1 Bil l 1 i w l l | i v ..u.. .<1.t>.s\ :l lil '1 ‘it .1 l iii ti 1: ii ii ti ii i Liquid Metal Fuel Reactors By K. r. A|der* The advantages and disadvantages of a liquid metal fuel reactor system are outlined In relation to other possible power reactors. Liquid metals which are possible fuel carriers and coolants are discussed, and in particular o comparison is drawn between a solution-type fuel using bismuth and a dispersion-type using sodium. The reasons for the choice of a sodium dispersion fuel for the A.A..E.C. research project are presented and the problems posed by such a reactor system are summarised. INTRODUCTION have good heat transfer characteristics, i.e.,Present trends of development ln nuclear high specic heat and thermal conductivity, temperatures to improve thermal eiciency, and A number of liquids are available ioi hightowards more irradiation-resistant fuels to temperature operation, and inclu.de oiganicachieve increased reactor reliability and greater compounds, fused inorganic salts and liquidfuel utilisation. metals. Organic liquids such as “Dowtherm" power reactors are towards higher operating °°up1ed with 1°“ vls°°sitY- ' “High temperature» operatleu requires (diphenyl-diphenyl oxide eutectic) have accept- denition. Considering existing large-scale able heat transfer properties’ Put °n1Y a Sm?“ power reactors, it may be said that the upper utleful t°nf1Pemt‘~u'° range mdlerent ram?‘temperature llmlts ere about 300°C for pres_ tion_stab1lity. Fused salts introduce problems surised water units and 450°C‘ for gas-cooled °f mgh n§utr°n captulfe n'md"at‘.°n mstabmtyieysteme Temperatures of 5o0.C and up eeu and corrosion of contamer material. be regarded 3,5 high in nuglear 1-e3,ctQ1~5_ The heat transfer coeicients of liquid metals Operation at temperatures higher than 500°C are high, thus allowing high heat ratings per should be possible with two types of coolant— unit of. reactqr .°°r° ‘mhlme .°r' alternatively’ gases and liquid metals. The Australian Atomic pert Em“ t°f nssned magergzl mveslifid‘ d Ltqlnd Energy Commission’s research program has as me aid syilemsdneet no . pre.ssu lfse ' dglllmg its basis the study of such high temperature ‘1’g“Sld°” "an afeglm "’§§melf§;‘§gan§S1§r"- systems applied to thermal reactors. Advanced glut. meta mare st: te tgnt rbem element‘ types of gas-cooled reactors are discussed by ra‘ 13' .1? ° the e? 31 3* t $1 SDalton (1958); this paper considers the pre- Orl mm Pres Elie“ '. ey ° .n° e°%mp°s°' ferred alternatives among the possible liquid sgnxlgé or ° erwlse su er In a mac or en"metal s stems. ' y All liquid metals present some problems of Ll UID ETAL COO TS compatibility and containment when considered The neeeeelty for lluuld eeoleute to operate for reactor service, and this factor, plus theat lugh temperatures has arisen lrl many lrl_ eect of the coolant on the neutron economy stances before the advent of nuclear power. °f_ fe _"ea'ct°_r>_ °°“5t1tul'° tw° °f the mamclassical examples are the General Eleetrle criteria in deciding the metal to be used. Company's mercury boiler for increased Unfortunately, there is no one liquid metal emliiellcy Of POWEI‘ Eelleratillt dB-ting from 1922 which combines all the desirable attributes for (Hackett, 1942), and the use °f liquid sodium a reactor coolant. Consequently, some com- l3O C001 8i1‘C!