CN114686184A - Method for modifying water-based and oil-based drilling fluid by using aza-graphene nanosheets - Google Patents
Method for modifying water-based and oil-based drilling fluid by using aza-graphene nanosheets Download PDFInfo
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Abstract
The invention discloses a method for modifying water-based and oil-based drilling fluid by using aza-graphene nanosheets, wherein the aza-graphene nanosheets with high nitrogen content are prepared into an aqueous solution and then mixed with the existing water-based or oil-based drilling fluid, and the synthesis of the high-nitrogen-content graphene material comprises the following specific preparation steps: s1, adding inorganic salt, performing high-speed ball milling on industrial NaCl or KCl crystal, carbon powder, urea and a metal organic compound, controlling the ball milling feeding mass ratio, ball milling time and ball milling rotation speed of the industrial NaCl or KCl crystal and the carbon powder, realizing the molecular level reconstruction of the NaCl or KCl and raw materials to obtain a carbon source precursor, and preparing the graphene with high nitrogen content by adding the inorganic salt.
Description
Technical Field
The invention relates to the technical field of oil and gas field drilling, in particular to a method for modifying water-based and oil-based drilling fluid by using aza-graphene nanosheets.
Background
The southwest work area of China petrochemical industry is mainly developed by southwest oil and gas companies, mining right areas span provinces and cities such as Sichuan, Chongqing, Yunnan and Guizhou, and drilling construction faces the difficulties of multiple points, wide range, high construction difficulty and the like. The main battlefield of exploration and development after 2018 turns to the Weirong shale gas and the Chuanxi gas field, and the drilling footage ratio of the Weirong shale gas and the Chuanxi gas field is greatly improved. Meanwhile, horizontal wells, ultra-deep wells and edge exploratory wells are increased year by year, the average drilling depth is gradually increased, and the average completed drilling depth is over 4000 meters in 2020.
In 2018-2020, various drilling and completion failures occur together in southwest oil and gas distribution company 48, which mainly comprises drill sticking failures (22 plays, 51.16%), tool failures (6 plays, 13.95%), drilling tool failures (3 plays, 6.98%), overflow failures (3 plays, 6.98%), well cementing failures (3 plays, 6.98%), casing failures (2 plays, 4.65%), well body quality failures (2 plays, 4.65%), well logging failures (1 plays, 2.33%), drill bit failures (1 plays, 2.33%), and drill sticking failures are still the main types of drilling and completion failures. From the time of failure loss, 1465.43d is lost in total due to the failure of the drilling and completion in 2018-2020. Wherein, the loss aging 1043.63d due to the drill sticking fault accounts for 71.22%, the loss aging 57.62d due to the tool fault accounts for 3.93%, the loss aging 32.15d due to the drilling tool fault accounts for 2.19%, the loss aging 90.24d due to the overflow fault accounts for 6.16%, the loss aging 36.07d due to the well cementation fault accounts for 2.46%, the loss aging 127.69d due to the casing fault accounts for 8.71%, the loss aging 43.63d due to the well body quality fault accounts for 2.98%, the loss aging 14.32d due to the logging fault accounts for 0.98%, and the loss aging 20.08d due to the drill bit fault accounts for 1.37%. Stuck-drill failures are the most age-losing failures.
At present, the plugging lubricity of the existing drilling fluid system at home and abroad basically meets the existing drilling needs, but in the drilling process of some new blocks, the problems of instability of the well wall of a lower stratum, later pressure supporting of a horizontal well and the like still exist by using the oil-based drilling fluid, so that the drilling cycle and the well completion cycle are prolonged, and therefore, a new drilling fluid technology is needed to be developed to solve the problems of instability of the well wall of the stratum, pressure supporting of the horizontal well, high friction resistance and the like.
By developing and applying the graphene plugging lubricant for drilling fluid to an oil-based drilling fluid system, the graphene plugging lubricant can be adsorbed to the surface of a well wall and embedded into fine cracks of a stratum to form an ultra-low permeability sealing interlayer, so that the lubricating property of the drilling fluid is improved, the graphene drilling fluid plugging lubricating system applied to a complex stratum is formed, the occurrence of complex drilling accidents is reduced, the accident handling time is prolonged, the cost reduction and the efficiency improvement are realized, and the graphene plugging lubricant has great significance for stable yield in southwest regions and acceleration of gas field development.
