314 8*%9 JournalofXi anuniversityoftechnology(2019)vol.35no.3 DOI:10.19322/j.cnki.issn.1006 4710.2019.03.007,-./01 / 234567,,, ( 8*%9 :; %<=>?@A, 8 710048) :!"#$%&!' (Ultrasound/SpongeIron/Potassium Persul fate,us/si/ps) ()*+,-,./ ' 0#$%1, ()*(Sulfadiazine, SD) ph 2 345+67 8-9:, ()* 15mg/L,; 2 25, 56 W, ph=9.0±0.1,' 0#$%1 0.4g/L 00.6g/L, ()* 30min+ <=93.3% US/SI/PS ()*+'>?@ABCDE US/SI/ PS ()* FGH( )0IHFGH(HO )+J@KL #$%+M NO8-9:, L, ()*30min+ PQRS93 %TU,XRD VW:#$% 9XY + Fe 2+! B > UQR #$%+&! :;#$%;' ; ()*!"#$:X703 %&' :A % $:1006 4710(2019)03 0314 06 犛狌犾犳犪犱犻犪狕犻狀犲犱犲犵狉犪犱犪狋犻狅狀犻狀狌犾狋狉犪狊狅狀犻犮犲狀犺犪狀犮犲犱狊狆狅狀犵犲犻狉狅狀 / 狆狅狋犪狊犻狌犿狆犲狉狊狌犾犳犪狋犲狊狔狊狋犲犿 LIWenying, WEIHong,ZHANGJiatong,YANG Xiaoyu (StateKeyLaboratoryofEco HydraulicsinNorthwestAridRegionofChina,Xi anuniversityoftechnology, Xi an710048,china) 犃犫狊狋狉犪犮狋 :Thedegradationofsulfadiazine(SD)intheultrasound/spongeiron/potassiumpersul fate(us/si/ps)system wasstudied.theinfluencingfactorssuchasaddingamountofpotassium persulfateandspongeiron,sulfadiazineconcentration,initialphvalueandtemperaturewerein vestigated.resultsshowedthatthesulfadiazinedegradationrateachieved93.3 %in30minun dertheexperimentalconditionsof15mg/lsulfadiazine,25,ultrasonicpower56 W,initialpH valueof9.0±0.1,potassiumpersulfateandspongeironaddingamountof0.4g/land0.6g/l, respectively.sulfadiazinedegradationintheus/si/pssystemfolowedpseudo firstorderkinet ics,withtheoxidationofsulfateandhydroxylradicalscontributedtosddegradation.therepli cationexperimentindicatedthatsulfadiazinedegradationratein30minstilremained93 % even ifspongeiron wasusedthreetimes.xrdanalysisshowedthattheferrousoxideproducedon spongeironsurfacemaintainedthecatalyticactivityofspongeirontoacertainextent. 犓犲狔狑狅狉犱狊 :ultrasound;spongeiron;potassiumpersulfate;sulfadiazine 45BC D(Sulfonamides)E 4 5 FG B H I J K L,M N O ; C H 45BHI N PQ RS C TUVW>, XY 9 N Z[ \] ^_`a bc V ( I G,45BC D X [1 4] J P(ng/L~μg/L), E N U V >, = OB J8 [2,4], 45BC D J = J ]? [1] R / + )* 23 I W N (HO ) / 4 :2018 12 29 : (51979223); (2017JM5082); (2013slkj 07) :!"#,$,%&',, ()* + E mail:331644417@qq.com
