3 years ago
Trivalent Zirconium and Hafnium Metal–Organic Frameworks for Catalytic 1,4-Dearomative Additions of Pyridines and Quinolines
Samuel S. Veroneau, Pengfei Ji, Wenbin Lin, Yang Song, Xuanyu Feng
We report the quantitative conversion of [MIV6(μ3-O)4(μ3-OH)4Cl12]6– nodes in the MCl2-BTC metal–organic framework into the [MIII6(μ3-O)4(μ3-ONa)4H6]6– nodes in MIIIH-BTC (M = Zr, Hf; BTC is 1,3,5-benzenetricarboxylate) via bimetallic reductive elimination of H2 from putative [MIV6(μ3-O)4(μ3-OH)4H12]6– nodes. The coordinatively unsaturated MIIIH centers in MIIIH-BTC are highly active and selective for 1,4-dearomative hydroboration and hydrosilylation of pyridines and quinolines. This work demonstrated the potential of secondary building unit transformation in generating electronically unique and homogeneously inaccessible single-site solid catalysts for organic synthesis.
Publisher URL: http://dx.doi.org/10.1021/jacs.7b09093
DOI: 10.1021/jacs.7b09093
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