CN116676078A - Amide type carbon quantum dot reinforced foam system and preparation method and application thereof - Google Patents
Amide type carbon quantum dot reinforced foam system and preparation method and application thereof Download PDFInfo
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- CN116676078A CN116676078A CN202310967133.5A CN202310967133A CN116676078A CN 116676078 A CN116676078 A CN 116676078A CN 202310967133 A CN202310967133 A CN 202310967133A CN 116676078 A CN116676078 A CN 116676078A
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 230
- 239000006260 foam Substances 0.000 title claims abstract description 152
- 150000001408 amides Chemical class 0.000 title claims abstract description 109
- 238000002360 preparation method Methods 0.000 title abstract description 28
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 68
- 239000007788 liquid Substances 0.000 claims abstract description 43
- 239000003945 anionic surfactant Substances 0.000 claims abstract description 28
- 239000007789 gas Substances 0.000 claims abstract description 21
- 238000003756 stirring Methods 0.000 claims description 78
- 239000000243 solution Substances 0.000 claims description 51
- 239000003921 oil Substances 0.000 claims description 49
- 238000000034 method Methods 0.000 claims description 31
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 24
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 23
- 229910017604 nitric acid Inorganic materials 0.000 claims description 23
- 239000006185 dispersion Substances 0.000 claims description 22
- 238000005187 foaming Methods 0.000 claims description 22
- 150000003973 alkyl amines Chemical class 0.000 claims description 21
- 238000001035 drying Methods 0.000 claims description 17
- 238000002156 mixing Methods 0.000 claims description 16
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 15
- 238000000120 microwave digestion Methods 0.000 claims description 15
- 230000033558 biomineral tissue development Effects 0.000 claims description 14
- 150000001875 compounds Chemical class 0.000 claims description 14
- 229910052757 nitrogen Inorganic materials 0.000 claims description 12
- 238000005406 washing Methods 0.000 claims description 12
- 150000004945 aromatic hydrocarbons Chemical class 0.000 claims description 11
- 239000010779 crude oil Substances 0.000 claims description 11
- 239000011259 mixed solution Substances 0.000 claims description 11
- 239000002904 solvent Substances 0.000 claims description 11
- 230000008569 process Effects 0.000 claims description 10
- DBMJMQXJHONAFJ-UHFFFAOYSA-M Sodium laurylsulphate Chemical compound [Na+].CCCCCCCCCCCCOS([O-])(=O)=O DBMJMQXJHONAFJ-UHFFFAOYSA-M 0.000 claims description 9
- 238000001816 cooling Methods 0.000 claims description 7
- 238000010438 heat treatment Methods 0.000 claims description 7
- 239000002245 particle Substances 0.000 claims description 7
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 6
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 6
- 239000008367 deionised water Substances 0.000 claims description 6
- 229910021641 deionized water Inorganic materials 0.000 claims description 6
- 238000009826 distribution Methods 0.000 claims description 6
- 238000011084 recovery Methods 0.000 claims description 6
- 239000011734 sodium Substances 0.000 claims description 6
- 229910052708 sodium Inorganic materials 0.000 claims description 6
- -1 nitrate ions Chemical class 0.000 claims description 5
- 235000011837 pasties Nutrition 0.000 claims description 5
- 229910002651 NO3 Inorganic materials 0.000 claims description 4
- 238000005119 centrifugation Methods 0.000 claims description 4
- 238000006243 chemical reaction Methods 0.000 claims description 4
- 238000004821 distillation Methods 0.000 claims description 4
- 239000005457 ice water Substances 0.000 claims description 4
- AOMUHOFOVNGZAN-UHFFFAOYSA-N N,N-bis(2-hydroxyethyl)dodecanamide Chemical compound CCCCCCCCCCCC(=O)N(CCO)CCO AOMUHOFOVNGZAN-UHFFFAOYSA-N 0.000 claims description 3
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 3
- 239000003570 air Substances 0.000 claims description 3
- 239000012752 auxiliary agent Substances 0.000 claims description 3
- HDMXIELEUKTYFR-UHFFFAOYSA-N bis(2-ethylhexyl) butanedioate;sodium Chemical compound [Na].CCCCC(CC)COC(=O)CCC(=O)OCC(CC)CCCC HDMXIELEUKTYFR-UHFFFAOYSA-N 0.000 claims description 3
- 125000004432 carbon atom Chemical group C* 0.000 claims description 3
- 239000001569 carbon dioxide Substances 0.000 claims description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 claims description 3
- 238000004140 cleaning Methods 0.000 claims description 3
- GVGUFUZHNYFZLC-UHFFFAOYSA-N dodecyl benzenesulfonate;sodium Chemical compound [Na].CCCCCCCCCCCCOS(=O)(=O)C1=CC=CC=C1 GVGUFUZHNYFZLC-UHFFFAOYSA-N 0.000 claims description 3
- 150000002191 fatty alcohols Chemical class 0.000 claims description 3
- 229940031957 lauric acid diethanolamide Drugs 0.000 claims description 3
- 238000004519 manufacturing process Methods 0.000 claims description 3
- 229920000609 methyl cellulose Polymers 0.000 claims description 3
- 239000001923 methylcellulose Substances 0.000 claims description 3
- 239000003345 natural gas Substances 0.000 claims description 3
- 229940051841 polyoxyethylene ether Drugs 0.000 claims description 3
- 229920000056 polyoxyethylene ether Polymers 0.000 claims description 3
- 229940080264 sodium dodecylbenzenesulfonate Drugs 0.000 claims description 3
- DAJSVUQLFFJUSX-UHFFFAOYSA-M sodium;dodecane-1-sulfonate Chemical compound [Na+].CCCCCCCCCCCCS([O-])(=O)=O DAJSVUQLFFJUSX-UHFFFAOYSA-M 0.000 claims description 3
- 238000009210 therapy by ultrasound Methods 0.000 claims description 3
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 3
- 239000012498 ultrapure water Substances 0.000 claims description 3
- 230000000694 effects Effects 0.000 abstract description 19
- 238000011161 development Methods 0.000 abstract description 6
- 238000000926 separation method Methods 0.000 abstract description 3
- 239000007787 solid Substances 0.000 abstract description 2
- 239000010426 asphalt Substances 0.000 description 31
- 239000004094 surface-active agent Substances 0.000 description 26
- 230000000052 comparative effect Effects 0.000 description 18
- 238000001179 sorption measurement Methods 0.000 description 18
- CTQNGGLPUBDAKN-UHFFFAOYSA-N O-Xylene Chemical compound CC1=CC=CC=C1C CTQNGGLPUBDAKN-UHFFFAOYSA-N 0.000 description 13
- 239000010410 layer Substances 0.000 description 13
- 238000006073 displacement reaction Methods 0.000 description 9
- 125000003368 amide group Chemical group 0.000 description 8
- 125000000129 anionic group Chemical group 0.000 description 7
- 230000000087 stabilizing effect Effects 0.000 description 7
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 6
- 239000003795 chemical substances by application Substances 0.000 description 6
- 230000003993 interaction Effects 0.000 description 6
- 239000003208 petroleum Substances 0.000 description 6
- 230000018109 developmental process Effects 0.000 description 5
- 239000012530 fluid Substances 0.000 description 5
- 239000002105 nanoparticle Substances 0.000 description 5
- 230000002028 premature Effects 0.000 description 5
- 239000002994 raw material Substances 0.000 description 5
- BHPQYMZQTOCNFJ-UHFFFAOYSA-N Calcium cation Chemical compound [Ca+2] BHPQYMZQTOCNFJ-UHFFFAOYSA-N 0.000 description 4
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 description 4
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 239000001110 calcium chloride Substances 0.000 description 4
- 229910001628 calcium chloride Inorganic materials 0.000 description 4
- 229910001424 calcium ion Inorganic materials 0.000 description 4
- 229910052799 carbon Inorganic materials 0.000 description 4
- 239000004088 foaming agent Substances 0.000 description 4
- 239000001257 hydrogen Substances 0.000 description 4