The reasonable use of proper nano materials can greatly improve the effects of various chemical working fluids (drilling fluid, well cementing cement paste, fracturing fluid and chemical displacement fluid … for improving the oil field recovery ratio) in the oil field, thereby greatly increasing the yield of oil and gas wells and improving the oil and gas recovery ratio. Bentonite (CN110205104B), montmorillonite (CN107652952A) and the like are used as the materials of the nano additive at present, but the additive has poor compatibility with the drilling fluid due to overlarge particle size. Although the chitosan graphene oxide (CN111808581A) additive is good in compound property, strong oxidants such as sodium periodate are needed in the oxidation process, and the requirement for environmental protection is not facilitated. Particularly in severe downhole environments such as high temperature and high salt, solid lubricants which are not affected by temperature and salt need to be used, and the existing lubricating materials include polymer pellets, glass pellets, ceramic pellets and graphite particles with a lamellar structure. For example, U.S. patent No. 2006/0122070A1 describes spherical graphite as a water-based drilling fluid lubricant, the graphite particles having an average particle size of greater than 120 mesh and greater than 65% of the graphite particles passing through an 80 mesh screen. The patent W02009/035758 describes a solid lubricant suitable for high temperature and high pressure deep and deep horizontal well water-based drilling fluids. The main component of the lubricant is spherical petroleum coke (60-100 meshes), and the lubricant is a byproduct of heavy oil fluidized coking or delayed coking. However, the solid lubricant in the prior art is generally hydrophobic on the surface, difficult to stably disperse in the water-based drilling fluid and easy to agglomerate. Agglomeration can lead to solid lubricant particles being easily screened out by the vibrating screen on the one hand, and can also lead to uneven distribution of lubricant particles in the drilling fluid, thereby impairing the lubricating effect on the other hand.
Disclosure of Invention
Aiming at the defects in the prior art, the invention provides the water-based and oil-based drilling fluid which is suitable for shale formations and has high lubricity and strong plugging property. In particular to a water-based drilling fluid and an oil-based drilling fluid with high lubrication, strong inhibition and strong plugging property suitable for a shale stratum and a preparation method thereof. The high lubricity comes from the interlayer slippage of the graphene nanosheet layer; the strong inhibition blocking property comes from the synergistic effect of the electron adsorption property of the nitrogen-doped graphene material with high nitrogen content and the drilling fluid, and the nitrogen content, the lamella size and the compounding capacity of the nitrogen-doped graphene and the drilling fluid determine the final blocking and lubricating property of the novel drilling fluid, and the strong inhibition blocking property and the high lubricating property are suitable for the requirements of shale gas drilling exploration and development.
The technical purpose is realized by the following technical scheme, the method for modifying the water-based and oil-based drilling fluid by using the aza-graphene nanosheets comprises the steps of preparing a water-based solution by using the aza-graphene nanosheets with high nitrogen content, and mixing the water-based solution with the existing water-based or oil-based drilling fluid, wherein the specific preparation steps for synthesizing the high-nitrogen-content graphene material are as follows:
s1, adding inorganic salt, ball-milling industrial NaCl or KCl crystals, carbon powder, urea and metal organic compounds at a high speed, and controlling the ball-milling feeding mass ratio, ball-milling time and ball-milling rotating speed of the industrial NaCl or KCl crystals and the carbon powder to realize the molecular level reconstruction of the NaCl or KCl and the raw materials to obtain a carbon source precursor;
s2, continuing the pyrolysis reaction, and limiting the escape of molecular nitrogen atoms in the precursor by using a molten salt high-temperature reaction medium to finally realize the synthesis of the high-nitrogen-content graphene material;
the preparation process of the aqueous solution is as follows:
adding the carbon source precursor and the dispersing agent obtained in the step S1 into a stirrer to be premixed with the raw materials; primarily crushing the mixture by a vibration screening machine; then heating and sintering by a nitrogen protection rotary furnace or a belt furnace at 800 ℃; then finely crushing by using a crusher or an airflow crusher, wherein the particle size of the flakes is 7-8 microns; then, adding a 500-liter ball mill for ball milling, wherein the ball mill is a zirconium ball with the diameter of 6.5 mm; then centrifugally separating the slurry by a centrifuge; then drying the mixture at 80 ℃ under the protection of nitrogen after vacuumizing by drying equipment; finally, packaging the powder or aqueous solution slurry for shipment;
and finally, compounding the aza-graphene water-based slurry with the drilling fluid to serve as the added aza-graphene modified water-based or oil-based drilling fluid.
