填料塔中有机胺吸收CO2气液传质的研究进展

doi:10.11949/0438-1157.20221076

摘要/Abstract

摘要：

胺法吸收CO₂是典型的气液传质和反应问题。填料塔作为化工生产中重要的气液分离设备，其填料层空隙率高的特性使得其具有传质效率高、生产能力大、操作弹性大等优点。本文主要依据填料塔持液量低、填料层压降小的流体力学性能和液泛气速高的操作特性，结合有机胺吸收CO₂的反应特点，基于传质理论，综述了操作温度、CO₂负荷与分压、惰性气体流速、液相流速和温度、有机胺种类和浓度以及填料类型对CO₂吸收过程中传质性能的影响。在后续研究中，可以从实验和模拟相结合的角度对填料塔中有机胺吸收CO₂气液传质和反应过程进行深入研究，进一步提高填料传质效率和提升溶剂吸收性能。

关键词: 填料塔, 传质, 有机胺, 二氧化碳捕集, 吸收

Abstract:

Amine absorption of CO₂ is a typical gas-liquid mass transfer and reaction process. As an important gas-liquid separation equipment in chemical production, packed columns have the advantages of high mass transfer efficiency, large production capacity, and large operation flexibility due to the high porosity of the packing layer. In this review, the mechanisms of CO₂ absorption with amines and the gas-liquid mass transfer models are introduced. Besides, the effects of operating temperature, CO₂ loading, CO₂ partial pressure, inert gas flow rate, liquid flow rate and temperature, the type and concentration of amines, and packing types on the mass transfer process in CO₂ absorption are summarized, based on the hydrodynamic properties of packed columns with low liquid holdup, low pressure drop in the packings and the operating characteristics with high gas velocity while fluids flooding. Finally, the directions of future studies are proposed, that in-depth research on gas-liquid mass transfer and reaction process in packed columns can be carried out from both experimental and simulation perspectives in terms of improving the mass transfer efficiency of packings and enhancing the amine absorption performance.

Key words: packed columns, mass transfer, amines, CO₂ capture, absorption

中图分类号:

TQ 051.8

王煦清, 严圣林, 朱礼涛, 张希宝, 罗正鸿. 填料塔中有机胺吸收CO₂气液传质的研究进展[J]. 化工学报, 2023, 74(1): 237-256.

Xuqing WANG, Shenglin YAN, Litao ZHU, Xibao ZHANG, Zhenghong LUO. Research progress on the mass transfer process of CO₂ absorption by amines in a packed column[J]. CIESC Journal, 2023, 74(1): 237-256.

图/表 15

图1 基于平衡和基于速率的气液传质模型示意图

Fig.1 Schematic diagram of equilibrium-stage and rate-based gas-liquid transfer models

图2 双膜模型示意图[60]

Fig.2 Schematic diagram of the two-film model[60]

图3 溶质渗透模型示意图[60]

Fig.3 Schematic diagram of the solute penetration model[60]

图4 填料塔内总体体积传质系数KGav 的计算[65]

Fig.4 Calculation of overall volume mass transfer coefficient KGav in the packed column[65]

表1 填料塔内单组分有机胺纯水溶液吸收CO2的实验条件和结果

Table 1 Experimental conditions and results for CO2 absorption by pure aqueous solutions of amines in packed column

