Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical

Several renewable energy schemes aim to use the chemical bonds in abundant molecules like water and ammonia as energy reservoirs. Because the O-H and N-H bonds are quite strong (>100 kcal/mol), it is necessary to identify substances that dramatically weaken these bonds to facilitate proton-couple...

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Bibliographic Details
Published in:Nature communications 2024-02, Vol.15 (1), p.1315-1315, Article 1315
Main Authors: Sinhababu, Soumen, Singh, Roushan Prakash, Radzhabov, Maxim R., Kumawat, Jugal, Ess, Daniel H., Mankad, Neal P.
Format: Article
Language:English
Subjects:
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140/131
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Aluminum
Ammonia
Bonding strength
Chemical bonds
Coordination
Electron transfer
Energy conversion
Humanities and Social Sciences
Hydrogen bonds
Ligands
Metals
multidisciplinary
Periodic table
Protons
Renewable energy
Science
Science (multidisciplinary)
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Summary:Several renewable energy schemes aim to use the chemical bonds in abundant molecules like water and ammonia as energy reservoirs. Because the O-H and N-H bonds are quite strong (>100 kcal/mol), it is necessary to identify substances that dramatically weaken these bonds to facilitate proton-coupled electron transfer processes required for energy conversion. Usually this is accomplished through coordination-induced bond weakening by redox-active metals. However, coordination-induced bond weakening is difficult with earth’s most abundant metal, aluminum, because of its redox inertness under mild conditions. Here, we report a system that uses aluminum with a redox non-innocent ligand to achieve significant levels of coordination-induced bond weakening of O-H and N-H bonds. The multisite proton-coupled electron transfer manifold described here points to redox non-innocent ligands as a design element to open coordination-induced bond weakening chemistry to more elements in the periodic table. Coordination-induced bond weakening (CIBW) by redox-active metals is used to weaken bonds in water and ammonia to facilitate proton-coupled electron transfer but achieving CIBW using aluminium as abundant metal is challenging. Here, the authors report a system that uses aluminum with a redox non-innocent ligand to achieve CIBW of O-H and N-H bonds.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-024-45721-1