Further, the inorganic salt is one of soluble halide, nitrate, sulfate, sodium salt and potassium salt, and the ratio of the inorganic salt to the carbon source is 1-100%.
Furthermore, the carbon source is one of phthalic anhydride compounds and anhydride compounds.
Further, the nitrogen source is selected from urea and metal organic compounds containing nitrogen atoms.
Furthermore, the roasting temperature of the aza-graphene is 600-900 ℃, the particle size of ball-milled zirconium beads is 3-8 micrometers in the preparation process of the water system slurry, and the ball-milling time is 1-4 hours.
Further, the formula of the water-based drilling fluid is as follows: 3% base slurry + 0.3% potassium + 5% SMP-2+ 5% SPNH + 0.3% PAC-LV + 3% QS-2+ 0.6% polyamine + 5% KCl + to 2.0g/cm 3.
Further, the low-density oil-based drilling fluid comprises the following formula: white oil: the weight of the brine is 80:20, 0.8 percent of main emulsion, 1.5 percent of auxiliary emulsion, 1.0 percent of wetting agent, 3.0 percent of organic soil, 3.0 percent of CaO, 8.0 percent of filtrate reducer, 3.0 percent of plugging agent for drilling fluid and 3 of weight increasing to 1.55 g/cm.
Further, the oil-based drilling fluid is Pengzhou 4-4 well slurry; the formula of the low-density oil-based drilling fluid is a Xiyou Wei formula.
In conclusion, the invention has the following technical effects:
the high melting point characteristic of the inorganic salt enables the salt to fill a reaction space in the preparation process of the aza-graphene, effectively prevents graphene lamellar aggregation and nitrogen atoms from escaping, the high-nitrogen content graphene preparation is achieved through the addition of the inorganic salt, meanwhile, the inorganic salt is consistent with the type of the underground salt, the salt does not need to be removed in the subsequent use process, and the aza-graphene slurry can be directly prepared and mixed with the existing water-based or oil-based drilling fluid for use.
Detailed Description
In the first embodiment, the first step is,
a method for modifying a water-based and oil-based drilling fluid by using aza-graphene nanosheets is characterized in that the aza-graphene nanosheets with high nitrogen content are mixed with the existing water-based or oil-based drilling fluid after being prepared into a water-based solution, wherein the synthesis of the graphene material with high nitrogen content specifically comprises the following steps:
s1, adding inorganic salt, performing high-speed ball milling on industrial NaCl or KCl crystal, carbon powder, urea and a metal organic compound, controlling the ball milling feeding mass ratio, the ball milling time and the ball milling rotating speed of the industrial NaCl or KCl crystal and the carbon powder, realizing the molecular level reconstruction of NaCl or KCl and raw materials, obtaining a carbon source precursor, and finally realizing the synthesis of the high-nitrogen-content graphene material. Compared with cracking without adding salt raw materials, the nitrogen content is improved from 2 percent to 4 percent under the condition of adding inorganic salt into a reaction medium, and the key work is to stabilize the nitrogen atom content to 6 percent.
