Transient analysis of pressure swing adsorption hydrogen purification process

doi:10.11949/0438-1157.20211103

Abstract

Abstract:

Pressure swing adsorption (PSA) is one of the most common technologies to produce high-purity hydrogen in the industry. However, in the actual production process, the distribution state of each component in the bed at different time cannot be observed. For this reason, simulation methods are used to study the dynamic change of each component in the bed from the feeding to the system reaching the steady state, which is essential to guide process improvement. In this study, an eight-bed PSA process was designed to purify hydrogen from steam methane reforming (SMR) gas and the activated carbon and 5A zeolite were used as adsorbent. The start-up procedure of PSA hydrogen production was performed, and the transient adsorption behaviors of each component in the bed during the three stages of adsorption, sequential release and flushing, as well as the transient adsorption behavior during the adsorption stage and the temperature variation in the bed after the system reached the cyclic steady state were analyzed. The results show that the heavy components move towards the top of the bed with the cycle during the adsorption as well as the sequential release. This phenomenon is the result of both inter-component competition for adsorption and the accumulation of fractions at the bottom of the bed in the flush regeneration mode. These factors can also, to some extent, cause the adsorption front of CO to enter too much on the 5A zeolite during the adsorption phase, making the CO content become a major limiting factor for process performance.

Key words: pressure swing adsorption, activated carbon, 5A zeolite, hydrogen production, numerical simulation, transient analysis

摘要：

变压吸附技术是工业上生产高纯氢气最常用的方法之一。然而，在实际生产过程中无法观察到塔内各组分在不同时刻的分布状态，因此借助模拟的手段来研究从投料至系统达到循环稳态期间各组分在塔内的动态变化规律，进而指导工艺改进是很有必要的。采用活性炭和5A分子筛为吸附剂，设计了八塔变压吸附工艺从蒸汽甲烷重整气中纯化氢气，模拟了变压吸附制氢开车过程，分析了开车过程中塔内各组分在吸附、顺放以及冲洗三个阶段以及循环稳态后吸附阶段瞬态吸附行为和塔内温度变化。结果表明，在吸附以及顺放等过程中重组分会随着循环周期向塔顶移动。这一现象是组分间竞争吸附和冲洗再生方式下重组分在床层底部累积两个作用因素共同导致的。这些因素在一定程度上也会造成CO的吸附前沿在吸附阶段就过多进入5A分子筛上，使得CO含量成为限制工艺性能的主要因素。

关键词: 变压吸附, 活性炭, 5A分子筛, 制氢, 数值模拟, 瞬态分析

CLC Number:

TQ 028.1

Chao ZHANG, Jian CHEN, Wenhua YIN, Yuanhui SHEN, Zhaoyang NIU, Xiuxin YU, Donghui ZHANG, Zhongli TANG. Transient analysis of pressure swing adsorption hydrogen purification process[J]. CIESC Journal, 2022, 73(1): 308-321.

张超, 陈健, 殷文华, 沈圆辉, 钮朝阳, 余秀鑫, 张东辉, 唐忠利. 变压吸附氢气纯化过程瞬态分析[J]. 化工学报, 2022, 73(1): 308-321.

Figures/Tables 18

Fig.1 Configuration diagram of eight-bed PSA process

Fig.2 Process schematic diagram of PSA

Table 1 The schedule of eight-bed PSA

时间/s	塔1	塔2	塔3	塔4	塔5	塔6	塔7	塔8
40	AD1	ER1	ER3	RP1	BD	PP1	ED3	ED1
40	AD2	PR	ER2	ER4	RP2	PP2	ED4	ED2
40	ED1	AD1	ER1	ER3	RP1	BD	PP1	ED3
40	ED2	AD2	PR	ER2	ER4	RP2	PP2	ED4
40	ED3	ED1	AD1	ER1	ER3	RP1	BD	PP1
40	ED4	ED2	AD2	PR	ER2	ER4	RP2	PP2
40	PP1	ED3	ED1	AD1	ER1	ER3	RP1	BD
40	PP2	ED4	ED2	AD2	PR	ER2	ER4	RP2
40	BD	PP1	ED3	ED1	AD1	ER1	ER3	RP1
40	RP2	PP2	ED4	ED2	AD2	PR	ER2	ER4
40	RP1	BD	PP1	ED3	ED1	AD1	ER1	ER3
40	ER4	RP2	PP2	ED4	ED2	AD2	PR	ER2
40	ER3	RP1	BD	PP1	ED3	ED1	AD1	ER1
40	ER2	ER4	RP2	PP2	ED4	ED2	AD2	PR
40	ER1	ER3	RP1	BD	PP1	ED3	ED1	AD1
40	PR	ER2	ER4	RP2	PP2	ED4	ED2	AD2

