Formulations with fluid loss control properties, methods of making and using the same

Abstract

This invention relates to the field of drilling fluid treatment agents, and discloses a formulation with reduced filtration loss properties, its preparation method, and its application. The method includes: (1) mixing an organic solvent, an oil-phase matrix material, and an organic hydrophilic modifier to carry out a first modification reaction, wherein the oil-phase matrix material is selected from asphalt and / or resin; (2) adding graphene material to the system obtained in step (1) to carry out a second modification reaction. The formulation prepared by this method can not only quickly form an oil film on the wellbore to seal cracks, but can also be widely used in well sections prone to wellbore instability at 60-120℃, while also effectively improving the lubrication performance of drilling fluids.

Description

Technical Field

[0001] This invention relates to the field of drilling fluid treatment agents, specifically to a formulation with reduced filtration loss properties, its preparation method, and its application. Background Technology

[0002] With the acceleration of deep formation drilling and shale oil and gas exploration and development, the formations encountered are becoming increasingly complex, making wellbore instability problems such as collapse, blockage, and stuck pipe more likely, severely restricting the progress of oil and gas exploration and development. Currently, anti-collapse treatment agents mainly utilize their own dimensions to inertly seal formation micro-fractures, improving the sealing ability of drilling fluids and blocking hydration pathways. However, inert sealing materials are limited by their own dimensions, requiring large dosages, sometimes exceeding 10%-20%. Asphalt-based materials are currently the most widely used sealing and anti-collapse materials both domestically and internationally. Representative international asphalt products include Chevron's Soltex series (sodium and potassium asphalt sulfonates), AVA's AVATEX and AVOIL FR / HT asphalt anti-collapse treatment agents, KMC's CONFI-TROL HT PLUS high softening point asphalt, BH DF's CARBO-TROLHT asphalt treatment agent, and Progress's PRO-TEX. Domestically, sodium asphalt sulfonate, emulsified asphalt, multi-softening-point asphalt powder, and natural asphalt powder have also been developed. However, asphalt-based deformable sealing materials are affected by their softening point, limiting their application temperature range to the vicinity of the softening point and resulting in a narrow effective operating temperature range. Therefore, it is often necessary to select and modify or compound asphalts with different softening points. Due to the special manufacturing process of petroleum asphalt and the influence of the production location on natural asphalt, it is difficult to achieve customized production of asphalts with different softening points. Currently available petroleum asphalt, coal tar pitch, and natural asphalt cannot cover all temperature sealing needs. The softening point of petroleum asphalt is mostly in the range of 40-100℃, while the softening point of natural asphalt in Xinjiang, my country, is 90-140℃, and the softening point of coal tar pitch is mainly 80-140℃. Because petroleum asphalt and natural asphalt have strong adhesion, their low-softening-point asphalt products are difficult to make into powder for use. Although coal tar pitch can be processed into powder materials, its adhesion is extremely poor. For temperatures below 120℃, it is difficult to produce powdered asphalt modified materials or the effect is extremely poor (coal tar pitch modification). Although emulsified asphalt can be used to produce liquid asphalt products, it suffers from severe stratification during long-term transportation or in cold weather. Furthermore, due to the limitations of the emulsification process, the asphalt used is mostly ordinary road asphalt with a softening point of 40-60℃, making it unsuitable for the 60-120℃ range. Currently, in shale oil and gas drilling, wellbore instability is most likely to occur in the 80-120℃ range. To address this challenge, it is necessary to develop a formulation with filtration loss reduction properties, along with its preparation method and application. Summary of the Invention

[0003] The purpose of this invention is to overcome the problems of existing technologies, such as the tendency of emulsified asphalt to separate into layers during long-term transportation or in cold weather, and the tendency of wellbore instability to occur in shale oil and gas drilling at 80-120℃. This invention provides a formulation with reduced filtration loss properties, its preparation method, and its application.

