结构化5A分子筛吸附床结构及工艺参数对N2/H2吸附性能的影响

doi:10.11949/0438-1157.20191349

摘要/Abstract

摘要：

利用吸附等温线获得动力学参数，建立了CFD模型，模拟了氢气/氮气在结构化5A分子筛吸附床中的吸附过程，研究了吸附剂层片间距、吸附剂厚度等结构参数和吸附压力、进气流量等工艺参数对混合气吸附效果的影响。结果表明：减小层片间距和吸附剂厚度可显著提高传质系数和床层利用率。增大吸附压力可提高床层利用率，但会减小传质系数。进气流量对传质系数的影响不明显，但当流量较大时，吸附容量和床层利用率均呈减小趋势。结构化5A分子筛吸附剂吸附性能良好。

关键词: 结构化5A分子筛, 吸附性能, 氢气提纯, 动力学模型

Abstract:

The kinetic parameters were obtained by adsorption isotherm, and the CFD model was established to simulate the adsorption process of hydrogen/nitrogen in the structured 5A molecular sieve adsorption bed. The effects of structural parameters such as the adsorbent sheet spacing and thickness and process parameters such as adsorption pressure and volume flow rate on the adsorption performance to the mixed gas were discussed. The results show that reducing sheet spacing and thickness are beneficial to the mass transfer coefficient and bed saturation degree. Increasing the adsorption pressure can improve the bed saturation degree, but will reduce the mass transfer coefficient. The effect of the flow rate on mass transfer coefficient is not obvious, but when the flow rate is high, both the adsorption capacity and the bed saturation degree decrease. The structured 5A molecular sieve adsorbent has good adsoption performance.

Key words: structured 5A molecular sieve, adsorption performance, hydrogen purification, kinetic modeling

中图分类号:

TQ 028.1

王鹏, 刘京雷, 张胜中, 范得权, 张英, 徐宏. 结构化5A分子筛吸附床结构及工艺参数对N₂/H₂吸附性能的影响[J]. 化工学报, 2020, 71(7): 3114-3122.

Peng WANG, Jinglei LIU, Shengzhong ZHANG, Dequan FAN, Ying ZHANG, Hong XU. Effect of structured 5A molecular sieve adsorption bed structure and process parameters on N₂/H₂ adsorption performance[J]. CIESC Journal, 2020, 71(7): 3114-3122.

图/表 15

表1 吸附床模型参数及初始值

Table 1 Adsorption bed model parameters and initial values

参数	数值
l/m	0.2
ρ/(kg·m^-3)	860
ε	0.4
T/K	298
$c N 2$ /%	25
$c H 2$ /%	75

表1 吸附床模型参数及初始值

Table 1 Adsorption bed model parameters and initial values

参数	数值
l/m	0.2
ρ/(kg·m^-3)	860
ε	0.4
T/K	298
$c N 2$ /%	25
$c H 2$ /%	75

图1 吸附剂结构对H2和N2穿透曲线的影响

Fig.1 Effect of different adsorbent structure on H2 and N2 breakthrough curve

表2 不同吸附剂结构下N2吸附量

Table 2 N2 adsorption capacity of different adsorbent structure

吸附剂

吸附压力/

MPa

穿透时间/

min

吸附量/

(mmol?g^-1)

表3 N2和H2在5A分子筛上的Langmuir拟合参数

Table 2 Fitting parameters of Langmuir model for N2 and H2 adsorption on 5A molecular sieve

参数	数值
$q m N 2$ /( mol·kg^-1)	2.265
$q m H 2$ /(mol·kg^-1)	1.155
$b N 2$ /MPa^-1	1.48
$b H 2$ /MPa^-1	0.117

表3 N2和H2在5A分子筛上的Langmuir拟合参数

Table 2 Fitting parameters of Langmuir model for N2 and H2 adsorption on 5A molecular sieve

参数	数值
$q m N 2$ /( mol·kg^-1)	2.265
$q m H 2$ /(mol·kg^-1)	1.155
$b N 2$ /MPa^-1	1.48
$b H 2$ /MPa^-1	0.117

