Nitrogen monoxide and calix[4]pyrrolato aluminate: structural constraint enabled NO dimerization
The dimerization of nitrogen monoxide (NO) is highly relevant in homo- and heterogeneous biochemical and environmental redox processes, but a broader understanding is challenged by the endergonic nature of this equilibrium. The present work describes NO-dimerization leveraged by structurally constra...
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| Main Authors: | , , , |
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| Format: | Article (Journal) |
| Language: | English |
| Published: |
17 Jun 2024
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| In: |
Chemical science
Year: 2024, Volume: 15, Issue: 28, Pages: 10803-10809 |
| ISSN: | 2041-6539 |
| DOI: | 10.1039/D4SC02378A |
| Online Access: | Verlag, kostenfrei, Volltext: https://doi.org/10.1039/D4SC02378A Verlag, kostenfrei, Volltext: https://pubs.rsc.org/en/content/articlelanding/2024/sc/d4sc02378a 
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| Author Notes: | Senta J. Kohl, Lukas M. Sigmund, Manuel Schmitt and Lutz Greb |
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| 520 | |a The dimerization of nitrogen monoxide (NO) is highly relevant in homo- and heterogeneous biochemical and environmental redox processes, but a broader understanding is challenged by the endergonic nature of this equilibrium. The present work describes NO-dimerization leveraged by structurally constrained aluminum and metal-ligand cooperativity at the anionic calix[4]pyrrolato aluminate(III). Quantum chemical calculations reveal the driving force for N-N bond formation, while reactivity tests shed light on subsequent redox chemistry and NO decomposition at metal surfaces. Inhibiting the dimerization pathway by saturating NO's unpaired electron with a phenyl group (nitrosobenzene) allows trapping the 1,2-adduct as a key intermediate. Elevated temperatures result in an unprecedented and high-yielding rearrangement of the calix[4]pyrrolato ligand scaffold. Kinetic and theoretical studies provide a comprehensive picture of the rearrangement mechanism and delineate systematics for ring modification of the prominent calix[4]pyrrole macrocycle. | ||
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