Vol. 63, No. 10, October 2013, pp. 1176∼1179
New Physics: Sae Mulli, DOI: 10.3938/NPSM.63.1176
Synthesis and Characterization of LuBa
2Cu
3O
zSuperconductors by Using of a Polymeric Precursor
Man Seok Lee · Ho Keun Lee
∗Department of Physics, Kangwon National University, Chuncheon 200-701, Korea
Sang-Il Seok
Korea Research Institute of Chemical Technology, Daejeon 305-343, Korea (Received 31 July 2013 : revised 6 August 2013 : accepted 10 October 2013)
The Pechini polymeric precursor method was successfully used to synthesize polycrystalline LuBa2Cu3Oz (Lu-123) superconducting compounds. The results of X-ray diffraction (XRD), Scan- ning electron microscopy (SEM) and resistivity measurements showed that the Lu-123 phase was formed when heated at temperatures between 860◦C and 880◦C under a 9% O2-91% N2 atmo- sphere after pyrolysis of the precursor at 350◦C for 5 h in air and 600◦C for 3 h in O2. The polycrystalline samples sintered at 880◦C under a low oxygen partial pressure revealed a single phase and showed superconductivity comparable to that of the sample prepared by using the solid state reaction method. Compared to the phase formation temperature of the sample prepared by the solid state reaction method, that of Lu-123 was found to be lower, possibly due to the fine particle size after the pyrolysis.
PACS numbers: 74.72.-h, 74.72.Jf, 74.62.Bf, 74.25.Fy
Keywords: Synthesis, LuBa2Cu3Oz, Polymeric precursor, Superconductivity
Polymeric precursor õ u § T Ó Þ X ¢ LuBa
2Cu
3O
z ¾ ¹ Å y ¢= k 8 ý ¶ ¥V R Ë õ m Í ¤ V R Ë ì Å
T
¹ ÿ ) o · T Ú£ Ó
∗y
©"é¶@/<Ƨ Óüto<Æõ, ðr ; 200-701
) o
ç ¡ G B
ô
DzDGo<ƽ¨"é¶, @/ 305-343
(2013¸7Z431{9~ÃÎ6£§, 2013¸8Z46{9ú&ñ:r~ÃÎ6£§, 2013¸10Z410{9>FSX&ñ)
Pechini polymeric precursorZOܼР&ñ LuBa2Cu3Oz (Lu-123) í¸^\¦½+Ë$íH½¨\¦ Ã
º'Ùþ¡. s ~½ÓZOܼР/BNl ׿ 350◦C\"f 5rçß, íßèìr0AlÐ 600◦C\"f 5rçß \PìrK ôÇ Êê 860∼880◦C:r¸%ò%i\"f9% O2-91% N2Ð\P%oLu-123©s+þA$íHd`¦XRDÐ,©l_ ±ú
É
ríßèìr·úܼÐ880◦C\"f þj7áxèôÇ õ_ éß{9©_Lu-123r¼#`¦½+Ë$í½+Éúe6£§`¦SEM
Ð8£¤&ñ#·úúe%3.q$½Ó8£¤&ñõ\"fe>:r¸H¦©ìøÍ6£xZOܼн+Ë$íôÇ õü<_ °ú
¤.¢¸ôǦ©ìøÍ6£xZOܼн+Ë$íôÇ âĺ\ qK±úÉr :r¸\"fLu-123©s+þA$íHd`¦'a8£¤Ùþ¡Ü¼ 9,s
HPolymeric precursorZOܼн+Ë$íôÇ âĺ \PìrK Êê ìr´úß¼l©@/&hܼРÉr כ\ lH כܼÐ[O"î÷&%3.
1176
This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License (http://creativecommons.org/licenses/by-nc/3.0) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.