吸收剂溶质	吸收剂浓度/ (kmol·m^-3)	填料种类	填料塔塔高/m	填料层高度/m	填料塔内径/mm	液相进料温度/℃	液相流速/ (m³·m^-2·h^-1)	惰性气体流速/ (kmol·m^-2·h^-1)	CO₂分压	CO₂负荷/ (mol·（mol 胺）^-1)	气相温度/℃	K_Ga_v /(kmol·m^-3·h^-1·kPa^-1)	文献
MEA	3.0~5.2	Gempak 4A	—	0.98/2.21	0.1	20/37	7.6~22.9	38.6	15.1%	—	—	0.83~0.91	[10]
MEA	3.0	BX	—	1.02	0.250	34~37	7.9	30.0	12.4%	—	—	—	[10]
DEEA	1.0~4.0	DX	1.70	—	28.0	20~60	3.90~11.70	30.5~43.52	3~15 kPa	0.05~0.20	20~60	0.09~0.22	[22]
MEA/ DEA/ DIPA^①/ MDEA^②/ AMP	3.0	DX	2.00	—	20.0	—	4.8~10.0	48.2	10%	0/ 0.25/ 0.40	25	0.85~2.93/ 0.18~1.15/ 0.11~0.45/ 0.02~0.09/ 0.22~0.95	[33]
MEA	3.0~7.0	DX	0.615~0.825	—	20.0	30~50	5.0~20.0	0.43~0.60 m³·m^-2·s^-1	3.7~15.2 kPa	0.2~0.6	—	0.14~3.14	[36]
MEA	1.0~3.0	DX	2.245	2.035	25.4	25	5.26~10.52	17.33~24.84	13.4%~14.8%	0.011~0.156	25	0.07~3.59	[65]
DEAB	1.0~3.0	DX	2.245	2.035	25.4	25	5.26~10.52	17.19~24.80	14.6%~14.8%	0.136~0.173	25	0.06~3.35	[65]
AMP	1.1~3.0	EX	1.77	0.055	19.0	24	6.1~14.6	46.2~96.8	10 kPa	—	—	0.16~1.07	[85]
MEA	2.0~5.0	Dixon环	—	1.40	24.0	30~50	3.98~9.29	24.98~39.45	14.8%~15.3%	0.008~0.230	30~50	0.26~0.40	[88]
DETA	1.0~4.0	Dixon环	—	1.40	24.0	30~50	2.65~7.56	28.78~46.62	15.1%~15.8%	0.052~0.819	30~50	0.25~1.28	[88]
DMEA	1.0~4.0	DX	1.70	—	28.0	20~60	3.90~11.70	26.11~43.52	6~20 kPa	0.05~0.30	25	0.08~0.15	[93]
MEA	3.0	拉西环	1.80	—	25.0	—	5.3/10.6/15.9	—	5%/10%/15%	0/0.1/0.2	—	0.08~0.59	[94]
DEAB	1.0~2.0	DX	2.15	—	275.0	25~40	3.90~7.80	17.85	—	0.09~0.28	25~40	0.04~0.18	[95]
MEA (5MPa高压)	1.0~4.0	金属丝网波纹填料	2.04	—	46.0	27~45	1.81~4.51	18.89~35.08	20%	—	—	0.18~5.29	[96]

表2 填料塔内单组分有机胺非纯水溶液吸收CO2的实验条件和结果

Table 2 Experimental conditions and results for CO2 absorption by non-pure aqueous solutions of amines in packed column

吸收剂	吸收剂浓度/ (kmol·m^-3)	填料种类	填料塔塔高/m	填料层高度/m	填料塔内径/mm	液相进料温度/℃	液相流速/ (m³·m^-2·h^-1)	惰性气体流速	CO₂分压	CO₂负荷/ (mol·（mol 胺）^-1)	气相温度/℃	K_Ga_v /(kmol· m^-3·h^-1·kPa^-1)	文献
MEA水溶液/ 甲醇溶液/ 等比例甲醇水溶液	5.0	DX	0.4	—	34.0	—	12~98 ml·min^-1	5/6/7/8/10 L·min^-1	15%	0.050~0.300	25	0.35~2.29/ 2.89~5.36/ 1.60~3.80	[42]
MEA甲醇水溶液	2.5~5.0	DX	1.7	—	28.0	10	2.92~16.09	24.37~63.54 kmol·m^-2·h^-1	6.7~13.8 kPa	0~0.373	—	0.19~3.70	[43]
MEA甲醇溶液	30%（质量）MEA	BX500/ Mellapale Y500/ 鲍尔环	2.5	—	DN150	—	20/30/40 L·h^-1	3/4/5 m³·h^-1	15%	—	—	4.57/ 3.35/ 3.30	[44]
MEA水溶液/ 甲醇溶液	15%~30%（质量）MEA	鲍尔环	2.0	—	97.0	35~55	0.75~1.25 L·min^-1	50~100 L·min^-1	5%~15% (物质的量)	—	27	0.60~2.42/ 0.95~5.45	[45]
MEA环丁砜水溶液	30%（质量）MEA& 20%（质量）环丁砜	Dixon环	—	1.21	28.0	30~60	3.90~11.70	26.11~43.52 kmol·m^-2·h^-1	9~20 kPa	0.2~0.4	—	0.17~5.63	[92]
MEA环丁砜水溶液	4/5 kmol·m^-3MEA& 5 kmol·m^-3环丁砜	DX	1.28	—	28.0	20~60	2.92~5.85	33.49~48.07 kmol·m^-2·h^-1	12~20 kPa	0.204~0.437	25	0.11~7.40	[97]
MEA甘油水溶液	10%/20%/30%（质量）MEA& 5%/10%/15%（质量）甘油	拉西环	0.5	—	50.0	30/37.5/45	85 ml·min^-1	4/5/6 L·min^-1	10%	—	—	0.31~0.63	[98]

