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1 w y wz 9«( 3y) 177~184, 2006 J. f the Krean Sciety fr Envirnmental Analysis ys» ƒ w p y ½ «Á«Á *Á y w, *swœ w y Characteristic Variatins f Heavy Metals in Fly Ashes frm MSW Incineratin Plants by Thermal Treatment Kim Sam-Cwan, Kwn Myung-Hee, Sng Geum-Ju*, and Jen Jng-Ju Natinal Institute f Envirnmental Research(NIER), Envirnment Research Cmplex, Segu Kyungse-dng, Inchen, Krea *Phang University f Science and Technlgy(POSTECH), Nam-gu Hyja-dng, Phang-si, Kyungsangbukd, Krea The characteristic variatins f heavy metals in fly ashes f municipal slid waste (MSW) incineratin plants were investigated by thermal treatment using a labratry-scale setup. The fly ashes were cllected frm spray dryer absrber/bag filter (SDA/BF) and electrstatic precipitatr (EP) and thermally treated fr three hurs at a different temperature f 350 C, 450 C and 550 C. Raw and thermally-treated fly ashes were analyzed by X- ray flurescence spectrmeter (XRF) and X-ray diffractmeter (XRD). XRF's results shwed that CaO was cntained at a rati f 40 % t 50 % in raw fly-ashes cllected by SDA/BF, and 10 % in raw fly-ashes cllected by EP. XRD's results shwed that raw fly ashes cllected by SDA/BF mainly cntained CaClOH, Ca(OH) 2 and CaC, but thse cllected by EP, NaCl, KCl and CaSO 4. Calcium cmpnent in raw fly ashes f SDA/BF was due t the spray f lime (Ca(OH) 2 ) fr cntrlling acidic pllutants at SDA. After thermal treatment f fly ashes frm SDA/BF, CaC rati was increased with the decrease f Ca(OH) 2. Ca(OH) 2 was decmpsed t CaO and H 2 O, then CaC was frmed frm the reactin f CaO with CO 2. Key wrds : Fly ash, Thermal Treatment, MSW, XRD, XRF 1. ú y y s» ƒwš, s» ƒ w ƒ š, ƒ w ƒ š. p, ƒ w ƒ z,» '90 ¾»» (Electrstatic Precipitatr) k (Wet Scrubber) '90 l k (Spray Dryer Absrber)» (Bag Filter) ³. k ƒ z (Ca(OH) 2 ) wš,» y k p (Duct) š, ƒ ƒwš. p, Pb, Cu, Cr, Cd, Hg w,, PCBs (Cplanar PCBs) x j (HCB) w» w 1-4),»e w w m w, w ƒ œ, y š. wùƒ Hagenmier w T whm crrespndence shuld be addressed. kscnier@me.g.kr
2 178 ½ «Á«Á Á š «w w» w w»., 350 C ~550 C k - w (C-Cl Bnd) ñ w 2,3,7,8-PCDDs /PCDFs (plychlrinated dibenz-p-dixins/plychlrinated dibenzfurans) Œ«w ù w yw y j». ù, š Š Ž ƒ» w k,» k. 500 C { (Metal Fume) k ƒ (Carryver) w»»» w. p, ½ 5) w 550 C 3 w w (Raw Fly Ash) w Pb 60~70%, Cr 50~ 80%, Cd 25~46%, Cu 5~29% w ùkû. w, ƒ», w k w 6-8), yw wxkƒ w p ùkú q 9-11). ù x ys» ƒ» 3 ƒ w yw y r, wz ù» v w» œ w » k sƒw» w x ys» ƒ 200 m/ A ƒ, 300m/ B ƒ, 400 m/ C ƒ w. 3 ƒ mf (Stker) ƒ s (Waste Heat Biler, WHB) š,» œ Fig ƒ A B ƒ e (SDA) e (BF) yw, C ƒ» e (EP) s ƒƒ w. r» œ x 12) 2 1w w, œ» yk w w š w w w x w 1,000 C¾ wƒ ƒ w 25 L», w x w (Fig. 2).» w, š (Thermal Fusin) w» n w wš» ü ƒ ¼ ù ƒ š,» ü ƒ Ÿ (Starved Air)» w» ü Fig. 1. Prcesses f incineratin plants t be studied.
