DE1592129B2 - PROCESS FOR REPROCESSING NUCLEAR FUEL ELEMENTS - Google Patents
PROCESS FOR REPROCESSING NUCLEAR FUEL ELEMENTSInfo
- Publication number
- DE1592129B2 DE1592129B2 DE19671592129 DE1592129A DE1592129B2 DE 1592129 B2 DE1592129 B2 DE 1592129B2 DE 19671592129 DE19671592129 DE 19671592129 DE 1592129 A DE1592129 A DE 1592129A DE 1592129 B2 DE1592129 B2 DE 1592129B2
- Authority
- DE
- Germany
- Prior art keywords
- uranium
- thorium
- fuel
- fluorination
- melt
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 238000000034 method Methods 0.000 title claims description 13
- 239000003758 nuclear fuel Substances 0.000 title claims description 6
- 238000012958 reprocessing Methods 0.000 title claims description 6
- 229910052770 Uranium Inorganic materials 0.000 claims description 20
- JFALSRSLKYAFGM-UHFFFAOYSA-N uranium(0) Chemical compound [U] JFALSRSLKYAFGM-UHFFFAOYSA-N 0.000 claims description 20
- 239000000203 mixture Substances 0.000 claims description 14
- GFRMDONOCHESDE-UHFFFAOYSA-N [Th].[U] Chemical compound [Th].[U] GFRMDONOCHESDE-UHFFFAOYSA-N 0.000 claims description 12
- 238000006243 chemical reaction Methods 0.000 claims description 10
- 238000003682 fluorination reaction Methods 0.000 claims description 10
- ZSLUVFAKFWKJRC-IGMARMGPSA-N 232Th Chemical compound [232Th] ZSLUVFAKFWKJRC-IGMARMGPSA-N 0.000 claims description 9
- 239000000155 melt Substances 0.000 claims description 9
- 229910052776 Thorium Inorganic materials 0.000 claims description 8
- 239000000463 material Substances 0.000 claims description 7
- 239000002245 particle Substances 0.000 claims description 7
- ZCUFMDLYAMJYST-UHFFFAOYSA-N thorium dioxide Chemical compound O=[Th]=O ZCUFMDLYAMJYST-UHFFFAOYSA-N 0.000 claims description 7
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 claims description 6
- 239000003513 alkali Substances 0.000 claims description 6
- 229910052731 fluorine Inorganic materials 0.000 claims description 6
- 239000011737 fluorine Substances 0.000 claims description 6
- 238000001556 precipitation Methods 0.000 claims description 6
- KRHYYFGTRYWZRS-UHFFFAOYSA-M Fluoride anion Chemical compound [F-] KRHYYFGTRYWZRS-UHFFFAOYSA-M 0.000 claims description 5
- 229910003452 thorium oxide Inorganic materials 0.000 claims description 5
- 238000004821 distillation Methods 0.000 claims description 4
- 238000000576 coating method Methods 0.000 claims description 3
- 238000001914 filtration Methods 0.000 claims description 3
- 150000001247 metal acetylides Chemical class 0.000 claims description 3
- 238000000926 separation method Methods 0.000 claims description 3
- 239000007787 solid Substances 0.000 claims description 3
- 239000011248 coating agent Substances 0.000 claims description 2
- 239000000446 fuel Substances 0.000 claims 11
- 150000003839 salts Chemical class 0.000 claims 5
- 238000009395 breeding Methods 0.000 claims 4
- 230000001488 breeding effect Effects 0.000 claims 4
- 238000002485 combustion reaction Methods 0.000 claims 3
- 230000004992 fission Effects 0.000 claims 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims 2
- 244000144987 brood Species 0.000 claims 2
- 125000004122 cyclic group Chemical group 0.000 claims 2
- 239000000126 substance Substances 0.000 claims 2
- 241000767684 Thoe Species 0.000 claims 1
- 150000001447 alkali salts Chemical class 0.000 claims 1
- 230000000712 assembly Effects 0.000 claims 1
- 238000000429 assembly Methods 0.000 claims 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims 1
- -1 carbides uranium thorium oxide Chemical class 0.000 claims 1
- 229910052799 carbon Inorganic materials 0.000 claims 1
- 238000005260 corrosion Methods 0.000 claims 1
- 230000007797 corrosion Effects 0.000 claims 1
- 230000009089 cytolysis Effects 0.000 claims 1
- 238000009792 diffusion process Methods 0.000 claims 1
- 239000010439 graphite Substances 0.000 claims 1
- 229910002804 graphite Inorganic materials 0.000 claims 1
- 239000012456 homogeneous solution Substances 0.000 claims 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 claims 1
- 239000011159 matrix material Substances 0.000 claims 1
- 229910052751 metal Inorganic materials 0.000 claims 1
