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SPECIAL SECTION: SELECTED PAPERS FROM THE 2018 INTERNATIONAL YOUTH NUCLEAR CONGRESS

Pyrolysis and High Performance Plasma Treatment Applied to Spent Ion Exchange Resins

[+] Author and Article Information
Hernán Ariel Castro

Programa Nacional de Gestión
de Residuos Radiactivos,
Comisión Nacional de Energía Atómica,
Centro Atómico Constituyentes,
Av. General Paz 1499,
San Martín 1650, Buenos Aires, Argentina;
Escuela de Ciencia y Tecnología,
Campus Miguelete,
Universidad Nacional de General San Martín,
Martín de Irigoyen 3100,
San Martín 1650,
Buenos Aires, Argentina
e-mail: hcastro@cnea.gov.ar

Raúl Ariel Rodríguez

Gerencia de Química,
Comisión Nacional de Energía Atómica,
Centro Atómico Constituyentes,
Av. General Paz 1499,
San Martín 1650, Buenos Aires, Argentina
e-mail: raularielrodriguez@cnea.gov.ar

Vittorio Luca

Programa Nacional de Gestión de
Residuos Radiactivos,
Comisión Nacional de Energía Atómica,
Centro Atómico Constituyentes,
Av. General Paz 1499,
San Martín 1650, Buenos Aires, Argentina
e-mail: vluca@cnea.gov.ar

Hugo Luis Bianchi

Gerencia de Química,
Comisión Nacional de Energía Atómica,
Centro Atómico Constituyentes,
Av. General Paz 1499,
San Martín 1650, Buenos Aires, Argentina;
Escuela de Ciencia y Tecnología,
Campus Miguelete,
Universidad Nacional de General San Martín,
Martín de Irigoyen 3100,
San Martín 1650, Buenos Aires, Argentina
e-mail: bianchi@cnea.gov.ar

1Corresponding author.

Manuscript received June 29, 2018; final manuscript received November 26, 2018; published online March 15, 2019. Assoc. Editor: Ignacio Gómez. This work was prepared while under employment by the Government of Argentina as part of the official duties of the author(s) indicated above, as such copyright is owned by that Government, which reserves its own copyright under national law.

ASME J of Nuclear Rad Sci 5(2), 020901 (Mar 15, 2019) (8 pages) Paper No: NERS-18-1045; doi: 10.1115/1.4042193 History: Received June 29, 2018; Revised November 26, 2018

Treatment and conditioning of spent ion exchange resins from nuclear facilities is a complex process that not only should contemplate obtaining a stable product suitable for long-term storage and/or disposal, but also have to take into account the treatment of secondary currents generated during the process. The combination of low temperature pyrolysis treatment and high performance plasma treatment (HPPT) of the off-gas generated could be a novel solution for organic matrix nuclear wastes with economic and safety advantages. In the present work, results of lab scale studies associated with the pyrolysis off-gas characterization and the performance and operating parameters influence on the removal of model compounds in a laboratory-scale flow reactor, using inductively coupled plasma under subatmospheric conditions, are shown. The pyrolysis off-gas stream was largely characterized and the evolution of main compounds of interest as function of temperature process was established. The results of plasma assays with the model compound demonstrate a high destruction and removal efficiency (>99.990%) and a good control over the final gas products. First results of a bench scale arrangement combining both processes are presented and bode well for the application of this combined technology.

