Temperature Control in Autothermal Reforming Reactor

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1 Korean Chem. Eng. Res., Vol. 45, No. 1, February, 2007, pp j mi s m i m j oh qç s Çms Ç e 1370 (2006 9o 26p r, o 13p }ˆ) Temperature Control in Autothermal Reforming Reactor Song Joo Kim, Ji Hoon Nam, Jietae Lee and Dong Hyun Kim Department of Chemical Engineering, Kyungpook National University, 1370 Sankyuk-dong, Buk-gu, Daegu , Korea (Received 26 September 2006; accepted 13 December 2006) k Copper-Zinc Oxide n ˆm ql v p p m rl l m. p hot-spotl 1cm l vrp p m rl, o p sq n m. p e vl p llp, p IMC-PI p rn l rl p pl. p rl 100e p v p p m ±5 o C l rl pl. p r p hot-spot vrp s l, rp rlp l pn p m. h Abstract Temperature control of an autothermal methanol reforming reactor which uses the copper-zinc oxide catalyst was studied. Temperature at 1cm below the hot-spot point in the reactor was used for the controlled variable, and the air flow rate was used for the manipulated variable. A first order plus time delay model was identified and controller parameters were obtained by applying the IMC-PI tuning rule to the identified model. With this controller, we could control the reforming reactor temperature within ± 5 o C over 100 hours. Change of the hot-spot point due to the catalyst degradation was investigated and it could be used to design an adaptive controller. Key words: Reformer, Temperature Control, Autothermal, Methanol, Copper-Zinc Oxide Catalyst 1. r, ~ l v, l v rk p to l l t p rop l, l rv, rv r rq,, ˆk, r edš p rn p. p n l rv r edšp }l d, ˆm, o, ˆ p l p d tp m r rp pe vr r ll ep ˆ p. p ep ˆm lp r pp, mm vp p rp, k l pn p, s sp ~ l vp p p p l p lv p [1, 2]. l rv edšp tn p, LPG, LNG p ˆm v l l l rv edšp tn l l n v p. ˆ l l rp l pp. l l n plp ˆ p p p l rv l pl l To whom correspondence should be addressed. jtlee@knu.ac.kr p p. p lp q l ep l tp p l rv edšp pp rv ep [1, 3]. v p lp ep tp l rp v p. p l el v p pp el l pl p k l nr p [1]. lr p n n sp n q s p. l rv edšp r no l p p l p p. p o v l rv edš p rp lrp q p. p q l edšp rl n l n rp, v lp l r ep v kk sp r rll r rl p p pn l. l rv l p l p k rp l rv rl edšl l lk n p p [4]. v ml pp pl p p r rm. p p lv l r v v nr p p rl lk, rl v p 12

2 p. p rp p rl p l l k rprl n [4, 5]. p r nr s r p n. v rp rp r p n l. r p rp o p p n v, l l n q l o krrp nrp n p o rll l e e rp lp p. r e r p l o edš p l rl v p kr nrp e m, p kk o hot-spotp o m m p m. 2. mi s m o ˆm ql v p l p m rl 13 l rvp l ˆmp }l d n l p rq, qtpp np l v p l v ˆ p p n vp l ˆ l p n lv p. ˆmp pn v pp v v p(steam reforming) ql v p(autothermal reforming)p p [6-8]. p tl ql v pp v v pl l n v kk q n p p, p l p n v kk., p v v p 75Í r p ql v p 56Í r p., ql v p l rvp p m q n v k l rvp l n k v r~ p r ƒv rp p. l ql v pp ˆ l e p mp ql v p p mi s m(autothermal reforming reaction) ql v pp pl p lp v v pl n p f p n l lp pl p pp. v p(partial-oxidation reforming) p. pp p [1, 3, 7]. OH(l) + 0.5O 2 CO 2 + 2H kj (1) OH(l) + H 2 O(l) 3H 2 + CO kj (2) OH 2H 2 + CO kj (3) CO + H 2 O(l) H 2 + CO 2-3 kj (4) r~ pep p. OH + x(o N 2 )+(1-2x)H 2 O (3-2x)H 2 +CO xN 2 (5) l x m ˆmp (1-2x) p ˆ p ˆ mr r l n p kp. x = 0p l p (5) l pp v v p (2), x = 0.5 p l l pp p (1)p. lr p p o x 0.23 r lk v l ep k 0.23 kk. 0.28l 0.32 pp p r v, p e l sq p rl o 0.26p ˆ m. Fig. 1. Experimental apparatus for the autothermal reforming system m ql v p e q Fig. 1l ˆ p [4]. v p v n p l v. v q v 25 mm, p 360 mmp, n q v 35 mm, p 320 mmp. n l start-upl n l p o l p p r~ kp, l ep eˆ o o om l p l e. k p p n p op. n p lr pp p o o bead }or p, ˆ l p. n p r m k p p l v p q l l. ˆm ql v pl n copper-zinc oxide p. Copper-zinc oxide nr s p 400 o C r p m l sinteringp pl r pl. p p r pl l p m nr p rl q. e l n copper-zinc oxide p psp ICI 53-1 m [4]l ˆ p. v p 65 gp, v p 30Í }o. v, v p 36 cmp p p 11 cmp. rl t AD-DA l el q~ rq rqp r (16 bit) n m. r p p p m, n p m, p p p m, p o, k p p ko pp, r q K-type lre MFC(mass flow controller), k (DP-cell) n m. sq p p op p o k p p o, l (heating band)p l p pp, sq MFC,, Thyristor n m. q PCm p p d l p, sq ql v pp p e s p, p m Korean Chem. Eng. Res., Vol. 45, No. 1, February, 2007