[0004] To achieve the above objectives, the first aspect of the present invention provides a method for preparing an agent with reduced filtration loss properties, characterized in that the method comprises:

[0005] (1) A first modification reaction is carried out by mixing an organic solvent, an oil phase matrix material and an organic hydrophilic modifier, wherein the oil phase matrix material is selected from asphalt and / or resin;

[0006] (2) Add graphene material to the system obtained by the reaction in step (1) to carry out the second modification reaction.

[0007] A second aspect of the present invention provides a formulation having filtration loss reduction properties, characterized in that the formulation is prepared by the method described in the first aspect of the present invention.

[0008] The third aspect of the present invention provides the application of the method described in the first aspect of the present invention in improving at least one of the lubrication performance, stability performance and filtration loss reduction performance of drilling fluids and preventing wellbore instability.

[0009] The formulation provided by this invention, based on the above technical solution, uses organic solvents, oil-phase matrix materials, organic hydrophilic modifiers, nanoparticles, and graphene as raw materials, and is prepared through oil-phase dispersion modification and graphene / nanoparticle modification. This formulation can not only rapidly form an oil film on the wellbore to seal fractures, making it widely applicable in well sections prone to wellbore instability at temperatures between 60-120℃, but also effectively improve the lubrication performance of drilling fluids. Detailed Implementation

[0010] The endpoints and any values ​​of the ranges disclosed herein are not limited to the precise ranges or values, and these ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of the various ranges, the endpoint values ​​of the various ranges and individual point values, and individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be considered as specifically disclosed herein.

[0011] To achieve the above objectives, the first aspect of the present invention provides a method for preparing an agent with reduced filtration loss properties, characterized in that the method comprises:

[0012] (1) Mixing an organic solvent, an oil-phase matrix material and an organic hydrophilic modifier to carry out a first modification reaction (surface modification, physical crosslinking), wherein the oil-phase matrix material is selected from asphalt and / or resin;

[0013] (2) Add graphene material to the system obtained by the reaction in step (1) to carry out the second modification reaction.

[0014] In some embodiments of the present invention, preferably, the organic solvent is selected from at least one of liquid hydrocarbon compounds, haloalkanes and liquid alcohols, more preferably from liquid hydrocarbon compounds, and more preferably from at least one of heptane, hexane, octane, gasoline, diesel, white oil, kerosene, solvent oil and naphtha.

[0015] In some embodiments of the present invention, preferably, the oil phase matrix material is selected from at least one of petroleum asphalt, natural asphalt, and resin, more preferably from at least one of 70# petroleum asphalt, 90# petroleum asphalt, 10# petroleum asphalt, Xinjiang Urho natural asphalt, Trinidad and Tobago Lake asphalt, Albanian natural asphalt, Qingchuan natural asphalt, Iranian natural asphalt, and coal tar pitch, polypropylene resin, chlorinated polypropylene resin, petroleum resin, oil-soluble phenolic resin, rosin resin, dammar resin, and terpene resin, more preferably from at least one of 70# petroleum asphalt, 90# petroleum asphalt, 10# petroleum asphalt, Xinjiang Urho natural asphalt, Trinidad and Tobago Lake asphalt, Albanian natural asphalt, C5 petroleum resin, and C9 petroleum resin.

[0016] In some embodiments of the present invention, preferably, the organic hydrophilic modifier includes an organosilicon modifier and / or an organic amine modifier.

[0017] In some embodiments of the present invention, preferably, the organosilicon modifier is selected from at least one substituted silane and / or organosilicon modifier selected from hydrocarbon groups, halogenated hydrocarbon groups, amino hydrocarbon groups, hydrocarbon oxygen groups, and hydrocarbon oxygen-substituted hydrocarbon oxygen groups. More preferably, it is selected from at least one of γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-methacryloyloxypropyltrimethoxysilane, organosilicon modifier, vinyltriethoxysilane, vinyltrimethoxysilane, vinyltri(β-methoxyethoxy)silane, isobutyltriethoxysilane, tridecafluorooctyltrimethoxysilane, aminopropyltrimethoxysilane coupling agent, hexadecyltrimethoxysilane, and γ-chloropropyltrichlorosilane. More preferably, it is selected from at least one of γ-aminopropyltriethoxysilane (KH550), organosilicon modifier, vinyltrimethoxysilane, aminopropyltrimethoxysilane coupling agent, and tridecafluorooctyltrimethoxysilane.

