Korean Chemical Engineering Research
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(2) Js M¬dG. ñkÍ Íß l s Ñ Ý«2 UV black light 4n¶ Y×Ñ. Äê HÇ òÑ 99% « ¤ofMÁSs Ý. ¯Ñ ågGÊ f « âo Ù«÷ = GÑ 99% « ¤ofMÁSs »É. 2. 2. 2. Abstract − In this study, mercury was removed by TiO2 using fluorescent light and sunlight, instead of UV lamps. A reactor was specially designed to increase the TiO2’s exposure to the light source and to make the rotational speed constant. The contacting surface area between mercury and adsorbents was increased by packing the adsorption bed with mixture of TiO2 and glass beads. The mercury removal efficiency was more than 99% under all light sources tested in this study. The mercury removal efficiency was more than 99% under the fluorescent light or sunlight which is harmless and cheap or free. Key words: Mercury, TiO2, Sunlight. 1.. C «. Ê Ñ J« æ2 U k³ g
(3) Ï î[ ¬ « æÊ À . K, ¤oo õßjÑ ¬D Ok³ Q ñ O« ½É =³ æ2 aê2 - ?³ ò = D³ æ2 ak³ <s À. ¤o ÎÜ 1òÑ
(4) Ñ îK É02 h Î 4? ÂWK z«. ¤o
(5) Î _
(6) Jk³ ²5ê HÇ õ ßjÑ K
(7) « Âh Î M
(8) 80%õ ó@G 2 ak³ <s À[2, 3]. æ2 ¤o =Ñ ¬g2 4 Ab@ 4? UOOK R, ~ ör« Ç2 ak³ ¯g ¸GD ÎÇ a« Y«. 1ê8 ¤o ~D¬íèÑ ·Éõ g 5 ÂhO g ªg US EPA(environmental protection agency)Í wGÊ ¯G2 Rör« à\Ê À2 Y_«. G@O, @ b@ ÍDK örk³ R, ~K ê2, !s ò0³ G2 õßj Î ?³ ò¤o =³ æ2 as Ýñ?Ê À[4]. õÍ) Os fMG2 ¬,J¯ örk³2 ¿j ô s Ë ¤ À. 6÷ ¤o Î Aè « ãGD AéÑ, í-. M O1éfÍ tDæ
(9) h Ñ ¬K î[« 4@Ê À. Oo ¾
(10) k³ Ñ 5s Âr ¤ Àk Ñ Jê2 UVs Í@Ê À. ¤÷ ÖSD Ùk³ ¤ H« 1æ2 ao A[Jk³ Ñ Ýñ ¯@Í uíÊ !¶ ÄK äfÍ «P´@Ê À. G@O, ¬D1o A[Jk³ Ñ Ý«@ :k÷ 1p.Í Ê 1 íH « Q2 UV s @nÊ À. U¾ ÎÜ õDä 1 òÑ ¤os WÇK O o Qo Îsõ Ê À. «Â ÂhÑ2 1990¸ Clean Air Act Amendmentsõ 0g 11í O(As, Be, Cd, Co, Cr, Hg, Mn, Ni, Pb, Sb, Se) s Íß ÁêJ¯ JÄ ÍDK D¬³ s f´G´ æ´À[1]. OÑ U¾ ¤oo ñ Oê2 - o Aè , ãK Kg † To. whom correspondence should be addressed. E-mail: [email protected]. ‡. « øéo õ§¬0/ 6ÎR /¤ _¸s ,Ä/ñ ·ÊæÉ5n. 170.
