CO2 混合物热物性在CCS研究中的作用：实验数据、理论模型和典型应用

doi:10.16085/j.issn.1000-6613.2018-0248

化工进展 ›› 2019, Vol. 38 ›› Issue (03): 1244-1258.DOI: 10.16085/j.issn.1000-6613.2018-0248

CO₂ 混合物热物性在CCS研究中的作用：实验数据、理论模型和典型应用

王珺瑶^1,²(),张月¹,邓帅¹,赵军¹(),孙太尉¹,李恺翔¹,徐耀锋¹

1. 天津大学中低温热能高效利用教育部重点实验室，天津 300350
2. 天津大学环境科学与工程学院，天津 300350

收稿日期:2018-01-28 修回日期:2018-12-07 出版日期:2019-03-05 发布日期:2019-03-05
通讯作者: 赵军
作者简介:<named-content content-type="corresp-name">王珺瑶</named-content>（1990—），女，博士研究生，研究方向为化学吸收法碳捕集。E-mail:<email>wangjunyao_hkust@126.com</email>。|赵军，教授，主要从事碳捕集和中低温热能高效利用研究。E-mail: <email>zhaojun@tju.edu.cn</email>。
基金资助:
国家自然科学基金面上项目(51876134)

Role of thermodynamic properties of CO₂ mixtures in CCS: data, models and typical applications

Junyao WANG^1,²(),Yue ZHANG¹,Shuai DENG¹,Jun ZHAO¹(),Taiwei SUN¹,Kaixiang LI¹,Yaofeng XU¹

1. Key Laboratory of Efficient Utilization of Low and Medium Grade Energy, Tianjin University, Tianjin 300350, China
2. School of Environmental Science and Engineering, Tianjin University, Tianjin 300350, China

Received:2018-01-28 Revised:2018-12-07 Online:2019-03-05 Published:2019-03-05
Contact: Jun ZHAO

摘要/Abstract

摘要：

二氧化碳捕集与封存（CCS）各工艺过程的设计、运行都依赖于对CO₂及其混合物热物理性质的深入理解。同时，CCS的规模化发展和商业化进程，对CO₂混合物及其热物性的准确性提出了更高的要求。本文从实验数据、理论模型和典型应用3个方面综述了CO₂及其混合物热物性的发展现状，并尝试对发展趋势进行归纳。在实验研究方面，CO₂混合体系的研究进展视组分不同，差异较大，其中CO₂-N₂、CO₂-CH₄、CO₂-H₂O和CO₂-H₂二元体系已形成较完善的物性数据库，而CO₂-NH₃、CO₂-NO _x 和CO₂-CO体系的物性数据还比较欠缺；在物性估算方面，面向CCS的物性估算模型研究自2008年开始活跃，基于不同理论构架，目前已逐步形成面向CCS的多元化的物性估算体系。物性研究在CCS中的应用主要体现在物性是支撑CCS过程研究的基础，其不准确性在过程模拟或计算中会被“放大”，从而影响过程评估的准确性，本文从物性在循环构建和能效分析中的作用以及CO₂水合物的形成3个方面入手做了说明。文章最后对面向CCS的物性研究趋势进行了梳理，对分子模拟技术、通用性强的物性估算模型和物性在过程设计和循环分析中的角色进行了展望。

关键词: 二氧化碳, 混合物, 热力学性质, 碳捕集与封存, 状态方程

Abstract:

