수소가스화기에서석탄의메탄화반응특성. Characteristics of Coal Methanation in a Hydrogasifier

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1 Korean Chem. Eng. Res., Vol. 44, No. 6, December, 2006, pp 수소가스화기에서석탄의메탄화반응특성 m Çl qç iyç m Çmm l v l o ˆr l r le o q 71-2 (2006 2o 14p r, o 8p }ˆ) Characteristics of Coal Methanation in a Hydrogasifier S. H. Lee, S. J. Yoon, Y. C. Choi, J. H. Kim and J. G. Lee Coal Conversion Research Center, Korea Institute of Energy Research, 71-2, Jang-dong, Yuseong-gu, Daejeon , Korea (Received February ; accepted August ) k ˆp d pl }l d(substitute natural gas, SNG) rs p o l l e lab-scale d (v : m, p :1.0m) pn m. d edšp k d tp, ˆ tpedš, d p, p q p lr. e p pm 600~800 o C, / ˆ 0.2~0.4, ˆtp 0.8~2.5 g/minp ol l. 6s p ˆe n e pm v ˆ l p ˆ r pp v mv v p ˆp s l ˆ. / ˆ v ˆ r pp v, ˆ p m. ˆ e tl ˆ p v ˆ r pp v mp, ˆt p 35 wtíp p ˆ r pp lp pl. h Abstract To investigate the characteristics of substitute natural gas (SNG) production from direct coal methanation, the continuous lab-scale entrained flow hydrogasifier (I.D. : m, Height : 1.0 m) was used in this experiment. The hydrogasification system consisted of high pressure gas handling system, high pressure coal feeder, entrained flow hydrogasifier, and unreacted char separator. The experiment was performed at the various conditions of reaction temperature (600~800 o C), H 2 /coal ratio (0.2~0.4), and coal feed rate (0.8~2.5 g/min). Although it was shown that carbon conversion was different trends with coals from the methanation results for 6 sample coals, the carbon conversion increased with increasing reaction temperature. And it increased with increasing H2/coal ratio, whereas the concentration of CH4 decreased. Also. the carbon conversion increased with the carbon content of coal sample and had a maximum value at volatile matter content of 35 wt. Key words: Coal, Hydrogasification, Methanation, Zero Emission, Hydrogen 1. ˆp }l d(substitute natural gas, SNG) rs r r l l mp 70 p e lp, oo p kr m }l d } eq r p vl kp. [1-3] l v v m mm r mmp l n l vpn p p p 90 v p tep n l l eq m. p p r r(zero emission coal alliance, ZECA)p ˆp mm vp v k r f, ˆ To whom correspondence should be addressed. jaegoo@kier.re.kr p }l d p ˆ, rp ~ sr p CO 2 m H 2 l l rv p [4,5]. ZECAl n d rp q p /ˆ p p ˆp }l dm o SNG r p ˆ, rl ˆp pn l n p p o p rp t rp. ˆ d l p }l d p, v pn l d pp pp d(co, H 2 ), p pp ˆp r eˆ p ˆ (methanation) m ˆp m k l vr ~ pl p ˆ d (hydro-gasification) pp [6]. l p ˆp d pp v, CO 2 l p d p n l p p. pl n o l 631

