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1 Journal of the Korean Electrochemical Society Vol. 11, No. 3, 2008, p» w ½ SDI ( : k) Recent Developments in Anode Materials for Li Secondary Batteries Sung-Soo Kim* Energy LAB, CRD center, Samsung SDI (Received August 18, 2008 : Accepted August 25, 2008) {»» œ š p HEV(Hybrid Electric Vehicle) IT wš. p p w k wš» y w w y š w. w» w, ƒ y ƒš p k e w j š w.» p ƒ y z z w w š w. Abstract : Li secondary batteries, which have been in successful commercialization, are becoming important technology as power sources in non-it application like HEV(Hybrid Electric Vehicle) as well as in portable electronics. It is not the overstatement that the commercialization of Li secondary battery was a result of the development of carbonaceous anode material and safety mechanisms. The R&D of electrode materials of Li secondary batteries is one of the core technologies in the development and it has enormous influences on various fields as well as on the battery industry. Here, the current research of anode materials is described and the underlying problems associated with development, advantages and drawbacks is analyzed. Keywords : Li secondary battery, Anode, Carbon, Graphite, Alloy. 1. p 1991 w ty m»» w p» wš. p w 1950 NASAƒ, w» p» w w» 30 ó k * augustine.kim@samsung.com y w ty. ty p t œ y mw, 10% w g ù, ƒ txw e y y e( ƒ )» w. ù», œ» w w w ww. p w p w e, 211
2 212 J. Korean Electrochem. Soc., Vol. 11, No. 3, 2008 w w m œw w, j 4ƒ w» w š w. w w w» w š w.» p ƒ w 4ƒ, p» breakthroughƒ ù ty k sww w r š w. 2. p 2-1. p»» p p w ù, û y y xkw ƒ ùkû p p w x» w xkw ƒ p t (dendrites) ü j» w. 1,2) p lf ƒ w k w p w w š, k p»yw ƒ p ƒ¾, yƒ yy ƒ w w Table 1. y p z * p (mah/g) (mah/g) s³ (V) (g/cc) p 3,800 - ~ ,~360 ~ gj - 0,~170 0~0.15 < g 4,200 ~1,000 0~ ,~700 0~ * z :( š w ) w š q j ùký» œw. x j š y š y», š y k w j p 372 mah/g w w» w g ù» w k y wš, š y k» ƒ w wš. š y z w w Fig. 1 Table 1 ùký k m ƒ û x p k t 3 V û ƒ. p Fig. 1. y. 3)
3 w»ywz, 11 «, 3 y, Fig. 2. x Unit cell (a) 1) x Unit cell (b). 2) ƒ 2 j w p š mw š k w š w. k» d s c w ABAB... d (hexagonal graphite) wù d ƒ x ABCABC... d x (rhombohedral graphite) sww. (graphite crystal) C w w» (Basal plane) c w sww (edge plane) ùkü. w k ùkü. p»yw w e,»»yw w y (inactive) ù w y (active) ùkü.»»yw p w e w» sww t»(surface group) x. y w y w k y k (graphitizable carbons) w, ƒ ƒ w. 2,500 o C w k ù y k (non-graphitzable carbons) w.» w» vp e (soft carbon) w, z w e (hard carbon) š w. y k y ƒ û (1,000 o C w) d s sww d C w d w w ùd (turbostratic Fig. 3. k turbostratic structure 3-D. 3) disorder) ƒ ƒw s d j»ƒ ƒw s d sww d. vp e 2,000 o C c w w d j w 3,000 o C. w» p (intercalation) p w ƒ 0.8 V sk ùkü z w w, 0.25 V w p ( k ) ù. p w k. Li x C C + xli + + xe ( :, : ) k y w Li k ü Li x C yw x w k y ù
4 214 J. Korean Electrochem. Soc., Vol. 11, No. 3, 2008 Fig. 5. d p l x. : š (schematic galvanostatic curve). : - š (schematic voltammetric curve). 4) Fig. 4. LiN(SO 2 CF 3 ) 2 /ethylene carbonate/dimethyl carbonate w (graphite Timrex KS 44) / š. (a) 1 st cycle and (b) 2 nd cycle, (C irr : ƒ, C rev : ƒ ). 4) k l Li k w,, x p ùkù. p lf w k j w e w. w vp e w w ƒw» 2,400 C w o y ƒ û k ùkù. vp e y 1,000 o C w ùkü. p m w ù» w ú V w ù p p ƒ û p d x wš w d w. p d» ü p ƒ ƒw p d d ƒ p LiC 6 k p d d kƒ. w p l w. w p l x w w d š š sk œ w w p ƒ ƒw l (stage) û l y p k ( ) w. w r w ƒ j d Fig. 6. l -1 k (In-plane). 7)
