Liquid–solid phase transition of hydrogen and deuterium in silica aerogel

Van Cleve, E.; Worsley, M. A.; Kucheyev, S. O.

doi:10.1063/1.4900540

Liquid–solid phase transition of hydrogen and deuterium in silica aerogel

Journal Article · Thu Oct 30 00:00:00 EDT 2014 · Journal of Applied Physics

DOI:https://doi.org/10.1063/1.4900540· OSTI ID:1409939

Van Cleve, E. ^[1]; Worsley, M. A. ^[1]; Kucheyev, S. O. ^[1]

Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Behavior of hydrogen isotopes confined in disordered low-density nanoporous solids remains essentially unknown. Here, we use relaxation calorimetry to study freezing and melting of H₂ and D₂ in an ~85%-porous base-catalyzed silica aerogel. In this work, we find that liquid–solid transition temperatures of both isotopes inside the aerogel are depressed. The phase transition takes place over a wide temperature range of ~4 K and non-trivially depends on the liquid filling fraction, reflecting the broad pore size distribution in the aerogel. Undercooling is observed for both H₂ and D₂ confined inside the aerogel monolith. Lastly, results for H₂ and D₂ are extrapolated to tritium-containing hydrogens with the quantum law of corresponding states.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1409939

Alternate ID(s):: OSTI ID: 22308149
OSTI ID: 1420473

Report Number(s):: LLNL-JRNL--656045

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 16 Vol. 116; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (32)

