石油储层微通道纳米颗粒吸附法双重减阻机制研究
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摘要
石油储层微通道纳米颗粒吸附法减阻技术是一种降低低渗透油田注水压力的新技术，其对我国低渗透油田的开发具有十分重要的意义。尽管纳米颗粒吸附法减阻技术矿场试验中普遍采用水基分散液，并可以取得显著的减阻效果，但是由于其内在机制尚不清楚，使得这项技术的发展和应用受到严重的制约。本文在此背景下，研究和提出了纳米颗粒吸附法减阻技术中纳米颗粒水基分散液的“力学-化学”双重减阻机制，并设计实验对其进行了较系统的验证。具体工作包括：
1）分析了纳米颗粒水基分散液中微乳液滴在储层微通道中的受力特征，计算了微乳液滴与微通道壁面间的作用能，提出了纳米颗粒水基分散液在储层微通道壁面的双重吸附机制。研究结果表明，纳米颗粒水基分散液在储层微通道壁面具有“表面活性剂-纳米颗粒”双重吸附特征。
2）分析了纳米颗粒水基分散液中表面活性剂在储层微通道壁面的吸附形式，并根据其吸附特征提出了基于表面活性剂作用的化学减阻机理。表面活性剂一方面通过吸附在微通道壁面的纳米颗粒吸附层上或者直接吸附在微通道壁面降低微通道壁面自由能，从而降低水分子与微通道壁面的作用来达到减阻目的；另一方面，水溶液中的表面活性剂胶束通过在微通道壁面附近形成一层“剪切诱导结构”，降低注入水的粘度，从而降低了水流阻力。
3）根据纳米颗粒吸附岩心薄片表面的微结构特征，分析了纳米颗粒吸附岩心薄片表面具有强疏水特征的物理机制。吸附了纳米颗粒后，岩心薄片表面覆盖了一层亚微米级的纳米颗粒团聚体，而每个纳米团聚体又是由若干纳米颗粒单体组成的粗糙结构，因此纳米颗粒吸附岩心薄片表面具有类似荷叶表面的“纳米-亚微米”双重微结构特征，从而体现出强疏水性或超疏水性。由于储层微通道的孔隙及孔喉特征，只有粒径较小的纳米颗粒团聚体和具有正态分布特征的纳米颗粒单体才能够进入微通道，因此，纳米颗粒吸附储层微通道壁面的双重结构特征及疏水性能弱于岩心薄片表面。
4）提出了以综合表面活性剂的化学减阻和以吸附疏水纳米颗粒产生的水流滑移效应的力学减阻为特色的“力学-化学”双重减阻机理：纳米颗粒被水基分散液携带至储层微通道，首先在微通道壁面形成一层纳米颗粒吸附层，随后在其上又吸附了一层亲水基朝外的表面活性剂。在注水初期，主要表现为表面活性剂的化学减阻作用，随着注水过程的进行，纳米颗粒吸附层表面的表面活性剂逐渐被“冲刷”干净，此时，主要表现为以疏水表面的水流滑移效应为主的力学减阻机制。
5）通过岩心薄片吸附实验验证了纳米颗粒水基分散液的双重吸附特征。研究发现，经纳米颗粒水基分散液处理后的岩心薄片表面体现为强亲水性，并且存在一层致密的纳米颗粒吸附层；水流冲刷之后岩心薄片表面的纳米颗粒吸附层依然存在，但表面已逐渐转变为强疏水性，表现出了“表面活性剂-纳米颗粒”的双重吸附特征。
6）通过开展岩心薄片吸附实验、接触角测试以及表面微结构测试，研究了纳米颗粒粒径、纳米颗粒浓度、吸附时间、吸附温度以及酸碱环境等因素对纳米颗粒吸附岩心薄片表面性能的影响规律，为现场工艺参数优选提供了指导。
7）应用MATLAB软件编制了基于径向基函数的支持向量机预测程序，在验证程序正确可用的基础上，将该模型用于纳米颗粒吸附法减阻技术效果的快速评价。结果表明该方法可以实现预测目的，但预测精度依赖于大量样本的补充。
Drag reduction by hydrophobic nanoparticles (HNPs) adsorption in reservoirmicro-channels is a new technology to decrease the injection pressure in lowpermeability oil field, and it is of great importance to enhance the oil recovery rate.Although the water-based HNPs dispersion was widely adopted in field tests andsignificant drag reduction was achieved, the development and deployment of thistechnology is severely constrained due to the lack of a deep understanding of itsmechanisms. The “mechanical-chemical” drag reduction mechanism of water-baseddispersion with HNPs was proposed and validated by a series of experiments. Morespecifically, main achievements are presented as follows.
1) Based on the mechanical characteristics and interaction energy calculation ofmicro-emulsion droplets in reservoir micro-channels, the dual drag reductionmechanism of water-based dispersion with HNPs was proposed. We found thatwater-based dispersion with HNPs has surfactant-HNPs double adsorptioncharacteristics on the wall of reservoir micro-channels.