3 생활폐기물 소각시설 비산재의 열처리에 의한 중금속 특성 변화 Fig Lab-scale thermal treatment setup used fr this study. 부온도 350 C, 450 C, 550 C에서 각각 3시간 열처리 하였다. 시료의 전처리 및 분석방법 물리적 특성분석 강열감량 (Ignitin Lss)은 폐기물공정시험방법 제 4장 제3항 강열감량 및 유기물함량 시험방법에 따라 분 석하였으며, 총 용존성 고형물 (Ttal Disslved Slids, TDS)은 시료를 폐기물공정시험법 제2장 제5항 용출 시험법에 따라 용출한 후 Standard Methd Slid 2540C (Ttal Disslved Slids Dried at 180 C) 방 법 에 따라 분석하였다. 입도분석은 비산재를 건조시 켜 분산제를 사용하지 않고 물을 가하여 초음파장치 (12.5 Watt)로 10분간 분산시킨 후 레이저 산란형 입도 분석기 (Mdel : 770 Accusizer, sensr HR-LD400) 로 분석하였다 화학적 특성분석 ph는 폐기물공정시험방법 제4장 제1항 수소이온농도 시험방법에 따라 시험한 후 수소이온농도 측정기 (Mdel : Crning M-240)로 측정하였으며 알칼리도 (Alkalinity)는 시료를 폐기물공정시험방법 제2장 제5항 용출시험방법에 따라 용출한 후 일본공업규격 (JIS) 0101 분석방법 중 산소비량 (ph 4.8) 시험방법에 따라 분석하였다. 이온성 물질 (Cl, SO )은 시료를 폐기물공 정시험방법 제2장 제5항 용출시험법에 따라 용출한 후 용출액을 이온 크로마토그래피 (In Chrmatgraphy, Mdel Dinex ED50)로 분석하였다 중금속 함량실험 비산재중 중금속의 함량실험은 EPA methd 3050B ) 13) ) 에 따라 전처리하여 유도결합플라즈마 발광광도계/질량 분석법 (Inductively Cupled Plasma Spectrphtmeter/Mass Spectrmetry, ICP/MS, Mdel: Elan600)으로 분석하였으며, 수은의 함량실험은 토양오염공 정시험방법 제4항 9항 수은분석방법에 따라 분석하였다 화학적 성분 및 조성 분석방법 산화물 성분, 특히 금속산화물의 조성분석을 위하여 원비산재와 열처리 후의 비산재를 105 C에서 건조시켜 X-Ray Flurescence (XRF, Mdel : Shimatuz XRF1700)로 UniQuant Methd를 사용하여 분석하였다. 또한 비산재의 성분은 X-Ray Diffractmeter (XRD, Mdel : Philips X'pert-MPD System)로 파장 Å(Cu)에서 Mnchrmatr를 사용하여 분석 하였다. 3. 결과 및 고찰 실험대상 비산재의 분석결과 본 연구를 위하여 선정된 소각시설 원비산재 (Raw Fly Ash)의 물리화학적 성질 및 중금속함량 등을 분석 한 결과를 Table 1에 나타내었다. 결과를 살펴보면, SDA/BF 비산재의 ph 및 알칼리도는 12.1 및 40~46 mgeq/l로, EP 비산재의 ph 및 알칼리도 6.7 및 1.2 mgeq/l 보다 높은 것으로 나타났다. 강열감량 및 탄소 함량도 SDA/BF 비산재가 7.5~10.4% 및 4.1~4.8%로 EP 비산재의 1.7% 및 1.0%보다 높게 나타났다. 이와 같은 이유는, EP 비산재는 소각로에서 배출가 스와 더불어 飛沫同伴 (Carryver) 되는 무기성 비산재 가 포집되는데 비해, SDA/BF 비산재는 SDA에서 산성 가스를 제거하기 위하여 소석회 (Ca(OH) )를 분무하고
4 180 ½ «Á«Á Á w BF w» w y k p (Duct) w ph e, k w EP w ùk ù q. wr, w SDA/BF Mg 9.8~14.4 mg/g > Zn 2.4~8.9 mg/g > Fe 4.0~ 4.3 mg/g, EP Zn 20.9 mg/g > Mg 19.2 mg/g > Fe 5.4 mg/g w, Hg SDA/BF ƒ 22~65 µg/g EP 0.5 µg/g w j ùkü., Hg w j,» BF (320 mesh) w w ù,»» Hg s, ƒ w q XRF y r» w XRF w Table 2 ùk þ. ƒ 21 w 100 % w ƒ ùkü A ƒ XRF r, 21 CaOƒ 50% wš, Cl 23%, Na 2 O 9%, K 2 O 5% š SiO 2 3% w ùkû. ù z y r, 9% w Na 2 