jian Lin, Sen Lin, Xiaodong Wang, Xianzhi Fu, Tao Zhang · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c14188 · 被引用次数：18 · 研究领域：Catalytic Processes in Materials Science、Electrocatalysts for Energy Conversion、Electronic and Structural Properties of Oxides

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 Ir 1 single-atom catalysts (SACs) that can break scaling-relation limitations, achieving exceptional propane dehydrogenation (PDH) performance. Simple H 2 IrCl 6 impregnation on carbon followed by NH 3 pyrolysis yields a catalyst that achieves ∼33% propane conversion and ∼92% propylene selectivity. It demonstrates a remarkable propylene time-space yield of 14976 mol C 3 H 6 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 NH 3 pyrolysis induces in situ substitution of Cl by N species to generate an Ir–O 2 N 2 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.