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References

Alexandratos, S. D. , 2009, “ Ion-Exchange Resins: A Restrospective From Industrial and Engineering Chemistry Research,” Ind. Eng. Chem. Res., 48(1), pp. 388–398. [CrossRef]
Wang, J. , and Wan, Z. , 2015, “ Treatment and Disposal of Spent Radioactive Ion-Exchange Resins Produced in the Nuclear Industry,” Prog. Nucl. Energy, 78, pp. 47–55. [CrossRef]
Wan, Z. , Xu, L. , and Wang, J. , 2016, “ Treatment of Spent Radioactive Anionic Exchange Resins Using Fenton-Like Oxidation Process,” Chem. Eng. J., 284, pp. 733–740. [CrossRef]
Zhu, Z. , Tang, X. , Yin, Z. , and Yu, W. , 2014, “ Sulfate Ion (SO42−) Release From Old and New Cation Exchange Resins Used in Condensate Polishing Systems for Power Plants,” Water Sci. Technol., 70(7), pp. 1188–1194. [CrossRef] [PubMed]
IAEA, 2002, “ Application of Ion Exchange Processes for the Treatment of Radioactive Waste and Management of Spent Ion Exchangers,” International Atomic Energy Agency, Vienna, Austria, Technical Report No. 408. https://www-pub.iaea.org/MTCD/Publications/PDF/TRS408_scr.pdf
Bridgwater, A. V. , 2012, “ Review of Fast Pyrolysis of Biomass and Product Upgrading,” Biomass Bioenergy, 38, pp. 68–94. [CrossRef]
Kaminsky, W. , 1985, “ Thermal Recycling of Polymers,” J. Anal. Appl. Pyrolysis, 8, pp. 439–448. [CrossRef]
Quek, A. , and Balasubramanian, R. , 2013, “ Liquefaction of Waste Tires by Pyrolysis for Oil and Chemicals—A Review,” J. Anal. Appl. Pyrolysis, 101, pp. 1–16. [CrossRef]
IAEA, 2006, “ Innovative Waste Treatment and Conditioning Technologies at Nuclear Power Plants,” International Atomic Energy Agency, Vienna, Austria, TECDOC No. 1504. https://www-pub.iaea.org/MTCD/Publications/PDF/te_1504_web.pdf
Pettersson, S. , and Kemmler, G. , 1984, “ Experience on Resin Pyrolysis,” Waste Management ‘84, Symposium on Waste Isolation in the U.S. Technical Programs and Public Education, Tucson, AZ, Mar. 11–15, Paper No. 6533.
Brähler, G. , and Slametschka, R. , 2012, “ Pyrolysis of Spent Ion Exchange Resins,” Waste Management Conference, Phoenix, AZ, Feb. 26–Mar. 1, p. 1667.
Luycx, P. , and Deckers, J. , 1999, “ Pebble Bed Pyrolysis for the Processing of Alpha Contaminated Organic Effluents,” Waste Management Conference, Tucson, AZ, Feb. 28–Mar. 4, Paper No. 37–3. http://archive.wmsym.org/1999/37/37-3.pdf
THOR Treatment Technologies, 2002, “ THORSM Steam Reforming Process for Hazardous and Radioactive Wastes,” THOR Treatment Technologies, Denver, CO, Report No. TR- SR02-1, Rev. 1.
Mollah, M. Y. A. , Schennach, R. , Patscheider, J. , Promreuk, S. , and Cocke, D. L. , 2000, “ Plasma Chemistry as a Tool for Green Chemistry, Environmental Analysis and Waste Management,” J. Hazard. Mater. B, 79(3), pp. 301–320. [CrossRef]
Yoshida, K. , Yamamoto, T. , Kuroki, T. , and Okubo, M. , 2009, “ Pilot-Scale Experiment for Simultaneous Dioxin and NOx Removal From Garbage Incinerator Emissions Using the Pulse Corona Induced Plasma Chemical Process,” Plasma Chem. Plasma Process., 29(5), pp. 373–386. [CrossRef]
Ojovan, M. I. , 2011, Handbook of Advanced Radioactive Waste Conditioning Technologies, Woodhead Publishing Limited, Cambridge, UK, Chap. 3.
Konjevic, N. , Ivkovic, M. , and Sakan, N. , 2012, “ Hydrogen Balmer Lines for Low Electron Number Density Plasma Diagnostics,” Spectrochim. Acta Part B, 76, pp. 16–26. [CrossRef]
Da-Zhi, J. , Zhong-Hai, Y. , Ping-Ying, T. , Kun-xiang, X. , and Jing-yi, D. , 2009, “ Hydrogen Plasma Diagnosis in Penning Ion Source by Optical Emission Spectroscopy,” Vacuum, 83, pp. 451–453.
Matsuda, M. , Funabashi, K. , Nishi, T. , and Yusa, H. , 1986, “ Decomposition of Ion Exchange Resins by Pyrolysis,” Nucl. Technol., 75(2), pp. 187–192. [CrossRef]
Dubois, M. A. , Dozol, J. F. , Nicotra, C. , Serose, J. , and Massiani, C. , 1995, “ Pyrolisis and Incineration of Cationic and Anionic Ion-Exchange Resins—Identification of Volatile Degradation Compounds,” J. Anal. Appl. Pyrolysis, 31, pp. 129–140. [CrossRef]
Park, S. D. , Kim, J. S. , Han, S. H. , and Jee, K. Y. , 2008, “ Distribution Characteristics of 14C and 3H in Spent Resins From the Canada Deuterium Uranium-Pressurized Heavy Water Reactors (CANDU-PHWRs) of Korea,” J. Radioanal. Nucl. Chem., 277(3), pp. 503–511. [CrossRef]
Luca, V. , Bianchi, H. L. , Allevatto, F. , Vaccaro, J. O. , and Alvarado, A. , 2017, “ Low Temperature Pyrolysis of Simulated Spent Anion Exchange Resins,” J. Environ. Chem. Eng., 5(4), pp. 4165–4172. [CrossRef]
Luca, V. , Bianchi, H. L. , and Manzini, A. C. , 2012, “ Cation Immobilization in Pyrolyzed Simulated Spent Ion Exchange Resins,” J. Nucl. Mater., 424(1–3), pp. 1–11. [CrossRef]
Castro, H. A. , Luca, V. , and Bianchi, H. L. , 2017, “ Study of Plasma Off-Gas Treatment From Spent Ion Exchange Resins Pyrolysis,” Environ., Sci. Pollut. Res., 25(22), pp. 21403–21410.
Rehman, F. , Lozano-Parada, J. H. , and Zimmerman, W. B. , 2012, “ A Kinetic Model for H2 Production by Plasmolysis of Water Vapours at Atmospheric Pressure in a Dielectric Barrier Discharge Microchannel Reactor,” Int. J. Hydrogen Energy, 37(23), pp. 17678–17690. [CrossRef]