- 229910052739 hydrogen Inorganic materials 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 239000012071 phase Substances 0.000 description 4
- 239000000843 powder Substances 0.000 description 4
- 230000002195 synergetic effect Effects 0.000 description 4
- 239000002699 waste material Substances 0.000 description 4
- 239000004215 Carbon black (E152) Substances 0.000 description 3
- 239000003153 chemical reaction reagent Substances 0.000 description 3
- 238000000605 extraction Methods 0.000 description 3
- 125000000524 functional group Chemical group 0.000 description 3
- 229930195733 hydrocarbon Natural products 0.000 description 3
- 150000002430 hydrocarbons Chemical class 0.000 description 3
- 239000007791 liquid phase Substances 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 230000005012 migration Effects 0.000 description 3
- 238000013508 migration Methods 0.000 description 3
- 239000002086 nanomaterial Substances 0.000 description 3
- 239000002135 nanosheet Substances 0.000 description 3
- 229920000642 polymer Polymers 0.000 description 3
- 239000011435 rock Substances 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 2
- 125000002843 carboxylic acid group Chemical group 0.000 description 2
- 230000005284 excitation Effects 0.000 description 2
- 230000002349 favourable effect Effects 0.000 description 2
- 230000015784 hyperosmotic salinity response Effects 0.000 description 2
- 230000001050 lubricating effect Effects 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 239000005543 nano-size silicon particle Substances 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- 229920002401 polyacrylamide Polymers 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 235000012239 silicon dioxide Nutrition 0.000 description 2
- 230000006641 stabilisation Effects 0.000 description 2
- 238000011105 stabilization Methods 0.000 description 2
- 239000003381 stabilizer Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 238000006557 surface reaction Methods 0.000 description 2
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 description 1
- 239000004593 Epoxy Substances 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000011575 calcium Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 239000003245 coal Substances 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- 238000005553 drilling Methods 0.000 description 1
- 238000001962 electrophoresis Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 238000011010 flushing procedure Methods 0.000 description 1
- 239000004872 foam stabilizing agent Substances 0.000 description 1
- 239000008398 formation water Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- 238000012994 industrial processing Methods 0.000 description 1
- 238000011005 laboratory method Methods 0.000 description 1
- 238000002386 leaching Methods 0.000 description 1
- 231100000956 nontoxicity Toxicity 0.000 description 1
- IOQPZZOEVPZRBK-UHFFFAOYSA-N octan-1-amine Chemical compound CCCCCCCCN IOQPZZOEVPZRBK-UHFFFAOYSA-N 0.000 description 1
- 230000020477 pH reduction Effects 0.000 description 1
- 230000035699 permeability Effects 0.000 description 1
- 238000005504 petroleum refining Methods 0.000 description 1
- 238000005424 photoluminescence Methods 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 230000001737 promoting effect Effects 0.000 description 1
- 239000011241 protective layer Substances 0.000 description 1
- 239000004576 sand Substances 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000008399 tap water Substances 0.000 description 1
- 235000020679 tap water Nutrition 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 238000001132 ultrasonic dispersion Methods 0.000 description 1
- 239000000230 xanthan gum Substances 0.000 description 1
- 229920001285 xanthan gum Polymers 0.000 description 1
- 229940082509 xanthan gum Drugs 0.000 description 1
- 235000010493 xanthan gum Nutrition 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/58—Compositions for enhanced recovery methods for obtaining hydrocarbons, i.e. for improving the mobility of the oil, e.g. displacing fluids
- C09K8/594—Compositions used in combination with injected gas, e.g. CO2 orcarbonated gas
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y20/00—Nanooptics, e.g. quantum optics or photonic crystals
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- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/02—Use of particular materials as binders, particle coatings or suspension media therefor
- C09K11/025—Use of particular materials as binders, particle coatings or suspension media therefor non-luminescent particle coatings or suspension media
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- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
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- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/65—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing carbon
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- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/58—Compositions for enhanced recovery methods for obtaining hydrocarbons, i.e. for improving the mobility of the oil, e.g. displacing fluids
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- C09K8/00—Compositions for drilling of boreholes or wells; Compositions for treating boreholes or wells, e.g. for completion or for remedial operations
- C09K8/58—Compositions for enhanced recovery methods for obtaining hydrocarbons, i.e. for improving the mobility of the oil, e.g. displacing fluids
- C09K8/584—Compositions for enhanced recovery methods for obtaining hydrocarbons, i.e. for improving the mobility of the oil, e.g. displacing fluids characterised by the use of specific surfactants
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N21/00—Investigating or analysing materials by the use of optical means, i.e. using sub-millimetre waves, infrared, visible or ultraviolet light
- G01N21/62—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light
- G01N21/63—Systems in which the material investigated is excited whereby it emits light or causes a change in wavelength of the incident light optically excited
- G01N21/64—Fluorescence; Phosphorescence
- G01N21/6428—Measuring fluorescence of fluorescent products of reactions or of fluorochrome labelled reactive substances, e.g. measuring quenching effects, using measuring "optrodes"
- G01N21/643—Measuring fluorescence of fluorescent products of reactions or of fluorochrome labelled reactive substances, e.g. measuring quenching effects, using measuring "optrodes" non-biological material
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- C09K2208/00—Aspects relating to compositions of drilling or well treatment fluids
- C09K2208/10—Nanoparticle-containing well treatment fluids
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Abstract
The application relates to the technical field of oil and gas field development engineering, in particular to an amide type carbon quantum dot reinforced foam system, a preparation method and application thereof, wherein the foam system comprises gas, amide type carbon quantum dots, anionic surfactant and water, the Zeta potential of the amide type carbon quantum dots is 10-25 mV, and the liquid separation half-life of the amide type carbon quantum dot reinforced foam system is 4136s-8160s. The application provides a gas, liquid and solid three-phase foam system, wherein an anionic surfactant and positively charged amide type carbon quantum dots in the three-phase foam system are adsorbed on a gas-liquid interface of foam through electrostatic attraction of charges and the surface activity of the carbon quantum dots, so that a stable sheet layer is formed on a bubble film, the mechanical strength of a foam liquid film can be greatly improved, and the rupture of the liquid film is effectively weakened, so that the foam has good stability.
