PSA
* *†
*
(2002 3 2 , 2002 7 15 )
Process Simulation for Hybrid System Consisting of Membrane Steam Reformers and a Layered PSA
Young-Jae Choi, Uk-June Lee*, Min Oh*† and Sung-Taik Chung
Department of Chemical Engineering, Inha University, Inchon 402-751, Korea
*Department of Chemical Engineering, Hanbat National University, Daejeon 305-719, Korea (Received 2 March 2002; accepted 15 July 2002)
-PSA ! "#$
%&'. ( ) * +( ,-. /0 PSA* +( -1,-2* 345 627, +( ?@ AB CD EFG H 16% IJK L 6M'. NO PQ RJS T U -G) H 0.31 P 0V#2* WXY O Z[+\ '] ^ Z[ _2* `Eab /0 PSA <
XO -1&27 99.999%* Pcd'. /0 PSA e '] WX JSf 'a o IJ>M'. pq a( -PSA kG#$ Oi L 6M'.
Abstract−In this study we propose hybrid system consisting of membrane steam reactors and a layered PSA process, and carry out theoretical analysis by means of modelling and process simulation. The proposed system is comprised of the reaction part including membrane reactors and separation part including a layer PSA column. Detailed mathematical description for each process is developed and dynamic simulation for the combined process is performed. The reaction part contains two mem- brane reactors and the methane conversion of the system is improved more than 1% comparing with the conventional one mem- brane reactor system. The hydrogen mole fraction at the exit of the membrane reactor is approximately 0.31 but in order to use it for a commercial purpose, layered PSA process, which includes two adsorbents, is employed. The purity of hydrogen gas at the exit of the layered PSA is 99.999%. By recycling all useful gases from the layered PSA except hydrogen to the membrane reactor as a feedstock, the process efficiency is highly improved. In particular, the hydrogen recovery is improved as much as 9% comparing with the non-recycle system. It is, therefore, concluded that the proposed hybrid system contributes to the effi- cient production of high purity hydrogen.
Key words: Membrane Reactor, PSA, Modeling, Simulation, Hybrid System, Novel Configuration
1.
! "#$% &'( ) , *+, ,
- . "#/0 12 34$% & 5607. 892- : "#;
NOX, SOX, CO, CO2 : < => ?@ ABC'2D EF: G H I JKL'2: "# ) MN 34 % &7. OP
'2 Q/ R, S T8 4U ) O> : 3S V
>0 W0 "#$% &'(, XY 3S V> :< R, Z 0 [\ 4] % OP^ _`'2 abc &7[1].
de : fg H 34 hi j k OP^ _`'2
R, l2m _` Q 8n4 opY qr$% &'(, de s St 0# : R, ; 0u v; 8n: GH wxy z: {07. |i} s 0# 3S V> ~; 7 |i } s :< ~S 4 ~x '2 n KK(,
: N0 :< ~- R 4
'2 P'2 , 7. ~- R 4 |i
†To whom correspondence should be addressed.
E-mail: minoh@hanbat.ac.kr
} s P'2 '2D P ~0 R= '2 c _'2: ~0 k LoY qr$(, 3S V> ~
E ; - ~0 4 ! 7[2].
s ~S 3S V> ~- ~ ¡ ¢B£S
¤ P^ 8ny :< ¥$¦'(, Adris [3]; 7
: |i} §s "# ¨ ©ª s ~S-: 3S V> ~ Q< P « ¬ % 0 Q 0P 8n
r ®7. Shu [4]; 7 U¯^U U°± |i} s KK, ©ª s ~S-: 3S V> ~ Q
²³P 8n r ®%, Xuu Froment[5, 6]: ~«x ´¤
. µ¶ ~S(plug flow reactor) « "# .y: ²³wxu ·, ¸¹ ®7. 0y: 8n 0- Barbieriu Di Maio[7]
" < 3S V> Q |i}-s ~Sy:
¢ ºº: zH ªV »y ¼ y, m~ 4U /, ½ g,
u ¾=: ¿ Q Àx 8nÁ7. 0 Â ÃÂ ~S ? Q< "4 r$Ä% Å, wxy ÆÇ
{ÈÉ ¤ ²³ wxu · ®7. Â ~S: OÊ, ~S Ë
~-: 0 : Ì7 ÍYb c-
4 Î{(, 0 wx ¡: A4 ~ Ï &Ð a
&Ä7. Madia [8]; Pd-Ag s ~S- , ~=x m~ 4U : / ~=: ¿ x v; ¤ 4K ªV» »BC' 2D 3S V> ~-: Àx Q 8n Á7. Í Ñ'2Ò: Ó0 ~S: @n-: ¡ ªÊ zH ( ¡0 ~S: Ô0_ hÕ n? Ö! :×Ø aÙ7. XY ~=: /0 Ú Û ~S-: K S
JK: f0 K ÜÝ OÊ, Þ: 0 AØ aÙ
%, ²³ wx Sß P « {Èà7. Kim [9];
|i} s ~S 0# 3S V> ~- áâ:
S -: P# " ®'(, ~S : ç _'2 Î{ è é * "# ®7. ) 0 0#
H2O/CH4 , m~ 4U / .% ¾ê ëO : »4
¡ Eì ¸¹ ®7.
