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1 Korean Chem. Eng. Res., Vol. 43, No. 1, February, 2005, pp Ks óslã Z / / k ãò H/ dhàhê ãò [wq ÁÉ2Ÿ (2004 6ö 8³ [, ö 18³ >) Efficient Desulfurization and Denitrification by Low Temperature Plasma Process Sung-Min Kim, Dong-Joo Kim and Kyo-Seon Kim Department of Chemical Engineering, Kangwon National University, 192-1, Hyoza-2-dong, Chunchon, Kangwon-do , Korea (Received 8 June 2004; accepted 18 October 2004) ß á õcñš2 :) U³ öm à_ñ g SO 2 Q SO 2 /NO fmáss ~ Gk, ñ6 à_ Í fmá SÑ Ùj2 s ªJk³ ÆGŒ. à_ ³Š ÍMF, :)?², ÍQÑ, ä í ð, (NO, SO 2, NH 3, H 2 O and O 2 ) s ~ GŒ. Íæ2 MF, :)?² 2 ÍQÑ«ÍWÑ 2 O 2 Q H 2 OÍ ƒíöñ SO 2 fmásê SO 2 /NO ŸQ fmáso ÍGŒ. K, NH 3 ð, Í Í O SO 2 /NO fmáso ÍGŒ. «Y J êëo NO x Q SO x õ fmg,.k :) U³ öm à_ ßj ª,ð É0³ Äî ÀŒ. È Abstract In this study, we have analyzed the removal efficiencies of SO 2 and SO 2 /NO by the pulsed corona discharge process and investigated the effects of several process variables on those removal efficiencies systematically. The effects of process variables such as applied voltage, pulse frequency, residence time, and initial concentrations of reactants (NO, SO 2, NH 3, H 2 O, and O 2 ) on the removal efficiency were analyzed. As the applied voltage, the pulse frequency or the residence time increases or as the O 2 or the H 2 O or the NH 3 concentration in the inlet feed gas stream increases, the SO 2 removal efficiencies and the simultaneous removal efficiencies of SO 2 /NO also increase. These experimental results can be used as a basis to design the pulsed corona discharge process to remove NO x and SO x. Key words: Desulfurization, Denitrification, Low Temperatune Plasma Process, Removal Efficiency 1. C «M Ž,hs y[k³ h äfí j ãdæš h Æ«21 D M ÊzÍÍj Æk³ 1íÊ ÀŒ. U¾ h Æ o Œñ Æ~tQ õî «h ÆÑŠ ÿt«ª f0šñ )[J s k _ Í æéœ. ³ öm à_ Ñ K %z %0 D o Eo õg íèdññ ggê SO x, NO x ço D1 í0s ŸQÑ s-o À2 ßY ŽÑ DÊ ñ6 ör D J, fj, h 1 éfys ÝUg k À 2 D ³ ÍæÊ ÀŒ. D y æ2 1òs k«d.g Š2 ßDJ óòñš 1í fmßj íè Ú jí gæ 2) MÑ2 :) ³ öm à_s «ÄgŠ D 1ís fmgd.k õgí lè¾,}æê ÀŒ. I5 ñ K %z %0 àro DF ÆQÑŠ ñ K öm To whom correspondence should be addressed. kkyoseon@kangwon.ac.kr s ³kE õí)ñ Wê 4zÍ) Ú 0dís fmg2 D «M Ë ª ÎhÑŠ äfg2 Í) ÜÍÍ SO 2 õ WÇGñ NO x, VOC(volatile organic compound), CO 2 Ùk³ e öñ! G Q)ÊÑŠ «Ë KgÍ)õ ŸQÑ s-o À2 á D y «4(Ê ÀŒ[1-5]. «D c U8 s Ý, ä Dõ DÊ MD4,DQ Ÿ³K Ž- gæõ ÄO À ðd ÉWÄ«kÎ IƒK ßYs äê Às O 4n ä D gæ kî Ñ GŒ. K, 8_K ³ Í ä D o òñ U æ, «âñ Ñw( HÍ JÊ ~,fmñ ÁêJ«Œ. U¾, äh ßjÍ ÍDG ³ c³ õ Í) s-d ³ íè«lè¾ «P (Ê ÀŒ[6-13]. Amirov Ù[14]o )T-Ë ³ ä D ÑŠ NO SO 2 f MÑ Ë s «J/Y Jk³ õgg2) OH, O 3, N Ù Ë«NO SO 2 fmñ s Âj2 ak³ ÝÊG Œ. Park Ù[15]o ³ öm Q)Ês «ÄK NO x fmñš SO 2 s õggk SO 2 Í CO 2 Q 竃íöñ! NO x 129

2 130 6 Æö6Ÿ?ö6/Ž fmás«íws îûgœ. Kimê Hong[16]o KM ßž ³ öms 0K NO x Q SO x ~gõ Y Gk, KM ßž, ä W gæ, õ s- ÆQ dõ 0g NO x Q SO x Í ~gæê fmás«íws ÝÊGŒ. DinelliQ Civitano[17]2 :) ³ ÑŠ õ á Í)³z NO x Q SO x ŸQ fmõ õgg k NO x Q SO x ðd, NH 3, ä D Í) 5, Hydrated lime Ù«NO x Q SO x fmásñ s c2 ak³ ÝÊGŒ. Kim Ù[18, 19]o :) ³ öm à_s «ÄK NO x fmñš ñ K dh Ú ½É ßs H1Rs ÄGñ õg GÊ ŸtHJ ½É U s ~ GŒ. (b( :) ³ öms «ÄK SO x Ú NO x fm õg2 Q«}æÉk ŸQ fmõ ÊsK ao í à_ d Í fmásñ Âj2 s ªJk³ ~ K õg2 4) ~ j :o =«Œ. á õgñš2 :) ³ öm ä Dõ «Ä K %z %0Q à_ dñ!ñ %z %0 U ê ŸQ fm õ ªJ Y s 0g ~ GŒ. 2. / á õgñš :) ³ öm ä Dõ «ÄK %z %0 õg õ.gš ÄK Y ßj í 2 Fig. 1ê çœ. Y ßj2 ä í c½ Ú f z, ä D, Mtà Ú f z -Ê Í ) +_z³ «P ÀŒ. NO, SO 2, NH 3, N 2 Ù D 2 ÎÎ MFCõ «ÄGñ _ àgœ. NO Ú SO 2 fm Y Q H 2 O s ÊsGD.g ³_ H 2 Oõ bubblerõ ÄGñ O 2 D Ñ dqe ä D ³ àgœ. O 2 D Ñ dê H 2 O Í ä D ³ àæd MÑ ŽG2 as ö(gd.g ùž s ÄGñ D 5 õ ³_Gj K(QZŒ. ä D³ àæ2 NH 3 Í ä D ³ àæd MÑ Œñ D Ëê ä G2 as ö (GD.gŠ NH 3 àžs Œñ D àžê ~-GŒ. NO Ú SO 2 fmõ.g á õgñš ÄK :) ³ öm ä D2 cylinder-wirek³š Y1 o 5cm«Ê L«2 38 cm«ä D é0o Pyrex«Œ. ³ è@ Mo ä D yññ jê )º -) Ž() 0.5 mm)«, [(o ä D žñ )º -) ak³ jgœ. [(Mo ò0k³ L «2 30 cm«œ[20]. ä DÑ ³ õ è@qÿd.g ÊMF è@d(kh Switching)õ ÄGŒ. Y ÑŠ ³ è@ MÑ àæ2 MF DQ c² 2 1Y³) é(tektronix TDS 220)õ Ä Gñ +_GŒ. ³ öm á NO x Ú SO x õ +_GD.g ä D gñ Electro-Chemical Gas Analyzer(Digitron, GreenLine MK