Description
Technical Field
The application relates to the technical field of oil and gas field development engineering, in particular to an amide type carbon quantum dot reinforced foam system and a preparation method and application thereof.
Background
Foam fluid is applied to oil fields at home and abroad for nearly 60 years. The foam has certain effects in various aspects of oil displacement, drainage gas production of water-containing gas wells, sand flushing, well drilling, profile control, water shutoff, acidification, cement well cementation, fracturing and other oil and gas field development. A large number of practices show that the foam fluid is an important means for protecting hydrocarbon reservoirs, preventing hydrocarbon reservoir pollution and improving hydrocarbon production. Many water flooding developed oil fields in China are in the middle and later stages of oil field development, and residual oil after water flooding exists in each oil field due to high water content and heterogeneity of a reservoir. Because the foam has the characteristics of large and small plugging, water plugging and oil plugging in the stratum, and the like, the surfactant also has the functions of reducing the interfacial tension of oil and water, changing the wettability of rock, and the like as a foaming agent. Therefore, the foam fluid has great significance for further improving the recovery ratio after water flooding.
Foamed fluids are a thermodynamically unstable system, the stability of which is characterized by the half-life of the foam. Existing natural or synthetic, built surfactants have better lathering volumes but generally have shorter half lives. When applied in a subterranean formation, the resulting foam needs to have a longer life to achieve the desired function, and the prior art often has enhanced stability by the addition of suitable foam stabilizers. For example, chinese patent document CN 102977872A (application No. 201210497895.5) discloses an enhanced foam oil displacement agent for enhanced recovery of crude oil by tertiary oil recovery, wherein the water-soluble high molecular polymer is a foam stabilizer, specifically polyacrylamide, partially hydrolyzed polyacrylamide or xanthan gum, the addition of the polymer increases the viscosity of the solution, the liquid drainage speed of the liquid film is reduced to prevent the liquid in the foam from being lost, and the permeability of the liquid film is reduced to prevent the gas in the foam from being diffused, so that the foam stability is enhanced. As the viscosity of the solution increases, more work is consumed to form a gas-liquid interface therein by dispersing the gas, so that under the condition of the same work, the larger the viscosity of the solution, the less the gas-liquid interface is generated, the smaller the foaming volume is, i.e. the foaming capacity of the foam is weakened. And the thickening agent has no foaming capacity, so that the foam viscosity is too high, the foam is difficult to inject into a stratum, and the residual foam stabilizer high polymer after foam displacement can pollute the stratum although the oil displacement agent in the system has a good displacement effect.
In recent years, foam systems reinforced by nanoparticles have also shown better performance. In the 6 th phase of the current chemical industry 2022, an article of the extended field hypotonic reservoir modified surfactant flooding enhanced recovery published by Peng Yi et al mentions the use of silica (SiO 2 ) And Boron Nitride (BN) particles to enhance the stability of the foam, experimental results demonstrate that the nanoparticles have a lower surface tension and a higher elastic modulus in the fluid. The synergistic effect of the surfactant-nanoparticle composition injected into the foam shows that the surfactant-nanoparticle composition enhances the stability of the foam in petroleum and maintains the flowability of the foam for crude oil in porous media. However, the cost of the nano silicon dioxide in the system is high, and the large-scale application of the oil field is difficult to realize.
In order to solve the problem of high cost of nano silicon dioxide, the material field searches for and discovers a novel carbon nano material named as carbon quantum dot, which not only has the characteristics of small size, large specific surface area, photoluminescence and the like of the nano material, but also has the characteristics of no toxicity, good biocompatibility and the like of the carbon material, when the carbon quantum dot is used for preparing an oil displacement agent, the prior art only mixes the carbon quantum dot with a liquid phase to prepare a solid-liquid two-phase oil displacement agent, such as Chinese patent documents CN 113372895A (202110702494.8) and CN 113528107A (202110787537.7), the carbon quantum dot and the liquid phase are mixed to prepare the oil displacement agent, the surfaces of the carbon quantum dot used in the two prior art are all negative potentials, the surfaces of the carbon quantum dot contain rich carboxyl, hydroxyl, epoxy and other functional groups, the good fluorescence characteristic is achieved, the carbon nano material also has good water solubility and certain surface interfacial activity, and the size structure belongs to nano particles. However, compared with the currently used amphiphilic surfactant, the surface interface activity of the amphiphilic surfactant is slightly insufficient, the two patents directly inject the amphiphilic surfactant serving as an oil displacement agent into an oil reservoir, so that the effect of the amphiphilic surfactant cannot be fully exerted, the carrying capacity of injected water is not strong, carbon quantum dots are easy to precipitate in the migration process of a fracture-cave stratum, and the amphiphilic surfactant is difficult to regulate and drive and is spread to a large-scale stratum oil reservoir.
Disclosure of Invention
The application aims to overcome the defects of the prior art, and provides an amide type carbon quantum dot reinforced foam system, a preparation method and application thereof.
In order to achieve the technical effects, the application adopts the following technical scheme:
an amide type carbon quantum dot reinforced foam system comprises gas, amide type carbon quantum dots, anionic surfactant and water,
the Zeta potential of the amide type carbon quantum dot is 10 to 25mV,
the half-life of the solution of the amide type carbon quantum dot reinforced foam system is 4136s-8160s.
The carbon quantum dot presents negative potential when being dissolved in water due to the carboxyl groups on the surface of the carbon quantum dot, so as to improve the surface activity of the carbon quantum dot.
Preferably, the gas is one of nitrogen, carbon dioxide, natural gas or air; the anionic surfactant is at least one of sodium bis (2-ethylhexyl) succinate, sodium dodecyl sulfate, sodium dodecyl sulfonate, sodium dodecyl benzene sulfonate, sodium alpha-alkenyl sulfonate, lauric acid diethanolamide, fatty alcohol polyoxyethylene ether sulfate or sodium methylcellulose.
Preferably, in the amide type carbon quantum dot reinforced foam system, the amide type carbon quantum dot, the anionic surfactant and water form a foam system solution, wherein in the foam system solution, the mass fraction of the amide type carbon quantum dot is 0.1-1.2%, the mass fraction of the anionic surfactant is 0.1-1.0%, and the balance is water; further preferably, the mass fraction of the amide type carbon quantum dots is 0.4-0.6%, the mass fraction of the anionic surfactant is 0.15-0.25%, and the balance is water.
The application also provides a preparation method of the amide type carbon quantum dot reinforced foam system, which comprises the following steps:
s1, adding amide type carbon quantum dots into a dispersing auxiliary, and adding water and stirring to form a uniform mixed solution when the amide type carbon quantum dots are completely dissolved and are pasty;
s2, stirring the mixed solution prepared in the step S1 until the dispersion auxiliary agent volatilizes, and carrying out ultrasonic treatment to obtain uniform and stable carbon quantum dot dispersion liquid;
s3, adding an anionic surfactant into the carbon quantum dot dispersion liquid, and uniformly stirring and mixing to form a compound solution;
s4, stirring and foaming the compound solution in gas to obtain the amide type carbon quantum dot reinforced foam system.
