Simultaneous Absorption and Desorption Isotherms of Various Hydrogen and Deuterium Mixtures between 20 and 120 °C Are Used to Determine the Activity Coefficients for Palladium-Hydride Solutions

Sharpe, Matthew

doi:10.1021/acs.jpcc.4c06976

Simultaneous Absorption and Desorption Isotherms of Various Hydrogen and Deuterium Mixtures between 20 and 120 °C Are Used to Determine the Activity Coefficients for Palladium-Hydride Solutions

Journal Article · Tue Feb 04 00:00:00 EST 2025 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.4c06976· OSTI ID:2511155

^[1]

University of Rochester, NY (United States)

A test bed was constructed to measure the absorption and desorption isotherms for palladium hydride using H₂, D₂, and various H₂/D₂ mixtures for temperatures in the range 20 °C ≤ T ≤ 120 °C. The pressure–composition–temperature isotherms were measured. The pressures obtained with mixtures between each pure isotope were monotonic, yet nonlinear. This nonlinear dependence of total pressure with feed gas protium concentration reveals the mixed isotope hydride system behaves nonideally. A thermodynamic model was adapted from the literature, which accounts for the nonideal nature of the mixed-isotope system. The measured data were used as constraints in this model in order to calculate the protium mole fractions in the hydride phase and the protium activity coefficients for palladium hydride at various temperatures and protium concentrations in the system. Knowing the protium mole fraction and activity coefficients allows for a priori calculation of the isotopologue distribution in the gas phase and the isotope distribution in the hydride phase, given a palladium temperature and equilibrium pressure.

View Journal Article

Research Organization:: University of Rochester, NY (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0004144

OSTI ID:: 2511155

Alternate ID(s):: OSTI ID: 2530201
OSTI ID: 2519015

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 6 Vol. 129; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (20)