[0018] In some embodiments of the present invention, preferably, the organosilicon modifier is selected from at least one of TEGO270, BYK331, BYK322 and BYK346.

[0019] In some embodiments of the present invention, preferably, the organic amine modifier is selected from alkyl and halogen-substituted quaternary ammonium salts, more preferably selected from at least one of trimethylammonium chloride, trimethylammonium bromide, triethylammonium chloride, triethylammonium bromide, hexadecyltrimethylammonium bromide, hexadecyltrimethylammonium chloride, dodecyl dimethylhydroxyethylammonium chloride, tetradecyl dimethylhydroxyethylammonium chloride, octadecyltrimethylammonium bromide, octadecyltrimethylammonium chloride and n-hexyltrimethylammonium bromide, more preferably selected from at least one of hexadecyltrimethylammonium bromide, hexadecyltrimethylammonium chloride, trimethylammonium bromide, trimethylammonium chloride, octadecyltrimethylammonium bromide, octadecyltrimethylammonium chloride and n-hexyltrimethylammonium bromide.

[0020] In some embodiments of the present invention, preferably, the graphene material is selected from at least one of graphene, graphene oxide, and nitrogen-doped graphene.

[0021] In some embodiments of the present invention, preferably, in step (1), the organic hydrophilic modifier further includes a polyoxyethylene ether modifier.

[0022] In some embodiments of the present invention, preferably, the polyoxyethylene ether modifier is selected from at least one of poly(oxyethylene) hexadecyl ether, dodecylphenol polyoxyethylene ether, nonylphenol polyoxyethylene ether, octylphenol polyoxyethylene ether, sec-octylphenol polyoxyethylene ether, tributylphenol polyoxyethylene ether, styrene-phenol polyoxyethylene ether, sodium octylphenol polyoxyethylene ether allyl succinate diester sulfonate, and allyl polyoxyethylene ether, and more preferably selected from at least one of dodecylphenol polyoxyethylene ether, octylphenol polyoxyethylene ether, styrene-phenol polyoxyethylene ether, and sodium octylphenol polyoxyethylene ether allyl succinate diester sulfonate.

[0023] In some embodiments of the present invention, preferably, in step (1), the materials added to the system also include nanoparticles.

[0024] In some embodiments of the present invention, preferably, the nanoparticles are selected from at least one of nano-calcium carbonate, nano-silica, nano-alumina, nano-titanium oxide, and nano-zinc oxide.

[0025] In some embodiments of the present invention, preferably, the particle size of the nanoparticles is 1-100 nm, more preferably 10-70 nm.

[0026] In this invention, the average particle size of the graphene material can be measured using a laser particle size analyzer.

[0027] In some embodiments of the present invention, preferably, the thickness of the graphene material is 0.3-10 nm, more preferably 0.3-5 nm.

[0028] In this invention, the thickness of the graphene material can be measured using an atomic force microscope.

[0029] In some embodiments of the present invention, preferably, based on parts by weight, relative to 100 parts of organic solvent, the amount of oil-soluble matrix material is 20-500 parts, the amount of organosilicon modifier is 1-20 parts, the amount of organic amine modifier is 1-20 parts, the amount of graphene material is 1-20 parts, the amount of polyoxyethylene ether modifier is 0-20 parts, and the amount of nanoparticles is 0-50 parts.

[0030] In some embodiments of the present invention, preferably, relative to 100 parts of organic solvent, the amount of oil-soluble matrix material is 50-200 parts, the amount of organosilicon modifier is 1-10 parts, the amount of organic amine modifier is 1-10 parts, the amount of graphene material is 1-10 parts, the amount of polyoxyethylene ether modifier is 1-10 parts, and the amount of nanoparticles is 10-30 parts.

[0031] In some embodiments of the present invention, preferably, the temperature of the first modification reaction is 10-120°C, more preferably 20-100°C, and the time is 1-24h, more preferably 4-12h.