5 w»ywz, 11 «, 3 y, Fig. 7. y k ù y k. 9) ƒ š š ùk ù sk vj(peak) xk ùkù. p d d ABAB... AAAA... y LiC 6 k w d w 5) p w ƒw. LiC 6 k» 10.3% ƒ w. 5,6) LiC 6 k d p d p w w k w LiC 6 k 372 mah/g w ùkü. ù y k k d w g š j»ƒ ƒ w» 2,500 o C š w y w. Fig. 7 y k ù y k (nongraphitizable carbon) ùkü. wr yƒ w y k d s sww x w» yƒ w. Fig. 8. y k ù y k La, Lc y. 11) ù kyœ k ƒ k j»(la, Lc) ƒw. Fig. 8 y k ù y k La, Lc y ùkü. l y k La 3,000 C o 100 nm. ù ù y k 10 nm. Lc ƒ y k 100 nm w ù y k 4nm ùkü. k d s (crystallites) j»ƒ» d s p œ ƒ w. 8,11) ƒ p c w d d s j» y w p w p ƒ w w. p w w sw» š w sk x š š ùkü. w e w k d s d š 3 w œ (micro pore) w w (armorphous structure) ùkü. 800 o C w w w e w vp e ƒ swwš w š ù, 1,000 o C w
6 216 J. Korean Electrochem. Soc., Vol. 11, No. 3, 2008 Fig. 11. w e p» (A) œ w w en (B). 13) Fig. 9. vp e (soft carbon, coke) j š. 12) Fig. 10. w e (hard carbon) j š. 12) e ƒ ùkü. w, ƒ p š p ùkü. p, p w 0.05 V û j sk. w e ƒ p k ù œ ü p j l(li cluster) x w» w ù, ƒ 1,000 o C ƒw, œ w ƒ w w e j w. w, œ w enƒ w p ƒ w š š. 30,31) p k 10% Fig. 12. vp e w e ƒ y ( : w e, : vp e ). 10) q w vp e w e p w œ j» yƒ. 14) Fig. 12 vp e w e ƒ y. v p e 1,000 o C w w ùkü 1800~2000 o C š z ƒ ƒw 372 mah/g. wr w e 1,000 o C w 600 mah/g ùkü, ƒ ƒw w 2,000 o C w œ w yƒ w vp e û ùkü. Fig ,400 o C vp e w k ùkü, 2 vp e ù w e 500~700 o C w sww. 3 k d d ù š w w»œ sww w e ùkü.
7 w»ywz, 11 «, 3 y, Fig. 13.» t p w x w t ) v w p z v y š w. Fig. 14. v y( ), 16) xsi v y ùkü (w, œ:») 2-3 /w p p Li Li-Al, Li-Si w mw ù, p w / y ƒ y w. w» w Li w (Si, In, Pb, Ga, Ge Sn, Al, Bi, Sb ) w m. 17) p w w (Li x M) x w» t III, IV, V w t Fig. 13 t w.
8 218 J. Korean Electrochem. Soc., Vol. 11, No. 3, 2008 w. Li x M xli + + xe + M ( :, : ) w - p û ü ù w ùkù p y k» w w û k. ù p ù ƒ p ƒ¾ ƒ š p t» k š w. Sn-Li Sn Li ƒ Li 2 Sn 5, LiSn, Li 5 Sn 2, Li 13 Sn 5 Li 22 Sn 5 yw x Li-Si Li 12 Si 7, Li 7 Si 3, Li 13 Si 4 Li 22 Si 5 yw x. k 6 1 p w p w, p j. p w p j» k w w p 100~300% v yƒ j. w ( p w x ) ùkù v y Fig. 14 ùkü. p- w (Li x M) w p ƒ» w v y w» w q ƒ ù j p j w. p w w y» k w» w v y y j ù w w y ƒ w. p w k y y w mw w w ƒ v w š, w. - p w y - p w - y / y (active/inactive) w 27) - p w /k w y w» w p w p w» ³ x ù y j w. y w j» w p» q ƒ ù. p ùkù v y w x ƒ ³ x w j»ƒ ³ x t ù f w» w j»ƒ ùký š š w. 28) 32.2γ 1 ( 2V)2V 2 d = crit E V 2» d crit : j», γ : t V : s (passion s ratio) V 0 :» v, V : v y p w w w w (multiphase metal) w w / j p» w. ( Sn) y w p w, x w ( Sn/SnSb) p w. Fig. 15 ùkù SnSbƒ 800~850 mv p w ù Sn û 650~700 mv w ƒ p w vq y j w w j p w k. 1 : SnSb + 3Li + 3e Li 3 Sb + Sn 2 : Sn + 4.2Li e Li 4.2 Sn w Ag3Sn/Sn LiAg2Sn/ Li4.4Sn + LiAg Li2AgSn Fig. 15. Sn p w. 16)
![w»ywz, 11 «, 3 y, 2008 219 Fig. 16. Nexelion ( œ : ). Table 2. Sn-Co w Nexelion p» ( m14430» ) Nexelion y Sn-Co w y LiCoO2 LiCoO2+Li (0.2C) 700 mah, 2.6 Wh t 4.2~3 V [MnCoNi]O2 yw 900 mah, 3.1 Wh 4.](/docs-images/80/81282621/images/9-0.jpg "2~2.5 V 395 Wh/l, 144 Wh/Kg 18 g 20 g 478 Wh/l, 158 Wh/Kg w ƒ p w k. w 2005» t y Sony Nexelion» Li ƒ w ƒ Sn-Co w k wš. Sony e g, w sƒw. p w ƒ û q. y Nexelion» w t Fig. 16 Table 2 ùkü.")
