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

Soumen Sinhababu, Roushan Prakash Singh, Maxim R. Radzhabov, Jugal Kumawat, Daniel H. Ess and Neal P. Mankad ()
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Soumen Sinhababu: University of Illinois Chicago
Roushan Prakash Singh: University of Illinois Chicago
Maxim R. Radzhabov: University of Illinois Chicago
Jugal Kumawat: Brigham Young University
Daniel H. Ess: Brigham Young University
Neal P. Mankad: University of Illinois Chicago

Nature Communications, 2024, vol. 15, issue 1, 1-7

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-45721-1

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