[0032] In some embodiments of the present invention, preferably, the temperature of the second modification reaction is 10-120°C, more preferably 20-100°C, and the time is 1-12h, more preferably 2-6h.

[0033] A second aspect of the present invention provides a formulation having filtration loss reduction properties, characterized in that the formulation is prepared by the method described in the first aspect of the present invention.

[0034] In some embodiments of the present invention, preferably, the formulation contains, based on the total weight of the modified oil-soluble matrix material, 0.05-5 wt% silicon, preferably 0.1-3% nitrogen, 0.05-5 wt% nitrogen, preferably 0.1-3 wt% polyoxyethylene ether, and 0-5 wt% polyoxyethylene ether.

[0035] In this invention, the contents of both silicon and nitrogen can be determined by elemental analysis.

[0036] In this invention, the content of the polyoxyethylene ether can be calculated based on the amount of each reactant added.

[0037] The third aspect of the present invention provides the application of the method described in the first aspect of the present invention in improving at least one of the lubrication performance, stability performance and filtration loss reduction performance of drilling fluids and preventing wellbore instability.

[0038] The present invention will be described in detail below through examples. Unless otherwise specified, all raw materials used in the following examples, comparative examples, and test cases are commercially available products.

[0039] Example 1

[0040] 100.0g of 0# diesel oil, 50.0g of Xinjiang Urho natural asphalt, 10.0g of silane coupling agent KH-550, and 10.0g of octadecyltrimethylammonium bromide were added to a 500.0mL three-necked flask. The reaction temperature was controlled at 100℃, and the reaction was carried out for 4 hours. Subsequently, 30.0g of nano-calcium carbonate (average particle size of 20nm) and 10.0g of monolayer graphene were added, and the reaction temperature was controlled at 100℃. The reaction was continued for 2 hours, and finally 210.0g of the formulation was obtained. Elemental analysis showed that the silicon content in the formulation was 1.1wt% and the nitrogen content was 2.6wt%.

[0041] Example 2

[0042] 100.0g of No. 3 white oil, 200.0g of No. 70 petroleum asphalt, 1.0g of TEGO270, and 1.0g of cetyltrimethylammonium bromide were added to a 500.0mL three-necked flask. The reaction temperature was controlled at 20℃, and the reaction was carried out for 12 hours. Subsequently, 10.0g of nano-silica (average particle size of 60nm) and 1.0g of graphene oxide were added, and the reaction temperature was controlled at 20℃, and the reaction was carried out for 6 hours. Finally, 313.0g of the preparation was obtained, in which the silicon content was 3.0wt% and the nitrogen content was 0.1wt%.

[0043] Example 3

[0044] 100.0 g of solvent oil, 100.0 g of Trinidad and Tobago Lake bitumen, 5.0 g of BYK331, and 5.0 g of octadecyltrimethylammonium chloride were added to a 500.0 mL three-necked flask. The reaction temperature was controlled at 80 °C, and the reaction was carried out for 6 h. Subsequently, 20.0 g of nano-titanium dioxide (average particle size of 50 nm) and 5.0 g of nitrogen-doped graphene were added, and the reaction temperature was controlled at 80 °C, and the reaction was carried out for 4 h. Finally, 235.0 g of the formulation was obtained, in which the silicon content was 0.3 wt% and the nitrogen content was 0.5 wt%.

[0045] Example 4

[0046] 100.0 g of solvent oil, 100.0 g of Trinidad and Tobago Lake bitumen, 10.0 g of silane coupling agent KH-550, 5.0 g of dodecylphenol polyoxyethylene ether, and 5.0 g of octadecyltrimethylammonium chloride were added to a 500.0 mL three-necked flask. The reaction temperature was controlled at 80 °C, and the reaction was carried out for 6 h. Subsequently, 20.0 g of nano-silica (average particle size of 30 nm) and 5.0 g of nitrogen-doped graphene were added, and the reaction temperature was controlled at 80 °C, and the reaction was carried out for 4 h. Finally, 235.0 g of the formulation was obtained, in which the silicon content was 1.5 wt%, the nitrogen content was 0.2 wt%, and the polyoxyethylene ether content was 2 wt%.

