Chemistry - A European Journal
Chemistry - A European Journal
5 years ago

Synthesis and Characterization of Bioinspired [Mo2Fe2]–Hydride Cluster Complexes and Their Application in the Catalytic Silylation of N2

Synthesis and Characterization of Bioinspired [Mo2Fe2]–Hydride Cluster Complexes and Their Application in the Catalytic Silylation of N2
Mizuki Tada, Yuna Araki, Yoichi Sakai, Yasuhiro Ohki
The hydride-supported [Mo2Fe2] cluster complex {Cp*Mo(PMe3)}2{FeN(SiMe3)2}2(H)8 (2 a; Cp*=η5-C5Me5) and its [Mo2Mn2] congener 2 b were synthesized from the reactions of Cp*Mo(PMe3)(H)5 (1) with M{N(SiMe3)2}2 (M=Fe, Mn). The amide-to-thiolate ligand-exchange reactions of complex 2 a with bulky thiol reagents (HSR; R=2,4,6-iPr3C6H2 (Tip), 2,6-(SiMe3)2C6H3 (Btp)) furnished the corresponding hydride-supported [Mo2Fe2](SR)2 cluster complexes. The [Mo2Fe2] clusters served as catalyst precursors for the reductive silylation of N2 and yielded ≈65–69 equivalents of N(SiMe3)3 relative to the [Mo2Fe2] clusters. Treatment of complexes 2 a and b with an excess of CNtBu resulted in the formation of dinuclear Mo−Fe and Mo−Mn complexes, which indicated that the [Mo2M2] cores (M=Fe, Mn) split into two dinuclear species upon accommodation of substrates. Reduction of N2: Taking inspiration from the biological process, hydride-supported [Mo2Fe2] cluster complexes are synthesized, characterized, and successfully used as catalyst precursors for the reductive silylation of N2 (see scheme).

Publisher URL: http://onlinelibrary.wiley.com/resolve/doi

DOI: 10.1002/chem.201702925

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