II)s jgñ +_GŒ. ³ öm ä DÑ ê ½É í0o gñ õ ê ~ D ½gÑ ÊÁS 1 õ jgñ fmgœ. Y o 5 FÑŠ }Gñ k, NO Ú SO 2 fmq à_ s <4ÝD.gŠ,gÆQk³ ÍMFo 50 kv, : ) c² Hz, ÍQÑo 7.2 sec, SO 2 ðd ppm, NO ðd ppms ÄGŒ. ³ öm =2 ä D³ Íæ2 MF, ä D =(Y1Q Ž«) ), ÍQ Ñ Ú àd ÆQ(D 5, ~ ) ÙÑ ÊKŒ[21]. á õgñš2 )T-Ë ³ öms «ÄK NO x, SO 2 fm Y s.g ÍMFs kv³ dqzœ. ä D SO ,500 ppmk³, NO ppmk³, NH ,200 ppmk³ dqzk ÍQÑo sec³, : ) c² Hz³ dqzœ. HÇ Y êëo 3 «Y } á +_K à èjõ ÄGŒ. 3. ûg Z +{ 3-1. (<? Ÿ {à SO 2 C» ÍMF Fig. 2ÑŠ ä D³ Íæ2 MF«SO 2 fmñ Âj2 s ðd SO 2 õ dqÿš +_GŒ. ä D³ Íæ2 : ) c² Q Í QÑo,g ÆQk³ GÊ, ä D³ Íæ2 MFs kv³ dqzk, ä D³ àæ2 ðd SO 2 Í 800, 1,200, 1,500 ppm³ A ÎÎÑŠ SO 2 fm ÁSs + Fig. 1. Schematic of experimental set up. C43 C1ƒ Fig. 2. SO 2 removal efficiencies for various initial SO 2 concentrations as a function of applied voltage (pulse frequency=200 Hz, residence time=7.2 s).

3 I# ñ K à_ñ K z Ú _GŒ. ä D³ Íæ2 MF«ÍO MÉË«Í(2 èñw(í ÍGñ SO 2 fm ä Ñ y K l Ë(O, O 3, OH, OH 2 2 ÍG ³ Ëê uñ dhä Ñ K SO 2 fmáso ÍGÊ ÀŒ. ÍMF«50 kv«ê ðd SO 2 Í 1,500 ppm ³ A2 SO 2 fmás«10%«é a«800 ppm³ A2 SO 2 fmás«29%³ ÍGŒ. «2 ðd SO 2 Í s ä D ÑŠ SO 2 fmñ gæ2 Ñ w(í Jk³ Q«1 Gj æ SO 2 fmás«ýg 2 ak³ ~ êœ ÍQÑ Fig. 3o ä D³ K½æ2 D Í QÑ(D K) d Í SO 2 fmñ Âj2 s Œ. ä D³ Íæ2 MF ê :) c² 2,g ÆQk³ GÊ, ÍQÑo 2.94, 5.43, 7.2 sec³ dqzs A ðd SO 2 dñ! SO 2 fm ÁS s ÎÎ +_GŒ. Í QÑ«ÍWÑ! ä D Ñ ê öm òñ SO 2 Í Ëå2 QÑ«L (Ê 1Ú QÑ Ÿ8 dhä Ñ g SO 2 Í Mhæ ³ SO 2 fmás«í GÊ ÀŒ. Fig. 2ÑŠsF ðd SO 2 Í ÍO SO 2 f Mõ.K ~É èñw( Šo ÝG ³ SO 2 fmás «ÝGÊ ÀŒ :) c² Fig. 4Ñ2 ä D³ Íæ2 MF :) c² dí SO 2 fmñ Âj2 s,œ. ä D³ Íæ2 MFê SO 2 ð D 2,g ÆQk³ GÊ, :) c² õ dqzs A ÍQÑ dñ!ñ SO 2 fm U s <4ÝIŒ. ÍMF : ) c² Í ÍWÑ!.QÑ MÉÑ Íg(2 èñ Fig. 4. SO 2 removal efficiencies for various residence times as a function of pulse frequency ([SO 2 ] 0 =800 ppm, applied voltage=50 kv). w(2 ÍGñ Qo Š l Ë«@ æê l Ëê uñ dhä Ñ g Qo Š SO 2 Í fmæ ³ SO 2 fmás«ígê ÀŒ. Í QÑ«ÍWÑ H QÑ Ÿ8 dhä Ñ g fmæ2 SO 2 Šo ÍK as Ý«Ê ÀŒ Í) Æ Fig. 52 D Æ dí SO 2 fmñ Âj2 s Œ. ä D³ Íæ2 MF, :) c², ðd SO 2 2,g ÆQ k³ GÊ, H 2 OQ O 2 ƒíñ!