Simulation and analysis of rapid pressure swing adsorption for hydrogen production

doi:10.11949/0438-1157.20201393

Abstract

Abstract:

At present, pressure swing adsorption is the main technology to produce hydrogen product gas from steam methane reformed gas in the industry. However, the rapid increase in energy demand makes the shortcomings of traditional pressure swing adsorption technology more obvious in terms of productivity. For this reason, a simulation study of hydrogen production from steam methane reformed gas by rapid pressure swing adsorption was carried out. The activated carbon and 5A zeolite were used as adsorbents and the numerical simulation and analysis of six bed rapid pressure swing adsorption process were carried out based on the measured adsorption data of each component in the feed gas on the two adsorbents. After analyzing the temperature, pressure and gas and solid concentration distribution in the bed, the three operating parameters of the feed flow rate, the height ratio of the two-layer adsorbent and purge-to-feed ratio have been investigated for the effect of the rapid pressure swing adsorption process performance. When the feed gas composition is H₂/CH₄/CO/CO₂=76%/3.5%/0.5%/20%, the adsorption pressure is 22 bar, the pressure of purge desorption is 1.0 bar, the feed flow rate is 0.8875 mol·s^-1, the adsorbent bed height ratio is 0.5∶0.5, and purge-to-feed ratio is 22.37%, the purity of H₂ is 99.90% and the recovery is 69.88%. At this time, the yield of H₂ is 0.4713 mol·s^-1. In contrast, although the H₂ recovery of the PSA process is 83.40%, the processing capacity is only 0.39 mol·s^-1, so the productivity is only 0.2472 mol·s^-1when the purity is 99.90%.

Key words: rapid pressure swing adsorption, double layer adsorbent, steam methane reforming, hydrogen production, numerical simulation

摘要：

目前工业上主要通过变压吸附技术从蒸汽甲烷重整气中制取氢产品气。然而，能源需求量的快速增加使得传统变压吸附技术在产量方面的不足越发明显。为此，进行了快速变压吸附从蒸汽甲烷重整气中制取氢气的模拟研究。采用活性炭和5A分子筛作为吸附剂，并以测得的原料气中各组分在两种吸附剂上的吸附数据为基础，进行了六塔快速变压吸附工艺的数值模拟与分析。在分析了塔内温度、压力和固相的浓度分布后，探究了进料流量、双层吸附剂高度比以及冲洗进料比三个操作参数对于快速变压吸附工艺性能的影响，结果表明：原料气组成为H₂/CH₄/CO/CO₂=76%/3.5%/0.5%/20%，吸附压力为22 bar（1 bar=10⁵ Pa），解吸吹扫压力为1.0 bar，处理量为0.8875 mol·s^-1，吸附剂床层高度比为0.5∶0.5，冲洗进料比为22.37%时，可获得H₂纯度99.90%，回收率69.88%，此时H₂产量为0.4713 mol·s^-1。相比之下，氢气纯度为99.90%时，尽管PSA工艺回收率为83.40%，但处理量只有0.39 mol·s^-1，因此H₂产量仅为0.2472 mol·s^-1。

关键词: 快速变压吸附, 双层吸附剂, 蒸汽甲烷重整, 制氢, 数值模拟

CLC Number:

TQ 028.1

NIU Zhaoyang, JIANG Nan, SHEN Yuanhui, WU Tongbo, LIU Bing, ZHANG Donghui. Simulation and analysis of rapid pressure swing adsorption for hydrogen production[J]. CIESC Journal, 2021, 72(2): 1036-1046.

钮朝阳, 江南, 沈圆辉, 吴统波, 刘冰, 张东辉. 快速变压吸附制氢工艺的模拟与分析[J]. 化工学报, 2021, 72(2): 1036-1046.