Zustandsdiagramm und thermodynamisches Verhalten der Systeme Pd/H ₂ und Pd/D ₂ bei normalen Temperaturen; H/D-Trenneffekte Wicke, E.; Nernst, G. H. Berichte der Bunsengesellschaft für physikalische Chemie, Vol. 68, Issue 3 https://doi.org/10.1002/bbpc.19640680303	journal	April 1964
Magnetic Susceptibility and Equilibrium Diagram of PdH _n Frieske, H.; Wicke, E. Berichte der Bunsengesellschaft für physikalische Chemie, Vol. 77, Issue 1 https://doi.org/10.1002/bbpc.19730770112	journal	January 1973
The H-Pd (hydrogen-palladium) System Manchester, F. D.; San-Martin, A.; Pitre, J. M. Journal of Phase Equilibria, Vol. 15, Issue 1 https://doi.org/10.1007/BF02667685	journal	February 1994
Path and mechanism of hydrogen absorption at Pd(100) Okuyama, H.; Siga, W.; Takagi, N. Surface Science, Vol. 401, Issue 3 https://doi.org/10.1016/S0039-6028(98)00020-X	journal	April 1998
Hydrogen isotope separation with palladium particle bed Fukada, Satoshi; Nishikawa, Masabumi Fusion Engineering and Design, Vol. 39-40 https://doi.org/10.1016/S0920-3796(98)00093-3	journal	September 1998
Hydrogen isotope separation by gas chromatography using Pd–Pt alloy Watanabe, Kuniaki; Matsuyama, Masao; Kobayashi, Tohru Fusion Engineering and Design, Vol. 39-40 https://doi.org/10.1016/S0920-3796(98)00160-4	journal	September 1998
Review of absorption and adsorption in the hydrogen–palladium system Jewell, L.; Davis, B. Applied Catalysis A: General, Vol. 310 https://doi.org/10.1016/j.apcata.2006.05.012	journal	August 2006
Solubility of hydrogen and its isotopes in metals from mixed gases San Marchi, C.; Somerday, B. P.; Larson, R. S. Journal of Nuclear Materials, Vol. 372, Issue 2-3 https://doi.org/10.1016/j.jnucmat.2007.02.016	journal	January 2008
Isotope effects in the kinetics of simultaneous H and D thermal desorption from Pd Leardini, F.; Fernández, J. F.; Bodega, J. Journal of Physics and Chemistry of Solids, Vol. 69, Issue 1 https://doi.org/10.1016/j.jpcs.2007.08.005	journal	January 2008
THE PALLADIUM-HYDROGEN EQUILIBRIUM AND PALLADIUM HYDRIDE ¹ Gillespie, Louis J.; Hall, Flemmon Porter Journal of the American Chemical Society, Vol. 48, Issue 5 https://doi.org/10.1021/ja01416a015	journal	May 1926
The Palladium-Deuterium Equilibrium Gillespie, Louis J.; Downs, William Richard. Journal of the American Chemical Society, Vol. 61, Issue 9 https://doi.org/10.1021/ja01878a071	journal	September 1939
Empirical Correlation of Equilibrium Separation Factors in the Pd−H₂/D₂ System with Temperature and Composition Ortiz, T. M.; Meyer, B. A.; Razani, A. Journal of Chemical & Engineering Data, Vol. 45, Issue 1 https://doi.org/10.1021/je990199z	journal	December 1999
Separation Factors for Hydrogen Isotopes in Palladium Hydride Luo, Weifang; Cowgill, Donald F.; Flanagan, Ted B. The Journal of Physical Chemistry C, Vol. 117, Issue 27 https://doi.org/10.1021/jp4032332	journal	June 2013
Evidence for ‘‘subsurface’’ hydrogen on Pd(110): An intermediate between chemisorbed and dissolved species Behm, R. J.; Penka, V.; Cattania, M. ‐G. The Journal of Chemical Physics, Vol. 78, Issue 12 https://doi.org/10.1063/1.444739	journal	June 1983
Measurement of Palladium Hydride and Palladium Deuteride Isotherms Between 130 K and 393 K Sharpe, M.; Shmayda, W. T.; Glance, K. Fusion Science and Technology, Vol. 76, Issue 5 https://doi.org/10.1080/15361055.2020.1740558	journal	July 2020
Palladium-tritium system Lässer, R. Physical Review B, Vol. 26, Issue 6 https://doi.org/10.1103/PhysRevB.26.3517	journal	September 1982
Solubility of hydrogen isotopes in palladium Lässer, R.; Klatt, K. -H. Physical Review B, Vol. 28, Issue 2 https://doi.org/10.1103/PhysRevB.28.748	journal	July 1983
The Palladium-Hydrogen System Flanagan, T. B.; Oates, W. A. Annual Review of Materials Science, Vol. 21, Issue 1 https://doi.org/10.1146/annurev.ms.21.080191.001413	journal	August 1991
TCAP Hydrogen Isotope Separation Using Palladium and Inverse Columns Heung, L. K.; Sessions, H. T.; Xiao, X. Fusion Science and Technology, Vol. 60, Issue 4 https://doi.org/10.13182/FST11-T39	journal	November 2011
Equilibrium H/D Separation Factors in Pd and in Nb Brodowsky, H.; Repenning, D. Zeitschrift für Physikalische Chemie, Vol. 114, Issue 114 https://doi.org/10.1524/zpch.1979.114.114.141	journal	January 1979

Similar Records

Measurement of Palladium Hydride and Palladium Deuteride Isotherms Between 130 K and 393 K

Journal Article · Mon Jul 06 20:00:00 EDT 2020 · Fusion Science and Technology · OSTI ID:1647469

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Absorption
Desorption
Hydrogen isotopes
Isotherms
Palladium

Simultaneous Absorption and Desorption Isotherms of Various Hydrogen and Deuterium Mixtures between 20 and 120 °C Are Used to Determine the Activity Coefficients for Palladium-Hydride Solutions

Citation Formats

References (20)

Similar Records

Related Subjects