The CNRS Research Program on the Thorium cycle ... - Pacen - IN2P3
The CNRS Research Program on the Thorium cycle ... - Pacen - IN2P3 The CNRS Research Program on the Thorium cycle ... - Pacen - IN2P3
Thorium Cycle – Molten Salt Reactors June 2008 temperature of the traps decides which molecular species is caught. This technique also allows a selective desorption of UF6. Simultaneously Np and a significant fraction (~90%) of Pu are extracted as PuF6 [ORN68] and NpF6. By means of a H2 flux, UF6 NpF6, PuF6 are then reduced back to UF4, NpF3 and PuF3 which are further reintroduced into the fuel salt. A difficulty of this method lies in that fluorine as well as UF6 (and most other gaseous reaction products) are very oxidizing species with a high corrosion potential. It becomes thus necessary to protect the vessel of the chemical reactor.
Thorium Cycle – Molten Salt Reactors June 2008 Stage 2.b in Fig.9.
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<strong>Thorium</strong> Cycle – Molten Salt Reactors June 2008<br />
temperature of <strong>the</strong> traps decides which molecular species is caught. This technique also allows a<br />
selective desorpti<strong>on</strong> of UF6. Simultaneously Np and a significant fracti<strong>on</strong> (~90%) of Pu are extracted<br />
as PuF6 [ORN68] and NpF6. By means of a H2 flux, UF6 NpF6, PuF6 are <strong>the</strong>n reduced back to UF4,<br />
NpF3 and PuF3 which are fur<strong>the</strong>r reintroduced into <strong>the</strong> fuel salt.<br />
A difficulty of this method lies in that fluorine as well as UF6 (and most o<strong>the</strong>r gaseous reacti<strong>on</strong><br />
products) are very oxidizing species with a high corrosi<strong>on</strong> potential. It becomes thus necessary to<br />
protect <strong>the</strong> vessel of <strong>the</strong> chemical reactor. <str<strong>on</strong>g>The</str<strong>on</strong>g> comm<strong>on</strong>ly used technique is that of <strong>the</strong> “frozen salt<br />
wall” [ORN66] in which <strong>the</strong> outside of <strong>the</strong> tank is cooled so as to generate an inside protective layer of<br />
crystallized salt with a width of approximately 1.5-2cm. <str<strong>on</strong>g>The</str<strong>on</strong>g> exo<strong>the</strong>rmic fluorinati<strong>on</strong> reacti<strong>on</strong> takes<br />
place in <strong>the</strong> middle of <strong>the</strong> column. This technique is already used by AREVA at an industrial level.<br />
In view of <strong>the</strong> solid experience already ga<strong>the</strong>red at ORNL giving str<strong>on</strong>g evidence for <strong>the</strong><br />
practicality and efficacy of <strong>the</strong> fluorinati<strong>on</strong> method, this stage 1 is not presently <strong>the</strong> subject of extensive<br />
studies by <str<strong>on</strong>g>CNRS</str<strong>on</strong>g> groups.<br />
V.B.2.b Stage 2 : Selective extracti<strong>on</strong> of remaining actinide and lanthanides<br />
As part of <strong>the</strong> GEN-IV strategy towards sustainable nuclear energy, TMSR-NM is also designed<br />
to burn fissile or fertile elements resulting from capture-decay processes inside <strong>the</strong> reactor. Thus <strong>the</strong><br />
salt processing should be able to extract all actinides in order to inject <strong>the</strong>m back into <strong>the</strong> reactor and<br />
simultaneously make sure <strong>the</strong>y d<strong>on</strong>’t enter <strong>the</strong> operati<strong>on</strong> waste stream. We have seen that fluorinati<strong>on</strong><br />
is effective <strong>on</strong> U and Np and has a partial (~90%) efficiency regarding Pu extracti<strong>on</strong>. <str<strong>on</strong>g>The</str<strong>on</strong>g> extracti<strong>on</strong> of<br />
<strong>the</strong> remaining Pu and <strong>the</strong> heavier elements such as Am remains to be d<strong>on</strong>e. In additi<strong>on</strong> within <strong>the</strong> Th-<br />
U <strong>cycle</strong> itself, a decisi<strong>on</strong> has to be taken regarding <strong>the</strong> relatively l<strong>on</strong>g-lived (27d) 233 Pa which ultimately<br />
will decay into 233 U. Whe<strong>the</strong>r it should be separated specifically or whe<strong>the</strong>r some waiting period will be<br />
imposed before effecting a sec<strong>on</strong>d fluorinati<strong>on</strong> (waiting period which will also influence o<strong>the</strong>r decays)<br />
will have to be decided when scientific informati<strong>on</strong> will be of sufficient quality.<br />
<str<strong>on</strong>g>The</str<strong>on</strong>g> <str<strong>on</strong>g>CNRS</str<strong>on</strong>g> teams have analyzed two opti<strong>on</strong>s to separate FPs such as lanthanides and alkaline<br />
earths: electrolysis and/or reducing extracti<strong>on</strong>. <str<strong>on</strong>g>The</str<strong>on</strong>g> experiments explore <strong>the</strong> electro-chemical<br />
behaviour of a LiF-ThF4 salt at 600°C in presence of lanthanides (we recall that safety c<strong>on</strong>straints<br />
have led us to avoid <strong>the</strong> BeF2 used in <strong>the</strong> MSBR c<strong>on</strong>cept). <str<strong>on</strong>g>The</str<strong>on</strong>g> electro-activity domain of this salt is<br />
ra<strong>the</strong>r extended as a c<strong>on</strong>sequence of <strong>the</strong> str<strong>on</strong>g solvatati<strong>on</strong> of ThF4 by free fluorides (see left part of<br />
Fig. 11) [DPI07, DSS08]. As far as extracti<strong>on</strong> <strong>on</strong> an inert electrode is c<strong>on</strong>cerned, this stability<br />
translates in a potential increase by about 260mV which allows <strong>the</strong> extracti<strong>on</strong> of Nd.<br />
Fig. 11 Comparis<strong>on</strong> between several redox potentials <strong>on</strong> a inert electrode (left) and <strong>on</strong> a liquid<br />
bismuth electrode (right). <str<strong>on</strong>g>The</str<strong>on</strong>g> figures also give <strong>the</strong> electro-activity domain in LiF-ThF4 at 600°C. (<strong>the</strong><br />
calculati<strong>on</strong>s are performed with <strong>the</strong> software HSC Chemistry versi<strong>on</strong> 4.1).<br />
<str<strong>on</strong>g>The</str<strong>on</strong>g> scheme adopted as reference for <strong>the</strong> Stage 2 is shown in Fig.12.<br />
An analysis of <strong>the</strong> performance of reducing extracti<strong>on</strong> in presence of a metal (Bi-Th) has led us<br />
to select this method for <strong>the</strong> reference scheme. It is indicated by <strong>the</strong> boxes labelled Stage 2.a and<br />
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