Figures/Tables 18

Fig.1 Configuration diagram of the six-bed RPSA and PSA process

Fig.2 Process schematic diagram of RPSA and PSA

Table 1 The schedule of six-bed RPSA

时间/s	塔1	塔2	塔3	塔4	塔5	塔6
10	AD1	ER1	ER3	BD	ED3	ED1
15	AD2	PR	ER2	PUR	COD	ED2
10	ED1	AD1	ER1	ER3	BD	ED3
15	ED2	AD2	PR	ER2	PUR	COD
10	ED3	ED1	AD1	ER1	ER3	BD
15	COD	ED2	AD2	PR	ER2	PUR
10	BD	ED3	ED1	AD1	ER1	ER3
15	PUR	COD	ED2	AD2	PR	ER2
10	ER3	BD	ED3	ED1	AD1	ER1
15	ER2	PUR	COD	ED2	AD2	PR
10	ER1	ER3	BD	ED3	ED1	AD1
15	PR	ER2	PUR	COD	ED2	AD2

Table 2 The schedule of six-bed PSA

时间/s	塔1	塔2	塔3	塔4	塔5	塔6
40	AD1	ER1	ER3	BD	ED3	ED1
50	AD2	PR	ER2	PUR	COD	ED2
40	ED1	AD1	ER1	ER3	BD	ED3
50	ED2	AD2	PR	ER2	PUR	COD
40	ED3	ED1	AD1	ER1	ER3	BD
50	COD	ED2	AD2	PR	ER2	PUR
40	BD	ED3	ED1	AD1	ER1	ER3
50	PUR	COD	ED2	AD2	PR	ER2
40	ER3	BD	ED3	ED1	AD1	ER1
50	ER2	PUR	COD	ED2	AD2	PR
40	ER1	ER3	BD	ED3	ED1	AD1
50	PR	ER2	PUR	COD	ED2	AD2

Table 3 Mathematical model of adsorption bed

	数学模型
质量守恒	$- ε b D a x, i ? 2 c i ? z 2 + ε b ? (v g c i) ? z + (ε b + (1 - ε b) ε p) ? c i ? t + ρ s (1 - ε b) ? q i ? t = 0$	(1)
	$ε b ? (v g c) ? z + (ε b + (1 - ε b) ε p) ? c ? t + ρ s (1 - ε b) ∑ i = 1 n ? q i ? t = 0$	(2)
	$D a x, i = 0.73 D m, i + v g r p ε b 1 + 9.49 ε b D m, i 2 v g r p$	(3)
能量守恒	$- ε b k g ? 2 T g ? z 2 + C v g v g ρ g ? T g ? z + ε b C v g ρ g ? T g ? t + P ? v g ? z + h f a p (T g - T s) + 4 h w D b (T g - T 0) = 0$	(4)
	$- k s ? 2 T s ? z 2 + C p s ρ s ? T s ? t + ρ s ∑ i = 1 n (C p a, i q i) ? T s ? t + ρ s ∑ i = 1 n Δ H i ? q i ? t - h f a p (T g - T s) = 0$	(5)
	$k w ? 2 T w ? z 2 + C p w ρ w ? T w ? z - h w 4 D b (D b + W t) 2 - D b 2 (T g - T w) + h a m b 4 (D b + W t) 2 (D b + W t) 2 - D b 2 (T w - T a m b) = 0$	(6)
动量守恒	$- ? P ? z = 150 μ (1 - ε b) 2 ε b 3 (2 r p ψ) 2 v g + 1.75 (1 - ε b) ρ g 2 r p ψ ε b 3 \| v g \| v g$	(7)
吸附等温式	$q i * = (I P 1, i + I P 2, i T s) I P 3, i e x p (I P 4, i / T s) P i 1 + ∑ i = 1 n (I P 3, i e x p (I P 4, i / T s) P i)$	(8)
线性推动力方程	$? q i ? t = k L D F, i (q i * - q i)$	(9)