Preferably, in the step S1, the dispersing aid is an alcohol with 1-4 carbon atoms, and the mass ratio of the amide type carbon quantum dots to the dispersing aid is 0.5-1:1.
The dispersing auxiliary has the main function of promoting the dispersion of the amide type carbon quantum dots in the solution, so that the adsorption effect of the amide type carbon quantum dots on a foam gas-liquid interface is enhanced, and the dispersing auxiliary can effectively promote the dispersion of the amide type carbon quantum dots under the mass ratio range.
Preferably, in the step S1, the water is deionized water or mineralized water; further preferably, the mineralized water has a mineralization degree ranging from 1000mg/L to 10000mg/L.
As the amide group amide type carbon quantum dot is positively charged, the anionic surfactant can be protected from the mineralization of formation water by utilizing the electrostatic repulsive interaction, so that the whole system has certain salt tolerance.
Preferably, in the steps S1 and S2, the stirring speed is 1000rpm, and the stirring time is 0.5h-1h; in the step S3, the stirring speed is 600rpm, and the stirring time is 0.5h-1h; in the step S4, the stirring speed is 8000rpm, and the stirring time is 2-7 min.
Preferably, the preparation method of the amide type carbon quantum dot comprises the following steps:
adding carbon quantum dots and alkylamine into an aromatic hydrocarbon solvent, preserving heat and stirring, and obtaining the amide type carbon quantum dots through reduced pressure distillation, centrifugation, washing and drying.
Preferably, the preparation method of the amide type carbon quantum dot specifically comprises the following steps:
a. adding the carbon quantum dots into an aromatic hydrocarbon solvent, stirring for 20-40 min, and uniformly mixing;
b. adding alkylamine under stirring, heating to 130-170 ℃ after adding, and stirring for 4h from timing to obtain an intermediate solution;
c. and (3) distilling the intermediate solution under reduced pressure to remove the aromatic hydrocarbon solvent, centrifuging, washing with water, and drying at 40-50 ℃ to obtain the amide type carbon quantum dots.
Further preferably, the mass ratio of the carbon quantum dots to the alkylamine is 1:1-3; more preferably, the mass ratio of the carbon quantum dots to the alkylamine is 1:1.5-2.5.
Further preferred alkylamines are alkylamines having a chain length of 3 to 8.
Further preferably, in the step a, the stirring time period is 30min; in the step b, heating to 150 ℃; in step c, the drying temperature was 45 ℃.
Further preferably, the ratio relationship of the carbon quantum dots to the aromatic hydrocarbon solvent is 1g:20-80mL; more preferably, the ratio of the carbon quantum dots to the aromatic hydrocarbon solvent is 1g:40-60mL.
The surface of the amide type carbon quantum dot used in the application carries polar amide groups, has larger specific surface area and surface structure, and has strong adsorption capacity on the surfactant. The compounded anionic surfactant-amide carbon quantum dots enable the surfactant molecules of the adsorption layer to be more closely distributed through intermolecular hydrogen bond or dipole moment interaction, so that the viscosity and elasticity of the adsorption layer are increased, the stability of the adsorption film is enhanced, and the foaming and foam stabilizing performances of the surfactant are improved.
Further preferably, in the step a, the preparation method of the carbon quantum dots is as follows:
adding residual oil into concentrated nitric acid for microwave digestion, cooling to room temperature after reaction, centrifuging, cleaning with ultrapure water, and drying to obtain the carbon quantum dots.
More preferably, in the step a, the preparation method of the carbon quantum dots is as follows:
1) Placing part of concentrated nitric acid into ice water bath, and stirring until the temperature is reduced to 2-6 ℃;
2) Adding the hydrotreated residual oil, adding the residual concentrated nitric acid, uniformly mixing, and stirring for 30min from timing to obtain an intermediate solution;
3) And (3) carrying out microwave digestion on the intermediate solution, cooling to room temperature, centrifuging, washing with water until nitrate ions are absent in the solution, and drying at 40-50 ℃ to obtain the carbon quantum dots.
Further preferably, the mass concentration of the concentrated nitric acid is 65%, and the mass ratio of the residual oil to the total concentrated nitric acid is 1 (5-30); the concentrated nitric acid used in step 1) accounts for 85% -95% of the total concentrated nitric acid mass.
Further preferably, in the step 3), the power of microwave digestion is 600W, and the duration of microwave digestion is 10min-30min; more preferably, the microwave digestion period is 25 minutes.
The carbon quantum dots obtained by AFM measurement are mostly concentrated between 1.3nm and 3.7nm, the average thickness of the lamellar is between 0.35nm and 2.10nm, and most of the nano-lamellar contains 1-3 layers. The prepared carbon quantum dot solution shows blue fluorescence under 365nm ultraviolet irradiation.
According to the application, the waste residual oil in the petroleum industry is used as a carbon source to prepare the carbon quantum dots, the raw materials are low in price, the prepared carbon quantum dots have good adaptability to the oil reservoir conditions, can be in continuous contact with residual oil drops in the oil reservoir, have a lubricating effect on the migration of the oil drops, improve the flowability of crude oil, and are favorable for stripping the crude oil from the rock surface. Meanwhile, the carbon quantum dot has rich oxygen-containing functional groups, can be connected with a side chain to perform surface functionalization, has certain surface activity, has good compatibility with a surfactant, and has excellent foaming effect and foam stabilizing effect.
The application also provides an application of the amide type carbon quantum dot reinforced foam system or the amide type carbon quantum dot reinforced foam system prepared by the preparation method,
on one hand, the fluorescent characteristic of the amide type carbon quantum dots is utilized to observe the particle distribution condition in the foam generation process;
another aspect is crude oil recovery in mineralized water areas.
Preferably, the mineralized water has a mineralization degree ranging from 1000mg/L to 10000mg/L.
The foam system provided by the application can be used for foam flooding, and the stable foam system is prepared by using the anionic surfactant and the carbon quantum dots for the first time, the surfactant is adsorbed on a bubble interface liquid film through the synergistic effect of the surfactant and the carbon quantum dots, and a compact layer is formed on the interface through the arrangement of the sheets of the carbon quantum dots, so that the viscoelasticity of the foam liquid film is increased, and the liquid discharge and gas diffusion of the foam are reduced; in addition, the application utilizes the waste residue oil in petroleum industry as raw material to prepare the carbon quantum dots, builds a carbon quantum dot reinforced foam system, reduces the cost, has simple preparation process and ensures that the prepared foam has longer stability. The amide type carbon quantum dots are used as foam stabilizing materials to improve the stability of foam, so that the petroleum industrial processing waste with huge annual output of residual oil can be fully utilized in the technical field of oil and gas field development engineering.
Compared with the prior art, the application has the beneficial effects that:
1. the application provides a gas, liquid and solid three-phase foam system, wherein an anionic surfactant and positively charged amide type carbon quantum dots in the three-phase foam system are adsorbed on a gas-liquid interface of foam through electrostatic attraction of charges and the surface activity of the carbon quantum dots, so that a stable sheet layer is formed on a bubble film, the mechanical strength of a foam liquid film can be greatly improved, and the rupture of the liquid film is effectively weakened, so that the foam has good stability.
