Mechanistic insights on the non-innocent role of electron donors: Reversible photocapture of CO2 by RuII-polypyridyl complexes

Nicolas Queyriaux, Wesley B. Swords, Hemlata Agarwala, Ben A. Johnson, Sascha Ott, Leif Hammarström

Research output: Contribution to journalArticle

Abstract

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.

Original languageEnglish
Pages (from-to)16894-16898
Number of pages5
JournalDalton Transactions
Volume48
Issue number45
DOIs
Publication statusPublished - Jan 1 2019

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Electrons
Ligands
Equilibrium constants
Quantum yield
triethanolamine
1-deoxy-1-morpholinofructose

ASJC Scopus subject areas

  • Inorganic Chemistry

Cite this

Mechanistic insights on the non-innocent role of electron donors : Reversible photocapture of CO2 by RuII-polypyridyl complexes. / Queyriaux, Nicolas; Swords, Wesley B.; Agarwala, Hemlata; Johnson, Ben A.; Ott, Sascha; Hammarström, Leif.

In: Dalton Transactions, Vol. 48, No. 45, 01.01.2019, p. 16894-16898.

Research output: Contribution to journalArticle

Queyriaux, Nicolas ; Swords, Wesley B. ; Agarwala, Hemlata ; Johnson, Ben A. ; Ott, Sascha ; Hammarström, Leif. / Mechanistic insights on the non-innocent role of electron donors : Reversible photocapture of CO2 by RuII-polypyridyl complexes. In: Dalton Transactions. 2019 ; Vol. 48, No. 45. pp. 16894-16898.
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