2) According to the adsorption properties of surfactants, the chemical dragreduction mechanism was investigated. First, surfactants adsorbed either on thesurface of the HNPs adsorption layer or directly on the wall of reservoirmicro-channels weaken the interaction between water molecules, and therefore reducethe drag. Second, surfactants dissolved in water solutions form a layer of“shear-induced structure” near the wall of reservoir micro-channels, which decreasesthe viscosity of the water and reduces the resistance of water flowing through thosemicro-channels.
3) Observations of microstructures of HNPs adsorbed on core slice surfaceprovide the physical or mechanical mechanism of forming a strong hydrophobicsurface. After HNPs adsorption treatment, the core slice surface appears the dual-scalemicro-structure characteristics similar to those of lotus leaves that are superhydrophobic. Such kind of dual-scale micro-structure, because diameters ofHNPs are not equal, surfaces of reservoir micro-channels adsorbed with HNPs alsohave similar dual-scale structure characteristics, and are hydrophobic; which in turnresults in large slip effects.
4) The dominance of chemical or mechanic mechanism of drag reduction ofwater-based dispersion with HNPs was further analyzed for different phases duringwater injection process. During the early phase of water injection, chemicalmechanism of surfactant drag reduction is dominant because of adsorption ofsurfactants. However, as most surfactants are washed away or removed from thesurface after certain period of water injection, the mechanical drag reductionmechanism induced by the slip effect of strong hydrophobic surfaces becomesdominant.
5) The dual drag reduction mechanism of water-based dispersion with HNPs wasverified through a series of experiments. Experimental observations indicate that acompact nano-particle-adsorption layer forms on the surface of the core slice treatedby water-based dispersion with HNPs, and experimental measurements show that thesurface is strong hydrophilic. The HNPs adsorption layer still exists after washing bywater for a while; However, the wettability of the core slice surface becomes stronghydrophobic, indicating that the surfactants adsorbed on the surface of HNPsadsorption layer have been gradually washed away.
6) The impact of some important factors, such as diameter and concentration ofnanoparticles, adsorption temperature, adsorption period and pH level, etc., weresystematically studied through core slices adsorption experiments, contact anglemeasurements and micro-structure imaging. Based on the experimental results, someoperating parameters of field tests were optimized.
7) Support vector machine (SVM) was used to establish a more comprehensiverapid evaluation system. A-SVR（Support Vector Regression） program with RBFkernel function was developed and verified. The method and the program developed can be used to effectively evaluate the drag reduction effects of the HNPs adsorptiontechnology. Our results show that the method is quite promising and the accuracyprediction depends on the size of training data set.
1）分析了纳米颗粒水基分散液中微乳液滴在储层微通道中的受力特征，计算了微乳液滴与微通道壁面间的作用能，提出了纳米颗粒水基分散液在储层微通道壁面的双重吸附机制。研究结果表明，纳米颗粒水基分散液在储层微通道壁面具有“表面活性剂-纳米颗粒”双重吸附特征。
2）分析了纳米颗粒水基分散液中表面活性剂在储层微通道壁面的吸附形式，并根据其吸附特征提出了基于表面活性剂作用的化学减阻机理。表面活性剂一方面通过吸附在微通道壁面的纳米颗粒吸附层上或者直接吸附在微通道壁面降低微通道壁面自由能，从而降低水分子与微通道壁面的作用来达到减阻目的；另一方面，水溶液中的表面活性剂胶束通过在微通道壁面附近形成一层“剪切诱导结构”，降低注入水的粘度，从而降低了水流阻力。
3）根据纳米颗粒吸附岩心薄片表面的微结构特征，分析了纳米颗粒吸附岩心薄片表面具有强疏水特征的物理机制。吸附了纳米颗粒后，岩心薄片表面覆盖了一层亚微米级的纳米颗粒团聚体，而每个纳米团聚体又是由若干纳米颗粒单体组成的粗糙结构，因此纳米颗粒吸附岩心薄片表面具有类似荷叶表面的“纳米-亚微米”双重微结构特征，从而体现出强疏水性或超疏水性。由于储层微通道的孔隙及孔喉特征，只有粒径较小的纳米颗粒团聚体和具有正态分布特征的纳米颗粒单体才能够进入微通道，因此，纳米颗粒吸附储层微通道壁面的双重结构特征及疏水性能弱于岩心薄片表面。
4）提出了以综合表面活性剂的化学减阻和以吸附疏水纳米颗粒产生的水流滑移效应的力学减阻为特色的“力学-化学”双重减阻机理：纳米颗粒被水基分散液携带至储层微通道，首先在微通道壁面形成一层纳米颗粒吸附层，随后在其上又吸附了一层亲水基朝外的表面活性剂。在注水初期，主要表现为表面活性剂的化学减阻作用，随着注水过程的进行，纳米颗粒吸附层表面的表面活性剂逐渐被“冲刷”干净，此时，主要表现为以疏水表面的水流滑移效应为主的力学减阻机制。
5）通过岩心薄片吸附实验验证了纳米颗粒水基分散液的双重吸附特征。研究发现，经纳米颗粒水基分散液处理后的岩心薄片表面体现为强亲水性，并且存在一层致密的纳米颗粒吸附层；水流冲刷之后岩心薄片表面的纳米颗粒吸附层依然存在，但表面已逐渐转变为强疏水性，表现出了“表面活性剂-纳米颗粒”的双重吸附特征。
6）通过开展岩心薄片吸附实验、接触角测试以及表面微结构测试，研究了纳米颗粒粒径、纳米颗粒浓度、吸附时间、吸附温度以及酸碱环境等因素对纳米颗粒吸附岩心薄片表面性能的影响规律，为现场工艺参数优选提供了指导。
7）应用MATLAB软件编制了基于径向基函数的支持向量机预测程序，在验证程序正确可用的基础上，将该模型用于纳米颗粒吸附法减阻技术效果的快速评价。结果表明该方法可以实现预测目的，但预测精度依赖于大量样本的补充。