!"#,V:,-./01 / 234567 315 [5] 5BC D J O 3 Fenton / [6] [7] UV/H 2O 2 γ /H 2O 2 V HO, Y(30~40μs), J ph, N / J + U,-] MV / [8] \, D J (U [9 11] E Fe 2+ / ph IJ23 Y,? JU " 9 % J, PQ, NJ01 (SI) ( /, (PS)( /,, -,0 1 / 4567(SD)J23S, (45 BC DJ)* G 1 ()* 1.1 +, 01 (! b " #, $ 9 N 95 %); ( % &,' 9 / );4567( () ( 0) "#,& 9N99 %), * :C 10H 10N 4O 2S, F +,1 -.(/T&,01 ( 0) "#); ( %&,U 2 34 "#);56 (' 78/ "#,& 9N99%);9 / : ( %&,' ';/ "#) 5minW, 0.22μm!, Aglient1200 %4567J,23 (: 23 =( 犆 0- 犆 )/ 犆 0 100 % (1) : 犆 0 ] 犆 ( 0 ] 狋 4 5 6 7 J (mg/l) 1.3.2 4567J HPLC % /TG( EclipsePlusC 18 (4.6mm 150mm, 5μm); (-.:,&=25 75(V V);c 10.0μL; 0.30mL/min; K Y269nm;G 30,,4 5 6 7 J 狋 R = 8.408min 1.3.3 J 3 TUVWG ( 5 min W ), 0.22μm! _ / K J, J 3 (: 3 =( 犆 PS- 犆 )/ 犆 PS 100% (2) : 犆 PS] 犆 ( ] 狋 J (mg/l) 1.3.4 *J % */T % > AS19 G(4mm 250 mm, ),AG19 G(4 mm 50mm, );S L,50 ma;,ecg Ⅲ KOH;,1.0 ml/min;c,25 μl;g,30 ;, * J 狋 R=13.867min 2 /0(1,1 4567J F Fig.1 Chemicalstructureofsulfadiazine 1.2 +,-. SCIENTZ ⅡD, - (< = I "#),> 8.0 mm? @ A,DC 1006 BCDEC Aglient1200 /T,> G1311A F,G 30,G1314C XL H Y IJ KL MNO 8ICS 1100 */T,> 2.1 23456789:;,- 56W 25 ph=9.0 ±0.1 PS]01 c (0.4g/L ]0.6 g/l,4567 15 mg/l, 4567J23 <+,2 P Q (RFC 30),ERSdionex AERS500 4mm R *S L 1.3 +,)* 1.3.1 4567J,-23 TUVW G 4 5 6 7 X N 200 ml Y, Q 250 mlz [, 1.0mol/LNaOH \ H 2SO 4 ]B ph ^, G 01 ],_,- ` T9abc )*,@ (1.5cm,2 4567J23 Fig.2 Sulfadiazinedegradation underdiferentreactionsystem
316 8*%9 (2019) 35 3,2,,-(US) US/SI SD J S, 4567J,- J ( (3)),B [12] US/PS SD J23 (7.08%,, -C / \ SO [13] 4-,,- V DJ SI/PS S R SD J23,23 24.17% 01 3\ J Fe 2+ / PS\ ( (4)),-cG. SI/PS J / S,SD J 2 3 93.3% E (, -. / 0 1 3 \ Fe 2+, / \ 9 [14] ( (5)~ (7)) S 2O 8 +,- 2SO 4 - (3) Fe 2+ +S 2O 8 +SO 4 +Fe 3+ (4) H 2O HO +H (5) HO +S 2O 8 S 2O 8- +HO - (6) HO +S 2O 8 HSO 4 - + +1/2O 2 (7) 4567J23 < TG ;, + 1 1 456723JTG ; Tab.1 Pseudo firstorderreactionkineticsofsulfadiazine indiferentreactionsystems 犓 /(10-3 min -1 ) 2 犚 US/ SI/PS SI /PS US/PS US/SI PS US 79.9 10.1 1.5 1.4 1.4 1.3 0.917 0.943 0.930 0.907 0.930 0.938 c (0.4g/L 0.5g/L 0.6g/L 0.7g/L,SD J2 3 ( 74.85% 79.9% 93.88% ]93.76% E ( 0 1 J c, \ Fe 2+,Fe 2+ / PS \ ( (4)),SD J23 01 c 0.8g/L,23 2P 44.57 % E ( Fe 2+ ] ( (8)),,SD J23 [15] Fe 2+ + Fe 3+ +SO 4 (8) 2.3 PS <8=> 2.1 B,0 1 c 0.6 g/l,ps 0.2~0.6g/L SD J23 +,4,4,PSc 0.2~0.4g/L,SD J 2 3 PS c J R PS c 0.2g/L 0.4g/L,SD J23 50.28% 93.88% PSc 0.5g/L,SD J 2 3, 2P PSE J,PS c 9,,-]01 J / \,SD J2 3 PS c, \ J (9)~(10) [16],SD 2 3 + S 2O 8 (9) +S 2O 8 SO 4 +S 2O 8- (10) 2.2 <8=> 2.1 B,0 1 c SD 23J +,3,4 c 456723J Fig.4 Efectofpotassiumpersulfatedosageon theremovalrateofsulfadiazine 2.4?@ 狆犎 8=>,3 01 c 456723 J Fig.3 Efectofspongeironaddingamounton sulfadiazinedegradation,3,01 c 0.4~0.7g/L,SD J23 c J R;01 2.1 B, 1.0 mol/l H 2SO 4 \ NaOH ]B ph ( 3.0 5.0 7.0 9.0 ]11.0( ±0.1),SD J23 <+,5, 5,pH (3.0 5.0 7.0 9.0 ] 11.0,SD J 2 3 ( 98.17% 97.01% 95.85% 93.88%]70.08%,SD J 2 3 ph
