水合物法平衡级分离CO2/N2流程模拟分析

doi:10.16085/j.issn.1000-6613.2019-1887

化工进展 ›› 2020, Vol. 39 ›› Issue (9): 3600-3607.DOI: 10.16085/j.issn.1000-6613.2019-1887

水合物法平衡级分离CO₂/N₂流程模拟分析

樊栓狮¹^,³(), 周静仁¹^,², 李璐伶¹^,², 魏纳¹, 李海涛¹

^1.西南石油大学油气藏地质及开发工程国家重点实验室，四川成都 610500
^2.深圳市燃气集团股份有限公司，广东深圳 518040
^3.华南理工大学传热强化与过程节能教育部重点实验室，广东广州 510640

出版日期:2020-09-05 发布日期:2020-09-11
通讯作者: 樊栓狮
作者简介:樊栓狮（1965—），男，教授，博士生导师，主要从事天然气水合物研究工作。E-mail：ssfan@scut.edu.cn。
基金资助:
国家自然科学基金(21736005);国家重点研发计划(2016YFC0304008);博士后基金、博士后特别资助(2017M623060);广州能源所开放基金(Y807kn1001);油气藏地质及开发工程国家重点实验室（西南石油大学）开放基金(PLN201816);四川省科技厅应用基础研究基金(2019YJ0351)

Simulation and analysis of CO₂/N₂separation process by equilibrium stage hydrate-based gas separation method

Shuanshi FAN¹^,³(), Jingren ZHOU¹^,², Luling LI¹^,², Na WEI¹, Haitao LI¹

^1.State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, Sichuan, China
^2.Shenzhen Gas Corporation Ltd. , Shenzhen 518040, Guangdong, China
^3.Key Laboratory of Enhanced Heat Transfer and Energy Conversation, Ministry of Education, South China University of Technology, Guangzhou 510640, Guangdong, China

Online:2020-09-05 Published:2020-09-11
Contact: Shuanshi FAN

摘要/Abstract

摘要：

化石燃料燃烧排放烟气中CO₂的量占CO₂总排放量的75%，为了缓解CO₂导致的全球温室效应，需将CO₂/N₂中的CO₂分离出来。水合物法分离是一种高效、低能耗的CO₂/N₂分离技术。本文研究了水合物法平衡级分离CO₂/N₂过程中，进料CO₂体积分数、反应条件与反应特性三者间的关系，利用CPA-SRK方程+Chen-Guo模型对其进行平衡级分离流程模拟分析。经计算发现，进料干基CO₂体积分数对水合物法分离CO₂/N₂工艺的反应压力、平衡级级数均有较大影响。随着体积分数的增加，反应压力呈减小趋势，减小幅度随体积分数增加而减小，当进料CO₂体积分数小于20%时，压力下降较快，当体积分数大于50%时，压力降低幅度变小。温度为277K时，CO₂体积分数小于10%时，需四个水合物平衡级分离才能得到满足要求的气样；当体积分数为10%~20%时，需三个水合物平衡级分离；体积分数大于30%时为两个水合物平衡级分离。温度对水合分离的反应压力有较大影响，但对所需平衡级分离级数的影响并不大。随着温度的升高，水合反应压力呈增加趋势，增加幅度随进料干基CO₂体积分数的增加而降低。针对所研究气样，在不同温度下，均需三个水合物平衡级分离才能达到工艺要求。

关键词: 水合物法气体分离, 流程模拟分析, 分离级, 平衡级

Abstract:

The amount of CO₂ emitted from fossil fuel combustion emissions accounts for 75% of total CO₂ emissions. In order to alleviate the global greenhouse effect caused by CO₂, CO₂ in CO₂/N₂ must be separated. Hydrate-based gas separation is an efficient, low-energy consumption CO₂/N₂ separation technology. In this paper, the relationship between CO₂ volume fraction, reaction conditions and reaction characteristics in the process of CO₂/N₂ separation by hydrate-based gas separation is studied. The CPA-SRK equation and Chen-Guo model are used to process simulation and analysis. It is found by calculation that the CO₂ volume fraction of the feed dry base has a great influence on the reaction pressure and the equilibrium level of the CO₂/N₂ separation process by the hydrate-based gas separation. With the increase of CO₂ volume fraction, the reaction pressure decreases, and the decrease decreases with the increase of volume fraction. When the CO₂ volume fraction of feed is less than 20%, the decrease is faster. When the volume fraction is greater than 50%, the pressure decrease becomes smaller. When the temperature is 277K and the CO₂ volume fraction is less than 10%, the four hydrate equilibrium stages are needed to obtain the required gas sample. At the same temperature, when the CO₂ volume fraction is 10%—20%, the three hydrate equilibrium stages are needed, and when the CO₂ volume fraction is greater than 30%, the separation needs two hydrate equilibrium stages. Temperature has a great influence on the reaction pressure of hydration separation, but it has little effect on the number of separation stages required. As the temperature increases, the hydration reaction pressure increases, and the increase decreases with the increase of the feed dry CO₂ volume fraction. For the gas sample studied, three hydrate equilibrium stages are required at different temperatures to achieve the process requirements.