JK íî O: ïâ- ]0{ ]-
# =>0 ðØ$% & R4U2Ò # 4U ñç
S 7ò _` z PSA ªÊ À¡P0% OP^
_`'2 abc &7. PSA ; R,/x óH ô :×
¤ V: õö÷'2 n$&'(, ø¡x ô ù0S
"0Ú ¨¥ ¤ 4K úÅ2 0ûc &7.
ü 8n- : V> ~'2Ò %ô: R,< ý
& s V> ~Su ¢ PSA2 n þÿ Fig. 1x v 0 ¥ % 0 Q 0P % B ®7. ¥ þÿ;
2V: |i} s ~S2 n ~x 2V: ðØ
¢ PSA2 n '2 { q7.
~ "# 2V: |i} s ~S BU; Choi [11] :
Z0 Ì% &7. hi- ü 8n- Choi [11] :< p
|i} s ~S BU: nu ~: P « "# ®7.
~- ?@ 4U G P=^ E ~=^
3S, N R=^ Î,, 0, : 0 ðØ
7. %ô: S : 4U x S Ë V: '2 n ¢ PSA ¾$ 4U4
7. PSA 4, õö, A, ö: 4úÅ2 n$ 0 z õöúÅ- 99.99% 0¢: %ô &'(, AúÅ
- ö ÿ4U ~: ¾n2 \ô B L9
íAÝ &7.
0u v; þÿ: 0P 8n , ü 8n-
Q P « ¬ Ë " r ®7. "
: wx ÆÇ {ÈÉ ²³x · ®'( 0 P
«x ": ¸3 ®7. ¸3 : P «
Sß : V>2Ò %ô: R, Þ þÿ
Q n ¥ % 0 Q " r ®'(, 0 S
2.
2-1.
s ~S ©ª4 $ V> ~0 Î{ x s
Fig. 1. Hybrid membrane-PSA system.
40 5 2002 10
R 4 $ '2 n$( 0 "
0 æì |i} s'2 n7. hi- Î~ 3S V> ~S u Ó ~S - ~x 4 ¨B ÎÉ7. 4~
- P ¡; R= z: X
0u v; L #Ï &'(, : P : i: ~0 0 Q QP ¼i Ý &7. XY |i } s; ¤ y2 n S¢ ÿ=2Ò 100%: 4 K% Ý &7 M- ~x 8 Å W; 8n4 0ûc7. |i} sy :
g w úÅ2 R$ g < 4 , ¨¥ À
7Ðx v; ±Å2 {Èq7[2].
(1)
Fig. 2- P'2 |i} s ~S-: s
V> ~ L {ÈÄ7. |i} s; ©ª ~ - R,
8gP'2 Ø'2D ©qB£%, ;
- ù; ¡ #7. |i} s 100% ô ! K s: ò : : : e: N0
2 4 ; è- R,Ï &7. |i} s "#
Qú : V> ~ ´!"- Q$ GH ÆM;
#x |i} g: 4#07. k {4, P^ |i} s:
è; ~ -: ù; ©ª ~ gu ½ g ·
7 Z0(, hi- ù; g 4K s ~Sy: p
0 ªÊ Hn7. g xA ! 34B£ Î _`;
s: $ %0 Z'2 .F- ªÊ &; |i} sy: ã Q
8n4 de y ªÊ op ! r$% &7[2].
