Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical
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 prot...
| Main Authors: | , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-02-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-45721-1 |
| _version_ | 1797273930872913920 |
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| author | Soumen Sinhababu Roushan Prakash Singh Maxim R. Radzhabov Jugal Kumawat Daniel H. Ess Neal P. Mankad |
| author_facet | Soumen Sinhababu Roushan Prakash Singh Maxim R. Radzhabov Jugal Kumawat Daniel H. Ess Neal P. Mankad |
| author_sort | Soumen Sinhababu |
| collection | DOAJ |
| description | 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. |
| first_indexed | 2024-03-07T14:51:10Z |
| format | Article |
| id | doaj.art-1251c1750e1442feb639bfe6c76d8c89 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-07T14:51:10Z |
| publishDate | 2024-02-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-1251c1750e1442feb639bfe6c76d8c892024-03-05T19:39:15ZengNature PortfolioNature Communications2041-17232024-02-011511710.1038/s41467-024-45721-1Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radicalSoumen Sinhababu0Roushan Prakash Singh1Maxim R. Radzhabov2Jugal Kumawat3Daniel H. Ess4Neal P. Mankad5Department of Chemistry, University of Illinois ChicagoDepartment of Chemistry, University of Illinois ChicagoDepartment of Chemistry, University of Illinois ChicagoDepartment of Chemistry and Biochemistry, Brigham Young UniversityDepartment of Chemistry and Biochemistry, Brigham Young UniversityDepartment of Chemistry, University of Illinois ChicagoAbstract 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.https://doi.org/10.1038/s41467-024-45721-1 |
| spellingShingle | Soumen Sinhababu Roushan Prakash Singh Maxim R. Radzhabov Jugal Kumawat Daniel H. Ess Neal P. Mankad Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical Nature Communications |
| title | Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical |
| title_full | Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical |
| title_fullStr | Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical |
| title_full_unstemmed | Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical |
| title_short | Coordination-induced O-H/N-H bond weakening by a redox non-innocent, aluminum-containing radical |
| title_sort | coordination induced o h n h bond weakening by a redox non innocent aluminum containing radical |
| url | https://doi.org/10.1038/s41467-024-45721-1 |
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