!"#,V:,-./01 / 234567 317 2P, N Jc, H + HO - W, Fe(OH) 2 I J \ [17], Fe 2+ / PS;,Fe 2+ Fe 3+ 9 /I 01, / Jc? @ _ 1.0 mol/l NaOH > SD X, ph ( 9.0±0.1,SD J 23 93.88%,US/SI/PS S / SD 2 3,?@ ph 9.0 J (: 犈犪 ln 犽 =ln 犃 - 犚犜 (11),US/SI/PS 2 3 SD J / C 犈犪 =20.577kJ/mol 2.6 DE 犛犗 4 B 犘犛 8":,7~8( 30min, SO 4 ] PS 3 J,5 ph 456723J Fig.5 EfectofinitialpHonsulfadiazinedegradation 2.5 ABC 犛犇 9:8=> 2.1B, ph=9.0±0.1, 01 c 0.6g/L,PSc 0.4g/L, SD 23 < J +, 6 ( 15 25 35 ]45, 30min,SD J23 ( 66% 93% 88% ] 85% 15 ~25,23 J R ;, 25, 23 2P,PSEG ]J /, Fe 2+ J /, R C D J \ [18],7 * Fig.7 Sulfateionconcentrationindiferentsystems,8 J 3 Fig.8 Decompositionrateofpotassiumpersulfate,7,US/SI/PS,SO 4 ] PS 3 RN US/PS ] SI/PS US SI PS / J US/PS SO 4 R 2 P, E (, - / \ J ( (12)) * *( (10)); c, J, * 2P,6 4567 J Fig.6 Efectoftemperatureonsulfadiazine degradation / G J Arrhenius" [19], HO +S 2O 8 HSO - 4 + +1/2O 2 (12) 2.7 # F& [14,20 21], ] HO J (1.6 10 7 ~7.7 10 7 L mol -1 s -1 ] 1.2 10 9 ~2.8 10 9 L mol -1 s -1,
318 8*%9 (2019) 35 3 100 ;56 ] HO J ( 4.0 10 5 ~9.1 10 5 L mol -1 s -1 ] 3.8 10 8 ~7.6 10 8 L mol -1 s -1, 1000 ; ] HO J ( 8.8 10 9 L mol -1 s -1 ]6.6 10 9 L mol -1 s -1 ] J [22], 56 HO?@ 5 6 ] SD 2 3 <JS, +,9,10 =?@ Fig.10 Reuseexperiments :Fe 0 (0.6g/L,PS (0.4g/L, ph=9.0,25,9 S 4567 J Fig.9 Freeradicalefectofinhibitorsonthe removalrateofsulfadiazine,9, 56 ] SD 23 G < J S c 5 6,30 min,sd J23 93.8 %2P 79.68 % 68 % 56, JS, US/SI/PS23 SD J E, N! I (SI), " PS SIJ ># $,23S 2 [23] % US/SI/PS,SD 30min &23 6.4%(,9), N ]56 (S J 68% ] 79.68%, US/SI/ PS23 SD JS '., / SD SIJ 2.8 8GHIJ,10, / = 3,SD 23 93% E (01,\ J Fe 2+ /I 01 (, G <. SD J S J 0 1 c X ) (XRD)*+, +,11, J01, J 0 1 2θ ( 45 65 77.5 ) -. J/0 1), J 01 \ J Fe 2+,Fe 3+ J /I 3 /,11 01 J X, Fig.11 XraydiagramsforHouhai ferricironwithdiferenttimes 1)US/SI/PSC S /234567, < TG ;;ph,ps RIc, V D4567J23 G 2)US/SI/PS J /S N SI J / 01 Y, =,2P J KL%&: [1]234,56,7 8,V.9 8:45BC D J 1 ; [J]. /,2017,36 (12):2574 2583. WANGJiawei,WEIHong,YANG Xiaoyu,etal.Oc currenceandecologicalriskofsulfonamideantibioticsin thesurfacewaterofthe WeiheXi'ansection[J].Envi ronmentalchemistry,2017,36(12):2574 2583. [2] BARAN W, ADAMEK E,ZIEMIANSKA,etal.
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