纳米SiO<sub>2</sub>/HPAM/SDS分散体系稳定性的改进及其对驱油性能的影响

陈五花; 王业飞; 何臻培; 丁名臣

纳米SiO₂/HPAM/SDS分散体系稳定性的改进及其对驱油性能的影响

陈五花^{1, 2, ,},
王业飞^{1, 2},
何臻培^{1, 2},
丁名臣^{1, 2}

1.
中国石油大学(华东), 非常规油气开发教育部重点实验室, 山东青岛 266580
2.
中国石油大学(华东)石油工程学院, 山东省油田化学重点实验室, 山东青岛 266580

基金项目:

国家科技重大专项"大型油气田及煤层气开发" 2016ZX05058-003-003

详细信息

中图分类号: TE39
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- 被引次数: 0
出版历程
- 收稿日期: 2020-07-07
- 修回日期: 2020-08-01
- 刊出日期: 2020-09-10

Improvement of stability of nano-SiO₂/HPAM/SDS dispersion systems and its effect on oil displacement performances

CHEN Wu-hua^{1, 2
, ,},
WANG Ye-fei^{1, 2},
HE Zhen-pei^{1, 2},
DING Ming-chen^{1, 2}

1.
Key Laboratory of Unconventional Oil&Gas Development, China University of Petroleum(East China), Qingdao 266580, China
2.
Shandong Key Laboratory of Oilfield Chemistry, School of Petroleum Engineering, China University of Petroleum(East China), Qingdao 266580, China

Funds:

the National Science and Technology Major Project of China 2016ZX05058-003-003

More Information

Corresponding author: CHEN Wu-hua, E-mail:cwh8157@163.com

摘要

摘要: 分析了60℃、1.0×10⁴ mg/L氯化钠盐水和模拟地层水中纳米SiO₂/HPAM/SDS分散体系的浊度实验及Zeta电位，发现Ca²⁺、Mg²⁺离子是体系失去稳定性的主要原因。根据沉降实验及Zeta电位分析仪探讨了降低pH值和添加络合剂对模拟地层水中纳米SiO₂/HPAM/SDS体系稳定性的改善效果及机理，同时利用流变仪及界面张力仪分析了两种方法对体系驱油性能的影响。结果表明，pH值降低，体系的Zeta电位绝对值降低，但SiO₂周围H⁺保护层的形成及水化作用力的增强改善了体系的稳定性；络合剂Na₂EDTA、ATMP和Na₄EDTA均能增强体系的稳定性，Na₂EDTA和ATMP络合Ca²⁺、Mg²⁺的同时降低了体系的pH值，而体系的黏度随pH值的降低急剧下降；Na₄EDTA加入后，体系的pH值增大，稳定配位化合物的形成使体系的Zeta电位绝对值、黏度、储能模量和损耗模量增加，降低界面张力的能力增强。因此，在SiO₂质量分数为0.5%的体系中加入质量分数为0.4%的Na₄EDTA（最佳质量分数），采收率提高了3.1%。
- 纳米SiO₂ /
- pH值 /
- 络合剂 /
- 稳定性 /
- 驱油性能
Abstract: The turbidity and Zeta potential experiments of nano-SiO₂/HPAM/SDS dispersion systems at 60 ℃, 1.0×10⁴ mg/L NaCl brine and simulated formation water were first investigated and the results indicated that Ca²⁺ and Mg²⁺ ions were responsible for the instability of dispersion system. Then, the methods of reducing pH value and adding chelating agents were used to improve the stability of nano-SiO₂/HPAM/SDS dispersion system in simulated formation water, and the improvement effects and mechanisms were discussed based on sedimentation experiments and Zetasizer. The influences of these two methods on the oil displacement performances of dispersion system were analyzed by rheometer and interfacial tensiometer. The experimental results suggested that with the decrease of pH value, the stability of dispersion system was enhanced by the protection of H⁺ in the SiO₂ double electric layer and the enhancement of hydration forces between particles although the absolute value of Zeta potential(|ζ|) of dispersion system decreased. All of the chelating agents including Na₂EDTA, ATMP and Na₄EDTA can improve the stability of dispersion system. Ca²⁺ and Mg²⁺ ions were complexed and pH value of dispersion system was decreased with the addition of Na₂EDTA and ATMP, however, the decrease of pH value resulted in a sharp deterioration in the viscosity of dispersion systems. With the addition of Na₄EDTA, the pH value of dispersion systems increased. The|ζ|, viscosity, storage modulus and loss modulus of dispersion systems all increased, which were benefited from the formation of stable complexes between Na₄EDTA, and Ca²⁺ and Mg²⁺. Meanwhile, the ability of dispersion system to reduce oil and water interfacial tension was enhanced. Thus, after addition of Na₄EDTA with mass ratio of 0.4% (optimal mass ratio)in dispersion system with nano-SiO₂ mass ratio of 0.5%, the oil recovery was increased by 3.1%.
- nano-SiO₂ /
- pH value /
- chelating agents /
- stability /
- oil displacement performance