Thermodynamic properties of CO₂ mixtures play a critical role in the whole chains of carbon capture and storage (CCS) process. In recent years, the rapid development of CCS technology and its scale-up and commercial applications issue new challenges to the research of CO₂ mixtures. In this paper, a literature review survey was conducted to identify the knowledge gap and the research progress of thermodynamic properties in terms of available experiment data, theoretical models and typical applications. In experimental aspect, there was great difference in the available data for different CO₂ mixture systems. In particular, there were many available experimental data for the CO₂-N₂, CO₂-CH₄, CO₂-H₂O and CO₂-H₂ mixture systems while few data were available for CO₂-NH₃, CO₂-NO _x and CO₂-CO systems. The study about the equations of states (EOS) became active since the year of around 2008. Based on different theory frameworks, many EOSs were further developed focusing on the application for CCS. In application aspect, the impact of thermodynamic properties on typical CCS process, thermodynamic cycle analysis as well as formation of CO₂ hydrates were further reviewed and summarized. Finally, it was attempted to summarize several potential research directions of thermodynamic properties in CCS including development of property estimation methods with both EOS and molecular simulation as well as the roles of thermodynamic properties in process and thermodynamic cycle analysis.

Key words: carbon dioxide, mixtures, thermodynamic properties, carbon capture and storage (CCS), equation of state (EOS)

中图分类号:

TK 123

王珺瑶, 张月, 邓帅, 赵军, 孙太尉, 李恺翔, 徐耀锋. CO₂ 混合物热物性在CCS研究中的作用：实验数据、理论模型和典型应用[J]. 化工进展, 2019, 38(03): 1244-1258.

Junyao WANG, Yue ZHANG, Shuai DENG, Jun ZHAO, Taiwei SUN, Kaixiang LI, Yaofeng XU. Role of thermodynamic properties of CO₂ mixtures in CCS: data, models and typical applications[J]. Chemical Industry and Engineering Progress, 2019, 38(03): 1244-1258.

图/表 11

表1 涉及CO2物性研究的代表性项目总结

项目名称	国别/地区	研究对象	研究过程	研究方法	来源
CO₂ QUEST	国际合作（英国、瑞典、法国、中国、比利时、希腊、加拿大、以色列）	CO₂混合物	CO₂运输和封存过程	物理模型和实验研究	[4]
CO₂ Interface-Transport-Interface-Storage (CO₂ IT IS)	挪威	CO₂混合物	CO₂运输和封存过程	物理模型和实验研究	[5]
CO₂ Dynamic	挪威	CO₂混合物	CO₂运输和封存过程	物理模型	[6]
CO₂ MIX Project	挪威/德国	CO₂混合物	CO₂压缩液化和运输过程	物理模型和实验研究	[7]
The Impact Project	国际合作（挪威、英国、荷兰、中国等）	CO₂混合物	CO₂运输和封存过程	物理模型和实验研究	[8]
Gas Annexes Project	法国	CO₂混合物	CO₂封存过程	物理模型和实验研究	[9]

图1 典型CCS过程的温度压力范围

表2 捕集后的CO2混合气成分[19,21]

气体种类	摩尔分数最小值/%	摩尔分数最大值/%
CO₂	75	99
N₂	0.02	10
H₂O	0.005	6.5
O₂	0.04	5
H₂	0.06	4
CH₄	0.7	4
Ar	0.005	3.5
NH₃	<10^?3	3
SO₂	<10^?3	1.5
H₂S/COS	0.01	1.5
NO _x	<0.002	0.3
CO	<10^?3	0.2
胺	<10^?3	0.01

