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Updated: Jan 22, 2026

Fabrication of Spatially Confined Complex Oxides

Fabrication of Spatially Confined Complex Oxides

Published on: July 1, 2013

Dinitrogen-Molybdenum Complex Induces Dinitrogen Cleavage by One-Electron Oxidation.

Akira Katayama¹, Takehiro Ohta^2,3, Yuko Wasada-Tsutsui¹

¹Department of Cooperative Major in Nanopharmaceutical Sciences, Graduate School of Engineering, Nagoya Institute of Technology, Gokiso, Showa, Nagoya, 466-8555, Japan.

Angewandte Chemie (International Ed. in English)

|July 9, 2019

Summary

This study demonstrates N2 cleavage in a molybdenum complex via one-electron oxidation, forming a molybdenum nitride. This nitrogen fixation pathway involves a transient dimeric intermediate, offering new insights into dinitrogen activation.

Keywords:

dinitrogen molybdenum oxidation reaction mechanisms structure elucidation

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Area of Science:

Inorganic Chemistry
Organometallic Chemistry
Nitrogen Fixation

Background:

Dinitrogen (N2) cleavage is crucial for nitrogen fixation.
Molybdenum complexes are key catalysts in nitrogen transformations.
Understanding N2 activation mechanisms is vital for developing efficient synthetic routes.

Purpose of the Study:

To investigate the N2 cleavage mechanism of trans-[Mo(depe)2(N2)2] (1) via one-electron oxidation.
To synthesize and characterize the resulting molybdenum nitride complex.
To elucidate the role of intermediate species in the N2 cleavage process.

Main Methods:

One-electron oxidation using a mild oxidant ([Cp2Fe][BArf4]).
Electrochemical oxidation of the molybdenum complex.
In situ resonance Raman and UV-vis spectroscopies.
Density-functional theory (DFT) calculations.

Main Results:

Synthesis of the molybdenum(IV) terminal nitride complex [Mo(depe)2N][BArf4] (2) from complex 1.
N2 cleavage occurs via a Mo(II)-N=N-Mo(II) intermediate.
Electrochemical oxidation also yields complex 2, with a transient dimeric Mo complex detected.
DFT calculations support a mechanism involving an unstable monomeric Mo(I) species and a dimeric intermediate with a zigzag transition state.

Conclusions:

One-electron oxidation effectively cleaves the N2 ligand in trans-[Mo(depe)2(N2)2].
A dimeric intermediate plays a critical role in the N2 cleavage pathway.
This work provides mechanistic insights into molybdenum-mediated dinitrogen activation.