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A lead( ii )– N ′-isonicotinoylpyrazine-2-carbohydrazonamide complex system as a converter of aerial carbon dioxide to carbonate under electrochemical conditions with the formation of a single-component white light-emitting phosphor

In this contribution, a novel binuclear heteroleptic complex [Pb 2 L 2 (CO 3 )]·2CH 3 CN·2MeOH (1·2CH 3 CN·2MeOH) is reported, which was fabricated by electrochemical oxidation of a lead anode under an ambient atmosphere in a CH 3 CN : MeOH solution of N ′-isonicotinoylpyrazine-2-carbohydrazonamide...

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Bibliographic Details
Published in:CrystEngComm 2024-08, Vol.26 (31), p.4205-4213
Main Authors: Mahmoudi, Ghodrat, Garcia-Santos, Isabel, Labisbal, Elena, Castiñeiras, Alfonso, Alizadeh, Vali, Gomila, Rosa M., Frontera, Antonio, Safin, Damir A.
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Language:English
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Summary:In this contribution, a novel binuclear heteroleptic complex [Pb 2 L 2 (CO 3 )]·2CH 3 CN·2MeOH (1·2CH 3 CN·2MeOH) is reported, which was fabricated by electrochemical oxidation of a lead anode under an ambient atmosphere in a CH 3 CN : MeOH solution of N ′-isonicotinoylpyrazine-2-carbohydrazonamide (HL). The CO 3 2− anion was produced from the conversion of aerial CO 2 by the Pb 2+ –L complex system under electrochemical conditions. In the structure of 1, ligand L exhibits a tridentate pincer-like N , N ′, O -coordination mode, while the CO 3 2− anion exhibits a tetradentate bridging coordination mode with one of the oxygen atoms exhibiting a bridging μ-coordination mode. The metal cations in the structure of 1 are in a five-membered N 2 O 3 coordination environment, formed by covalent bonds. The molecular structure of 1·2CH 3 CN·2MeOH is stabilized by a pair of intermolecular Pb⋯N tetrel bonds formed with one of the NH 2 nitrogen atoms of an adjacent complex molecule and with the acetonitrile nitrogen atom, and one Pb⋯O tetrel bond formed with the carbonyl oxygen atom of the other adjacent complex molecule, yielding a 2D supramolecular sheet. This sheet is further stabilized by intermolecular N–H⋯N acetonitrile and N–H⋯O carbonate hydrogen bonds and π Pyrazine ⋯π Pyridine interactions. The optical properties of the complex were revealed by UV-vis spectroscopy and spectrofluorimetry in MeOH. It was established that the described complex is emissive upon excitation at 340 nm with a broad band from about 500 nm to 780 nm with a maximum at ∼580 nm, accompanied by a shoulder at ∼620 nm. The CIE-1931 chromaticity coordinates of (0.28, 0.36) fall within the white gamut of the chromaticity diagram. Thus, complex 1 is a single-component white light-emitting phosphor.
ISSN:1466-8033
1466-8033
DOI:10.1039/D4CE00562G