图2 吸附剂性能评价系统1—减压阀；2—截止阀；3—三通阀；4—压力煲；5—背压阀；MFC—流量控制器

Fig2 Adsorbent performance evaluation system

图3 氮气实验和模拟穿透曲线的比较

Fig.3 Comparison of N2 experimental and simulation breakthrough curve

图4 不同层片间距下H2和N2穿透曲线的比较

Fig.4 Comparison of breakthrough curves of H2 and N2 with different laminate spacing

表4 层片间距对氮气传质系数和吸附剂容量的影响

Table 4 Effect of laminate spacing on mass transfer coefficient and adsorbent loading for nitrogen

层片间距/mm

传质系数/s^-1

穿透吸附量/

(mmol·g^-1)

饱和吸附量/

(mmol·g^-1)

图5 不同层片厚度下H2和N2穿透曲线的比较

Fig.5 Comparison of breakthrough curves of H2 and N2 with different laminate thickness

表5 层片厚度对氮气传质系数和吸附剂容量的影响

Table 5 Effect of laminate thickness on mass transfer coefficient and adsorbent loading for nitrogen

层片厚度/

传质系数/

s^-1

穿透吸附量/

(mmol·g^-1)

饱和吸附量/

(mmol·g^-1)

图6 不同吸附压力下H2和N2穿透曲线的比较

Fig.6 Comparison of breakthrough curves of H2 and N2 for different pressure

表6 吸附压力对氮气传质系数和吸附剂容量的影响

Table 6 Effect of adsorption pressure on mass transfer coefficient and adsorbent loading for nitrogen

吸附压力/

MPa

传质系数/

s^-1

穿透吸附量/

(mmol·g^-1)

图7 不同进气流量下H2和N2穿透曲线的比较

Fig.7 Comparison of breakthrough curves of H2 and N2 for different inlet flow

表7 进气流量对氮气传质系数和吸附容量的影响

Table 7 Effect of flow rate on mass transfer coefficient and adsorbent loading for nitrogen

进气流量/

(ml·min^-1)

表8 无效层长度和床层利用率

Table 8 Length of unused bed and bed saturation degree

吸附条件		床层利用率/%	无效层长度/cm
层片间距/mm(层片厚度0.8 mm)	0.2	51.1	9.78
	0.5	48.2	10.36
	0.8	45.7	10.86
层片厚度/mm(层片间距0.2 mm)	0.4	68.2	6.36
	0.6	61.8	7.64
	0.8	51.1	9.78
吸附压力/MPa(流量100 ml·min^-1)	0.2	46.3	10.74
	0.4	51.1	9.78
	0.8	57.5	8.51
进气流量/(ml·min^-1)（压力0.4 MPa）	60	60.1	7.98
	100	51.1	9.78
	140	45.2	10.96

