Optimal Remediation of TCE-contaminated Groundwater using Direct Current and Fe<sup>0</sup>

전체 글

(1) , 35, 3 , 229-239, 2002 Econ. Environ. Geol., 35(3), 229-239, 2002.

(2)

(3) . . . . .

(4) . . . . . . Optimal Remediation of TCE-contaminated Groundwater using Direct Current and Fe0 Ji-Won Moon1, Hi-Soo Moon1*, Yul Roh2, Heonki Kim3 and Yungoo Song1 1. Department of Earth System Sciences, Yonsei University, 134 Shinchon-dong, Seodaemun-ku, Seoul, 120749, Korea 2 Environmental Sciences Division, Oak Ridge National Laboratory P.O. Box 2008, Oak Ridge, TN 37831-6038, USA 3 Department of Environmental System Engineering, Hallym University, Okchon-dong 1, Chunchon, Kangwon-do, 200-702, Korea. The objective of this study was to design an optimal electro-remediation system for TCE contaminated water using zero valent iron (ZVI) and direct current (DC). A series of column experiments were conducted to evaluate the effects of electrode arrangement and the location of permeable iron barrier in the column on the TCE removal efficiency and iron corrosion process. In twelve different combinations of ZVI and/or DC application in the test columns, the rate of reductive degradation of TCE was improved with simultaneous application of both ZVI and DC compared to that used ZVI only. The most effective arrangement of electrode and ZVI for TCE removal from water was a column set with ZVI and cathode installed at the down gradient, respectively.. permeable reactive barrier, direct current, zero valent iron installation, electrode arrangement. .

(5) !" ! #!$ %& '(" )*

(6) +, - ./012 34 5 6 78 9 : ;"$

(7) <= >

(8) < =04 ?@ ABCD EFGH4 !I JFKL M 1NO <= $ !1 PQRS T$ MP $ UP QR V +W @S XY ZS '( )* [\] ^_`4 !ab P QR .

(9) .

(10)

(11) . . . . . . :.

(12) . ! " #$ %&'( )* + " ,-. / 01 234 567 +08 5 679 : ,* ;<= 31>? @ AB 0C <D <E FE GHI J KLMN 0 567 OPQR * 8S . . . . . . .

(13) . !!"#. $

(14) . . 0V 567 3W &X Y@ Z[R T \]@ ^V . _< , ^ `[R ab9 '*8 c " .d "_ _ * %e

(15) 564 ;fX Zg hi " 560 .j hi[ kf08 c l 56mf no _I* [1M* , 3 p 3 [R nq r ZLQ stX. . . T< U10 10 Q08. !!%.

(16) . . . . '. . !!!. *Corresponding author: [email protected]. . . . (.

(17) kf hinq u

(18) kf m0- v w x ytZJ9 U1,* z [1{ Z| Zt Z} hi[ G0 )8 cV- ~;

(19) <=* 3 [ [ nq0 (;M )HI 567< U1M* 56Q J s t0 567 3W

(20) Q \]9 z ,* _. {8 ^ @ l d nq,< U1 3 )f 8S st 56Q0 U1M 8. ytZ9 01 T f 0 / OPQI U1 234 567<= Z S4 09 PHI J[ T / b?* . m 0HN ~ 2 34 567< yt ZJ9 HI

(21) \]9 ¡.( 234 567 3W9 d ( ,* . ¢£,8 ¤ JG 234 567 + d [19 ¥¦ ,* ¤ I=* KL ; no §m hi w¢4/ 3 )8 O PQ hi< £¨,* & ©Z@ 56.j h i[9 ª «¤08 ( @ ©Z@ A¬ 234 567 Ai< 8S,¦ £¨ 3 )HN ~ ®@ ¯ 0< °± 567 OP ² ³1@ 567 ,3. ´ * K<= µ,8* ¶9 ·¸8 x ,3p 1 ¹ º< » º/ ¼ ½L * 567 0" ¾/ ¿,À8 °Á= Â <=* ¬; [ 3 [ nq <

(22) d9 .;,^ yt ZJ / 01 234 5679 < ¾Ã « ¾Ã½ÃX Z} ÄÅnq< °± KL\]9 ÆÇÈ( .d 0?[R v. ¾Ã nq9 ,( ,À8 0* ¹ ¤J G 9 :L ÆÉP A¬567< ytZJ Ê Ë ÇÌÁ d [1 3 Uf/ (É,( 0" 567< Í \ / ÆÇÈ* È8 8S nq 08 °Á= Â ² *

(23) d< ¾Ã,( ,* ytZJ9 01 234 5 67 ¾ "_ uÎI= U1 3 )9 ¶HI ¨%{8 . . ). . . . *. . + .