[0047] Example 5

[0048] The method of Example 3 was followed, except that nano-titanium dioxide was not added, and the amount of nitrogen-doped graphene added was 10g, and the final formulation was obtained.

[0049] Example 6

[0050] The procedure was carried out according to Example 4, except that γ-glycidoxypropyltrimethoxysilane was used instead of BYK331 to obtain the final formulation.

[0051] Example 7

[0052] The method of Example 4 was followed, except that tetradecyl dimethyl hydroxyethyl ammonium chloride was used instead of octadecyl trimethyl ammonium chloride, and the final formulation was obtained.

[0053] Example 8

[0054] The method of Example 4 was followed, except that terbutylphenol polyoxyethylene ether was used instead of dodecylphenol polyoxyethylene ether, and the final formulation was obtained.

[0055] Example 9

[0056] The method was carried out according to Example 3, except that ethanol was used instead of solvent oil to obtain the final formulation.

[0057] Example 10

[0058] The method was carried out according to Example 3, except that coal tar pitch was used instead of Lake Trinidad and Tobago pitch to obtain the final formulation.

[0059] Example 11

[0060] The method of Example 3 was followed, except that the amount of nitrogen-doped graphene was 0.6 g, the amount of BYK331 was 0.3 g, and the amount of octadecyltrimethylammonium chloride was 21.5 g, and the final formulation was obtained.

[0061] Comparative Example 1

[0062] The procedure was carried out according to Example 3, except that BYK331 was replaced with octadecyltrimethylammonium chloride, and the final formulation was obtained.

[0063] Comparative Example 2

[0064] The procedure was carried out according to Example 3, except that octadecyltrimethylammonium chloride was replaced with BYK331, and the final formulation was obtained.

[0065] Comparative Example 3

[0066] The method was carried out according to Example 3, except that graphene was replaced with an oil-phase matrix material to obtain the final formulation.

[0067] Comparative Example 4

[0068] The method of Example 4 was followed, except that BYK331 and octadecyltrimethylammonium chloride were replaced with oil phase matrix materials to finally obtain the formulation.

[0069] Comparative Example 5

[0070] The method of Example 3 was followed, except that the solvent oil was replaced with Trinidad and Tobago Lake bitumen, and the final formulation was obtained.

[0071] Comparative Example 6

[0072] The method was carried out according to Example 3, except that the bitumen from Lake Trinidad and Tobago was replaced with octadecyltrimethylammonium chloride, and the final formulation was obtained.

[0073] Comparative Example 7

[0074] The method was carried out according to Example 3, except that nitrogen-doped graphene and nano-titanium dioxide were added to a three-necked flask along with other materials and reacted at 80°C for 10 hours to finally obtain the formulation.

[0075] Test case

[0076] (1) Evaluation of the performance of temperature-responsive deformation-modulated materials

[0077] First, the formulations, lubricants, and emulsified asphalt prepared in each embodiment and comparative example were added to 5 wt% bentonite slurry that had been pre-hydrated for at least 24 hours. The mixture was stirred at high speed at 10,000 rpm for 20 minutes. The lubrication performance of the collected samples was compared and evaluated according to the test methods specified in the Technical Requirements for Lubricants for Drilling Fluids (Q / CNPC 88-2003). The experimental results of the formulations, lubricants, and emulsified asphalt prepared in each embodiment and comparative example are shown in the table below.

[0078] Table 1

[0079]

[0080]

[0081] As can be seen from the table above, the lubricating properties of the formulation prepared by this invention are slightly better than those of commercially available lubricants and significantly better than those of emulsified asphalt.

[0082] (2) Stability evaluation

[0083] The formulations prepared in each example and comparative example were tested with commercially available emulsified asphalt. The samples were placed in a refrigerator at -15°C for 48 hours, and then removed to observe their condition.

[0084] Table 2. Stability Performance Evaluation of Examples and Comparative Examples

[0085]

[0086]

[0087] As can be seen from the table above, the drilling fluid lubricating forming film sealing material prepared by this invention effectively solves the stability problem of emulsified asphalt products.