2 632 pe Ëo tëm Ë q Ëpq v lk d p l l p l pn p p p. ˆ ~ pp m p ƒ vp n q l, kv v d pl COm H 2 p pl p d r p rp en n r tl pp, ˆ p vr pl p d rp q l p [5, 6]. v m, op p r kp r l n v pp m, k ˆl ˆ p d l l ˆp. l l d p pn l pm, / ˆ, ~ tp, ˆp s l d p p m. 2. m ˆp d e p l rp o l l n(labscale) d p pn m. l n d edšp k d tp, k ˆ, d p, q v, d edš(gc, HP 6890)p l pp Fig. 1l ˆ l [7]. k d t p d e l n m srp o v MFC pn l r rp tp p mp, d pl ~ l dtp t p p t p p l v q m. d p p v p mp p 1mp, m rl o 5 kw o l n mp pm 1,200 o Cp. p p m r o l K-type lr (thermocouple) mp p l r m m rl (han young, P-100) 10 o r m. p p k p k (valcom, VPMC-A3) v p p ee p r m. p p l tp ˆp l l l p v o l ˆ tp l p m. p p l p l l k p o ov m. ˆ e p p l r ožl p ˆp srp ožp r rl p f (0.3~3 g/min)p sr. n r e d p p k p q v k q p k p p ov m. e p Œ p o 1 n d(n 2 )m p Œp lp, p dp (secondary gas)m p p l tp m. p p p k p p k p k l p k r p f s p ov m. p l lp d q l k sr (back pressure regulator) l. p k rl rrp k sr p lv vl p š n pp v r n l n m. d t ˆ dp r o l NDIR type analyzer(model) l r mp r~ dp p GCl p m. q p krp l p k p 4 l r l rk v e p dm ˆp tpp m. ˆp t p, v p pm, k ˆ dp q v (model : PCL812) PCl rq m. Fig.1. Lab-scale hydrogasification system. Table 1. Proximate and elemental analysis of sample coals Coal Alaska Curragh Cyprus Datong Drayton Kideco Proximate Analysis (daf. wt ) Ash Volatile Matter Fixed Carbon Ultimate Analysis (daf. wt ) C H N S o44 o k

3 d l ˆp ˆ p 633 ~ d pp p e rl p qs p ~ v pn l r ~p v p k p 80 k v deˆ e p ee m. p l d p v kp m k p 800 o C, 80 k v de kr e p ee m. e 0.3~3 g/min tp mp p p q v d pn l r m. e tp p o m v deˆ p dp MFC n l o k v de p p p ee p r m. p r ˆl 1~2e k nr s p v e s l }l d rs p s m. p p krp o l 90 k p p p k p d p p p ~ tpp p p ~ e p p p m. ~ d e l n e p l l n p olˆ(kideco, Drayton ˆ ) 6sp mp, p r pp l o l 200 mesh p p e p e mp p Table 1l ˆ l. 3. y ˆp d pp p l p char p d pp el v q pp. C+2H 2 Ë CH 4 (1) d p l tp ˆp s, l l p p, charp, charp d p p rp pl. p pp }l d lp r mp l p d pp el v lk. Lee [6]p l e p ˆ p l 60 k p p kl d pp n pl m. r~ ˆ l l l p ˆ p k p 5Í p m [7]. Kideco ˆ Drayton ˆp pm l ˆ r pp Fig. 2 l ˆ l. p p k p d pp n 66 k p mp Kidecoˆ Draytonˆp 2.5 g/min, 1.6 g/min p tp m. ˆ r pp d tp ˆ d m t p ˆp ˆ (CH 4 (g)/carbon(g)) r m. l p p m v ˆ r pp v p k p. Kidecoˆp m v l rp v m, Draytonˆp rml v p mp ml v m. rml p p p ˆ p k ˆ r pp kp m v pp r ˆ p p r p v p m. p rp l l pl ˆp l m l m p n ˆ [7]. TGA q l Antelope ˆp d p e ˆ r p p 90Ím [1]. Karczm Porada[8, 9]p p m 750 K p l d s p m p mp r d p pp v eˆ o rr p n k p k m n m. p 2.5 MPap p s l d l p C 1 ~C 3 p ˆ pp l l 5 p m. / ˆ ˆ r p d s l m p Kidecoˆp e Fig. 3l ˆ l. e k p 66 k p ~ tp p 2.5 g/minp m. l pm 800 Cp n ~rp ˆ r pp d o pv, m d p qkvp k p. p m m tl l p p ~ e p 3.1, 2.0, 1.7 sec p. Lee [7]p / ˆ v, ˆ r pp v mp Fig. 2m v Fig.G2. Carbon conversion with reaction temperature (P : 66 atm). Fig.G3. Carbon conversion with H 2 /coal ratio. Korean Chem. Eng. Res., Vol. 44, No. 6, December, 2006

