期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 56, 期 21, 页码 5872-5876出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201701504
关键词
dinitrogen; molybdenum; nitrogen fixation; pincer ligand; protonation
资金
- European Research Council (ERC) [646747]
- Fond der Chemischen Industrie
The coupling of electron- and proton-transfer steps provides a general concept to control the driving force of redox reactions. N-2 splitting of a molybdenum dinitrogen complex into nitrides coupled to a reaction with Bronsted acid is reported. Remarkably, our spectroscopic, kinetic, and computational mechanistic analysis attributes N-N bond cleavage to protonation in the periphery of an amide pincer ligands rather than the {Mo-N-2-Mo} core. The strong effect on electronic structure and ultimately the thermochemistry and kinetic barrier of N-N bond cleavage is an unusual case of a proton-coupled metal-to-ligand charge transfer process, highlighting the use of proton-responsive ligands for nitrogen fixation.
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