‘8.fl5 exhaust valves since 1928 (Heron, prgmjse must be reached in making a selection, 1928). and other aspects of the reactor design so Ideally, a lluuld coolant for e thermal reactor affect this selection that a number of research Should have low capture cl-oss_sectl°n for prolects on nuclear reactors utilising different thermal neutrons, 9, 10w melting point, high liquid metal coolants are in progress in the boiling point, and a low vapour pressure in Western world (Williams, 1954; Siegel, 1955; , the operating temperature range. It must be H°m9J1, 1956; Abra-ha-m 1957)- compatible with constructional and container materials which it contacts in the reactor core “gum M“-Al"c°°LEDs¢l:.g LIQUH) METAL‘ and external circuit, so that negligible cor- FUELLED S Ms rosion or mass transfer of these materials Liquid {T189511 ooolants offer the opportunity will occur. It is desirable for the coolant to of operating reactors with conventional Woo have good radiation stability and a low level fuel lemellts at high temlloratllres and jlndel‘ of induced radioactivity after neutron irradia- ¢°nd1l71°1"1$ 91? high fuel I‘§1I1$- The addltlollal tion to avoid the necessity for heavy shielding stel? °f lmlxlng the fuel _1I1_l5}I1_1'at@1Y With theof elreult components external to the reactor coolant increases the possibilities of high rat- core, and to minimise health hazards should }1’18S,_ and also removes the problem of the leaks develop. Axiomatically, the coolant must ITYB-11194910“ behaV1°"1' °f fuel elements- The desire to develop reactors having high reliability and: good fuel utilisation has focused Esl;aAl)1l?;!1:rlieBg1t;.At:I!:1lgl§:?f;§yr;3:gleg:‘lls§}g-gob%§fe?;§€ attention on irradiation damage in fuels since PAGE 346 SECTION 2 iI ‘ Z. I 1. 5 ma»ourtat..~W,a i. 3‘ e 1 3 I: i 1 1i \ -i l s 5 I 1 / é/s 2?.e 1 In general, high temperature operation No low melting point alloys with high aggravates the problems of fuel element dam- uranium or plutonium contents and reasonably age, and to utilise the advantages of liquid low thermal neutron capture cross-section are metqi cooling it would be highly desirable to known. Consequently, the other attractive eliminate them altogether. A possible method liquid metal fuels are those based on low melt- " is to use fuel intimately -mixed with the ing point metals with good heat transfer and ' coolant so that mechanical irradiation damage nuclear properties. Liquid uranium and ~x_»1¥_“_ 553““ago I lug_°___§____;§n_“__mm_z I _ga___a§I’ 7'3:8 I$6 2g_2_sU “gsB_U§¢_5°885%__§____P‘__63$ gag_:O>E__Qm _ 8 VJI IO2_p_8__:N2E _ ~____M__3zDN _9§_E2cg2_Q_§_:2I _ g__U=§_uf“____w82gag‘E255g2§_____o°§_ U_ 2~_____3gu “SEgag:03?5%_§g_°6°" __ GB_Q_%____w>_a8255asU3:gE;£__gg ;__g___&g_o l _~Oid“GOU#305“ I} MW __“gas“B2rm;2_P8“8_$3_56°?E;I E303335 :____’sags$2 QQE35¢_o°8eEaas2_:___8g'2E;E;_ EEED25805$39%S05%3TooO330° a_=____§§__O€$_$Eo50°_____8M=8g_O__3__8T50_I8wso3Ogsm“E8 5QBH83;UEEOU _=_B___Ow__358g__sEO________:_8Q8“GO”_:_83;_%H0§anion50mM5632 LM‘_m_<'_ \N ’_'AV(‘vg 2;2‘(P)k +k‘ IH»/>>1t (Kv1mv__J__V2‘$IX~U$_‘V(} I’LV IV,‘VJYV)’/‘lP,WnAVjV“Wm:h;_W_m;_\~vv__v\VC1_v:_‘_r"(!¥:L ')_)_\)I\71>_'_~L _‘>Y1_1QAl,‘»\HwyS>_k_;__‘i____/IQ_§__‘__~(U’g_kvk.;v_"lW_k__[&<4TI_‘V_) 'My_z H__ V7‘KJ’ky ‘i§%Jv‘§_;vg_’“Q9‘dz_‘1‘‘ 'g:‘.’§~?Z‘T€\;¥i~ ' i, l r 6 i»e..<.».,,.>.-,.lh..<.s4»-V<§7V4 '5 ,,._..’-.- .~<»\¢wl v<<*\/~'4v&'*"v‘1-y» -.......l.,, 2 3 -u 5 w 1 1 solubility of plutonium will not be considered is a slurr in which the dis rfurther, because supplies of this element are negligible solubility in the liquid? iidlgilifrfnot likely to be available in Australia in the perature gradient mass transfer and consequentnear future. Also, plutonium fuelled systems particle growth is also negligible. Such slurrieshave lower possibilities in conversion factor, could be based on any of the preferred liquidwhich is likely to affect their economy adversely. metal cooiants, and could contain insoluble The thermal neutron capture cross-section ‘uanlun? °°mp°“nds such 9'?‘ T.Jo=' U0 °r U361»oi lithium is so unfavourable that this metal or uranium metal where this is insoluble. Againwould have to exhibit outstanding advantages bismuth appears most attractive because of itsin other properties to make it attractive for fa'v°umb1e °r°Ss's?