表3 填料塔内混合胺溶液吸收CO2的实验条件和结果

Table 3 Experimental conditions and results for CO2 absorption by mixed amine solution in packed column

吸收剂溶质	吸收剂浓度/ (kmol·m^-3)	填料种类	填料塔塔高/m	填料层高度/m	填料塔内径/mm	液相进料温度/℃	液相流速/ (m³·m^-2·h^-1)	惰性气体流速/ (kmol·m^-2·h^-1)	CO₂分压	CO₂负荷/ (mol·(mol 胺)^-1)	气相温度/℃	K_Ga_v /(kmol· m^-3·h^-1·kPa^-1)	文献
MEA-MDEA/ DEA-MDEA/ MEA-AMP/ DEA-AMP	3.0 (摩尔比1∶1)	DX	2.00	—	20.0		4.8~10.0	48.2	10%	0/ 0.25/ 0.40	25	0.22~0.46/ 0.17~0.20/ 0.73~0.87/ 0.42~0.44	[33]
MEA-MDEA	3.0~7.0 (摩尔比1∶3、 1∶1和3∶1)	DX	0.615~0.825	—	20.0	30.0~50.0	5.0~20.0	0.43~0.60 m³·m^-2·s^-1	3.7~15.2 kPa	0.2~0.6	—	0.05~3.34	[36]
MEA-MDEA	摩尔比0.5∶2.3、0.8∶2.1和1.16∶1.95	DX	2.15	—	27.5	25/30/45	2.8/3.8/5.0	—	—	0.05/0.17/0.25	25	0.09~0.28/ 0.18~0.71/ 0.44~0.89	[99]
PZ-DETA/ AEPZ-DETA	DETA+PZ/ AEPZ共30% (其中PZ/AEPZ占10%)	Dixon环	—	0.70	39.0	30~60	6.10~12.36	27.39~65.48	6.1%~14.1%	≤0.04	—	0.42~0.76/ 0.37~0.72	[100]
PZ-AMP (0.1~4.0MPa高压)	20%~40%（质量） (摩尔比1∶4)	金属丝网波纹填料	2.04	—	46.0	30~45	2.89~3.97	33~51	—	—	30~45	0.002~0.02	[101]
PZ-AMP (0.1~5.0MPa高压)	30%（质量） [PZ：3%/5%/7%/9%（质量）]	金属丝网波纹填料	2.04	—	46.0	30	2.89~4.33	33	30%~50%	—	30	0.001~0.02	[102]
MEA-DEEA	3.0 (摩尔比1∶1)	Dixon环	1.28	—	28.0	25~50	3.90~9.75	26.11-39.17	6~18 kPa	0.18~0.32	25	0.11~0.92	[103]
MEA-DEEA	2.0~5.0 (摩尔比1∶1)	DX	—	1.25	28.0	30~70	3.90~11.70	30.47~47.87	6~18 kPa	0.15~0.35	—	0.14~2.24	[104]
MEA-DMEA	6.0 (摩尔比5∶1)	DX	1.70	1.25	28.0	20~60	2.92~5.85	33.49~48.07	12~20 kPa	0.204~0.437	25	0.03~0.81	[105]
MEA-1DMA2P^①	6.0 (摩尔比5∶1)	DX	1.70	1.25	28.0	13.03~50.08	2.92~5.85	33.49~48.07	12~20 kPa	0.204~0.437	25	0~5.75	[106]