Table 3 Mathematical model of adsorption bed

	数学模型
质量守恒	$- ε b D a x, i ? 2 c i ? z 2 + ε b ? (v g c i) ? z + (ε b + (1 - ε b) ε p) ? c i ? t + ρ s (1 - ε b) ? q i ? t = 0$	(1)
	$ε b ? (v g c) ? z + (ε b + (1 - ε b) ε p) ? c ? t + ρ s (1 - ε b) ∑ i = 1 n ? q i ? t = 0$	(2)
	$D a x, i = 0.73 D m, i + v g r p ε b 1 + 9.49 ε b D m, i 2 v g r p$	(3)
能量守恒	$- ε b k g ? 2 T g ? z 2 + C v g v g ρ g ? T g ? z + ε b C v g ρ g ? T g ? t + P ? v g ? z + h f a p (T g - T s) + 4 h w D b (T g - T 0) = 0$	(4)
	$- k s ? 2 T s ? z 2 + C p s ρ s ? T s ? t + ρ s ∑ i = 1 n (C p a, i q i) ? T s ? t + ρ s ∑ i = 1 n Δ H i ? q i ? t - h f a p (T g - T s) = 0$	(5)
	$k w ? 2 T w ? z 2 + C p w ρ w ? T w ? z - h w 4 D b (D b + W t) 2 - D b 2 (T g - T w) + h a m b 4 (D b + W t) 2 (D b + W t) 2 - D b 2 (T w - T a m b) = 0$	(6)
动量守恒	$- ? P ? z = 150 μ (1 - ε b) 2 ε b 3 (2 r p ψ) 2 v g + 1.75 (1 - ε b) ρ g 2 r p ψ ε b 3 \| v g \| v g$	(7)
吸附等温式	$q i * = (I P 1, i + I P 2, i T s) I P 3, i e x p (I P 4, i / T s) P i 1 + ∑ i = 1 n (I P 3, i e x p (I P 4, i / T s) P i)$	(8)
线性推动力方程	$? q i ? t = k L D F, i (q i * - q i)$	(9)

Table 4 Mathematical model of auxiliary equipment

设备	数学模型
压缩机	$? d W = P c i n V i n η p γ γ - 1 P c o u t P c i n γ - 1 γ - 1$ $W c y c l e = ∫ 0 t c y c l e d W, ? γ = C p C v$	(10)
缓冲罐	$? T (∑ i = 1 n n i C p g, i) ? t = ∑ b i n = 1 N i n F b i n T b i n y i C p g, i - F b o u t T b o u t y i C p g, i$	(11)
缓冲罐	$? n i ? t = ∑ b i n = 1 N i n F b i n y i - ∑ b o u t = 1 N o u t F b o u t y i$	(11)
线性阀门	$F = C V (P v i n ? - ? P v o u t)$	(12)

Table 4 Mathematical model of auxiliary equipment

设备	数学模型
压缩机	$? d W = P c i n V i n η p γ γ - 1 P c o u t P c i n γ - 1 γ - 1$ $W c y c l e = ∫ 0 t c y c l e d W, ? γ = C p C v$	(10)
缓冲罐	$? T (∑ i = 1 n n i C p g, i) ? t = ∑ b i n = 1 N i n F b i n T b i n y i C p g, i - F b o u t T b o u t y i C p g, i$	(11)
缓冲罐	$? n i ? t = ∑ b i n = 1 N i n F b i n y i - ∑ b o u t = 1 N o u t F b o u t y i$	(11)
线性阀门	$F = C V (P v i n ? - ? P v o u t)$	(12)

Table 5 Process performance indicator

指标	数学模型
纯度	$p u r i t y H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F o u t d t$	(13)
回收率	$r e c o v e r y H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F i n y i n, H 2 d t$	(14)
生产量	$p r o d u c t i v i t y H 2 = 60 R T s t a n ∫ 0 t a d F o u t y o u t, H 2 d t P s t a n t c y c l e$	(15)

