Study on rapid construction of microemulsion system based on EACN of crude oil measured by the direct method

Abstract

The purpose of this study is to delineate the applicability of the direct method for determining the equivalent alkane carbon number (EACN), a crucial parameter in the hydrophilic-lipophilic deviation (HLD) theory, and to validate the efficacy of microemulsion systems formulated using this theory. The workload associated with constructing microemulsion systems can be substantially minimized through the application of the HLD theory, yet the accuracy and efficiency of this approach necessitate verification. Notably, the scope of application for the direct method in measuring EACN remains ambiguous. To address this, three different crude oil samples were analyzed, with their EACN values measured using the direct method. Subsequently, based on these measurements, microemulsion systems were screened and constructed according to the HLD theory. Adaptability experiments, interfacial tension assessments, and core displacement experiments were conducted to evaluate the system’s performance and its capacity to enhance oil recovery. The results indicate that the direct method has limitations in measuring the EACN of crude oil, particularly for heavy oils with complex compositions, but it is suitable for light oils with simpler compositions. Furthermore, the core displacement experiment revealed that for light oil from Xinghua Oilfield, the formulated system achieved a notable increase in recovery by 15.44%, demonstrating a significant enhancement in oil recovery.

Keywords

EACN / The HLD theory / Microemulsion flooding system / Cores displacement experiment / EOR

CRediT authorship contribution statement

Yibo Li: Methodology. Min Yang: Writing-original draft, Investigation. Tianshuang He: Writing-review & editing. Jutao Chen: Writing-review & editing.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

We greatly appreciate the financial support from The Science and Technology Department of Sichuan Province (2024NSFSC0198).

References

[1] L.B.L. Santos, A.C.M. Silva, K.R.O. Pereira, et al., Microemulsions stabilized with nanoparticles for EOR: a review, J, J. Mol. Liq. 391 (2023), https://doi.org/10.1016/j.molliq.2023.123271.

[2] T. Hoar, J. Schulman, Transparent water-in-oil dispersions: the oleopathic hydro-micelle, J. Nature 152 (3847) (1943) 102-103, https://doi.org/10.1038/152102a0.

[3] J.H. Schulman, W. Stoeckenius, L.M. Prince, Mechanism of formation and structure of micro emulsions by electron microscopy, J. Phys. Chem. 63 (10) (1959) 1677-1680, https://doi.org/10.1021/j150580a027.

[4] C. Leyu, L. Yingcheng, H. Xiujuan, et al., Mechanism, challenge and research advance in microemulsion-foam EOR, J. Fine Chem. 39 (1) (2022) 56-64, https://doi.org/10.13550/j.jxhg.20210655.

[5] W. Changqing, Research progress of enhanced oil recovery by microemulsion flooding technology, J. Chem. Eng. Equip. (1) (2023) 209-210, https://doi.org/10.19566/j.cnki.cn35-1285/tq.2023.01.032.

[6] C. Chuanzhi, W. Zijian, W. Zhongwei, et al. J. China Univ. Petrol. (, Effect of low-salinity water flooding on rock wettability based on DLVO theory, Ed. Nat. Sci.) 44 (1) (2020) 106-114, https://doi.org/10.3969/j.issn.1673-5005.2020.01.012.

[7] S. Na, Z. Liqiang, S. Jichao, Self-assembly of surfactants regulated by weak interactions (IV) Application in ionic conduction, J. China Surfact. Deterg. Cosmet. 49 (4) (2019) 214-219, https://doi.org/10.3969/j.issn.1001-1803.2019.04.002.

[8] Y. Daiyin, Y. Konghang, H. Kai, Winsor phase diagram method for studying the influence of salt and alcohol on the oil displacement performance of dodecyl betaine system, J. Oilfield Chem. 35 (1) (2018) 119-124 + 130, https://doi.org/10.19346/j.cnki.1000-4092.2018.01.022.

[9] C. Zhonghua, L. Huabin, C. Baoge, Study on the relation between level of IFT and enhanced oil recovery, J. Offshore Oil (3) (2005) 53-57, https://doi.org/10.3969/j.issn.1008-2336.2005.03.010.

[10] C. Yongmei, W. Hanhui, Y. Jiayong, Study of middle phase microemulsion formed by Petroleum sulfonate, J. Acta Phys. -Chim. Sin. 16 (8) (2000), https://doi.org/10.3866/PKU.WHXB20000810.

[11] W. Xiaojiang, Study on Preparation of Middle Phase Microemulsion System and Microscopic Oil Displacement Mechanism, D. Northeast Petroleum University, 2023, https://doi.org/10.26995/d.cnki.gdqsc.2023.000203.

[12] W.C. Griffin, J. Soc. Cosmet. Classification of surface-active agents by" HLB", Chem. 1 (1949) 311-325.

[13] Z. Ting, Z. Su’an, W. He, Research progress on preparation and stability of food-grade microemulsion, J. Farm Prod. Proc. 16 (2019) 67-70, https://doi.org/10.16693/j.cnki.1671-9646(X).2019.08.056.