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图 1 不同盐环境下纳米SiO₂/HPAM/SDS分散体系的浊度随时间的变化

Figure 1 Turbidity of nano-SiO₂/HPAM/SDS dispersion systems versus time at different salt environments

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图 2 不同分散体系的浊度随时间的变化

Figure 2 Turbidity of different dispersion systems versus time

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图 3 不同HPAM浓度下纳米SiO₂ /HPAM/SDS分散体系的浊度随时间的变化

Figure 3 Turbidity of nano-SiO₂/HPAM/SDS dispersion systems versus time at different HPAM concentrations

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图 4 不同pH值的纳米SiO₂/HPAM/SDS分散体系静置10 d时的状态

Figure 4 Visual status of nano-SiO₂/HPAM/SDS dispersion systems with different pH values after 10 d

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图 5 纳米SiO₂/HPAM/SDS分散体系不同pH值下的Zeta电位

Figure 5 Zeta potentials of nano-SiO₂/HPAM/SDS dispersion systems at different pH values

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图 6 纳米SiO₂对HPAM/SDS溶液降低界面张力的影响

Figure 6 Effect of nano-SiO₂ on the interfacial tension reduction capacity of HPAM/SDS solutions

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图 7 pH值对纳米SiO₂/HPAM/SDS分散体系黏度的影响

Figure 7 Influence of pH value on viscosities of nano-SiO₂/HPAM/SDS dispersion systems

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图 8 添加络合剂的纳米SiO₂/HPAM/SDS分散体系静置10 d时的状态

Figure 8 Visual status of nano-SiO₂/HPAM/SDS dispersion systems with chelating agents after 10 d

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图 9 添加络合剂的纳米SiO₂/HPAM/SDS分散体系的pH值及Zeta电位

Figure 9 pH values and Zeta potentials of nano-SiO₂/HPAM/SDS dispersion systems with chelating agents

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图 10 分散体系黏度与Na₄EDTA质量分数的关系

Figure 10 Relations between viscosities of dispersion systems and Na₄EDTA mass ratio

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图 11 Na₄EDTA对分散体系黏弹性的影响

Figure 11 Effect of Na₄EDTA on the viscoelastic properties of dispersion systems

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图 12 Na₄EDTA对分散体系降低界面张力的影响

Figure 12 Effect of Na₄EDTA on the interfacial tension reduction capacity of dispersion systems

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图 13 Na₄EDTA对分散体系分油率的影响

Figure 13 Effect of Na₄EDTA on the oil separation rate of dispersion systems

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表 1 纳米SiO₂/HPAM/SDS分散体系的Zeta电位

Table 1 Zeta potential of nano-SiO₂/HPAM/SDS dispersion systems

w (SiO₂)/%	0.2	0.5	1.0	1.5
Formation water	-29.7	-24.2	-21.1	-18.8
NaCl solution	-45.3	-39.1	-37.6	-33.5

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表 2 岩心参数及各阶段采收率

Table 2 Physical parameters of core samples and oil recovery at each production stage

Pore volume V/mL	Permeability /(10^-3 μm²)	Original oil saturation /%	Chemical formula	Recovery /%
Pore volume V/mL	Permeability /(10^-3 μm²)	Original oil saturation /%	Chemical formula	water flood recovery	tertiary recovery	final recovery
11.0	1358.0	76.4	SiO₂/HPAM/SDS	41.0	23.9	64.9
10.8	1345.0	77.2	SiO₂/HPAM/SDS + Na₄EDTA	40.8	27.0	67.8

下载: 导出CSV

参考文献(25)