2. The amide group carried by the amide type carbon quantum dot prepared by the application belongs to a polar group, and has large specific surface and surface structure, and strong adsorption capacity on the surfactant. The compounded anionic surfactant-amide carbon quantum dots enable the surfactant molecules of the adsorption layer to be more closely distributed through intermolecular hydrogen bonds or dipole moment interactions, so that the viscosity and elasticity of the adsorption layer are increased, the stability of the adsorption film is enhanced, and the foaming and foam stabilizing performances of the surfactant are improved.
3. The amide carbon quantum dot reinforced foam system provided by the application has good salt tolerance, so that tap water or mineralized water with a certain mineralization degree can be used for preparation, and the foam system can be applied to areas with mineralized water such as deserts or beaches for crude oil extraction.
4. In the amide type carbon quantum dot reinforced foam system provided by the application, the amide type carbon quantum dot has fluorescence excitation performance, so that the foam system can be utilized to research the particle distribution condition in foam generation, and a powerful support is provided for the application research of the foam system.
Drawings
FIG. 1 is an AFM scanning image of the amide type carbon quantum dots prepared in example 2;
FIG. 2 is a plot of the height of an AFM scan based on amide type carbon quantum dots prepared in example 2;
fig. 3 is a FITR spectrum of the carbon quantum dots prepared in example 1 and example 2.
Detailed Description
The reagents and experimental equipment used in the examples and comparative examples of the present application are all commercially available conventional reagents and experimental equipment, for example, the residual oil source is residual oil in the petroleum refining process in a petroleum refinery, and the sources and types of other reagents and experimental equipment are not described in detail.
The application provides a preparation method of asphalt-based carbon quantum dots by using residual oil, which comprises the steps of adding residual oil into concentrated nitric acid for microwave digestion, cooling to room temperature after reaction, cleaning with ultrapure water after centrifugation, and drying to obtain the carbon quantum dots; specifically, the preparation method of the asphalt-based carbon quantum dot specifically comprises the following steps:
1) Placing part of concentrated nitric acid into ice water bath, and stirring until the temperature is reduced to 2-6 ℃;
2) Adding the hydrotreated residual oil, adding the residual concentrated nitric acid, uniformly mixing, and stirring for 30min from timing to obtain an intermediate solution;
3) And (3) carrying out microwave digestion on the intermediate solution, cooling to room temperature, centrifuging, washing with water until nitrate ions are absent in the solution, and drying at 40-50 ℃ to obtain the carbon quantum dots.
In the above process, the hydrotreatment of the residuum in step 2) may be carried out using any of the existing hydrotreating modes as desired, such as any of the fixed bed, ebullated bed or suspended bed techniques described in journal literature, current state of application and development of residuum hydrotreating technology (any Wen Po, li Xuejing. Chemical evolution. 2013,32 (5): 1006-1013, 1144), or other existing hydrotreating processes.
Preferably, the mass concentration of the concentrated nitric acid is 65%, and the mass ratio of residual oil to total concentrated nitric acid is 1 (5-30); the concentrated nitric acid used in the step 1) accounts for 85% -95% of the total concentrated nitric acid mass; in the step 3), the microwave digestion power is 600W, and the microwave digestion time is 10-25 min; more preferably, the duration of microwave digestion is 25 minutes.
The carbon quantum dots obtained by AFM measurement are mostly concentrated between 1.3nm and 3.7nm, and mostly contain nano sheets with 1-3 layers, wherein the average thickness of the sheets is between 0.35nm and 2.10 nm. The prepared carbon quantum dot solution shows blue fluorescence under 365nm ultraviolet irradiation.
According to the preparation method, the waste residual oil in the petroleum industry is used as a carbon source to prepare the carbon quantum dots, the raw materials are low in price, the prepared carbon quantum dots are good in condition adaptability to oil reservoirs, can be continuously contacted with residual oil drops in the oil reservoirs, generate a lubricating effect on oil drop migration, improve the flowability of crude oil, and are favorable for stripping the crude oil from the surface of rock. Meanwhile, the carbon quantum dot has rich oxygen-containing functional groups, can be connected with a side chain to perform surface functionalization, has certain surface activity, has good compatibility with a surfactant, and has excellent foaming effect and foam stabilizing effect.
In order to enable the carbon quantum dots to have positive potential and polar groups, the application provides a method for modifying the carbon quantum dots, which comprises the steps of adding the carbon quantum dots and alkylamine into an aromatic hydrocarbon solvent, carrying out heat preservation and stirring, carrying out reduced pressure distillation, centrifuging, washing and drying to obtain the amide type carbon quantum dots, wherein the carbon quantum dots can be coal-based carbon quantum dots, asphalt-based carbon quantum dots and carbon quantum dots prepared from other raw materials.
Specifically, the preparation method of the amide type carbon quantum dot specifically comprises the following steps:
a. adding carbon quantum dots into aromatic hydrocarbon solvent such as xylene, stirring for 20-40 min, and mixing well;
b. adding alkylamine which is alkylamine with chain length of 3-8 under stirring, heating to 130-170 ℃ after the addition is completed, and stirring and reacting for 4 hours from timing to obtain an intermediate solution;
c. and (3) distilling the intermediate solution under reduced pressure to remove dimethylbenzene, centrifuging, washing with water, and drying at 40-50 ℃ to obtain the amide type carbon quantum dots.
In the preparation method of the amide type carbon quantum dots, the mass ratio of the carbon quantum dots to the alkylamine is 1:1-3; preferably, the mass ratio of the carbon quantum dots to the alkylamine is 1:1.5-2.5. In the step a, the stirring time is 30min; in the step b, heating to 150 ℃; in step c, the drying temperature was 45 ℃. The ratio relation of the carbon quantum dots to the dimethylbenzene is 1g:20-80mL; more preferably, the ratio of the carbon quantum dots to the dimethylbenzene is 1g:40-60mL.
The surface of the amide type carbon quantum dot used in the application carries polar amide groups, has larger specific surface area and surface structure, and has strong adsorption capacity on the surfactant. The compounded anionic surfactant-amide carbon quantum dots enable the surfactant molecules of the adsorption layer to be more closely distributed through intermolecular hydrogen bond or dipole moment interaction, so that the viscosity and elasticity of the adsorption layer are increased, the stability of the adsorption film is enhanced, and the foaming and foam stabilizing performances of the surfactant are improved.
Based on the prepared amide type carbon quantum dots, the application provides an amide type carbon quantum dot reinforced foam system which comprises gas, amide type carbon quantum dots, anionic surfactant and water,
the Zeta potential of the amide type carbon quantum dot is 10 to 25mV,
the half-life of the solution of the amide type carbon quantum dot reinforced foam system is 4136s-8160s.
Preferably, in the amide carbon quantum dot reinforced foam system, the foam mass of the foam system is 45% -98%; further preferably, the foam mass of the foam system is 60% -80%. The high foam quality means that the system has higher foaming multiple and strong foaming capacity, the low foam quality can improve the liquid carrying capacity of the system in a high water-containing area, and the system can be applied to different types of oil reservoirs through the foam quality in the range.