3 14 të v ËpvˆË 150 o C p p p n p rl p l ql p n. Thyristorp rkp sq l l p l r p sr l o m l p p p Œ p eq. k p p r Œp, p p Œp. Œp k p p o p 0.6 g/minp p p o p 650 ml/min r p. p p e (5)l x 0.26l p. Start-upp r rp l, 100 p l p p qd m dp m 500 o C r l p. p p m r ˆ sq o p sr. p p k p p o p r p RPM p o p r MFC tlv. v ep PCm p pd, MFC PCm l DA(digital-to-analog) e p p v. p Œp k p p ml/min r k o p Œp p p p m l tn l p. 3. o Š m oh rl p p rr vrp m m, s q p o p m. r p e rp l o p(identification) qlp n. l l l v p pv, l l q p n p p rp pn l r p p p n m. p p rrl [5]l l p. r p p e vl r m. v RIT () s Us () Gs ke θs = () = τs+ 1 RIT(s): p m U(s): o e rp rp k, e τ, e vl θ. rl p PID k vp velocity ˆ mp [5], e p 0.1 m. p rl ˆ anti-reset windupp p, l q r qlp n l. o l p p u krp 300 3,000 pp p r m. v, rl p 3, p. rl p IMC p n m [5]. 4. y 4-1. o (steady state) p e p rl, r r ˆ p k. Start-up rp, p kp Œp p p m r ˆl p. v, e l p l p r ˆ ll. k p v p k p o kl p r ˆ t m., e e ml p l p p n m 70~80 o C, p p p m o45 o k (6) Fig. 2. A typical reactor temperature profile at 1 cm below the hot-spot point. 40~50 Cl o p lr. p, ~ w e p hot-spot o l p p m r ˆpv p k. e, hot-spot o l v p e p, o ± 30 o C r ˆ., v p t pr v kkp, v pr ˆ v kk. Hot-spot o l p } p n l n pp k plp, rl vp p Ž., p e p hot-spot 1 cm k l p r ˆ p k. Fig. 2l p nr p e k pr ov mp p p m ˆ p, ± 10 o C p v p m. p r ˆ p e p v m. Hot-spotl p p v, rll n rr p lp pl. m p v p k p p vr Œp o p v l m p k. p v p t m n l m eˆ pp p my si p (air)p Œpl p p m l p p e vl m. DA e l k p p p t nm pp p p t n l qlp m. k p p p pr oveˆ, MFC sq l p p l p m p k. Hot-spot 1cm l p p, r ˆ p lp m r lp p p } o e p m. Fig. 3l p ˆ p. kp p p lp p s 0.058e 10s = Us () 38.9s + 1 p, pp p p lp p s e 6s = Us () 85.3s + 1 pl. r p p e (8)p e (7)p p k (7) (8)