参考文献 30

1	张士元, 谢鹏飞, 田振兴, 等. 膜分离技术在催化重整PSA尾气中氢气回收的应用[J]. 当代化工, 2019, 48(3): 643-646.
	Zhang S Y, Xie P F, Tian Z X, et al. Application of membrane separation technology in hydrogen recovery from catalytic reforming PSA tail gas[J]. Contemporary Chemical Industry, 2019, 48(3): 643-646.
2	方靓, 肖金生, 皮埃尔·贝纳德, 等. 氢气纯化变压吸附循环的热效应[J]. 工程热物理学报, 2018, 39(5): 168-175.
	Fang L, Xiao J S, Benard P, et al. Thermal effects on pressure swing adsorption cycles for hydrogen purification[J]. Journal of Engineering Thermophysics, 2018, 39(5): 168-175.
3	田进军, 王绪远, 杨学敏, 等. 从炼油厂含氢气体中回收氢气的研究[J]. 炼油技术与工程, 2016, 46(5): 6-9.
	Tian J J, Wang X Y, Yang X M, et al. Study on recovery of hydrogen from hydrogen containing gas in the refinery[J]. Petroleum Refinery Engineering, 2016, 46(5): 6-9.
4	曹伟波, 王丽军, 李希. 壁流蜂窝式微填充床制备及变压吸附中的应用[J]. 浙江大学学报（工学版）, 2017, 51(4): 777-783.
	Cao W B, Wang L J, Li X. Fabrication of wall-flow honeycomb micro packed bed and application in pressure swing adsorption process[J]. Journal of Zhejiang University (Engineering Science), 2017, 51(4): 777-783.
5	Ichiura H, Kubata Y, Wu Z H, et al. Preparation of zeolite sheet using a papermaking technique[J]. Journal of Materials Science, 2001, 36(4): 913-917.
6	Jose A D, Agueda V I, Uguina M A, et al. Adsorption and diffusion of H₂, CO, CH₄, and CO₂ in BPL activated carbon and 13X zeolite: evaluation of performance in pressure swing adsorption hydrogen purification by simulation[J]. Industrial & Engineering Chemistry Research, 2014, 53(40): 15414-15426.
7	郭海亮. 固态吸附剂的探究[J]. 中国石油和化工标准与质量, 2014, 34(6): 269.
	Guo H L. Research on solid adsorbent[J]. China Petroleum and Chemical Standard and Quality, 2014, 34(6): 269.
8	段雪, 陆军. 二维纳米复合氢氧化物: 结构、组装与功能[M]. 北京: 科学出版社, 2013: 28-35.
	Duan X, Lu J. Two-Dimensional Nanocomposite Hydroxides: Structure, Assembly and Function[M]. Beijing: Science Press, 2013: 28-35.
9	Moran A, Talu O. The role of pressure drop on rapid pressure swing adsorption performance[J]. Industrial & Engineering Chemistry Research, 2017, 56(19): 5715-5723.
10	Bowie G K, Denis J C. Pressure swing adsorption with axial or centrifugal compression machinery: US6488747B1[P]. 2002-11-03.
11	Arto O, Farid A, Antoni P T, et al. Laminated adsorbents with very rapid CO₂ uptake by freeze-casting of zeolites[J]. ACS Applied Materials & Interfaces, 2013, 5(7): 2669-76.
12	Rezaei F, Grahn M. Thermal management of structured adsorbents in CO₂ capture processes[J]. Industrial & Engineering Chemistry Research, 2016, 51(10): 4025-4034.
13	丁兆阳, 韩治洋, 石文荣, 等. 快速变压吸附制氧动态传质系数模拟分析[J]. 化工学报, 2018, 69(2): 759-768.
	Ding Z Y, Han Z Y, Shi W R, et al. Analysis of dynamic effective mass transfer coefficients of rapid pressure swing adsorption process for oxygen production[J]. CIESC Journal, 2018, 69(2): 759-768.
14	Rezaei F, Webley P. Optimum structured adsorbents for gas separation processes[J]. Chemical Engineering Science, 2009, 64(24): 5182-5191.
15	居沈贵, 刘晓勤, 马正飞, 等. 含CO体系在载铜吸附剂上吸附动态性能（2）: 数学模型化研究[J]. 南京化工大学学报, 2003, 22(2): 17-22.
