The presented work was explicitly concentrated on creating a correlated connection between theoretical and experimental applications via designing and developing three membrane electrodes, including three different cyclodextrins as modifier ionophores. They were decorated with sodium tetraphenylborate as an anionic exchanger and dioctyl phthalate as a plasticizer to analyze benazepril hydrochloride in the pure and pharmaceutical dosage form. Molecular modeling applications were applied to expect the structure of the inclusion complexes of benazepril hydrochloride and cyclodextrins. Experimental design approaches were used for the optimization of the composition of the most promising candidate sensor. Three independent parameters, including the amount of plasticizer (DOP), ion-pair, and ionophore (β-CD), were utilized to build up the mathematical design. Here the Response Surface Methodology (RSM) relied on central composite design (CCD) to estimate and optimize these independent factors. Derringer’s desirability function was proceeded to optimize the slope of benazepril using the most promising candidate sensor. The suggested optimum conditions were 0.29 mg of DOP, 9.54 mg of β-CD, and 9.03 mg of the ion-pair. The optimized sensor had a linear range of (1 × 10−5–1 × 10−2 mol.l−1) and a limit of detection of 5.01 × 10−6 mol.l−1. The developed methods were validated according to IUPAC recommendations.
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