Journal
CHEMISTRY OF MATERIALS
Volume 30, Issue 4, Pages 1277-1284Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.7b04619
Keywords
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Funding
- U.S. Department of Energy, National Nuclear Security Administration [DE-NA0003763]
- NASA Ames Research Center [NNA06CB93G]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF NNCI-1542205]
- National Natural Science Foundation of China [21422704, 11605118]
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At the Hanford Site in southeastern Washington state, the U.S. Department of Energy intends to treat 56 million gallons of legacy nuclear waste by encasing it in borosilicate glass via vitrification. This process ineffectively captures radioactive pertechnetate (TcO4-) because of the ion's volatility, thereby requiring a different remediation method for this long-lived (t(1/2) = 2.1 x 10(5) years), environmentally mobile species. Currently available sorbents lack the desired combination of high uptake capacity, fast kinetics, and selectivity. Here, we evaluate the ability of the chemically and thermally robust Zr-6-based metal organic framework (MOF), NU-1000, to capture perrhenate (ReO4-), a pertechnetate simulant, and pertechnetate. Our material exhibits an excellent perrhenate uptake capacity of 210 mg/g, reaches saturation within 5 min, and maintains perrhenate uptake in the presence of competing anions. Additionally, experiments with pertechnetate confirm perrhenate is a suitable surrogate. Single-crystal X-ray diffraction indicates both chelating and nonchelating perrhenate binding motifs are present in both the small pore and the mesopore of NU-1000. Postadsorption diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) further elucidates the uptake mechanism and powder X-ray diffraction (PXRD) and Brunauer-Emmett-Teller (BET) surface area analysis confirm the retention of crystallinity and porosity of NU-1000 throughout adsorption.
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