表3 CO2混合物pVTxy实验数据

混合物	文献数量	相关文献	数据范围			研究现状
混合物	文献数量	相关文献	温度/K	压力/MPa	X(CO₂)	CCS相关文献	实验数据点
注: √表示实验数据点较多，已开展基于CCS过程的实验； △表示实验数据点有局限性，已开展基于CCS过程的实验； ?表示实验数据点较少，且实验数据年份较早。
CO₂-N₂	31	[18,21,26,33,34,35]	208～303	0.6～21.4	0.15～0.999	[27,33,34,35]	√
CO₂-O₂	13	[18,21,26,33,34,35]	218～298	0.9～20	0.15～0.99	[33,34,35,36]	△
CO₂-H₂	8	[18,21]	218～303	0.9～172	0.07～0.999	[27]	√
CO₂-CH₄	19	[18,21,34]	152～320	0.6～48	0.026～0.99	[34]	√
CO₂-Ar	6	[18,21,26,33,34,35]	223～299	1.5～20	0.24～0.99	[33,34,35]	△
CO₂-NH₃	2	[18]	413～513	4.3～81.7	0.023～0.33	—	?
CO₂-SO₂	4	[18,21,30,32]	273～418	1.1～29	0.03～0.98	[30,32]	?
CO₂-H₂S	8	[18,21,31]	248～365	0.3～41	0.01～0.97	[31]	?
CO₂-N₂O	1	[18]	293～307	5.3～7.2	0.28～0.88	—	?
CO₂-NO/N₂O₄	2	[18,21]	262～328	0.17～9.0	0.005～0.88	—	?
CO₂-CO	5	[18,21,26,37]	223～343	0.1～20	0.20～0.996	[37]	?
CO₂-H₂O	>50	[38]	251～623	0.1～350	0.08～1	[38]	√
CO₂-N₂-O₂	3	[18,39]	218～273	5.1～13	0.15～0.96	—	?
CO₂-N₂-H₂	1	[21]	253～302	2.1～8.7	0.93～0.95	[27]	△
CO₂-N₂-Ar	1	[28]	268～303	3.52～7.66	0.90～0.98	[28]	△
CO₂-N₂-CH₄	6	[18,40,41]	220～293	6～11	0.27～0.99	—	?
CO₂-Ar-H₂	1	[28]	268～301	3.26～8.91	0.90～0.98	[28]	△
CO₂-CO-H₂	3	[18,42,43]	233～303	4～20	0.17～0.99	—	?
CO₂-CH₄-H₂S	1	[18]	222～239	2.1～4.8	0.024～0.78	—	?
CO₂-CH₄-H₂O	5	[21]	243～432	0.1～100	0.001～0.83	—	?
CO₂-O₂-Ar-N₂	1	[21]	253～293	7.1～9.0	0.90	[29]	?