Synthesis and Characterization of LuBa2Cu3Oz Superconductors· · · – Man SeokLeeet al. 1177
PACS numbers: 74.72.-h, 74.72.Jf, 74.62.Bf, 74.25.Fy Keywords:½+Ë$í, LuBa2Cu3Oz, Polymeric precursor,í¸
I. " e  ] Ø
1987¸ 90 K _ í¸ e>:r¸\¦ ?/H Y- Ba-Cu-O > í¸^ Wu1px [1]\_K %6£§Ü¼Ðµ1Ï
|
)aÊê s í¸^HYBa2Cu3O7−z >_½¨$í`¦°úH כܼРµ1ß)&ܼ 9, s#Q Y@/ @/ÂÒìr_ BÐÀÓ "é¶è
\
¦ Y @/u¨88¸ 90 K_í¸^½+Ë$íHd s
Ц[2]÷&%3.ÕªQBÐÀÓ"é¶è׿Ce (cesium), Tb (terbium) x9 Lu (lutetium) _ âĺH 123 ©s +þA
$í
÷&t ·ú§H כܼР·ú94R M®o [2–4]. :£¤y Lu_ â Ä
º 900◦C ∼ 1000◦C_ :r¸%ò%i\"f :x©_ ¦©ìøÍ6£x ZO
ܼÐH &ñ ZOß¼Lu-123 ©s +þA$í÷&t ·ú§6£§s ¸ú
· ú
94R e [5]. ÕªX< þjH Lee [6] H Bĺ a%vÉr \P
%
o :r¸ x9 íßè ìr·ú\"f ¦©ìøÍ6£xZOܼРéß{9©_
Lu-123ZOß¼ í¸^\¦½+Ë$íH~½ÓZO`¦%6£§Ü¼Ðµ1ß+ÀI
. :r½¨H Õª_ ½¨\ lìøÍ# çH|9ôÇD¥½+Ës 0
p
xôÇ polymeric precursor~½ÓZOܼÐZOß¼Lu-123í¸
^
\¦ ½+Ë$í¦ Õª :£¤$í`¦ ¦©ìøÍ6£xZOܼР½+Ë$íôÇ r¼# _
:£¤$íõq§Ùþ¡.
II. ÷ m Ç] M ö U ê s 0 n É
r
¼#Ér ¦©ìøÍ6£xZOõ Polymeric precursor ~½ÓZOܼÐ
½
+Ë$íÙþ¡. ¦©ìøÍ6£xZO\ _ôÇ r¼#_ ½+Ë$íÉr ÃЦëH³ [6] \ lÕüt)a ~½ÓZOܼРú'÷&%3ܼ 9, ½+Ë$í M: íH¸ 99.9% s©_Lu2O3, BaCO3 x9 CuO ìr´ús s6 x÷&%3
. Polymeric Precursor ~½ÓZO\ _ôÇr¼#_ ½+Ë$íÉrs
~
½ÓZOܼРY-123 í¸^\¦ ½+Ë$íôÇ âĺ [7]\¦ ½Óܼ
Ð #Q tн+Ë$ís r¸÷&%3.
:r ½¨_ ~½ÓZO\"fH $ 99.9% íH¸\¦ tH LuN3O9 ìr´úõ 99.999% íH¸ BaCO3, CuO_ ìr´ú
`
¦s6 x¦ªs:r_qLu:Ba:Cu = 1:2:3s ÷&¸2¤
&
ñ|¾Óo ôÇÊê,yìr´ú`¦60%|9íß6 xÓo\V,¦ \P# 6
xKôÇ +' D¥½+Ërv¦ 8úx FK5Åqs:r_ 1.2C_ ]tq ëß p
ucitric acid\¦'#çH{9>D¥½+Ë÷&#QeHmetal citrate 6 xÓo`¦ëß[þt%3.