(24) . . !!%#. -. . !!.. . . . . . !!,#. . /. .

(25) . !! . . . &. . - . 0///#. 0// . ). 1 2 34 . . !!" . . 0///. . 2 . !!!. . . &. . . . &. . - . 0///#. . 0//. . . . .

(26) . . & < KL ³@ h[R J[ T ;0N 0« »@ Z JHI ³1,- Zg 56 ³0 Çy ;Ï WM Ð,( )8 0V 56 <= JI ³1,* Q@ Ñ 56 I<= £¨,* ¶I hi<= ÒÓ{ I yÔ[R Z 0 » A º/ :L 31> ?HI 0 . 3KL<= £¨ 3 . G08

(27) . .

(28) . . !!". . . 5. . . . 0. . . 6.

(29) .

(30) . . !!". ,3 p< ¹Õ,* z Y@ S4Ö¦. ¹Õ,i 8´ Y@ 560 £¨8 -3.

(31)

(32) . . !!". 8-3)7−. −. -370 7). 0V 569 ×* . . 04Qg I KLM* 5Ø56<= Ù;{ hÚJZ½* 08 0« . »0 56< Û^,i J[ T ÜÝ@ º I ³1M* » ¯Ý ¬,8 &. 7/:/;7/:0. 6. . . 9&. !.%. . /.

(33) .

(34) . . !!". . 7-37). −. . 8. 7-3)7. 234 567 .d "_ Þ3* 5670 ß9 ,* U1 J[ T 569 : 56mf08 / U1,* +< )= àÕ[ R _* º/ : ¯º ¨4 ©ZHI 5670

(35) M* ¶0N 0* 567 p < ²Q9 ©Zá 2349 ªâ8 cV d [1 ¯º ©ZHI R 234 567p ,3 0 @ ~; ¨[ n q<= £¨,* ¶HIf È(M( )8 . . . . . 1 . . !!%. 234 567 \]9 b? ½L < l ytZJ9 01 Z 0 \ . )* ¶H I ÏRMã8 0 z T ³@ » ºX lZJ< Z HI £¨ J[ T ³108 ytZJ9 01 KL ³@ ¦ » º ; ZK L ;<= 0N äå< ¾Ã{ % Z}<= £ ¨M* 56@ 8´ Y8 . - . 0///. . . &. . .

(36) ! " < . −. . 8 70. T 9 ½L

(37) { ,3* p<= ¡ t3/ 01L ³,À( 0< n49 < -çpã8 U1{ * (Bf0N 8± ^ è0 U1,À8 I

(38) { .? ,3* é£ p hi< ÒÓM* ¶9 ê, ½L / 1 1Ý ? ? < ëÇ äå ¿ U1,ÀHN ¬; kf/ , ½L 9 ¿< ëÇ / 01 pp ìZ,À8

(39) { U ,3* HIí . =>> -370 7)8-3)70 7−. ?. . 06 3/.. . !%,# ' - . <'.

(40). &. !!:. . '4. . (<. .

(41). . ? .

(42) .

(43) . . . ?. ? .

(44)

(45) . 9 B 3'

(46)

(47) . and chemical composition of filing materials and simulated waters. Simulated waters. Filing materials Peerless Fe Fe Fe0, Fe2+Fe3+2O4 C (%) <4 Pb (mg/L) 58.46 Ni (mg/L) 256.8 Co (mg/L) 946.5 Mn (mg/L) 5105 Mg (mg/L) 41.48 Cu (mg/L) 3823 Ca (mg/L) 803.4 Al (mg/L) 61.1 Na (mg/L) 298 Specific surface area 1.2125 m2/g CEC 0.56 meq/mol Porosity 65.00% Quartz sand Porosity 45.00%. Schematic. &. !!:A ' 3< . &. ´}<=* & T/ ,* J 9 ( 5i S}<=* æ ®@ 3 . / £¨â 8. 0. . .

