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Effect of Additives Nb2O5 and Cr2O3 on Creep of UO2

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Q/1'+&9" 1'(+9,+6(R" 09&1'" 21U+2!" B+61,(+B" 1'" ]10P" #3P" " Y(" 12" 2++'" (-&(" (-+" 09&1'" 21U+" 2(+&B1/G" 1',9+&2+" A1(-" LMCK>",.',+'(9&(1.'"%'(1/"1("/+F+/2".JJ"&("&",.',+'(9&(1.'".J"&M.%("HP>")./T"(."">"@H"p)P""3("-10-"2(9+22+2"

(5)

B12/.,&(1.'<,.'(9.//+B",9++6P"3("/.A+9"2(9+22+2"Q/6=H"D8&R!"&"9.%0-/G"/1'+&9"B+6+'B+',+".'"2(9+22!"(G61,&/" .J" B1JJ%21.'" ,9++6" A&2" .M2+9F+BP" 32" '.(+B" 1'" Q7&AM91B0+" +(" &/P" #X?#R!" 1(" 12" (-+" /.A+9" 2(9+22" 9+01.'2!" (G61J1+B" MG" &" /1'+&9" 2(9+22" B+6+'B+',+" .J" ,9++6" 9&(+!" 1'" A-1,-" (-+" ).2(" 69.)1'+'(" ,9++6" ).B+2" .,,%9" B%91'0"'.9)&/"9+&,(.9".6+9&(1'0",.'B1(1.'2P"

"

" " 9" " " " " N"

0 0.002 0.004 0.006 0.008 0.01

5 10 15 20 25 30 35 40 45 50 [Nb

2O5]

Mean grain size (

µ

m)

Measured Interpolated

""""""""

0 0.002 0.004 0.006 0.008 0.01

10−10 10−9 10−8 10−7 10−6 10−5 10−4 [Nb

2O5] Creep rate (1/s) Measured

Calculated Calculated, dg=15 µm

Calculated, dg=30 µm

" "

]10%9+"#P""Q9R"D+&2%9+B"09&1'"21U+"F+92%2"LMCK>")./+"J9&,(1.'".J"5KC"B.6+B"1'"2&)6/+2"(+2(+B"MG"

7&AM91B0+"+("&/P"Q#X?#RP"QNR"D+&2%9+B",9++6"9&(+2"Q7&AM91B0+"+("&/P"#X?#R"F+92%2",&/,%/&(+B"F&/%+2"Q-+9+R" &2"&"J%',(1.'".J"LMCK>")./+"J9&,(1.'"1'"5KC"&("&'"&66/1+B"2(9+22".J"CH"D8&"&("#>C@"^P""*-+"B&2-+B"&'B"

B&2-<B.(",%9F+2"2-.A",.)6%(&(1.'2")&B+"&(",.'2(&'("09&1'"21U+2P"" "

7&AM91B0+"+("&/P"Q#X?#R"%2+B"(-+"L&M&99.<O+991'0",9++6"J.9)%/&"A1(-"/&((1,+"B1JJ%21F1(G!"&2"1'";`P"Q>&R!"(." +F&/%&(+" (-+19" +S6+91)+'(&/" B&(&P" O.A+F+9!" (-+G" B." '.(" 69.F1B+" '%)+91,&/" F&/%+2" J.9" (-+" J.9)&(1.'" +'+901+2" .J" (-+" B+J+,(2" '.9" 26+,1JG" (-+" /&((1,+" B1JJ%21F1(G" .J" %9&'1%)" F&,&',1+2P" a1:+A12+!" (-+G" B." '.(" +S6/1,1(/G"01F+"(-+"J%//"+S69+221.'"J.9"e5vd!"A-1,-"(-+G"-&F+"2%66.2+B/G"%(1/1U+BP"71',+"7&AM91B0+"+("&/Pq2"

