Mechanistic insights on the non-innocent role of electron donors: reversible photocapture of CO2 by RuII-polypyridyl complexes
The ability of [RuII(tButpy)(dmbpy)(MeCN)]2+ (1-MeCN) to capture CO2, with the assistance of triethanolamine (TEOA), has been assessed under photocatalytically-relevant conditions. The photolability of 1-MeCN has proven essential to generate a series of intermediates which only differ by the nature...
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| Veröffentlicht in: | Dalton transactions : an international journal of inorganic chemistry 2019-12, Vol.48 (45), p.16894-16898 |
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| container_issue | 45 |
| container_start_page | 16894 |
| container_title | Dalton transactions : an international journal of inorganic chemistry |
| container_volume | 48 |
| creator | Queyriaux, Nicolas Swords, Wesley B Agarwala, Hemlata Johnson, Ben A Ott, Sascha Hammarström, Leif |
| description | The ability of [RuII(tButpy)(dmbpy)(MeCN)]2+ (1-MeCN) to capture CO2, with the assistance of triethanolamine (TEOA), has been assessed under photocatalytically-relevant conditions. The photolability of 1-MeCN has proven essential to generate a series of intermediates which only differ by the nature of their monodentate ligand. In DMF, ligand photoexchange of 1-MeCN to give [RuII(tButpy)(dmbpy)(DMF)]2+ (1-DMF) proceeds smoothly with a quantum yield of 0.011. However, in the presence of TEOA, this process was disrupted, leading to the formation of a mixture of 1-DMF and [RuII(tButpy)(dmbpy)(TEOA)]+ (1-TEOA). An equilibrium constant of 3 was determined. Interestingly, 1-TEOA demonstrated an ability to reversibly catch and release CO2 making it a potentially crucial intermediate towards CO2 reduction. |
| doi_str_mv | 10.1039/c9dt03461g |
| format | Article |
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The photolability of 1-MeCN has proven essential to generate a series of intermediates which only differ by the nature of their monodentate ligand. In DMF, ligand photoexchange of 1-MeCN to give [RuII(tButpy)(dmbpy)(DMF)]2+ (1-DMF) proceeds smoothly with a quantum yield of 0.011. However, in the presence of TEOA, this process was disrupted, leading to the formation of a mixture of 1-DMF and [RuII(tButpy)(dmbpy)(TEOA)]+ (1-TEOA). An equilibrium constant of 3 was determined. 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| identifier | ISSN: 1477-9226 |
| ispartof | Dalton transactions : an international journal of inorganic chemistry, 2019-12, Vol.48 (45), p.16894-16898 |
| issn | 1477-9226 1477-9234 |
| language | eng |
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| source | Royal Society Of Chemistry Journals; Alma/SFX Local Collection |
| subjects | Carbon dioxide Donors (electronic) Ligands Triethanolamine |
| title | Mechanistic insights on the non-innocent role of electron donors: reversible photocapture of CO2 by RuII-polypyridyl complexes |
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