Dissolution of CH4 in the crude oil system: behaviors and mechanisms

doi:10.16085/j.issn.1000-6613.2020-1801

Abstract

Abstract:

In order to study the dissolution process of methane (CH₄) in the crude oil system, the dissolution behavior of CH₄ in crude oil systems at different temperatures and pressures was systematically studied by means of CH₄ solubility test and molecular simulation. Taking n-heptane as the base oil, wax, colloid, and asphaltene content as influencing factors, the corresponding crude oil system was constructed according to L₁₆ (4³) orthogonal table. Two specific proportion crude oil systems of Shengli crude oil and Nanyang crude oil were constructed, with a total of 18 crude oil systems. The molecular dynamics method was used to simulate the dissolution of CH₄ in different crude oil systems. The reliability of the simulation was verified by experimental results. The results show that in the range of bubble point pressure, with the increase of dissolved gas pressure, the amount of CH₄ dissolved gradually increases, but the position of CH₄ dissolved may change. When the dissolved gas pressure is low, CH₄ molecules are more dispersed in the crude oil system, and with the increase of CH₄ dissolved amount, some CH₄ molecules will accumulate. The dissolution of CH₄ in crude oil system is a physical dissolution process, and the Van der Waals force is the main mechanical action in the process of CH₄ dissolution. The larger the free volume fraction of crude oil system is, the larger the dissolution space can be provided for CH₄. The influence of crude oil macromolecules on CH₄ dissolution is wax < colloid < asphaltene and the mechanical action mode of CH₄ dissolution is not changed by crude oil macromolecules. The linear relationship between the interaction energy and the volume change of crude oil system is revealed by mechanical model, which promotes the understanding on the dissolution of CH₄ in crude oil system molecular-level.

Key words: methane, crude oil, dissolution, molecular simulation, Van der Waals force, free volume

摘要：

为了研究甲烷（CH₄）在原油体系中的溶解过程，本文采用CH₄溶解度测试和分子模拟相结合的方式，系统研究了不同温度、压力条件下CH₄在原油体系中的溶解行为。以正庚烷为基础油，蜡、胶质、沥青质含量为影响因素，按照L₁₆(4³)正交表构建相应的原油体系，并构建胜利原油和南阳原油两种特定比例的原油体系，共18种原油体系。利用分子动力学方法模拟了CH₄分子在不同原油体系中的溶解过程，并利用试验结果验证了模拟的可靠性。结果表明：在泡点压力范围内，随着溶气压力的增加，CH₄溶解量逐渐增大，但其溶解位置可能发生变化；当溶气压力较低时，CH₄分子较为分散地分布在原油体系中，随着CH₄溶解量的增多，部分CH₄分子会发生聚集；CH₄在原油体系中的溶解为物理溶解过程，且CH₄溶解过程中范德华力为主要的力学作用方式；原油体系自由体积分数越大，能够为CH₄提供的溶解空间越大；原油大分子对CH₄溶解量影响程度依次为：蜡<胶质<沥青质，且原油大分子未改变CH₄溶解的力学作用方式，并通过力学模型揭示了相互作用能与原油体系体积变化量的线性关系，促进对CH₄在原油体系中溶解的分子级理解。

关键词: 甲烷, 原油, 溶解, 分子模拟, 范德华力, 自由体积

CLC Number:

TH382

LI Bingfan, LIU Gang, CHEN Lei. Dissolution of CH₄ in the crude oil system: behaviors and mechanisms[J]. Chemical Industry and Engineering Progress, 2021, 40(8): 4205-4222.

李秉繁, 刘刚, 陈雷. CH₄在原油体系中溶解规律及影响机理[J]. 化工进展, 2021, 40(8): 4205-4222.

Figures/Tables 28

References 41

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试验压力	胜利原油		南阳原油
试验压力	表观黏度（10s^-1） /Pa·s	平均降黏率 /%	表观黏度（10s^-1） /Pa·s	平均降黏率 /%
常压	1.65	—	32.18	—
1	1.52	7.88	30.84	4.16
2	1.40	15.15	29.55	8.17

试验压力	胜利原油		南阳原油
试验压力	表观黏度（10s^-1） /Pa·s	平均降黏率 /%	表观黏度（10s^-1） /Pa·s	平均降黏率 /%
常压	1.65	—	32.18	—
1	1.52	7.88	30.84	4.16
2	1.40	15.15	29.55	8.17

体系	组分	密度/g·cm^-3		相对误差/%
体系	组分	模拟值	试验值	相对误差/%
1	111	0.662	0.684	3.22
2	122	0.85	0.87	2.30
3	133	0.885	0.933	5.14
4	144	1.035	1.012	2.2
5	212	0.843	0.857	1.63
6	221	0.777	0.798	2.63
7	234	0.994	0.996	0.20
8	243	0.951	0.973	2.26
9	313	0.862	0.899	4.12
10	324	0.97	0.986	1.62
11	331	0.854	0.874	2.29
12	342	0.938	0.969	3.20
13	414	0.966	0.98	1.43
14	423	0.925	0.946	2.22
15	432	0.875	0.915	4.37
16	441	0.905	0.942	3.93
17	胜利原油	0.862	0.878	1.82
18	南阳原油	0.842	0.875	3.77