2-2. PSA
ü 8n- "#$ PSA ; ¤ 4K: R=0 ¨B
Hn$K '% %ô: R, Z P'2 % &' {, ¾$ 4U4 44K(, , 0,, 0,) 02 0 Q G: (; %b4 Hn7. ), X õö4 X
Q<- *; õö 4K2 0 OÊ V: õö "#<
- L %ô: S +7. 0 OÊ 7Õ >: õö
V: õö÷ "#Ý &'{, ]ì#x m: ò
¢ õö BU "# Z0 -ë 7. õö2 õö
x X- N0 Ì0 ox i0" 5A4 "#$Ä'(,
"0Ú; \ 4úÅ2Ò öúÅ 0.S/K 4V: úÅ2 n
$q7. "0Ú ¨¥ ÷- qr$ SüP^ úÅy
Q è: »u ÷ -: Þ µ¶_ Fig. 3x Fig. 4
{ÈÄ7[10].
Fig. 4 {ÈÉ \ 4úÅ(I)- ~S @n- {u xS
x E ~= R=^ CH4, CO2, H2, CO4 õö÷'2
¾$â- õöúÅ: è/K 4 úÅ07. 01 úÅ2-
4, CO2, H2, CO4 Åg f$K( é õö>^ CH4, CO2, H2, CO õö$%, î õö>: R=^ H24 q7. õö÷ @n2 { R
=^ H2; ä] ä]7. 7Ð'2 QS/K è0 2
K! $ Â AúÅ(III)2 0K(, 0 úÅ- õö é õö
>: ^ CH4, CO2, CO4 Â_'2 3c {Í! $% 0
y; s ~S2 ô $ \"#7. 4Ks'2 Â_'2 N2
4U ¾ B£( ÷ : é õö> 6 öúÅ(VI)
ì( "0Ú 4ì% \ 4úÅ2 0q7.
3.
¥ þÿ: ~^ |i} s ~S Q P «
5 ðØ ¢6 0P %; Choi [11] :< r$Ä'(, ü 8n- ~ Q P «; 0 6 n ®7. )
8 SÞ 0¢SÞ07.
9 BU; 07.
F D A⋅ ---l PH
2,r PH
2,p
( – )[Nm3⁄h]
=
Fig. 2. Principle of membrane reforming.
Fig. 3. Pressure history in the bed for the layered PSA process.
Fig. 4. Flow direction in the bed for the PSA process.
: SÞ¢x õö "0: =>Ó; LDF(Linear Driving Force)
«2 B7.
; ±Å Extended Langmuir *'2 [7.
< õö÷ -: èé Darcy’s Law hÕ7.
= z õö÷: nP^ ^ê(úâP, >) ?Î 7.
@ g, ñ .% Q ~O_ n? ABÝ &7.
=> K*
(2) õö 2: i : =>Ó g*; 7Ðx v0 LDF«
2 [7.
(3) qi* i 4U¢x ¢B & õö/07.
¨P x OCõö %bÝ OÊ: 7Å õö; 7Ðx v0 Extended Langmuir * "#Á7.
(4)
JK K*
(5) õö -: è: » 7Ðx v0 Darcy’s Law2 [
Á7.
(6)
õö- úÅ: GH OÅ ; 7Ðx v7.
OÅ:
I. \ 4úÅ
@z=0 (7a)
@z=0 (7b)
@z=L (7c)
@z=L (7d)
II. õö úÅ
@z=0 (8a)
@z=0 (8b)
@z=L (8c)
@z=L (8d)
III. ÂAúÅ
@z=0 (9a)
@z=0 (9b)
@z=L (9c)
@z=L (9d)
IV. öúÅ
@z=0 (10a)
@z=0 (10b)
@z=L (10c)
@z=L (10d)
úÅ-: valve: ¢B Table 1 {ÈÄ'( =ì æ Å» Table 2 {ÈÄ7.
) Langmuir isothermx LDF « ±D ¤ iEÒ ;
Table 3 {ÈÄ7[10].
PSA : ï · S P=^ H2: ô, ø¡ K2- 7Ðx v0 : ®7.
