Preparation and Performance Evaluations of an Ultra-low Permeability Film-Forming Agent Based on Graphene Modification
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摘要: 为阻止钻井液滤液进入地层，维持井壁稳定、保护储层，采用改进的Hummers方法对石墨烯表面进行活化处理，引入羧基、羟基、环氧基等活性基团，与优选的单体在活化石墨烯表面接枝聚合，制备了一种基于石墨烯修饰的超低渗透成膜剂SMSL。采用红外光谱仪、元素分析仪、原子力显微镜、同步热分析仪等分析了超低渗透成膜剂SMSL的分子结构、微观形貌特征及其分散状态。采用压力传递试验、岩石自渗吸试验和电镜扫描等评价了超低渗透成膜剂SMS的致密成膜封堵特性，并评价了超低渗透成膜剂SMSL与水基钻井液的配伍性。评价结果表明，超低渗透成膜剂SMSL的分子结构达到了设计要求，可显著降低岩石的压力传递及自渗吸作用，与高效聚合物成膜剂相比其页岩成膜效率提高162.96%，致密砂岩自渗吸能力降低88.74%，与水基钻井液的配伍性较好。研究结果表明，钻井液中加入超低渗透成膜剂SMSL，可在井壁上形成致密膜，能够阻止钻井液滤液进入地层，维持井壁稳定和保护储层。Abstract: In order to prevent the drilling fluid filtrate from entering the formation, to maintain the wellbore stability and to protect the reservoir, a procedure to activate a graphene surface was conducted by using a modified Hummers method. It introduced carboxyl, hydroxyl, epoxy groups and other active groups, resulting in a kind of graphene modified film-forming agent SMSL with ultra-low permeability. It was prepared by grafting copolymerization with selected monomers on the surface of active graphene. The molecular structure, micro morphology and dispersive state of SMSL were analyzed by the infrared spectrometer, the element analyzer, the atomic force microscope and the synchronous thermal analyzer. Researchers used pressure transfer tests, core self-seepage tests and SEM to evaluate the dense film-forming plugging characteristics of SMSL and the compatibility of SMSL with the water-based drilling fluid. The results showed that the molecular structure of SMSL met the design requirements, and it could significantly reduce the pressure transfer and self-seepage effect of rocks. Specifically, the shale film-forming efficiency was 162.96% higher than that of the conventional polymer film-forming agent, the self-seepage capacity of tight sandstone was decreased by 88.74%, with very good compatibility with the water-based drilling fluid. The research indicated that when SMSL was added into the drilling fluid, a dense film can form on the wellbore to prevent the filtrate from entering the formation and thus can maintain wellbore stability and protect the reservoir.
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Keywords:
- ultra-low permeability /
- film-forming agent /
- graphene /
- plugging /
- drilling fluid
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图 2 活化石墨烯和超低渗透成膜剂SMSL的红外光谱
Figure 2. Infrared spectrum of active graphene and film-forming agent SMSL with ultra-low permeability
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图 3 活化石墨烯的原子力显微镜观察结果
Figure 3. Observation result by atom force microscope(AFM) of active graphene
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图 7 岩心自发渗吸装置示意
1.可动钢化玻璃板；2.天平挂钩；3.天平托盘；4.精密电子天平；5.防风罩；6.数据传输线；7.计算机数据接收装置；9.试液容器；8.精密升降台；10.岩心夹持器
Figure 7. Schematic diagram of a device for a core self-seepage test
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图 9 环境扫描电镜观测的SMSL在API滤失滤饼中的存在形态
Figure 9. The morphology of SMSL in API filter cake observed by environmental SEM
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图 10 扫描电镜观测的页岩封堵端面的微观形貌特征
Figure 10. The micro-morphological characteristics of shale plugging surface observed by SEM
表 1 页岩在不同流体下的渗透率和膜效率
Table 1 Permeability and membrane efficiency of shale under different fluids
测试流体 渗透率/10–4mD 膜效率 4%NaCl水溶液 3.720 0.074 4%NaCl + 2%LSF 0.756 0.108 4%NaCl + 2%SMNF 0.486 0.167 4%NaCl + 2%SMSL 0.302 0.284 4%NaCl + 2%SMSL + 2%SMNF 0.035 0.392 
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表 2 钻井液性能测试结果
Table 2 Test results of drilling fluid properties
密度/（kg·L–1） 条件 表观黏度/（mPa·s） 塑性黏度/（mPa·s） 动切力/Pa 静切力/Pa API滤失量/mL 高温高压滤失量/mL 1.8 加入前 38.0 26.0 12.0 2.5/5.5 4.0 10.4 加入后 35.0 23.0 12.0 2.5/5.0 3.2 8.2 2.0 加入前 36.0 26.0 13.0 3.0/5.5 3.8 9.6 加入后 36.0 24.0 12.0 2.5/6.0 2.8 8.0 2.2 加入前 42.0 29.0 13.0 4.0/7.5 3.8 10.0 加入后 44.0 29.0 15.0 3.5/7.0 2.6 7.4
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