title: Hydrate composite particles for ocean carbon sequestration: field verification.
abstract: This paper reports on the formation and dissolution of CO2/seawater/CO2 hydrate composite particles produced during field experiments in Monterey Bay, CA using a CO2 injector system previously developed in the laboratory. The injector consisted of a coflow reactor wherein water was introduced as a jet into liquid CO2, causing vigorous mixing of the two immiscible fluids to promote the formation of CO2 hydrate that is stable at ambient pressures and temperatures typical of ocean depths greater than approximately 500 m. Using flow rate ratios of water and CO2 of 1:1 and 5:1, particulate composites of CO2 hydrate/liquid CO2/seawater phases were produced in seawater at depths between 1100 and 1300 m. The resultant composite particles were tracked by a remotely operated vehicle system as they freely traveled in an imaging box that had no bottom or top walls. Results from the field experiments were consistent with laboratory experiments, which were conducted in a 70 L high-pressure vessel to simulate the conditions in the ocean at intermediate depths. The particle velocity and volume histories were monitored and used to calculate the conversion of CO2 into hydrate and its subsequent dissolution rate after release into the ocean. The dissolution rate of the composite particles was found to be higher than that reported for pure CO2 droplets. However, when the rate was corrected to correspond to pure CO2, the difference was very small. Results indicate that a higher conversion of liquid CO2 to CO2 hydrate is needed to form negatively buoyant particles in seawater when compared to freshwater, due primarily to the increased density of the liquid phase but also due to processes involving brine rejection during hydrate formation.
authors.affiliation: Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, Tennessee 37831-6181, USA. tsourisc@ornl.gov
authors.forename: Costas
authors.initials: C
authors.lastname: Tsouris
authors.forename: Peter
authors.initials: P
authors.lastname: Brewer
authors.forename: Edward
authors.initials: E
authors.lastname: Peltzer
authors.forename: Peter
authors.initials: P
authors.lastname: Walz
authors.forename: David
authors.initials: D
authors.lastname: Riestenberg
authors.forename: Liyuan
authors.initials: L
authors.lastname: Liang
authors.forename: Olivia R
authors.initials: OR
authors.lastname: West
mesh_terms: D001274:Atmospheric Pressure; D002245:Carbon Dioxide / Q000737:chemistry*; D004784:Environmental Monitoring; D008962:Models, Theoretical; D012623:Seawater / Q000737:chemistry*; D012995:Solubility
chemical_list: D002245:Carbon Dioxide