εt∂Ci( )z
---∂t ρa∂qi( )z ---∂t
+ ∂
∂z---(εbu z( )Ci( )z) ∂2
∂z2
--- D[ z⋅Ci( )z ] +
–
=
∀z∈(0 L, )
∂qi( )z
∂t
---=ki(qi*( )z –qi( )z) ∀z∈[0 L, ]
qi*( )z qsibiPi( )z 1 biPi( )z
i=1 NoComp
∑
+
---
= ∀z∈[0 L, ]
∂
∂t----[(εtρgcpg+ρbcps)⋅T z( )] ∂
∂z
---[εbu z( ) ρ⋅ gcpgT z( )] –
=
+Kz ∂2T z( )
∂z2
--- ρa ∆Ha i, ∂qi ---∂t
⋅
∑
i –UD----⋅[T z( )–Text( )z]⋅
⋅ +
∀z∈[0 L, ]
∂P z( )
---∂z –180µ ε⋅ ⋅b u z( )(1–εb)2 dp2εb3 ---
= ∀z∈[0 L, ]
Dz∂Ci( )z
∂z ---
– εbu 0( ) yRE_0 i,PRE_0 R T⋅ RE_0 --- C– i( )L
⋅
=
P 0( )=PRE_0
∂Ci( )L ---∂z =0 εbu L( )=0
Dz∂Ci( )0 ---∂z
– εbu 0( ) yAD_0 i,PAD_0 R T⋅ AD_0 --- C– i( )0
⋅
=
P 0( )=PAD_0
∂Ci( )L ---∂z =0
εbu L( ) QAD_L ---A
Patm
P L( ) ---
⋅
=
∂Ci( )0 ---∂z =0 P 0( )=PBD_0
∂Ci( )L ---∂z =0 εbu L( )=0
∂Ci( )0 ---∂z =0
εbu 0( ) QD_0 ---A
Patm P 0( ) ---
⋅
=
Dz∂Ci( )z
∂z ---
– εbu L( ) yD_L i,PD_L R T⋅ D_L --- C– i( )L
⋅
=
P L( )=PD_L
Table 1. Operating sequence for valves
STEP Valve 1 Valve 2 Valve 3-R Valve 3-P Valve 4
I Open Close Close Close Close
II Open Open Close Close Close Product
III Close Close Open Close Close Recycle
IV Close Close Close Open Open Purge
Table 2. Parameters used in the simulation
Physical properties of bed and adsorbent
AC layer ZE layer
Bed length (cm) 5
Bed inner dia. (cm) 1
Bed density (g/cm3) 544 691
Bed porosity 0.36 0.36
Particle density (g/cm3) 850 1,080
Heat capacity of adsorbent (cal/g⋅Κ) 6.590 6.904
*AC: Activated carbon, ZE: Zeolite 5A
40 5 2002 10
(11)
(12)
S- purityH2 GS ¨¥: õöúÅ- õö÷ K{ ä]
ä] Þ4U z H2 4U: ¡0(, recoveryH2 GS
¨¥ õö÷ 2 ¾ H24U: ò Q õöúÅ- ä]
-: ¡07.
4.
4-1.
þE PDAEs BU: ì< n S <- ¤ 4K _`0
"#Ï &'{, Method of Lines(MOL) _` Sü F2 "# ® 7. MOL _`- GE _* {È{ & ½ Q E
Eå ðØ ¢E/ Q _* BU'2 » !
7[12].
½ Q Eå 7åe"*'2 S QP^ ì
<`'2 N`, H`, MWR(Method of Weighted Residual), OC(Orthogonal Collocation) _` 0 &7. .¤{ [\/K: GE
_*: ì<` Q 0P 8n4 Gq Æu X ì<
`x: ±Å HY H 0P e 4D< G% &K '' (, "#ê: hi ì<`0 w$ Z0 Î~P07. hi - ü 8n &- º 4K: ì<` "# ¨P" r ®'(, Ix & 4] JK0 & _` Sß 0P 8n qr ®7[12].
