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The natural minerals pyrite and chalcopyrite have been used as the indicator electrode sensors using acetonitrile and propionitrile as solvents. The results show the exceptional advantage of pyrite and chalcopyrite as electrochemical sensors and also the possibility of the application of these electrodes for the determination in nonaqueous solutions where glass electrode shows many defaults. The behaviour of the pyrite and chalcopyrite indicator electrodes in nitriles were checked by titrating several bases and acids of different strengths using protons and lyate ions generated by the oxidation of some gallic acid esters and dihydroxy phenols, as well as m-cresol and 3-metoxy phenol. The results obtained by using these electrodes were compared with those obtained by the application of a glass electrode under the same conditions, and good agreement, reproducibility and accuracy were obtained. The standard deviation of the determination of the investigated acids and bases was less than 0.9%. In the potentiometric titrations with pyrite and chalcopyrite indicator electrodes, the potential is instantaneously established throughout. Both electrodes can be used without any time limit or without considerable divergence in potentials. ©2011 Sociedade Brasileira de Química.