Intensification of low-grade methane enrichment in nitrogen mixture by CH<sub>4</sub>/CO<sub>2</sub> displacement

QU Donglei; YANG Ying; QIAN Zhiling; LI Ping; YU Jianguo

doi:10.11949/0438-1157.20200416

您当前的位置：

首页 >

文章列表页 >

Intensification of low-grade methane enrichment in nitrogen mixture by CH₄/CO₂ displacement

Separation engineering | 更新时间：2026-07-24

- Intensification of low-grade methane enrichment in nitrogen mixture by CH₄/CO₂ displacement
- CIESC Journal Vol. 71, Issue 12, Pages: 5599-5609(2020)
- 作者机构：
  
  华东理工大学化工学院，化学工程联合国家重点实验室，上海 200237
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20200416
  CLC： TQ 028.1
- Received：21 April 2020，
  
  Revised：2020-06-08，
  
  Online First：17 December 2020，
  
  Published：05 December 2020
- 稿件说明：
移动端阅览
曲冬蕾, 杨颖, 钱智玲, 李平, 于建国. CH₄/CO₂混合气置换强化含氮低品质甲烷的浓缩[J]. 化工学报, 2020, 71(12): 5599-5609 DOI: 10.11949/0438-1157.20200416.

QU Donglei, YANG Ying, QIAN Zhiling, LI Ping, YU Jianguo. Intensification of low-grade methane enrichment in nitrogen mixture by CH₄/CO₂ displacement[J]. CIESC Journal, 2020, 71(12): 5599-5609 DOI: 10.11949/0438-1157.20200416.
曲冬蕾, 杨颖, 钱智玲, 李平, 于建国. CH₄/CO₂混合气置换强化含氮低品质甲烷的浓缩[J]. 化工学报, 2020, 71(12): 5599-5609 DOI: 10.11949/0438-1157.20200416. DOI：

QU Donglei, YANG Ying, QIAN Zhiling, LI Ping, YU Jianguo. Intensification of low-grade methane enrichment in nitrogen mixture by CH₄/CO₂ displacement[J]. CIESC Journal, 2020, 71(12): 5599-5609 DOI: 10.11949/0438-1157.20200416. DOI：

摘要

针对CO

置换吸附分离CH

过程中CO

再生困难的问题，采用少量产品气CH

真空吹扫以提高CO

的解吸效果，并以解吸得到的CH

/CO

混合气为置换步骤的置换气，通过置换来强化含氮低品质甲烷的浓缩过程。以自制椰壳活性炭为吸附剂，对CH

/CO

混合气置换强化吸附回收含氮低品质甲烷工艺过程进行了实验与模拟研究。在gPROMS软件中建立并求解固定床吸附分离模型方程，预测了CH

、N

和CO

在自制椰壳活性炭上的竞争吸附穿透曲线，通过预测结果和实验的对比，验证了数学模型方程的准确性。对比了不同置换气强化吸附分离低品质甲烷的效果，结果表明CH

/CO

混合气置换强化相对于CO

置换强化可获得更高纯度产品。进行了CH

/CO

混合气置换强化真空变压吸附循环实验，可以将14%的CH

和53%的CH

/CO

联合富集到98.8%，同时获得77.8%的回收率。

Abstract

To solve the problem of CO

uncompleted desorption in the process of CO

displacemen

t enhancing the adsorption separation of CH

a small amount of product gas CH

was used as purge gas to improve the CO

desorption. CH

/CO

mixture gas obtained from desorption step was recycled as the displacement gas to enhance the enrichment of low-grade methane in nitrogen mixture. In this work

the research conducted the experiments for CH

separation using CH

/CO

displacement intensification adsorption and the laboratory-made coconut shell activated carbon as sorbent. The mathematical models were built in gPROMS and the accuracy of models was verified by comparison of simulations and CH

/CO

breakthrough experiments. The performance of enrichment of low-grade methane with displacement intensification using different displacer was compared. The result showed that the process with CH

/CO

displacement had higher purity product than CO

displacement. The CH

/ CO

mixed gas replacement enhanced vacuum pressure swing adsorption cycle experiment was carried out

which can jointly enrich 14% CH

/ N

and 53% CH

/CO

to 98.8%

and at the same time obtain a recovery rate of 77.8%.

关键词

Keywords

references

政府间气候变化专门委员会. 气候变化2014: 综合报告[R].日内瓦, 2013.

Intergovernmental Panel on Climate Change. Synthesis Report: Climate Change 2014[R]. Geneva, 2013.

Effendy S, Xu C, Farooq S. Optimization of a pressure swing adsorption process for nitrogen rejection from natural gas[J ] . Industrial & Engineering Chemistry Research, 2017, 56 : 5417-5431.

