PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUEL

The relevance of the research is based on the rationale for creating suitable environment for fuel thermochemical treatment to ensure simultaneous ceramic fuel conversion into powder-like material, complete recladding of reaction product, and volatile fission products entrapment (tritium, iodine-129...

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Main Authors: Pavel V. Aksyutin, Anton S. Dyachenko, Andrey Yu. Zhabin, Ivan I.Zherin
Format: Article
Language:Russian
Published: Tomsk Polytechnic University 2021-08-01
Series:Известия Томского политехнического университета: Инжиниринг георесурсов
Subjects:
Online Access:http://izvestiya.tpu.ru/archive/article/view/3301/2521
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author Pavel V. Aksyutin
Anton S. Dyachenko
Andrey Yu. Zhabin
Ivan I.Zherin
author_facet Pavel V. Aksyutin
Anton S. Dyachenko
Andrey Yu. Zhabin
Ivan I.Zherin
author_sort Pavel V. Aksyutin
collection DOAJ
description The relevance of the research is based on the rationale for creating suitable environment for fuel thermochemical treatment to ensure simultaneous ceramic fuel conversion into powder-like material, complete recladding of reaction product, and volatile fission products entrapment (tritium, iodine-129, carbon-14, radioactive noble gases) from fuel composition prior to hydrometallurgical processes. The main aim is to find main process parameters of NxOy-O2-CO2-H2O (steam) oxidizing mixture which can be used for thermochemical treatment of cladded fuel containing ceramic uranium dioxide. Subjects: solution of nitric acid and oxalic acid composition, NxOy-O2-CO2-H2O (steam) oxidizing mixture, sample of new fuel element containing uranium dioxide. Methods: investigational studies, conductometric and potentiometric titration, gravimetric and and X-ray phase analysis, morphological studies, gas chromatography. The results. The main physical and chemical rules of fabricating NxOy-O2-CO2-H2O (steam) oxidizing mixture were studied for thermochemical treatment of fuel containing uranium dioxide. It was found that generation of gas bearing nitrogen dioxide (26 vol. %), nitrogen monoxide (20 vol. %), carbon dioxide (44 vol. %) and water vapor (10 vol. %) was the result of passing acids mixture (nitric acid – 380 g/l, oxalic acid – 80 g/l) at the rate of 5 column volumes per hour through Pt/Cr2O3/ZrO2 catalyst layer at 368–373 K. It is preferable to implement nitrogen monoxide full oxidation and gas catalytic activation by means of Pt/Cr2O3/ZrO2 packing at 413 K and height of packed bed to column diameter ratio as 5:1. Upon doing that, oxidizing mixture has the following composition: nitrogen dioxide (41 vol. %), nitrogen monoxide (6 vol. %), carbon dioxide (42 vol. %), water vapor (6 vol. %) and oxygen (5 vol. %). Ability in principle to convert ceramic fuel containing non-irradiated uranium dioxide in zirconium cladding into powder-like triuranium octoxide was proven by using NxOy-O2-CO2-H2O (steam) mixture as an oxidizing agent following catalytic activation. We made powder-like material separated from zirconium cladding in full which corresponds to molecular formula U3O8 from X-ray phase and gravimetric analyses, O/U=2,67.
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spelling doaj.art-bb6a792255f04c9bbb5327066364ea4a2022-12-22T03:44:40ZrusTomsk Polytechnic UniversityИзвестия Томского политехнического университета: Инжиниринг георесурсов2500-10192413-18302021-08-013328182710.18799/24131830/2021/8/3301PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUELPavel V. Aksyutin0Anton S. Dyachenko1Andrey Yu. Zhabin2Ivan I.Zherin3Mining and Chemical CombineMining and Chemical CombineMining and Chemical CombineNational Research Tomsk Polytechnic UniversityThe relevance of the research is based on the rationale for creating suitable environment for fuel thermochemical treatment to ensure simultaneous ceramic fuel conversion into powder-like material, complete recladding of reaction product, and volatile fission products entrapment (tritium, iodine-129, carbon-14, radioactive noble gases) from fuel composition prior to hydrometallurgical processes. The main aim is to find main process parameters of NxOy-O2-CO2-H2O (steam) oxidizing mixture which can be used for thermochemical treatment of cladded fuel containing ceramic uranium dioxide. Subjects: solution of nitric acid and oxalic acid composition, NxOy-O2-CO2-H2O (steam) oxidizing mixture, sample of new fuel element containing uranium dioxide. Methods: investigational studies, conductometric and potentiometric titration, gravimetric and and X-ray phase analysis, morphological studies, gas chromatography. The results. The main physical and chemical rules of fabricating NxOy-O2-CO2-H2O (steam) oxidizing mixture were studied for thermochemical treatment of fuel containing uranium dioxide. It was found that generation of gas bearing nitrogen dioxide (26 vol. %), nitrogen monoxide (20 vol. %), carbon dioxide (44 vol. %) and water vapor (10 vol. %) was the result of passing acids mixture (nitric acid – 380 g/l, oxalic acid – 80 g/l) at the rate of 5 column volumes per hour through Pt/Cr2O3/ZrO2 catalyst layer at 368–373 K. It is preferable to implement nitrogen monoxide full oxidation and gas catalytic activation by means of Pt/Cr2O3/ZrO2 packing at 413 K and height of packed bed to column diameter ratio as 5:1. Upon doing that, oxidizing mixture has the following composition: nitrogen dioxide (41 vol. %), nitrogen monoxide (6 vol. %), carbon dioxide (42 vol. %), water vapor (6 vol. %) and oxygen (5 vol. %). Ability in principle to convert ceramic fuel containing non-irradiated uranium dioxide in zirconium cladding into powder-like triuranium octoxide was proven by using NxOy-O2-CO2-H2O (steam) mixture as an oxidizing agent following catalytic activation. We made powder-like material separated from zirconium cladding in full which corresponds to molecular formula U3O8 from X-ray phase and gravimetric analyses, O/U=2,67.http://izvestiya.tpu.ru/archive/article/view/3301/2521mixture of nitric and oxalic acidscatalytic decompositionoxidizing mixturecatalytically-active material packingceramic fuelpowder-like material
spellingShingle Pavel V. Aksyutin
Anton S. Dyachenko
Andrey Yu. Zhabin
Ivan I.Zherin
PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUEL
Известия Томского политехнического университета: Инжиниринг георесурсов
mixture of nitric and oxalic acids
catalytic decomposition
oxidizing mixture
catalytically-active material packing
ceramic fuel
powder-like material
title PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUEL
title_full PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUEL
title_fullStr PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUEL
title_full_unstemmed PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUEL
title_short PRODUCTION OF NxOy-O2-CO2-H2O (steam) FOR THERMOCHEMICAL TREATMENT OF IRRADIATED UO2 FUEL
title_sort production of nxoy o2 co2 h2o steam for thermochemical treatment of irradiated uo2 fuel
topic mixture of nitric and oxalic acids
catalytic decomposition
oxidizing mixture
catalytically-active material packing
ceramic fuel
powder-like material
url http://izvestiya.tpu.ru/archive/article/view/3301/2521
work_keys_str_mv AT pavelvaksyutin productionofnxoyo2co2h2osteamforthermochemicaltreatmentofirradiateduo2fuel
AT antonsdyachenko productionofnxoyo2co2h2osteamforthermochemicaltreatmentofirradiateduo2fuel
AT andreyyuzhabin productionofnxoyo2co2h2osteamforthermochemicaltreatmentofirradiateduo2fuel
AT ivanizherin productionofnxoyo2co2h2osteamforthermochemicaltreatmentofirradiateduo2fuel