CO2在醚酯溶剂中的溶解度测定及热力学计算

doi:10.11949/0438-1157.20190360

摘要/Abstract

摘要：

采用恒定容积法，在温度353.15、363.15、373.15 K下，测定了CO₂在丙二醇甲醚醋酸酯(PMA)、二丙二醇甲醚醋酸酯(DPMA)、乙二醇丁醚醋酸酯(BAC)以及乙二醇苯醚醋酸酯(EPA)中的溶解度数据，压力最高可达11.73 MPa。结果表明CO₂在醚酯体系中溶解度受温度、压强的影响较大，压强一定时，CO₂在醚酯中溶解度随温度升高而减小；温度一定时，随着压强增大而增大；相同条件下，CO₂在四种醚酯中溶解度大小为PMA＜ EPA＜BAC＜DPMA。通过变形Clausius - Clapeyron方程，计算得到CO₂在醚酯溶剂中的Gibbs自由能Δ_sol G，溶解焓变Δ_sol H和熵变 Δ_sol S等热力学性质，从宏观热运动角度进一步解释了CO₂的溶解机理，为开发新型CO₂物理吸收剂提供理论支撑。

关键词: 溶解度, 恒定体积法, CO₂, 醚酯溶剂, 热力学性质

Abstract:

In this study, the solubility of CO₂in propylene glycol monomethyl ether acetate (PMA), di(propylene glycol) methyl ether acetate (DPMA), 2-butoxyethyl acetate (BAC) and acetic acid 2-phenoxyethyl ester (EPA) was measured at the temperature variations from 353.15 K to 373.15 K rang up to 11.73 MPa by the constant-volume method. Results showed that the solubility of CO₂ in the ether esters solvents decreased with the increasing of temperature, increased with the increasing of pressure, and the solubility was PMA<EPA<BAC<DPMA, which was greatly affected by temperature and pressure. Meanwhile, thermodynamic properties of the Gibbs free energy Δ_sol G, enthalpy change Δ_sol H and entropy change Δ_sol S of CO₂ + ether ester system at different temperatures were also calculated by transformed Clausius-Clapeyron equation, further explained the dissolution mechanism of CO₂ from the perspective of macroscopic thermal motion, and provided theoretical support for the development of new CO₂ physical absorbents.

Key words: solubility, constant-volume method, CO₂, ether ester solvents, thermodynamic properties

中图分类号:

O 642.4⁺²

徐学满, 桂霞, 云志. CO₂在醚酯溶剂中的溶解度测定及热力学计算[J]. 化工学报, 2019, 70(11): 4113-4122.

Xueman XU, Xia GUI, Zhi YUN. Solubility determination and thermodynamic calculation of CO₂in several ether esters[J]. CIESC Journal, 2019, 70(11): 4113-4122.

图/表 18

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试剂	CAS	纯度	来源
CO₂	124-38-9	0.9999	创达气体
PMA	108-65-6	分析纯	阿拉丁
DPMA	88917-22-0	分析纯	阿拉丁
BAC	112-07-2	分析纯	阿拉丁
EPA	6192-44-5	分析纯	阿拉丁

试剂	CAS	纯度	来源
CO₂	124-38-9	0.9999	创达气体
PMA	108-65-6	分析纯	阿拉丁
DPMA	88917-22-0	分析纯	阿拉丁
BAC	112-07-2	分析纯	阿拉丁
EPA	6192-44-5	分析纯	阿拉丁

设备	规格	精度	供应商
高压相平衡釜	95 ml/35 MPa	±0.05 ml	海安华达
气体缓冲室	130 ml/50 MPa	±0.05 ml	海安华达
Pt-100铂电阻温度计	253~473 K	±0.1 K	OMEGA
硅芯片压力传感器	0~50 MPa	±1 KPa	OMEGA

设备	规格	精度	供应商
高压相平衡釜	95 ml/35 MPa	±0.05 ml	海安华达
气体缓冲室	130 ml/50 MPa	±0.05 ml	海安华达
Pt-100铂电阻温度计	253~473 K	±0.1 K	OMEGA
硅芯片压力传感器	0~50 MPa	±1 KPa	OMEGA