(11) õ «ÄK ¤oBM. TiO2. 171. o Ägõ äj æD Aé«. èM ÙÑ Q« Äæ2 5R%zßj(wet scrubber)Ñ2 u s ¤ÄUs «ÄGñ d¤os ÄgQ- õÍ) OÑ fMK. 6÷ ò¤o o MÉgÆÍ 5d 6s  gÆ«D AéÑ ä « 4? Ê D Ñ dÍ j ³´÷@ :4 JÄ« @ :. «6K «K˳ ¯g, ¤o s MdGs2 õg2 ¬z~ M ò ¤os ¬ k³ GÊ À. MÑ TiO õ «ÄGñ VOCs÷ ñ Os fMGs2 õ gÍ Q4@Ê À. DÊ è,ê «·Ñ G
(12) Fig. 1Ñ Ý2 aê ç« TiO ½ÉËÑ òs ù´?j æ
(13) TiO UK ä k³ ¯g ,
(14) Ñ OH ¶s GÊ «a« ò¤os dQk³ TiO Q HgO «Ñ ãK dHY« æ´, DÍ)³z ò¤o« fMê[5]. á õgÑ2 ñk³ «Â - <s@Ê ¤« Ä«K TiO Q Ñw@ WÍ ¿Ê ¯Ñ KgK É ¬U j, K@WÄ « IK Ù«÷ = s «ÄGñ ¤ofM Y×s ¤}G . äD2 D ¤oê ôf [ñ
(15) Js M¬dG
(16) ä U s 5 ¤ À´ ɯG. ò« ÁSJk³ ·êO ¤ À´ K-WÃõ ´?Ék, äDõ ¡M ÍDGj ªG . K, K òs «ÄGñ ¤ofMÁSs WGG. 10. 2. 2. 2. 2. 2. Fig. 1. Mechanistic description of Hg capture by UV irradiated TiO2 (Lee et al.[5]).. J¯ ôOk³2 ¤os ôfÑ Û4&DÍ ÎË. K, D ò¤os dQÿ2 a õÍ)õ 0g æ2 ¤o s f´O ¤ À2 ÁêJ¯ ör O G÷¯), ao ³ ò = ¤o« dÍ æ
(17) (Hg ->Hg ), uK s | ÄUÑ 0. 2+. 2. Fig. 2. XRD patterns of TiO2 samples tested on this study. Korean Chem. Eng. Res., Vol. 43, No. 1, February, 2005.
(18) «Ääö«=äö6ÎR. 172. 2.. / . Z \ 2 ÆJk³ - «Äæ2 ³ Degussa P25 Q ³á Ishihara Q Junsei Chemical TiO -Ê Kh U) HdH(?) KA100s ÄG. Degussa P25Q U)Hd H(?) KA100, Junsei Chemical TiO o powder = as g½Gñ ÄGÊ, Ishihara TiO 2 anatase 30% ¤ÄUs QÆg powderõ »É. Î TiO powder _ o X-ray diffraction(XRD)³ ~G. Degussa P252 anataseQ rutile WÍ u 80 : 20«Ék, Ishihara TiO Q U)HdH(?) KA100o pure anataseÊ, Junsei Chemical TiO 2 pure rutile «É. Î powder XRD Ò¡s Fig. 2Ñ ÷ É. TiO õ l dGD .K òo ñkÍ l s Íß Ñ ÷ 2 ak³ <sD UV black(Philips TLD 36 w/08, 125 cm long, 36 W lamp)ê UV sterilizing(Philips GB36TB, 125 cm long, 36 W lamp), fluorescent(Osram Fl-40D, 125 cm long, 40 W), blue lightõ ÄG Ê, Ñw@ WÍ Ç2 = Ñ Y×s ¤}G. òo ²ßs ÊsGñ >Gk ò ²ßê relative intensityõ Fig. 3Ñ ÷ É 2-2. /#𣠳ä Ùk³ Y×O ¤ Àj Ù ¿DÑ b 's fÊGÊ, UV black light÷ UV sterilizing lightõ ÄO A KgK oÑ ôæ@ :´ ]o+ 4¿5³ óLs jG . äD O³ ¤o~D(VM3000, Mercury Instruments, ³)Q õGñ äD Má ¤o õ YQÑk³ +_G . Y×ßjõ Fig. 4Ñ Ñ÷¾ ÷ É. Fig. 5Ñ å ¤ 2-1. TiO2 TiO2 powder. 2. 2. 2. 2. 2. 2. 2. Fig. 4. Schematic diagram of the experimental setup.. ¤@¤ C43× C1 2005 2 . Fig. 3. Wave length and relative intensity of tested light sources.. À׫, äD2 o ·êõ .g pyrex³ fÊGÊ, ¤o fM ÁSs ÍQÿD .g K-WÃQ TiO õ HYGñ J o TiO ³ D ¤oê [ñ
(19) Js M¬dG. äD õ ¡M ÍDGj fÊGñ äD 8 TiO Í òÑ M¬K ôæj G. 2-3. c Øl` ò¤o 5õ oil bathõ ÄGñ ³_Gj K@G
(20) carrier gas N õ 75 sccmk³ àGÊ airõ 1,500 sccmk³ à G. ³_5³ 8_dî Ab@ by-passQ- ¤o õ ³ _Gj K@K á Y×G. ¤o ?½ Í 8_dê áÑ ä D \k³ D ¤os sÝ ò« óæÉs A äD Má ¤o õ +_G. äDõ ³_³ ¡MQ- TiO 2. 2. 2. 2. 2.