D¥½+Ë6 xÓoÉrrotary evaporatorÐy·ú7£xÀÓ#metal citric salts`¦ %3Ér Êê 'ôÇ citric acid 1 g {© 2 ml_
∗E-mail: [email protected]
Fig. 1. XRD patterns calcined at 860◦C for samples pre- pared by (a) solid state reaction method and (b) poly- meric precursor method.
ethylene glycol\¦ V,#Q D¥½+˦ 130◦C\"f poly- merizationìøÍ6£x\_# ¦&h¸0q+þA_polymeric pre- cusor\¦ %3%3. sXO> %3#Q precursor\¦ ¸Ér\"f 350◦CÐ 5rçß \PìrK r Êê Z>> ìrW# r 600◦CÐO2Û¼ìr0Al\"f5rçß\PìrK# p[jìr
´ ú
`¦ %3%3. ¦©ìøÍ6£xZOܼРr¼#`¦½+Ë$í½+É M:¸ q§
\
¦0AK %6£§ D¥½+Ë#ìrW)aìr´ú`¦600◦C\"f°ú Ér
¸|õrçßܼÐ\P%oÙþ¡.sÊê_\P%oHþjHLee [6] \ _K ½¨)a ~½ÓZOܼРlíÐ # 860◦CÐ 9%
O2, 91% N2D¥½+ËÛ¼ìr0Al\"f10rçßè%i¦1lx {9
ôÇ D¥½+ËÛ¼ ìr0AlÐ ¿º \5g 870◦C\"f 10r ç
ß, 880◦C\"f10rçß è# &ñ ZOß¼ í¸^
\
¦½+Ë$í%i.
èü< è\ Ér X- r]X (XRD; X-ray diffrac- tion) ìr$3Ér Cu Kα`¦ s6 xôÇ X- r]X©u (PAN- alytical X’pert-pro MPD) s6 x÷&%3ܼ 9,r¼#_{9¸ x9
p[j¸fÉr ¦ìrK0px ÅÒ &³pâ (SEM; scan- ning electron microscope, Hitachi S-4800)ܼР¸÷&%3
. r¼#_ q$½Ó :£¤$íÉr ÉrÛ¦`¦s6 x# ]XÃÌ)a4éß
]X&hZOܼÐ10 mA_ÀÓ\¦ fË98£¤&ñÙþ¡.
1178 New Physics: Sae Mulli, Vol. 63, No. 10, October 2013
Fig. 2. (XRD patterns sintered at 880◦C for samples prepared by (a) solid state reaction method and (b) poly- meric precursor method.
III. ÷ m Ç] M ö + s Ç Ê Ý õ m Í º 8 ý
Figure 1Ér ¦©ìøÍ6£xZOõ polymeric precursor ZOܼ
Ð %3#Q ìr´ú`¦ 860◦C\"f èôÇ(calcined)Êê %3#Q
X-r]XJ`¦Ð#ïr.¦©ìøÍ6£xZOܼн+Ë$í)a r
¼#_ âĺ f Lu-123 ©s +þA$í÷&t 3lw¦ ÅÒÐ BaCuO2, Lu2BaCuO5 x9CuO ©s'a8£¤÷& 9 sH Lee [6]'a8£¤ôÇ õü<{9uôÇ.s\ qKpolymeric pre- cursor ~½ÓZOܼР½+Ë$í)a X- r]X J(b)Ér BaCuO2, Lu2BaCuO5 x9 CuO © ü@ Fig. 1\ ³ðr)a ü< °ú s Lu-123©_ÅÒr]Xs'a8£¤)a.sHpolymeric pre- cursorZOܼÐ%3#Qìr´ú_âĺ s:r¸\"fLu-123© s
+þA$íHd`¦_p9,"fpolymeric precursorZOܼ
Ð ìr´ú`¦ ïrq ¦©ìøÍ6£xZOܼРïrqôÇ ìr´ú\ q K
бúÉr :r¸\"fLu-123©`¦+þA$ír~´Ãºe6£§`¦ t
rHכܼÐ^¦Ãºe. Fig. 2Hz´+«>~½ÓZO\"f /
å
LôÇ ]X\ þj7áx&hܼР880◦C\"f èôÇ (sin- tered) Êê %3#Q X- r]X J`¦ Ð#ÅÒ 9, ¿º âĺ
¸¿º _ éß{9©r¼#s½+Ë$íHd`¦Ð#ïr. 123> ½¨ o
íßoÓüt_ {9ìøÍ&h è x9 è õ&ñ\"fH ÃЦëH
³[5]\/åL)aü< °ú s ÅÒÐ900◦C∼950◦C:r¸%ò
% i
\"f è9,èÉrÅÒÐ900◦C∼1000◦C:r¸%ò
% i
\"f'K.s M:\P%oH /BNl ¢¸Híßèìr0Al
\
"f 'Kt¦ e. s\ qK :r ½¨_ Lu-123 í
¸^_ ½+Ë$íõ&ñ\"fH10%_ ±úÉríßèìr·úìr0A
Fig. 3. SEM photographs after pyrolysis at 600◦C for samples prepared by (a) solid state reaction method and (b) polymeric precursor method.
