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Title: A multi-phase, micro-dispersion reactor for the continuous production of methane gas hydrate

Abstract

A continuous-jet hydrate reactor originally developed to generate a CO2 hydrate stream has been modified to continuously produce CH4 hydrate. The reactor has been tested in the Seafloor Process Simulator (SPS), a 72-L pressure vessel available at Oak Ridge National Laboratory. During experiments, the reactor was submerged in water inside the SPS and received water from the surrounding through a submersible pump and CH4 externally through a gas booster pump. Thermodynamic conditions in the hydrate stability regime were employed in the experiments. The reactor produced a continuous stream of CH4 hydrate, and based on pressure values and amount of gas injected, the conversion of gas to hydrate was estimated. A conversion of up to 70% was achieved using this reactor.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [1]
  1. ORNL
  2. Oak Ridge Associated Universities (ORAU)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
FE USDOE - Office of Fossil Energy (FE)
OSTI Identifier:
958940
DOE Contract Number:
DE-AC05-00OR22725
Resource Type:
Journal Article
Resource Relation:
Journal Name: Industrial & Engineering Chemistry Research; Journal Volume: 48; Journal Issue: 13
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; GAS HYDRATES; HYDRATES; METHANE; ORNL; PRESSURE VESSELS; PRODUCTION; SIMULATORS; STABILITY; THERMODYNAMICS; WATER; CARBON DIOXIDE; Gas hydrates; methane hydrate; hydrate reactor

Citation Formats

Taboada Serrano, Patricia L, Ulrich, Shannon M, Szymcek, Phillip, McCallum, Scott, Phelps, Tommy Joe, Palumbo, Anthony Vito, and Tsouris, Costas. A multi-phase, micro-dispersion reactor for the continuous production of methane gas hydrate. United States: N. p., 2009. Web. doi:10.1021/ie8019517.
Taboada Serrano, Patricia L, Ulrich, Shannon M, Szymcek, Phillip, McCallum, Scott, Phelps, Tommy Joe, Palumbo, Anthony Vito, & Tsouris, Costas. A multi-phase, micro-dispersion reactor for the continuous production of methane gas hydrate. United States. doi:10.1021/ie8019517.
Taboada Serrano, Patricia L, Ulrich, Shannon M, Szymcek, Phillip, McCallum, Scott, Phelps, Tommy Joe, Palumbo, Anthony Vito, and Tsouris, Costas. 2009. "A multi-phase, micro-dispersion reactor for the continuous production of methane gas hydrate". United States. doi:10.1021/ie8019517.
@article{osti_958940,
title = {A multi-phase, micro-dispersion reactor for the continuous production of methane gas hydrate},
author = {Taboada Serrano, Patricia L and Ulrich, Shannon M and Szymcek, Phillip and McCallum, Scott and Phelps, Tommy Joe and Palumbo, Anthony Vito and Tsouris, Costas},
abstractNote = {A continuous-jet hydrate reactor originally developed to generate a CO2 hydrate stream has been modified to continuously produce CH4 hydrate. The reactor has been tested in the Seafloor Process Simulator (SPS), a 72-L pressure vessel available at Oak Ridge National Laboratory. During experiments, the reactor was submerged in water inside the SPS and received water from the surrounding through a submersible pump and CH4 externally through a gas booster pump. Thermodynamic conditions in the hydrate stability regime were employed in the experiments. The reactor produced a continuous stream of CH4 hydrate, and based on pressure values and amount of gas injected, the conversion of gas to hydrate was estimated. A conversion of up to 70% was achieved using this reactor.},
doi = {10.1021/ie8019517},
journal = {Industrial & Engineering Chemistry Research},
number = 13,
volume = 48,
place = {United States},
year = 2009,
month = 1
}
  • Research is underway at NETL to understand the physical properties of methane hydrates. Five key areas of research that need further investigation have been identified. These five areas, i.e. thermal properties of hydrates in sediments, kinetics of natural hydrate dissociation, hysteresis effects, permeability of sediments to gas flow and capillary pressures within sediments, and hydrate distribution at porous scale, are important to the production models that will be used for producing methane from hydrate deposits. NETL is using both laboratory experiments and computational modeling to address these five key areas. The laboratory and computational research reinforce each other by providingmore » feedback. The laboratory results are used in the computational models and the results from the computational modeling is used to help direct future laboratory research. The data generated at NETL will be used to help fulfill The National Methane Hydrate R&D Program of a “long-term supply of natural gas by developing the knowledge and technology base to allow commercial production of methane from domestic hydrate deposits by the year 2015” as outlined on the NETL Website [NETL Website, 2005. http://www.netl.doe.gov/scngo/Natural%20Gas/hydrates/index.html]. Laboratory research is accomplished in one of the numerous high-pressure hydrate cells available ranging in size from 0.15 mL to 15 L in volume. A dedicated high-pressure view cell within the Raman spectrometer allows for monitoring the formation and dissociation of hydrates. Thermal conductivity of hydrates (synthetic and natural) at a certain temperature and pressure is performed in a NETL-designed cell. Computational modeling studies are investigating the kinetics of hydrate formation and dissociation, modeling methane hydrate reservoirs, molecular dynamics simulations of hydrate formation, dissociation, and thermal properties, and Monte Carlo simulations of hydrate formation and dissociation.« less
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  • Methane hydrate found in marine sediments is thought to contain gigaton quantities of methane and is considered an important potential fuel source and climate-forcing agent. Much of the methane in hydrates is biogenic, so models that predict the presence and distribution of hydrates require accurate rates of in situ methanogenesis. We estimated the in situ methanogenesis rates in Hydrate Ridge (HR) sediments by coupling experimentally derived minimal rates of methanogenesis to methanogen biomass determinations for discrete locations in the sediment column. When starved in a biomass recycle reactor Methanoculleus submarinus produced ca. 0.017 fmol methane/cell/day. Quantitative polymerase chain reaction (QPCR)more » directed at the methyl coenzyme M reductase subunit A (mcrA) gene indicated that 75% of the HR sediments analyzed contained <1000 methanogens/g. The highest methanogen numbers were mostly from sediments <10 meters below seafloor. By combining methanogenesis rates for starved methanogens (adjusted to account for in situ temperatures) and the numbers of methanogens at selected depths we derived an upper estimate of <4.25 fmol methane produced/g sediment/day for the samples with fewer methanogens than the QPCR method could detect. The actual rates could vary depending on the real number of methanogens and various seafloor parameters that influence microbial activity. However, our calculated rate is lower than rates previously reported from such sediments and close to the rate derived using geochemical modeling of the sediments. These data will help to improve models that predict microbial gas generation in marine sediments and determine the potential influence of this source of methane on the global carbon cycle.« less
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