体系	组分	密度/g·cm^-3		相对误差/%
体系	组分	模拟值	试验值	相对误差/%
1	111	0.662	0.684	3.22
2	122	0.85	0.87	2.30
3	133	0.885	0.933	5.14
4	144	1.035	1.012	2.2
5	212	0.843	0.857	1.63
6	221	0.777	0.798	2.63
7	234	0.994	0.996	0.20
8	243	0.951	0.973	2.26
9	313	0.862	0.899	4.12
10	324	0.97	0.986	1.62
11	331	0.854	0.874	2.29
12	342	0.938	0.969	3.20
13	414	0.966	0.98	1.43
14	423	0.925	0.946	2.22
15	432	0.875	0.915	4.37
16	441	0.905	0.942	3.93
17	胜利原油	0.862	0.878	1.82
18	南阳原油	0.842	0.875	3.77

正庚烷（25℃）				胜利原油（40℃）				南阳原油（40℃）
压力 /MPa	试验值 /mol·mol^-1	计算值 /mol·mol^-1	相对误差 /%	压力 /MPa	试验值 /mmol·g^-1	计算值 /mmol·g^-1	相对误差 /%	压力 /MPa	试验值 /mmol·g^-1	计算值 /mmol·g^-1	相对误差 /%
3.67	0.163	0.161	4.294	0.5	0.262	0.263	0.382	0.5	0.236	0.179	24.175
6.96	0.276	2.657	7.246	1	0.433	0.498	15.067	1	0.399	0.422	5.793
10.3	0.376	0.355	7.181	1.5	0.629	0.695	10.576	1.5	0.530	0.602	13.518
13.7	0.470	0.455	5.319	2	0.758	0.837	10.490	2	0.633	0.712	12.405
17.01	0.539	0.525	4.453	—	—	—	—	—	—	—	—

Dissolution of CH₄ in the crude oil system: behaviors and mechanisms

CH₄在原油体系中溶解规律及影响机理

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Figures/Tables 28

References 41

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体系	组合情况	体系内分子个数
体系	组合情况	蜡分子	胶质	沥青质
1	111	0	0	0
2	122	0	5	5
3	133	0	11	11
4	144	0	25	25
5	212	5	0	5
6	221	5	5	0
7	234	5	11	25
8	243	5	25	11
9	313	11	0	11
10	324	11	5	25
11	331	11	11	0
12	342	11	25	5
13	414	25	0	25
14	423	25	5	11
15	432	25	11	5
16	441	25	25	0
17	胜利原油	13	4	0
18	南阳原油	25	0	4

体系	原油体系体积/?³	体系	原油体系体积/?³
体系1	22777.56	体系10	68951.63
体系2	38182.82	体系11	45008.31
体系3	50821.36	体系12	66071.80
体系4	80052.22	体系13	73341.38
体系5	33501.69	体系14	53874.80
体系6	32650.47	体系15	62628.34
体系7	77681.58	体系16	63042.01
体系8	74932.23	体系17	36543.51
体系9	43913.76	体系18	41314.62

体系	参数	20℃	40℃	60℃	80℃	体系	参数	20℃	40℃	60℃	80℃
2	V_L	1.817	1.675	1.582	1.511	11	V_L	1.756	1.656	1.568	1.515
	P_L	1.870	1.904	2.157	2.250		P_L	1.906	2.111	2.302	2.568
	R²	0.997	0.997	0.996	0.995		R²	0.992	0.987	0.988	0.985
3	V_L	1.479	1.403	1.330	1.258	12	V_L	1.277	1.186	1.103	1.058
	P_L	2.020	2.258	2.438	2.595		P_L	2.335	2.573	2.593	2.894
	R²	0.998	0.998	0.998	0.997		R²	0.997	0.998	0.999	0.998
4	V_L	0.945	0.900	0.859	0.797	13	V_L	1.122	1.052	1.008	0.965
	P_L	2.910	3.263	3.556	3.908		P_L	2.572	2.714	3.020	3.306
	R²	0.997	0.998	0.999	0.998		R²	0.998	0.998	0.995	0.995
5	V_L	1.855	1.725	1.608	1.527	14	V_L	1.564	1.450	1.380	1.331
	P_L	1.863	1.899	1.926	2.064		P_L	1.962	2.118	2.381	2.578
	R²	0.992	0.991	0.989	0.989		R²	0.998	0.996	0.993	0.993
6	V_L	1.885	1.751	1.672	1.603	15	V_L	1.391	1.289	1.205	1.150
	P_L	1.436	1.561	1.619	1.659		P_L	2.225	2.376	2.541	2.820
	R²	0.995	0.991	0.991	0.990		R²	0.998	0.999	0.998	0.999
7	V_L	0.992	0.926	0.858	0.822	16	V_L	1.443	1.345	1.262	1.174
	P_L	2.694	3.007	3.194	3.431		P_L	2.196	2.344	2.488	2.622
	R²	0.999	0.997	0.998	0.999		R²	0.997	0.997	0.997	0.995
8	V_L	1.233	1.158	1.099	1.056	17	V_L	1.869	1.734	1.652	1.586
	P_L	2.406	2.696	3.014	3.207		P_L	1.627	1.710	1.836	2.047
	R²	0.998	0.997	0.997	0.996		R²	0.991	0.988	0.989	0.986
9	V_L	1.702	1.612	1.510	1.421	18	V_L	1.757	1.673	1.578	1.493
	P_L	2.016	2.164	2.391	2.582		P_L	1.924	2.117	2.358	2.572
	R²	0.984	0.983	0.983	0.978		R²	0.997	0.995	0.997	0.995
10	V_L	1.025	0.935	0.860	0.824
	P_L	2.620	2.778	3.086	3.404
	R²	0.998	0.996	0.993	0.993