Table 2 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)
	$k w ? 2 T w ? z 2 + C p w ρ w ? T w ? t - h w 4 D b (D b + W t) 2 - D b 2 (T g - T w) + h a m b 4 (D b + W t) 2 (D b + W t) 2 - D b 2 (T w - T a m b) = 0$	(6)
Ergun方程	$- ? P ? z = 150 μ (1 - ε b) 2 ε b 3 (2 r p ψ) 2 v g + 1.75 (1 - ε b) ρ g 2 r p ψ ε b 3 \| v g \| v g$	(7)
LDF方程	$? q i ? t = k L D F, i (q i * - q i)$	(8)
吸附等温式	$q i * = q m, i b i P i 1 + ∑ i = 1 n b i P i$ , $b i = b 0 e x p - Δ H i R g T$	(9)

Table 2 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)
	$k w ? 2 T w ? z 2 + C p w ρ w ? T w ? t - h w 4 D b (D b + W t) 2 - D b 2 (T g - T w) + h a m b 4 (D b + W t) 2 (D b + W t) 2 - D b 2 (T w - T a m b) = 0$	(6)
Ergun方程	$- ? P ? z = 150 μ (1 - ε b) 2 ε b 3 (2 r p ψ) 2 v g + 1.75 (1 - ε b) ρ g 2 r p ψ ε b 3 \| v g \| v g$	(7)
LDF方程	$? q i ? t = k L D F, i (q i * - q i)$	(8)
吸附等温式	$q i * = q m, i b i P i 1 + ∑ i = 1 n b i P i$ , $b i = b 0 e x p - Δ H i R g T$	(9)

Table 3 Process performance indicator

指标	数学模型
纯度	$p u r i t y H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F o u t d t$	(10)
回收率	recovery $H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F i n y i n, H 2 d t$	(11)
生产量	$p r o d u c t i v i t y H 2 = 60 R T s t a n ∫ 0 t a d F o u t y o u t, H 2 d t P s t a n t c y c l e$	(12)

Table 3 Process performance indicator

指标	数学模型
纯度	$p u r i t y H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F o u t d t$	(10)
回收率	recovery $H 2 = ∫ 0 t a d F o u t y o u t, H 2 d t ∫ 0 t a d F i n y i n, H 2 d t$	(11)
生产量	$p r o d u c t i v i t y H 2 = 60 R T s t a n ∫ 0 t a d F o u t y o u t, H 2 d t P s t a n t c y c l e$	(12)

Table 4 Parameters of activated 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_LDF,CH4/s^-1	0.195	0.147
k_LDF,CO/s^-1	0.15	0.063
k_LDF,CO2/s^-1	0.0355	0.0135
k_LDF,H2/s^-1	0.7	0.7
k_LDF,N2/s^-1	3.0	2.5

Table 4 Parameters of activated 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_LDF,CH4/s^-1	0.195	0.147
k_LDF,CO/s^-1	0.15	0.063
k_LDF,CO2/s^-1	0.0355	0.0135
k_LDF,H2/s^-1	0.7	0.7
k_LDF,N2/s^-1	3.0	2.5

Table 5 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_pw/(kJ·kg^-1·K^-1)	0.5024
h_w/(W·m^-2·K^-1)	94.0
T_amb/K	298.15

Table 5 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_pw/(kJ·kg^-1·K^-1)	0.5024
h_w/(W·m^-2·K^-1)	94.0
T_amb/K	298.15

Table 6 Extended Langmuir adsorption model fitting parameters

组分	T/K	活性炭				5A 分子筛
组分	T/K	q_m/(mmol·g^-1)	b₀/bar^-1	R	ΔH/(kJ·mol^-1)	q_m/(mmol·g^-1)	b₀/bar^-1	R	ΔH/(kJ·mol^-1)
H₂	298.15	3.85	5.48×10^-5	0.9996	-12.84	0.76	7.70×10^-4	0.9995	-9.23
	308.15	4.32	5.12×10^-5	0.9997		0.67	8.57×10^-4	0.9996
	318.15	2.21	1.06×10^-4	0.9994		0.65	8.47×10^-4	0.9997
CO	298.15	6.72	9.10×10^-6	0.9998	-22.58	2.24	6.14×10^-6	0.9991	-29.77
	308.15	6.22	9.13×10^-6	0.9998		2.20	6.58×10^-6	0.9993
	318.15	5.50	9.68×10^-6	0.9997		2.27	6.14×10^-6	0.9997
CO₂	298.15	7.96	2.52×10^-6	1.0000	-29.08	4.35	7.60×10^-6	0.9990	-35.97
	308.15	7.32	3.20×10^-6	0.9998		4.14	9.74×10^-6	0.9982
	318.15	6.59	4.17×10^-6	1.0000		3.96	9.12×10^-6	0.9956
CH₄	298.15	7.21	1.73×10^-5	0.9999	-22.70	3.73	5.91×10^-5	0.9996	-20.64
	308.15	6.75	1.98×10^-5	0.9998		3.54	5.37×10^-5	1.0000
	318.15	6.14	2.38×10^-5	0.9998		3.63	5.12×10^-5	1.0000
N₂	298.15	3.48	1.87×10^-4	1.0000	-15.99	2.75	3.98×10^-5	0.9999	-20.65
	308.15	3.38	1.94×10^-4	0.9997		2.67	4.16×10^-5	0.9997
	318.15	3.30	2.01×10^-4	0.9998		2.59	4.33×10^-5	1.0000