4 634 pe Ëo tëm Ë q Ëpq Fig. 4. CH 4 concentration with H 2 /coal ratio. Fig. 6. Carbon conversion with fixed carbon content in sample coal. p ˆp s s l p p p. l p lv ˆ r p pm p m p p. 800 o C, 50 kl Alaska, Curragh, Cyprus ˆp ~ tp p l ˆ r pp l Fig. 5l ˆ l. l ~ e p tp p v ˆ r pp ˆl m. ˆp s p l ˆ r p p p ˆ. ˆp v l ˆ r pp d l ˆp e p wkr pl Fig. 5. Carbon conversion with coal feed rate. ˆl p p p p l v. Sheth [10]p v / d e l p kp v r~ d p m. / ˆ l ˆp r l Fig. 4l ˆ l. l / ˆ v ˆp p ˆ. p Fig. 3p l p, ~ e p v m p. tp ˆ p pr tp v l dl p kp v l rp ˆ dp m p l v. e p Lee [7]p m p. p rp / ˆ v pl l p v l pp p f ˆ r p p v p [7]. Kideco, Drayton ˆp nm p p ˆ o44 o k Fig. 7. Carbon conversion with volatile matter content in sample coal.

5 l v k ˆ p kp v p. p l d pp nl ~ e p v o l p p ˆ p p q p k p p. pm, / ˆ, ~ tp p nr s l ˆ r p, }l dp ˆ p s l p p k p. p ˆp s p p. l m l l m p rˆ m p d pl m p p. pl Fig. 6 7l ˆp r ˆ m p l ˆ r pp l ˆ l. l ˆ p ˆ p v e m l ˆ p r pp v p ˆ. p m p v v p m. p p p l l p l ˆ p r pp v 35 wtí p p pl l ˆ p kp tl p r pp lv p l v. 4. r rl n d p p o l lab-scale d l e m. pm 600 o Cl 800 o C v p ˆl d p p v m. Kideco ˆp m v l ˆ r pp 10~30Í v mp Drayton ˆp 5~35Í v m. / ˆ v ˆ r pp v mp p m l d p qk. d p }l d s p ˆ k p ˆ l. nr d l ˆp ˆ p 635 s l ˆp p ˆ r p }l dp s p p ˆ l. pl ˆp s l d p l ˆ r pp, ˆl l p rˆ p v ˆ r pp v mp p 35 wtí p p r pp ˆ l. y 1. Ziock, H. J., Anthony, E. J., Brosha, E. L., Garzon, G. D., Jhonson, A. A., Kramer, A., Lackner, K. S., Lau, F., Mukundan, R., Nawaz, M., Robison, T.W., Roop, B., Ruby, J., Smith, B.F. and Wang, J., 19th Pittsburgh Coal Conference, Pittsburgh, USA, 25-2(2002). 2. Meyer, M. and Koss, U., 20th Pittsburgh Coal Conference, Pittsburgh, USA, 23-2(2003). 3. Wang, J. and Anthony, E.J., 20th Pittsburgh Coal Conference, Pittsburgh, USA, 21-4(2003). 4. Lee, S.H., ETIS, 26, 32(2005). 5. ZECA Corporation, Suite 502, 205 Ninth Avenue SE, Calgary, Alberta, T2G 0R3, Canada, 6. Lee, J. G., Lee, S. H., Choi, Y. C. and Kim, J. H., 5Th China- Korea Joint Workshop on Clean Energy Technology, Proceedings, 270(2004). 7. Lee, S. H., Lee, J. G., Kim, J. H. and Choi, Y. C., Fuel, 85, 803 (2006). 8. Karcz, A. and Porada, S., Fuel, 74, 806(1995). 9. Karcz, A. and Porada, S., Fuel, 75, 641(1996). 10. Sheth, A. C., Sastry, C., Yeboah, Y. D., Xu, Y. and Agarwal, P., Fuel, 83, 557(2004). Korean Chem. Eng. Res., Vol. 44, No. 6, December, 2006

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