A.9:".JJ+92"&"2%1(&M/+"M+',-)&9:"J.9"(-+").B+/"%2+B"-+9+!"A+"J.%'B"1(2"9+&669&12&/"`%1(+"A.9(-A-1/+P" "

c+" -&F+" %2+B" ;`2P" Q>&R!" QIR<Q=R" (." 9+(9.B1,(" (-+" ,9++6" 9&(+" &2" &" J%',(1.'" .J" LMCK>",.',+'(9&(1.'" &'B"

(+)6+9&(%9+P"L.(+"(-&("21',+" u L o

L D

D .. "(-+'" m uv Uve5vd

L u L

L D D D

D > A " !"&'B"DUv"12"26+,1J1+B"1'"*&M/+"C" QD&(U:+" #XIIRP" *-+" U+9." B.6&'(" ,.',+'(9&(1.'" /1)1(" J.9" e5vdA5vQH!TR" &(" #>C@" ^" 12"

#H C

@b #P#?C #H

$ 2 " K K !"A-1,-"'++B2"(."M+"&,,.%'(+B"J.9"MG"2,&/1'0"(-+"/&((1,+"B1JJ%21F1(GP"D.9+"+S6/1,1(/G" " " R ! H Q 5 R ! Q 5 R Q R ! Q T T y T D T y D v v Uv uv

L " !" Q?R"

"

A-+9+" y" 12" (-+" B.6&'(" ,.',+'(9&(1.'P" ]%9(-+9).9+!" 1'" .%9" ,.)6%(&(1.'2" J.9" LMCK>!" A+" ,-..2+" #[C

P >

"

A

C 1'";`P"QIR"&'B"&22%)+"&'"1'1(1&/"1)6%91(G"/+F+/".J":14234$8")./+"J9&,(1.'P"*-+"9+2%/(2".J".%9" ,.)6%(&(1.'2" (.0+(-+9" A1(-" )+&2%9+)+'(2" &9+" B+61,(+B" 1'" ]10P" #4P" Y(" 12" 2++'" J9.)" (-12" J10%9+" (-&(" (-+" ,&/,%/&(+B",9++6"9&(+2"J.//.A"(-+"(9+'B".J")+&2%9+)+'(2"A1(-"&'".F+9+2(1)&(1.'"&("HPH#")./+"J9&,(1.'".J" LMCK>P"L+F+9(-+/+22!".%9"9+2%/(2"&9+",.)6&9&M/+"(.!"M%("'.("(-+"2&)+"&2"(-.2+"9+6.9(+B"MG"7&AM91B0+"+("&/P"

Q#X?#RP""Y'"]10P"#4"J.9"(-+"2&:+".J",.)6&912.'!"A+"-&F+"&/2."6/.((+B"(-+"9+2%/(2".J",&/,%/&(1.'2",&991+B".%(" A1(-",.'2(&'("09&1'"21U+2".J"#>"p)"&'B"@H"p)P"

(6)

Creep of UO2 doped with Cr2O3" "

7G2(+)&(1," -10-<(+)6+9&(%9+" ,9++6" 9&(+" )+&2%9+)+'(2" &2" &" J%',(1.'" (+)6+9&(%9+" &'B" &66/1+B" 2(9+22" .'" B.6+B"5KC!"1'"6&9(1,%/&9"A1(-"N9CK@"&BB1(1F+!"&9+"F+9G"9&9+"1'"(-+".6+'"/1(+9&(%9+!"B+261(+"1(2"&66/1,&(1.'2"1'"

,.))+9,1&/"9+&,(.9"J%+/P"*-+9+"12!"-.A+F+9!"&"#XXI"+S6+91)+'(&/"2(%BG"MG"V%0&G"+("&/P"Q#XXIR".'",9++6".J" 5KC<N9CK@",.)6.%'BP"Y'").9+"B+(&1/!"(-+19",9++6"(+2(2"A+9+"B.'+"MG",.)69+221.'"%'B+9"&90.'".9"9+B%,1'0"

