Batch treatability studies for a Cr(VI)-contaminated glacial soil from a Cr plating facility were conducted using 1X and 2X the stoichiometric ratio of calcium polysulfide (CPS). The pH of the treated soil increased from 6 to 11 upon CPS addition, but progressively returned to 8-8.5 over the course of 1 year. The 1X dosage maintained a highly reducing environment up to 21 days of monitoring with the samples exposed to atmospheric oxygen, while 2X was reducing up to 180 days of curing. The EPA regulatory method for solid Cr(VI) could not reliably predict Cr(VI) in the treated solid due to ongoing reduction during the test. SPLP results showed that the CPS created an apparent Cr(VI) mobilization during the first 60 days of treatment, with subsequent decrease in soluble Cr(VI) up to 1 year of monitoring. Synchrotron micro-X-ray analyses at 60 days curing showed that Cr(VI) was predominantly bound as highly insoluble PbCrO4 that precipitated in the interstitial pores of the soil, with very little to no Cr(VI) associated with the abundant iron oxyhydroxides. Despite its spatial accessibility and due to its low solubility, PbCrO4 was recalcitrant to treatment, which proceeded only very slowly as judged by the SPLP data. It is concluded that, while CPS has a long residence time in the environment and is a promising reductant, in situ reduction is not an efficient treatment method for soils with highly insoluble Cr(VI) compounds, especially in surficial layers such as the one studied. (C) 2010 Elsevier B.V. All rights reserved.