Confined Pyrolysis within Metal-Organic Frameworks to Uniform Ru3 Clusters for Efficient Oxidation of Alcohols
Shufang Ji, Chen Yuanjun, Qiang Fu, Yifeng Chen, Juncai Dong, Wenxing Chen, Zhi Li, Yu Wang, Lin Gu, Wei He, Chen Chen, Qing Peng, Yu Huang, Xiangfeng Duan, Dingsheng Wang, Claudia Draxl, Yadong Li
J. Am. Chem. Soc. 139, 9795-9798 (2017)
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 Ru3(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 Ru3 clusters stabilized by nitrogen species (Ru3/CN) were obtained. Importantly, we found that Ru3/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 Ru3/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.