9 w»ywz, 11 «, 3 y, Fig. 16. Nexelion ( œ : ). Table 2. Sn-Co w Nexelion p» ( m14430» ) Nexelion y Sn-Co w y LiCoO2 LiCoO2+Li (0.2C) 700 mah, 2.6 Wh t 4.2~3 V [MnCoNi]O2 yw 900 mah, 3.1 Wh 4.2~2.5 V 395 Wh/l, 144 Wh/Kg 18 g 20 g 478 Wh/l, 158 Wh/Kg w ƒ p w k. w 2005» t y Sony Nexelion» Li ƒ w ƒ Sn-Co w k wš. Sony e g, w sƒw. p w ƒ û q. y Nexelion» w t Fig. 16 Table 2 ùkü. p w j p w p w w w w w» w. w w» p w y (active phase; ) p w y (inactive phase; ) w y v q y j w w. 16) w w p w j» ywš p w p w ü w p w p w yw w. w p w w w y p w j x ù ƒ p w w w y w. j p w x w t y w. SnO, SnO 2 Sn x Al y B z P p O n y» j p w Li 2 O Sn x w ƒ j Li2O ü ù j» Sn ƒ sw y (Sn)/ y (Li 2 O) w x w j Sn Li ƒ w. j. SnO + 2Li + + 2e Sn + Li 2 O ù y Li 2 O x» ƒ w f p j š. w ƒ w w» w p w w ( Sn) ƒ p w ( Fe, Ni, Mn, Co ) yw x w. w x y w w. yw p» w yw w š p w (Sn) p w w w p w p w ù v y y g w w k. p w (, Si, Sn,...) p w ü w k p p w v y w ù y j w. w p w p w v y w ù v y w ³ y w» š w p w. w w y Si TiN, TiB 2, SiC p w yww w x w w x w Si w w / j p. ù p w v w y p
10 220 J. Korean Electrochem. Soc., Vol. 11, No. 3, 2008 k š p w mw p ƒ Li Si y y y w k p ù p y w w. w t y Li 4 O 12 ƒ. y 16d q e(octahedral sites) Li Ti yw w 8a e (tetrahedral sites) ù Li w Li[Li 1/3 /3 ]O 4 ùký. p Fig. 17. Li 4 O 12 y x š. 29) ü vƒ y ƒ wì ü p y ƒ j. y ù j» 15) w š wƒ p w. p 1.5 V ƒ 150 mah/g. Fig. 17 Li 4 O 12 y x š. Anatase ypk body-centered tetragonal (I4 1 /amd) a = Å c=9.502å g/ml. p»y w Li x Ti 1 O 2 x w ƒ 0.5¾.»yw Li 0.05 TiO 2 tetragonal Li 0.5 TiO 2 orthorhombic two-phase sx w š»yw 1.8 V(Li/Li + ) (Fig. 18). 18,19) Ti 1 O 2 + xli + + xe = Li x Ti 1 O 2 (x=0~0.5) Rutile ypk»yw y ù LiTiO 2 rocksalt x wš»yw ƒ 4.5% vq ƒ w anatase w potential sloping p (Fig. 18) ƒ. 20) Li(Li 1/3 /6 )O 4 (Li 4 O 12 ) w y ùkü zero strain 21-23).»yw 175 mah/g š 1.55 V(Li/Li + ) (Fig. 19)» w skw sk ùkü. 1 z k v x w». Li 1 (Li 1/3 /6 )O 4 Li 2 (Li 1/3 /6 )O 4 œ Fdm ƒƒ Å Å y % ùkü. yƒ w p w. Li 1 (Li 1/3 /6 )O 4 + Li + + e = Li 2 (Li 1/3 /6 )O 4 Fig. 18. Anatase rutile TiO 2 y p. Anatase, rutile ramsdellite TiO 2 [30] TiO 2 -B 24,25) Li 4 O 12 titanium oxideƒ p»yw y ùkü 170~250 mah/g ù ƒ 26) 1.5~1.8 V(Li/Li + ) p» k w». wr ù j» (rock-salt structure) y MO(M:Co, Ni, Fe ) p ù j» x w y w ù Li 2 O sw. 26) CoO.