Oƒ 550 C 3 z 4% wš w 350~550 C ƒ yƒ j w ùkü. Hg wš» q B ƒ 21 CaOƒ 40% wš, Cl 27%, Na 2 O 10%, K 2 O 7% š SiO 2 4% w ùkù, w A ƒ w ùkû. A ƒ B ƒ» ƒ w» w k z (Ca(OH) 2 ) w» q. wr, 15), Chang 16) w k š š w œ ƒ SiO 2ƒ 24~36%, 22% š w. ƒ œ w» œ ƒ w e s», A B ƒ ƒ y (Grate) x mf (Stck) ƒ» w x SDA/BF w ƒ x ƒ» w q. Table 1. Physic-chemical prperties f raw fly ash Items Raw Fly Ash Raw Fly Ash Items A B C A B C ph Mg (mg/g) Lss n Ignitin (%) Cr (mg/g) Alkalinity (mgeq/l) Mn (mg/g) TDS (mg/l) Fe (mg/g) Cl - (mg/l) 21,241 28,992 23,123 Cu (mg/g) SO 4 (mg/l) 1,036 1,076 5,080 Zn (mg/g) Cntent f Carbn (%) Cd (mg/g) Average Diameter (µm) Pb (mg/g) As (mg/g) Hg (µg/g)
5 ys» ƒ w p y 181 w, z y A ƒ Cl K 2 O ƒw w, Na 2 O MgO, Al 2, SiO 2, P 2 O 5, S, CaO ƒ ùkû. XRF ƒ xk, yw wxk y» A ƒ ƒw ƒ y w, B ƒ ƒ ü 950 C 1 2 y y j» w (NH 3 ) š ((NH 3 ) 2 CO, Urea) Œw» xk ƒ ù w A ƒ xk d, ƒ w ùkü d C ƒ XRF r, 21 Cl 29% ƒ w š, Na 2 O 23%, K 2 O 15%, CaO 10% š SiO 2 6% ùkû. ƒ Na 2 O Cl, S ƒ wš ù MgO, CaO, Al 2, SiO 2, P 2 O 5 ƒw ù kû. p, y w œ» w ƒw mf ƒ p»» w, C ƒ ƒ A B ƒ CaO ƒ ûš w Na, K Cl w» ƒ» w q XRD y XRD Table 2. Cmpsitinal percent f each heavy metal in raw & thermally-treated fly ashes (Unit : dry weight %) Fly Ash A Fly Ash B Fly Ash C Items Raw Raw Raw Na 2 O Mg Al SiO P 2 O S Cl K 2 O CaO TiO Cr Fe CuO ZnO PbO Br MnO SrO CdO BaO SnO SUM Remark : Figures in table are the cmpsitinal percent f each heavy metal t summatin f ttal items as 100%.
6 182 ½ «Á«Á Á w Fig. 3~5 ùkþ., A ƒ Fig. 3 e yw CaClOH > Ca(OH) 2 >CaC > CaSO 4 w ùkû ù, z CaClOH > CaC >Ca(OH) 2 > CaSO 4 ùkù Ca(OH) 2ƒ š CaCƒ ƒ. z (CaC ) ƒ, z (Ca(OH) 2 ) y e (Lime, CaO) y, ye yk w z q. Ca(OH) 2 CaO + H 2 O CaO + CO 2 CaC B ƒ Fig. 4 e yw Ca(OH) 2 > CaClOH > CaC >CaSO 4 w ùkû ù, z CaC > CaClOH > Ca(OH) 2 >CaSO 4 Ca(OH) 2ƒ š CaCƒ ƒ. wr, C ƒ Fig. 5 NaCl KCl e yw CaSO 4 w ùkûš, z f yƒ ùkû NaCl 800 C wƒ ƒ w, 350~550 C q ƒ ù» q. wr, C ƒ ƒ NaCl KCl w s» ƒ», w CaSO 4ƒ w v p, š «Ÿ Ÿ š (CaSO 4 ) m (Clay) ƒ» w q ~300m ys» ƒ SDA/BF EP 350 C, 450 C, 550 C ƒƒ 3 w, z yw y p X- xÿ» (XRF) X- z»(xrd) w r. 1. SDA/BF e k w Fig. 3. XRD spectrum f raw and thermally-treated fly ashes frm MSW incineratin plant A.