Key words: hydrate-based gas separation, process simulation and analysis, separation stages, equilibrium stage

中图分类号:

TE645

樊栓狮, 周静仁, 李璐伶, 魏纳, 李海涛. 水合物法平衡级分离CO₂/N₂流程模拟分析[J]. 化工进展, 2020, 39(9): 3600-3607.

Shuanshi FAN, Jingren ZHOU, Luling LI, Na WEI, Haitao LI. Simulation and analysis of CO₂/N₂separation process by equilibrium stage hydrate-based gas separation method[J]. Chemical Industry and Engineering Progress, 2020, 39(9): 3600-3607.

参考文献

1	BLOMEN E, HENDRIKS C, NEELE F. Capture technologies: Improvements and promising developments[J]. Energy Procedia, 2009, 1(1): 1505-1512.
2	ZHU L, HE Y D, LI L L, et al. Thermodynamic assessment of SNG and power polygeneration with the goal of zero CO₂ emission[J]. Energy, 2018, 149: 34-46.
3	ZHU L, HE Y D, LI L L, et al. Tech-economic assessment of second-generation CCS: chemical looping combustion[J]. Energy, 2018, 144: 915-927.
4	樊栓狮, 尤莎莉, 郎雪梅, 等. 笼型水合物膜分离和捕获二氧化碳研究进展[J]. 化工进展, 2020, 39(4): 1211-1218.
4	FAN S S, YOU S L, LANG X M, et al. Separation and capture carbon dioxide by clathrate-hydrate membranes: a review[J]. Chemical Industry and Engineering Progress, 2020, 39(4): 1211-1218.
5	SINGH D, CROISET E, DOUGLAS P L, et al. Techno-economic study of CO₂ capture from an existing coal-fired power plant: MEA scrubbing vs. O₂/CO₂ recycle combustion[J]. Energy Conversion & Management, 2003, 44(19): 3073-3091.
6	HO M T, ALLINSON G, DIANNE E, et al. Comparison of CO₂ separation options for geo-sequestration: are membranes competitive?[J]. Desalination, 2006, 192(1/2/3): 288-295.
7	田华, 孙瑞, 宋春风, 等. 耦合膜分离的新型CO₂低温捕集系统性能优化[J]. 化工进展, 2020, 39(7): 2844-2892.
7	TIAN H, SUN R, SONG C F, et al. Performance optimization of novel hybrid cryogenic CO₂ capture process with membrane separation[J]. Chemical Industry and Engineering Progress, 2020, 39(7): 2844-2892.
8	WANG Y, LANG X, FAN S S. Hydrate capture CO₂ from shifted synthesis gas, flue gas and sour natural gas or biogas[J]. Journal of Energy Chemistry, 2013, 22(1): 39-47.
9	ZHU L, LI L, ZHU J, et al. Analytical methods to calculate water content in natural gas[J]. Chemical Engineering Research and Design, 2015, 93: 148-162.
10	马庆兰, 雷雅慧, 陈光进. 非平衡级法气体混合物吸收-水合双塔分离单元的模拟计算[J]. 化工学报, 2015， 66(5): 1748-1759.
10	MA Q L, LEI Y H, CHEN G J. Simulation of absorption-hydration separation unit for gas mixture by non-equilibrium stage approach[J] CIESC Journal, 2015， 66(5): 1748-1759.
11	ADEYEMO A, KUMAR R, LINGA P, et al. Capture of carbon dioxide from flue or fuel gas mixtures by clathrate crystallization in a silica gel column[J]. International Journal of Greenhouse Gas Control, 2010, 4(3): 478-485.
12	MAHABADIAN M A, CHAPOY A, BURGASS R, et al. Development of a multiphase flash in presence of hydrates: experimental measurements and validation with the CPA equation of state[J]. Fluid Phase Equilibria, 2016, 414: 117-132.
13	KANG S P, LEE H. Recovery of CO₂ from flue gas using gas hydrate:? thermodynamic verification through phase equilibrium measurements[J]. Environmental Science & Technology, 2000, 34(20): 4397-4400.