Preferably, the gas is one of nitrogen, carbon dioxide, natural gas or air; the anionic surfactant is at least one of sodium bis (2-ethylhexyl) succinate, sodium dodecyl sulfate, sodium dodecyl sulfonate, sodium dodecyl benzene sulfonate, sodium alpha-alkenyl sulfonate, lauric acid diethanolamide, fatty alcohol polyoxyethylene ether sulfate or sodium methylcellulose.
Preferably, in the amide type carbon quantum dot reinforced foam system, the amide type carbon quantum dot, the anionic surfactant and water form a foam system solution, wherein in the foam system solution, the mass fraction of the amide type carbon quantum dot is 0.1-0.9%, the mass fraction of the anionic surfactant is 0.1-1.0%, and the balance is water; further preferably, the mass fraction of the amide type carbon quantum dots is 0.4-0.6%, the mass fraction of the anionic surfactant is 0.15-0.25%, and the balance is water.
The application also provides a preparation method of the amide type carbon quantum dot reinforced foam system, which comprises the following steps:
s1, adding amide type carbon quantum dots into a dispersing auxiliary, and adding water and stirring to form a uniform mixed solution when the amide type carbon quantum dots are completely dissolved and are pasty;
s2, stirring the mixed solution prepared in the step S1 until the dispersion auxiliary agent volatilizes, and carrying out ultrasonic treatment to obtain uniform and stable carbon quantum dot dispersion liquid;
s3, adding an anionic surfactant into the carbon quantum dot dispersion liquid, and uniformly stirring and mixing to form a compound solution;
s4, stirring and foaming the compound solution in gas to obtain the amide type carbon quantum dot reinforced foam system.
Preferably, in the step S1, the dispersing aid is an alcohol with 1-4 carbon atoms, and the mass ratio of the amide type carbon quantum dots to the dispersing aid is 0.5-1:1.
Preferably, in the step S1, the water is deionized water or mineralized water; further preferably, the mineralized water has a mineralization degree ranging from 1000mg/L to 10000mg/L.
Preferably, in the steps S1 and S2, the stirring speed is 1000rpm, and the stirring time is 0.5h-1h; in the step S3, the stirring speed is 600rpm, and the stirring time is 0.5h-1h; in the step S4, the stirring speed is 8000rpm, and the stirring time is 2-7 min.
The application also provides an application of the amide type carbon quantum dot reinforced foam system or the amide type carbon quantum dot reinforced foam system prepared by the preparation method,
on one hand, the fluorescent characteristic of the amide type carbon quantum dots is utilized to observe the particle distribution condition in the foam generation process;
on the other hand, crude oil extraction is carried out in mineralized water areas.
Preferably, the mineralization degree of the mineralized water in the mineralized water area ranges from 1000mg/L to 10000mg/L.
The application will be further described with reference to examples and figures.
Example 1:
in this example, the residual oil is used to prepare the asphalt-based carbon quantum dots, and the preparation method is as follows:
1) Placing 140g of 65% concentrated nitric acid in an ice water bath, and stirring until the temperature is reduced to 4 ℃;
2) Adding 10g of hydrotreated residual oil, adding 14g of concentrated nitric acid, completely leaching the residual oil stuck on the cup wall into the solution, uniformly mixing, and placing the solution on a magnetic stirrer for stirring for 30min from the time of adding to the time of finishing the adding to obtain an intermediate solution;
3) And (3) carrying out microwave digestion on the intermediate solution for 25min at 600W power, cooling to room temperature, centrifuging for multiple times, washing with water until nitrate ions are absent in the solution, and drying at 45 ℃ to obtain the carbon quantum dots.
The asphalt-based carbon quantum dots obtained by AFM measurement are mostly concentrated between 1.3 and 3.7 nm. The average thickness of the lamellar is between 0.35nm and 2.10nm, and most of the lamellar contains nano-lamellar with 1-3 layers. The prepared asphalt-based carbon quantum dot solution shows blue fluorescence under 365nm ultraviolet irradiation.
Example 2:
an amide type carbon quantum dot is prepared by using the asphalt-based carbon quantum dot prepared in the embodiment 1, and the preparation method specifically comprises the following steps:
adding the prepared asphalt-based carbon quantum dots and alkylamine into dimethylbenzene, continuously stirring at 150 ℃, and finally obtaining the amide-based asphalt-based carbon quantum dots through reduced pressure distillation, washing and filtering, wherein the preparation method specifically comprises the following steps of:
a. adding 5g of the prepared asphalt-based carbon quantum dots into a beaker, then adding 10mL of dimethylbenzene, stirring for 30min on a magnetic stirrer, and uniformly mixing;
b. adding 10g of n-octylamine while stirring by a glass rod, gradually heating to 150 ℃ after adding, and stirring on a magnetic stirrer for reaction for 4 hours;
c. and (3) distilling the reacted solution under reduced pressure to remove dimethylbenzene, centrifuging for multiple times in a centrifuge, washing with water, and drying at 45 ℃ to obtain the amide type asphalt-based carbon quantum dots.
As shown in figures 1-2, the surface of the prepared amide type carbon quantum dot carries polar amide groups, has larger specific surface area and surface structure, and has strong adsorption capacity on surfactant. The compounded anionic surfactant-amide carbon quantum dots enable the surfactant molecules of the adsorption layer to be more closely distributed through intermolecular hydrogen bond or dipole moment interaction, so that the viscosity and elasticity of the adsorption layer are increased, the stability of the adsorption film is enhanced, and the foaming and foam stabilizing performances of the surfactant are improved.
As shown in fig. 3, the upper curve is the modified amide-based asphalt-based carbon quantum dot prepared in example 2, and the lower curve is the asphalt-based carbon quantum dot prepared in example 1, and as can be seen from fig. 3, the carboxylic acid groups on the surface of the carbon quantum dot are replaced by amide groups after modification.
To verify the influence of the mass ratio of the carbon quantum dots to the alkylamine in the preparation process of the amide type carbon quantum dots, the amide type carbon quantum dots were prepared according to the mass ratio and the method, except that the mass ratio of the carbon quantum dots to the alkylamine was 1:1 and 1:3, which are respectively used as example 3 and example 4.
For the amide type carbon quantum dots prepared in example 1-example 4, 0.01% wt% of carbon quantum dot dispersion liquid was used to determine the Zeta potential by using a WALLIS Zeta potential electrophoresis apparatus, and the measured potentials were-34.2 mV, 10mV, 22.5mV and 25mV in this order. The carbon quantum dots prepared in example 1 are negative potential, while the amide type carbon quantum dots prepared in examples 2-4 are positive potential, which indicates that the carbon quantum dots have positive polarity and polar amide groups on the surfaces in the modification process.
Examples 2-4 show that the Zeta potential of the carbon quantum dots increases with increasing ratio of alkylamine to carbon quantum dots, indicating that amide groups are reacted to replace carboxylic acid groups on the surface of the carbon quantum dots, and example 4 shows that the Zeta potential increases less than example 2, although the ratio of alkylamine is increased, indicating that the amide group substitution on the carbon quantum dots tends to saturate.
