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Title: Synthesis of zeolite materials for noble gas separation

Abstract

Currently used zeolites will be characterized using gas sorption analysis, SEM, XRD, and Raman spectroscopy.

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:
1395258
Report Number(s):
SRNL-STI-2017-00614
TRN: US1800058
DOE Contract Number:
AC09-08SR22470
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; ZEOLITES; RARE GASES; X-RAY DIFFRACTION; SCANNING ELECTRON MICROSCOPY; RAMAN SPECTROSCOPY

Citation Formats

Achey, R., Rivera, O., Hunter, D., and Wellons, M. Synthesis of zeolite materials for noble gas separation. United States: N. p., 2017. Web. doi:10.2172/1395258.
Achey, R., Rivera, O., Hunter, D., & Wellons, M. Synthesis of zeolite materials for noble gas separation. United States. doi:10.2172/1395258.
Achey, R., Rivera, O., Hunter, D., and Wellons, M. 2017. "Synthesis of zeolite materials for noble gas separation". United States. doi:10.2172/1395258. https://www.osti.gov/servlets/purl/1395258.
@article{osti_1395258,
title = {Synthesis of zeolite materials for noble gas separation},
author = {Achey, R. and Rivera, O. and Hunter, D. and Wellons, M.},
abstractNote = {Currently used zeolites will be characterized using gas sorption analysis, SEM, XRD, and Raman spectroscopy.},
doi = {10.2172/1395258},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2017,
month = 9
}

Technical Report:

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  • 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 leadermore » 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.« less
  • 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
  • 'The objective of this program is to rationally design and synthesize imprinted sol-gel SiO{sub 2} and SiO{sub 2}/M{prime}O{sub 2} (M{prime} = Ti, Zr) materials containing Si-X-L binding groups through template approaches and develop a scientific basis for metal ion binding and recognition by such imprinted organofunctional materials. These hydrophilic metal oxide-based materials are expected to remove metal ions from aqueous solutions intrinsically fast (in comparison to hydrophobic organic polymers), and the imprinted binding sites are expected to exhibit enhanced selectivity and affinity of target metal ions. This report summarizes research after the first eight months of a three-year project. Themore » authors have successfully prepared sol-gel materials grafted with organic ligands specific for binding target RCRA metal ions. When these organofunctional sol-gel materials are exposed to solutions containing target metal ions, they quickly remove the metal ions from aqueous solutions. In many such sol-gel materials, the metal ions absorbed in the sol-gel materials can be easily removed to regenerate the organofunctional sol-gel materials for subsequent cycles of metal ion removal. Work has commenced in two main areas: (1) preliminary evaluation of target ion binding and imprinting effects, (2) studies of mesoporous materials for the separation of large metal ions such as UO{sub 2}{sup 2+} and TcO{sub 4}.'« less
  • Current cost estimates for the environmental remediation of contaminated installations under the auspices of the Department of Energy (DOE) are staggering. On this basis alone, there is a critical need to develop the scientific basis for new approaches to the treatment and disposal of toxic metal ions from wastes or contaminated areas at many DOE sites. The overall goal of this project is to rationally design and synthesize imprinted, hybrid inorganic-organic sol-gel materials containing metal binding sites through template approaches, and to develop a scientific basis for metal ion binding and recognition by such tailored hybrid inorganic-organic materials. After removalmore » of the template M, functionalized cavities are created which contain both grafted binding sites and functionality inherent to the silica network (Si-OH, Si-O-Si). These cavities are expected to ''recognize'' and bind the target metal ions through the high affinities between the binding sites and M, and their retained shapes. Our approaches utilize both the metal ion binding and the tailored impressions of the template metal ions in the imprinted cavities. Such imprinted organofunctional sol-gel networks are expected to exhibit both high selectivity and capacity for binding targeted ions in fluid waste streams. The principles of sol-gel chemistry and imprinting techniques will guide our approaches to optimize the chemical and physical properties of the imprinted organofunctional sol-gel materials. Cold isotopes or non-radioactive surrogate ions of similar size and charge will be used in imprinting investigations to minimize hazardous waste production. The design strategy we will follow is based on imprinted binding sites cross-linked by rigid, hydrophilic inorganic SiO{sub 2} or MiO{sub 2} networks. These hydrophilic metal oxide-based materials are expected to exhibit fast ion mass transfer and binding kinetics in comparison to functionalized hydrophobic organic polymers. Success in this research will lead to a novel class of materials tailored for toxic metal recognition/separation with enhanced capacity and selectivity. It will also provide the scientific basis for such recognition and the development of a new generation of technologies for more efficient toxic metal removal. Furthermore, these research results should be directly applicable to DOE Environmental Management (EM) missions.« less
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