11 w»ywz, 11 «, 3 y, Fig. 19. Li 4 O 12 x p. Fig. 20. CoO, NiO, FeO. 21) Co + 2Li Li 2 O + Co» w Li 2 O l CoO x w w ù j» t w ú. w ƒ y ù j» w ƒ w š. w ƒ w p Fig. 20 ùkü 0.8 V š j ùkù. 3. p» w Breakthrough œw k w /w, š y w» w š Li 4 O 12 y ¾ r. w y w» š, šz e v w š q w. ƒ ùy y w w z š š, k, t v wd š š. x y p ¾ {»» w ey y ƒ y, m š» w. w x ¾ š, š w p ƒ q, w w ƒ v w q. š x 1. Handbook of Carbon, Graphite, Diamond and Fullerenes, Noyes Publications, William Andrew Publishing, Park Ridge NJ. (1993). 2. Chemistry and Physics of carbon - A series of Advances, 5: Walker PL Jr, Deposition, Structure and properties of Pyrolytic Carbon, Marcel Dekker, CRC Press, Boca, Florida. (1969). 3. J.-M. Tarascon and M. Armand, Nature, 414, 359 (2001). 4. M. Winter et al., Insertion Electrode Materials for Lithium Batteries, Adv. Mater. 10. No. 10 (1998). 5. X. Y. Song, K. Kinoshita, and T. R. Tran, J. Electrochem. Soc. 143, L120 (1996). 6. D. Billaud, E. McRae, and A. Herold, Mat. Res. Bull. 14, 857 (1979). 7. Walter A. van Schalkwijk, Bruno Scrosati, Advances in Lithium ion Batteries, Kluwer Academic/Publishers (2002). 8. M. winter, J. O. Besenhard, M. E. Spahr, and P. Novak, Adv. Mat., 10, 725 (1998).
12 222 J. Korean Electrochem. Soc., Vol. 11, No. 3, I. Mochida, S. H. Yoon, Y. Korai, K. Kanno, Y. Sakai, and M. Komatsu. In: H. Marsh, F. Rodriguez-Reinoso, eds. Science of Carbon Materials. Alcante, Spain: Publicaciones de la Universidad de Alicante (2000). 10. J. R. Dahn, T. Zheng, Y. Liu, and J. S. Xue, Science 270, 590 (1995). 11. J. R. Dahn, A. K. Sleigh, H. Shi, J. N. Reimers, Q. Zhong, and B. N. Way, Electrochim. Acta 38, 1179 (1993). 12. Gholam-Abbas Nazri, Gianfranco Pistoia, Lithium batteries Science and Technology. Kluwer Academic Publishers (2004). 13. M. Winter, K. C. Moeller; and J. O. Basenhard, in: Science and Technology of Lithium Batteries, Gholam- Abbas Nazri, Gianfranco Pistoia Eds., kluwer Academic Publishers. 14. Y. Nishi, in: Lithium Ion Batteries, M. Wakihara, and O. Yamamoto, Eds., Kodansha/Wiley-VCH, Tokyo/Weinheim, chapter.8 (1998). 15. R. Spotnitz, J. Franklin, Journal of power sources 113, 81(2003). 16. M. Winter and J. O. Besenhard, Electrochim. Acta 45, 31 (1999). 17. R. A. Huggins, J. Power Sources, 81-82, (1999). 18. S. W. Oh, S. H. Park, and Y. K. Sun, J. Power Sources, 161, (2006). 19. H. Yamada, T. Yamato, I. Moriguchi, and T. Kudo, Solid State Ionics, 175, (2004). 20. E. Baudrin, S. Cassaignon, M. Koelsch, J.-P. Jolivot, L. Dupont, and J.-M. Tarascon, Electrochem. Commun., 9, (2007). 21. M. Julien, M. Massot, and K. Zaghib, J. Power Sources, 136, (2004). 22. K. Ariyoshi, R. Yamato, and T. Ohzuku, Electrochimica Acta, 51, 1125 (2005). 23. T. Ohzuku, S. Takeda, and M. Iwanaga, J. Power Sources 81-82, (1999). 24. A. R. Armstrong, G. Armstrong, J. Canales, and P. G. Bruce, J. Power Sources, 146, (2005). 25. T. Brousse, R. Marchand, P.-L. Taberna, and P. Simon, J. Power Sources, 158, (2006). 26. A. Kuhn, R. Amandi, and F. Garcia-Alvarado, J. Power Sources, 92, (2001). 27. K. D. Kepler, J. T. Vaughey, and M. M. Thackeray, J. Power Sources, 81-82, (1999). 28. J. Wolfenstine, J. Power sources, 79, 111 (1999). 29. T. Ohzuku, A. Ueda, and N. Yamamoto, J. Electrochem. Soc. 142, 1431 (1995). 30. A. Kuhn, R. Amandi, and F. Garcia-Alvarado, J. Power Sources, 92, (2001). 31. P. Polzot, S. Laruelle, S. Grugeon, L. Dupont, and J. M. Tarascon, Nature, 407, 496 (2000).