P/MPa	x ₁	y ₁	K ₁	K ₂	δ
T = 353.15 K
0.64	0.0771	0.9994	12.9624	0.0007	0.0007
1.38	0.1053	0.9987	9.4843	0.0015	0.0004
2.19	0.1456	0.9982	6.8558	0.0021	0.0005
3.01	0.1787	0.9979	5.5842	0.0026	0.0003
3.78	0.2217	0.9975	4.4993	0.0032	0.0002
4.62	0.2618	0.9969	3.8079	0.0042	0.0009
5.52	0.3061	0.9963	3.2548	0.0053	0.0007
6.36	0.3361	0.9955	2.9619	0.0068	0.0006
7.17	0.3892	0.9942	2.5545	0.0095	0.0004
8.13	0.4348	0.9936	2.2852	0.0113	0.0002
9.28	0.4956	0.9924	2.0024	0.0151	0.0007
10.31	0.5525	0.9911	1.7938	0.0199	0.0003
11.12	0.6003	0.9905	1.6500	0.0238	0.0005
T = 363.15 K
0.63	0.0675	0.9979	14.7837	0.0023	0.0009
1.35	0.1012	0.9970	9.8518	0.0033	0.0002
2.29	0.1314	0.9962	7.5814	0.0044	0.0007
3.24	0.1651	0.9954	6.0291	0.0055	0.0005
4.15	0.2034	0.9946	4.8899	0.0068	0.0003
5.22	0.2518	0.9931	3.9440	0.0092	0.0004
6.47	0.3043	0.9925	3.2616	0.0108	0.0009
7.45	0.3528	0.9913	2.8098	0.0134	0.0007
8.64	0.4105	0.9904	2.4127	0.0163	0.0005
9.88	0.4684	0.9883	2.1099	0.0220	0.0003
10.81	0.5255	0.9876	1.8794	0.0261	0.0009
T = 373.15 K
0.82	0.0642	0.9971	15.5312	0.0031	0.0007
1.89	0.1035	0.9954	9.6174	0.0051	0.0004
2.83	0.1304	0.9946	7.6273	0.0062	0.0002
3.75	0.1604	0.9928	6.1895	0.0086	0.0006
4.86	0.2033	0.9921	4.8800	0.0099	0.0007
5.91	0.2537	0.9914	3.9078	0.0115	0.0002
6.97	0.2822	0.9889	3.5397	0.0155	0.0005
7.81	0.3235	0.9882	3.0547	0.0174	0.0003
8.65	0.3578	0.9868	2.7580	0.0206	0.0004
9.84	0.4092	0.9853	2.4079	0.0249	0.0007
10.84	0.4557	0.9842	2.1598	0.0290	0.0002
11.73	0.5019	0.9833	1.9592	0.0335	0.0009

CO₂在醚酯溶剂中的溶解度测定及热力学计算

Solubility determination and thermodynamic calculation of CO₂in several ether esters

