“…To test the sensitivity of the mass balance to the selected value of ␦ 34 S pyr , we performed the calculations using different values of ␦ 34 S pyr (Ϫ10‰ and 0‰ CDT ), which respectively apportion 61 and 81% of the riverine sulfate to sulfide oxidation, 33 and 14% to gypsum dissolution, with 5% coming from atmospheric deposition. Based on the studies of Taylor (2004) and Taylor and Beaudoin, 2000), the fact that no evaporite deposits have been mapped within the watersheds considered by this study (Wheeler and McFeely, 1991), and constraints imposed by carbon isotope systematics (described further on), we conclude that the average isotopic composition of sulfides in the study area must be closer to 0‰ CDT and therefore that 81% of the sulfate in the rivers originates from sulfide weathering. For rivers where the ␦ 34 S SO4 is more negative than 0‰ CDT , it is assumed that all non-atmospheric sulfate in these rivers can be attributed to pyrite oxidation.…”