表4 CO2混合物物性估算研究现状（2008—2017）

序号	研究机构	物性	CO₂混合物体系	状态方程	主要结论	参考文献	年份
1	挪威科技大学；挪威科技工业研究院	VLE pρT	CO₂-N₂; CO₂-O_2; CO₂-CH₄; CO₂-N₂-O₂	SRK SRK-Peneloux PR Lee-Kesler SPUNG/SRK GERG-2004	GERG-2004的估算精度最高（除了在估算CO₂-O₂体系VLE性质时误差达到20%）； SPUNG可能成为较好估算精度和较短估算时间的折中选择	[50]	2012
		VLE pρT	CO₂-H₂O	SPUNG-vdW SRK- vdW ; SRK-HV	SPUNG在估算密度性质时比SRK更精确； SRK-HV在估算VLE性质时优于SPUNG；参比流体和参比状态方程的选取对SPUNG的估算精度有较大影响	[53]	2014
		VLE pρT	CO₂-H₂O	ECS-HV SPUNG- vdW	提出一种新的扩展对比态状态方程ECS；新的状态方程在估算CO₂-H₂O体系的VLE和密度性质时都具有较高的精度； ECS估算精度较SPUNG有了很大的提高； ECS估算时间与SPUNG在相同数量级	[54]	2015
2	德国波鸿大学	VLE	CO₂-N₂ CO₂-O₂ CO₂-Ar CO₂-CH₄	SRK-vdW GERG-2008 EOS-CG	实验测量了CO₂-N₂/O₂/Ar/CH₄在278～298K之间的相平衡性质；当杂质含量较低时，SRK-vdW、GERG-2008和EOS-CG都有较好的估算精度	[72]	2014
2		VLE pρT	CO₂-H₂O/N₂/O₂/Ar/CO H₂O-N₂/O₂/Ar/CO N₂-O₂/Ar/CO O₂-Ar/CO Ar-CO	EOS-CG，GERG-2008 LKP SRK-vdW	在GEGR-2008的基础上，提出了EOS-CG模型，该模型以CCS为背景过程；相比于GERG-2008，EOS-CG模型很大程度上提高了针对CCS混合流体的热物性估算精度	[57]	2016
3	法国洛林大学	VLE pρT 黏度	CO₂- N₂O CO₂+ NO/N₂O₂	PR- vdW SRK- vdW	应用蒙特卡洛分子模拟获得了CO₂-NO/N₂O₂体系缺失的相平衡实验数据； PR-vdW和SRK-vdW在估算CO₂-NO _x 体系VLE性质时都具有较好的精度	[71]	2012
		VLE 混合焓变	含有CO₂、N₂、H₂O、Ar、SO₂、O₂、N₂和碳氢化合物的二元体系	E-PPR78-vdW	将E-PPR78扩展应用到包含SO₂、O₂和NO的二元体系	[60]	2015
		VLE	含有CO₂、SO₂、O₂、NO、H₂O和碳氢化合物的二元体系	E-PPR78 PC-SAFT	E-PPR78和PC-SAFT都能够较好的估算大多数二元体系的VLE性质；对大多数二元体系，E-PPR78比PC-SAFT的估算精度高；应用蒙特卡洛分子分子模拟或得了实验缺失的相平衡数据	[62]	2017
		VLE 混合焓变	含有CO₂、CH₄、N₂、O₂、Ar、H₂、H₂S、COS、SO₂、NH₃、NO、NO₂、N₂O₄、N₂O、CO和H₂O的二元体系；含有CO₂、CH₄、CO、H₂S、N₂和H₂的三元体系	E-PPR78-vdW	将E-PPR78扩展到包含COS、NH₃、NO/N₂O₂、N₂O的二元体系；E-PPR78适用于多数CCS混合流体二元和三元体系的VLE和混合焓变的物性估算	[61]	2017
4	丹麦技术大学；希腊塞萨洛尼基亚里士多德大学	VLE LLE pρT VLE pρT	CO₂和水, 醇类, 二醇类，碳氢化合物的二元体系	CPA	CPA对上述二元体系的VLE，LLE和密度性质估算具有较好精度	[64]	2010
		VLE LLE pρT VLE pρT		CPA SRK-HV	CPA对上述二元体系的VLE和密度性质估算具有较好精度	[65]	2014