l
ü< 860◦C∼900◦C a%vÉr :r¸ %ò%i_\P%o ׿כ¹
Hz´+«>õ[6]\HKèx9èz´+«>s ú'
÷
&%3. :£¤y Lu-123©s +þA$í÷&H õ&ñ\"f BaCuO2, Lu2BaCuO5x9CuO©sצ#Q[þt%3¦^¦ÃºeܼټРs
[þt©s Lu-123ܼШ8Hd`¦trôÇ. "f\P% o
\ Ér Lu-123 ©_ +þA$íõ&ñÉr úd&hܼР6£§õ
° ú
Ér /BNd(1)Ð ³ð&³½+Éúe.
0.5Lu2BaCuO5+ 1.5BaCuO2+CuO+
(0.25−x/2)O2→LuBa2Cu3O7−x (1) Figure 1\ èß ü< °ú s 860◦C \P%o\"f ©+þA
$í
:£¤$í_ o eH כ Ér ¿º ~½ÓZOܼРïrq)a ìr
´ ú
\ #Q"se6£§`¦r9,s\¦¸l0AK
¿
º ~½ÓZO\"f600◦Cаú Ér ¸|ܼР\P%oôÇÊê %3#Q
ìr´ú`¦ SEMܼÐ'a¹1ÏôÇ õ Fig. 3\ e
.¦©ìøÍ6£xZOܼн+Ë$íôÇìr´ú(a)H{9_ß¼l 0.5µm∼4µms9{9 ¦ØÔ>ìríHכ `¦ ^¦Ãº e
¦polymeric precursorZOܼн+Ë$íôÇìr´ú(b)H{9 _
ß¼l0.1µm∼1µmÐ p[j9{9[þts "fÐ Ó
ü
æ5g4R"f é#Qo +þAIÐìríH כ `¦ ^¦ ú e. Õª
QÙ¼Ðpolymeric precursor ZO`¦s6 xp[jôÇìr´ú
`
¦½+Ë$í½+Éúeܼ 9 sÐK©@/&hܼбúÉr :r¸_
\P
%oиLu-123©s+þA$í÷&HכܼÐ^¦Ãºe.:r
½¨_õH¢¸ôÇ polymeric precursorZOs p[jìr´ú _
½+Ë$ís 0px# ¦©ìøÍ6£xZO\ qK Êê}_ ]j\
¸ Ä»o½+É כܼР«Ñ)a. Fig. 4H 880◦CÐ þj7áx è
ôÇr¼#_SEM'a8£¤õs.
Figure 4(a)\ Ð#ïr¦©ìøÍ6£xZOܼн+Ë$íôÇr¼#Ð
Fig. 4(b)\ Ð#ïr polymeric precursor ZOܼн+Ë$í ô
Çr¼#_ p[j½¨¸ Ð ux9ôÇ כ `¦·úú e. s
Synthesis and Characterization of LuBa2Cu3Oz Superconductors· · · – Man SeokLeeet al. 1179
Fig. 4. SEM photographs for Lu-123 bulk samples pre- pared by (a) solid state reaction method and (b) poly- meric precursor method.
