Reversible CO 2 binders under ambient conditions are of significant interest for multiple applications in sensing and capture technologies. In this paper, a general systematic way to evaluate CO 2 receptors with π-systems is put forward. A series of receptors (five pyridine-based and one triazine-based) are evaluated as CO 2 binders in terms of number of hydrogen bonding sites, strength of hydrogen bond donors, and number of nucleophilic sites. The binding of CO 2 to the receptors was probed by computational models, absorption spectroscopy, fluorescence spectroscopy, cyclic voltammetry, and 1 H NMR studies. Multiple solvents with varying ionic strength additives are probed to analyze the effects on CO 2 -bound intermediates. The receptors were screened progressively down-selecting through the different analytical techniques arriving at a promising pyridine receptor, which shows evidence of CO 2 binding with each of the analytical techniques. The diaminopyridine motif demonstrates reversible CO 2 binding and has convenient substitution sites for derivatization to incorporate into functional sensor systems.
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