[0088] (3) Evaluation of sealing performance

[0089] The formulations prepared in each example and comparative example were tested against commercially available emulsified asphalt and lubricants. The drilling fluid used for testing consisted of 4 wt% prehydrated bentonite slurry (other components being water) + 2 wt% of the test sample. The high-temperature and high-pressure static fluid loss evaluation method was used for evaluation. The test temperatures were 60℃ and 120℃. The high-temperature and high-pressure fluid loss of the sample at 100℃ was determined according to the provisions of 7.2 in GB / T 16783.2. The test results are shown in Table 3.

[0090] Table 3

[0091]

[0092] As can be seen from the table above, the formulation prepared by this invention can quickly form an oil film on the well wall to seal the cracks. Graphene / nanoparticle modification can not only utilize the cross-linking effect of its nano- and micro-scale particles with oil phase solvents and matrix materials to supplement the sealing capacity at the nano- and micro-scale, but also significantly reduce the filtration loss of drilling fluid, thereby blocking the hydration channel and reducing the intrusion of drilling fluid filtrate into the formation.

[0093] As can be seen from the results in Tables 1 to 3, the embodiments using the technical solution of the present invention have beneficial effects such as improving the lubrication performance, stability performance, and filtration loss reduction performance of drilling fluid, and preventing wellbore instability, compared with the comparative examples and the prior art.

[0094] The preferred embodiments of the present invention have been described in detail above; however, the present invention is not limited thereto. Within the scope of the inventive concept, various simple modifications can be made to the technical solutions of the present invention, including combinations of various technical features in any other suitable manner. These simple modifications and combinations should also be considered as the content disclosed in the present invention and are all within the protection scope of the present invention.

Claims

1. A method for preparing a formulation with filtration loss reduction properties, characterized in that, The method includes: (1) A first modification reaction is carried out by mixing an organic solvent, an oil phase matrix material and an organic hydrophilic modifier, wherein the oil phase matrix material is selected from asphalt and / or resin; (2) Add graphene material to the system obtained by the reaction in step (1) to carry out the second modification reaction.

2. The method according to claim 1, wherein, The organic solvent is selected from at least one of liquid hydrocarbon compounds, haloalkanes and liquid alcohols, preferably from liquid hydrocarbon compounds, and more preferably from at least one of heptane, hexane, octane, gasoline, diesel, white oil, kerosene, solvent oil and naphtha.

3. The method according to claim 1 or 2, wherein, The oil phase matrix material is selected from at least one of petroleum asphalt, natural asphalt, and resin, preferably from at least one of 70# petroleum asphalt, 90# petroleum asphalt, 10# petroleum asphalt, Xinjiang Urho natural asphalt, Trinidad and Tobago Lake asphalt, Albanian natural asphalt, Qingchuan natural asphalt, Iranian natural asphalt, and coal tar pitch, polypropylene resin, chlorinated polypropylene resin, petroleum resin, oil-soluble phenolic resin, rosin resin, dammar resin, and terpene resin, preferably from at least one of 70# petroleum asphalt, 90# petroleum asphalt, 10# petroleum asphalt, Xinjiang Urho natural asphalt, Trinidad and Tobago Lake asphalt, Albanian natural asphalt, C5 petroleum resin, and C9 petroleum resin.

