Atomic Coordination Editing Achieves Ultraproductive Single-Atom Catalysts with Ultralow Loadings
A collaborative team led by Academician Zhang Tao, Researcher Wang Xiaodong, and Researcher Lin Jian from the Dalian Institute of Chemical Physics, together with Academician Fu Xianzhi and Professor Lin Sen from Fuzhou University, has made significant progress in regulating the microenvironment around single atoms. They successfully prepared highly efficient single-atom catalysts with ultralow loadings via microenvironment coordination editing.
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 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.
The related research findings have been published in the Journal of the American Chemical Society under the title "Atomic Coordination Editing Achieves Ultraproductive Single-Atom Catalysts with Ultralow Loadings". The co-first authors of this work are Dr. Cao Liru (DICP, Group 1503) and Dr. Wei Fenfei (Nanjing University). This research was supported by projects from the National Natural Science Foundation of China, the Liaoning Revitalization Talents Program, the Dalian Outstanding Young Sci-Tech Talent Support Program, and the Youth Innovation Promotion Association of CAS. (Text/Images by Cao Liru)
Article Link: https://doi.org/10.1021/jacs.5c14188