14	LINGA P, ADEYEMO A, ENGLEZOS P. Medium-pressure clathrate hydrate/membrane hybrid process for postcombustion capture of carbon dioxide[J]. Environmental Science & Technology, 2008, 42(1): 315-320.
15	陈玉亮, 李玉星, 唐建峰, 等. 水合物法分离CO₂+N₂混合气实验与模拟计算[J]. 化工进展, 2010, 29
15	(S2): 66-73.
15	CHEN Y L, LI Y X, TANG J F, et al. Experimantal and simulation of separation from CO₂+N₂via forming hydrate[J].Chemical Industry and Engineering Progress, 2010, 29 (S2): 66-73.
16	ZHANG J, YEDLAPALLI P, LEE J W. Thermodynamic analysis of hydrate-based pre-combustion capture of[J]. Chemical Engineering Science, 2009, 64(22): 4732-4736.
17	HERSLUND P J, THOMSEN K, ABILDSKOV J, et al. Modelling of tetrahydrofuran promoted gas hydrate systems for carbon dioxide capture processes[J]. Fluid Phase Equilibria, 2014, 375: 45-65.
18	HERSLUND P J, THOMSEN K, ABILDSKOV J, et al. Modelling of cyclopentane promoted gas hydrate systems for carbon dioxide capture processes[J]. Fluid Phase Equilibria, 2014, 375: 89-103.
19	LINGA P, KUMAR R, ENGLEZOS P. The clathrate hydrate process for post and pre-combustion capture of carbon dioxide[J]. Journal of Hazardous Materials, 2007, 149(3): 625-629.
20	LI L, ZHU L, FAN J. The application of CPA-vdWP to the phase equilibrium modeling of methane-rich sour natural gas hydrates[J]. Fluid Phase Equilibria, 2016, 409: 291-300.
21	李璐伶. 基于水合物分离法捕集CO₂热力学模型及流程模拟研究[D]. 成都：西南石油大学, 2017.
21	LI L L. Study on thermodynamic model and the calculation of process for CO₂ capture by hydrate based gas separation[D]. Chengdu：Southwest Petroleum University, 2017.
22	李璐伶, 樊栓狮, 温永刚, 等. 水合物法分离CH₄/CO₂研究现状及展望[J]. 化工进展, 2018, 37(12): 4596-4605.
22	LI L L， FAN S S, WEN Y G,et al. Hydrate based gas separation technology for CH₄/CO₂ mixtures: a review[J].Chemical Industry and Engineering Progress, 2018, 37(12): 4596-4605.
23	OLIVEIRA M B, COUTINHO J A P, QUEIMADA A J. Mutual solubilities of hydrocarbons and water with the CPA EoS[J]. Fluid Phase Equilibria, 2007, 258 (1): 58-66.
24	MAHMOUDJANLOO H, IZADPANAH A A, OSFOURI S, et al. Modeling liquid-liquid and vapor-liquid equilibria for the hydrocarbon+N-formylmorpholine system using the CPA equation of state[J]. Chemical Engineering Science, 2013, 98: 152-159.
25	CHEN G J, GUO T M. Thermodynamic modeling of hydrate formation based on new concepts[J]. Fluid Phase Equilibria, 1996, 122(1/2): 43-65.
26	CHEN G J, GUO T M. A new approach to gas hydrate modelling[J]. Chemical Engineering Journal, 1998, 71(2): 145-151.
27	LI S, FAN S, WANG J, et al. CO₂ capture from binary mixture via forming hydrate with the help of tetra-n-butyl ammonium bromide[J]. Journal of Natural Gas Chemistry, 2009, 18(1): 15-20.
28	YANG W, LI S, LI X, et al. Analysis of a new liquefaction combined with desublimation system for CO₂ separation based on N₂/CO₂ phase equilibrium[J]. Energies, 2015, 8(9): 9495-9508.

[1]	齐永君，翁惠新. 催化精馏过程模拟稳态模型的研究进展 [J]. 化工进展, 2010, 29(4): 600-.
[2]	孔丁峰，柳建华，王瑾，张良，方志云，邬志敏. 单级氨吸收式制冷机精馏塔数值模拟与实验 [J]. 化工进展, 2010, 29(10): 1825-.

水合物法平衡级分离CO₂/N₂流程模拟分析

Simulation and analysis of CO₂/N₂separation process by equilibrium stage hydrate-based gas separation method

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 2

编辑推荐

Metrics

本文评价