[14] J. Salager, M. Bourrel, R. Schechter, et al., Mixing rules for optimum phase-behavior formulations of surfactant/oil/water systems, J. Soc. Petrol. Eng. 19 (5) (1979) 271-278, https://doi.org/10.2118/7584-PA.

[15] J. Salager, J. Morgan, R. Schechter, et al., Optimum formulation of surfactant/water/oil systems for minimum interfacial tension or phase behavior, J. Soc. Petrol. Eng. 19 (2) (1979) 107-115, https://doi.org/10.2118/7054-PA.

[16] E.J. Acosta, J.S. Yuan, A.S. Bhakta, J. Surfact. The characteristic curvature of ionic surfactants, Deterg. 11 (2008) 145-158, https://doi.org/10.1007/s11743-008-1065-7.

[17] H. Yoga, N. Gasimli, R. Johns, Reliable EACN Determination for Dead and Live Crude in Microemulsion Systems, C, International Petroleum Technology Conference, 2024 D021S059R003, https://doi.org/10.2523/iptc-23685-MS.

[18] W. Zhanghui, M. Yanbing, Hui’e L, et al., Correlations between alcohol content or solubilization parameter and equivalent alkane carbon number of oil mixtures for optimum middle phase microemulsions, CIESC J. 67 (4) (2016) 1399-1404, https://doi.org/10.11949/j.issn.0438-1157.20151150.

[19] W. Rongsayamanont, S. Soonglerdsongpha, N. Khondee, et al., Formulation of crude oil spill dispersants based on the HLD concept and using a lipopeptide biosurfactant, J, J. Hazard Mater. 334 (2017) 168-177, https://doi.org/10.1016/j.jhazmat.2017.04.005.

[20] L. Cash, J.L. Cayias, G. Fournier, et al., The application of low interfacial tension scaling rules to binary hydrocarbon mixtures, J. Coll. Interf. Sci. 59 (1) (1977) 39-44, https://doi.org/10.1016/0021-9797(77)90336-8.

[21] J.-M. Aubry, J.F. Ontiveros, J.-L. Salager, et al., Use of the normalized hydrophilic-lipophilic-deviation (HLDN) equation for determining the equivalent alkane carbon number (EACN) of oils and the preferred alkane carbon number (PACN) of nonionic surfactants by the fish-tail method (FTM), J. Adv. Coll. Interf. Sci. 276 (2020) 102099, https://doi.org/10.1016/j.cis.2019.102099.

[22] S.M. Pushpala, M.J. Michnick, Characterization of crude oils by alkane value as an aid in the selection of a micellar system for a surfactant flood, SPE Oilfield Geother. Chemi. Symp. (1983), https://doi.org/10.2118/11774-ms.

[23] G. Shutang, M. Xiren, Generation of low interfacial tension and determination of the eacn of daqing crude oil, J. Oilfield Chem. (2) (1985) 96-102, https://doi.org/10.19346/j.cnki.1000-4092.1985.02.002.

[24] H. Yianhua, L. Xiouning, An investigation on the methods for determing crude oil’s eacn values, J. Oilfield Chem. (4) (1987) 293-298, https://doi.org/10.19346/j.cnki.1000-4092.1987.04.007.

[25] S. Queste, J.L. Salager, R. Strey, et al., The EACN scale for oil classification revisited thanks to fish diagrams, J. Coll. Interf. Sci. 312 (1) (2007) 98-107, https://doi.org/10.1016/j.jcis.2006.07.004.

[26] L. Delforce, F. Duprat, J.-L. Ploix, et al., Fast prediction of the equivalent alkane carbon number using graph machines and neural networks, J. ACS omega 7 (43) (2022) 38869-38881, https://doi.org/10.1021/acsomega.2c04592.s002.

[27] L. Tianliang, Z. Guicai, P. Haihua, et al., Study on Optimizing Method for SP Binary Flooding System with Ultra-low IFT, C. 2017 International Field Exploration and Development Conference, 2017. Chengdu, China.

[28] J.L. Cayias, R.S. Schechter, W.H. Wade, Modeling crude oils for low interfacial tension, J. Soc. Petrol. Eng. 16 (6) (1976) 351-357, https://doi.org/10.2118/5813-pa.

[29] P. Fei, Z. Zaixu, Z. Xiaoxuan, et al., Impact of anionic and cationic surfactants interfacial tension on the oil recovery enhancement, J. Powder Technol. 373 (2020) 93-98, https://doi.org/10.1016/j.powtec.2020.06.033.

[30] S. Kumar, T. Ahmad, S. Shankhwar, et al., Evaluation of interfacial properties of aqueous solutions of anionic, cationic and non-ionic surfactants for application in enhanced oil recovery, J. Tenside Surfact. Deterg. 56 (2) (2019) 138-149, https://doi.org/10.3139/113.110607.