Table 5 Process performance indicator

指标	数学模型
纯度	$p u r i t y H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F o u t d t$	(13)
回收率	$r e c o v e r y H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F i n y i n, H 2 d t$	(14)
生产量	$p r o d u c t i v i t y H 2 = 60 R T s t a n ∫ 0 t a d F o u t y o u t, H 2 d t P s t a n t c y c l e$	(15)

Table 6 Parameter of activate carbon and 5A zeolite adsorbent

物性参数	活性炭	5A分子筛
$ρ b$ /(kg·m^-3)	522.0	698.0
C_p_s/(kJ·kg^-1·K^-1)	1.047	0.92
r_p/m	0.00115	0.00157
$ε b$	0.433	0.357
$ε p$	0.61	0.65
$Ψ$	0.9	1.0
$k L D F, C H 4$ /s^-1	0.195	0.147
k_LDF_,_CO/s^-1	0.15	0.063
$k L D F, C O 2$ /s^-1	0.0355	0.0135
$k L D F, H 2$ /s^-1	0.7	0.7

Table 6 Parameter of activate carbon and 5A zeolite adsorbent

物性参数	活性炭	5A分子筛
$ρ b$ /(kg·m^-3)	522.0	698.0
C_p_s/(kJ·kg^-1·K^-1)	1.047	0.92
r_p/m	0.00115	0.00157
$ε b$	0.433	0.357
$ε p$	0.61	0.65
$Ψ$	0.9	1.0
$k L D F, C H 4$ /s^-1	0.195	0.147
k_LDF_,_CO/s^-1	0.15	0.063
$k L D F, C O 2$ /s^-1	0.0355	0.0135
$k L D F, H 2$ /s^-1	0.7	0.7

Table 7 Parameters of adsorption bed

参数	数值
H_b/m	1.0
W_t/m	0.002
D_b/m	0.2
$ρ w$ /(kg·m^-3)	7800
C_p_w/(kJ·kg^-1·K^-1)	0.5024
h_w/(W·m^-2·K^-1)	94.0
T_amb/K	298.15

Table 7 Parameters of adsorption bed

参数	数值
H_b/m	1.0
W_t/m	0.002
D_b/m	0.2
$ρ w$ /(kg·m^-3)	7800
C_p_w/(kJ·kg^-1·K^-1)	0.5024
h_w/(W·m^-2·K^-1)	94.0
T_amb/K	298.15

Fig.3 Adsorption isotherms of four components on 5A zeolite and activated carbon

Table 8 Extended Langmuir adsorption model fitting parameters

参数	活性炭				5A分子筛
参数	CH₄	CO	CO₂	H₂	CH₄	CO	CO₂	H₂
IP₁/(mol·kg^-1·bar^-1)	0.02386	0.03385	0.02880	0.01694	0.005833	0.01185	0.01003	0.004314
IP₂/K	5.62×10^-5	9.07×10^-5	7.00×10^-5	2.10×10^-5	1.19×10^-5	3.13×10^-5	1.86×10^-5	1.06×10^-5
IP₃/bar^-1	3.48×10^-3	2.31×10^-4	0.0100	6.25×10^-5	6.05×10^-4	0.02020	1.5781	0.002515
IP₄/K	1159	1751	1030	1229	1731	763.0	207.0	458.0
R	0.9998	0.9999	0.9998	1.0000	0.9917	0.9988	0.9919	0.9984
ΔH/(kJ·mol^-1)	-22.70	-22.58	-29.08	-12.84	-20.64	-29.77	-35.97	-9.23

Fig.4 Gas temperature distribution of RPSA and PSA

Fig.5 Pressure distribution of RPSA and PSA

Fig.6 Solid phase concentration profiles of CO, CO2, CH4 and H2

Fig.7 Effect of feed flow rate on RPSA performance

Fig.8 Effect of layer ratio of AC/5A zeolite on RPSA performance

Fig.9 Effect of purge-to-feed ratio on RPSA performance

Fig.10 Comparison of H2 yield and recovery of the two processes

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