(21) õ «ÄK ¤oBM. TiO2. 173. ÁS Öéõ Fig. 6Ñ ÷ É. ÖéÑ å ¤ À׫ UV black, UV sterilizing, fluorescent, = ÎÑ2 TiO powder ÜÍÑ ¿j s ç@ :Ê 99% « ¤ofMÁ Ss Ýk, ¤ofM2 ²ßp. 300-400 nm UV black lightÑ Íß uñ äs Ýk÷ Ù«÷ = Ñ òs Æ á à³ ¤o« fMæ2 uñ ä ê o ¤of MÁSs Ýñ?É. Í« IGÊ 0Äk³ Q« Äæ2 U)HdH(?) TiO 2 = ê UV blackÑ 99% « ¤ ofMÁSs Ýk ÙÑ 80% « ¤ofMÁS s ÷ É. K, 400 nm« ²ßs ÍD blue lightÑ 85%Ñ Í bÒ ¤ofMÁSs ÝÊ, Junsei Chemica rutile form TiO ÎÑ2 ¤ofMÁS« 99% « G2) «2 TiO Í anataseÝ rutile³ A Ö
(22) H ²ßÑ l s Ý« D Aé«. 3-2. {çKï ÿ£ cÐ ØÏh äD 8 TiO Í òÑ ôæ´ ¤ofMÁS« 99% « ³ A Í)õ US EPA Ontario Hydro örs «ÄGñ ¤ o dHÜ¥³ _
(23) ~s G. ê Í) OÑ d¤ oo ]æ@ :IÊ ò¤oO« Â
(24) ]æÉ. !¶ ä Dõ @û áÑ2 d¤o =³ æ2 a« 4n¶ TiO Ñ dHôæ´ ¤o« fMæÉ. DÊ õgÑ TiO ³ ¤os ôG2 ÜM XRD êQ zYê[7]. 3-3. cg» |ð Z g| l !ê TiO õ «Äg ¤os fMG
(25) ðD ¤o 80%b@ G2 QÑs +_GÊ, « )«õ «Äg l ! 1 g« fMK ¤o ê TiO 1 g« fMK ¤o s ªG . Table 1Ñ & ôf ²êY× êõ ÷ É. ,Ñ å ¤ À׫, l !« TiO Ñ Wg ÍÍ IG÷ ÁSs ÊsG ñ f s ªG
(26) TiO Í l !Ñ Wg K@WÍ Jj Ç. ²êQÑ ó«OÏ ôf GWÄs Ý8G
(27) TiO Í
(28) K ÄG. K, l !o õÍ)Í Î³ÑQ ç« Ê5³ A, õ ÎsÍ ÀÊ ôÁSo
(29) Ï ©´D. 2. 2. Fig. 5. Experimental reactor for mercury removal. 1. Inlet 5. TiO2 powder 2. Pyrex reactor 6. Glass beads 3. Outlet 7. Mercury analyzer 4. Light source 8. Filter. 2 2. Í òÑ M¬K ôî ¤ À´ K@G. òs YÙGÊ ³ _QÑ òÑ ôg ¤ofMÁSs ªK áÑ ÙGñ ä ñzõ e¯O ¤ ÀÉ. äD gÑ æ2 Í)Ëo  h h (EPA)Ñ à¯ê Ontario Hydro örs «ÄGñ Í ) Ñ ¤o dHÜ¥(ò¤o, d¤o)³ õ +_G. Ontario Hydro öro ñ ÄU Ñ ÎÎ ñ ÜÍ ¤os Ä gQ- ¤o dHÜ¥³ _
(30) J +_s O ¤ À2 ör«. 2-4. {çKï ÿ cÐ Ø l` Í) ¤o dHÜ¥ õ +_GD .g Âh EPA Ontario Hydro örs >G. « öro !dtèMÑ æ2 Í) Ñ ò¤o, d¤o, ½É¤o Ú ¤o s +_G2) Äî ¤ À. Hg Q Hg õ ÎÎ ñ ÄU Ñ ÄgQ- õ +_O ¤ À2) 3Í@ ¤Us ÄG 8 í »-Iõ ÄK. O 3í »-IÑ2 KCl¤ÄUs ´? ´ Hg õ ¯RG 4d~ »-IÑ2 HNO -H O ¤ÄUs ´ SO Ñ s fG2 òOs G Hg ¤
(31) Ñ ¯WK. 5-7d~ »-IÑ2 KMnO -H SO ¤ÄUs ´ Hg õ ¯RK. K@L K í »-IÑ2 Y-rs £DGñ Í) O ¤~« fMê[6]. 2-5. cg» |ð Z g| ¤os fMGD .g ôf³ Íß Q« ÄæÊ À2 l ! ê ²êQÑs WGGñ ÝI. ço ÆQÑ l !ê TiO õ ä DÑ Ê ðD ¤o 80%b@ G2 QÑs +_G . ¤ofM D Ú f s WGGD .g l !o U¥K s-Í æ@ :o ao >GÊ, TiO 2 K@WÄ« IK ÙGÑ Y×s G. 0. 2+. 2+. 3. 2 2. 0. 2. 0. 4. 2. 2. 2. 2. 2. 2. 2. 2. 4. 2. 2. 3.. 2. û G. 3-1. cg»ós Y×Ñ º)T ê òê TiO. 2. 5.. û «. TiO powderQ K-WÃõ äDÑ Ê ñ6 òÑ ¬K ¤ ofMÁSs Y×g á ê {ê ço ·s . (1) = GÑ TiO õ «ÄGñ Í) ò¤o 99% « fMÍ ÍDG. Y×Ñ Äê HÇ òÑ ¤ofMÁ S« 99% « «ÉÊ ä kÎ }Ë. à« Ä«GÊ jWÄ«÷ K@WÄ« IK ÙÑ 99% « ¤ofM ÁSs Ý. (2) Ontario Hydro örs «ÄGñ ¤o Ü¥ õ +_K ê, òs Æ G
