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Methane emissions from streams and rivers have recently been recognized as an important component of global greenhouse budgets. Stream methane is lost as evasion to the atmosphere or in-stream methane oxidation. Previous studies have quantified evasion and oxidation with point-scale measurements. In this study, dissolved gases (methane, krypton) were injected into a coastal plain stream in North Carolina to quantify stream CH4 losses at the watershed scale. Stream-reach modeling yielded gas transfer and oxidation rate constants of 3.2 ± 0.5 and 0.5 ± 1.5 d-1, respectively, indicating a ratio of about 6:1. The resulting evasion and oxidation rates of 2.9 mmol m-2 d-1 and 1,140 nmol L-1 d-1, respectively, lie within ranges of published values. Similarly, the gas transfer velocity (K600) of 2.1 m d-1 is consistent with other gas tracer studies. This study illustrates the utility of dissolved-gas tracers for evaluating stream methane fluxes. In contrast to point measurements, this approach provides a larger watershed-scale perspective. Further work is needed to quantify the magnitude of these fluxes under varying conditions (e.g., stream temperature, nutrient load, gradient, flow rate) at regional and global scales before reliable bottom-up estimates of methane evasion can be determined at global scales. [ABSTRACT FROM AUTHOR]

Per- and polyfluoroalkyl substances (PFAS) are known to be highly persistent in groundwater, making it vital to develop new approaches to important practical questions such as the time scale for future persistence of PFAS in contaminated groundwater. In the approach presented here, groundwater from beneath streambeds was analyzed for PFAS and age-dated using SF 6 and 3 H/ 3 He. The results were coupled with groundwater flux measurements in a convolution approach to estimate past and future PFAS concentrations in groundwater discharge to the streams. At our test site near the Cape Fear River (CFR) of North Carolina, PFAS were detected in groundwater up to 43 years old, suggesting that some PFAS entered groundwater immediately or shortly after fluorochemical production began at the nearby Fayetteville Works. Results are consistent with little to no retardation in groundwater for perfluoroethers such as hexafluoropropylene oxide-dimer acid (HFPO-DA) and perfluoro-2-methoxypropanoic acid (PMPA), the two most abundant PFAS, with mean concentrations of 229 and 498 ng/L, respectively. Future PFAS concentrations in groundwater discharge to streams were estimated to remain above current MCL or health advisory levels through at least 2050 or 2060 (using 3 H/ 3 He and SF 6 , respectively). Recent atmospheric deposition data suggest lower but non-negligible amounts of PFAS may continue to enter groundwater, likely further extending PFAS persistence in groundwater and the adjacent CFR. This approach shows promise for giving an overall perspective on persistence of PFAS in groundwater discharge from a broad contaminated area.