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P/MPa	x ₁	y ₁	K ₁	K ₂	δ
T = 353.15 K
0.42	0.0816	0.9999	12.2537	0.0001	0.0002
0.95	0.1092	0.9997	9.1548	0.0003	0.0003
1.71	0.1459	0.9983	6.8424	0.0020	0.0007
2.46	0.1867	0.9979	5.3449	0.0026	0.0009
3.29	0.2286	0.9975	4.3635	0.0032	0.0005
4.27	0.2854	0.9971	3.4937	0.0041	0.0004
5.17	0.3334	0.9968	2.9898	0.0048	0.0009
6.09	0.3828	0.9966	2.6034	0.0055	0.0007
6.95	0.4342	0.9962	2.2943	0.0067	0.0002
7.79	0.4909	0.9957	2.0283	0.0084	0.0003
8.61	0.5448	0.9955	1.8273	0.0099	0.0009
9.46	0.5959	0.9949	1.6696	0.0126	0.0006
10.44	0.6497	0.9946	1.5309	0.0154	0.0007
T = 363.15 K
0.63	0.0781	0.9998	12.8015	0.0002	0.0004
1.48	0.1072	0.9995	9.3237	0.0006	0.0002
2.42	0.1473	0.9988	6.7807	0.0014	0.0003
3.39	0.1866	0.9981	5.3489	0.0023	0.0009
4.28	0.2468	0.9976	4.0421	0.0032	0.0007
5.33	0.2918	0.9972	3.4174	0.0040	0.0002
6.34	0.3489	0.9965	2.8561	0.0054	0.0004
7.51	0.4085	0.9952	2.4362	0.0081	0.0003
8.45	0.4605	0.9944	2.1594	0.0104	0.0006
9.52	0.5178	0.9931	1.9179	0.0143	0.0009
10.56	0.5672	0.9928	1.7504	0.0166	0.0005
11.38	0.6095	0.9909	1.6258	0.0233	0.0007
T = 373.15 K
0.71	0.0717	0.9985	13.9261	0.0016	0.0003
1.63	0.1014	0.9973	9.8353	0.0030	0.0004
2.59	0.1387	0.9967	7.1860	0.0038	0.0002
3.64	0.1758	0.9951	5.6604	0.0059	0.0009
4.71	0.2189	0.9944	4.5427	0.0072	0.0007
5.68	0.2613	0.9929	3.7998	0.0096	0.0002
6.88	0.3079	0.9913	3.2196	0.0126	0.0005
7.96	0.3611	0.9905	2.7430	0.0149	0.0003
8.98	0.4155	0.9885	2.3791	0.0197	0.0004
10.07	0.4668	0.9872	2.1148	0.0240	0.0002
11.36	0.5322	0.9864	1.8534	0.0291	0.0007

P/MPa	x ₁	y ₁	K ₁	K ₂	δ
T = 353.15 K
0.38	0.0875	0.9999	11.4274	0.0001	0.0004
0.99	0.1263	0.9998	7.9161	0.0002	0.0002
1.55	0.1679	0.9995	5.9529	0.0006	0.0007
2.25	0.2119	0.9987	4.7131	0.0016	0.0005
2.98	0.2547	0.9984	3.9199	0.0021	0.0003
3.83	0.3169	0.9976	3.1480	0.0035	0.0007
4.41	0.3714	0.9971	2.6847	0.0046	0.0005
5.35	0.4321	0.9965	2.3062	0.0062	0.0004
6.23	0.4851	0.9959	2.0530	0.0080	0.0002
6.94	0.5465	0.9954	1.8214	0.0101	0.0003
7.81	0.6017	0.9943	1.6525	0.0143	0.0005
8.66	0.6497	0.9938	1.5296	0.0177	0.0007
9.61	0.7028	0.9931	1.4131	0.0232	0.0004
T = 363.15 K
0.45	0.0782	0.9991	12.7762	0.0010	0.0002
1.22	0.1125	0.9985	8.8756	0.0017	0.0004
2.07	0.1645	0.9982	6.0681	0.0022	0.0005
3.03	0.2036	0.9976	4.8998	0.0030	0.0003
3.92	0.2468	0.9968	4.0389	0.0042	0.0007
4.84	0.2918	0.9962	3.4140	0.0054	0.0009
5.87	0.3489	0.9975	2.8590	0.0038	0.0002
6.81	0.4101	0.9964	2.4297	0.0061	0.0007
7.95	0.4775	0.9955	2.0848	0.0086	0.0004
8.89	0.5305	0.9941	1.8739	0.0126	0.0005
9.93	0.5796	0.9936	1.7143	0.0152	0.0002
10.75	0.6369	0.9925	1.5583	0.0207	0.0003
T = 373.15 K
0.77	0.0713	0.9987	14.0070	0.0014	0.0005
1.34	0.0925	0.9975	10.7838	0.0028	0.0002
2.15	0.1225	0.9964	8.1339	0.0041	0.0004
3.17	0.1709	0.9957	5.8262	0.0052	0.0009
4.31	0.2227	0.9942	4.4643	0.0075	0.0003
5.54	0.2802	0.9929	3.5435	0.0099	0.0005
6.62	0.3312	0.9913	2.9931	0.0130	0.0002
7.79	0.3939	0.9887	2.5100	0.0186	0.0004
8.86	0.4558	0.9872	2.1659	0.0235	0.0009
10.06	0.5085	0.9864	1.9398	0.0277	0.0007
11.34	0.5631	0.9847	1.7487	0.0350	0.0003