(32) dHôs 0g TiO Í ¤oê complexõ Gñ ¤os fMG. (3) ¤ofMÁS« Y×Ñ º)Tê TiO powder ÜÍÑ !¶ 2 ¿j s ç@ :I. @ 400 nm « ²ßs ÍD 2. 2. 2. ÜÍÑ !ñ ¤ofM. powder. 2. Korean Chem. Eng. Res., Vol. 43, No. 1, February, 2005.
(33) 174. Fig. 6. Hg removal efficiency under various light sources.. ¤@¤ C43× C1 2005 2 . «Ääö«=äö6ÎR.
(34) õ «ÄK ¤oBM. TiO2. Table 1. Comparison between TiO2 and activated carbon Average time to reach 80% of the initial Hg conc. Amount of Hg per gram of adsorbent Estimated cost per gram of Hg. TiO2 -570 hrs. Activated carbon -40 hrs. -48.0 mg -2.5 mg -$0.015 -$0.20 ($0.0025/g TiO2) ($0.0017/g AC). blue light Î, rutile« 99% « fMÁS³ 85% anatase Ý ÊÁS ¤ofM Ds Ý2), «2 TiO Í anataseÝ rutile³ A Ö
(35) H ²ßÑ l s Ý«D Aé«. 2. [ ÷ á IÉ2 TÎR G¤~ »Ç2 HéÑ ù_ê ËUJ¯ fÉ ÌÑ Q Kd Ë-¥ñ _« Ý Ã?n.. S+S. 175. ity Planning and Standards and Office of Research and Development, Washington, DC(1998). 2. Owens, T. M. and Biswas, P., “Vapor Phase Sorbent Precursors for Toxic Metal Emissions Control from Combustors,” Ind. Eng. Chem. Res., 35(3), 792-798(1996). 3. Lee, T. G., Hedrick, E. and Biswas, P., “Comparison of Hg0 Capture Efficiencies of Three in situ Generated Sorbents,” AlChE J., 47(4), 954-961(2001). 4. Lengyel, Jr. J., DeVito, M. S. and Bilonick, R. A., “Interlaboratory and Intralaboratory Variability in the Analysis of Mercury in Coal,” J. Air & Waste Mgmnt. Assocn., 46(4), 317-326(1996). 5. Lee, T. G., Biswas, P. and Hedrick, E., “Overall Kinetics of Heterogeneous Elemental Mercury Reactions on TiO2 Sorbent Particles with UV Irradiation,” Ind. Eng. Chem. Res., 43(6), 1411-1417(2004). 6. U.S. EPA, The Ontario Hydro Method, Draft Manual, U.S. Government Printing Office, Washington, D.C.(1998). 7. Wu, C. Y., Lee, T. G., Tyree, G., Arar, E. and Biswas, P., “Capture of Mercury in Combustion Systems by In Situ Generated Titania Particles with UV Irradiation,” Environ. Eng. Sci., 15(2), 137-148(1998).. 1. U.S. Environmental Protection Agency, “Mercury Study Report to Congress,” EPA Report; EPA-452/R-97-003, Office of Air Qual-. Korean Chem. Eng. Res., Vol. 43, No. 1, February, 2005.
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