[31] K. Al-Azani, S. Abu-Khamsin, M. Alotaibi, et al., Synergistic performance of an in-house synthesized cationic Gemini surfactant for enhanced oil recovery under harsh conditions, J. Fuel 374 (2024) 132359, https://doi.org/10.1016/j.fuel.2024.132359.

[32] A. Witthayapanyanon, J.H. Harwell, D.A. Sabatini, Hydrophilic-lipophilic deviation (HLD) method for characterizing conventional and extended surfactants, J. Coll. Interf. Sci. 325 (1) (2008) 259-266, https://doi.org/10.1016/j.jcis.2008.05.061.

[33] D. Schirone, G. Tartaro, L. Gentile, et al., An HLD framework for cationic ammonium surfactants, J. JCIS Open 4 (2021) 100033, https://doi.org/10.1016/j.jciso.2021.100033.

[34] J.-L. Salager, R. Antón, J.M. Anderez, et al., Formulation des microémulsions par la méthode du HLD. Editions TI. https://doi.org/10.51257/a-v1-j2157, 2001.

[35] E. Acosta, E. Szekeres, D.A. Sabatini, et al., Net-average curvature model for solubilization and supersolubilization in surfactant microemulsions, J. Langmuir 19 (1) (2003) 186-195, https://doi.org/10.1021/la026168a.

[36] G. Broze, Handbook of Detergents, Part A: Properties, CRC Press, 1999, https://doi.org/10.1201/b10985.

[37] L. Jin, A. Jamili, Z. Li, et al., Physics based HLD-NAC phase behavior model for surfactant/crude oil/brine systems, J. Petrol. Sci. Eng. 136 (2015) 68-77, https://doi.org/10.1016/j.petrol.2015.10.039.

[38] J.-L. Salager, A. Graciaa, R. Marquez, Analyzing the surfactant classification confusion through the HLD formulation equation, J. JCIS Open 8 (2022) 100060, https://doi.org/10.1016/j.jciso.2022.100060.

[39] X. Wang, J. Liu, X. Wu, et al., A comprehensive study of the enhanced oil recovery potential of low-salinity water in heavy oil sandstone reservoir, J, J. Mol. Liq. 413 (2024) 126038, https://doi.org/10.1016/j.molliq.2024.126038.

[40] S. Ge, L. Shi, H. Liang, et al., Low-viscosity thermal-responsive epoxy emulsion for high-temperature and high-salinity reservoirs: plugging characteristics and core displacement test, J. Geoenergy Sci. Eng. 243 (2024) 213289, https://doi.org/10.1016/j.geoen.2024.213289.

[41] S.H. Jang, G.A. Pope, Microemulsion phase behavior of live crude oil and revisiting the EACN framework for crude oils, J. Coll. Surf. A: Physicochem. Eng. Aspect. 670 (2023) 131565, https://doi.org/10.1016/j.colsurfa.2023.131565.

[42] W. Wan, J. Zhao, J.H. Harwell, et al., Characterization of crude oil equivalent alkane carbon number (EACN) for surfactant flooding design, J. Dispers. Sci. Technol. 37 (2) (2016) 280-287, https://doi.org/10.1080/01932691.2014.950739.

[43] W. Yulin, J. Aihua, F. Yimin, Studies on the phase behavior of microemulsion based on sodium dodecyl sulfonate/alcohol/alkane/NaCl aqueous solution, J. Zhejiang Chem. Industr. (8) (2008) 10-14, https://doi.org/10.3969/j.issn.1006-4184.2008.08.005.

[44] F. Zhan, Middle-Phase Microemulsions Formulated with Low Surfactant Concentration for Enhanced Oil Recovery, 2021, https://doi.org/10.27342/d.cnki.gscdu.2021.005854.

[45] L. Fang, L. Ganzuo, F. Wei, et al., The studies of middle phase microemulsion formed by mixed anionic/cationic surfactants, J. Acta Chimica Sinica (1) (1996) 1-6.

[46] M.S.W. Nordiyana, M. Khalil, B.M. Jan, et al., Formation and phase behavior of winsor type III jatropha curcas-based microemulsion systems, J. Surfact. Deterg. 19 (4) (2016) 701-712, https://doi.org/10.1007/s11743-016-1814-y.

[47] X. Xu, A. Saeedi, K. Liu, An experimental study of combined foam/surfactant polymer (SP) flooding for carbone dioxide-enhanced oil recovery (CO₂-EOR), J. Petrol. Sci. Eng. 149 (2017) 603-611, https://doi.org/10.1016/j.petrol.2016.11.022.

[48] P. Wanfen, T. Yanli, Z. Tianhong, The oil displacement performance research of surfactant flooding in the low permeability reservoirs, J. Special. Petrochem. 34 (1) (2017) 21-25, https://doi.org/10.3969/j.issn.1003-9384.2017.01.005.

[49] F. Hussain, A. Zeinijahromi, P. Bedrikovetsky, et al., An experimental study of improved oil recovery through fines-assisted water flooding, J. Petrol. Sci. Eng. 109 (2013) 187-197, https://doi.org/10.1016/j.petrol.2013.08.031.