表4 KGav 经验/半经验模型

Table 4 Semi- or empirical models for KGav

文献	K_Ga_v 拟合经验式	适用体系
[22]	$K G a v = L 0.18 0.5718 α e q - α C P C O 2 + 0.0489$	CO₂-DEEA体系规整填料 AAD：3%
[22]	$K G a v = 0.2526 L 0.177 C 0.2451 P C O 2 0.173 α - α e q - 0.0074$	CO₂-DEEA体系规整填料 AAD：8%
[65]	$K G a v = 0.194 L 0.5 α e q - α C P C O 2 + 0.155$	CO₂-DEAB体系 DX型规整填料 AAD：18%
[85]	$K G a v = 2.119 L 0.5 α e q - α C P C O 2 - 0.0193$	CO₂-AMP体系 EX型规整填料
[86]	$K G a v = F L μ L 23 1 + 5.7 α e q - α C e 0.0067 T - 3.4 P C O 2$	CO₂-MEA体系传统散装填料
[88]	$K G a v = L μ L 0.67 0.00805 α e q - α C e 0.0067 T - 3.4 P C O 2 - 0.000221$	CO₂-MEA体系 Dixon环形填料 AAD：14%
[88]	$K G α v = L 0.67 G I 0.08 0.752 × α e q - α C P C O 2 + 0.142$	CO₂-DETA体系 Dixon环形填料 AAD：16%
[90,95]	$K G a v = 1.0233 L 0.6 α e q - α C P C O 2 - 0.0071$	CO₂-DEAB体系 DX型规整填料 AAD：14.57%
[92]	$K G a v = L 0.43 G I 0.09 0.4955 α e q - α C e 0.00587 T - 0.081 P C O 2 - 0.4958$	CO₂-MEA&环丁砜体系 Dixon环形填料 AAD：10.2%
[93]	$K G a v = L 0.23 0.6144 α e q - α C P C O 2 + 0.02327$	CO₂- DMEA体系 Dixon环形填料 AARD^①：4.59%
[97]	$K G a v = 5.01 × 10 - 0.8 L 2.2058 T 3.07 α e q - α 1.99 C 3.058 G I 0.4926 P C O 2 4.124 + 0.17953$	CO₂-MEA&环丁砜体系 DX型规整填料 AAD：7.8%
[99]	$K G a v = 0.9254 e - 0.0032 c M D E A c M E A e - 4 α e - 10.325 x C O 2 L 0.8531 e 0.1438 C S e - 595.211 T$	CO₂-MEA+MDEA体系 Dixon环形填料 AAD：20.9%
	$K G a v = e - 1.1 α e - 14.3 x C O 2 L 0.559 e 0.3665 C S e - 511.5 T$	CO₂-MEA+MDEA体系 Dixon环形填料 AAD：21.7%
	$K G a v = e 0.04 c M D E A c M E A e - 3.65 α e - 11.4 x C O 2 L 0.91 e 0.2 C S e - 443 T$	CO₂-MEA+MDEA体系 Dixon环形填料 AAD：22.8%
[100]	$K G a v = 12.658 L 0.557 G I 0.118 e 1.576 W P Z / W D E T A W t o t a l e - 0.047 P C O 2 - 1303 / T$	CO₂-PZ+DETA体系 Dixon环形填料 AARD：5.35%
[100]	$K G a v = 4.191 L 0.726 G I 0.140 e 0.0234 W A E P Z / W D E T A W t o t a l e - 0.035 P C O 2 - 1337 / T$	CO₂-AEPZ+DETA体系 Dixon环形填料 AARD：7.32%
[103]	$K G a v = L 0.45 1.5816 α e q - α C P C O 2 + 0.0526$	CO₂-MEA+DEEA体系 Dixon环形填料 AAD：10.4%
[105]	$K G a v = 0.3441 L 1.45 T 1.65 α e q - α 3.18 G I P C O 2 1.48$	CO₂-MEA+DMEA体系 DX型规整填料 AARD：9.93%
[106]	$K G α v = 6.5601 L 0.349 α e q - α 1.315 C P C O 2$	CO₂-MEA+1DMA2P体系 DX型规整填料 AARD：9.03%