Q-GB9.0+'&(+B" &90.'R" )1/1+%" &(" B1JJ+9+'(" (+)6+9&(%9+2" #IC@<#XC@" ^" .'" %'199&B1&(+B" 26+,1)+'2P" *-+" )+&2%9+)+'(2" .J" ,9++6" 9&(+" A+9+" B.'+" %'B+9" &" ,.'2(&'(" (+)6+9&(%9+" &(" 2(9+22+2" F&9G1'0" J9.)" CH" (." =H" D8&P"*-+"N9CK@",.',+'(9&(1.'2".J"5KC"26+,1)+'2"A+9+"eHPH!"HPHC>!"HPHI!"HP#!"HPCd"A(TP"*-+"09&1'"21U+"&2"

&"J%',(1.'".J"N9CK@"1'")./+"J9&,(1.'"J.9"(-+"26+,1)+'2"12"B+61,(+B"1'"]10P"C3P"3BB1(1.'".J"N9CK@"2(9.'0/G"

1',9+&2+2"(-+",9++6"9&(+"9+/&(1F+"(."(-&(".J"6%9+"5KC"1'"&90.'"&().26-+9+P"

"

" " 9" " " " " N"

0 1 2 3 4

x 10−3 0 10 20 30 40 50 60 70 80

[Cr2O3]

Grain size (

µ

m)

Measured Interpolated

""""""""

0 1 2 3 4

x 10−3 10−10 10−9 10−8 10−7 10−6 10−5

[Cr2O3]

Creep rate (1/s)

T = 1573 K T = 1673 K T = 1773 K

" "

]10%9+"CP"Q9R"D+&2%9+B"09&1'"21U+"F+92%2"N9CK@")./+"J9&,(1.'".J"5KC"B.6+B"1'"2&)6/+2"QV%0&G"+("&/P"

#XXIRP"QNR"D+&2%9+B",9++6"9&(+2"QV%0&G"+("&/P"#XXIR"F+92%2",&/,%/&(+B"F&/%+2"-+9+"Q_R"&2"&"J%',(1.'".J"

N9CK@")./+"J9&,(1.'"1'"5KC"&("&'"&66/1+B"2(9+22".J"[>"D8&"&("B1JJ+9+'("(+)6+9&(%9+2P""

" "

O+9+!" A+" &22%)+" (-&(" B1JJ%21F+" ,9++6" 12" 0.F+9'+B" MG" (-+" B1JJ%21.'" .J" %9&'1%)" 1'(+92(1(1&/2" &'B" .SG0+'" F&,&',1+2!"1P+P"A+"-&F+"%2+B";`2P"Q>MR<Q>,R"&'B"QIR<Q=R"(."9+(9.B1,("(-+",9++6"9&(+"&2"&"J%',(1.'".J""N9CK@"

)./+"J9&,(1.'"&'B"(+)6+9&(%9+P""O.A+F+9!"21',+"(-+" ,&(1.'"B1JJ%21F1(G"12")%,-"/.A+9"(-&'"(-&(".J"&'1.'!" .'/G"(-+"J.9)+9"A1//",.'(9./"B1JJ%21.'</1)1(+B"B+J.9)&(1.'!"1P+P" u

L o

L D

D .. "(-+'" m Uie5id

ui L u L

L D D D

D > A " !"

&'B"DUi"12"26+,1J1+B"1'"*&M/+"C"Qa1B1&9B"#XIIRP""*-+"U+9."B.6&'(",.',+'(9&(1.'"/1)1(2"e5idA5iQH!TR"&("

(-+",.'21B+9+B"(+)6+9&(%9+2"'++B"(."M+"&,,.%'(+B"J.9"MG"2,&/1'0"(-+"/&((1,+"B1JJ%21F1(G"&2"M+J.9+" " " R ! H Q 5 R ! Q 5 R Q R ! Q T T y T D T y D i i Ui ui

L " P" QXR"

"

O+9+!" A+" -&F+" 2+/+,(+B" (-.2+" B&(&" J9.)" QV%0%&G" +(" &/P" #XXIR" (-&(" 2++)" (." M+" ).9+" &66/1,&M/+" (." %9&'1%)b.SG0+'" 2+/J<B1JJ%21.'!" 1P+P!" (-.2+" &(" (+)6+9&(%9+2" #>=@" (." #==@" ^" &'B";a "[>" D8&P" *." 0+(" &"

