Observation of the growth process of icy materials in interparticle spaces: phase-contrast X-ray imaging of clathrate hydrate

The visualization of temperature-controlled crystal growth and dissociation of tetrahydrofuran clathrate hydrates and ice in the interparticle spaces between beads is presented. Phase-contrast X-ray imaging using synchrotron X-ray radiation is a unique technique to study clathrate hydrates coexisting with both ice and liquid water and is used here to observe tetrahydrofuran hydrate and ice formation in situ. The nondestructive images obtained reveal a morphology change of tetrahydrofuran clathrate hydrate grown under isothermal temperature conditions at 253 K, which may be caused by the thermal history of crystallization of the clathrate hydrate. In addition, the water freezing process in the interparticle spaces between is observed using phase-contrast X-ray imaging. This method is useful for understanding the kinetics of clathrate hydrates in interparticle spaces. (author)