Aerogels—Airy Materials: Chemistry, Structure, and Properties Hüsing, Nicola; Schubert, Ulrich Angewandte Chemie International Edition, Vol. 37, Issue 1-2, p. 22-45 https://doi.org/10.1002/(SICI)1521-3773(19980202)37:1/2<22::AID-ANIE22>3.0.CO;2-I	journal	February 1998
The Quantum Mechanical Distribution Function of Molecular Systems: Translational and Rotational Motions Friedmann, H. Advances in Chemical Physics https://doi.org/10.1002/9780470143506.ch6	book	January 1962
Super-Compressibility of Ultralow-Density Nanoporous Silica Kucheyev, S. O.; Stadermann, M.; Shin, S. J. Advanced Materials, Vol. 24, Issue 6 https://doi.org/10.1002/adma.201103561	journal	January 2012
Freezing of molecular hydrogen and its isotopes in porous vycor glass Beaudoin, G.; Haljan, P.; Paetkau, M. Journal of Low Temperature Physics, Vol. 105, Issue 1-2 https://doi.org/10.1007/BF00754630	journal	October 1996
Quantum theory of condensed permanent gases I the law of corresponding states De Boer, J. Physica, Vol. 14, Issue 2-3 https://doi.org/10.1016/0031-8914(48)90032-9	journal	April 1948
Thermal anomalies in supercooled parahydrogen in Vycor porous glass Brewer, D. F.; Rajendra, J. C. N.; Thomson, A. L. Physica B: Condensed Matter, Vol. 194-196 https://doi.org/10.1016/0921-4526(94)90673-4	journal	February 1994
Study of H2 confined in the highly ordered pores of MCM-48 Glanville, Y. J.; Pearce, J. V.; Sokol, P. E. Chemical Physics, Vol. 292, Issue 2-3 https://doi.org/10.1016/S0301-0104(03)00099-5	journal	August 2003
Low temperature hydrogen which has not solidified Brewer, D. F.; Rajendra, J.; Sharma, N. Physica B: Condensed Matter, Vol. 165-166 https://doi.org/10.1016/S0921-4526(90)81134-A	journal	August 1990
Thermoporometry by differential scanning calorimetry: experimental considerations and applications Landry, Michael R. Thermochimica Acta, Vol. 433, Issue 1-2 https://doi.org/10.1016/j.tca.2005.02.015	journal	August 2005
The Determination of Pore Volume and Area Distributions in Porous Substances. I. Computations from Nitrogen Isotherms Barrett, Elliott P.; Joyner, Leslie G.; Halenda, Paul P. Journal of the American Chemical Society, Vol. 73, Issue 1 https://doi.org/10.1021/ja01145a126	journal	January 1951
The Densities of Liquid Tritium, 20.6 to 29°K. ¹ Grilly, E. R. Journal of the American Chemical Society, Vol. 73, Issue 11 https://doi.org/10.1021/ja01155a089	journal	November 1951
Adsorption of Gases in Multimolecular Layers Brunauer, Stephen; Emmett, P. H.; Teller, Edward Journal of the American Chemical Society, Vol. 60, Issue 2, p. 309-319 https://doi.org/10.1021/ja01269a023	journal	February 1938
A Quasi-Elastic and Inelastic Neutron Scattering Study of H₂ in Zeolite Fu, H.; Trouw, F.; Sokol, P. E. Journal of Low Temperature Physics https://doi.org/10.1023/A:1021881516198		August 1999
Heat Capacity Measurements on Small Samples at Low Temperatures Bachmann, R.; DiSalvo, F. J.; Geballe, T. H. Review of Scientific Instruments, Vol. 43, Issue 2 https://doi.org/10.1063/1.1685596	journal	February 1972
Formation of Crystal Nuclei in Liquid Metals Turnbull, D. Journal of Applied Physics, Vol. 21, Issue 10 https://doi.org/10.1063/1.1699435	journal	October 1950
Condensed hydrogen for thermonuclear fusion Kucheyev, S. O.; Hamza, A. V. Journal of Applied Physics, Vol. 108, Issue 9 https://doi.org/10.1063/1.3489943	journal	November 2010
Relaxation calorimeter for hydrogen thermoporometry Van Cleve, E.; Worsley, M. A.; Kucheyev, S. O. Review of Scientific Instruments, Vol. 84, Issue 5 https://doi.org/10.1063/1.4803180	journal	May 2013
Light-ion-irradiation-induced thermal spikes in nanoporous silica Kucheyev, S. O.; Wang, Y. M.; Hamza, A. V. Journal of Physics D: Applied Physics, Vol. 44, Issue 8 https://doi.org/10.1088/0022-3727/44/8/085406	journal	February 2011
Confinement effects on freezing and melting Christenson, Hugo K. Journal of Physics: Condensed Matter, Vol. 13, Issue 11 https://doi.org/10.1088/0953-8984/13/11/201	journal	March 2001
Freezing and melting of hydrogen confined in nanoporous silica Kucheyev, S. O.; Van Cleve, E.; Worsley, M. A. Journal of Physics: Condensed Matter, Vol. 26, Issue 22 https://doi.org/10.1088/0953-8984/26/22/225004	journal	May 2014
Specific heats of hydrogen, deuterium, and neon in porous Vycor glass Tell, J. L.; Maris, H. J. Physical Review B, Vol. 28, Issue 9 https://doi.org/10.1103/PhysRevB.28.5122	journal	November 1983
Thermal conductivity of condensed D-T and T 2 Collins, G. W.; Souers, P. C.; Fearon, E. M. Physical Review B, Vol. 41, Issue 4 https://doi.org/10.1103/PhysRevB.41.1816	journal	February 1990
Heat capacity and torsional oscillator studies of molecular hydrogen in porous Vycor glass Torii, R. H.; Maris, H. J.; Seidel, G. M. Physical Review B, Vol. 41, Issue 10 https://doi.org/10.1103/PhysRevB.41.7167	journal	April 1990
Supercooling of molecular hydrogen in zeolite Rall, M.; Brison, J. P.; Sullivan, N. S. Physical Review B, Vol. 44, Issue 17 https://doi.org/10.1103/PhysRevB.44.9639	journal	November 1991
Freezing and melting of fluids in porous glasses Molz, Eric; Wong, Apollo P. Y.; Chan, M. H. W. Physical Review B, Vol. 48, Issue 9 https://doi.org/10.1103/PhysRevB.48.5741	journal	September 1993
Structure of D 2 in zeolite Fang, M. P.; Sokol, P. E.; Wang, Y. Physical Review B, Vol. 50, Issue 17 https://doi.org/10.1103/PhysRevB.50.12291	journal	November 1994
Molecular hydrogen in porous Vycor glass De Kinder, Jan; Bouwen, August; Schoemaker, Dirk Physical Review B, Vol. 52, Issue 22 https://doi.org/10.1103/PhysRevB.52.15872	journal	December 1995
Hydrogen in porous Vycor glass Schindler, M.; Dertinger, A.; Kondo, Y. Physical Review B, Vol. 53, Issue 17 https://doi.org/10.1103/PhysRevB.53.11451	journal	May 1996
Curvature-dependent metastability of the solid phase and the freezing-melting hysteresis in pores Petrov, Oleg; Furó, István Physical Review E, Vol. 73, Issue 1 https://doi.org/10.1103/PhysRevE.73.011608	journal	January 2006
Growth of Highly Oriented Deuterium Crystals in Silicon Nanochannels Hofmann, T.; Kumar, P.; Enderle, M. Physical Review Letters, Vol. 110, Issue 6 https://doi.org/10.1103/PhysRevLett.110.065505	journal	February 2013
Supercooling of Liquid Hydrogen Seidel, G. M.; Maris, H. J.; Williams, F. I. B. Physical Review Letters, Vol. 56, Issue 22 https://doi.org/10.1103/PhysRevLett.56.2380	journal	June 1986
Beta-Layering in Foam-Lined Surrogate IFE Targets Hoffer, J. K.; Sheliak, J. D.; Geller, D. A. Fusion Science and Technology, Vol. 50, Issue 1 https://doi.org/10.13182/FST06-A1217	journal	July 2006

Cited By (1)

Effect of wetting on nucleation and growth of D ₂ in confinement Zepeda-Ruiz, L. A.; Sadigh, B.; Shin, S. J. The Journal of Chemical Physics, Vol. 148, Issue 13 https://doi.org/10.1063/1.5020068	journal	April 2018

Similar Records

Liquid–solid phase transition of hydrogen and deuterium in silica aerogel

Journal Article · Tue Oct 28 00:00:00 EDT 2014 · Journal of Applied Physics · OSTI ID:22308149

Hydrogen Crystallization in Low-Density Aerogels

Journal Article · Mon Mar 16 20:00:00 EDT 2015 · Langmuir · OSTI ID:1409956

Related Subjects

36 MATERIALS SCIENCE
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY

Liquid–solid phase transition of hydrogen and deuterium in silica aerogel

Citation Formats

References (32)

Cited By (1)

Similar Records

Related Subjects