ñ SO 2 fmáss ÆGŒ. D Í QÑ«7.2 sec ³ A, SO 2 Q N 2 D Os àgñ ³ ömgs A2 SO 2 fmás«10%«(o SO 2 +N 2 +O 2 ÑŠ 2 SO 2 fmás«14%³, -Ê SO 2 +N 2 +O 2 +H 2 OÑŠ2 SO 2 f MÁS«29%³ ÍGŒ. «2 ~ê Í ƒíöñ! NO Ú SO 2 H ä Ñ îñg2 d (O, O 3, OH, OH 2 ) «ÍGñ dhä Ñ K SO 2 H Í ÍG ³ SO 2 fmás«ígd Aé«Œ. ä D ³ SO 2 +N 2 O s Ä s Î, SO 2 ÊÑw( MÉËê )[J GM (R 1) Œñ ~ÉË(N * 2, O)ê ä (R 2,3)Ñ g SO SO 3 ³ M hæ ³ SO 2 fm ÁS«10% ÍK as Ý«Ê ÀŒ[16, 22]. Fig. 3. SO 2 removal efficiencies for various initial SO 2 concentrations as a function of residence time (pulse frequency=200 Hz, applied voltage=50 kv). e+so 2 SO+O+e (1) N * 2 +SO 2 N 2 +SO+O (2) SO 2 +O SO 3 (3) 3-2. (<?Ÿ {à NO SO 2 C» ðd Korean Chem. Eng. Res., Vol. 43, No. 1, February, 2005

4 132 6 Æö6Ÿ?ö6/Ž ÆQk³ GÊ, NO ðd õ 100, 200, 300 ppmk³, SO 2 ðd õ 0, 800, 1,200, 1,500 ppmk³ ÎÎ dqzœ. á õgñš ÄK à_ ÑŠ +_ê NO 2 2 ðd NO Ñ 1% _ ³ Œ. «2 NO³z NO 2 æéké OH OH 2 Ëê uñ ä Ñ g z~ NO 2 «HNO 3 ³ dê ak³ êœ.! Š á õgñš2 NO dos à_ dñ!,œ. ðd NO Í 100 ppm Î, NO Š fmqñ2 fmás«68%³ +_æé k SO 2 õ 800 ppm «ƒí s AÑ2 fmás«89%³ u 21% ÍŒ. SO 2 ƒíñ!ñ NO fm ÁS ÍÑ K _ek èno 4) äê àí ÇŒ. K ÍD k³ á õ gñšsf H 2 OQ ê O 2 (10%)õ SO 2, NOQ Wÿ ³ öm ä DÑ àk Î, Œ{ê ço ä Ñ g NO fm ÁS«ÍO Àk ÝŒ áj fm èn ä«gêœ[7]. 2NO+O 2 2NO 2 NO 2 +SO 2 +H 2 O H 2 SO 4 +NO Fig. 5. SO 2 removal efficiencies for various gas compositions as a function of residence time ([SO 2 ] 0 =800 ppm, applied voltage=50 kv). SO 2 ðd Í 1,200, 1,500 ppm³ A NO fmáso NO Š fmqýœ2 ÍG(O ðd SO 2 ÍÑ!ñ NO f MÁSo Æ ÝG2 as Ý«Ê ÀŒ. «2 ðd SO 2 Í ÍO NO fmo 4n SO 2 fmõ.k dhä Ñ Qo «ÄÞD Aé«êJk³ NO fmõ. K Mt Ñw( Š«ÝK a«œ. ðd NO Í ÍWÑ! NO fmõ.k ~É èñw( Šo ÝGñ NO f MÁS«ÝGÊ ÀŒ. Fig. 6. NO removal efficiencies for various initial NO concentrations as a function of initial SO 2 concentration (applied voltage=50 kv, residence time=7.2 s). Fig. 6o NOQ SO 2 õ ŸQÑ àgs A SO 2 ðd dq NO ðd dí NO fmñ Âj2 s ÝñcÊ À Œ. ä D³ Íæ2 MF, :) c², D ÍQÑo,g C43 C1ƒ Fig. 7. SO 2 removal efficiencies for various initial NO concentrations as a function of initial SO 2 concentration (applied voltage= 50 kv, residence time=7.2 s).