(48) 0)70 −80)−7) 7-37)8 7-3)7− -37)8-3)7)7−. Physical characteristics.

(49) . . 7-37)8 7-3)7− 0)8")77" −. (? @. . pH Eh (mV) EC (µS/cm) DO (mg/L) Temperature (oC) Alkalinity as HCO3 (mg/L) Chloride (mg/L) Nitrate (mg/L) Phosphate (mg/L) Sulfate (mg/L) Sodium (mg/L) Ferrous iron (mg/L) Total iron (mg/L) MES Biological Buffer TCE (µg/L). diagram of experimental set-up.. Minimum. Maximum. 5.51 612.1 91.3 3.62 18.8 7.52 6.20 12.02 8.94 8.99. 6.91 957.9 196.2 5.60 26.9 14.98 8.62 12.70 9.49 9.73. < 0.01 < 0.01. < 0.01 < 0.01. 597.4. 2485. Used source materials. NaHCO3 0.2 mM NaCl 0.2 mM NaNO3 0.2 mM NaH2PO42H2O 0.1 mM Na2SO4 0.1 mM 0.9 mM. C6H13NO4S 0.2 mM.

(50)

(51) / 01 e 1 < U1{ 56äå äåHI îï mHI ,À8 @ ÕQ 0 p I , ÖðIí <

(52)

(53) / OPQ@ <= ð,^ U1,ÀH 01,^ Z}9 ²,À8 Z} ÕQ@ N Â[R 4Q@ 8´ Y8 ðfKñ* {

(54)

(55) @ I l ytZJ< ²,À8 äå S@ 9 01,^ ,À8 Â @ Z} ÄÅ< °± ?. / òóoKô ² K 0N Ý õcöç X Y0 e äå 0÷/ ,( )8 » 0l OP Q ÆÇÈ ½ ¶0I / õ ,À8 * ¾ < øÝJ Kô@ u JJ = ùK / 01 Ã è0 ytZJ ÊX ÄÅ9 w ¶0N * . ,^ Kô,À8 r d<= ?t< ¾Ã{ U{

(56) { ,3 [ n49 ú äåõ8 Z} ÄÅ9 (É ¶08 w[ ¬ û9 .f ,ÀHN m x î * 5 zI ï ¬ nqHI 9 ,À8 . ,t< ¾Ã{ z0N Â <=* ³{ % äå0 Ý * ? ,t< < ¾Ã{ z/ U ¶ ü ý0/ .I z .* ôaU * ?tX ,t< %% ¾Ã ¶< S x ¬;,. þ8 °Á= äå@ 0N %% }9 .N wL Í \ . )*/ ÆÇÈ ½ äå0 * ytZJ 0 äåÿ* . ¾Ã{ K@ ¬ QÝH 8 %% <= äå0N X * ?t< L

(57) I OP,ÀHI OP K< L= . 1 è* Z}0 ´} @ S} }9 .- 9 ;9 äå ß ¾ÃK0 ,* K< l 0 ¾Ã{ z/ U ¶08 %% Z}@ : = ; äå< wL 0Ä . OPMãHI }0 ,0: 1I % 8I K äå< Ñ ? X Ô,¦ ,ÀHN 0« ¾ÃK9 l @ ôaU =X Y0 ² / }ü< L h,^ w I OP 3 è8 °Á= Â ² * { ,3 ü ,À8 I :¬,À8 .

(58) > @. ) . 1. . 0. <. 1*. . @ . . . ( .

(59) . (C . 6:. .. . $ . . . :. I+. . 0% . <? D 9

(60)

(61) . 5 . . .;:/ 06.;/6/ #. ? . E6A. F3. . . 0.

(62) . . . .,A. . ?.

(63) . . . . 6;"A.

(64) #. . . >. 3. . 0.

(65). ?. >

(66)

(67) . . 6. . . (3<&'+? GD. . . 3<< . 0. <?. <. . 6. H

(68) . . . 3== . =?. =. . . 3

(69) .

(70) > . . 3 . 1*. ?. . . 0,!:. 0. 6. . 1. 399 . 9?. . . < ;<. = . 9. <. = ;. . . . 0%!6. ?. . 9. . . .

