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Potentiometric sensing devices were prepared based on ion-selective membranes (ISM) containing Hamilton-type receptors incorporated into polymer membranes. Measurement capabilities of these devices were evaluated and exhibit near-Nernstian sensitivities in several different aqueous matrices, demonstrating the utility of Hamilton receptors within polymer membranes for potentiometric detection of barbiturates in water. This work also investigates the effects of receptor preorganization on sensor performance and compares these effects to those observed for similar receptor systems in solution.