5 I# ñ K à_ñ K z Ú Fig. 8. NO removal efficiencies for various initial NO concentrations as a function of applied voltage ([SO 2 ] 0 =800 ppm, pulse frequency =200 Hz, residence time=7.2 s). Fig. 9. NO removal efficiencies for various initial NO concentrations as a function of applied voltage ([SO 2 ] 0 =800 ppm, pulse frequency =200 Hz, residence time=7.2 s). Fig. 7o Fig. 6ê ço à_æqñš NOQ SO 2 õ ŸQÑ à Gs A NOQ SO 2 ðd dí SO 2 fmñ Âj2 s Œ. ðd SO 2 Í 1,200, 1,500 ppm ³ A2 ðd NO Í ppmb( g SO 2 fmásñ à s Ùj( :(O ðd SO 2 Í 800 ppmk³ WGJ I ³ A2 SO 2 fmás«wgj j Ê ÀŒ. ðd NO Š«100 ppmz ÍWÑ! Fig. 6ÑŠQ ço «K³ SO 2 fmõ.k. ~É Ñw( Šo ÝG ³ SO 2 fmás«ýgê ÀŒ. ðd SO 2 Í ÍWÑ! SO 2 fmõ.g Qo Š M tñw(í gös Ý«Ê ÀŒ ÍQÑ Fig. 8Ñ2 ä D³ K½æ2 D ÍQÑ«NOQ SO 2 ŸQ fmñ Âj2 s,œ. ä D³ Íæ2 MF, : )c², SO 2 ðd 2,g ÆQk³ GÊ, NO ðd õ 100, 200, 300 ppmk³, ä D³ K½æ2 D ÍQÑs sec³ dqzœ. Fig. 6ê 7ÑŠsF NOOs Š fm s AÝŒ NOQ SO 2 õ ŸQ fm s A NO fmás«ígê À Œ. D ÍQÑ«ÍO ä D ÑŠ H QÑ Ÿ8 NO Hä Ñ g NO fmás«ígê ÀŒ. ðd NO Í ÝWÑ! NO fmõ.k ~É èñw( Šo ÍG NO fmás«ík as Ý«Ê ÀŒ ÍMF Fig. 92 ä D³ Íæ2 MF«NOQ SO 2 ŸQ fmñ Âj2 s Œ. ä D³ Íæ2 :) c², D Í QÑ, SO 2 ðd 2,g ÆQk³ GÊ, ä D³ Í æ2 MFo kv³, ðd NO 2 100, 200, 300 ppmk Fig. 10. NO removal efficiencies for various initial NO concentrations as a function of pulse frequency ([SO 2 ] 0 =800 ppm, applied Voltage=50 kv, residence time=7.2 s). ³ dqzœ. Fig. 8ÑŠsF NOOs Š fm s AÝŒ NOQ SO 2 õ ŸQ fm s A NO fmás«j Ê ÀŒ. ä D³ Íæ2 MF«ÍWÑ! ä D à Korean Chem. Eng. Res., Vol. 43, No. 1, February, 2005

