Investigation of a Dual-Bed Autothermal Reforming of Methane for Hydrogen Production

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1 Investigation of a Dual-Bed Autothemal Refoming of Methane fo Hydogen Poduction Amonchai Aponwichanop *, Manatsanan Wasuleewan, Yaneepon Patchaavoachot, and Suttichai Assabumungat Depatment of Chemical Engineeing, Faculty of Engineeing, Chulalongkon Univesity, Bangkok 10330, Thailand, Amonchai.A@chula.ac.th This pape pesents a pefomance analysis of a dual-bed autothemal efome of methane fo hydogen poduction. The fist section of Pt/Al O 3 catalyst is designed fo oxidation eaction, wheeas the second one involves steam efoming eaction based on Ni/MgAl O 4 catalyst. A one dimensional, non-isothemal eacto model was employed to examine the efome pefomance egading impotant opeating conditions such as H O/CH 4 feed atio; O /CH 4 feed atio, tempeatue and location of steam feed. The simulation esults indicate that when the dual-bed efome was opeated at the H O/CH 4 feed atio of and O /CH 4 feed atio of , the methane convesion of 93% and the H /CO poduct atio of highe than.9 wee obtained. In addition, it was found that adding steam at lowe tempeatues to the steam efoming section of the dual-bed efome can poduce the synthesis gas with a highe H /CO atio. 1. Intoduction Hydogen is consideed a clean and sustainable enegy that can be efficiently conveted into many useful enegy foms. In addition, it is a significant enegy souce along with the development of a fuel cell technology. Pesently, most hydogen is deived fom methane using vaious efoming methods, i.e., steam efoming, patial oxidation and autothemal efoming. Although a steam efoming povides the highest hydogen yield compaed with the othe efoming pocesses, it involves a highly endothemic eaction, which equies high extenal heat souce. In a patial oxidation pocess, methane is combusted unde a condition of limited oxygen. Although a lage enegy input is not needed fo this pocess, hydogen yield is a majo concen. Recently, vaious studies have been conducted to develop an autothemal efoming pocess by coupling an endothemic steam efoming with an exothemic patial oxidation (Hoang and Chan, 007; Wang, 008; De Casto et al., 010). The heat balance of both the eactions leads to a themally neutal pocess and thus a moe compact system (Authayanun et al., 010). In the autothemal efoming pocess, a consecutive eaction pathway that a total oxidation of pat of fuel is caied out to poduce CO and H O, followed by a steam efoming of the emaining fuel with steam, is occued. Since the oxidation eaction is faste than the efoming eaction, a lage tempeatue gadient in the autothemal efome is geneally obseved. The pesence of a hot spot in the autothemal efome

2 may affect stability and safety of the pocess and sevee catalyst deactivation by sinteing and cabon fomation (Li et al., 006). In ode to contol the eaction tempeatue, the autothemal efome should be opeated unde suitable conditions. Pevious investigations showed that the addition of moe steam to the autothemal efome deceases the efome tempeatue and inceases hydogen yield because the methane oxidation is less ponounced (Simeone et al., 008). Consideing an opeation of the autothemal eacto, Ni-based catalyst is nomally employed to catalyze both steam efoming and oxidation eactions. Howeve, the use of diffeent catalysts fo each eaction in the autothemal eacto is moe effective (Zhu et al., 004; Li et al., 006; Meng et al., 010). In this wok, a pefomance of the dual-bed autothemal efoming of methane fo hydogen poduction is analyzed. A non-isothemal, one-dimensional eacto model is used to investigate the efome pefomance in tems of methane convesion and H /CO poduct atio. The effects of H O/CH 4 feed atio, O /CH 4 feed atio and tempeatue and location of steam feed ae examined to detemine an optimal condition of the dual-bed autothemal efome.. Mathematical model of a dual-bed autothemal efome A dual-bed autothemal efome is geneally an adiabatic fixed-bed eacto in which the catalyst bed is divided into two sections, as schematically epesented in Figue 1. The fist section involves the oxidation eaction based on Pt/Al O 3 catalyst, wheeas the second one involves the steam efoming eaction based on Ni/MgAl O 4 catalyst. The efome feeds consist of methane, steam and ai. Methane is eacted with oxygen to poduce cabon dioxide and steam - Eq. (1). Then, the emaining methane and the othe gaseous components ente the second catalytic zone, whee hydogen-ich gas is poduced via steam efoming and wate gas-shift eactions (Eqs. ()-(4)). In this study, it was assumed that the oxidation section occupies the eacto volume of 10%. CH + O CO + H O 4 CH + H O CO + 3H 4 CO + H O CO + H CH + H O CO + 4H 4 o ΔΗ = 80.3 kj/mol (1) ΔΗ 0 = 06. kj/mol () o ΔΗ = 41. kj/mol (3) o ΔΗ = kj/mol (4) Figue 1: Schematic of a dual-bed autothemal efome.