Table 7 Initial conditions of adsorption bed

Initial conditions

$y i z = 0,$ $y i n e r t z = 1,$ $q i z = 0,$ $q i n e r t z = q * i n e r t$ ,

$c i z = P y i R g T$ , $P z = P f e e d$ , $T g z = T s z = T w z = T f e e d$

Table 7 Initial conditions of adsorption bed

Initial conditions

$y i z = 0,$ $y i n e r t z = 1,$ $q i z = 0,$ $q i n e r t z = q * i n e r t$ ,

$c i z = P y i R g T$ , $P z = P f e e d$ , $T g z = T s z = T w z = T f e e d$

Table 8 The boundary conditions for each step of PSA process

Step	z=0	z=L
吸附 (AD1, AD2)
	$P z = 0 = P i n l e t$	$P z = L = P o u t l e t$
	$- ε b D a x, i ? c i ? z z = 0 = u z = 0 (c i z = 0 + - c i z = 0 -)$	$? c i ? z z = L = 0$
	$k g C v g ρ g ? T g ? z z = 0 = u z = 0 (T g z = 0 + - T g z = 0 -)$	$? T g ? z z = L = 0$
	$k s C p s ρ s ? T s ? z z = 0 = u z = 0 (T s z = 0 + - T s z = 0 -)$	$? T s ? z z = L = 0$
	$k w C p w ρ w ? T w ? z z = 0 = u z = 0 (T w z = 0 + - T w z = 0 -)$	$? T w ? z z = L = 0$
均压降 (ED1, ED2, ED3, ED4)
	$u z = 0 = 0$	$P z = L = P o u t l e t$
	$? c i ? z z = 0 = 0$	$? c i ? z z = L = 0$
	$? T g ? z z = 0 = 0$	$? T g ? z z = L = 0$
	$? T s ? z z = 0 = 0$	$? T s ? z z = L = 0$
	$? T w ? z z = 0 = 0$	$? T w ? z z = L = 0$
顺放 (PP1, PP2)
	$u z = 0 = 0$	$P z = L = P o u t l e t$
	$? c i ? z z = 0 = 0$	$? c i ? z z = L = 0$
	$? T g ? z z = 0 = 0$	$? T g ? z z = L = 0$
	$? T s ? z z = 0 = 0$	$? T s ? z z = L = 0$
	$? T w ? z z = 0 = 0$	$? T w ? z z = L = 0$

Table 8 The boundary conditions for each step of PSA process

Step	z=0	z=L
吸附 (AD1, AD2)
	$P z = 0 = P i n l e t$	$P z = L = P o u t l e t$
	$- ε b D a x, i ? c i ? z z = 0 = u z = 0 (c i z = 0 + - c i z = 0 -)$	$? c i ? z z = L = 0$
	$k g C v g ρ g ? T g ? z z = 0 = u z = 0 (T g z = 0 + - T g z = 0 -)$	$? T g ? z z = L = 0$
	$k s C p s ρ s ? T s ? z z = 0 = u z = 0 (T s z = 0 + - T s z = 0 -)$	$? T s ? z z = L = 0$
	$k w C p w ρ w ? T w ? z z = 0 = u z = 0 (T w z = 0 + - T w z = 0 -)$	$? T w ? z z = L = 0$
均压降 (ED1, ED2, ED3, ED4)
	$u z = 0 = 0$	$P z = L = P o u t l e t$
	$? c i ? z z = 0 = 0$	$? c i ? z z = L = 0$
	$? T g ? z z = 0 = 0$	$? T g ? z z = L = 0$
	$? T s ? z z = 0 = 0$	$? T s ? z z = L = 0$
	$? T w ? z z = 0 = 0$	$? T w ? z z = L = 0$
顺放 (PP1, PP2)
	$u z = 0 = 0$	$P z = L = P o u t l e t$
	$? c i ? z z = 0 = 0$	$? c i ? z z = L = 0$
	$? T g ? z z = 0 = 0$	$? T g ? z z = L = 0$
	$? T s ? z z = 0 = 0$	$? T s ? z z = L = 0$
	$? T w ? z z = 0 = 0$	$? T w ? z z = L = 0$