6 134 6 Æö6Ÿ?ö6/Ž Fig. 11. NO removal efficiencies for various initial NH 3 concentrations as a function of applied voltage (pulse frequency=200 Hz, residence time=7.2 s, [SO 2 ] 0 =800 ppm, [NO] 0 =100 ppm). æ2 Ñw(Í ÍGñ l 2 ÍG Ê NO fmõ.k dhä o } ( ³ NO fmás«í GÊ ÀŒ :) c² Fig. 10ÑŠ2 ä D³ Íæ2 :) c² dí NO Ú SO 2 ŸQ fmñ Âj2 s ÝñgŒ. ä D³ Íæ2 MF, D Í QÑ, SO 2 ðd 2,g ÆQk³ GÊ, ä D³ Íæ2 :) c² Hz³, ðd NO 2 100, 200, 300 ppmk³ dqzœ. :) c² Í ÍWÑ!.QÑ àmt«ígñ MÉË«Í(2 èñw(í ÍG ³ NO fmás«ígê ÀŒ DHn4 Fig. 11ê 122 DHn4 ƒíñ!ñ NOQ SO 2 fmu s ÎÎ Œ. ä D³ Íæ2 :) c², D Í QÑ, SO 2 ðd, NO ðd 2,g ÆQk³ GÊ, ä D³ Íæ2 MFs kv³, ä D³ àæ2 ðd NH ,400 ppmk³ dqzœ. ÍMF«50 kv ³ A, Fig. 11ÑŠ ä D³ NH 3 Í àæ( :s A2 NO fmáso 89%«É a«nh 3 Í 2,400 ppmk³ àgs A2 NO fmás«99.8%³ ÍGÊ Fig. 12ÑŠ NH 3 õ àg( :s A2 SO 2 fmáso 25%«É2) NH 3 õ 2,400 ppmk³ àwñ! SO 2 fmáso 71%³ ÍGŒ. NH 3 õ ƒíwñ! NH 3 Í SO 2 Q uíj ä Gñ Œ DH((NH 4 ) 2 SO 4 GÊ ê zdh,ñ NOÍ NH 3 Q Wÿ ô ä s ³kÿD AéÑ NO Ú SO 2 fmás«j ÍG2 ak³ ~ êœ. C43 C1ƒ Fig. 12. SO 2 removal efficiencies for various initial NH 3 concentrations as a function of applied voltage (pulse frequency=200 Hz, residence time=7.2 s, [SO 2 ] 0 =800 ppm, [NO] 0 =100 ppm). 4. û «á õgñš2 :) ³ öm ä Dõ «ÄGñ à_ dí SO 2 fmq NO Ú SO 2 ŸQfMÑ Âj2 s Y J k³ ~ Gk, à_ s ~ GD.g ðd NO Ú SO 2, ÍMF, D ÍQÑ, :) c², D Æ, D Hn4 Ùs dqzœ. (1) ä DÑ Íæ2 MFê :) c² Í ÍO, ä D ³ K½æ2 D ÍQÑ«ÍO SO 2 fmáso Í Gk, ðd SO 2 Í ÝO ä D³ àê SO 2 fmáso ÍGŒ. (2) SO 2 +N 2 HYÍ)Ñ ~ê Í ƒíöñ! SO 2 f MÁSo ÍGŒ. (3) NO Ú SO 2 ŸQ fmq SO 2 ƒí2 NO fmñ à s cé(o NO ƒí2 SO 2 fmñ à s c( :IŒ. (4) NO Ú SO 2 ŸQ fmq D ÍQÑê ÍMF, :) c² Í Í O NO Ú SO 2 fmáso ÍGŒ. (5) NO Ú SO 2 ŸQ fmq ƒíæ2 NH 3 Í ÍO NO Ú SO 2 fmáso j ÍG2), U¾ NH 3 Í 2,400 ppm³ A NO2 M Œ fmæék SO 2 Íß o f MÁSs á Y p.ñš»éœ. á õgñš Y Jk³», ê2 à_ ÆQ dñ!ñ ªJ ÁS ~ ê Yf NO x Ú SO x fm à_ñ dgñ JÄWÑ À ÁSJ ÒM ÆQ Ú Mt Ýõ.K ßj íè Ñ y K _Ýõ fào Às ak³ D êœ.

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