- 239000002184 metal Substances 0.000 claims 1
- 239000003921 oil Substances 0.000 claims 1
- 229910052760 oxygen Inorganic materials 0.000 claims 1
- 239000001301 oxygen Substances 0.000 claims 1
- WJWSFWHDKPKKES-UHFFFAOYSA-N plutonium uranium Chemical compound [U].[Pu] WJWSFWHDKPKKES-UHFFFAOYSA-N 0.000 claims 1
- 239000002574 poison Substances 0.000 claims 1
- 231100000614 poison Toxicity 0.000 claims 1
- 239000002296 pyrolytic carbon Substances 0.000 claims 1
- 230000002285 radioactive effect Effects 0.000 claims 1
- 239000002901 radioactive waste Substances 0.000 claims 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims 1
- 229910010271 silicon carbide Inorganic materials 0.000 claims 1
- 238000000638 solvent extraction Methods 0.000 claims 1
- 239000007858 starting material Substances 0.000 claims 1
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 claims 1
- SANRKQGLYCLAFE-UHFFFAOYSA-H uranium hexafluoride Chemical compound F[U](F)(F)(F)(F)F SANRKQGLYCLAFE-UHFFFAOYSA-H 0.000 description 8
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- 239000002244 precipitate Substances 0.000 description 4
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 description 3
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 229910052783 alkali metal Inorganic materials 0.000 description 3
- 150000001340 alkali metals Chemical class 0.000 description 3
- 229910000040 hydrogen fluoride Inorganic materials 0.000 description 3
- 239000011261 inert gas Substances 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- MZFRHHGRNOIMLW-UHFFFAOYSA-J uranium(4+);tetrafluoride Chemical compound F[U](F)(F)F MZFRHHGRNOIMLW-UHFFFAOYSA-J 0.000 description 2
- 229910001854 alkali hydroxide Inorganic materials 0.000 description 1
- 229910001515 alkali metal fluoride Inorganic materials 0.000 description 1
- 150000008044 alkali metal hydroxides Chemical class 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000005119 centrifugation Methods 0.000 description 1
- 239000003638 chemical reducing agent Substances 0.000 description 1
- 230000000994 depressogenic effect Effects 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- KAQHZJVQFBJKCK-UHFFFAOYSA-L potassium pyrosulfate Chemical compound [K+].[K+].[O-]S(=O)(=O)OS([O-])(=O)=O KAQHZJVQFBJKCK-UHFFFAOYSA-L 0.000 description 1
- DJOHOFCGSNZSNN-UHFFFAOYSA-N potassium uranium Chemical compound [K].[U] DJOHOFCGSNZSNN-UHFFFAOYSA-N 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000000047 product Substances 0.000 description 1
Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21C—NUCLEAR REACTORS
- G21C19/00—Arrangements for treating, for handling, or for facilitating the handling of, fuel or other materials which are used within the reactor, e.g. within its pressure vessel
- G21C19/42—Reprocessing of irradiated fuel
- G21C19/44—Reprocessing of irradiated fuel of irradiated solid fuel
- G21C19/48—Non-aqueous processes
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G43/00—Compounds of uranium
- C01G43/04—Halides of uranium
- C01G43/06—Fluorides
- C01G43/063—Hexafluoride (UF6)
- C01G43/066—Preparation
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E30/00—Energy generation of nuclear origin
- Y02E30/30—Nuclear fission reactors
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W30/00—Technologies for solid waste management
- Y02W30/50—Reuse, recycling or recovery technologies
Landscapes
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Plasma & Fusion (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Life Sciences & Earth Sciences (AREA)
- General Life Sciences & Earth Sciences (AREA)
- Geology (AREA)
- Inorganic Chemistry (AREA)
- Inorganic Compounds Of Heavy Metals (AREA)
Description
Aufgabe der Erfindung ist es daher, ein Verfahren zum Wiederaufarbeiten- von Kernbrennstoffelementen aus Uran-Thorium-Mischoxid oder Uran-Thorium-Mischcarbid zu schaffen, bei dem auf wirtschaftliche Weise eine Abtrennung durch Fluorierung möglich ist.The object of the invention is therefore to provide a method for reprocessing nuclear fuel elements from uranium-thorium mixed oxide or uranium-thorium mixed carbide, in which on economic Way, a separation by fluorination is possible.