Fig.3 Effect of feed flow rate, layer ratio of AC/5A zeolite and purge-to-feed ratio on PSA performance

Fig.4 Dynamic profile of mole fraction of each component in the top of bed

Fig.5 Gas phase concentration profile of N2 at the end of adsorption

Fig.6 Gas phase concentration of H2, CO, CO2 and CH4 at the end of adsorption

Fig.7 Gas phase concentration profiles of H2, CO, CO2 and CH4 at the end of sequential release

Fig.8 Solid phase concentration profiles of H2, CO, CO2 and CH4 at the end of flushing

Fig.9 Gas phase concentration of H2, CO, CO2 and CH4 in the adsorption stage after cycling steady state

Fig.10 Temperature distribution, pressure profile within adsorption bed, and desorption gas distribution at the bottom of the bed at cycle steady state

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[3]	Congqi HUANG, Yimei WU, Jianye CHEN, Shuangquan SHAO. Simulation study of thermal management system of alkaline water electrolysis device for hydrogen production [J]. CIESC Journal, 2023, 74(S1): 320-328.
[4]	Zhanyu YE, He SHAN, Zhenyuan XU. Performance simulation of paper folding-like evaporator for solar evaporation systems [J]. CIESC Journal, 2023, 74(S1): 132-140.
[5]	Yifei ZHANG, Fangchen LIU, Shuangxing ZHANG, Wenjing DU. Performance analysis of printed circuit heat exchanger for supercritical carbon dioxide [J]. CIESC Journal, 2023, 74(S1): 183-190.
[6]	Zhiguo WANG, Meng XUE, Yushuang DONG, Tianzhen ZHANG, Xiaokai QIN, Qiang HAN. Numerical simulation and analysis of geothermal rock mass heat flow coupling based on fracture roughness characterization method [J]. CIESC Journal, 2023, 74(S1): 223-234.
[7]	Song HE, Qiaomai LIU, Guangshuo XIE, Simin WANG, Juan XIAO. Two-phase flow simulation and surrogate-assisted optimization of gas film drag reduction in high-concentration coal-water slurry pipeline [J]. CIESC Journal, 2023, 74(9): 3766-3774.
[8]	Longyi LYU, Wenbo JI, Muda HAN, Weiguang LI, Wenfang GAO, Xiaoyang LIU, Li SUN, Pengfei WANG, Zhijun REN, Guangming ZHANG. Enhanced anaerobic removal of halogenated organic pollutants by iron-based conductive materials: research progress and future perspectives [J]. CIESC Journal, 2023, 74(8): 3193-3202.
[9]	Lei XING, Chunyu MIAO, Minghu JIANG, Lixin ZHAO, Xinya LI. Optimal design and performance analysis of downhole micro gas-liquid hydrocyclone [J]. CIESC Journal, 2023, 74(8): 3394-3406.
[10]	Chen HAN, Youmin SITU, Bin ZHU, Jianliang XU, Xiaolei GUO, Haifeng LIU. Study of reaction and flow characteristics in multi-nozzle pulverized coal gasifier with co-processing of wastewater [J]. CIESC Journal, 2023, 74(8): 3266-3278.
[11]	Xiaosong CHENG, Yonggao YIN, Chunwen CHE. Performance comparison of different working pairs on a liquid desiccant dehumidification system with vacuum regeneration [J]. CIESC Journal, 2023, 74(8): 3494-3501.
[12]	Wenzhu LIU, Heming YUN, Baoxue WANG, Mingzhe HU, Chonglong ZHONG. Research on topology optimization of microchannel based on field synergy and entransy dissipation [J]. CIESC Journal, 2023, 74(8): 3329-3341.
[13]	Rui HONG, Baoqiang YUAN, Wenjing DU. Analysis on mechanism of heat transfer deterioration of supercritical carbon dioxide in vertical upward tube [J]. CIESC Journal, 2023, 74(8): 3309-3319.
[14]	Yuanhao QU, Wenyi DENG, Xiaodan XIE, Yaxin SU. Study on electro-osmotic dewatering of sludge assisted by activated carbon/graphite [J]. CIESC Journal, 2023, 74(7): 3038-3050.
[15]	Kexin HUANG, Tong LI, Anqi LI, Mei LIN. Mode decomposition of flow field in T-junction with rotating impeller [J]. CIESC Journal, 2023, 74(7): 2848-2857.