Yousef A M, El-Maghlany W M, Eldrainy Y A, et al. Upgrading biogas to biomethane and liquid CO2: a novel cryogenic process[J ] . Fuel, 2019, 251 : 611-628.

高婷, 林文胜, 顾安忠, 等. 利用吸附余压预冷的煤层气氮膨胀液化流程[J ] . 天然气工业, 2009, 29 (2): 117-147.

Gao T, Lin W S, Gu A Z, et al. Integrated process of nitrogen expansion and liquefaction for precooling CBM by adsorbing residue pressure[J ] . Natural Gas Industry, 2009, 29 (2): 117-147.

李雯, 王志, 李潘源, 等. 用于甲烷-氮气体系分离的膜技术研究进展[J ] . 化工学报, 2016, 67 (2): 404-415.

Li W, Wang Z, Li P Y, et al. Progress in membrane technology for CH4-N2 separation[J ] . CIESC Journal, 2016, 67 (2): 404-415.

Wu T, Diaz M C, Zheng Y, et al. Influence of propane on CO2/CH4 and N2/CH4 separations in CHA zeolite membranes[J ] . Journal of Membrane Science, 2015, 473 : 201-209.

Zong Z, Carreon M A. Thin SAPO-34 membranes synthesized in stainless steel autoclaves for N2/CH4 separation[J ] . Journal of Membrane Science, 2017, 524 : 117-123.

Wang S, Guo Q, Liang S, et al. Preparation of Ni-MOF-74/SBS mixed matrix membranes and its application of CH4/N2 separation[J ] . Separation and Purification Technology, 2018, 199 : 206-213.

Zhang Y Y , Xie Y J, Zhu Y, et al. Energy consumption analysis for CO2 separation from gas mixtures with liquid absorbents[J ] . Energy Procedia, 2014, 61 : 2695-2698.

Matsui H, Jia J, Tsuji T, et al. Microsecond simulation study on the replacement of methane in methane hydrate by carbon dioxide, nitrogen, and carbon dioxide-nitrogen mixtures[J ] . Fuel, 2020, 263 : 116640.

Yang X, Li Z, Zhang C Z , et al. Practical separation performance evaluation of coal mine methane upgrading with carbon molecular sieves[J ] . Chemical Engineering Journal, 2019, 367 : 295-303.

Yang H W , Yin C B, Jiang B, et al. Optimization and analysis of a VPSA process for N2/CH4 separation[J ] . Separation and Purification Technology, 2014, 134 : 232-240.

Yin C, Sun W, Yang H W, et al. Optimization of three-bed VPSA system for biogas upgrading[J ] . Chemical Engineering Science, 2015, 135 : 100-108.

刘海庆, 吴一江, 杨颖, 等. 沸石ZSM-5吸附回收低浓度煤层气中CH4[J ] . 化工学报, 2016, 67 (5): 1931-1941.

Liu H Q, Wu Y J, Yang Y, et al. Adsorption and recovery of low concentration coal-bed methane by zeolite ZSM-5[J ] . CIESC Jo urnal, 2016, 67 (5): 1931-1941.

Gu M, Zhang B, Qi Z D , et al. Effects of pore structure of granular activated carbons on CH4 enrichment from CH4/N2 by vacuum pressure swing adsorption[J ] . Separation and Purification Technology, 2015, 146 : 213-218.

Guo Y, Hu J L, Liu X W, et al. Scalable solvent-free preparation of [Ni3(HCOO)6 ] frameworks for highly efficient separation of CH4 from N2[J ] . Chemical Engineering Journal, 2017, 327 : 564-572.

Tang R L, Dai Q B, Liang W W, et al. Synthesis of novel particle rice-based carbon materials and its excellent CH4/N2 adsorption selectivity for methane enrichment from low-rank natural gas[J ] . Chemical Engineering Journal, 2020, 384 : 123388.

Xiao G, Saleman T L, Zou Y, et al. Nitrogen rejection from methane using dual-reflux pressure swing adsorption with a kinetically-selective adsorbent[J ] . Chemical Engineering Journal, 2019, 372 : 1038-1046.

杨颖, 曲冬蕾, 李平, 等. 低浓度煤层气吸附浓缩技术研究与发展[J ] . 化工学报, 2018, 69 (11): 4518-4529.

Yang Y, Qu D L, Li P, et al. Research and development on enrichment of low concentration coal mine methane by adsorption technology[J ] . CIESC Journal, 2018, 69 (11): 4518-4529.

Yang J F, Bai H H, Shang H, et al. Experimental and simulation study on efficient CH4/N2 separation by pressure swing adsorption on silicalite-1 pellets[J ] . Chemical Engineering Journal, 2020, 388 : 124222.