S2, continuing the pyrolysis reaction, and limiting the escape of molecular nitrogen atoms in the precursor by using a molten salt high-temperature reaction medium to finally realize the synthesis of the high-nitrogen-content graphene material;
the aqueous solution was prepared as follows:
adding the carbon source precursor and the dispersing agent obtained in the step S1 into a stirrer to be premixed with the raw materials; primarily crushing the mixture by a vibration screening machine; then heating and sintering by a nitrogen protection rotary furnace or a belt furnace at 800 ℃; then finely crushing by using a crusher or an airflow crusher, wherein the particle size of the flakes is 7-8 microns; then, adding a 500-liter ball mill for ball milling, wherein the ball mill is a zirconium ball with the diameter of 6.5 mm; then centrifugally separating the slurry by a centrifuge; then drying the mixture at 80 ℃ under the protection of nitrogen after vacuumizing by drying equipment; finally, packaging the powder or aqueous solution slurry for shipment;
and finally, compounding the aza-graphene water-based slurry with the drilling fluid to serve as the added aza-graphene modified water-based or oil-based drilling fluid.
The high-nitrogen-content graphene material mainly comprises pyridine nitrogen, pyrrole nitrogen, graphitized nitrogen and aminated nitrogen, the high-nitrogen content means that the surface atomic content of the whole material is 4-8%, and is different from the low-nitrogen content of 1-3% of the common aza-graphene material, and the field experiment shows that the graphene nitrogen atomic content and the synergistic lubrication plugging efficiency of the drilling fluid are in positive correlation.
The inorganic salt is one of soluble halide, nitrate, sulfate, sodium salt and potassium salt, and the ratio of the inorganic salt to the carbon source is 1-100%.
The carbon source is one of phthalic anhydride compounds and anhydride compounds.
The nitrogen source is selected from urea and metal organic compound containing nitrogen atom.
The preparation roasting temperature of the aza-graphene is 600-900 ℃, the particle size of ball-milled zirconium beads is 3-8 micrometers in the preparation process of the water system slurry, and the ball-milling time is 1-4 hours.
The formula of the water-based drilling fluid comprises: 3% base slurry + 0.3% potassium + 5% SMP-2+ 5% SPNH + 0.3% PAC-LV + 3% QS-2+ 0.6% polyamine + 5% KCl + to 2.0g/cm 3.
The formula of the low-density oil-based drilling fluid comprises: white oil: the weight of the brine is 80:20, 0.8 percent of main emulsion, 1.5 percent of auxiliary emulsion, 1.0 percent of wetting agent, 3.0 percent of organic soil, 3.0 percent of CaO, 8.0 percent of filtrate reducer, 3.0 percent of plugging agent for drilling fluid and 3 of weight increasing to 1.55 g/cm.
The formula of the oil-based drilling fluid is Pengzhou 4-4 well slurry; the formula of the low-density oil-based drilling fluid is a Xiyou Wei formula.
The key technology for preparing the high-nitrogen-content graphene material comes from the fact that inorganic salt compounds are required to be added in the graphene preparation process, the compounds come from underground scenes, and mainly contain halogen salts such as sodium chloride, potassium chloride, calcium chloride, magnesium chloride and the like, and nitrates such as sodium nitrate, potassium nitrate, magnesium nitrate and the like; the carbon source material in the invention is from an environment-friendly acid anhydride or phthalic anhydride compound; the nitrogen source is urea, and the metal organic compound such as phthalocyanine, porphyrin and other nitrogen-containing organic compounds. The key technology for obtaining the high-nitrogen content is that inorganic salt is added in the preparation process, the high-melting-point characteristic of the inorganic salt enables the salt to fill a reaction space in the preparation process of the aza-graphene, so that graphene lamellar aggregation and nitrogen atom escape are effectively prevented, and the high-nitrogen content graphene is prepared by adding the inorganic salt. Meanwhile, because the inorganic salts and the downhole salts are consistent in type, the salts are not required to be removed in the subsequent use process, and the aza-graphene slurry can be directly prepared and mixed with the existing water-based or oil-based drilling fluid for use.
The aza-graphene water-based slurry is compounded with the drilling fluid, and the influence of the added aza-graphene on the performances of the water-based drilling fluid, the oil-based drilling fluid and the low-density drilling fluid is respectively inspected.
(1) Effect of nano-graphene on the Performance of Water-based drilling fluids
Table 1 impact of nano-graphene on drilling fluid conventional performance
And (4) conclusion: description of high-temperature high-pressure dehydrated mud cake: the mud cake is obviously improved, and the mud cake added with the graphene is thinner and more compact.
