Energetics and Mechanism of Dinitrogen Cleavage at a Mononuclear Surface Tantalum Center: A New Way of Dinitrogen Reduction

摘要

Synthesis of ammonia from dinitrogen (N2) is one of the most important reactions not only in industry but also in biology. In industry, the Haber-Bosch process involves a heterogeneous catalytic reaction in which N2 and H2 react on a supported Fe or Ru nano-particle catalyst at high temperature (350-550 °C) and pressure (150-350 atm). In biology, several types of nitrogenases catalyze the conversion of N2 to ammonia at ambient temperature and pressure. For decades, enormous efforts have been made to split the robust N≡N bond under mild conditions. Multimetal cooperation was found to be the rule for N2 activation with a few exceptions, such as molybdenum and tungsten complexes.