½e" Q ìP _`'2 BFDM(Backward Finite Difference Method)
_`: OÊ I0 #0 ! 0ûKS Á'{, 0 _`: ìHP
^ wØ^ ìP ,(Numerical diffusion) [¢0 {ÈL'2D
ÆM0 & Z'2 R$Ä7. OC _`: OÊ ü BUx
" õö÷ "#$ ªÊ *; wx {ÈM Z'2 Ì% $%
&'(, ü õö÷: OÊ NOÝ wx Ì®7. .¤{ 0 _`; Þ Q e" BØ'2D e"7å*: N4 ù
K! $( 4 2K úM0 &, Þ: n½ H
&Ä'(, hi- ü 8n: " 0 _` "# r$
Ä7[12].
õö÷: ç _ hi 10V: H2 {PÄ'(, H
- 3N e": OC on finite elements method "# ®7. ¢
¢B 0.S/K: ¨P¨ Q " r ®% ¨P¨
1ß ½#'2 Å, ®7. Þ0 ¢¢B 0.S/K(PSA: O Ê GSP ¢¢B) " r ®'( RSÒ¢- T ²rB½;
9,212ß 0Ä7.
4-2.
Shu [4]: ²³- s ~S á: 4 500oC2 ÎÝ Û
~S @n-: ¡; 43.5%2 Ì% $Ä'(, ¨Î -
¨P" wx 43.61%2 0.11%: ÍN Ì®7. ) Jang [10]
Park [14]: i0" o'2 q ¢ PSA ²³
-u ¨Î (o/i0" )- : ô · ® Û −0.25%-0.17% "0: ÍN Ì®7. 0u v; · s ~Su PSA Q «5 ":
purityH
2
u L( )
tad_start tad_end
∫
CH2( )dtLu L( )
tad_start tad_end
∫
NoCompi∑
=1 Ci( )dtL---
=
recoveryH
2
u L( )
tad_start tad_end
∫
CH2( )L dtu 0( )
tcy cle_start tcy cle_end
∫
CH2( )dt0---
=
Table 3. Langmuir isotherm parameters, mass-transfer coefficient of LDF model and heats of adsorption
Component ai,1×103[mol/g] ai,2[K] bi,0×107[1/mmHg] bi,1[K] −∆Ha[cal/mol] ki[1/sec]
AC ZE AC ZE AC ZE AC ZE AC ZE AC ZE
CH4 −1.78 −0.29 1.98 1.04 26.60 6.44 1,446.7 1,862.1 4,482 4,635 0.4 0.2
CO2 −14.2 02.09 6.63 0.63 33.03 0.67 1,496.6 3,994.3 6,112 12,128 0.1 0.1
H2 04.32 01.24 0.0 0.36 06.72 2.20 1,850.5 1,159.3 1,879 1,486 1.0 1.0
CO 00.92 −0.58 0.52 0.83 07.86 2.53 1,730.9 2,616.3 3,986 6,954 0.3 00.15
*AC: Activated Carbon, ZE: Zeolite 5A
Fig. 5. Membrane reactor system.
Fig. 6. Methane conversion profile for Case 1 and Case 2.
¸3 ®7.
4-2-1. s ~S: ¡ ·
ü 8n Q¢ BU^ |i} s ~Su PSA z Uä ~
<V |i} s ~S n- Fig. 5u v; 1V s ~
S2 n BU(Case 1) x 2V s ~S2 n BU(Case 2)-: : ¡ · Ìâ Fig. 6x v0 v; ¡2 Bã B½: µ¶ hi : ¡ A¡0 N0 Ì0!
7. Case 1: @n- ¡; 43.61%0% case 2: @ n- ¡; 50.83%2 2V: s ~S BU0 v;
Ô02 0ûq 1V: s ~SÌ7 : ¡0 î 16.6% 4/
¢ Z a &7. 0 case 2: n¢ 01 ~S:
'2 ô m~4U G¾Ø'2D -:
: N ù! y W'2D Î{! 7. ), 01 ~S- : : N ~- R 4 '2 Åg 0
¨ ! $( hi- 0 ~ _'2 Xë0! 7. hi - 54P^ ~0 Åg K$ Þ: ¡ ù0! 7.
4-2-2. õö÷-: ¿ ¡ »
õö÷-: ¿ ¡ » · Ìâ Fig. 7x v0 õö
÷ ¾n-: : ¿ ¡; 0.3280% õö÷ @n x ä]
-: : ¿ ¡; 0.9999 0Ä7. Fig. 8- GSP ¢¢
u v0 õöúÅ(II úÅ)- é õö>^ y0
q$ & õö õö$% î õö>^ õö÷ x â- : ¿ ¡0 34Ø a &7.
