The effects of pH on sulfur-induced passivity degradation of Alloy 800 in simulated crevice chemistries were evaluated using electrochemical impedance spectroscopy (EIS), secondary ion, mass spectroscopy (SIMS), and Mott-Schottky analysis methods. Experimental results reveal that the detrimental effect of impurities containing sulfur at the reduced or intermediate oxidation level (S-x) on the passivity of Alloy 800 depends significantly on the solution pH. In neutral crevice (NC) chemistry containing chloride ions, the S-x obstructs the healing process during repassivation, retards the dehydration reaction and also incorporates H, OH and S into the passive film. However, the detrimental effect of S-x is insignificant in an alkaline crevice (AKC) solution due to a change in surface adsorption and surface charge. Impurities containing sulfur at the reduced or intermediate oxidation level would cause Alloy 800 to lose its passivity and become active in an acidic crevice (AC) chemistry. Experimental evidence also indicates that the solution pH alters the semiconductor type of the surface film from n-type in NC solution to p-type in AKC solution. (C) 2014 The Electrochemical Society. All rights reserved.