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w y wz 10«3y 259~264 (2010.12.) Journal of Korean Society of Urban Environment w gj p p y Á Á½k * w m œw Á* w y œw (2010 9 28, 2010 10 12 k) Characteristics of Antiwashout Underwater Concrete for Reduction
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w y wz 8«( 2y) 57~61, 2005 J. of the Korean Society for Environmental Analysis p w w Á Á w w» y l Analysis of Influence Factors and Corrosion Characteristics of Water-pipe in Potable Water System Jae Seong
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Journal of the Korean Chemical Society 2007, Vol. 51, No. 4 Printed in the Republic of Korea w x - w y *Á š w w w yw (2007. 3. 28 ) Case Study on Verbal Interactions of Teacher-Small Group StudentsG in
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y, 38«, 6y, 699-705, 2005 Econ. Environ. Geol., 38(6), 699-705, 2005 t sÿ y xk 1 Á s 2Á z 1 Á½ 1 Á e 3 1 w y w,» w, 2w y w, 3š w y w Chemical Speciation of Heavy Metals in Geologic Environments on the
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2007, Vol. 51, No. 2 Printed in the Republic of Korea xw yw w w» e w z Á Á y Áw # Á k * w yw w w w w w # w w w (2006. 10. 30 ) Influences of Current Education Programs for Preservice Chemistry Teachers
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Journal of the Korean Chemical Society Printed in the Republic of Korea w yw w w ½ Á Áw Á k * w yw w w w w w (2006. 8. 9 ) Relationship between Conceptual Understanding and Mapping Errors Induced in Learning
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32«4ByÁ 2012 7 pp. 233 ~ 242 œ w w w y œ r Estimation of Domestic Water Supply Benefit Using Demand Function Approach ³ Á Á½¼yÁ Yeo, Kyu DongÁYi, Choong SungÁKim, Gil HoÁLee, Sang Won Abstract In the past,
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w wz 16«2y Kor. J. Clin. Pharm., Vol. 16, No. 2. 2006 ü t xy y w tœ ½ BÁ x BC B y w w w C y w w w Current Status and Expectations of Orphan Drugs in Korea -In point of supplying medicines for the rare
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Jurnal f the Krean Ceramic Sciety Vl. 44, N. 9, pp. 502~509, 2007. Examinatin n Applicatin f High-Perfrmance Cncrete using Fine Fly Ash as Replacement Material f Silica Fume Bum-Sik Lee, Sang-Kyu Kim,
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w wz J. Kor. Soc. Cloth. Ind. 8«2y, 2006 Vol. 8, No. 2, pp.177-182(2006) x w e w 1) Á Ÿ 1) Á»û 2) 1) ƒm w q w 2) w w w The Effect of Media on Taking Plastic Surgery Chong-Hee Yun 1), Su-Kwang Sung 1) and
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w CAD/CAM wz 15«3y 2010 6 pp. 189-203 œ w w *, **, x***, v ** The Conceptual Design of Semi-submersible Type Mobile Harbor Using Axiomatic Design Principles Joohee Lee*, Seongjin Yoon**, Hyun Chung***
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w m y Vol. 16(4), p. 53~61, 2011 œ 광물찌꺼기에함유된오염물질의안정화를위한표면차폐재의성능평가 ½ ³ 1 Á 1 *Á½ 2 Á½ 2 Á 3 Á 3 1 w œ w œw, 2 ( ) f lp, 3 w Ÿw œ Ÿw» Evaluation of Surface Water-preventing Materials on Stabilization of
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