Fig. 9 GSP ¢¢B ÓÁ Û, GS Q õö÷ feed
endu product end-: u : ¿¡ B Z07. õö
÷: product end(z=L)- : ¿¡; 4úÅ MM 34 õöúÅ- : ¿¡0 d%2 ùKâ- %ô: 4 Fig. 7. H2 mole fraction profile of PSA inlet and outlet.
Fig. 8. Component mole fraction profile at adsorption step(cyclic steady- state).
Fig. 9. Component mole fraction profile for one cycle at cyclic steady-state.
Fig. 10. Hydrogen recovery profile.
40 5 2002 10
Z a &'(, ) ; õö õö$ : {ÍK ' Ð a &7.
4-2-3. ô ø¡ ·
Fig. 10- PSA: ÂAúÅ- ö 4U s ~
½ hÕ Ø: B2 {ÈÄ7. ßS 200ß/K ; ø¡
Ì0% &'{, . Ë \ô B ù; ø¡ Ì0% &'( G SP ¢¢B 0.Y Û(î 1,300ß) \ô ; 0.695, ô : OÊ 0.6342 \ô B î 9.6% 4/ 34Ø a &7. Fig. 11
; \ô Åu ô Å-: ô {ÈÄ7. OÊ
& : ô 99.999%2 {È\'(, \ô : OÊ ô
A] Æ4 ^ Z'2 {È\7.
4-2-4. õö÷-: »
Fig. 12 õö÷-: » 3NL ½- {ÈÄ7.
: úÅ hi 4U¢y0 õö õö öx ìâ-
: : » Ì®7. õöy0 õö$â- õö :<
4 ¢_ ®74 öx ìâ- ö2 ^< 4 b A a &7.
5.
ü 8n 2V: |i} s ~Su PSA 0 wÿ þ ÿ0 ¥ $Ä'( 0 Q 0P 8n4 r$Ä7. 0P 8n: nÞP^ _`'2 ¥ Q P «5 ¨ P"4 r$Ä7. `- a: u v0 ¥ BU: ~
^ 2V: |i} s ~S-: : ¡0 S×: 1V: s
~S n Ì7 î 16.6% ùÐ a &Ä7. ) |i} s ~
S: ~- { ÿ4U PSA Ø'2D 99.999%
ø ; |i} s ~S \ô BC'2D L9: \o
ô ~- BU: wÿ Q 0P 8n
l2m ¢ : Vp V {: BãM'2 #
! "#Ï & Z'2 "97.
0 aÆ; 1999c ^ Q·: KL : 8n$ÄÐ (INHA-20348).
A : cross-sectional area of bed, area of the membrane [m2] b : Langmuir isotherm parameter [mmHg−1]
C : gas-phase concentration [mol/m3] cp : heat capacity [J/g · K]
dp : particle diameter [m]
D : apparent diffusion coefficient [m2/hr ] D : bed diameter [m]
Dz : diffusivity [m2/sec]
∆H : heat of adsorption [J/mol]
k : mass-transfer coefficient [sec−1] Kz : thermal conductivity [J/m · sec · k]
l : membrane thickness [m]
P : pressure in the bed, at each step [Pa]
Patm : Atmospheric Pressure [Pa]
q* : equilibrium adsorbed-phase concentration [mol/g]
q : concentration of adsorbate in solid phase [mol/g]
qs : saturation concentration of adsorbate in solid phase [mol/g]
Q : volume flow-rate [m3/sec]
R : ideal gas constant [m3· Pa/mol · K]
T : gas-phase temperature [K]
t : time [sec]
U : overall heat transfer coefficient [W/m2· K]
u : interstitial velocity [m/sec]
y : mole fraction [-]
z : length of the bed [m]
ε : porosity [-]
bar Fig. 11. Hydrogen purity profile.
Fig. 12. Temperature profile in 3-dimensional field for cyclic steady-state.
ρ : density [g/m3] µ : gas viscosity [Pa · s]
a : adsorbent AD : adsorption step b : bed
BD : blow-down step D : desorption step g : gas phase i : component p : permeation side RE : repressurization step r : reaction side s : particle t : total bed
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