低黏二氰胺类离子液体乙烯汽液相平衡研究

doi:10.11949/0438-1157.20190080

摘要/Abstract

摘要：

从工业废气中回收分离乙烯（C₂H₄）具有重要意义，选用了三种低黏度二氰胺类离子液体，分别测定了293.15~333.15 K下其密度、黏度等物化性质，研究了其对乙烯（C₂H₄）吸收性能。采用非随机（局部）双液体模型（NRTL）关联了三种二元体系溶解度数据，实验值与计算值的平均相对偏差均小于3%。结果表明，低黏度二氰胺类离子液体对C₂H₄气体吸收性能良好，其中阳离子侧链长度增加和羟基功能团引入可增强对C₂H₄溶解度。同时，离子液体1-丁基-3-甲基咪唑二氰胺盐（[Bmim][DCN]）经过3次的吸收解吸循环，仍可以保持较好的C₂H₄吸收性能，表明该离子液体循环稳定性好，而1-丁基-3-甲基咪唑二氰胺盐（[Bmim][DCN]）对乙烯吸收量较高，具有作为C₂H₄吸收剂的潜力。

关键词: 离子液体, 二氰胺类, 乙烯, 吸收, 解吸

Abstract:

Three dicyandiamide-based ionic liquids with low viscosity were selected as absorbent for ethylene absorption. The physicochemical properties such as density and viscosity were measured at 293.15－333.15 K, and their properties were studied. The NRTL model was used to correlate the solubility data for the three binary systems. The average relative deviations (ARDs) between the experimental and calculated values of the three binary systems are 2.47%, 2.54% and 1.19%, respectively. The results show that the low viscous dicyandiamide-based ionic liquids presented good C₂H₄ absorption performance. The solubility of C₂H₄ in ionic liquids is improved by increasing the length of side-chain and introducing hydroxyl group in the imidazole cation. The C₂H₄ solubility would increase with decreasing temperature or increasing pressure. Furthermore, these ionic liquids such as [Bmim][DCN] exhibited outstanding reversibility after 3 times of absorption/desorption circulation. [Bmim][DCN] has the better C₂H₄ solubility than the other two, showing the potential to be C₂H₄ absorbent.

Key words: ionic liquid, dicyandiamide-based, ethylene, absorption, desorption

中图分类号:

TQ 028.8

杨瑞, 董丽, 陈嵩嵩, 成卫国, 曹俊雅. 低黏二氰胺类离子液体乙烯汽液相平衡研究[J]. 化工学报, 2019, 70(7): 2439-2447.

Rui YANG, Li DONG, Songsong CHEN, Weiguo CHENG, Junya CAO. Vapor-liquid equilibrium of ethylene in low viscous dicyanamide-based ionic liquids[J]. CIESC Journal, 2019, 70(7): 2439-2447.

图/表 14

图1 汽液相平衡实验装置

Fig.1 Experimental equipment for gas-liquid phase equilibrium

图2 323.15 K [Bmim][PF6]吸收C2H4溶解度与文献数据对比

Fig.2 C2H4 absorption capacity of [Bmim][PF6] in this work and literatures at 323.15 K

图3 二氰胺类离子液体密度随温度的变化

Fig.3 Densities of dicyandiamide-based ionic liquids at different temperatures

表1 离子液体密度关联系数

Table 1 Constants for density of Eq. (7)

样品	A/(g $?$ cm^-3)	B $×$ 10⁴/(g $?$ cm^-3)	R²
[Emim][DCN]	1.38784	-6.6	0.99998
[Bmim][DCN]	1.24988	-6.2	0.99968
[Hemim][DCN]	1.38923	-6.7	0.99995

表1 离子液体密度关联系数

Table 1 Constants for density of Eq. (7)

样品	A/(g $?$ cm^-3)	B $×$ 10⁴/(g $?$ cm^-3)	R²
[Emim][DCN]	1.38784	-6.6	0.99998
[Bmim][DCN]	1.24988	-6.2	0.99968
[Hemim][DCN]	1.38923	-6.7	0.99995

图4 二氰胺类离子液体黏度随温度的变化

Fig.4 Viscosity of dicyandiamide-based ionic liquids at different temperatures

表2 离子液体黏度关联系数

Table 2 Constants for viscosity of Eq. (8)

样品	D/(mPa $?$ s)	C/K	T₀/K	R²
[Emim][DCN]	0.1408	725.5	137.9	0.996508
[Bmim][DCN]	0.3392	486.3	187.3	0.996941
[Hemim][DCN]	0.1992	614.4	185.4	0.992966

表2 离子液体黏度关联系数

Table 2 Constants for viscosity of Eq. (8)

样品	D/(mPa $?$ s)	C/K	T₀/K	R²
[Emim][DCN]	0.1408	725.5	137.9	0.996508
[Bmim][DCN]	0.3392	486.3	187.3	0.996941
[Hemim][DCN]	0.1992	614.4	185.4	0.992966