4. The method according to any one of claims 1-3, wherein, The organic hydrophilic modifier includes organosilicon modifiers and / or organic amine modifiers; Preferably, the organosilicon modifier is selected from at least one substituted silane and / or organosilicon modifier selected from hydrocarbon groups, halogenated hydrocarbon groups, amino hydrocarbon groups, hydrocarbon oxygen groups, and hydrocarbon oxygen-substituted hydrocarbon oxygen groups. More preferably, it is selected from at least one of γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-methacryloyloxypropyltrimethoxysilane, organosilicon modifier, vinyltriethoxysilane, vinyltrimethoxysilane, vinyltri(β-methoxyethoxy)silane, isobutyltriethoxysilane, tridecafluorooctyltrimethoxysilane, aminopropyltrimethoxysilane coupling agent, hexadecyltrimethoxysilane, and γ-chloropropyltrichlorosilane. More preferably, it is selected from at least one of γ-aminopropyltriethoxysilane, organosilicon modifier, vinyltrimethoxysilane, aminopropyltrimethoxysilane coupling agent, and tridecafluorooctyltrimethoxysilane. Preferably, the organic amine modifier is selected from alkyl and halogen-substituted quaternary ammonium salts, more preferably from at least one of trimethylammonium chloride, trimethylammonium bromide, triethylammonium chloride, triethylammonium bromide, hexadecyltrimethylammonium bromide, hexadecyltrimethylammonium chloride, dodecyl dimethylhydroxyethylammonium chloride, tetradecyl dimethylhydroxyethylammonium chloride, octadecyltrimethylammonium bromide, octadecyltrimethylammonium chloride and n-hexyltrimethylammonium bromide, and even more preferably from at least one of hexadecyltrimethylammonium bromide, hexadecyltrimethylammonium chloride, trimethylammonium bromide, trimethylammonium chloride, octadecyltrimethylammonium bromide, octadecyltrimethylammonium chloride and n-hexyltrimethylammonium bromide.

5. The method according to any one of claims 1-4, wherein, The graphene material is selected from at least one of graphene, graphene oxide, and nitrogen-doped graphene.

6. The method according to any one of claims 1-5, wherein, In step (1), the organic hydrophilic modifier further includes a polyoxyethylene ether modifier; Preferably, the polyoxyethylene ether modifier is selected from at least one of poly(oxyethylene) hexadecyl ether, dodecylphenol polyoxyethylene ether, nonylphenol polyoxyethylene ether, octylphenol polyoxyethylene ether, sec-octylphenol polyoxyethylene ether, tributylphenol polyoxyethylene ether, styrene-phenol polyoxyethylene ether, sodium octylphenol polyoxyethylene ether allyl succinate diester sulfonate, and allyl polyoxyethylene ether, and more preferably from at least one of dodecylphenol polyoxyethylene ether, octylphenol polyoxyethylene ether, styrene-phenol polyoxyethylene ether, and sodium octylphenol polyoxyethylene ether allyl succinate diester sulfonate.

7. The method according to any one of claims 1-6, wherein, In step (1), the materials added to the system also include nanoparticles; Preferably, the nanoparticles are selected from at least one of nano-calcium carbonate, nano-silica, nano-alumina, nano-titanium oxide, and nano-zinc oxide; Preferably, the nanoparticles have a particle size of 1-100 nm, more preferably 10-70 nm; And / or, the thickness of the graphene material is 0.3-10 nm, preferably 0.3-5 nm.

8. The method according to any one of claims 1-7, wherein, By weight, relative to 100 parts of organic solvent, the amount of oil-soluble matrix material is 20-500 parts, the amount of organic hydrophilic modifier is 1-20 parts, the amount of graphene material is 1-20 parts, the amount of polyoxyethylene ether modifier is 0-20 parts, and the amount of nanoparticles is 0-50 parts. Preferably, relative to 100 parts of organic solvent, the amount of oil-soluble matrix material is 50-200 parts, the amount of organosilicon hydrophilic modifier is 1-10 parts, the amount of graphene material is 1-10 parts, the amount of polyoxyethylene ether modifier is 1-10 parts, and the amount of nanoparticles is 10-30 parts.

9. The method according to any one of claims 1-8, wherein, The temperature of the first modification reaction is 10-120℃, preferably 20-100℃, and the time is 1-24h, preferably 4-12h; Preferably, the temperature of the second modification reaction is 10-120℃, more preferably 20-100℃, and the time is 1-12h, more preferably 2-6h.

10. A formulation having the property of reducing filtration loss, characterized in that, The formulation is prepared by the method described in any one of claims 1-9.

11. The application of the method according to any one of claims 1-9 in improving at least one of the lubrication performance, stability performance and filtration loss reduction performance of drilling fluid and preventing wellbore instability.

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