Table 2 influence of nano graphene on drilling fluid inhibition performance
Table 3 effect of nano graphene on drilling fluid lubricating properties
| Temperature (. degree.C.) | Conditions of the experiment | Pressing and holding type |
| Base pulp | Aging at 130 deg.C for 16h | 0.19435 |
| Base slurry + 0.5% graphene | Aging at 130 deg.C for 16h | 0.17914 |
| Base slurry + 1% graphene | Aging at 130 deg.C for 16h | 0.15379 |
(2) Effect of nano-graphene on oil-based drilling fluid performance
Table 1 impact of nano-graphene on drilling fluid conventional performance
Table 2 effect of nano graphene on drilling fluid lubricating properties
| Temperature (. degree.C.) | Conditions of the experiment | KfPressing and holding type |
| Well slurry | Aging at 150 deg.C for 16h | 0.161 |
| Well slurry + 0.5% graphene | Aging at 150 deg.C for 16h | 0.148 |
| Well slurry + 1% graphene | Aging at 150 deg.C for 16h | 0.0845 |
(3) Performance impact of nano-graphene on low density oil-based drilling fluids
The new formula of the slurry is white oil: the brine (25% CaCl2) was 80:20+ 0.8% primary emulsion + 1.5% secondary emulsion + 1.0% wetting agent + 3.0% organic soil + 3.0% CaO + 8.0% fluid loss additive + 3.0% plugging agent for drilling fluids (FDM-1) + weighted to 1.55g/cm 3.
TABLE 1 influence of nanographene on drilling fluid Performance
In conclusion, due to the high-melting-point characteristic of the inorganic salt, the salt fills the reaction space in the preparation process of the aza-graphene to effectively prevent graphene sheet layer aggregation and nitrogen atoms from escaping, the high-nitrogen content graphene is prepared by adding the inorganic salt, and meanwhile, the inorganic salt is consistent with the underground salt in type, so that the salt is not required to be removed in the subsequent use process, and the aza-graphene slurry can be directly prepared and mixed with the existing water-based or oil-based drilling fluid for use.
The present embodiment is only for explaining the present invention, and it is not limited to the present invention, and those skilled in the art can make modifications of the present embodiment without inventive contribution as needed after reading the present specification, but all of them are protected by patent law within the scope of the claims of the present invention.
Claims (8)
1. A method for modifying a water-based and oil-based drilling fluid by using aza-graphene nanosheets is characterized by comprising the following steps:
the aza-graphene nano-sheet with high nitrogen content is prepared into a water-based solution and then mixed with the existing water-based or oil-based drilling fluid, wherein the synthesis of the high nitrogen-content graphene material comprises the following specific preparation steps:
s1, adding inorganic salt, performing high-speed ball milling on industrial NaCl or KCl crystals, carbon powder, urea and a metal organic compound, and controlling the ball milling feeding mass ratio, the ball milling time and the ball milling rotating speed of the industrial NaCl or KCl crystals and the carbon powder to realize the molecular level reconstruction of the NaCl or KCl and the raw materials to obtain a carbon source precursor;
s2, continuing the pyrolysis reaction, and limiting the escape of molecular nitrogen atoms in the precursor by using a molten salt high-temperature reaction medium to finally realize the synthesis of the high-nitrogen-content graphene material;
the preparation process of the aqueous solution is as follows:
adding the carbon source precursor and the dispersing agent obtained in the step S1 into a stirrer to be premixed with the raw materials; primarily crushing the mixture by a vibration screening machine; then heating and sintering at 800 ℃ by a nitrogen protection rotary furnace or a belt furnace; then finely crushing by using a crusher or an airflow crusher, wherein the particle size of the flakes is 7-8 microns; then, adding a 500-liter ball mill for ball milling, wherein the ball mill is a zirconium ball with the diameter of 6.5 mm; then centrifugally separating the slurry by a centrifuge; then drying the mixture at 80 ℃ under the protection of nitrogen after vacuumizing by drying equipment; finally, packaging the powder or aqueous solution slurry for shipment;
and finally, compounding the aza-graphene water-based slurry with the drilling fluid to serve as the added aza-graphene modified water-based or oil-based drilling fluid.