Example 5:
an amide type carbon quantum dot reinforced foam system comprises gas, amide type carbon quantum dots, an anionic surfactant and water, wherein the Zeta potential of the amide type carbon quantum dots is 22.5mV,
the half-life of the liquid separation of the amide type carbon quantum dot reinforced foam system is 5220s;
the gas is nitrogen; the anionic surfactant is sodium dodecyl sulfate.
In the amide type carbon quantum dot reinforced foam system, the amide type carbon quantum dot, the anionic surfactant and water form a foam system solution, in the foam system solution, the mass fraction of the amide type carbon quantum dot is 0.5%, the mass fraction of the anionic surfactant is 0.2%, and the balance is water,
the preparation method of the amide type carbon quantum dot reinforced foam system comprises the following steps:
s1, dissolving 0.5g of amide type asphalt-based carbon quantum dot powder with 1g of ethanol, adding 100ml of deionized water for dissolving when the amide type asphalt-based carbon quantum dot powder is completely dissolved in the ethanol and is pasty, and stirring at 1000rpm to form a uniform mixed solution;
s2, stirring the mixed solution for more than 3 hours, waiting for ethanol to volatilize, and then dispersing by adopting ultrasonic to obtain uniform and stable asphalt-based carbon quantum dot dispersion liquid, wherein the ultrasonic power is 500W and the dispersion time is 2 hours;
s3, adding 0.2g of anionic foaming agent sodium dodecyl sulfate into the asphalt-based carbon quantum dot dispersion liquid, and uniformly mixing at a low speed stirring at 600rpm to form a compound solution; in this step, in order to prevent premature foaming, low-speed stirring is used;
s4, stirring the compound dispersion liquid for 3 minutes at a speed of 8000rpm by using a Waring Blender method, and continuously introducing nitrogen into the tank body in the stirring process to obtain the stable amide carbon quantum dot reinforced foam system.
To verify the effect of the addition concentration of the amide-type carbon quantum dots on the properties of the foam system in the above preparation method, the foam system was prepared according to the above mass ratio and method, except that the addition concentrations of the amide-type pitch-based carbon quantum dots in the liquid phase were 0.1wt% and 1.2wt%, respectively, as examples 6 and 7, respectively.
Example 8:
the application of the amide type carbon quantum dot reinforced foam system is that the fluorescent characteristic of the amide type carbon quantum dot is utilized to observe the particle distribution condition in the foam generation process;
part of the foam in different generation stages is taken and placed under a fluorescence microscope, and the distribution of fluorescent particles on the foam is observed under the excitation and irradiation of 365nm ultraviolet light.
Example 9:
an application of an amide carbon quantum dot reinforced foam system is to carry out crude oil extraction in a mineralized water area;
the mineralization degree of mineralized water in the mineralized water area ranges from 1000mg/L to 10000mg/L.
Comparative example 1:
as a comparative example, it was made from the following components in mass concentration percentage: sodium dodecyl sulfate 0.2%, calcium chloride 0.2% and water up to 100%.
The preparation method of the foam system comprises the following steps:
step 1: adding 100ml of deionized water into 0.2g of anionic foaming agent sodium dodecyl sulfate for dissolution, and uniformly mixing by adopting low-speed stirring at 600rpm to form a compound solution; in this step, in order to prevent premature foaming, low-speed stirring is used;
step 2: adding 0.1g of calcium chloride into the compound solution, and stirring and mixing uniformly at 600rpm to form a uniform mixed solution; in this step, in order to prevent premature foaming, low-speed stirring is used;
step 3: stirring the compound dispersion liquid for 3 minutes at a speed of 8000rpm by using a Waring Blender method, and continuously introducing nitrogen into the tank body during stirring to obtain stable nitrogen foam.
To verify the effect of different mineralizations on the foam system, foam systems were prepared according to the above mass ratios and methods, except that the calcium ion concentrations were 0% and 0.25%, as comparative example 2 and comparative example 3, respectively.
Comparative example 4:
the reinforced foam system based on the synergistic stabilization of the asphalt-based carbon quantum dots is prepared from the following components in percentage by mass: sodium dodecyl sulfate 0.2%, amide type asphalt-based carbon quantum dots 0.2%, calcium chloride 0.1%, and water to 100%.
The preparation method of the enhanced foam system based on the synergistic stabilization of the amide-based asphalt-based carbon quantum dots comprises the following steps:
step 1: firstly, dissolving amide type asphalt-based carbon quantum dot powder by using ethanol, and adding 100ml of deionized water for dissolving and stirring at 1000rpm to form a uniform mixed solution when the amide type asphalt-based carbon quantum dot powder is completely dissolved in the ethanol and is pasty;
step 2: stirring the mixed solution for more than 3 hours, waiting for ethanol to volatilize, and then adopting ultrasonic dispersion to obtain uniform and stable asphalt-based carbon quantum dot dispersion liquid, wherein the ultrasonic power is 500W, and the dispersion is carried out for 2 hours;
step 3: adding 0.2g of anionic foaming agent sodium dodecyl sulfate into the asphalt-based carbon quantum dot dispersion liquid, and uniformly mixing by adopting low-speed stirring at 600rpm to form a compound solution; in this step, in order to prevent premature foaming, low-speed stirring is used;
step 4: adding 0.1g of calcium chloride into the compound solution, and uniformly mixing by adopting low-speed stirring at 600 rpm; in this step, in order to prevent premature foaming, low-speed stirring is used;
step 5: stirring the compound dispersion liquid for 3 minutes at a speed of 8000rpm by using a Waring Blender method, and continuously introducing nitrogen into the tank body during stirring to obtain stable nitrogen foam.
To verify the effect of different mineralizations on the foam system, foam systems were prepared according to the above mass ratios and methods, except that the calcium ion concentration was 0.25%,0.4%, as comparative example 5 and comparative example 6, respectively.
To verify the effect of amide-type carbon quantum dots in a foam system, foam systems were prepared according to the mass ratios and methods of comparative examples 4 to 6, except that the unmodified carbon quantum dots provided in example 1 were used in equal amounts instead of the amide-type carbon quantum dots, respectively as comparative examples 7 to 9.
The raw materials used in the examples and comparative examples are prepared amide type asphalt-based carbon quantum dots, and foamability and stability of the products of each example are evaluated by using a conventional laboratory method Waring Blender method.
100mL of foaming liquid is stirred for 3 minutes at 8000rpm by adopting a Waring Blender method, after stirring is completed, the foam is poured into a 1000mL measuring cylinder, the initial volume of the foam and the time for 50mL of liquid in the foam to be separated out are recorded at normal temperature and normal pressure, and the stability of the foam can be verified.
The composition, foam volume, foam quality and liquid half-life performance data of the foam systems prepared in examples 5-7 and comparative examples 1-9 are shown in Table 1.
TABLE 1 composition, foam volume, foam quality and liquid half-life of foam systems
As shown in the data of table 1, compared with examples 5-7, the comparative example 1 has obviously prolonged liquid separation half-life of the nitrogen foam reinforced by the asphalt-based carbon quantum dots compared with the nitrogen foam without adding the asphalt-based carbon quantum dots, and greatly enhanced foam stability; meanwhile, the addition of the asphalt-based carbon quantum dots has little influence on the foaming volume of the foam, and the reinforced nitrogen foam still has good foaming capacity.