	Ju S G, Liu X Q, Ma Z F, et al. Dynamic adsorption characteristics of mixtures containing CO on adsorbent loaded with cuprous salt (2): Mathematic model research[J]. Journal of Nanjing University of Chemical Technology, 2003, 22(2): 17-22.
16	康蕊, 厉彦忠, 杨宇杰, 等. 轴向导热对板翅式换热器传热性能的影响[J]. 西安交通大学学报, 2017, (2): 140-148.
	Kang R, Li Y Z, Yang Y J, et al. Performance evaluation of plate-fin heat exchanger considering effect of axial heat conduction[J]. Journal of Xi an Jiaotong University, 2017, (2): 140-148.
17	Chan K C, Chao C Y H, Wu C L. Measurement of properties and performance prediction of the new MWCNT-embedded zeolite 13X/CaCl₂ composite adsorbents[J]. International Journal of Heat and Mass Transfer, 2015, 89: 308-319.
18	朱红钧. FLUENT15.0流场分析实战指南[M]. 北京: 人民邮电出版社, 2015: 376-379.
	Zhu H J. FLUENT15.0 Flow Field Analysis Practical Guide[M]. Beijing: Post & Telecom Press, 2015: 376-379.
19	赵俊霞. 变压吸附空分制氧循环过程模拟研究[D]. 郑州: 郑州大学, 2016.
	Zhao J X. Simulation Research on Pressure Swing Adsorption Cycle of Air Separation for Oxygen[D]. Zhengzhou: Zhengzhou University, 2016.
20	刘学武, 李文秀, 郑国锋, 等. 13X沸石分子筛低温变压吸附CO₂/CH₄实验研究[J]. 天然气化工, 2017, (2): 5-8.
	Liu X W, Li W X, Zheng G F, et al. Low-temperature pressure swing adsorption of CO₂/CH₄ on zeolite 13X[J]. Natural Gas Chemical Industry, 2017, (2): 5-8.
21	Zheng X G, Liu Y S, Liu W H. Two-dimensional modeling of the transport phenomena in the adsorber during pressure swing adsorption process[J]. Industrial & Engineering Chemistry Research, 2010, 49(22): 11814-11824.
22	Cybulski A, Moulijn J A. Structured Catalysts and Reactors[M]. 2nd ed. CRC Press, 2006.
23	辜敏, 鲜学福. 煤层气变压吸附分离理论与技术[M]. 北京: 科学出版社, 2015.
	Gu M, Xian X F. The Theory and Technology of Pressure Swing Adsorption for Coal Bed Gas Separation[M]. Beijing: Science Press, 2015.
24	龙春霞, 丁琴, 关建郁. 吸附等温方程参数估算方法的分析[J]. 离子交换与吸附, 2012, 28(3): 211-220.
	Long C X, Ding Q, Guan J Y. Analysis of estimation method for adsorption isotherm parameters[J]. Ion Exchange and Adsorption, 2012, 28(3): 211-220.
25	柯斯乐 E L. 扩散流体系统中的传质[M]. 王宇新, 姜忠义, 译. 2版. 北京: 化学工业出版社, 2002: 67-68.
	Kosler E L. Diffusion Mass Transfer in Fluid Systems[M]. Wang Y X, Jiang Z Y, trans. 2nd ed. Beijing: Chemical Industrial Press, 2002: 67-68.
26	近藤精一, 石川达雄, 安部郁夫. 吸附科学[M]. 李国希, 译. 北京: 化学工业出版社, 2006: 107-108.
	Kondo S, Ishikawa T, Abe I. Adsorption Science[M]. Li G X, trans. Beijing: Chemical Industrial Press, 2006: 107-108.
27	蒋龙飞, 彭磊, 于萍, 等. 5A分子筛分离工业异己烷中低含量正己烷[J]. 能源化工, 2016, 37(3): 57-62.
	Jiang L F, Peng L, Yu P, et al. Separate small amounts of n-hexane from industrial isohexane on 5A molecular sieves[J]. Energy Chemical Industry, 2016, 37(3): 57-62.
28	Helfferich F G. Principles of adsorption & adsorption processes[J]. AIChE Journal, 1985, 31(3): 523-524.
29	刘京雷, 王浩, 张胜中, 等.泡沫镍负载5A分子筛结构化吸附材料的制备及性能[J].环境工程学报, 2020, 14(1): 165-172.
	Liu J L, Wang H, Zhang S Z, et al. Preparation and properties of structured adsorbent materials with foam nickel loaded with 5A molecular sieve[J]. Chinese Journal of Environmental Engineering, 2020, 14(1): 165-172.
30	Rezaei F, Webley P. Structured adsorbents in gas separation processes[J]. Separation and Purification Technology, 2010, 3(27): 243-256.