Figures

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Fig. 1

Scheme of the experimental plasma system arrangement: (1) sample, (2) injection heater, (3) quartz reactor, (4) cold trap, (5) chemical resistant vacuum pump, (6) high resolution spectrometer, (7) multigas analyzer, (8) gas mass spectrometer, (9) scrubber, (10) mass flow controllers, (11) RF generator, (12) RF matching network, (13) sampling point, and (14) computer

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Fig. 2

Scheme of the bench scale pyrolysis and HPPT system

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Fig. 3

Thermal gravimetric analyses of samples of ion exchange resins under Ar

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Fig. 4

Two-dimensional mass spectra of gas pyrolysis byproducts in argon atmosphere for both types of resins as a function of the temperature. The colors indicate the signal intensity for each m/z ratio where blue is low intensity and red is high intensity.

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Fig. 5

Normalized counts evolution of trimethylamine (ESI-MS condensate analysis) and sulfur dioxide (direct gas mass spectrometry) as a function of the increasing pyrolysis temperature

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Fig. 6

Normalized counts evolution of carbon dioxide (direct gas mass spectrometry) as a function of the increasing pyrolysis temperature

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Fig. 7

Evaluation of DRE for butylamine as function of the specific energy (PW/Q) in presence and absence of O2 in the reaction medium. The molar fractions of the compounds in the inlet mixture were in the ranges: XAr = 0.75–0.90, XH2O = 0.08–0.20, Xbutylamine = 0.002–0.005, and XO2 = 0–0.04.

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Fig. 8

CH (C–X) and CN (B–X) radicals emission spectra as function of the molar fraction of water in the reaction medium (XH2O = 0.01, 0.06, 0.11 and 0.17)

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Fig. 9

Influence of O2 in the reaction medium in the selectivity of formation of CO, CO2, NOx and H2 for the treatment of n-butylamine 10 wt %/wt solution (0: no O2, S.B.: O2 in stoichiometric balance; Exc.: O2 in excess)

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Fig. 10

Influence of the residence time (tR) of the model compound in the reaction medium in the final products (a), and in the CH radical emission spectra's (C–X) (b)

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Fig. 11

Peak intensities of different compounds of interest from anionic resin pyrolysis off-gas stream with and without plasma treatment

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