7 ys» ƒ w p y 183 Fig. 4. XRD spectrum f raw and thermally-treated fly ashes frm MSW incineratin plant B. Fig. 5. XRD results f raw and thermally-treated fly ashes frm MSW incineratin plant C. 40~46 mgeq/l, 4.1~4.8%, EP 1.2 mgeq/l, 1.0% ùkû., EP ƒ ƒ» ƒ s w, SDA/BF
8 184 ½ «Á«Á Á ƒ» w» w z (Ca(OH) 2 ) y k w» e k w ùkù q. 2. XRF SDA/BF Ca 40~50% wš š, Cl, Na, K 37~44% 4 90% wš. EP Cl 30% ƒ, Na, K, Ca 48% 4 77% wš. 3. XRD, SDA/BF ƒ w z w CaClOH, Ca(OH) 2, CaC e sw š, EP s» ƒ» w» NaCl, KCl v p ƒ» w CaSO 4ƒ š ùkû. 4. z XRD, SDA/BF Ca(OH) 2ƒ š CaCƒ ƒ ùkû, z(ca(oh) 2ƒ w ƒ w ye (CaO) y š yk w z (CaC ) q. EP j yƒ ùkû, NaCl 800 C wƒ ƒ w» q. š x 1. Karl Jachim Thme-Kzmiensky, Thermische Abfallbehandlung, EF-Verl.fuer Energie-und Umwelttechnik, 1994, Hng, K. J., Tkunaga, S. and Kajiuchi, T., Extractin f heavy metals frm MSWI incineratr fly ashes by chelating agents, Jurnal f Harzardus Materials, B75, 2000, Osak, M. and Kim, Y. J., Influence f cexisting surface-active agents n leachability f dixin in raw and treated fly ash frm an MSW incineratr, Chemsphere, 54, 2004, The Internatinal Ash Wrking Grup, Municipal slid waste incineratr residues, 1997, , Studies in Envirnmental Science 67, Elsevier. 5. ½ «,», ¼, «,, y y,,,,, 2001, s» ƒ ƒ w (II)- -, y, NIER N K.Y. Chiang, K.S. Wang, F.L. Lin, and W.T. Chu, Chlride effects n the speciatin and partitining f heavy metal during the municipal slid waste incineratin prcess, Sci. Ttal Envirn. 203, 1997, K.S. Wang, K.Y. Chiang, S. M.Lin, C.C. Tsai, C.J. Sun, Effects f chlrides n emissins f txic cmpunds in waste incineratin: Study n partitining characteristics f heavy metal, Chemsphere 38, 1999, M. Wbst, H. Wichmann, M. Bahadir, Distributin behavir f heavy metals investigated in a labratryscale incineratr, Chemsphere 44, 2001, Susan Budavari, The Merk Index, 11th editin, 1989, Merk & C., Inc., U.S.A. 10. Rbert H. Perry, Dn Green, Perry's Chemical Engineers Handbk, 6th editin, 1984, McGraw- Hill, Singapre. 11. Rbert C. Weast, CRC Handbk f Chemistry and Physics, 65th editin, 1984, CRC Press, Flrida. 12. y, s» œ x, Standard methds 2540C, Ttal Suspended Slids Dried at 180 C. 14. Envirnmental Prtectin Agency, Methd 3050B : Acid digestin f sediments sludge and sils, x, «, y, w s» wz, Vl.18, N.4, 2001, F.Y. Chang and M.Y. Wey, Cmparisn f the characteristics f bttm and fly ashes generated frm varius incineratin prcesses, Jurnal f Hazardus Materials, 2006, B138,
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