4 ˆm ql v p l p m rl 15 Fig. 3. Step responses for positive (a) and negative (b) input changes. Fig. 4. PI control responses designed by the IMC-PI tuning rule. p. p p r ˆ pr k tp p m p p m d p ˆ. v, s nl p m p p. e le e (8) yp p p. e p n r ˆl l e p p ppp ˆ. rl p o p p lk. Ž pp p n p re. s 0.074e 8s = Us () 54.4s + 1 p p p v l llv p. p p r p Ž p p p. p o p l x p l p ov lp r kv pp q s p. v, x 0.23 pr e v pp vv k op p v pp m. p sql p k p p p l p p m k. p DA p 1,500l re. k p p o l pp p o l p k p m. p p m l t m p rlp, k p o p m p v p n e rp, pp rv n ss m. p m., k p p o p reˆ p o p rl o p n m Tuning e (9)l tlv p e vl p Ž pn l PI r l p IMC p m. rl rn kv p pv kk. Fig. 4l PI rl ˆ l. r 20l 300 o Cp, 400l 280 o Cp m. PI rl n m, IMC-PI o, v p e 16 m. r rp ±5 o C ov r l p n l p r l e km (9) Fig. 5. Long-time operation under the PI control. p m. k p p, er op p, p p s p n p t rl l npp p. tn n p r l feedforward ˆ p rl pp p p. PID rl rn l k, p pv kk. p e (9) k p p e vlp e l rl rll qp p p n l p p. PI rl p p Ž. Fig. 5 qe k ±5 o Cp m o m rl l t. p nrp x p 0.3r ov p pp, n p t pr v kp k p. 100l e kp nrp, }pl p n l k 3e k rl e p l k. Fig. 6l ˆ l. v p r ˆ ±5 o Cp v p pv, 100l e p v l v p ±10 o C ˆ p, rp m lv m. p p r q lt p. m e p pp, r p p 0.08~010, e 80~90 pp p mp, e vlp p ll. Ž p m e p l Korean Chem. Eng. Res., Vol. 45, No. 1, February, 2007

5 16 të v ËpvˆË Fig. 6. Operation after 100 hours from loading new catalysts. š lp, r ˆl p v p p l r p š l. rp rl o q vp rp hot-spotp o e p m. e e p 8e r mp, k 100 e kp hot-spot o r m., ~ e l r hot-spot o trp k 0cm e m. 12pw e l p o 3.3 cm mp o 0.3 cm/day r p. p p r pl p rl lp nrp p Ž, p p e p p. 5. p v v pp lrp eˆ q l v p rl n rp l m. v p krrp nr rp rl o on p v t m. pp r ˆ o p l p e l rn l l p e m rp p }k. l l q p r e ep s l p l. e p o rp s p l, m rl o l v e m. kr nr s p } o e p m. ~ nrl pp lp p pn 1 kw p v p l 100e p n k v p p m ±5 o C l rl m., qe k o m ov e l 5e p lp v p nr m. p e p rp p r v k p m l o s p rs p. p o s p r p o l ov rl n, p e l p p l p v p p l rl edšp n p. v p p scale-upl rl edšp l n p p. y 1. Kim, D. H., A Study on Improvement of Fuel Cell Reformer, Minis. Ener. Res.,( ). 2. Pukrushpan, J. T., Stefanopoulou, A. G. and Peng, H., Control of Fuel Cell Power Systems, Springer, London(2004). 3. Kim, J. Y., The Production of Hydrogen for Fuel Cell by Methanol Partial Oxidation Reforming, MS Thesis, Depart. Chem. Eng., Kyungpook Nat. Univ.,(1999). 4. Kim, S. J., Temperature Control in the Methanol Autothermal Reforming Reactor for the Production of Fuel Cell Hydrogen, MS Thesis, Depart. Chem. Eng., Kyungpook Nat. Univ.,(2000). 5. Seborg, D. E., Edgar, T. F. and Mellichamp, D. A., Process Dynamics and Control, Wiley, New York(1989). 6. Dusterwald, H. G., Hohlein, B., Kraut, H., Meusinger, J., Peters, R. and Stimming, U., Chem. Eng. Technol., 20(7), 617(1997). 7. Lattner, J. R. and Harold, M. P., Appl. Catal. B: Environ., 56(1-2), 149(2005). 8. Lattner, J. R. and Harold, M. P., Catal. Today, 120(1), 78 (2007). o45 o k

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