表3 [Bmim][DCN]的密度、黏度测定值与文献值对比

Table 3 Comparison of measured density and viscosity of [Bmim][DCN] with its literature data

温度/K	密度^①/(g·cm^-1)		相对偏差/%	黏度^②/(mPa?s)		相对偏差/%
温度/K	实验值	文献值	相对偏差/%	实验值	文献值	相对偏差/%
293.15	1.068682	1.06396	0.44	33.562	33.15	-1.24
303.15	1.062988	1.05757	0.51	22.574	22.92	1.51
313.15	1.056648	1.05112	0.53	16.235	16.72	2.90
323.15	1.050358	1.04494	0.52	12.273	12.74	3.67
333.15	1.044137	1.03873	0.52	9.519	10.04	5.19

表4 三种离子液体在不同温度和压力下对乙烯的溶解度和φ1V、γ1的实验值

Table 4 Solubility, φ1Vand γ1 of C2H4 in three ionic liquids at different pressures and temperatures

T/K	p/kPa	x₁	φ₁^V	γ₁
C₂H₄+[Emim][DCN]
303.15	265.28	0.0182	0.984	0.989
303.15	407.47	0.0272	0.975	1.007
303.15	613.45	0.0424	0.96	0.96
303.15	1016.93	0.0666	0.939	0.988
303.15	1353.59	0.0856	0.919	1.001
313.15	297.67	0.0167	0.983	1.097
313.15	563.65	0.0318	0.969	1.078
313.15	931.95	0.0533	0.949	1.041
313.15	1219.53	0.0668	0.933	1.069
313.15	1446.23	0.0831	0.921	1.007
323.15	325.18	0.0160	0.984	1.192
323.15	551.82	0.0279	0.972	1.144
323.15	832.69	0.0403	0.958	1.176
323.15	1216.45	0.0616	0.939	1.103
323.15	1431.95	0.0767	0.929	1.031
333.15	402.39	0.0185	0.981	1.12
333.15	740.07	0.0338	0.966	1.11
333.15	942.78	0.0442	0.957	1.072
333.15	1312.68	0.0622	0.94	1.043
333.15	1557.77	0.0733	0.93	1.038
C₂H₄+[Bmim][DCN]
303.15	253.80	0.0208	0.984	1.043
303.15	466.68	0.0373	0.972	1.057
303.15	684.74	0.0537	0.958	1.061
303.15	907.81	0.0724	0.945	1.03
303.15	1109.56	0.0891	0.933	1.01
313.15	228.67	0.0172	0.986	1.082
313.15	512.98	0.0381	0.975	1.083
313.15	748.98	0.0558	0.963	1.066
313.15	940.58	0.0686	0.951	1.075
313.15	1160.98	0.0855	0.94	1.052
323.15	363.27	0.0222	0.983	1.175
323.15	659.11	0.0466	0.967	1.079
323.15	961.330	0.0683	0.952	1.058
323.15	1080.60	0.0772	0.946	1.046
323.15	1338.41	0.0963	0.933	1.024
333.15	353.08	0.0210	0.984	1.248
333.15	580.35	0.0384	0.973	1.111
333.15	813.26	0.0542	0.963	1.089
333.15	1053.51	0.0720	0.952	1.051
333.15	1217.06	0.0810	0.945	1.071
C₂H₄+[Hemim][DCN]
303.15	395.17	0.0285	0.976	1.051
303.15	551.66	0.0386	0.966	1.068
303.15	766.63	0.0535	0.954	1.062
303.15	952.33	0.0669	0.943	1.042
303.15	1306.31	0.0918	0.922	1.019
313.15	379.32	0.0223	0.979	1.137
313.15	557.07	0.0327	0.969	1.126
313.15	707.14	0.0433	0.961	1.07
313.15	953.86	0.0585	0.948	1.058
313.15	1173.65	0.0714	0.936	1.05
323.15	380.56	0.0212	0.981	1.11
323.15	539.47	0.0291	0.973	1.14
323.15	746.96	0.0423	0.963	1.072
323.15	969.73	0.5055	0.952	1.05
323.15	1161.48	0.0659	0.943	1.049
333.15	367.57	0.0181	0.983	1.181
333.15	589.29	0.0311	0.973	1.093
333.15	804.135	0.0426	0.964	1.078
333.15	967.27	0.0519	0.956	1.056
333.15	1155.61	0.0615	0.948	1.053

表4 三种离子液体在不同温度和压力下对乙烯的溶解度和φ1V、γ1的实验值

Table 4 Solubility, φ1Vand γ1 of C2H4 in three ionic liquids at different pressures and temperatures