3 A one-dimensional model was employed to investigate the pefomance of the autothemal efoming of methane in a dual-bed efome: Mole balance equations fo component i: 4 dni = (1 ε) Aρcat υη i ji, j (5) dz j = 1 Enegy balance equations: 4 dt nc i p, i = (1 ε) Aρcat ηjj ( ) j dz ΔΗ (6) i j= 1 The value of the effectiveness facto (η j ) of the eactions - Eqs. (1-4) - used to account fo a intapaticle tanspot limitation ae 0.05, 0.07, 0.70 and 0.06, espectively (Chan et al., 005). The kinetic ate expession fo the total oxidation, steam efoming and wate gas-shift eactions ae extacted fom Halabi et al. (008) as shown below: k p p k p p 1a CH4 O 1b CH4 O 1 = + ox ox ox ox + KCH p 4 CH + K 4 O p O + K CH p 4 CH + K 4 O p O (1 ) (1 ).5 3 k / ph ( p CH p 4 HO ph p CO / K eq,) = (1 + KCO pco + KH ph + KCH pch + KH O ph O / ph ) 4 4 k / p ( p p p p / K eq ) 3 H CO HO H CO,3 3 = (1 + KCO pco + KH p H + K CH p 4 CH + K 4 HO pho / ph ) k4 / ph ( p CH p 4 HO ph p CO / K eq,4) 4 = (1 + KCO pco + KH ph + KCH pch + KH O ph O / ph ) 4 4 (7) (8) (9) (10) Tables 1 and show the Ahenius kinetic paametes of eaction ate constants and the Van t Hoff paametes fo species adsoption used fo calculation of eaction ate and equilibium constants, espectively. Table 1: Reaction equilibium constants and Ahenius kinetic paametes Reaction k 0j (mol/(kg cat s)) Ea j (kj/mol) K 0j H j 1 k 1,a ba k 1,b ba k ba k ba k ba Table : Van t Hoff paamete fo species adsoption K oi ΔH ads,i (J/mol) K oi ΔH ads,i (J/mol) K 0 CH ba K CO ba K 0 O ba K H ba K CH ba K HO

4 Mole faction of component xch4 xho xo xco xco xh Length (m) Figue : Composition pofiles in a dual-bed autothemal eacto at standad conditions. 3. Results and discussion The fixed-bed efome consideed in this wok is of cylindical shape with 0.04 m in diamete and 1 m in length. Unde the standad conditions, steam and oxygen ae mixed with methane and intoduced to the efome at the tempeatue of 800 K and the atios of 1.5 and 0.5, espectively. Figue shows the composition pofile of each component in the dual-bed autothemal efome. In the oxidation section, O is completely eacted with CH 4 and H O and CO ae poduced. When the poduct gas passes though the efoming section, CH 4 and H O ae apidly consumed to geneate H, CO and CO. It is obseved that H is moe poduced due to the wate gas-shift eaction. Consideing a efome tempeatue of the dual-bed efome, it is found that the tempeatue inceases shaply and eaches to its maximum value of 169 K in the oxidation section and then dops to 1063 K due to an incease in the methane efoming ate. In compaison with a conventional autothemal efome, the dual-bed efome povides a highe maximum tempeatue, wheeas the outlet tempeatue is identical. 3.1 Effect of H O/CH 4 feed atio A H O/CH 4 feed atio is vaied in the ange of while an O /CH 4 feed atio is kept constant at 0.5. The esults show that the methane convesion deceases but the H /CO poduct atio inceases with inceasing the H O/CH 4 feed atio. When moe steam is added to the efome, the eacto tempeatue is educed which in tun leads to lowe efoming and oxidation ates. In addition, the equilibium of the wate gas shift eaction moves towads the poduct side, esulting in a highe H /CO poduct atio. This implies that the addition of steam has a key effect on the efoming ates and the tempeatue of autothemal eacto. Howeve, it can be obseved that an incease in the H O/CH 4 feed atio fom 1.0 to.5 has no impact on the methane convesion. This is because O is moe active than steam; theeby, the oxidation eaction is moe significant than the efoming eaction. Compaing with a conventional efome, when opeating at the H O/CH 4 feed atio of , the dual-bed efome shows slightly highe