[1]	刘潇潇.聚驱后聚/表二元驱驱油效果及流度控制研究[D].大庆: 东北石油大学, 2015. http://cdmd.cnki.com.cn/Article/CDMD-10220-1015362756.htm LIU Xiao-xiao. Study on displacement effect factors of surfactant-polymer system and method of mobility control after polymer[D]. Daqing: Northeast Petroleum University, 2015. http://cdmd.cnki.com.cn/Article/CDMD-10220-1015362756.htm
[2]	THOMAS S, ALI S M F, SCOULAR J R, VERKOCZY B. Chemical methods for heavy oil recovery[J]. J Can Pet Technol, 2001, 40(3):56-61. http://www.researchgate.net/publication/266663654_chemical_methods_for_heavy_oil_recovery
[3]	李美蓉, 柳智, 宋新旺, 马宝东, 张文.金属阳离子对聚丙烯酰胺溶液黏度的影响及其降黏机理研究[J].燃料化学学报, 2012, 40(1):43-47. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=rlhxxb201201007 LI Mei-rong, LIU Zhi, SONG Xin-wang, MA Bao-dong, ZHANG Wen. Effect of metal ions on the viscosity of polyacrylamide solution and the mechanism of viscosity degradation[J]. J Fuel Chem Technol, 2012, 40(1):43-47. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=rlhxxb201201007
[4]	ZHANG L, ZHANG D, JIANG B. The rheological behavior of salt tolerant polyacrylamide solutions[J]. Chem Eng Technol, 2006, 29:395-400. doi: 10.1002/ceat.200500306
[5]	孙宠.纳米SiO₂颗粒稳定泡沫体系的研制及性能评价[D].大庆: 东北石油大学, 2018. http://cdmd.cnki.com.cn/Article/CDMD-10220-1018163133.htm SUN Chong. Preparation and performance evaluation of modified nano silica stabilized foam system[D]. Daqing: Northeast Petroleum University, 2018. http://cdmd.cnki.com.cn/Article/CDMD-10220-1018163133.htm
[6]	王瑶.纳米流体在储层岩芯表面的铺展及其驱油机理研究[D].西安: 西安石油大学, 2015. http://d.wanfangdata.com.cn/thesis/Y2796652 WANG Yao. A study on nanofluids spreading on the reservoir cores surface and its displacement mechanism[D]. Xian: Xi'an Shiyou University, 2015. http://d.wanfangdata.com.cn/thesis/Y2796652
[7]	CORREDOR R L M, SARAPARDEH A H, HUSEIN M M, DONG P M.Rheological behavior of surface modified silica nanoparticles dispersed in partially hydrolyzed polyacrylamide and xanthan gum solutions:Experimental measurements, mechanistic understanding, and model development[J].Energy Fuels, 2018, 32(10):10628-10638. doi: 10.1021/acs.energyfuels.8b02658
[8]	MOHAMMED B A, KOUROSH R, RADZUAN J, ALI E B.Appraising the impact of metal-oxide nanoparticles on rheological properties of HPAM in different electrolyte solutions for enhanced oil recovery[J]. J Pet Sci Eng, 2019, 172:1057-1068. doi: 10.1016/j.petrol.2018.09.013
[9]	BINKS B P, RODRIGUES J A, FRITH W J. Synergistic interaction in emulsions stabilized by a mixture of silica nanoparticles and cationic surfactant[J]. Langmuir, 2007, 23(14):3626-3636. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=6a1d23b02d38902303096e6876a206f6
[10]	KHALILINEZHAD S S, CHERAGHIAN G, ROAYAEI E, TABATABAEE H, KARAMBEIGI M S. Improving heavy oil recovery in the polymer flooding process by utilizing hydrophilic silica nanoparticles[J]. Energy Source Part A, 2017, 12:1-10. doi: 10.1080/15567249.2014.881931
[11]	SAHA R, UPPALURI R V S, TIWARI P. Silica nanoparticle assisted polymer flooding of heavy crude oil:Emulsification, rheology, and wettability alteration characteristics[J]. Ind Eng Chem Res, 2018, 57:6364-6376. doi: 10.1021/acs.iecr.8b00540
[12]	覃孝平.改性纳米SiO₂/AA/AM共聚物提高波及效率的可行性研究[D].成都: 西南石油大学, 2014. http://cdmd.cnki.com.cn/Article/CDMD-10615-1014419507.htm TAN Xiao-ping. The feasible research of improving sweep efficiency using the modified nano-SiO₂/AA/AM copolymer[D]. Chengdu: Southwest Petroleum University, 2014. http://cdmd.cnki.com.cn/Article/CDMD-10615-1014419507.htm