Examples 5-7 show that as the concentration of the pitch-based carbon quantum dots in the foam system increases, the adsorption amount of the pitch-based carbon quantum dots on the foam gas-liquid interface increases, and the foam stability improves.
As can be seen from comparison of comparative examples 4-6 and comparative examples 1-3, the asphalt-based carbon quantum dot reinforced foam system has significantly enhanced calcium ion resistance compared with the foam system without asphalt-based carbon quantum dots, which indicates that the asphalt-based carbon quantum dot reinforced foam system has a certain mineralization resistance. After adding the nano-sheets to the surfactant dispersion, the positively charged nano-sheets are adsorbed on the negatively charged surfactant, and Ca is avoided due to the mutual repulsive interaction of the same charges 2+ The anionic surfactant is influenced, so that a protective layer is formed, the mechanical strength of the foam liquid film is increased, and the foam stability is improved.
Comparison of comparative examples 4-6 and comparative examples 7-9 shows that the unmodified carbon quantum dot reinforced foam also has certain mineralization resistance, but comparison of comparative example data with the same calcium ion concentration shows that the mineralization resistance effect of the unmodified carbon quantum dot is not as good as that of the modified carbon quantum dot reinforced foam.
Claims (10)
1. An amide type carbon quantum dot reinforced foam system is characterized by comprising gas, amide type carbon quantum dots, an anionic surfactant and water,
the Zeta potential of the amide type carbon quantum dot is 10 to 25mV,
the half-life of the solution of the amide type carbon quantum dot reinforced foam system is 4136s-8160s;
the gas is one of nitrogen, carbon dioxide, natural gas or air;
the anionic surfactant is at least one of sodium bis (2-ethylhexyl) succinate, sodium dodecyl sulfate, sodium dodecyl sulfonate, sodium dodecyl benzene sulfonate, sodium alpha-alkenyl sulfonate, lauric acid diethanolamide, fatty alcohol polyoxyethylene ether sulfate or sodium methylcellulose.
2. The amide-type carbon quantum dot reinforced foam system according to claim 1, wherein in the amide-type carbon quantum dot reinforced foam system, the amide-type carbon quantum dot, the anionic surfactant and water form a foam system solution, and in the foam system solution, the mass fraction of the amide-type carbon quantum dot is 0.1% -1.2%, the mass fraction of the anionic surfactant is 0.1% -1.0%, and the balance is water.
3. The amide type carbon quantum dot reinforced foam system according to claim 2, wherein in the foam system solution, the mass fraction of the amide type carbon quantum dots is 0.4-0.6%, the mass fraction of the anionic surfactant is 0.15-0.25%, and the balance is water.
4. A method for preparing the amide type carbon quantum dot reinforced foam system as claimed in any one of claims 1 to 3, comprising the following steps:
s1, adding amide type carbon quantum dots into a dispersing auxiliary, and adding water and stirring to form a uniform mixed solution when the amide type carbon quantum dots are completely dissolved and are pasty;
s2, stirring the mixed solution prepared in the step S1 until the dispersion auxiliary agent volatilizes, and carrying out ultrasonic treatment to obtain uniform and stable carbon quantum dot dispersion liquid;
s3, adding an anionic surfactant into the carbon quantum dot dispersion liquid, and uniformly stirring and mixing to form a compound solution;
s4, stirring and foaming the compound solution in gas to obtain the amide type carbon quantum dot reinforced foam system.
5. The method according to claim 4, wherein in the step S1, the dispersing aid is an alcohol having 1 to 4 carbon atoms, and the mass ratio of the amide type carbon quantum dots to the dispersing aid is 0.5 to 1:1;
in the step S1, the water is deionized water or mineralized water; the mineralization degree of the mineralized water ranges from 1000mg/L to 10000mg/L;
in the steps S1 and S2, the stirring rotation speed is 1000rpm, and the stirring time is 0.5h-1h; in the step S3, the stirring speed is 600rpm, and the stirring time is 0.5h-1h; in the step S4, the stirring speed is 8000rpm, and the stirring time is 2-7 min.
6. The method of claim 4, wherein the method of preparing the amide type carbon quantum dots in step S1 comprises the following steps:
adding carbon quantum dots and alkylamine into an aromatic hydrocarbon solvent, preserving heat and stirring, and obtaining the amide type carbon quantum dots through reduced pressure distillation, centrifugation, washing and drying, wherein the method comprises the following steps:
a. adding the carbon quantum dots into an aromatic hydrocarbon solvent, stirring for 20-40 min, and uniformly mixing;
b. adding alkylamine under stirring, heating to 130-170 ℃ after adding, and stirring for 4h from timing to obtain an intermediate solution;
c. and (3) distilling the intermediate solution under reduced pressure to remove the aromatic hydrocarbon solvent, centrifuging, washing with water, and drying at 40-50 ℃ to obtain the amide type carbon quantum dots.
7. The method according to claim 6, wherein the mass ratio of the carbon quantum dots to the alkylamine is 1:1.5-2.5;
the alkylamine is alkylamine with chain length of 3-8;
in the step a, the stirring time is 30min; in the step b, heating to 150 ℃; in the step c, the drying temperature is 45 ℃;
the ratio relation of the carbon quantum dots to the aromatic hydrocarbon solvent is 1g:20-80mL.
8. The method of claim 6, wherein in step a, the method of preparing the carbon quantum dots comprises:
adding residual oil into concentrated nitric acid for microwave digestion, cooling to room temperature after reaction, cleaning with ultrapure water after centrifugation, and drying to obtain the carbon quantum dots, wherein the method comprises the following steps:
1) Placing part of concentrated nitric acid into ice water bath, and stirring until the temperature is reduced to 2-6 ℃;
2) Adding the hydrotreated residual oil, adding the residual concentrated nitric acid, uniformly mixing, and stirring for 30min from timing to obtain an intermediate solution;
3) Cooling the intermediate solution to room temperature after microwave digestion, centrifuging, washing with water until nitrate ions are absent in the solution, and drying at 40-50 ℃ to obtain the carbon quantum dots;
the mass concentration of the concentrated nitric acid is 65%, and the mass ratio of residual oil to total concentrated nitric acid is 1 (5-30); the concentrated nitric acid used in the step 1) accounts for 85% -95% of the total concentrated nitric acid mass;
in the step 3), the microwave digestion power is 600W, and the microwave digestion time is 10-30 min.
9. The use of the amide type carbon quantum dot reinforced foam system according to any one of claims 1 to 3 or the amide type carbon quantum dot reinforced foam system produced by the production method according to any one of claims 4 to 8,
on one hand, the fluorescent characteristic of the amide type carbon quantum dots is utilized to observe the particle distribution condition in the foam generation process;
another aspect is crude oil recovery in mineralized water areas.
10. The use according to claim 9, wherein the mineralized water has a mineralization degree in the range of 1000mg/L to 10000mg/L.
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