°t1°n'.but m°st °f the p'°b'thermal l-eaetem Similar reasoning applies lems associated with this metal are with con- to lead, its cross-section being much lower Fame!‘ matenam am.‘ lf these can be S°1Ved=than that of lithium, but still high compared "‘ “PPe‘“$ m°‘° 1°g1°a1 t° use bismuth as 3with bismuth In both eases these elements solution type fuel rather than in a. slurry. It occur in nature as mixtures of isotopes with remams' then‘ t° °°ns1d?' .Wh=ih°1" 9‘ slurrywidely diering nuclear properties, and an in- formed “nth any other hqmd 11.18"‘ has Sui‘teresting possibility is the use of the low cent advantages to compete with a bismuth capture cross-section isotopes lithium '7 and S°l“t‘°n' lead 208 as reactor coolants. Present isotope $°dil-1m and DOW-Ssium have negligible $01\1-separation processes are not likely to produce bility T01‘ uranium, and 11611138 0011161 be used aslead 208 economically, but the greater ease of slurry vehicles for the metal or its compounds.isotope separation with light elements may mean P099-Ssillm has Door nuclear D1‘0P61‘¢ie$, and isthat lithium '1 is a feasible coolant in the more diiwli to contain than sodium, and itsfuture, only advantage appears to be a lower melt- » Both lead and lithium dissolve many other i1l{lgKp°im' Alloys of potassium and sodiumeeal an S . .. ( a ) have been used (Trocki, 1955) as reactor w‘?h°°J3>§€‘.‘i§23"m§&ii.1§?“$%“‘l’l§§Z fgggngii ,i;;m.m,beinihadd@i todiculties appear not insuperable (Homan, 6 me g pom ° e coo an‘ 1955, 1956). However, bismuth also exhibits T," *1?em_1a1 n°11'¢r°11 capture cross-seqon ofslight solubility for many other metals, and it s°dmm '5 hlgh compared, w1_7h that °f b1sm“th~should he emphasised that the magnitude oi but reference to_'I'able I indicates that the heatthe_eon.osi°h problems in the use Oi this metal transfer properties of sodium are much better was not apparent from a study of its properties, than th°$e °f Plsmuu?‘ Th“ m"?9‘ns that lessbut emerged as a result of a considerable re~ S°di",m °°°1a'nt 15 requlred for 3' g1Yen heat Wt‘Search program (Weeks. l955)_ put, l.e., the poor nuclear properties of sodium are partly offset by its good thermal properties.Liquid fuels of higher uranium content may In an insoluble sliu-ry type fuel, the fissilebe made by adding amounts of ssile material material concentration is not dependent on aexceeding the saturation solubility in bismuth metallurgical property of the coolant. A-liquid,and lead. In both cases uranium forms an in- metal fuel could be made, based on sodium andtermetallic compound with the coolant (U'Bi,, containing uranium, in which the neutron lossesUPb,) and the result is a slurry of the relevant to the coolant would be no greater than in acompound in equilibrium with liquid metal bismuth solution fuel, and in which a similarslilgtioniil The solnbiliitly of li.lli:,nium in lite liquid fuel rating could be achieved.p se creases rapi wi rise of m era- ture in both systems, gnd this causes dillculty COMPAMSON BETWEEN MSMUTH ANDwhen the slurry ows in a circuit of varying SODWM A5 FUEL CARRERS :1ei‘!1€)8I'8,l2i;l1‘8S. as woulélmocicur insa. iieactortaiid Metallurgical aspectsea exc anger com a ion. ma par ices - -dissolve preferentially in the hot region be- se§,c§°§;‘1e”§§éf,a§§§§§,fi"§° ntfigalggflgfgiln rsiicause of their greater surface to volume ratio, nding suitable container materials for a his_ and P1'e°iPita'ti°n in the °°ld regmn tends to muth-uranium fuel solution Workers at Brook-occur °n the remaining °°arse Pa1'ti°1°S- The haven National Laboratory.