A benzothiadiazole based molecule for CO2 capture and reduction in multiple reduced states

• Using small organic molecular redox carriers to reversibly capture CO2 is a promising approach to mitigate the ongoing climate crisis. Some variants of this type of molecule can catalyse the reduction of CO2 into valuable chemicals. 2,1,3-benzothiadiazole (BT) is an interesting unit due to its proven interaction with CO2 upon reduction and the ease to tune its structure. In this work, the molecule 2,1,3-benzothiadiazole-4,7-dicarbonitrile (BTDN) is studied for CO2 and reduction at its different reduced states. The work is carried out with a combination of (spectro-)electrochemical and computational studies. In cyclic voltammetry, one can see a clear interaction between BTDN and CO2 upon BTDN’s second reduction and the appearance of a large current in its third reduction, in the presence of CO2. DFT calculations show a large variety of possible CO2-bound species that can potentially match the experimental data. The binding of CO2 on BTDN is shown to be irreversible upon the oxidation of the species, especially with low concentrations of CO2. From gas chromatography and NMR experiments, small amounts of CO and oxalate were detected after bulk electrolysis.

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NATURVETENSKAP  -- Kemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences (hsv//eng)

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