[1]	金正浩, 封立杰, 李舒宏. 氨水溶液交叉型再吸收式热泵的能量及分析[J]. 化工学报, 2023, 74(S1): 53-63.
[2]	李锦潼, 邱顺, 孙文寿. 煤浆法烟气脱硫中草酸和紫外线强化煤砷浸出过程[J]. 化工学报, 2023, 74(8): 3522-3532.
[3]	李艳辉, 丁邵明, 白周央, 张一楠, 于智红, 邢利梅, 高鹏飞, 王永贞. 非常规服役超临界锅炉的微纳尺度腐蚀动力学模型建立及应用[J]. 化工学报, 2023, 74(6): 2436-2446.
[4]	王承泽, 顾凯丽, 张晋华, 石建轩, 刘艺娓, 李锦祥. 硫化协同老化零价铁增效去除水中Cr（Ⅵ）的作用机制[J]. 化工学报, 2023, 74(5): 2197-2206.
[5]	郑杰元, 张先伟, 万金涛, 范宏. 丁香酚环氧有机硅树脂的制备及其固化动力学研究[J]. 化工学报, 2023, 74(2): 924-932.
[6]	周桓, 张梦丽, 郝晴, 吴思, 李杰, 徐存兵. 硫酸镁型光卤石转化钾盐镁矾的过程机制与动态规律[J]. 化工学报, 2022, 73(9): 3841-3850.
[7]	马语峻, 刘向军. 多孔陶瓷膜烟气水分回收理论与模型研究[J]. 化工学报, 2022, 73(9): 4103-4112.
[8]	霍猛, 彭晓婉, 赵金, 马秋伟, 邓春, 刘蓓, 陈光进. 基于COSMO-RS的离子液体吸收CO的溶剂筛选及H₂/CO分离实验[J]. 化工学报, 2022, 73(12): 5305-5313.
[9]	宋谦石, 王潇伟, 张威, 汪小憨, 李浩文, 乔瑜. 无机元素对生物质焦炭-CO₂气化反应性的催化/抑制作用研究及模型构建[J]. 化工学报, 2022, 73(11): 5240-5250.
[10]	张牧星, 张小松, 丁烨, 宋翼. 氧化石墨烯膜间距对电渗析空气除湿特性影响的分子动力学研究[J]. 化工学报, 2021, 72(S1): 63-69.
[11]	张梦飞, 张玲, 李晓闯, 祖韵秋, 黄明, 石宪章, 刘春太. 厚壁橡胶制品非等温硫化过程模拟与实验研究[J]. 化工学报, 2021, 72(4): 2065-2075.
[12]	李梦钖, 高明, 左启蓉, 章立新, 赵玉刚. 过冷壁面液滴中四丁基溴化铵水合物生成的可视化研究[J]. 化工学报, 2021, 72(4): 2094-2101.
[13]	李超凡, 温玉娟, 曹楠, 孙东, 宋晓明, 杨悦锁. 耐低温对硝基苯酚降解菌的降解动力学研究[J]. 化工学报, 2021, 72(3): 1692-1701.
[14]	杨诗, 蔡阳, 李长平, 李雪辉. 磷钨酸负载锆基金属有机骨架PTA@MOF-808的制备及其吸附脱硫性能[J]. 化工学报, 2021, 72(3): 1722-1731.
[15]	毛桃嫣, 邹敏婷, 郑成, 曾昭文, 伍旭贤, 肖润辉, 彭思玉. 微波化学反应的无量纲准数动力学模型研究：以偶氮二异丁脒盐酸盐（AIBA）分解反应为例[J]. 化工学报, 2021, 72(3): 1364-1371.

结构化5A分子筛吸附床结构及工艺参数对N₂/H₂吸附性能的影响

Effect of structured 5A molecular sieve adsorption bed structure and process parameters on N₂/H₂ adsorption performance

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 15

参考文献 30

相关文章 15

编辑推荐

Metrics

本文评价