(71) 3.

(72) . . . 6.

(73) 3?. 3. . . . . . . 0. + . . . 1

(74) . :;0/. + . . Schematic diagram of columns with different ZVI installation and electrode arrangement. The left side of each column is inlet of artificial groundwater..

(75) .

(76) ! " Iõcü / 01

(77) ?<= 1> ~49 Ù;, ½L L Kô,À8 X KLº< @ 08 #sKL 9 ³,^ 3 HI ZZff äå 1¹º û9 Ù;,À8 Ù;@ ºR < <E< L=* X µ 0 dÓ{ . dÓ{ z 0ø "< / 01,À( HI Kô,ÀHp Cf< L äå p<= gI ¹Õ 9 ¶0N %% È; Ù;,À8 * 1> é£M !", Ð 8 / 01,À8

(78) <= ÖUI { 0/ 1 Î* r è0 %% KM 8´ Kô< 01Mã8 Î é£4 ² / ¾Ã, þ@ äå9 l # é£ 1¹ » 0C º/ ¼ ½L < f,*$ % . ÖU äå0 * / : â ¬; kf/ È^Ú8 / U1,À8 % Î FE ¡t3I z<* 8 < f,* %% ó ,À8 ¿<= X KLº kf* Î r ü. &8 " w"ý< kfÞ/ '0 ½L

(79) 9 01L k,^ 1¹ 56º9 9 01L m[HI v,ÀH- kf Þ. X ªM 0?[R ( )ò9 ** Ð,À8 23 µ 0 dÓ{ . 4 567@ 3[ ;ê! "< h[R ª $ '- ., /= < . ). 9. &. . (

(80) . '.

(81) . . &. ).

(82) . =

(83) . &. *1. 9. )*

(84) D

(85) . 6/ . /60 . . .6/<. /0:. . . )(3:. <

(86). ,.:/.

(87) . .

(88) = D <. 91. //. &. <. 9. &.

(89)

(90)

(91)

(92) . . 9. . . 3. . . .

(93) 3>

(94). . D D <

(95) . 9 > . 8/.;. 1. 1. . :. /. . &(<. &.

(96) . . 9. 0/. . . :/6:. 3 3

(97) . ///; ://. 6. . <. *. . ? .

(98) '-. . <. 9=3,0". . . . /. . . <

(99) . 6/. = >

(100) . . /:6. . . (<. Breakthrough curves of TCE through columns packed with different ZVI installation and electrode arrangement..

(101) .

(102) MMF. function coefficients and regression results for columnal experiments. Coeeficients of MMF function. a. b. c. d. C/C0 r. Integrated Treatment C/C0 effect 1000* (%). C0/2 (mL). C0 (ppb). Measured normalized effecta. Combination. Calculated Synergic normalized effect(a/b) b effect. 500*. 1000*. Aa. 0.0002258 11.25983 1.060246 0.8960395 0.9964 0.897. 1.017. 1.036. 979.548. 2.045. 13.1273. 1256. 2568. Ab. 0.0012047 9.301505 4.205710 0.1694200 0.9583 0.800. 0.992. 1.083. 958.424. 4.158. 3.7679. 1209. 5028. Ac. 0.0003298 5.481229 0.9984507 0.7678002 0.9814 0.861. 0.954. 0.972. 925.915. 7.409. 9.1989. 1126. 8340. Ba. 0.0058437 2186.477 0.8590021 1.841723 0.9759 0.593. 0.840. 0.853. 770.023. 22.998. 77.3975. 597. 13738. Bb -0.0108940 146.1777 0.9551469 1.221579 0.9788 0.622. 0.889. 0.926. 819.854. 18.015. 65.0545. 1654. 29794. Ab+Ba. 18766. 1.59. Bc -0.0120400 36.26596 0.9216668 0.8487296 0.9688 0.528. 0.775. 0.834. 719.147. 28.085. 86.4601. 1126. 31617. Ac+Ba. 22078. 1.43. Ca. 0.0970142 1600.629 0.9882349 1.764508 0.9249 0.702. 0.964. 0.981. 891.503. 10.850. 58.7135. 866. 9395. Cb. 0.0245094 293.9793 0.9618962 1.341551 0.9644 0.608. 0.897. 0.932. 823.569. 17.643. 70.4853. 709. 12510. Ab+Ca. 14423. 0.87. Cc -0.0249040 37.69200 1.009547 0.8586752 0.9665 0.576. 0.851. 0.915. 787.819. 21.218. 70.9080. 2273. 48239. Ac+Ca. 17735. 2.72. Da -0.0209966 672.5574 0.8944265 1.320458 0.9852 0.340. 0.752. 0.832. 664.745. 33.526. 171.0060. 1299. 43543. Ba+Ca. 23133. 1.88. Db -0.0191107 2187.649 0.8587402 1.521042 0.9586 0.275. 0.730. 0.809. 634.647. 36.535. 200.1495. 1475. 53904. Ab+Da. 48570. 1.11. Bb+Cb. 42304. 1.27. Ac+Da. 51883. 1.27. Bc+Cc. 79855. 0.82. Dc -0.0088223 9284.693 0.8547326 2.010142 0.9812 0.449. *Integration of treated water volume (mL).. 0.826. 0.847. 735.147. 26.485. 112.6049. 2485. 65814.