5 methane convesion and gives the hydogen-ich gas with a lowe H /CO atio due to the inceased efome tempeatue. Fo an opeation at the H O/CH 4 feed atio of moe than.5, the methane convesion and the tempeatue outlet of the conventional and dual bed efome decease with inceasing the H O/CH 4 atio because a high amount of steam in feed lowes the oxidation and efoming ates. 3. Effect of O /CH 4 feed atio In this section, the effect of O /CH 4 feed atio on the efome pefomance is studied. The H O/CH 4 feed atio is kept constant at 1.4. The esults indicate that when the content of O in the feed steam is highe, the methane convesion inceases but the H /CO poduct atio deceases. An incease in the O /CH 4 feed atio aises the ate of methane oxidation which in tun inceases the efome tempeatue and thus, the steam efoming eaction is moe ponounced. Howeve, wate gas-shift eaction disfavos a high tempeatue opeation, moe CO in the poduct steam emains. Simila esult is obseved fo a convention autothemal efome. 3.3 Effect of steam feed position Since the addition of steam has a significant effect on the dual-bed autothemal eacto, especially in the steam efoming section. The position of steam feed is investigated hee and it is found that adding steam in the oxidation section of the efome does not affect the methane convesion and the H /CO poduct atio. This is because the oxidation eaction dominates the efome pefomance in this section. Howeve, the addition of steam in the steam efoming section (z = m) leads to a educed methane convesion while the H /CO poduct atio can be impoved due to an inceased ate of the wate gas shift eaction. At z > 0.15 m, the steam efoming pocess is completely caied out and thus, the vaiations in the methane convesion and H /CO poduct atio ae not obseved. 3.4 Effect of steam feed tempeatue An impact of the steam tempeatue on the methane convesion and H /CO poduct atio is studied. Steam with diffeent tempeatues vaying between 400 and 800 K is intoduced to the efome at z = 0.10 m. The simulation esults show that an incease in the feed tempeatue of steam ises the efome tempeatue. As a esult, the oxidation and efoming eaction ates is inceased and a highe methane convesion can be obseved. By contast, feeding steam with a highe tempeatue deceases the H /CO poduct atio due to a deceased wate gas-shift eaction. 4. Conclusions In this wok, a dual-bed autothemal efome in which two pack beds of Pt/Al O 3 and Ni/MgAl O 4 is connected in seies, to poduce hydogen fom methane was investigated by using a one-dimensional model unde steady-state and non-isothemal conditions. The simulation esults show that the dual-bed autothemal eacto povides highe eacto tempeatue and methane convesion compaed with a conventional fixed-bed efome. When the dual-bed eacto was opeated with the H O/CH 4 atio of and O /CH 4 atio of , the methane convesion and H /CO poduct atio ae moe than 93% and.9. Adding moe steam at the same tempeatue of feed steam into

6 the steam efoming section can impove both methane convesion and H /CO poduct atio. When steam is added at lowe tempeatues, it was found that the H /CO poduct atio is enhanced even the methane convesion is lowe. 5. Acknowledgement Suppot fom the Thailand Reseach Fund and the National Reseach Univesity Poject of CHE and the Ratchadaphiseksomphot Endowment Fund (EN80A) is gatefully acknowledged. Refeences Authayanun, S., Aponwichanop, A., Paengjuntuek, W. and Assabumungat, S., 010, Themodynamic study of hydogen poduction fom cude glyceol autothemal efoming fo fuel cell applications, Intenational Jounal of Hydogen Enegy, 35, Chan, S.H., Hoang, D.L. and Ding, O.L., 005, Tansient pefomance of an autothemal efome-a -D modeling appoach, Intenational Jounal of Heat and Mass Tansfe, 48, De Casto J., Rivea-Tinoco R. and Bouallou C., 010, Hydogen poduction fom natual gas: Autothemal efoming and CO captue, Chemical Engineeing Tansactions, 1, Halabi, M.H., de Coon, M.H.J.M., van de Schaaf, J., Cobden, P.D. and Schouten, J.C., 008, Modeling and analysis of autothemal efoming of methane to hydogen in a fixed bed efome, Chemical Engineeing Jounal, 137, Hoang, D.L. and Chan, S.H., 007, Expeimental investigation on the effect of natual gas composition on pefomance of autothemal efoming, Intenational Jounal of Hydogen Enegy, 3, Li, B., Kado, S., Mukainakano, Y., Nuunnabi, M., Miyao, T., Naito, S., Kunimoi, K. and Tomishige, K., 006, Tempeatue pofile of catalyst bed duing oxidative steam efoming of methane ove Pt-Ni bimetallic catalysts, Applied Catalysis A: Geneal, 304, Meng, F., Chen, G., Wang, Y. and Liu, Y., 010, Metallic Ni monolith Ni/MgAl O 4 dual-bed catalysts fo the autothemal patial oxidation of methane to synthesis gas, Intenational Jounal of Hydogen Enegy, 35, Simeone, M., Salemme, L., Scognamiglio, D., Allouis, C. and Volpicelli, G., 008, Effect of wate addition and stoichiomety vaiations on tempeatue pofiles in an autothemal methane efoming eacto with Ni catalyst, Intenational Jounal of Hydogen Enegy, 33, Wang, H.M., 008, Expeimental studies on hydogen geneation by methane autothemal efoming ove nickel-based catalyst, Jounal of Powe Souces, 177, Zhu, J., Rahuman, M.S.M., van Ommen, J.G. and Leffets, L., 004, Dual catalyst bed concept fo catalytic patial oxidation of methane to synthesis gas, Applied Catalysis A: Geneal, 59,

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