Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 29, Pages 9795-9798Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b05018
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Funding
- China Ministry of Science and Technology [2016YFA (0202801)]
- National Natural Science Foundation of China [21521091, 21390393, U1463202, 21471089, 21671117]
- German Research Foundation (DFG) through the Collaborative Research Center [SFB-658]
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Here we report a novel approach to synthesize atomically dispersed uniform clusters via a cage-separated precursor preselection and pyrolysis strategy. To illustrate this strategy, well-defined Ru-3(CO)(12) was separated as a precursor by suitable molecular-scale cages of zeolitic imidazolate frameworks (ZIFs). After thermal treatment under confinement in the cages, uniform Ru-3 dusters stabilized by nitrogen species (Ru-3/CN) were obtained. Importantly, we found that Ru-3/CN exhibits excellent catalytic activity (100% conversion), high chemoselectivity (100% for 2-aminobenzaldehyde), and significantly high turnover frequency (TOF) for oxidation of 2-aminobenzyl alcohol. The TOF of Ru-3/CN (4320 h(-1)) is about 23 times higher than that of small-sized (ca. 2.5 nm) Ru particles (TOF = 184 h(-1)). This striking difference is attributed to a disparity in the interaction between Ru species and adsorbed reactants.
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