(103) . 100*.

(104) ! " pl uk ê!0I < U1{ kf* d 56;f/ (É « f/ .I 56;f ý0* ¬,8( 3 3 <= + £,M* µ / ,( ,ÀH - 0 P-.< °Á kf Þ/ È0I ( )8 < T 56< .d "_ Þ3 )ò ? ~;<= 3/ Lp* ¶@ /0y R

(105) Q kf 56Q hi[9 (É , þ8 °Á= ^V e Kô² < .d [ « äåõ8 u kf< ý0. )HN x OP{ Sf %% 8I { ÜÝ ukfX D >

(106)

(107) 9 ,À8 K ' >

(108) 0 .d 1@ ?. / È^Öã { w]9 4 û HI 56Èi % 7I äå0 .d \]0 1@ ¶HI 8 ç8 (ab + cx ) Y = --------------------;M þ( Ä"M* kf* m ¡ (b + x ) .< °Á ¡..9 È0*$ 0* : ÿ * % 1@ m «¤< &. M* 56 8< = R{ ¶HI= Â <=* m9 <= Z} ÄÅ ¾Ã½Ã< °Á Þ / 01L ¬;,¦ (;á .,ÀH- u . 2M- ~ äå0 ¬ p<= .d &@ "kf/ ÈR8 cV-

(109) m< mÞ w]9 9K]I 2L Èi . &. ///. *1. *1. . . . . . . . . . . =. . 9. &. d. - . //. ://. ///. <. 2 >>

(110) ? 0. d. 5. . 1. 0///. *.

(111)

(112) . .

(113) . <. =. . . 9?. . . . Changes in physical properties of column effluent as the function of treated water volume: (a) flow rates; (b) direct current (mA); (c) resistivity (kΩ); (d) electric conductivity (µS/cm). Symbols are same in Fig. 3.. .

(114)

(115) .

(116). . Variations in chemical characteristics (pH, Eh, and DO) for each column. Symbols are same in Fig. 3.. Z5[HI m0 ªM* b9 :8 5i Ù;{ Z;û 9 56Èi OP S0 ?[HI ®@ äå0 .d ;0 [¦ -ç<H- c 8´HI* ; 0 ³@ ¶HI -ç8 =3 äå@ u< 3 È8 ;0 =H- 0 i= ý ¡.,* b9 ÈR8 x ZZffû ß u<* Ñ. c ( 560 ý P-Mi= äå0 ç äå< wL 1¦ {8 OPQ0 è* äå<=* Ñ Þ. 2M þ>8 5i OP0 )* äå <= 1" 1>@ u ?[ 1"Ý % í @½ < 0* ¡.. 2{8 äå<= * 8± äå<=X U40 ZA è* ¬[R ) " . . . ". . . 93. 3. . ". 93

(117) . =?. =. . . . . <3. . : . . //. ). 1. :?. . ). ?. !; /. . . =?. 9?. 6;:. ). = 93 . . ,B0 £¨ 8 x ºJZ½ * < °Á ª,æ 0? KL. ¬- þ* í 1>0 MI 8 ¡.,* b0 C -ç8 cV sÎÿ u 7.// <= 76// p l m[R ª. -ç-* äå@ äå08 1¹ ºÝ ß u 0ãH- äå9 l OP0 ¾Ã{ äå<=* sÎ «ÿ K *1 plI ¿;Mã8 . 9. *1. . . =?. ?. 9 . :. . . Z/ 01, þ* äå wL Èi ?tX ,t< %% ¾Ã äå .