体系	组合情况	分子个数			溶解量 /mmol·g^-1
体系	组合情况	蜡分子	胶质	沥青质	溶解量 /mmol·g^-1
1	111	0	0	0	13.959
2	122	0	5	5	1.817
3	133	0	11	11	1.479
4	144	0	25	25	0.945
5	212	5	0	5	1.855
6	221	5	5	0	1.885
7	234	5	11	25	0.992
8	243	5	25	11	1.233
9	313	11	0	11	1.702
10	324	11	5	25	1.025
11	331	11	11	0	1.756
12	342	11	25	5	1.277
13	414	25	0	25	1.122
14	423	25	5	11	1.564
15	432	25	11	5	1.391
16	441	25	25	0	1.443
水平K₁		4.550	4.660	4.761	—
水平K₂		1.491	1.573	1.585	—
水平K₃		1.440	1.405	1.495	—
水平K₄		1.380	1.225	1.021	—
极差R		3.170	3.435	3.740	—
因子主次		3	2	1	—

体系	碳占比	体系	碳占比
体系1	7.00	体系10	18.54
体系2	10.64	体系11	11.06
体系3	14.21	体系12	15.13
体系4	20.33	体系13	18.50
体系5	10.14	体系14	15.06
体系6	9.05	体系15	14.04
体系7	19.01	体系16	14.50
体系8	16.62	体系17	9.85
体系9	13.22	体系18	11.91

体系	等量吸附热/kJ·mol^-1	平均值/kJ·mol^-1
体系1	4.912~5.564	5.268
体系2	4.543~4.743	4.609
体系3	4.381~4.597	4.451
体系4	4.126~4.219	4.163
体系5	4.565~4.790	4.639
体系6	4.629~4.872	4.689
体系7	4.175~4.247	4.210
体系8	4.277~4.406	4.323
体系9	4.434~4.635	4.514
体系10	4.211~4.291	4.246
体系11	4.509~4.718	4.577
体系12	4.284~4.490	4.354
体系13	4.245~4.336	4.285
体系14	4.313~4.540	4.387
体系15	4.403~4.609	4.480
体系16	4.342~4.590	4.421
体系17	4.597~4.837	4.664
体系18	4.48~4.687	4.551

体系	液体分子所占有的体积/?³	自由的体积/?³	自由体积分数/%
体系1	21210.66	1966.90	8.486
体系2	36588.23	1594.59	4.176
体系3	48823.01	1998.35	3.932
体系4	78514.80	1537.42	1.921
体系5	32011.95	1489.74	4.447
体系6	30797.41	1853.06	5.675
体系7	76103.78	1577.80	2.031
体系8	73082.61	1849.62	2.468
体系9	42138.28	1775.48	4.043
体系10	67452.92	1498.71	2.174
体系11	43092.17	1916.14	4.257
体系12	64227.34	1844.46	2.792
体系13	71665.13	1676.25	2.286
体系14	52325.56	1549.24	2.876
体系15	60674.83	1953.51	3.119
体系16	60820.33	2221.68	3.524
体系17	34698.63	1844.88	5.048
体系18	39594.58	1720.04	4.163

体系	原油体系体积模量/GPa	体积膨胀系数
体系1	1.925	17.382
体系2	2.195	15.243
体系3	2.526	13.240
体系4	4.001	8.361
体系5	2.102	15.917
体系6	1.972	16.966
体系7	3.731	8.966
体系8	2.966	11.280
体系9	2.378	14.068
体系10	3.725	8.980
体系11	2.304	14.516
体系12	2.867	11.667
体系13	3.449	9.700
体系14	2.803	11.933
体系15	2.448	13.667
体系16	2.625	12.746
体系17	2.052	16.301
体系18	2.308	14.493

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