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Beryllium Atom Mediated Dinitrogen Activation via Coupling with Carbon Monoxide.
Guohai Deng1, Sudip Pan2,3, Guanjun Wang1
1Collaborative Innovation Center of Chemistry for Energy Materials, Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials, Fudan University, Shanghai, 200438, China.
Angewandte Chemie (International Ed. in English)
|June 26, 2020
Summary
Researchers explored reactions of beryllium atoms with dinitrogen and carbon monoxide, forming novel isomers. These findings demonstrate nitrogen activation via carbon monoxide coupling mediated by a main group atom.
Area of Science:
- Inorganic Chemistry
- Quantum Chemistry
- Spectroscopy
Background:
- Investigating the reactivity of main group elements with small molecules like dinitrogen (N2) and carbon monoxide (CO) is crucial for understanding chemical bonding and activation processes.
- Beryllium (Be), a light main group element, exhibits unique electronic properties that can influence its interactions with N2 and CO.
Purpose of the Study:
- To synthesize and characterize novel beryllium-containing complexes formed from reactions with dinitrogen and carbon monoxide.
- To elucidate the bonding nature and electronic structure of these complexes using experimental and computational methods.
- To explore the potential of beryllium-mediated reactions for activating the strong triple bond in dinitrogen.
Main Methods:
- Matrix isolation spectroscopy in solid argon at cryogenic temperatures.
- Laser ablation of beryllium atoms.
- Quantum chemical calculations, including charge and energy decomposition analysis.
Main Results:
- Formation of two isomers, end-on bonded NNBeCO and side-on bonded (η2-N2)BeCO, which are nearly isoenergetic.
- The end-on isomer possesses a triplet ground state, while the side-on isomer has a singlet ground state.
- Photoexcitation leads to rearrangement into the NBeNCO isomer, an isocyanate complex with a triplet ground state, indicating N-N bond cleavage.
Conclusions:
- The electronic configuration of beryllium in these complexes involves an excited 2s0 2p2 state, facilitating metal-ligand bonding through σ donation and π backdonation.
- These results showcase the activation of dinitrogen, with complete N-N bond cleavage, through coupling with carbon monoxide mediated by beryllium.
- This study highlights a novel pathway for nitrogen fixation mediated by a main group element.
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