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

Author

Listed:
  • 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)

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.

Suggested Citation

  • Soumen Sinhababu & Roushan Prakash Singh & Maxim R. Radzhabov & Jugal Kumawat & Daniel H. Ess & Neal P. Mankad, 2024. "Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical," Nature Communications, Nature, vol. 15(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45721-1
    DOI: 10.1038/s41467-024-45721-1
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    References listed on IDEAS

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    1. Pablo Garrido-Barros & Joseph Derosa & Matthew J. Chalkley & Jonas C. Peters, 2022. "Tandem electrocatalytic N2 fixation via proton-coupled electron transfer," Nature, Nature, vol. 609(7925), pages 71-76, September.
    2. Jingjing Zhang & Christian Mück-Lichtenfeld & Armido Studer, 2023. "Photocatalytic phosphine-mediated water activation for radical hydrogenation," Nature, Nature, vol. 619(7970), pages 506-513, July.
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