Metal hydride differential scanning calorimetry as an approach to compositional determination of mixtures of hydrogen isotopologues and helium

Robinson, David B.; Luo, Weifang; Cai, Trevor Y.; Stewart, Kenneth D.

doi:10.1016/j.ijhydene.2015.08.033

Title: Metal hydride differential scanning calorimetry as an approach to compositional determination of mixtures of hydrogen isotopologues and helium

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Abstract

Gaseous mixtures of diatomic hydrogen isotopologues and helium are often encountered in the nuclear energy industry and in analytical chemistry. Compositions of stored mixtures can vary due to interactions with storage and handling materials. When tritium is present, it decays to form ions and helium-3, both of which can lead to further compositional variation. Monitoring of composition is typically achieved by mass spectrometry, a method that is bulky and energy-intensive. Mass spectrometers disperse sample material through vacuum pumps, which is especially troublesome if tritium is present. Moreover, our ultimate goal is to create a compact, fast, low-power sensor that can determine composition with minimal gas consumption and waste generation, as a complement to mass spectrometry that can be instantiated more widely. We propose calorimetry of metal hydrides as an approach to this, due to the strong isotope effect on gas absorption, and demonstrate the sensitivity of measured heat flow to atomic composition of the gas. Peak shifts are discernible when mole fractions change by at least 1%. A mass flow restriction results in a unique dependence of the measurement on helium concentration. We present a mathematical model as a first step toward prediction of the peak shapes and positions. Themore »« less

Authors:

Robinson, David B. ^[1];

^[1]; Cai, Trevor Y. ^[1]; Stewart, Kenneth D. ^[1]

Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Publication Date:: Sat Sep 26 00:00:00 EDT 2015

Research Org.:: Sandia National Lab. (SNL-CA), Livermore, CA (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1236210

Alternate Identifier(s):: OSTI ID: 1423496

Report Number(s):: SAND-2015-8659J; SAND-2014-17706J
Journal ID: ISSN 0360-3199; PII: S036031991502114X

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Accepted Manuscript

Journal Name:: International Journal of Hydrogen Energy

Additional Journal Information:: Journal Volume: 40; Journal Issue: 41; Journal ID: ISSN 0360-3199

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; H2; D2; He; Pd; DSC; desorption

Citation Formats


                    Robinson, David B., Luo, Weifang, Cai, Trevor Y., and Stewart, Kenneth D. Metal hydride differential scanning calorimetry as an approach to compositional determination of mixtures of hydrogen isotopologues and helium.  United States: N. p., 2015. 
Web.  doi:10.1016/j.ijhydene.2015.08.033.

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                    Robinson, David B., Luo, Weifang, Cai, Trevor Y., & Stewart, Kenneth D. Metal hydride differential scanning calorimetry as an approach to compositional determination of mixtures of hydrogen isotopologues and helium.  United States.  https://doi.org/10.1016/j.ijhydene.2015.08.033

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                    Robinson, David B., Luo, Weifang, Cai, Trevor Y., and Stewart, Kenneth D. Sat .  
"Metal hydride differential scanning calorimetry as an approach to compositional determination of mixtures of hydrogen isotopologues and helium".  United States.  https://doi.org/10.1016/j.ijhydene.2015.08.033.  https://www.osti.gov/servlets/purl/1236210.

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@article{osti_1236210,

  title        = {Metal hydride differential scanning calorimetry as an approach to compositional determination of mixtures of hydrogen isotopologues and helium},

  author       = {Robinson, David B. and Luo, Weifang and Cai, Trevor Y. and Stewart, Kenneth D.},

  abstractNote = {Gaseous mixtures of diatomic hydrogen isotopologues and helium are often encountered in the nuclear energy industry and in analytical chemistry. Compositions of stored mixtures can vary due to interactions with storage and handling materials. When tritium is present, it decays to form ions and helium-3, both of which can lead to further compositional variation. Monitoring of composition is typically achieved by mass spectrometry, a method that is bulky and energy-intensive. Mass spectrometers disperse sample material through vacuum pumps, which is especially troublesome if tritium is present. Moreover, our ultimate goal is to create a compact, fast, low-power sensor that can determine composition with minimal gas consumption and waste generation, as a complement to mass spectrometry that can be instantiated more widely. We propose calorimetry of metal hydrides as an approach to this, due to the strong isotope effect on gas absorption, and demonstrate the sensitivity of measured heat flow to atomic composition of the gas. Peak shifts are discernible when mole fractions change by at least 1%. A mass flow restriction results in a unique dependence of the measurement on helium concentration. We present a mathematical model as a first step toward prediction of the peak shapes and positions. The model includes a useful method to compute estimates of phase diagrams for palladium in the presence of arbitrary mixtures of hydrogen isotopologues. As a result, we expect that this approach can be used to deduce unknown atomic compositions from measured calorimetric data over a useful range of partial pressures of each component.},

  doi          = {10.1016/j.ijhydene.2015.08.033},

  journal      = {International Journal of Hydrogen Energy},

  number       = 41,

  volume       = 40,

  place        = {United States},

  year         = {Sat Sep 26 00:00:00 EDT 2015},

  month        = {Sat Sep 26 00:00:00 EDT 2015}

}

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