Saleman T L, Li G, Ruffor T E, et al. Capture of low grade methane from nitrogen gas using dual-reflux pressure swing adsorption[J ] . Chemical Engineering Journal, 2015, 281 : 739-748.

韩治洋, 丁兆阳, 韩旸湲, 等. 真空变压吸附分离氮气甲烷的模拟与控制[J ] . 化工学报, 2018, 69 (2): 750-758.

Han Z Y, Ding Z Y, Han Y Y, et al. Simulation and control of vacuum pressure swing adsorption for N2/CH4 separation[J ] . CIESC Journal, 2018, 69 (2): 750-758.

Sun W N, Shen Y H, Zhang D H, et al. A systematic simulation and proposed optimization of the pressure swing adsorption process for N2/CH4 separation under external disturbances[J ] . Industrial & Engineering Chemistry Research, 2015, 54 (30): 7489-7501.

Han Z Y, Xing R, Zhang D H, et al. Vacuum pressure swing adsorption system for N2/CH4 separation under uncertainty[J ] . Chemical Engineering Research and Design, 2019, 142 : 245-256.

Yang X, Liu Y S, Li Z Y, et al. Vacuum exhaust process in pilot-scale vacuum pressure swing adsorption for coal mine ventilation air methane enrichment[J ] . Energies, 2018, 11 : 1030.

Liu C M, Zhou Y P, Sun Y, et al. Enrichment of coal-bed methane by PSA complemented with CO2 displacement[J ] . AIChE J., 2011, 57 (3): 645-654.

Yang Y, Wu Y J, Liu H Q, et al. Enrichment of ventilation air methane by adsorption with displacement chromatography technology: experiment and numerical simulation[J ] . Chemical Engineering Science, 2016, 149 : 215-228.

Qu D L, Yang Y, Qian Z L, et al. Enrichment of low-grade methane gas from nitrogen mixture by VPSA with CO2 displacement process: modeling and experiment[J ] . Chemical Engineering Journal, 2020, 380 : 122509.

Qu D L, Yang Y, Lu K, et al. Microstructure effect of carbon materials on the low-concentration methane adsorption separation from its mixture with nitrogen[J ] . Adsorption, 2018, 24 (4): 357-369.

Farooq S, Ruthven D M, Boniface H A. Numerical simulation of a pressure swing adsorption oxygen unit[J ] . Chemical Engineering Science, 1989, 44 (12): 2809-2816.

Glueckauf E, Coates J I. Theory of chromatography(Ⅳ): The influence of incomplete equilibrium on the front boundary of chromatograms and on the effectiveness of separation[J]. Journal of the Chemical Society (Resumed), 1947: 1315-1321.

Sips R. On the Structure of a catalyst surface [J ] . Journal of Chemiacal Physics, 1948, 16 : 490-495.

Edwards M F, Richardson J F. Gas dispersion in packed beds[J ] . Chemical Engineering Science, 1968, 23 (2): 109-123.

Do D D. Adsorption Analysis: Equilibria and Kinetics [M]. London: Imperial College Press, 1998.

Views

下载量

CSCD

Alert me when the article has been cited

提交

Tools

Publicity Resources

Biogas upgrading by vacuum pressure swing adsorption process

Influence mechanism of free guest molecules in liquid phase on decomposition kinetics of CO₂-CH₄ hydrates

Research on integrated process of cryogenic CO2 removal under supercritical pressure and liquefaction for biogas

Effect of Ba content on chemical looping dry reforming of methane performance of (La0.5Sr0.5)1-xBaxFe0.6Co0.4O3

Modeling and simulation of CH4/N2 separation process with two absorption-adsorption columns using ZIF-8 slurry

Related Author

TIAN Caixia

SHEN Yuanhui

ZHANG Donghui

GAN Hainan

SONG Shangfei

LI Yunchao

WU Wenyu

ZHU Yumo

Related Institution

State Key Laboratory of Chemical Engineering, School of Chemical Engineering and Technology, Tianjin University

Shifang Environment Protection & Bio-technology

National Engineering Research Center for Safe Oil & Gas Pipeline Transportation, Beijing Key Laboratory of Urban Gas Distribution Technology, Key Laboratory of Petroleum Engineering of the Ministry of Education, College of Mechanical and Storage & Transportation Engineering, China University of Petroleum

Tianfu Yongxing Laboratory, Research Center for New Principles and Technology of Carbon Capture

Sinopec Engineering Incorporation

⁰

Intensification of low-grade methane enrichment in nitrogen mixture by CH4/CO2 displacement

DOI：10.11949/0438-1157.20200416

摘要

Abstract

关键词

Keywords

references

Intensification of low-grade methane enrichment in nitrogen mixture by CH₄/CO₂ displacement