(118) . ?. 0. = . .

(119) ! " \]9 æ û< wL ? ,t< < ¾ äå@ OPQ oÝ0 R$ wL Í Ã,* \ äå z { ÜÝÚ \ f ÄI .d 1( ÜÝ< )=f 8 HI % ÄI \ . 8 cV- ytZJ P=I

(120) \]0 .d 18( 3 3 9 01,* z \ äå@ ÄI )8 % \ ?D9 .C 5i \ äå@ ÄI

(121) É \ . EF9 Æ u m< ÞÝ9 9K]I 563 « Z 3 )8 0* 9 01 zX ytZJ9 / 01 < 01,* z T< 01M* Z 5[R ª b@ äåõ8 . º< L ê"M* ZX < L L ¬; |QHI ,3/ ,À8 ,æÁf ä M* Z< G\ . £¨9 8 x å p<= ø } Þ< °± äå p g =X 3 äå<=X Y@ ê¯< n 0< ;0 -ç-* ¶HI ÈR8 0V m HI 56ÈæÁf äå@ Ä ¡ª@ u äå p OPR . ¯M f. &@ »3º9 ©Zi= }9 ª äå@ ÄI ºM «¤0N 0V ©Z ² ³1@ äå äå<=X Y@ Í \ * -ç- þ*8 x X ytZJ9 < 01 ² / 3W y²{8 5i Ù;{ Z;û0 01,^ Í \ @ ytZJ9 %% H [HI U1,^ ,* z È8 U1HI äå BHI Z;û0 ¡.,*$ [@ ;@ %%< L M* ÜÝ 0?HI M J¢ Zt RS9 ø,N x "3 p 1¹ * ?D\ / ºL Èi Ù;{ ² X %% 0C4K Ý0 1@ ¶9 ø8 0* Z Zffû0 ç äå< wL 1¦ M* ¶HI T n9 01,^ º ² / w 9 « äå0 .d z3,N äå B08 ~ '©{8 =3 äå@ u< 3 È8 ;0 äå z OP{ S0 äå =H- 0 i= ý ¡.,* b9 < wL Ñ Ä- ®´<f I,( 0V ² / - È0*$ u< ©Z0 '

(122) ß9 çJ¶@

(123) É \]0 EP8( 3 3 )8 , «¤R ¶HI ¨%{8 0* =3

(124) äå0 :[R ~K@ ´}9 ,t< ¾Ã,* ¶0 w U@ \]9 È0* 0. .j40 8 [ \ . 1@ ¶HI -ç-*$ 0* 3 Ä < ,3 0êb Z 0êb0 5 <3 äå<= ) Þ. 2M þ@ ¶@ 5 R z Z 0mf. ø%,-õ Ei= 5 60 u< "A{ ¶ Ë ÇÌÁ U{ ,3 p 60 dMã «¤HI ¨%{8 , z ?tØ< ´}0 ¾Ã MæÁ < ZLQ S0 w[ [ µ «¤< ¢ f X ²M )HI ytZ/ L' z £ ZKL » 1L. ¬- þ>´9 Æ ,t Ø< ´}0 ¾Ã { zÈ8 { 3 )8 5i OP0 )* # n äå ÜÝ@ E- X ytZJ9 < 01,* <= 1" 1>@ uí » 1L< °± 1 z %% 01,* zÈ8 \] Í\ ¹0C ¡.I ZKLf VW J¢ £¨,^ ´ * 8 S}9 < ¾Ã z ¯0 £ }<= £¨M* 0C< L ¡.. ¨,^ êU4 Ms0- c l "§m9 (; 2{8 äå<= 56³ 0/K;f<= £¨ * b0 )HN 0« Næ 9 ) ,B@ 8± äå<= U40 ZA £, O* 5i ´}9 < ¾Ã z l ytZ M þHI 0Z äå U1 Qº OK JHIí J¢ M* Z< L G M þ@ äå G< T/ P,¦ MN * ºM þ( R ¬[ ?HI ¨%{8 äå 3 )8* J . ³ [1 <= :[HI ¡.. 2M þ@ ¶ M( )´9 È^Ú8 @ U1{ U ,3 n49 .Q z AB c ( ytZJ9 01, þ* 0" ZKL< J £¨ HI ) 567< \ . 1* , ¡.. £¨,* ÉX9 È^Ö* ¶08 0 . . 9 = 7. . 0%.. . ... *0. . . 9?=?7?. . 0%. 9=7. . . /.0. .

