Review on cryogenic technologies for CO<sub>2</sub> removal from natural gas

doi:10.1007/s11708-022-0821-0

Front. Energy

2022, Vol. 16

Issue (5) : 793-811 https://doi.org/10.1007/s11708-022-0821-0

REVIEW ARTICLE

Review on cryogenic technologies for CO₂ removal from natural gas

Yujing BI, Yonglin JU(

)

Institute of Refrigeration and Cryogenics, Shanghai Jiao Tong University, Shanghai 200240, China

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Abstract

CO₂ in natural gas (NG) is prone to condense directly from gas to solid or solidify from liquid to solid at low temperatures due to its high triple point and boiling temperature, which can cause a block of equipment. Meanwhile, CO₂ will also affect the calorific value of NG. Based on the above reasons, CO₂ must be removed during the NG liquefaction process. Compared with conventional methods, cryogenic technologies for CO₂ removal from NG have attracted wide attention due to their non-polluting and low-cost advantages. Its integration with NG liquefaction can make rational use of the cold energy and realize the purification of NG and the production of by-product liquid CO₂. In this paper, the phase behavior of the CH₄-CO₂ binary mixture is summarized, which provides a basis for the process design of cryogenic CO₂ removal from NG. Then, the detailed techniques of design and optimization for cryogenic CO₂ removal in recent years are summarized, including the gas-liquid phase change technique and the gas-solid phase change technique. Finally, several improvements for further development of the cryogenic CO₂ removal process are proposed. The removal process in combination with the phase change and the traditional techniques with renewable energy will be the broad prospect for future development.

Keywords cryogenic CO₂ removal purification of natural gas (NG) biogas upgrading CH₄-CO₂ binary system

Corresponding Author(s): Yonglin JU

Online First Date: 29 March 2022 Issue Date: 28 November 2022

Cite this article:

Yujing BI,Yonglin JU. Review on cryogenic technologies for CO₂ removal from natural gas[J]. Front. Energy, 2022, 16(5): 793-811.

URL:

https://academic.hep.com.cn/fie/EN/10.1007/s11708-022-0821-0
https://academic.hep.com.cn/fie/EN/Y2022/V16/I5/793

Fig.1 Qualitative pressure-temperature diagram of CO₂-CH₄ binary system.

Tab.1 Experimental research on phase behavior and CO₂ frost points of CH₄-CO₂ binary mixture

Tab.2 Theoretical research on characteristics of CH₄-CO₂ binary mixture

Fig.2 Ryan-Holmes process.

Fig.3 Dual-pressure distillation tower process.

Fig.4 Extractive distillation process for CO₂ separation (adapted with permission from Ref. [56].)

Fig.5 Process scheme of removal of CO₂ from acid gas.

Fig.6 Principal process flow diagram of low-temperature CO₂ removal from biogas.

Fig.7 A low-temperature removal of CO₂ from biogas combining distillation and flash.

Fig.8 Cryogenic process based on frosting and defrosting.

Fig.9 Cryogenic sublimation capture process based on the expansion cycle.

Fig.10 Internal structure of the distillation tower of the CFZ process.

Fig.11 Flow diagram of the CryoCell process.

Fig.12 Schematic of the hybrid cryogenic distillation process.

Tab.3 Differences between proposed CO₂ removal techniques based on gas-liquid phase change

Ref.	Feed gas composition (mole fraction)	Feed gas condition	Operation conditions	Effect	Total energy/MJ·kg^?1CO₂)	Method	Proposed process
[67]	81.39%N₂ + 11.63%CO₂ + 6.98%O₂	333 K, 0.12 MPa	Frost: 156 K; defrost: 217 K, 0.52 MPa	90%CO₂ removal	0.65–1.25	Experiment	Two alternate heat exchangers
[68]	–	–	112 K	5.7 × 10^?6 ppm CO₂	–	Analysis and calculation	Heat and mass transfer analysis
[69]	1%CO₂ + 99%CH₄	293 K, 0.7MPa	132.5 K, 5 MPa	2 × 10^?3 ppm	–	HYSYS simulation	Anti-sublimation process
[70]	75%N₂ + 20%CO₂ + 5%H₂O	373 K, 0.1 MPa	123 K	–	–	Experiment and simulation	Cryogenic bed
[71]	15%CO₂ + 7%H₂O + 75%N₂ + 3%O₂	312.8 K, 0.1 MPa	155 K	90%CO₂ removal	1.03	Aspen Plus simulation	Anti-sublimation process
[72]	5%CO₂ + 95%CH₄	–	6 MPa	–	–	Experiment	Cyclone separator
[73–75]	87%N₂ + 13%CO₂	298 K	168 K	85%CO₂ removal	3.4	Experiment and Numerical simulation	Stirling refrigerator
[76]	80%N₂ + 20%CO₂	300 K, 0.1 MPa	0.106 MPa, 140-165 K	41.2%–95.9% CO₂ removal	0.32–8.53	Experiment and EES simulation	CO₂ sublimation visualization test
[77,78]	99.5%CH₄ + 0.5%CO₂	308.15 K, 15 MPa	164.5 K, 1.5 MPa	5 × 10^?5ppm CO₂	–	HYSYS simulation	PLNG process
[79]	40%CH₄ + 59%CO₂ + 0.5%H₂S + H₂O	303 K, 0.150 MPa,	195 K, 3.44 MPa	3%(mole fraction) CO₂	5.22 MJ/kg bio-LNG	HYSYS simulation	Cryogenic upgrading bio-LNG plant
[80]	75%, 90%CO₂ + CH₄	–	133.4–167.4 K, 0.4–1.4 MPa	0.09%–0.85% (mole fraction)CO₂	0.094–2.5 MW	HYSYS simulation and experiment	Cryogenic packed bed
[81]	79.6%CH₄ + 18.5% CO₂ + 1.5%N₂ + others	311 K, 4.134 MPa	183.7–226 K, 3.79 MPa	0.234%(mole fraction) CO₂	–	Exxon program	CFZ process
[82]	31.3%CH₄ + 58%CO₂ + 9.7%N₂ + others	301.5 K, 7.2 MPa	–	0.3%(mole fraction) CO₂	20% less than Selexol	Experiment	CFZ process
[85]	13%, 21%, 40%, 60%CO₂ + CH₄	208–223 K, 5.5–6.5 MPa	–	3%, 4%, 14%, and 26%(mole fraction) CO₂	0.734–0.845	CryoFlash and HYSYS simulation	CryoCell process
[86]	50%–70%CO₂ + 39.7%–20%CH₄ + others	–	4 MPa	0.006%–0.1%(mole fraction)CO₂	235–262 MW	Aspen Plus simulation	Hybrid cryogenic rectification network

Tab.4 Differences between proposed CO₂ removal techniques based on gas-solid and combined phase change

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