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Title: Synthesis of Zeolite Materials for Noble Gas Separation

Abstract

Microporous zeolite adsorbent materials are widely used as a medium for separating gases. Adsorbent gas separation systems can run at ambient temperature and require minimal pressure to flow the input gas stream across the adsorbent bed. This allows for low energy consumption relative to other types of separation systems. Specific zeolites also have a high capacity and selectivity for the gases of interest, leading to compact and efficient separation systems. These characteristics are particularly advantageous for the application of signatures detection for non-proliferation, which often requires portable systems with low power draw. Savannah River National Laboratory currently is the leader in using zeolites for noble gas sampling for non-proliferation detection platforms. However, there is a constant customer need for improved sampling capabilities. Development of improved zeolite materials will lead to improved sampling technology. Microwave-assisted and conventional hydrothermal synthesis have been used to make a variety of zeolites tailored for noble gas separation. Materials characterization data collected in this project has been used to help guide the synthesis of improved zeolite materials. Candidate materials have been down-selected based on highest available surface area, maximum overall capacity for gas adsorption and highest selectivity. The creation of improved adsorbent materials initiated in thismore » project will lead to development of more compact, efficient and effective noble gas collectors and concentrators. The work performed in this project will be used as a foundation for funding proposals for further material development as well as possible industrial applications.« less

Authors:
 [1];  [1];  [1];  [1]
  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
Publication Date:
Research Org.:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1395975
Report Number(s):
SRNL-STI-2017-00637
TRN: US1800002
DOE Contract Number:
AC09-08SR22470
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ZEOLITES; RARE GASES; HYDROTHERMAL SYNTHESIS

Citation Formats

Achey, R., Rivera, O., Wellons, M., and Hunter, D. Synthesis of Zeolite Materials for Noble Gas Separation. United States: N. p., 2017. Web. doi:10.2172/1395975.
Achey, R., Rivera, O., Wellons, M., & Hunter, D. Synthesis of Zeolite Materials for Noble Gas Separation. United States. doi:10.2172/1395975.
Achey, R., Rivera, O., Wellons, M., and Hunter, D. Mon . "Synthesis of Zeolite Materials for Noble Gas Separation". United States. doi:10.2172/1395975. https://www.osti.gov/servlets/purl/1395975.
@article{osti_1395975,
title = {Synthesis of Zeolite Materials for Noble Gas Separation},
author = {Achey, R. and Rivera, O. and Wellons, M. and Hunter, D.},
abstractNote = {Microporous zeolite adsorbent materials are widely used as a medium for separating gases. Adsorbent gas separation systems can run at ambient temperature and require minimal pressure to flow the input gas stream across the adsorbent bed. This allows for low energy consumption relative to other types of separation systems. Specific zeolites also have a high capacity and selectivity for the gases of interest, leading to compact and efficient separation systems. These characteristics are particularly advantageous for the application of signatures detection for non-proliferation, which often requires portable systems with low power draw. Savannah River National Laboratory currently is the leader in using zeolites for noble gas sampling for non-proliferation detection platforms. However, there is a constant customer need for improved sampling capabilities. Development of improved zeolite materials will lead to improved sampling technology. Microwave-assisted and conventional hydrothermal synthesis have been used to make a variety of zeolites tailored for noble gas separation. Materials characterization data collected in this project has been used to help guide the synthesis of improved zeolite materials. Candidate materials have been down-selected based on highest available surface area, maximum overall capacity for gas adsorption and highest selectivity. The creation of improved adsorbent materials initiated in this project will lead to development of more compact, efficient and effective noble gas collectors and concentrators. The work performed in this project will be used as a foundation for funding proposals for further material development as well as possible industrial applications.},
doi = {10.2172/1395975},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Oct 02 00:00:00 EDT 2017},
month = {Mon Oct 02 00:00:00 EDT 2017}
}

Technical Report:

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  • Currently used zeolites will be characterized using gas sorption analysis, SEM, XRD, and Raman spectroscopy.
  • Molecular simulations are used to assess the ability of metal-organic framework (MOF) materials to store and separate noble gases. Specifically, grand canonical Monte Carlo simulation techniques are used to predict noble gas adsorption isotherms at room temperature. Experimental trends of noble gas inflation curves of a Zn-based material (IRMOF-1) are matched by the simulation results. The simulations also predict that IRMOF-1 selectively adsorbs Xe atoms in Xe/Kr and Xe/Ar mixtures at total feed gas pressures of 1 bar (14.7 psia) and 10 bar (147 psia). Finally, simulations of a copper-based MOF (Cu-BTC) predict this material's ability to selectively adsorb Xemore » and Kr atoms when present in trace amounts in atmospheric air samples. These preliminary results suggest that Cu-BTC may be an ideal candidate for the pre-concentration of noble gases from air samples. Additional simulations and experiments are needed to determine the saturation limit of Cu-BTC for xenon, and whether any krypton atoms would remain in the Cu-BTC pores upon saturation.« less
  • Conventional Shultz-Flory catalysts suffer from the inherent non-selective product distributions of Shultz-Floryian kinetics. Development of the Mobil M technology is the first major breakthrough in synthetic fuel technology in 5 decades. To utilize the Mobil M technology, synthesis gas produced from the gasification of coal must first be converted to methanol. The high pressures and/or high recycle ratios necessary because of the thermodynamics of the methanol synthesis reaction, make the overall cost of this approach prohibitive in today's economy. The logical extension of the Mobil M technology is to use bifunctional Pentasil based catalysts to provide a single reactor routemore » from synthesis gas to high octane gasoline. Various methods exist to incorporate the CO reduction function with the Pentasil zeolite. The direct synthesis approach which has been largely overlooked by investigators to date, will be emphasized in this research. 193 references, 110 figures, 28 tables.« less
  • The objective is to synthesize a wide variety of 10-membered ring zeolites, particularly ZSM-5, incorporate transition metals during synthesis and by other techniques, determine sorption properties, and syngas conversions as a function of materials parameters. Of general significance was finding that ZSM-5 could be synthesized in a wide variety of systems and with a wide range of particle size that could be controlled by synthesis parameters. Of particular interest was confirming a UC patent that ZSM-5 could be crystallized in an organic-free system (Na/sub 2/O-Al/sub 2/O/sub 3/-SiO/sub 2/-H/sub 2/O). A SiO/sub 2//Al/sub 2/O/sub 3/ ratio of 60 was found optimummore » for rate of ZSM-5 crystallization, and high H/sub 2/O/Na/sub 2/O ratios of about 2000 produced larger crystals to 40..mu..m. A self-contained, integrated, computerized laboratory containing the essential analytical equipment (x-ray diffractometer, Cahn sorption balance, CDS catalytic activity unit) was designed and assembled.« less
  • An electron impact ion source has been designed for generation of noble gas ions in a compact isotope separator. The source utilizes a circular filament that surrounds an ionization chamber, enabling multiple passes of electrons through the ionization chamber. This report presents ion optical design and the results of efficiency and sensitivity measurements performed in an ion source test chamber and in the compact isotope separator. The cylindrical design produced xenon ions at an efficiency of 0.37% with a sensitivity of ~24 µA /Pa at 300 µA of electron current.