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Title: Kinetics of hydrogen isotope exchange in β-phase Pd-H-D

Abstract

Hydrogen isotope gas exchange within palladium powders is examined using a batch-type reactor coupled to a residual gas analyzer (RGA). Furthermore, the exchange rates in both directions (H2 + PdD and D2 + PdH) are measured in the temperature range 178–323 K for the samples with different particle sizes. The results show this batch-type exchange is closely approximated as a first-order kinetic process with a rate directly proportional to the surface area of the powder particles. An exchange rate constant of 1.40 ± 0.24 μmol H2/atm cm2 s is found for H2 + PdD at 298 K, 1.4 times higher than that for D2 + PdH, with an activation energy of 25.0 ± 3.2 kJ/mol H for both exchange directions. Finally, a comparison of exchange measurement techniques shows these coefficients, and the fundamental exchange probabilities are in good agreement with those obtained by NMR and flow techniques.

Authors:
 [1];  [1]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1235301
Report Number(s):
SAND-2015-4492J
Journal ID: ISSN 1932-7447; 590571
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal Issue: 32; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Luo, Weifang, and Cowgill, Donald F. Kinetics of hydrogen isotope exchange in β-phase Pd-H-D. United States: N. p., 2015. Web. doi:10.1021/acs.jpcc.5b06848.
Luo, Weifang, & Cowgill, Donald F. Kinetics of hydrogen isotope exchange in β-phase Pd-H-D. United States. https://doi.org/10.1021/acs.jpcc.5b06848
Luo, Weifang, and Cowgill, Donald F. 2015. "Kinetics of hydrogen isotope exchange in β-phase Pd-H-D". United States. https://doi.org/10.1021/acs.jpcc.5b06848. https://www.osti.gov/servlets/purl/1235301.
@article{osti_1235301,
title = {Kinetics of hydrogen isotope exchange in β-phase Pd-H-D},
author = {Luo, Weifang and Cowgill, Donald F.},
abstractNote = {Hydrogen isotope gas exchange within palladium powders is examined using a batch-type reactor coupled to a residual gas analyzer (RGA). Furthermore, the exchange rates in both directions (H2 + PdD and D2 + PdH) are measured in the temperature range 178–323 K for the samples with different particle sizes. The results show this batch-type exchange is closely approximated as a first-order kinetic process with a rate directly proportional to the surface area of the powder particles. An exchange rate constant of 1.40 ± 0.24 μmol H2/atm cm2 s is found for H2 + PdD at 298 K, 1.4 times higher than that for D2 + PdH, with an activation energy of 25.0 ± 3.2 kJ/mol H for both exchange directions. Finally, a comparison of exchange measurement techniques shows these coefficients, and the fundamental exchange probabilities are in good agreement with those obtained by NMR and flow techniques.},
doi = {10.1021/acs.jpcc.5b06848},
url = {https://www.osti.gov/biblio/1235301}, journal = {Journal of Physical Chemistry. C},
issn = {1932-7447},
number = 32,
volume = 119,
place = {United States},
year = {Wed Jul 22 00:00:00 EDT 2015},
month = {Wed Jul 22 00:00:00 EDT 2015}
}

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Cited by: 8 works
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Works referenced in this record:

Interaction of Hydrogen Isotopes with Transition Metals and Intermetallic Compounds
book, January 1996


NMR Measurement of Exchange of Deuterium between Palladium–Deuteride and Deuterium Gas
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Thermodynamic and Kinetic Characterization of Hydrogen−Deuterium Exchange in β-Phase Palladium
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Some Thermodynamic Properties of the H 1 H 2 , H 2 H 2 Molecules and Compounds Containing the H 2 Atom
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Role of molecular diffusion in the theory of gas flow through crimped-capillary leaks
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