0..B"J1(".J";`P"QIR"(."+S6+91)+'(&/"B&(&"&("(-+"B1JJ+9+'("(+)6+9&(%9+2!"A+"A+9+",.)6+//+B"(."9+&BZ%2("(-+" ,9++6" J&,(.9"CA&,,.9B1'0/GP"*-&(" 12!" A+" %2+B"CA"@>!"CA"#>H" &'B"CA"[HH" &("T"#>=@!"T "#I=@"

&'B"T "#==@" ^!" 9+26+,(1F+/GP" ]%9(-+9).9+!" (." B&)6+'" (-+" ,.)6%(+B" F&/%+" .J" (-+" %9&'1%)" 1'(+92(1(1&/" ,.',+'(9&(1.'" &(" (-+" F+9G" /.A" B.6&'(" ,.',+'(9&(1.'!" &2" M+J.9+!" A+" &22%)+B" &'" 1'1(1&/" 1)6%91(G" /+F+/" .J"

(7)

"

*-+"9+2%/(2".J".%9").B+/",.)6%(&(1.'2"&9+"69+2+'(+B"1'"]10P"C4!"A-1,-",.)6&9+2"(-+")+&2%9+B",9++6"9&(+" F&/%+2"&0&1'2("(-+",&/,%/&(+B".'+2P""N.'21B+91'0"(-+"%',+9(&1'(G"1'"(-+")+&2%9+)+'(2"Q%6"(."&M.%("!#?TR!" (-+"9+(9.B1,(1.'2"&9+"J&19/G"0..BP"*-+")+&2%9+B"B&(&"B+61,(+B"1'"]10P"#4"&9+"(-+"9+2%/(2".J"B19+,("J1("(."(-+" 9&A"B&(&"&2"01F+'"1'"QV%0%&G"+("&/P"#XXIRP"

" "

?A!D3!!AEG)

"

Frenkel defect formation energy

"

3" :+G" 6&9&)+(+9" 1'" (-+" 6%(&(1F+" ).B+/" 12" (-+" J.9)&(1.'" +'+90G" .9" +'(-&/6G" .J" (-+" .SG0+'" 6&19" ]9+':+/" B+J+,(2" HF!" -+9+" B+'.(+B" MGE#\" 2++" *&M/+" #P" *." 1//%2(9&(+" (-12!" A+" -&F+" 6/.((+B" (-+" ,&/,%/&(+B" ,.',+'(9&(1.'".J"(-+"%9&'1%)"F&,&',G"&2"&"J%',(1.'".J"B.6&'("QDCK>"A"LMCK>R",.',+'(9&(1.'"1'"]10P"@3P"Y("

12"2++'"(-&("&"F&91&(1.'".J"@BE#B["+f")&:+2"&"/&90+"1)6&,(".'"(-+",.',+'(9&(1.'".J"(-+"F&,&',1+2P"*-12"

1'"(%9'"210'1J1,&'(/G"&JJ+,(2"(-+"/&((1,+"B1JJ%21F1(G"&'B"(-+9+MG"(-+",9++6"9&(+".J"(-+"J%+/!"2++";`2P"Q=R<Q?RP" "

*-+" F&/%+" .J" E#AHF" Q*&M/+" #R" ,&'" M+" )+&2%9+B" J9.)" .SG0+'" B1JJ%21.'" +S6+91)+'(2" .'" '+&9/G" 2(.1,-1.)+(91," 5KC!" A-1,-" 12" F+9G" B1JJ1,%/(" (." )&1'(&1'" B%91'0" (-+" +S6+91)+'(" QD&(U:+" #X?=RP" *&M/+" #"

