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:
-
- 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}
}
Web of Science
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Works referencing / citing this record:
Calcium Hydride Cation [CaH] + Stabilized by an NNNN-type Macrocyclic Ligand: A Selective Catalyst for Olefin Hydrogenation
journal, August 2017
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Molecular Calcium Hydride: Dicalcium Trihydride Cation Stabilized by a Neutral NNNN-Type Macrocyclic Ligand
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