Drag reduction by hydrophobic nanoparticles (HNPs) adsorption in reservoirmicro-channels is a new technology to decrease the injection pressure in lowpermeability oil field, and it is of great importance to enhance the oil recovery rate.Although the water-based HNPs dispersion was widely adopted in field tests andsignificant drag reduction was achieved, the development and deployment of thistechnology is severely constrained due to the lack of a deep understanding of itsmechanisms. The “mechanical-chemical” drag reduction mechanism of water-baseddispersion with HNPs was proposed and validated by a series of experiments. Morespecifically, main achievements are presented as follows.
1) Based on the mechanical characteristics and interaction energy calculation ofmicro-emulsion droplets in reservoir micro-channels, the dual drag reductionmechanism of water-based dispersion with HNPs was proposed. We found thatwater-based dispersion with HNPs has surfactant-HNPs double adsorptioncharacteristics on the wall of reservoir micro-channels.
2) According to the adsorption properties of surfactants, the chemical dragreduction mechanism was investigated. First, surfactants adsorbed either on thesurface of the HNPs adsorption layer or directly on the wall of reservoirmicro-channels weaken the interaction between water molecules, and therefore reducethe drag. Second, surfactants dissolved in water solutions form a layer of“shear-induced structure” near the wall of reservoir micro-channels, which decreasesthe viscosity of the water and reduces the resistance of water flowing through thosemicro-channels.
3) Observations of microstructures of HNPs adsorbed on core slice surfaceprovide the physical or mechanical mechanism of forming a strong hydrophobicsurface. After HNPs adsorption treatment, the core slice surface appears the dual-scalemicro-structure characteristics similar to those of lotus leaves that are superhydrophobic. Such kind of dual-scale micro-structure, because diameters ofHNPs are not equal, surfaces of reservoir micro-channels adsorbed with HNPs alsohave similar dual-scale structure characteristics, and are hydrophobic; which in turnresults in large slip effects.
4) The dominance of chemical or mechanic mechanism of drag reduction ofwater-based dispersion with HNPs was further analyzed for different phases duringwater injection process. During the early phase of water injection, chemicalmechanism of surfactant drag reduction is dominant because of adsorption ofsurfactants. However, as most surfactants are washed away or removed from thesurface after certain period of water injection, the mechanical drag reductionmechanism induced by the slip effect of strong hydrophobic surfaces becomesdominant.
5) The dual drag reduction mechanism of water-based dispersion with HNPs wasverified through a series of experiments. Experimental observations indicate that acompact nano-particle-adsorption layer forms on the surface of the core slice treatedby water-based dispersion with HNPs, and experimental measurements show that thesurface is strong hydrophilic. The HNPs adsorption layer still exists after washing bywater for a while; However, the wettability of the core slice surface becomes stronghydrophobic, indicating that the surfactants adsorbed on the surface of HNPsadsorption layer have been gradually washed away.
6) The impact of some important factors, such as diameter and concentration ofnanoparticles, adsorption temperature, adsorption period and pH level, etc., weresystematically studied through core slices adsorption experiments, contact anglemeasurements and micro-structure imaging. Based on the experimental results, someoperating parameters of field tests were optimized.
7) Support vector machine (SVM) was used to establish a more comprehensiverapid evaluation system. A-SVR（Support Vector Regression） program with RBFkernel function was developed and verified. The method and the program developed can be used to effectively evaluate the drag reduction effects of the HNPs adsorptiontechnology. Our results show that the method is quite promising and the accuracyprediction depends on the size of training data set.
引文
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