2-.A2" &" 2+/+,(+B" /12(" .J" F&/%+2",&/,%/&(+B"MG"F&91.%2"B+'21(G"J%',(1.'&/" (-+.9G"&669.S1)&(1.'2".9"V]*2" e+S,+6("j&,:2.'"+("&/P"Q#X?=R!"A-1,-"%2+"(-+"D.((<a1((/+(.'"&669.S1)&(1.'dP"]9.)"(-12"(&M/+!"A+"2++"(-&(" (-+"ii3"9+2%/("Q]9+G22"+("&/P" CHH>R"&09++2"A+//"A1(-"(-+"M+2("+2(1)&(+"F&/%+"9+,.))+'B+B"MG"D&(U:+!" A-+9+&2" (-+" aV3" _"U" 9+2%/(" .J" 3'B+922.'" +(" &/P" QCH##R" ,.'J.9)2" A1(-" (-+" +S6+91)+'(&//G" B+(+9)1'+B" 9+2%/(".J"^1)"&'B"K/&'B+9"Q#X?#RP"L+F+9(-+/+22" J.9HF!"(-+9+" 12"&"9&'0+".J"F&/%+2!"J9.)" @PI" (."[PX" +f!" 9+2%/(+B"J9.)"F&91.%2",.)6%(&(1.'2P"

"

Effective diffusivity

"

*-+",.'(9.//1'0")+,-&'12)"J.9"B1JJ%21.'&/",9++6"1'"5KC"12"(-+"B1JJ%21.'".J"%9&'1%)P"32",&'"M+"2++'"J9.)"

*&M/+"C!"(-+9+"12"&"/&90+"B126&91(G"M+(A++'"(-+"&,(1F&(1.'"+'(-&/61+2".J"B1JJ%21.'",.+JJ1,1+'(2"9+6.9(+B"MG" F&91.%2"&%(-.92"1'"(-+"/1(+9&(%9+P"*-+G"F&9G"J9.)"#P?"+f"QD&(U:+"#XIXR!"@PX"+f"QO&A:1'2<3/,.,:"#XI?R"(." [P="+f"Q]9.2(<32-MG"#X?CR"J.9"DUv&'B"@PH"+f"J.9"DUi"Qa1B1&9B"#XIIRP"8/.(2".J"(-+"B1JJ%21.'",.+JJ1,1+'(2" Q*&M/+"CR"F+92%2"(+)6+9&(%9+"9+F+&/"(-+19".F+9&//"B1JJ+9+',+2P"""*-+"1'(91'21,"B1JJ%21.'",.+JJ1,1+'("DUi(-&(" A+"-&F+"%(1/1U+B"J.9",9++6".J"N9CK@<B.6+B"5KC"12"/.A+9"(-&'"(-+"DUv%2+B"J.9"LMCK><B.6+B"5KC"QD&(U:+"

#XIXRP" " D.9+.F+9!" B+261(+" (-+" /&90+" B1JJ+9+',+" M+(A++'" (-+" &,(1F&(1.'" +'(-&/61+2" J.9"DUv.M(&1'+B" MG" D&(U:+" Q#XIXR" &'B" (-&(" J9.)" O&A:1'2<3/,.,:" Q#XI?R!" (-+19" .F+9&//" 9+2%/(2" &9+" '.(" 2." /&90+P" *-+" (A." 9+/&(1.'2",9.22".'+"&'.(-+9"&("&M.%("#=>H"^!"&M.F+"A-1,-"(-+"/&((+9".F+9(&:+2"(-+"J.9)+9P"K'"(-+",.'(9&9G!" (-+"DUv9+,.))+'B+B" MG" ]9.2(" &'B" 32-MG" 12" )%,-" /.A+9" (-&'" (-+" .(-+9" (A." QD&(U:+" #XIX!" O&A:1'2< 3/,.,:" #XI?R" M+/.A" #?HH" ^\" 2++" *&M/+" CP" " 8&9(" .J" (-12" B1JJ+9+',+" ,&'" M+" B%+" (." (-+" B1JJ+9+'(" 1)6%91(G" /+F+/2".J"(-+" 5KC"2&)6/+2P""Y'"]10P"@4!"A+"-&F+"6/.((+B"(-+"/&((1,+"B1JJ%21F1(G"&,,.9B1'0" (.";`P"Q?R"&2"&"