(Weeks 1955) haveresult is particle growth to such an extent that shown that the most promising ’end readily dep°Sm°n and eventual bmcking (“Plugging”) available constructional materials for bismuthof the circuit occur. Any system containing circuits are steels containing 25 — 5 per centparticles in equilibrium with a solution is prone chromium and some molyhdeiium hut low iii to this eecti which is 3' case °f “tempemture nickel and carbon However the eyxtent of cor-gradient ma-SS transfer.” For example, the rosion and mass‘ transfer in these materialssyst°m’th°rmm“bi$muth has been mvestigated has led to investigation of corrosion-inhibitingfor possible use as a neutron absorbing blanket additives in the bismuth Additions of mag_for thermal reactors, but the thorium content hesium as a deoxideht end zirconium as an required is such that 9- slurry °f ThBi= in bis‘ inhibitor have been found benecial and themuth is ne°e55ary- The alloy systems th°ri“m' mechanism of inhibition has been proved to bebismuth and umni“m'bismuth are Very snmlar» the formation of a lm of zirconium nitride onand particle growth of the ThBi, is p1’°‘/3118 the surface of the steel the nitrogen being an:i.Bsei‘ious problem in such a blanket design inherent impurity in all steels. Horsley, work-ar on, 1957). ing at. Harwell, has shown that deliberate ad-The "nal alternative for a liquid metal fuel dition of further nitrogen to the steel prolongs POWER REACTORS PAGE 349 i. , él i r 1 1 oo'_».,s.1¢.-.-e.v~* ‘!..*Lv¢1°P¢d- Thus, on the basis Of <=<>m- theoretically by Dalton and Thompson (1957)Patibmty with °°ntain°1'5' s°di“m has distinct who concluded that short-term variations ofadvantages °"e1' bismuth fuel concentration by more than 2 per cent.Engineering “necks in the circulating ‘fuel/coolant would have ...s:e:>s.oi»_ [vi i .3: .. 5 . '2 ,,-\§¢§A:gL"_4'\!!4>LI"77'~4‘l1*‘P‘\“,“l§"‘ ¢l’:?_€\'!.Q is .2:_wK".?4<~‘ w$ Not all of the many possible combinations of I of oxidation of reactive metals in sodium will be fuel, moderator, and container maieriais have i studied by chemists and metallurgists as part of been dismissed, but the aim has been to imii. ”*‘* I the Austmllan P1'°Je°t- cate the main reasoning behind the current Z” . research programme, and the nature of theIn the case of a liquid metal fuel containing . - ne particles, neither of these systems can be problems Involved‘ . a°1°Pted1 because b°th depend 5°!‘ 1’em°"a1 °f Sufficient design calculations have been done “~ °xYgen °n a 1°W‘Ve1°citY 1'ea°ti°n Vessel» which to indicate that the sodium-based system is a would allow settling of the fuel. A third alter- promising one if the iecimoiogicai pi-0b1em5 min native is tn‘? use °f _a' sQ1u'°1e “gettelm in Fhe be solved. Design of a liquid metal fuel reactor sodium, of which calcium is the most promiS1l1g- experiment must await satisfactory completion é P1'e1in_1ina1'Y Wm‘? mdi_°3'te$_ that ¢°1'1'°$i°¥1 °f of compatibility and uid ow studies. which beryllium metal m sodium 15 reduced ¢0nS1de1'- involve considerable metallurgical, chemical, and ably by the presence of calcium (Bett, 1958). engineering efiom However, calcium and nickel interact, and the effect of calcium additions on nickel-bearing stainless steels is being studied. Initial results REFERENQ5 indicate that the quantity of calcium required ABRAHAM’ B_ M" FLOTow_ H_ E_ and CARLSON‘ £01’ ‘g9tte1'ing" has negligible eectfl on 13/8/1 R. D. (1957).—Second Nuclear Engineering and stainless steel (Bett, 1958)_ Science Conference, Philadelphia, March, 1957. Rt» .a- ,;_£ _, _ , A.E.C.L. REPORT ORR-590, Catalogue of Nuclear * The use of UBe,,, as fuel addition may provide Reactors. * a!1°'1hel‘ method Of Oxygen 0°lltl‘01- Fission Of BALL J. G., (1955).—J. Inst. Met., London, a4, 229. umnium at°"{*$ in the °°mP°“_nd_ Panicles will BAR'1:ON, P. .1., and GREENWOOD, G. w., (1957).