ArticleAngewandte Chemie (International ed. in English)2021
Dioxygen Activation and Pyrrole α-Cleavage with Calix[4]pyrrolato Aluminates: Enzyme Model by Structural Constraint.
Article in Angewandte Chemie (International ed. in English), 2021. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 12 papers.
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12 citing papers in PubMed.
- Activation of Dioxygen via Neodymium-Alkali Metal Clusters.Journal of the American Chemical Society · 2026Article
- COJournal of the American Chemical Society · 2025Article
- Diverse Superatomic Magnetic and Spin Properties of AuACS central science · 2025Article
- Understanding Nanoparticle Electronic Spin-State Dynamics and Properties Using Variable-Temperature, Variable-Field Magnetic Circular Photoluminescence.Chemphyschem : a European journal of chemical physics and physical chemistry · 2025Review
- Nitrogen monoxide and calix[4]pyrrolato aluminate: structural constraint enabled NO dimerization.Chemical science · 2024Article
- Calix[4]pyrrolato-germane-(thf)Journal of the American Chemical Society · 2023Article
- Four-Electron Reduction of OJournal of the American Chemical Society · 2023Article
- Calix[4]pyrrolato gallate: square planar-coordinated gallium(iii) and its metal-ligand cooperative reactivity with COChemical science · 2022Article
- Calix[4]pyrrolato Aluminate Catalyzes the Dehydrocoupling of Phenylphosphine Borane to High Molar Weight Polymers.Angewandte Chemie (International ed. in English) · 2022Article
- Calix[4]pyrrolato Stannate(II): A Tetraamido Tin(II) Dianion and Strong Metal-Centered σ-Donor.Angewandte Chemie (International ed. in English) · 2022Article
- Towards deeper understanding of multifaceted chemistry of magnesium alkylperoxides.Communications chemistry · 2021Article
- Dioxygen Activation and Pyrrole α-Cleavage with Calix[4]pyrrolato Aluminates: Enzyme Model by Structural Constraint.Angewandte Chemie (International ed. in English) · 2021Article
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6 authors.
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Abstract
The present work describes the reaction of triplet dioxygen with the porphyrinogenic calix[4]pyrrolato aluminates to alkylperoxido aluminates in high selectivity. Multiconfigurational quantum chemical computations disclose the mechanism for this spin-forbidden process. Despite a negligible spin-orbit coupling constant, the intersystem crossing (ISC) is facilitated by singlet and triplet state degeneracy and spin-vibronic coupling. The formed peroxides are stable toward external substrates but undergo an unprecedented oxidative pyrrole α-cleavage by ligand aromatization/dearomatization-initiated O-O σ-bond scission. A detailed comparison of the calix[4]pyrrolato aluminates with dioxygen-related enzymology provides insights into the ISC of metal- or cofactor-free enzymes. It substantiates the importance of structural constraint and element-ligand cooperativity for the functions of aerobic life.
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