Diese Aufgabe wird gemäß der Erfindung dadurch gelöst, daß der Kernbrennstoff nach dem Entfernen der Umhüllung und gegebenenfalls nach Umwandlung der Carbide in eine Mischung von U3O8 und ThO2 in einer Pyrosulfatschmelze aufgelöst wird, worauf in die Schmelze festes Alkalyhydroxid in solcher Menge eingebracht wird, daß die Lösung alkalisch reagiert und daß das durch Ausfällen und anschließendes Filtrieren oder Zentrifugieren im Gemisch mit Thoriumoxid als Alkaliuranat anfallende Uran in bekannter Weise durch Fluorieren und Abdestillieren als Uranhexafluorid abgetrennt wird.This object is achieved according to the invention in that the nuclear fuel is dissolved in a pyrosulfate melt after removing the coating and optionally after converting the carbides into a mixture of U 3 O 8 and ThO 2 , whereupon solid alkali hydroxide is introduced into the melt in such an amount that the solution reacts alkaline and that the uranium obtained by precipitation and subsequent filtration or centrifugation in a mixture with thorium oxide as alkali uranium is separated in a known manner by fluorination and distillation as uranium hexafluoride.
Zur Durchführung der Fluorierung des angefallenen Niederschlages sind die folgenden Maßnahmen geeignet. Das bei der Fällung im Gemisch mit Thoriumoxid anfallende Alkaliuranat wird durch Einwirken von gasförmigem Fluorwasserstoff HF bei Temperaturen zwischen 450 und 55O°C in ein Gemisch von UO2F2 und Alkalifluorid umgewandelt und imThe following measures are suitable for carrying out the fluorination of the accumulated precipitate. The alkali uranium obtained during the precipitation in a mixture with thorium oxide is converted into a mixture of UO 2 F 2 and alkali fluoride by the action of gaseous hydrogen fluoride HF at temperatures between 450 and 550 ° C. and im
ίο Anschluß daran durch elementares Fluor, gegebenenfalls im Gemisch mit inerten Gasen wie Stickstoff od. dgl. bei Temperaturen zwischen 350 und 55O0C fluoriert. Die Umwandlung des angefallenen Kaliumuranats in Uranhexafluorid erfolgt somit nach den Reaktionsgleichungenίο Subsequently od by elemental fluorine, optionally in admixture with inert gases such as nitrogen. like. at temperatures between 350 and 55O 0 C fluorinated. The conversion of the resulting potassium uranium into uranium hexafluoride thus takes place according to the reaction equations
K2U2O7 + 6 HF 2 UO2F2 + 2 KF + 3 H2OK 2 U 2 O 7 + 6 HF 2 UO 2 F 2 + 2 KF + 3 H 2 O
TTr. „ , o_ 350 bis 5500C TTC , ■._ UO2F2 + 2F2 > UF6+ O2 TTr . ", O _ 350 to 550 0 C TTC , ■ ._ UO 2 F 2 + 2F 2 > UF 6 + O 2
Nach einer anderen sehr zweckmäßigen Maßnahme zur Durchführung des erfindungsgemäßen Verfahrens wird das beim Fällen im Gemisch mit Thoriumoxid anfallende Alkaliuranat durch Einwirkung einer Mischung von Fluorwasserstoff und eines gasförmigen Reduktionsmittels wie SO2 oder NH3 bei Temperaturen zwischen 400 und 5000C in eine Mischung von Urantetrafluorid und Alkalifluorid umgewandelt, worauf in einer weiteren Verfahrensstufe bei einer Temperatur zwischen 350 und 55O0C das Urantetrafluorid durch Einwirken von elementarem Fluor, gegebenenfalls in einer Mischung mit einem inerten Gas wie Stickstoff od. dgl., in Uranhexafluorid umgewandelt wird. Der Reaktionsablauf erfolgt dann nach den GleichungenAccording to another very useful measure for carrying out the process according to the invention, the alkali uranium obtained in the precipitation in a mixture with thorium oxide is converted into a mixture of uranium tetrafluoride by the action of a mixture of hydrogen fluoride and a gaseous reducing agent such as SO 2 or NH 3 at temperatures between 400 and 500 ° C. and alkali metal fluoride is converted, optionally followed od in a further process stage at a temperature between 350 and 55O 0 C, the uranium tetrafluoride by exposure to elemental fluorine in admixture with an inert gas such as nitrogen. the like., is converted into uranium hexafluoride. The reaction then takes place according to the equations