(125)

(126) . &. . . 9. . 9?<?79 . 9<79 . . 0%. =?. . . . 9. . . . . 93 3 =3. . . . . . . =? = 9. 9. . . . = . . . . . . =3. //. =? . . . '*. . . = . . . . . . −. ). . ). ?. . . D. .

(127) . . &. 3>

(128)

(129) . . .

(130) . .

(131)

(132) . . <? <. <. 3 . !!6. 9. < . ). .

(133) .

(134) . −. ). .

(135) * ?<= OK î9 0Y

(136) 3. ÇZ U{ ,3/ U1 ¶< R,* ¶HI [A{ 8 U{ ,3 ³ U1{ % 31> p . e Æ\ 49 ] «¤< p L

(137) <= * 0/ º4 / 01L no9 ,À*$ 560 P-.< °Á ^O j0 ?{ ¶f ?D9 ¬ f,À9 ¶HI [A{8 ÜÝ0 / u Lf m[R º JZ½ ª. -ç-* äå@ S 0 ® «¤< \]9 (É, þ( 567 3W9 î.8i ? äå0 d U1.j 5 67 ¾Ã08 0* ? äå z ð{

(138) \ * E 56Q0 % _ d < L` OP0 ºMi= m[R T/ ¬H* ß9 ,À´ 9 8 0V T 56 ;f. % ý0/ È0 *$* ^V . .j40 )8 0* 56mf. º J { úeÞ3 r 1¹ºÝ 1¹ Ý ,3 p ´0C G< úz aª, «¤08 ,3 p ´0C@ hi 9 Èb 3 )* º& c9 dHI ¯9 nd8 °Á= m[HI » 3 ¨49 £¨ â8 ~ ) X 3* » ¯9 3 )* ø¨ ¢ <ÍJHI ³18 °Á= Â ² / /eHI f< ø¨9 g. äå9 01 d ìZ ² . ÈO{8i æ d< Ô$ ² / *9 3 )9 ¶HI h ?{8 . . ).

(139) @.

(140) . I I. . I '. .":#. ). .6!#. #. I ). I . &' ? ?>> . ..,#. .6.. ). . ). . :/// 1. 93. . . .

(141) * 0 «¤HI ¨%{8 5i äå \]9 (É, þ( 567 3W 9 (É8i OPÝ0 [´<f I,( ÿ ºJZ½ ª. m[HI £ ¨ äå0 .d d U1 .j 23 4 567 ¾Ã 08 0 / :L ,3 p

(142) Q 0 234 567 @ ytZJ9 U1,* z M* S È8 ytZJ9 < 01,* z 1Ý0 ¡ 3 )HN Z} ÄÅ ¾Ã ½Ã< °± ~K0 ÏRMã8 cVI ¾Ã w10- n ¾Ã< [R 0 .L* z 8± + `ìag/ ¢1,^ \]9 } j 3 )´9 È^Ö* "_ uÎ/ ¶HI ¨%{8 . . . :///. . 1. ?3

(143) . . &. . . . . . . . . . . . . ). . . . . $. . 9 D . Â k¤ µU/ µ,¦ ,^Öl Ñ K µU ½J PµHI ªU OÌ8 Â * ÕA m[u nb w< L 3-Mã´9 ·oÌ8 p< pQ LÚ q S<¦ r @ ªU/ OÌ8 . . 5 0///303 6 //3//"36 . . . !!".