õH polymeric precursorZOܼРr¼#`¦½+Ë$í¦
©ìøÍ6£xZO\ qK r¼#_e>x9¸\¦ß¼>¾Ó©r~´0px
$í
sZ}6£§`¦trôÇ.s[þtþj7áxè)ar¼#_q$½Ó 8
£¤&ñ õFig. 5\ e.q$½Ó_ ß¼lH¿º r
¼#s_Ä»<Ê`¦Ð#ÅÒ 9,$½Ós0s÷&H :r¸H
¦©ìøÍ6£xZO_âĺ88 KÕªo¦polymeric precursorZO _
âĺ86 KÐ _Ä»<Ê`¦Ð#ïr.
IV. + s Ç Â ] Ø
Pechini polymeric precursor ZOܼР&ñ LuBa2Cu3Oz (Lu-123) í¸^\¦ ½+Ë$íH ½¨
\
¦ ú'Ùþ¡Ü¼ 9, Õª õ 860 ∼ 880◦C¸ %ò%i\"f 9%
O2-91% N2Ð \P%o éß{9©_ ZOß¼ Lu-123 í
¸^\¦ ½+Ë$í½+É Ãº e6£§`¦ Ð%i. ¢¸ôÇ polymeric precursor ZOܼРìr´ú r¼#`¦ ½+Ë$í ¦©ìøÍ6£xZO\ q
K p[jôÇìr´ú½+Ë$ís 0px¦, sÐK©@/&hܼ
бúÉr :r¸\"fLu-123©`¦+þA$ír~´Ãºe`¦ ÷rm
Ð ux9ôÇè^\¦ ½+Ë$í½+É Ãºe6£§`¦ ·ú úe%3
. Polymeric precursor ~½ÓZOܼР½+Ë$í)a r¼#_ e>
:r¸H ¦©ìøÍ6£xZOܼР½+Ë$íôÇ r¼#õ _ Ä»Ùþ¡.
"fPolymeric precursor~½ÓZO`¦s6 xZ}Érx9¸ _
Lu-123 í¸^ Óüt|9_ ½+Ë$ís 0px# e>x9¸ _
¾Ó©\6£x6 x½+Éúe`¦כܼР\V©)a.
Fig. 5. Resistivityvs.temperature data for LuBa2Cu3Oz samples prepared by (a) solid state reaction method and (b) polymeric precursor method.
P c
p 8 ý ò k >
:r ½¨_ XRD 8£¤&ñÉr y©"é¶@/<Ƨ /BN1lxz´+«>z´_þv'a _
©qÐ8£¤&ñ÷&%3.
REFERENCES
[1] M. K. Wu, J. R. Ashburn, C. J. Torng, P. H. Hor and R. L. Menget al., Phys. Rev. Lett.58, 908 (1987).
[2] P. H. Hor, R. L. Meng, Y. Q. Wang, L. Gao and Z.
J. Huanget al., Phys. Rev. Lett.58, 1891 (1987).
[3] J. M. Tarascon, W. R. McKinnon, L. H. Greene, G.
W. Hall and E. M. Vogel, Phys. Rev. B 36, 226 (1987).
[4] A. R. Moodenbaugh, M. Suenaga, T. Asano, R. N.
Shelton and H. C. Ku et al., Phys. Rev. Lett. 58, 1885 (1987).
[5] E. Hodorowicz, S. A. Hodorowicz and H. A. Eick, J.
Alloys Compd.181, 442 (1992).
[6] H. K. Lee, J. Supercond. Novel Magn. 25, 2519 (2012).
[7] H. K. Lee, D. Kim and S. I. Suck, J. Appl. Phys.65, 2563 (1989).