Na2UO4+6HF+SO2 UF4 + 2 NaF + 3 H2O + SO3 Na 2 UO 4 + 6HF + SO 2 UF 4 + 2 NaF + 3 H 2 O + SO 3
oderor
undand
3K2U2O7 + 30HF + 4NH3 3K 2 U 2 O 7 + 30HF + 4NH 3
6KF6KF
+ 2N2 + 2N 2
ΤΤϋ , _ 350bis550°C T„ UF4 + F2 > UF6 ΤΤϋ , _ 350 to 550 ° C T " UF 4 + F 2 > UF 6
Nach einer weiteren zweckmäßigen Abwandlung der Maßnahmen zur Durchführung des Verfahrens gemäß der Erfindung wird das bei der Fällung im Gemisch mit Thoriumoxid anfallende Alkaliuranat nach Abtrennen von der Schmelze bei einer Temperatur von etwa 4500C mittels elementarem Fluor im Wirbelschichtofen fluoriert. Die Fluorierung erfolgt somit nach der ReaktionsgleichungAccording to a further advantageous modification of the measures for implementing the method according to the invention is fluorinated, the resulting in the precipitation mixture with thoria Alkaliuranat after separation from the melt at a temperature of about 450 0 C by means of elemental fluorine in the fluidized bed furnace. The fluorination thus takes place according to the reaction equation
Na2UO4+ 4F2 Na 2 UO 4 + 4F 2
350 bis 550° C350 to 550 ° C
UF6 + 2NaF + 2O2 UF 6 + 2NaF + 2O 2
Das anwesende Thoriumdioxid wird bei den jeweiligen Maßnahmen zur Fluorierung des Alkaliuranats ebenfalls allerdings nur zum Teil fluoriert. Es hat sich jedoch gezeigt, daß dadurch die quantitative Bildung und Verflüchtigung von Uranhexafluorid nicht gestört wird. Der große Vorzug des Verfahrens gemäß der Erfindung besteht darin, daß das Uran aus dem in der Schmelze gebildeten Niederschlag leicht und vollständig als flüchtiges Uranhexafluorid abtrennbar ist.The thorium dioxide present is used during the respective measures to fluorinate the alkali metal uranium but also only partially fluorinated. However, it has been shown that this allows quantitative formation and volatilization of uranium hexafluoride is not disturbed. The great advantage of the method according to the Invention is that the uranium from the precipitate formed in the melt easily and completely can be separated as volatile uranium hexafluoride.
1. In 30 g einer Kaliumpyrosulfatschmelze wurden 10 g intakte Uran-Thorium-Mischoxidpartikeln
eingetragen, wobei das Atomverhältnis von Uran zu Thorium 1: 5 betrug, und in einem geschlossenen
Reaktionsgefäß bei 700 bis 80O0C innerhalb einer Zeit von 21I2 Stunden quantitativ in Lösung
gebracht. Anschließend wurden der Schmelze bei etwa 600° C 30 g festes NaOH zugesetzt. Der ausgefallene
Niederschlag von Alkaliuranat und Alkalidiuranat sowie von Thoriumoxid wurde durch Filtration durch ein Sinterfilter von der
Schmelze abgetrennt. Im Anschluß daran wurde das Gemenge im Wirbelschichtofen 1 Stunde lang
mit elementarem Fluor bei 5000C zur Reaktion
gebracht und das abdestillierte Uranhexafluorid in einer auf minus 6O0C gehaltenen Kühlfalle
niedergeschlagen. Wie die anschließende Analyse ergab, war das Uran quantitativ als Uranhexafluorid
verflüchtigt worden, während das Thorium als teilweise fluoriertes Produkt im Rückstand
verblieb. Der im Thoriumrückstand festgestellte Urangehalt lag bei 0,05%.
