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. 2017 Sep 7;8(1):485.
doi: 10.1038/s41467-017-00526-3.

Capture of organic iodides from nuclear waste by metal-organic framework-based molecular traps

Baiyan Li  1 , Xinglong Dong  2 , Hao Wang  1 , Dingxuan Ma  3 , Kui Tan  4 , Stephanie Jensen  5 , Benjamin J Deibert  1 , Joseph Butler  4 , Jeremy Cure  4 , Zhan Shi  3 , Timo Thonhauser  5   6 , Yves J Chabal  4 , Yu Han  2 , Jing Li  7
Affiliations

Capture of organic iodides from nuclear waste by metal-organic framework-based molecular traps

Baiyan Li et al. Nat Commun. .

Abstract

Effective capture of radioactive organic iodides from nuclear waste remains a significant challenge due to the drawbacks of current adsorbents such as low uptake capacity, high cost, and non-recyclability. We report here a general approach to overcome this challenge by creating radioactive organic iodide molecular traps through functionalization of metal-organic framework materials with tertiary amine-binding sites. The molecular trap exhibits a high CH3I saturation uptake capacity of 71 wt% at 150 °C, which is more than 340% higher than the industrial adsorbent Ag0@MOR under identical conditions. These functionalized metal-organic frameworks also serve as good adsorbents at low temperatures. Furthermore, the resulting adsorbent can be recycled multiple times without loss of capacity, making recyclability a reality. In combination with its chemical and thermal stability, high capture efficiency and low cost, the adsorbent demonstrates promise for industrial radioactive organic iodides capture from nuclear waste. The capture mechanism was investigated by experimental and theoretical methods.Capturing radioactive organic iodides from nuclear waste is important for safe nuclear energy usage, but remains a significant challenge. Here, Li and co-workers fabricate a stable metal-organic framework functionalized with tertiary amine groups that exhibits high capacities for radioactive organic iodides uptake.

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Conflict of interest statement

The authors declare no competing financial interests.

Figures

Fig. 1
Fig. 1
The design strategy. A schematic illustrating the design of a recyclable MOF molecular trap for effective capture of radioactive organic iodides from nuclear waste
Fig. 2
Fig. 2
Characterization of MIL-101-Cr and tertiary amine functionalized MIL-101-Cr. a PXRD patterns of MIL-101-Cr, MIL-101-Cr-TED, and MIL-101-Cr-HMTA. b FT-IR spectra of MIL-101-Cr, MIL-101-Cr-TED, and MIL-101-Cr-HMTA collected on samples after dehydration at 150 °C, the inset shows the mode associated with the C-N stretching vibration, at 1054 cm−1 in MIL-101-Cr-TED and 995 cm−1 in MIL-101-Cr-HMTA, based on refs , . Note that the weak band at 1059 cm−1 in MIL-101-Cr-HMTA spectrum is due to the CNC deformation vibration. The assignment of MOF phonon modes are based on ref. . c Solid 1H NMR spectra of MIL-101-Cr, TED, HMTA, MIL-101-Cr-TED, and MIL-101-Cr-HMTA. d N2 sorption isotherms of MIL-101-Cr, MIL-101-Cr-TED, and MIL-101-Cr-HMTA collected at 77 K
Fig. 3
Fig. 3
The CH3I capture performance. a Sorption isotherms of CH3I in MIL-101-Cr-TED, MIL-101-Cr-HMTA, and selected benchmark sorbent materials at 150 °C with partial pressure of 0.2 atm for CH3I. b Comparing the saturated CH3I uptake in MIL-101-Cr-TED, MIL-101-Cr-HMTA, and selected benchmark sorbent materials at 150 °C with partial pressure of 0.2 atm for CH3I. c The CH3I uptake at 150 °C under dry and humidity (RH = 81%) conditions by breakthrough experiment (back row: dry conditions; front row: humid conditions), (insert) the uptake drop ratio by comparing the CH3I uptake of dry and humid conditions. d Decontamination factors of CH3I by MIL-101-Cr-TED under simulated conditions representing gas mixtures produced during CH3I reprocessing, which include CH3I (50 ppm), H2O, HNO3, NO2, and NO at 150 °C. e The recyclability of MIL-101-Cr-TED for CH3I capture. f Decontamination factors of total iodine (CH3I and I2) by MIL-101-Cr-TED, MIL-101-Cr-HTMA, and comparable samples Ag0@MOR and HISL under the simulated conditions of an off-gas mixture: I2 (150 ppm), CH3I (50 ppm), H2O, HNO3 and NOx at 150 °C
Fig. 4
Fig. 4
The mechanism of CH3I capture by MIL-101-Cr-TED and MIL-101-Cr-HMTA. a The elemental mapping of CH3I loaded MIL-101-Cr-TED. b The elemental mapping of CH3I loaded MIL-101-Cr-HMTA. c Solid 1H NMR spectra of MIL-101-Cr-TED and CH3I@MIL-101-Cr-TED. d Solid 1H NMR spectra of MIL-101-Cr-HMTA and CH3I@MIL-101-Cr-HMTA. e XPS spectra of N(1s) for MIL-101-Cr-TED and CH3I@MIL-101-Cr-TED (gray, experiment curves; red, blue, and green: fitted curves; orange: baselines). f XPS spectra of N(1s) for MIL-101-Cr-HMTA and CH3I@MIL-101-Cr-HMTA (gray, experiment curves; red, blue, and green: fitted curves; orange: baselines). g In situ IR spectra (green) of ~150 Torr CH3I exposed MIL-101-Cr-TED referenced to the activated MIL-101-Cr-TED; and IR absorption spectra (red) of activated MIL-101-Cr-TED referenced to KBr pellet in vacuum (<20 mtorr). h In situ IR spectra (green) of ~150 Torr CH3I exposed MIL-101-Cr-HMTA referenced to the activated MIL-101-Cr-HMTA; and IR absorption spectra (red) of activated MIL-101-Cr-HMTA referenced to KBr pellet (<20 mtorr). i Ion exchange efficiencies of an anionic dye (Orange G or OG) by pristine MIL-101-Cr-TED and MIL-101-Cr-HMTA and functionalized CH3I@MIL-101-Cr-TED and CH3I@MIL-101-Cr-HMTA as a function of time
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References

    1. World energy needs and nuclear power. World Nuclear Associationhttp://www.world-nuclear.org/information-library/current-and-future-gene....
    1. Haefner, D. R. & Tranter, T. J. Methods of Gas Phase Capture of Iodine from Fuel Reprocessing Off-Gas: a Literature Survey. Report No. INL/EXT-07-12299 (Idaho National Laboratory, 2007).
    1. Clément, B. et al. State of the Art Report on Iodine Chemistry. Report No. NEA/CSNI/R(2007)1 (International Atomic Energy Agency/International Nuclear Information System, 2007).
    1. Bruffey, S. H. et al. A Literature Survey to Identify Potentially Problematic Volatile Iodine-Bearing Species Present in Off-Gas Streams. Report No. FCRD-MRWFD-2015-000421, ORNL-SPR-2015/290, INL/EXT-15-35609 (2015).
    1. Bruffey, S. H., Jubin, R. T. & Jordan, J. A. Organic Iodine Adsorption by AgZ under Prototypical Vessel Off-Gas Conditions. Report No. FCRD-MRWFD-2016-000357; ORNL/TM-2016/568 (2016).

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