J%',(1.'" .J" &" 6+'(&F&/+'(" B.6&'(" ,.',+'(9&(1.'" %21'0" (-+" (-9++" +)6191,&/"DUv" F&91&'(2" /12(+B" 1'" *&M/+" C" QD&(U:+"#XIX!"O&A:1'2<3/,.,:"#XI?!"]9.2(<32-MG"#X?CRP"

"

Y'".%9",.)6%(&(1.'2".J"B1JJ%21.'&/",9++6"A+".'/G",.'21B+9+B"(-+"/&((1,+".9"F./%)+"B1JJ%21F1(GDL!"1P+P"(-+" ,.'(91M%(1.'".J"09&1'<M.%'B&9G",&(1.'"B1JJ%21F1(G"DB"QN.M/+",9++6R"A&2"'.("(&:+'"1'(."&,,.%'(P""V126&9&(+" F&/%+2"Q399-+'1%2"9+/&(1.'2R".J"DBJ.9"%9&'1%)"1.'2"1'"5KC"-&F+"M++'"9+6.9(+B"1'"(-+"/1(+9&(%9+"M&2+B".'"

(8)

" " "

" " 9" " " " " """""""""N"

0 0.002 0.004 0.006 0.008 0.01

100 102 104 106 108 1010

[M2O5]

Normalized concentration, U

v T = 1573 K

E 1 = 3 eV E1 = 3.5 eV

E 1 = 4 eV

""""""""

0 0.002 0.004 0.006 0.008 0.01

10−18 10−16 10−14 10−12

[M2O5]

D L

(m

2 /s)

T = 1573 K,E 1 = 3.5 eV

U

v Mat69

U

v Haw68

Uv McN63

" "

]10%9+"@P"Q9R"N.)6%(&(1.'2".J"(-+"%9&'1%)"F&,&',G",.',+'(9&(1.'"5v"F+92%2"(-+"6+'(&F&/+'("B.6&'("

,.',+'(9&(1.'"1'"5KC"J.9"(-9++"F&/%+2".J"(-+"]9+':+/"&'1.'"6&19"+'+90G"E#"&(""T"#>=@P"QNR"*-+"

,.99+26.'B1'0",.)6%(&(1.'2".J"(-+"/&((1,+"B1JJ%21F1(G"DL"&("E#"@P>"+f"&'B"T"#>=@!"6+9";`P"Q?R!"J.9" (-9++"+S6+91)+'(&/"1'(91'21,"B1JJ%21F1(1+2".J"5v"h"D&(IX"QD&(U:+"#XIXR!"O&AI?"QO&A:1'2<3/,.,:"#XI?R!"

D,LI@"&((91M%(+B"(."8P"D,L&)&9&""Q]9.2(<32-MG"#X?CR\"2++"*&M/+"CP" "

Effect of temperature and stress

"

a+(" %2" '.A" B12,%22" (-+" +JJ+,(" .J" 2(9+22" .'" ,9++6" 9&(+P" Y(" 12" A+//" :'.A'" (-&(" 2+F+9&/" B+J.9)&(1.'" )+,-&'12)2" &9+" 1'F./F+B" 1'" .S1B+2" A1(-" J/%.91(+" ,9G2(&/" 2(9%,(%9+!" 1'" 6&9(1,%/&9" 5KC"&'B" *-KC" Q]9.2(<

32-MG" #X?CRP" N-&'0+2" J9.)" .'+" )+,-&'12)" (." &'.(-+9" )&'1J+2(" &2" ,-&'0+2" .J" 2/.6+" .'" (-+"/.0<!" F2P"

;

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0 20 40 60 80 100 10−8

10−7 10−6 10−5 10−4

Stress (MPa)

Creep rate (1/s)

T = 1453 K

T = 1537 K

T = 1563 K

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