期刊
NATURE CHEMISTRY
卷 11, 期 2, 页码 154-160出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41557-018-0167-8
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资金
- Swiss National Science Foundation [200021_162430, 200021_178793]
- Ecole Polytechnique Federale de Lausanne (EPFL)
- Swiss National Science Foundation (SNF) [200021_162430] Funding Source: Swiss National Science Foundation (SNF)
Cooperativity between metal centres is identified as a crucial step in dinitrogen reduction both for the industrial Haber-Bosch process and for the natural fixation of nitrogen by nitrogenase enzymes, but the mechanism of N-2 reduction remains poorly understood. This is in large part because multimetallic complexes that reduce and functionalize dinitrogen in the absence of strong alkali reducing agents are crucial to establish a structure-activity relationship, but remain extremely rare. Recently, we reported a multimetallic nitride-bridged diuranium(III) complex capable of reducing and functionalizing dinitrogen. Here we show that an analogous complex assembled with an oxo instead of a nitride linker also effects the four-electron reduction of dinitrogen, but the reactivity of the resulting oxo-(N-2) complex differs significantly from that of the nitride-(N-2). Computational studies show a different bonding scheme for the dinitrogen where the bridging nitride does participate in the binding and consequent activation of N-2, while the oxide does not.
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