表4 CO2混合物物性估算研究现状（2008—2017）

序号	研究机构	物性	CO₂混合物体系	状态方程	主要结论	参考文献	年份
1	挪威科技大学；挪威科技工业研究院	VLE pρT	CO₂-N₂; CO₂-O_2; CO₂-CH₄; CO₂-N₂-O₂	SRK SRK-Peneloux PR Lee-Kesler SPUNG/SRK GERG-2004	GERG-2004的估算精度最高（除了在估算CO₂-O₂体系VLE性质时误差达到20%）； SPUNG可能成为较好估算精度和较短估算时间的折中选择	[50]	2012
		VLE pρT	CO₂-H₂O	SPUNG-vdW SRK- vdW ; SRK-HV	SPUNG在估算密度性质时比SRK更精确； SRK-HV在估算VLE性质时优于SPUNG；参比流体和参比状态方程的选取对SPUNG的估算精度有较大影响	[53]	2014
		VLE pρT	CO₂-H₂O	ECS-HV SPUNG- vdW	提出一种新的扩展对比态状态方程ECS；新的状态方程在估算CO₂-H₂O体系的VLE和密度性质时都具有较高的精度； ECS估算精度较SPUNG有了很大的提高； ECS估算时间与SPUNG在相同数量级	[54]	2015
2	德国波鸿大学	VLE	CO₂-N₂ CO₂-O₂ CO₂-Ar CO₂-CH₄	SRK-vdW GERG-2008 EOS-CG	实验测量了CO₂-N₂/O₂/Ar/CH₄在278～298K之间的相平衡性质；当杂质含量较低时，SRK-vdW、GERG-2008和EOS-CG都有较好的估算精度	[72]	2014
2		VLE pρT	CO₂-H₂O/N₂/O₂/Ar/CO H₂O-N₂/O₂/Ar/CO N₂-O₂/Ar/CO O₂-Ar/CO Ar-CO	EOS-CG，GERG-2008 LKP SRK-vdW	在GEGR-2008的基础上，提出了EOS-CG模型，该模型以CCS为背景过程；相比于GERG-2008，EOS-CG模型很大程度上提高了针对CCS混合流体的热物性估算精度	[57]	2016
3	法国洛林大学	VLE pρT 黏度	CO₂- N₂O CO₂+ NO/N₂O₂	PR- vdW SRK- vdW	应用蒙特卡洛分子模拟获得了CO₂-NO/N₂O₂体系缺失的相平衡实验数据； PR-vdW和SRK-vdW在估算CO₂-NO _x 体系VLE性质时都具有较好的精度	[71]	2012
		VLE 混合焓变	含有CO₂、N₂、H₂O、Ar、SO₂、O₂、N₂和碳氢化合物的二元体系	E-PPR78-vdW	将E-PPR78扩展应用到包含SO₂、O₂和NO的二元体系	[60]	2015
		VLE	含有CO₂、SO₂、O₂、NO、H₂O和碳氢化合物的二元体系	E-PPR78 PC-SAFT	E-PPR78和PC-SAFT都能够较好的估算大多数二元体系的VLE性质；对大多数二元体系，E-PPR78比PC-SAFT的估算精度高；应用蒙特卡洛分子分子模拟或得了实验缺失的相平衡数据	[62]	2017
		VLE 混合焓变	含有CO₂、CH₄、N₂、O₂、Ar、H₂、H₂S、COS、SO₂、NH₃、NO、NO₂、N₂O₄、N₂O、CO和H₂O的二元体系；含有CO₂、CH₄、CO、H₂S、N₂和H₂的三元体系	E-PPR78-vdW	将E-PPR78扩展到包含COS、NH₃、NO/N₂O₂、N₂O的二元体系；E-PPR78适用于多数CCS混合流体二元和三元体系的VLE和混合焓变的物性估算	[61]	2017
4	丹麦技术大学；希腊塞萨洛尼基亚里士多德大学	VLE LLE pρT VLE pρT	CO₂和水, 醇类, 二醇类，碳氢化合物的二元体系	CPA	CPA对上述二元体系的VLE，LLE和密度性质估算具有较好精度	[64]	2010
		VLE LLE pρT VLE pρT		CPA SRK-HV	CPA对上述二元体系的VLE和密度性质估算具有较好精度	[65]	2014

表4 CO2混合物物性估算研究现状（2008～2017）

序号	研究机构					参考文献	2012
		VLE pρT	CO₂和烷烃类二元体系	CPA SRK PR	将CPA的应用范围由n-eicosane（n-C₂₀）扩展到了hexatriacontane （n-C₃₆）； CPA能够应用于CO₂和烷烃类二元体系的VLE和密度性质估算	[66]	2015
		VLE VLLE	含CO₂、醇类和水的三元和四元体系	CPA	CPA能够较精确地估算前述多元体系的VLE和VLLE性质	[67]	2015
		VLE VLLE	CO₂和烷烃类、水、二醇类的多元体系	CPA	CPA能够较精确地估算前述多元体系的VLE和VLLE性质	[68]	2016
		VLE VLLE	CO₂-烷烃类 CO₂-二醇类 CO₂-H₂O	CPA qCPA	在CPA的基础上引入了电四极矩校正项，进而提出了qCPA qCPA极大地提高了CO₂-n-alkane体系的VLE和VLLE估算精度	[69]	2016
5	瑞典皇家理工学院；瑞典梅拉达伦大学	VLE	CO₂-N₂； CO₂-O₂； CO₂-Ar; CO₂-CH₄; CO₂-H₂S; CO₂-SO₂	PR/PT/RK/S RK/3P1T/-vdW	CO₂-N₂/O₂/Ar体系建议用PT； CO₂-CH₄/H₂S体系建议用PR； CO₂-SO₂体系建议用3P1T；利用实验数据回归二元交互系数能够很大程度提高立方型状态方程的估算精度	[51]	2009
6	法国石油与新能源研究院	VLE pρT 黏度	CO₂-N₂O； CO₂-NO/N₂O₂	PR SRK	采用蒙特卡洛分子模拟的方法回归了CO₂-NO _x 体系缺失的实验数据并拟合了PR、SRK状态方程二元交互系数； PR和SRK对VLE性质的估算结果都较好； PR对两相区的液相密度估算较SRK更接近蒙特卡洛分子模拟的结果	[71]	2012
7	意大利米兰理工大学	VLE	含有CO₂，H₂，N₂，O₂，Ar，CO，CH₄，	PR+EOS / $α r e s E, γ$	PR+EOS/ $α r e s E, γ$ 对所研究的23种二元体系的VLE性质都有较好的估算精度	[70]	2016