Ein beim Ausfällen aus einer Pyrosulfatschmelze gebildeter Niederschlag von K2U2O7 + ThO2,
wobei das Atomverhältnis zwischen Uran und Thorium 1: 5 betrug, wurde in einem Wirbelschichtofen,
dessen Ofenkörper aus reinem Sinterkonind bestand, bei einer Ofentemperatur zwischen
500 und 55O0C 2V2 Stunden mit Fluorwasserstoff
behandelt. Dabei wurde das Uran des eingesetzten Gemisches quantitativ zu UO2F2 umgesetzt. Das Reaktionsgut fiel pulvrig an. Die anschließende
Verflüchtigung des Urans als Uranhexafluorid erfolgte in der gleichen Anlage durch
l^stündige Reaktion mit elementarem Fluor. Die Uranausbeute war dabei größer als 99,5 %.1. 10 g of intact uranium-thorium mixed oxide particles were introduced into 30 g of a potassium pyrosulfate melt, the atomic ratio of uranium to thorium being 1: 5, and in a closed reaction vessel at 700 to 80O 0 C within a period of 2 1 I 2 hours Quantitatively brought into solution. Then 30 g of solid NaOH were added to the melt at about 600 ° C. The resulting precipitate of alkali metal uranate and alkali metal diuranate and also of thorium oxide was separated from the melt by filtration through a sintered filter. Subsequently, the mixture in the fluidized bed furnace was placed for 1 hour with elemental fluorine at 500 0 C to the reaction and depressed the distilled uranium hexafluoride in a minus maintained at 6O 0 C cold trap. As the subsequent analysis showed, the uranium had been volatilized quantitatively as uranium hexafluoride, while the thorium remained in the residue as a partially fluorinated product. The uranium content found in the thorium residue was 0.05%.
A precipitate of K 2 U 2 O 7 + ThO 2 formed during precipitation from a pyrosulphate melt, the atomic ratio between uranium and thorium being 1: 5, was in a fluidized bed furnace, the furnace body of which consisted of pure sintered cones, at a furnace temperature between 500 and 550 0 C 2V treated with hydrogen fluoride for 2 hours. The uranium in the mixture used was quantitatively converted to UO 2 F 2 . The reaction material was obtained in powder form. The subsequent volatilization of the uranium as uranium hexafluoride took place in the same plant by reacting with elemental fluorine for an hour. The uranium yield was greater than 99.5%.
Claims (1)
Priority Applications (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19671592129 DE1592129C (en) | 1967-12-21 | 1967-12-21 | Process for the reprocessing of nuclear fuel elements |
FR1596241D FR1596241A (en) | 1967-12-21 | 1968-12-20 | |
GB1226198D GB1226198A (en) | 1967-12-21 | 1968-12-20 |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19671592129 DE1592129C (en) | 1967-12-21 | 1967-12-21 | Process for the reprocessing of nuclear fuel elements |
DEK0064276 | 1967-12-21 |
Publications (3)
Publication Number | Publication Date |
---|---|
DE1592129A1 DE1592129A1 (en) | 1972-03-09 |
DE1592129B2 true DE1592129B2 (en) | 1972-08-24 |
DE1592129C DE1592129C (en) | 1973-03-22 |
Family
ID=
Also Published As
Publication number | Publication date |
---|---|
DE1592129A1 (en) | 1972-03-09 |
GB1226198A (en) | 1971-03-24 |
FR1596241A (en) | 1970-06-15 |
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Legal Events
Date | Code | Title | Description |
---|---|---|---|
C3 | Grant after two publication steps (3rd publication) | ||
E77 | Valid patent as to the heymanns-index 1977 | ||
8339 | Ceased/non-payment of the annual fee |