Observing methane hydrate dissolution rates under sediment cover

Dissolution rates of naturally occurring gas hydrates vary by orders of magnitude across studies suggesting that environmental factors may influence hydrate dissolution. To determine the role that sediment cover plays in hydrate dissolution, we used a mini-pore fluid array sampler (mPFA) to continuo...

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Veröffentlicht in:Marine chemistry 2015-05, Vol.172 (C), p.12-22
Hauptverfasser: Wilson, R.M., Lapham, L.L., Riedel, M., Holmes, M.E., Chanton, J.P.
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Sprache:eng
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Zusammenfassung:Dissolution rates of naturally occurring gas hydrates vary by orders of magnitude across studies suggesting that environmental factors may influence hydrate dissolution. To determine the role that sediment cover plays in hydrate dissolution, we used a mini-pore fluid array sampler (mPFA) to continuously collect sediment porewater adjacent to a hydrate outcrop and maintain it at in situ pressure for later analysis. This allowed us to measure in situ dissolved hydrocarbon concentrations in the porewater over time without sample loss due to degassing. We deployed the mPFA at a hydrate outcrop at Barkley Canyon on the Cascadia Margin for nine months. This novel approach yielded concentration data that were used to determine the steady-state dissolution rate of the hydrate outcrop and test predictions of the diffusion-control model for dissolution in the field. In the lab, we conducted a series of experiments with artificial hydrate to directly compare dissolution rates between exposed and sediment-covered hydrate. The dissolution rate of the natural hydrate outcrop covered with sediment was 0.06cmy−1. The laboratory experiments of sediment-covered hydrate yielded dissolution rates of 0.6±0.5cmy−1 (n=5). In both laboratory and field observations, the dissolution rate of hydrates exposed directly to bulk water (3.9±1.7cmy−1 and 3.5cmy−1 respectively) was at least an order of magnitude faster than the dissolution rate of sediment covered hydrate. These results are consistent with expectations of diffusion-control and support this model of hydrate dissolution. In nature, sediment may account for the persistence of hydrate in otherwise methane-depleted environments by increasing the diffusive boundary layer and slowing the rate of molecular diffusion via porosity/tortuosity effects. We provide a number of “Lessons Learned” for improving the instrument design and for consideration during future studies. •Sediment influence on hydrate dissolution was studied in the field and lab•In the field, CH4(aq) concentrations were at or below theoretical saturation•Dissolution of natural hydrate blanketed by 15cm thick sediment was measured•This covered hydrate dissolved at a slower rate than nearby exposed hydrates•In the lab, exposed hydrate dissolved faster than covered hydrate
ISSN:0304-4203
1872-7581
DOI:10.1016/j.marchem.2015.03.004