表4 CO2混合物物性估算研究现状（2008～2017）

序号	研究机构					参考文献	2012
		VLE pρT	CO₂和烷烃类二元体系	CPA SRK PR	将CPA的应用范围由n-eicosane（n-C₂₀）扩展到了hexatriacontane （n-C₃₆）； CPA能够应用于CO₂和烷烃类二元体系的VLE和密度性质估算	[66]	2015
		VLE VLLE	含CO₂、醇类和水的三元和四元体系	CPA	CPA能够较精确地估算前述多元体系的VLE和VLLE性质	[67]	2015
		VLE VLLE	CO₂和烷烃类、水、二醇类的多元体系	CPA	CPA能够较精确地估算前述多元体系的VLE和VLLE性质	[68]	2016
		VLE VLLE	CO₂-烷烃类 CO₂-二醇类 CO₂-H₂O	CPA qCPA	在CPA的基础上引入了电四极矩校正项，进而提出了qCPA qCPA极大地提高了CO₂-n-alkane体系的VLE和VLLE估算精度	[69]	2016
5	瑞典皇家理工学院；瑞典梅拉达伦大学	VLE	CO₂-N₂； CO₂-O₂； CO₂-Ar; CO₂-CH₄; CO₂-H₂S; CO₂-SO₂	PR/PT/RK/S RK/3P1T/-vdW	CO₂-N₂/O₂/Ar体系建议用PT； CO₂-CH₄/H₂S体系建议用PR； CO₂-SO₂体系建议用3P1T；利用实验数据回归二元交互系数能够很大程度提高立方型状态方程的估算精度	[51]	2009
6	法国石油与新能源研究院	VLE pρT 黏度	CO₂-N₂O； CO₂-NO/N₂O₂	PR SRK	采用蒙特卡洛分子模拟的方法回归了CO₂-NO _x 体系缺失的实验数据并拟合了PR、SRK状态方程二元交互系数； PR和SRK对VLE性质的估算结果都较好； PR对两相区的液相密度估算较SRK更接近蒙特卡洛分子模拟的结果	[71]	2012
7	意大利米兰理工大学	VLE	含有CO₂，H₂，N₂，O₂，Ar，CO，CH₄，	PR+EOS / $α r e s E, γ$	PR+EOS/ $α r e s E, γ$ 对所研究的23种二元体系的VLE性质都有较好的估算精度	[70]	2016

图2 CO2混合物物性估算在CCS过程中的应用

图3 杂质对CCS过程的影响

图4 单一组分气体水合物相图

图5 水合物法分离CO2的表现（p=3.5～11MPa，T=0.55～3℃）[97,98,99,100,101,102,103,104,105,106]

图6 物性是工程热力学研究的基础

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CO₂ 混合物热物性在CCS研究中的作用：实验数据、理论模型和典型应用

Role of thermodynamic properties of CO₂ mixtures in CCS: data, models and typical applications

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