P/MPa	x ₁	y ₁	K ₁	K ₂	δ
T = 353.15 K
0.45	0.1073	0.9981	9.3020	0.0021	0.0005
0.83	0.1653	0.9975	6.0345	0.0030	0.0003
1.33	0.2174	0.9970	4.5860	0.0038	0.0006
1.96	0.2674	0.9959	3.7244	0.0056	0.0004
2.69	0.3231	0.9952	3.0802	0.0071	0.0004
3.33	0.3831	0.9946	2.5962	0.0088	0.0006
4.21	0.4391	0.9937	2.2630	0.0112	0.0007
5.03	0.4968	0.9928	1.9984	0.0143	0.0003
5.86	0.5518	0.9905	1.7950	0.0212	0.0005
6.63	0.6136	0.9886	1.6111	0.0295	0.0003
7.51	0.6675	0.9873	1.4791	0.0382	0.0004
8.41	0.7126	0.9857	1.3832	0.0498	0.0006
9.27	0.7665	0.9833	1.2828	0.0715	0.0002
T = 363.15 K
0.67	0.0983	0.9954	10.1261	0.0051	0.0004
1.25	0.1427	0.9869	6.9159	0.0153	0.0002
2.03	0.1992	0.9844	4.9418	0.0195	0.0007
2.66	0.2579	0.9836	3.8139	0.0221	0.0009
3.63	0.3112	0.9825	3.1571	0.0254	0.0001
4.42	0.3691	0.9812	2.6584	0.0298	0.0004
5.43	0.4262	0.9798	2.2989	0.0352	0.0005
6.46	0.4893	0.9783	1.9994	0.0425	0.0003
7.74	0.5642	0.9775	1.7325	0.0516	0.0006
8.68	0.6163	0.9764	1.5843	0.0615	0.0008
9.69	0.6664	0.9757	1.4641	0.0728	0.0002
10.59	0.7175	0.9733	1.3565	0.0945	0.0005
11.24	0.7516	0.9715	1.2926	0.1147	0.0004
T = 373.15 K
0.89	0.0925	0.9942	10.7481	0.0064	0.0007
1.53	0.1225	0.9878	8.0637	0.0139	0.0002
2.44	0.1734	0.9861	5.6869	0.0168	0.0004
3.41	0.2263	0.9854	4.3544	0.0189	0.0005
4.37	0.2871	0.9831	3.4242	0.0237	0.0002
5.52	0.3475	0.9815	2.8245	0.0284	0.0007
6.67	0.4071	0.9762	2.3979	0.0401	0.0003
7.82	0.4709	0.9747	2.0699	0.0478	0.0004
9.33	0.5315	0.9728	1.8303	0.0581	0.0002
10.37	0.5854	0.9711	1.6589	0.0697	0.0005
11.29	0.6434	0.9705	1.5084	0.0827	0.0007

T/K	H/MPa
T/K	DPMA	BAC	EPA	PMA
353.15	13.62	15.01	17.49	20.02
363.15	16.31	18.42	19.66	22.46
373.15	18.95	20.96	22.97	25.03

溶剂	Δ_sol G/(kJ·mol^-1)	Δ_sol H/(kJ·mol^-1)	Δ_sol S/(J·mol^-1·K^-1)
DPMA	15.38	-18.23	-92.55
BAC	15.75	-17.54	-91.67
EPA	15.94	-14.93	-85.01
PMA	16.37	-12.36	-79.11

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