[13]	郑超.表面改性纳米二氧化硅的制备及其对HPAM驱油性能的影响[D].开封: 河南大学, 2017. http://cdmd.cnki.com.cn/Article/CDMD-10475-1017227144.htm ZHENG Chao.Preparation of surface modified nanosilica and its impact on enhanced oil recovery of HPAM solution[D]. Kaifeng: Henan University, 2017. http://cdmd.cnki.com.cn/Article/CDMD-10475-1017227144.htm
[14]	王海英, HPAM溶液黏度影响因素研究及络合剂的选择[D].大庆: 东北石油大学, 2014. http://cdmd.cnki.com.cn/Article/CDMD-10220-1014384402.htm WANG Hai-ying. Study in the factors that influence HPAM solution viscosity and select the complexing agent[D]. Daqing: Northeastern Petroleum University, 2014. http://cdmd.cnki.com.cn/Article/CDMD-10220-1014384402.htm
[15]	AMIRI A, ØYE G, SJOBLOM J. Influence of pH, high salinity and particle concentration on stability and rheological properties of aqueous suspensions of fumed silica[J]. Colloid Surface A, 2009, 349:43-54. doi: 10.1016/j.colsurfa.2009.07.050
[16]	陈五花, 王业飞, 何臻培, 丁名臣.纳米SiO₂/HPAM/NaCl分散体系的稳定性、流变性及驱油性能研究[J].燃料化学学报, 2020, 48(5):568-576. http://www.ccspublishing.org.cn/article/id/75fab549-3c5c-4c15-9aa9-aaaadaa26470 CHEN Wu-hua, WANG Ye-fei, HE Zhen-pei, DING Ming-chen.Stability, rheology and displacement performance of nano-SiO₂/HPAM/SDS dispersion systems[J]. J Fuel Chem Technol, 2020, 48(5):568-576. http://www.ccspublishing.org.cn/article/id/75fab549-3c5c-4c15-9aa9-aaaadaa26470
[17]	沈钟, 赵振国, 康万利.胶体与表面化学[M].北京:化学工业出版社, 2012, 5. SHEN Zhong, ZHAO Zhen-guo, KANG Wan-li. Colloid and Surface Chemistry[M]. Beijing:Chemical Industry Press, 2012, 5.
[18]	AHUALLI S, IGLESIAS G R, WACHTER W. Adsorption of anionic and cationic surfactants on anionic colloids:Supercharging and destabilization[J]. Langmuir, 2011, 27(15):9182-9192. doi: 10.1021/la201242d
[19]	李慧.莠灭净悬浮剂的制备及其稳定性研究[D].泰安: 山东农业大学, 2012. http://cdmd.cnki.com.cn/Article/CDMD-10434-1012487277.htm LI Hui. Study on the preparation and stability of Ametryne suspension concentrate[D]. Taian: Shandong Agultural University, 2012. http://cdmd.cnki.com.cn/Article/CDMD-10434-1012487277.htm
[20]	彭陈亮, 闵凡飞, 赵晴, 李宏亮.微细矿物颗粒表面水化膜研究现状及进展综述[J].矿物学报, 2012, 32(4):515-522. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=kwxb201204009 PENG Chen-liang, MIN Fan-fei, ZHAO Qing, LI Hong-liang. A review:Research status and process on hydration layers near fine mineral particles[J]. Acta Mineral Sin, 2012, 32(4):515-522. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=kwxb201204009
[21]	张云.分析化学[M].上海:同济大学出版社, 2003, 9. ZHAN Yun. Analytical Chemistry[M]. Shanghai:Tongji University Press, 2003, 9.
[22]	张荣华, 朱志良, 邓守权, 倪亚明. ATMP对钙、镁离子阻垢作用机理的配位化学研究[J].工业水处理, 2003, 23(7):25-27. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=gyscl200307008 ZHANG Rong-hua, ZHU Zhi-liang, DENG Shou-quan, NI Ya-ming. Study on the coordination chemistry of ATMP with Ca²⁺, Mg²⁺ in aqueous solution[J]. Ind Water Treat, 2003, 23(7):25-27. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=gyscl200307008
[23]	李晓阳. Ca(EDTA)^2-络合物及有机酸钙的量化计算研究[D].北京: 中国石油大学(北京), 2016. http://cdmd.cnki.com.cn/Article/CDMD-11414-1018700792.htm LI Xiao-yang. The quantum chemical calculation of Ca(EDTA)^2- complex and organic acid calcium compound[D]. Beijing: China University of Petroleum(Beijing), 2015. http://cdmd.cnki.com.cn/Article/CDMD-11414-1018700792.htm
[24]	孟祥灿.胱氨酸盐型Gemini表面活性剂的合成及驱油性能研究[D].青岛: 中国石油大学(华东), 2013. http://cdmd.cnki.com.cn/Article/CDMD-10425-1015025005.htm MENG Xiang-can. Study on synthesis and oil displacement property of cystine Gemini surfactants[D]. Qingdao: China University of Petroeum(East China), 2013. http://cdmd.cnki.com.cn/Article/CDMD-10425-1015025005.htm
[25]	MAHMOUD M, ATTIA A, AL-HASHIN H. EDTA chelating agent/seawater solution as enhanced oil recovery fluid for sandstone reservoirs[J]. J Pet Sci Eng, 2017, 152:275-283 doi: 10.1016/j.petrol.2017.03.019