- ; E release beiylllum atoms, and it is hoped that AERE M/R,2310, in the higher chemical activity of this beryllium BERGLIN, Q ;,_ w_,_-(195-7)_ Private commimi¢,,__ ~ 3 compared with the moderator material will re- tlon. sult in continuous “gettering" of oxygen with BETT, F. L., and DRAYCOTT, A., (1958).--Private lliil.-u; ,. out appreciable corrosion of the moderator. This ¢°mm11Ill¢&';l°n- ~ hypothesis will be evaluated by irradiation ex- CAIRNS, R. 0., (1957).—Prlvate communication. periments in HIFAR. DALTON, G. 0. J., (1957). Private communication. T In addition to the problems of oxygen im- DALTON, G. c. J., (1953). Proceedings of this Ti purity, ssion products_ released within the sYmP°s1“m- 1 r sodium may cause corrosion and mass transfer D“;YER- °- E--1§'=66'f11-» (1955)-— ’°°- “ - °“ - ~ l . - En 955 vol 9 .. I . Th " ' ' 'it ;. 9f moderator and mrcuit- matfrims k -e fiyfem FISHER, R. w., and wmonns, G. R., (l956).—- ; .. ' : Y , v,;7~;.. M. t» is so complex that experlmen a wor , in u ing Am L b t Iowa state C°"ege_ Contact ~ irradiation tests, will provide the only real guide. w -§’fo5_ Hg“ $7 its It may be seen m general that a °P“$1d°'?b1e GRISON, E., (C.E.A., France), (1956).--Private com- amount of metallurgical research is required munlgatign, before the fuel-coolant, moderator. and con- HACKETT, M_ N_ (1942)___.'1‘i-gn5_ Am Soc, Mech If structional materials for a reactor can be Eng1's.,64i64'1. ' 2 dened. HERON, s. D., (1928).—U.S. Patent 1610965. , HICKMAN, B. s., (1958).-—Private communication. 5 - SUMMARY oiioiiglgiiin, E. E. and MANLY. W. n., (1956).- fj The reasons for the choice of a sodium-based HOFFMAN, E. E. and MANLY, W. Di. $11955).- L 1 liquid metal fuel system as a high temperature lfgléglear Ens 8v Science Congress. Cleve an , ec., * ‘z reactor study in Australia may be summarised P . as f°11°w$=- AERE M/Bis-la. ' HORSLEY G. W. and MASKREY. J. T.. (l957).—— : (1) A liquid metal fuel system has potential x::i.i.Y. J. w., (1958).—'1‘he Prep-l'ati0i:l of mic 1"'?i; - - ' - uranium powder by the hydride process. Proceed § l advantages in high fuel rating, high lugs of this symposium. I’ bl-l1'!1'11Pl and high tempera-t“1'e operation’ MOGARD, H, (1955)-Observations on the corro-t l A the latter leading t0 high thermal slon or uraniuin in liquid sodium. Proc. Int. Cont. K » emciency. At. En-. 1955. vol. 9. P5118- . POWER REACTOR5 PAGE 353 r~ > 1:ti».,,;.. qr. , gm », P» 1 4 c’;.;i»’>‘",.~ , I-1; . . in ~;.;:~+» 1» 3' / n f M ‘ ea*:;.)4.um¥- SIEGEL, S., CARTER, R. L., BOWMAN, F. E., HAY- THE METAL BERYLLIUM, (1956). —— AmericanW, »' WARD, B. R., (1955).--Basic Technology or the Society for Metals. > Sodium Graphite Reactor. Proceedings of Geneva Conf., 1955, Vol. 9, P.a21. TROCKI, '12, et a1.,_ (1955).—S0dium and potassium alloy tor reactor cooling and steam generation. Prue. TAYLOR, J. w., FORD, s. 1)., (1955).—Solid Metal Int <1<>11f- Ah En-- 1955, V°1- 9, P241-—Liquid Metal interaction studies, Part II, Contact U.s.A.E.C., (1955). — Liquid Metals Handbook.§It;1g%l:i72I;e1atlonships for Sodium on Solids. AERE sodium-NQK Supp1ement_ U.S.A.E.C., (1955).—The Reactor Handbook. V01. ‘ .= TEITEL, R. J., (1952).—The Uranium-Lead System. 2, Engineering» A-E-C-11 3646~ . ~ I?,, \ 9.? iv ~\ ~ > 1* e ;<§1'<§’ kg» r 7 N J!'- Metals 4- 4. 397, API11, 1952- WEEKS, J. R., et a1., (1955).—Corrosion problemsFROST. B. Rh T" MASKSEYI J_ T" (1952)___The with bismuth uranium fuels. Proc. Int. Cont. At. System Uranium-Lead. AERE M/R.1027. f§"J§f;5'1;§§§'_ 9' P341‘ (see M“ N“°1°°m°s 12' 7' TEITEL, R. J., GURINSKY, D. H., and BRYNER, WILLIAMS, C. and MILES, F. L., (1954).—L1q'nid s_ J_, (1954).-Liquid Metal Fuels and Breeder Blan- Metal Fuel Reactor Systems for Power. Nucleonicl kets. Nucleonics 12, '7, 14, July, 1954. 12, 7, 11. 1 ‘ire .1 1 » \ v l X 1 5;, 5?»? b , \ < W, ‘ >, "L x ,, .. e »>;_*,At! \ ’» » € I \ A- 1 ¢ 1 PX‘. ¢ ;~~ a 1 J PAGE 354 SECTION 2 ~,/ {V l 4:, ,1? r ,.1 Q1 A; 7~<