(144) . ( . . !! #. - . !!:. − . J

(145) . . !!%. . . . . . . . . ""

(146) # " $ %& ''

(147)

(148) ( "

(149) ))( * "+ "

(150) , -+!. +) ( ) #

(151) . ' !' / 0 , 1 0+

(152) 2 ) , " 3 '' 4"+ "

(153) , *

(154)

(155) 0+ 1 " $ '' *

(156) + * )+

(157) * . e äå " X ytZJ9 < U1,* z & J[ T/ P0 Ï RMãHN 0" ¾Ã{ OPQ S9 (ÉL 3 « ,t< / ¾Ã,( Z} ÄÅ@ ?t< S}9 ,t <* ´}9 ¾Ã,* äå0 .d 1@ \]9 -çpã8 0* Z ì êb 3 Ä. 5. M* zI= ø %,-õ Z 0mf. iÉi= KL56< Ö . . . . . +) , !

(158) % , 5 !. 0. . cd ce fR gh ij + k

(159) lB d mDnb oXp 2?<dL !. . . 3

(160) . . . ) )+* " 4 ( ) * )! ) *

(161) () * (" ) # 5 ! 5 1 ) 1 # $$ " 2 %0 ''5 6 ) *

(162) , " , ( + " ", " !. 7 (

(163) #

(164) 5!5 & , & 8) 94 6 : 0 "

(165) ;) 1. %2 , < +( 1& < ") =1 8

(166) < %

(167) * $1 " 2 $1 '' < *

(168) "!)

(169) ) *

(170)

(171) "

(172) +) , *

(173) ! ,) * >!?> ' , + "@

(174) +(A 94:&?.

(175) ! " $! A. 9 2. 4",. :

(176). & 7 . 9 2. 4", :. .

(177) " "

(178) ! ( " , + "@ +) ,

(179) ? ;" " (

(180) !. & )2 !6 B () # $

(181) 7+ 4 # . * " ;") * (" * ( . 0 " : " C : '' , " * 7 .

(182) % )) F ) * )).

(183) " ) * " )+

(184) + ! , ( + ") ( ) ' . !. /'.

(185) ! " (" *

(186) ! !. $ 2 % B % " #. $ ''' $

(187) " )

(188) ))) , +

(189)

(190) +( ) 1 B " $ 5/ ! $ ) &1 " 2 %0 '' 4"+ ". 4 D & #D

(191)

(192) )) $% " $ B!# . .

(193) , *

(194) " ( ) 7 (

(195) #

(196) / .!.. ( ". , + "@ . +) ,. !

(197) . # B

(198) < . . . 1. 5! 5. # 0 " 4 " $ ''.

(199) " ! "

(200) , *

(201) "

(202) ) +) ,

(203)

(204) ! "+( " " , * ( * ( " @ ( ) 5 .!/ . $ , 1 '' " % " " :

(205). #+ " %+

(206) ) 48 ''' 6 ) *

(207) . <)) * ) , ) B +) >. "+ 7

(208) " E % ( . .'. ** , " (" . %

(209) ) 1 :"

(210) )2 11 $

(211) @)2 61 # (. "+) #

(212) 5!5/. 4$ B7) # " 8 '' 3 ",!. 2 %0 1 ) & # $$ " 2

(213) . " * (;"! , @ )) 7 ( 7

(214) ) . 04 '' 4(" , , + " @ @ . + +)!

(215) ; ""!7" 7 ) !.

(216) (

(217) )E (

(218) )" ) 7 . #

(219) . 5!5.. "), 0 + " 8 $ 4(" . %

(220)

(221) ) B 0+ 3 8 ) 3 4 D & , & " & #D %* (

(222) + * . .

(223) 7 E $

(224) ,

(225) . )) #

(226) 5'! 5 % +7 ; $ ' 5 <

(227) ) *

(228) (

(229) -+

(230) 7 %, ( %)) 9;* " 55 4 " 1 ''. < 7 ) * , +

(231) E $ )+( " * " ,

(232) + #

(233) ' '5!'. 4 D ''/

(234) (

(235) (" * " +!. /! ,

(236) $ ""

(237) # " $ %& '/ )! * ( *

(238) , "

(239) ( + ") ! #

(240) / . ! 5. 8 ) &1 % 2 0= " <

(241) %1 '' F!

(242) * " " , )

(243) " *

(244) * ( ( 7

(245) )( 7 (;" ( , +

(246) + #

(247) //!//.. q r s 1 t. . .. '. q r s uvwx. . 5. .. .

(248)