Journal
AMERICAN MINERALOGIST
Volume 100, Issue 5-6, Pages 1203-1208Publisher
MINERALOGICAL SOC AMER
DOI: 10.2138/am-2015-4929
Keywords
Neutron diffraction; methane hydrate; carbon dioxide/methane exchange; Fourier density maps
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Funding
- National Science Foundation [DGE0801470]
- Spallation Neutron Source through the Scientific User Facilities Division, Office of Basic Energy Sciences
- Office of Fossil Energy through Field Work Proposal FEAB111 Hydrate Formation and Dissociation in Simulated and Field Samples.
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The exchange of carbon dioxide for methane in natural gas hydrates is an attractive approach to harvesting CH4 for energy production while simultaneously sequestering CO2. In addition to the energy and environmental implications, the solid solution of clathrate hydrate (CH4)(1-x)(CO2)(x)center dot 5.75H(2)O provides a model system to study how the distinct bonding and shapes of CH4 and CO2 influence the structure and properties of the compound. High-resolution neutron diffraction was used to examine mixed CO2/CH4 gas hydrates. CO2-rich hydrates had smaller lattice parameters, which were attributed to the higher affinity of the CO2 molecule interacting with H2O molecules that form the surrounding cages, and resulted in a reduction in the unit-cell volume. Experimental nuclear scattering densities illustrate how the cage occupants and energy landscape change with composition. These results provide important insights on the impact and mechanisms for the structure of mixed CH4/CO2 gas hydrate.
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