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Dinitrogen binding and activation at a molybdenum-iron-sulfur cluster
Alex McSkimming1,2, Daniel L M Suess3
1Department of Chemistry, Massachusetts Institute of Technology, Cambridge, MA, USA.
Nature Chemistry
|May 28, 2021
Summary
Researchers created a synthetic iron-sulfur (Fe-S) cluster capable of binding and activating nitrogen (N2). This breakthrough advances understanding of nitrogen fixation, a vital process for life.
Area of Science:
- Bioinorganic Chemistry
- Organometallic Chemistry
- Catalysis
Background:
- Nitrogenases catalyze the essential conversion of atmospheric nitrogen (N2) to ammonia (NH3).
- Synthetic models of nitrogenase cofactors are crucial for understanding their mechanisms.
- Direct observation of N2 binding to synthetic Fe-S clusters has been challenging.
Purpose of the Study:
- To design and synthesize a novel Fe-S cluster capable of coordinating and activating N2.
- To investigate the electronic and structural changes upon N2 binding.
- To elucidate the role of covalent interactions in N2 activation.
Main Methods:
- Synthesis of a [MoFe3S4] cluster embedded in a protective ligand environment.
- Characterization of the resulting complex using X-ray crystallography and spectroscopy.
- Investigation of N2 binding and activation through structural and electronic analyses.
Main Results:
- A well-defined coordination complex, [MoFe3S4]2(μ-η1:η1-N2), capable of binding N2 at iron (Fe) centers was successfully prepared.
- The N-N bond in the coordinated N2 ligand was significantly weakened.
- Substitution with a titanium (Ti) metalloradical enhanced charge transfer to N2, generating Fe-N multiple bond character and indicating N2 activation.
Conclusions:
- The synthetic Fe-S cluster demonstrates effective N2 binding and activation, mimicking aspects of nitrogenase function.
- N2 activation is associated with shortened Fe-S distances and charge transfer across the cluster.
- Covalent interactions within the cluster are critical for N2 binding and subsequent activation.
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