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Title: Molecular environmental science using synchrotron radiation:Chemistry and physics of waste form materials

Abstract

Production of defense-related nuclear materials has generated large volumes of complex chemical wastes containing a mixture of radionuclides. The disposition of these wastes requires conversion of the liquid and solid-phase components into durable, solid forms suitable for long-term immobilization [1]. Specially formulated glass compositions, many of which have been derived from glass developed for commercial purposes, and ceramics such as pyrochlores and apatites, will be the main recipients for these wastes. The performance characteristics of waste-form glasses and ceramics are largely determined by the loading capacity for the waste constituents (radioactive and non-radioactive) and the resultant chemical and radiation resistance of the waste-form package to leaching (durability). There are unique opportunities for the use of near-edge soft-x-ray absorption fine structure (NEXAFS) spectroscopy to investigate speciation of low-Z elements forming the backbone of waste-form glasses and ceramics. Although nuclear magnetic resonance (NMR) is the primary technique employed to obtain speciation information from low-Z elements in waste forms, NMR is incompatible with the metallic impurities contained in real waste and is thus limited to studies of idealized model systems. In contrast, NEXAFS can yield element-specific speciation information from glass constituents without sensitivity to paramagnetic species. Development and use of NEXAFS for eventualmore » studies of real waste glasses has significant implications, especially for the low-Z elements comprising glass matrices [5-7]. The NEXAFS measurements were performed at Beamline 6.3.1, an entrance-slitless bend-magnet beamline operating from 200 eV to 2000 eV with a Hettrick-Underwood varied-line-space (VLS) grating monochromator, of the Advanced Light Source (ALS) at LBNL. Complete characterization and optimization of this beamline was conducted to enable high-performance measurements.« less

Authors:
;
Publication Date:
Research Org.:
Ernest Orlando Lawrence Berkeley NationalLaboratory, Berkeley, CA (US)
Sponsoring Org.:
USDOE Director. Office of Science. Office of Basic EnergySciences. Chemical Sciences Geosciences and Biosciences Division,Environmental Management Science Program, Pacific Northwest NationalLaboratory
OSTI Identifier:
881830
Report Number(s):
LBNL-53219
R&D Project: 000000; TRN: US0603011
DOE Contract Number:  
DE-AC02-05CH11231
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION; 36 MATERIALS SCIENCE; 43 PARTICLE ACCELERATORS; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; ADVANCED LIGHT SOURCE; CHEMICAL WASTES; FINE STRUCTURE; NUCLEAR MAGNETIC RESONANCE; PHYSICS; RADIATION CHEMISTRY; RADIATIONS; SPECTROSCOPY; SYNCHROTRONS; WASTE FORMS; WASTES

Citation Formats

Lindle, Dennis W., and Shuh, David K. Molecular environmental science using synchrotron radiation:Chemistry and physics of waste form materials. United States: N. p., 2005. Web. doi:10.2172/881830.
Lindle, Dennis W., & Shuh, David K. Molecular environmental science using synchrotron radiation:Chemistry and physics of waste form materials. United States. doi:10.2172/881830.
Lindle, Dennis W., and Shuh, David K. Mon . "Molecular environmental science using synchrotron radiation:Chemistry and physics of waste form materials". United States. doi:10.2172/881830. https://www.osti.gov/servlets/purl/881830.
@article{osti_881830,
title = {Molecular environmental science using synchrotron radiation:Chemistry and physics of waste form materials},
author = {Lindle, Dennis W. and Shuh, David K.},
abstractNote = {Production of defense-related nuclear materials has generated large volumes of complex chemical wastes containing a mixture of radionuclides. The disposition of these wastes requires conversion of the liquid and solid-phase components into durable, solid forms suitable for long-term immobilization [1]. Specially formulated glass compositions, many of which have been derived from glass developed for commercial purposes, and ceramics such as pyrochlores and apatites, will be the main recipients for these wastes. The performance characteristics of waste-form glasses and ceramics are largely determined by the loading capacity for the waste constituents (radioactive and non-radioactive) and the resultant chemical and radiation resistance of the waste-form package to leaching (durability). There are unique opportunities for the use of near-edge soft-x-ray absorption fine structure (NEXAFS) spectroscopy to investigate speciation of low-Z elements forming the backbone of waste-form glasses and ceramics. Although nuclear magnetic resonance (NMR) is the primary technique employed to obtain speciation information from low-Z elements in waste forms, NMR is incompatible with the metallic impurities contained in real waste and is thus limited to studies of idealized model systems. In contrast, NEXAFS can yield element-specific speciation information from glass constituents without sensitivity to paramagnetic species. Development and use of NEXAFS for eventual studies of real waste glasses has significant implications, especially for the low-Z elements comprising glass matrices [5-7]. The NEXAFS measurements were performed at Beamline 6.3.1, an entrance-slitless bend-magnet beamline operating from 200 eV to 2000 eV with a Hettrick-Underwood varied-line-space (VLS) grating monochromator, of the Advanced Light Source (ALS) at LBNL. Complete characterization and optimization of this beamline was conducted to enable high-performance measurements.},
doi = {10.2172/881830},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Mon Feb 28 00:00:00 EST 2005},
month = {Mon Feb 28 00:00:00 EST 2005}
}

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