The influence of the presence of sulphate on methanogenesis in the backfill of a Canadian nuclear fuel waste disposal vault: a laboratory study

Microbial gas production in the clay-based buffer and backfill materials of a nuclear waste disposal vault could produce gas bubbles or a separate gas phase, depending on quantities produced and the kinetics of the process. Gas production may affect the performance of the clay-based barriers. Results from previous laboratory experiments suggested that the presence of backfill or backfill clay prevented methane production in groundwater systems, likely because of inherently high sulphate concentrations in the clay. The work presented here shows that methane production in groundwater/clay systems is possible, but only at sulphate concentrations <35 mg/L. Sulphate concentrations in laboratory systems were lowered by the addition of Ba, and also by natural (microbiological or chemical) processes occurring over time (almost 700 d). Nutrient additions (acetate, diesel fuel) appeared to increase the magnitude of methane production but not necessarily speed the onset of methanogenesis. A high pH did not reduce or enhance methanogenesis, and the role of Fe in creating suitable conditions was not clear. Methane production rates in laboratory systems containing groundwater and backfill or backfill clay ranged from 0.1 to 0.125 mole%/d. In the presence of Ba-acetate, a rate as high as 0.7 mole%/d was observed. It is recommended that all microbial gas production experiments be continued for an adequate period of time, because of the considerable time required to develop suitable conditions for methanogenesis in laboratory systems. Methane production rates in water-limited clay environments, such as those expected in a nuclear fuel waste disposal vault, are needed as well as modelling of methane production for incorporation into vault performance optimization and safety assessments. (author)