2. The method of claim 1 for modifying a water-based and oil-based drilling fluid with aza-graphene nanoplatelets, wherein: the inorganic salt is one of soluble halide, nitrate, sulfate, sodium salt and potassium salt, and the ratio of the inorganic salt to the carbon source is 1-100%.
3. The method of claim 1 for modifying a water-based and oil-based drilling fluid with aza-graphene nanoplatelets, wherein: the carbon source is one of phthalic anhydride compounds and anhydride compounds.
4. The method of claim 1 for modifying a water-based and oil-based drilling fluid with aza-graphene nanoplatelets, wherein: the nitrogen source is selected from urea and metal organic compound containing nitrogen atom.
5. The method of claim 1 for modifying a water-based and oil-based drilling fluid with aza-graphene nanoplatelets, wherein: the preparation roasting temperature of the aza-graphene is 600-900 ℃, the particle size of ball-milled zirconium beads is 3-8 micrometers in the preparation process of the water system slurry, and the ball-milling time is 1-4 hours.
6. The method of claim 1 for modifying a water-based and oil-based drilling fluid with aza-graphene nanoplatelets, wherein: the formula of the water-based drilling fluid comprises: 3% base slurry + 0.3% potassium + 5% SMP-2+ 5% SPNH + 0.3% PAC-LV + 3% QS-2+ 0.6% polyamine + 5% KCl + to 2.0g/cm 3.
7. The method of claim 1 for modifying a water-based and oil-based drilling fluid with aza-graphene nanoplatelets, wherein: the formula of the low-density oil-based drilling fluid comprises: white oil: the weight of the brine is 80:20, 0.8 percent of main emulsion, 1.5 percent of auxiliary emulsion, 1.0 percent of wetting agent, 3.0 percent of organic soil, 3.0 percent of CaO, 8.0 percent of filtrate reducer, 3.0 percent of plugging agent for drilling fluid and 3 of weight increasing to 1.55 g/cm.
8. The method of claim 1 for modifying a water-based and oil-based drilling fluid with aza-graphene nanoplatelets, wherein: the formula of the oil-based drilling fluid is Pengzhou 4-4 well slurry; the formula of the low-density oil-based drilling fluid is a Xiyou Wei formula.
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| CN202211254947.6A CN115627157B (en) | 2022-03-24 | 2022-10-13 | Application of high-nitrogen graphene nanosheets in oil-based drilling fluid |
| CN202211254949.5A CN115627158B (en) | 2022-03-24 | 2022-10-13 | Application of high-nitrogen graphene nanosheets in water-based drilling fluid |
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| CN202211254947.6A Active CN115627157B (en) | 2022-03-24 | 2022-10-13 | Application of high-nitrogen graphene nanosheets in oil-based drilling fluid |
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| CN110257128A (en) * | 2019-06-28 | 2019-09-20 | 中国人民解放军空军勤务学院 | Nitrogen-doped graphene/silicon carbide microsphere nano composite material, preparation and application |
| CN113637464B (en) * | 2020-04-27 | 2022-12-09 | 中国石油化工股份有限公司 | Anti-sloughing drilling fluid and preparation method and application thereof |
| CN114015421B (en) * | 2021-12-09 | 2022-12-20 | 西南石油大学 | Preparation method and application of fully-adaptive modified nano-graphene plugging type anti-sloughing drilling fluid |
| CN114214047A (en) * | 2022-01-24 | 2022-03-22 | 西南石油大学 | Outer-soft inner-rigid multi-walled carbon nanotube nano plugging agent and oil-based drilling fluid |
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2022
- 2022-03-24 CN CN202210296033.XA patent/CN114686184A/en active Pending
- 2022-10-13 CN CN202211254947.6A patent/CN115627157B/en active Active
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Also Published As
| Publication number | Publication date |
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| CN115627158B (en) | 2023-07-21 |
| CN115627157B (en) | 2023-07-21 |
| CN115627157A (en) | 2023-01-20 |
| CN115627158A (en) | 2023-01-20 |
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