T/K	p/kPa	x₁	φ₁^V	γ₁
C₂H₄+[Emim][DCN]
303.15	265.28	0.0182	0.984	0.989
303.15	407.47	0.0272	0.975	1.007
303.15	613.45	0.0424	0.96	0.96
303.15	1016.93	0.0666	0.939	0.988
303.15	1353.59	0.0856	0.919	1.001
313.15	297.67	0.0167	0.983	1.097
313.15	563.65	0.0318	0.969	1.078
313.15	931.95	0.0533	0.949	1.041
313.15	1219.53	0.0668	0.933	1.069
313.15	1446.23	0.0831	0.921	1.007
323.15	325.18	0.0160	0.984	1.192
323.15	551.82	0.0279	0.972	1.144
323.15	832.69	0.0403	0.958	1.176
323.15	1216.45	0.0616	0.939	1.103
323.15	1431.95	0.0767	0.929	1.031
333.15	402.39	0.0185	0.981	1.12
333.15	740.07	0.0338	0.966	1.11
333.15	942.78	0.0442	0.957	1.072
333.15	1312.68	0.0622	0.94	1.043
333.15	1557.77	0.0733	0.93	1.038
C₂H₄+[Bmim][DCN]
303.15	253.80	0.0208	0.984	1.043
303.15	466.68	0.0373	0.972	1.057
303.15	684.74	0.0537	0.958	1.061
303.15	907.81	0.0724	0.945	1.03
303.15	1109.56	0.0891	0.933	1.01
313.15	228.67	0.0172	0.986	1.082
313.15	512.98	0.0381	0.975	1.083
313.15	748.98	0.0558	0.963	1.066
313.15	940.58	0.0686	0.951	1.075
313.15	1160.98	0.0855	0.94	1.052
323.15	363.27	0.0222	0.983	1.175
323.15	659.11	0.0466	0.967	1.079
323.15	961.330	0.0683	0.952	1.058
323.15	1080.60	0.0772	0.946	1.046
323.15	1338.41	0.0963	0.933	1.024
333.15	353.08	0.0210	0.984	1.248
333.15	580.35	0.0384	0.973	1.111
333.15	813.26	0.0542	0.963	1.089
333.15	1053.51	0.0720	0.952	1.051
333.15	1217.06	0.0810	0.945	1.071
C₂H₄+[Hemim][DCN]
303.15	395.17	0.0285	0.976	1.051
303.15	551.66	0.0386	0.966	1.068
303.15	766.63	0.0535	0.954	1.062
303.15	952.33	0.0669	0.943	1.042
303.15	1306.31	0.0918	0.922	1.019
313.15	379.32	0.0223	0.979	1.137
313.15	557.07	0.0327	0.969	1.126
313.15	707.14	0.0433	0.961	1.07
313.15	953.86	0.0585	0.948	1.058
313.15	1173.65	0.0714	0.936	1.05
323.15	380.56	0.0212	0.981	1.11
323.15	539.47	0.0291	0.973	1.14
323.15	746.96	0.0423	0.963	1.072
323.15	969.73	0.5055	0.952	1.05
323.15	1161.48	0.0659	0.943	1.049
333.15	367.57	0.0181	0.983	1.181
333.15	589.29	0.0311	0.973	1.093
333.15	804.135	0.0426	0.964	1.078
333.15	967.27	0.0519	0.956	1.056
333.15	1155.61	0.0615	0.948	1.053

表5 亨利常数的系数

Table 5 Parameters of Henry constants in this work

系统(i)+(S)	a_iS	b_iS
C₂H₄+[Emim][DCN]	0.0457	0.0087
C₂H₄+[Bmim][DCN]	1.0177	0.0047
C₂H₄+[Hemim][DCN]	-0.1276	0.0089

表6 NRTL模型参数

Table 6 Parameters of NRTL model in this work

系统(1)+(2)	α	τ₁₂⁽⁰⁾	τ₁₂⁽¹⁾	τ₂₁⁽⁰⁾	τ₂₁⁽¹⁾	ARD/%
C₂H₄+[Emim][DCN]	0.449	105.874	-9.789	1.183	-356.459	2.47
C₂H₄+[Bmim][DCN]	0.313	130.173	-9.717	0.877	-252.221	2.54
C₂H₄+[Hemim][DCN]	0.086	89.4897	-10.064	84.413	299.8386	1.19

图5 三种离子液体在不同温度对C2H4的溶解度

Fig.5 Solubilities of C2H4 in three ionic liquids at different temperatures

图6 313.15 K下C2H4在不同阳离子的离子液体中的溶解度

Fig.6 Solubilities of C2H4 in three different cation ionic liquids at 313.15 K

图7 323.15 K下C2H4在不同阴离子的离子液体中的溶解度

Fig.7 Solubilities of C2H4 in three different anion ionic liquids at 323.15 K

图8 [Bmim][DCN]的吸收循环性能

Fig.8 Absorption cycles of [Bmim][DCN] at 313.15 K

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