表4 KGav 经验/半经验模型

Table 4 Semi- or empirical models for KGav

文献	K_Ga_v 拟合经验式	适用体系
[22]	$K G a v = L 0.18 0.5718 α e q - α C P C O 2 + 0.0489$	CO₂-DEEA体系规整填料 AAD：3%
[22]	$K G a v = 0.2526 L 0.177 C 0.2451 P C O 2 0.173 α - α e q - 0.0074$	CO₂-DEEA体系规整填料 AAD：8%
[65]	$K G a v = 0.194 L 0.5 α e q - α C P C O 2 + 0.155$	CO₂-DEAB体系 DX型规整填料 AAD：18%
[85]	$K G a v = 2.119 L 0.5 α e q - α C P C O 2 - 0.0193$	CO₂-AMP体系 EX型规整填料
[86]	$K G a v = F L μ L 23 1 + 5.7 α e q - α C e 0.0067 T - 3.4 P C O 2$	CO₂-MEA体系传统散装填料
[88]	$K G a v = L μ L 0.67 0.00805 α e q - α C e 0.0067 T - 3.4 P C O 2 - 0.000221$	CO₂-MEA体系 Dixon环形填料 AAD：14%
[88]	$K G α v = L 0.67 G I 0.08 0.752 × α e q - α C P C O 2 + 0.142$	CO₂-DETA体系 Dixon环形填料 AAD：16%
[90,95]	$K G a v = 1.0233 L 0.6 α e q - α C P C O 2 - 0.0071$	CO₂-DEAB体系 DX型规整填料 AAD：14.57%
[92]	$K G a v = L 0.43 G I 0.09 0.4955 α e q - α C e 0.00587 T - 0.081 P C O 2 - 0.4958$	CO₂-MEA&环丁砜体系 Dixon环形填料 AAD：10.2%
[93]	$K G a v = L 0.23 0.6144 α e q - α C P C O 2 + 0.02327$	CO₂- DMEA体系 Dixon环形填料 AARD^①：4.59%
[97]	$K G a v = 5.01 × 10 - 0.8 L 2.2058 T 3.07 α e q - α 1.99 C 3.058 G I 0.4926 P C O 2 4.124 + 0.17953$	CO₂-MEA&环丁砜体系 DX型规整填料 AAD：7.8%
[99]	$K G a v = 0.9254 e - 0.0032 c M D E A c M E A e - 4 α e - 10.325 x C O 2 L 0.8531 e 0.1438 C S e - 595.211 T$	CO₂-MEA+MDEA体系 Dixon环形填料 AAD：20.9%
	$K G a v = e - 1.1 α e - 14.3 x C O 2 L 0.559 e 0.3665 C S e - 511.5 T$	CO₂-MEA+MDEA体系 Dixon环形填料 AAD：21.7%
	$K G a v = e 0.04 c M D E A c M E A e - 3.65 α e - 11.4 x C O 2 L 0.91 e 0.2 C S e - 443 T$	CO₂-MEA+MDEA体系 Dixon环形填料 AAD：22.8%
[100]	$K G a v = 12.658 L 0.557 G I 0.118 e 1.576 W P Z / W D E T A W t o t a l e - 0.047 P C O 2 - 1303 / T$	CO₂-PZ+DETA体系 Dixon环形填料 AARD：5.35%
[100]	$K G a v = 4.191 L 0.726 G I 0.140 e 0.0234 W A E P Z / W D E T A W t o t a l e - 0.035 P C O 2 - 1337 / T$	CO₂-AEPZ+DETA体系 Dixon环形填料 AARD：7.32%
[103]	$K G a v = L 0.45 1.5816 α e q - α C P C O 2 + 0.0526$	CO₂-MEA+DEEA体系 Dixon环形填料 AAD：10.4%
[105]	$K G a v = 0.3441 L 1.45 T 1.65 α e q - α 3.18 G I P C O 2 1.48$	CO₂-MEA+DMEA体系 DX型规整填料 AARD：9.93%
[106]	$K G α v = 6.5601 L 0.349 α e q - α 1.315 C P C O 2$	CO₂-MEA+1DMA2P体系 DX型规整填料 AARD：9.03%

图5 在6 kmol·m-3 MEA-DMEA(摩尔比5∶1)溶液中KG随温度的变化[105]

Fig.5 Effect of temperature on KG in 6 kmol·m-3 MEA-DMEA (molar ratio=5∶1) aqueous solution[105]

图6 KGav 随CO2负荷变化[93,99]

Fig.6 Effect of CO2 loading on KGav[93,99]

图7 KGav 随液相流速变化

Fig.7 Effect of liquid flow rate on KGav

图8 KGav 随CO2分压变化

Fig.8 Effect of CO2 partial pressure on KGav

图9 KGav 随惰性气体流速变化

Fig.9 Effect of inert gas flow rate on KGav

图10 KGav 随液相进料温度变化

Fig.10 Effect of liquid feed temperature on KGav

图11 KGav 随胺溶液浓度变化

Fig.11 Effect of the amine concentration on KGav

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填料塔中有机胺吸收CO₂气液传质的研究进展

Research progress on the mass transfer process of CO₂ absorption by amines in a packed column

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