CN107063935B - A kind of measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase - Google Patents
A kind of measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase Download PDFInfo
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N13/00—Investigating surface or boundary effects, e.g. wetting power; Investigating diffusion effects; Analysing materials by determining surface, boundary, or diffusion effects
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N13/00—Investigating surface or boundary effects, e.g. wetting power; Investigating diffusion effects; Analysing materials by determining surface, boundary, or diffusion effects
- G01N2013/003—Diffusion; diffusivity between liquids
Abstract
The present invention relates to a kind of measurement CO2Single liquid phase drop of pressure method is combined by diffusion process and the method for diffusion coefficient between water-oil phase, this method with Two Liquid Phases extension Modeling The Concentration Profiles, the CO measured according to drop of pressure method2Diffusion coefficient in single liquid phase can directly obtain CO by extending Modeling The Concentration Profiles2Concentration distribution in two liquid phases, and then obtain CO2Diffusion coefficient between water-oil phase.Present method avoids directly measure CO2Pressure when being spread to Two Liquid Phases improves computational accuracy when subsequent experimental data processing, and operation is more succinct；Meanwhile method of the invention is more in line with the diffusion characteristic under high temperature and pressure, avoids and there are problems that pressure fluctuation under conditions of Two Liquid Phases diffusion pressure drop is smaller so that result of calculation is more in line with the actual conditions spread under high temperature and pressure.
Description
Technical field
The present invention relates to a kind of measurement CO2Diffusion process and the method for diffusion coefficient, belong to oil gas field between water-oil phase
The technical field of Development Engineering.
Background technology
In recent years, global demand of petroleum increases rapidly, and oil-gas exploration and development object is increasingly sophisticated, and reserves are sampled increasingly
Difference.The nontraditional reservoirs such as heavy crude reservoir, hyposmosis compact oil reservoir will be as the important object of oil and gas development from now on.In unconventional oil
In the numerous development schemes hidden, CO is noted2Production technique is due to its economical and efficient and meets wanting for reduction greenhouse gas emission instantly
It asks and is widely used.
Note CO2Production technique includes mainly CO2It drives, CO2It handles up and CO2Water-air two-phase flow drive etc..In the application of these technologies
In the process, the CO of injection2Three-phase system, CO can be formed with water flooding, injection water and crude oil2It can be in single liquid phase and oil
It is diffused mass transfer between water two-phase.CO2Diffusion can reduce oil water interfacial tension, viscosity of crude and enable to
Crude oil expands, to be conducive to the extraction of oil reservoir Crude Oil.For CO2Diffusion in three-phase system is studied, and is had
Help predict CO2Swept volume in oil reservoir improves nontraditional reservoir ultimate recovery and finally realizes high-efficiency mining.Cause
This, measures CO2Diffusion process and diffusion coefficient between water-oil phase is for applying CO2Technique to high-efficiency develops oil reservoir meaning weight
Greatly.
Currently, measuring CO2The method of diffusion coefficient in oil phase or water phase is mostly improved drop of pressure method, with
《Journal of Petroleum Science and Engineering》25 phases in 2005 in periodical《Measurement
of gas diffusivity in heavy oils》The method mentioned in one text is more mature.The method is surveyed due to only needing
Determine the pressure change in diffusion process, need not directly measure the concentration in diffusion process, measurement is efficient and convenient, to extensive
Using.However, such method can only be used as measuring CO2Diffusion coefficient when being spread to single liquid phase is not suitable for measuring CO2To two
Diffusion coefficient when alternate diffusion, if by such method for measuring CO2When diffusion process between water-oil phase, CO2In list
The amount for the substance for diffusing into another liquid phase in the time of position is smaller, causes pressure drop smaller, and conventional pressure manometers are difficult to accurately capture,
The continuous mode duration is longer and balances pressure and is difficult to determine.In addition, the CO under high temperature and pressure2Not in above-critical state and pole
Stablize, causes the pressure measured in experimentation big ups and downs occur so that pressure curve is difficult to accurately obtain.
Chinese patent literature CN104237079A discloses a kind of measurement CO2The experimental method and dress of diffusion coefficient in water
It sets.Experimental provision includes mainly data collecting system, constant-temperature heating system, pH meter probe, diffusion using fixed diffusion length
Kettle, pressure sensor, temp probe etc., pH meter probe are mounted on the bottom end cover of diffusion kettle, and pressure sensor is mounted on upper end cover,
Heating coil outside temp probe one end connection diffusion kettle, the other end are connect with constant-temperature heating system.It is carried out in spreading kettle real
When testing, diffusion kettle it is mounted on bearings, rotation diffusion kettle simulate tilted stratum, according to The Ideal-Gas Equation using pressure come
Calculate CO2Initial concentration, according to data collecting system acquisition pH value calculate CO2Amount of hydrolysis, draw CO2Amount of hydrolysis with
Time subduplicate matched curve, obtains slope k, and diffusion coefficient D is acquired according to computation model, which only measures
CO2Diffusion coefficient in water can not measure the diffusion coefficient between water-oil phase.
Chinese patent literature CN104502236A discloses a kind of measurement CO2System is spread into oil phase diffusion process from water phase
The method of number and equilibrium concentration.U-tube bottom aqueous phase is saturated CO by this method2, form saturated carbon sour water, the injection of U-tube upper end
CO2, crude oil is injected in lower end, according to improved PVT pressure decline methods, by measuring CO2Pressure becomes caused by being spread to saturated carbon sour water
Change, CO can be found out in conjunction with drop formula2CO after diffusion coefficient from water phase to oil phase and balance when being spread from2In crude oil
Equilibrium concentration.CO can be only determined by experiment in this method2From pressure change of the water phase into oil phase diffusion process, but experiment obtains
The falloff curve fluctuation obtained is larger, brings great error to the processing of subsequent experimental result, and measurement process is complicated.
Therefore, how simple and fast method test CO is utilized2Diffusion process and diffusion coefficient become between water-oil phase
There is technical problem to be solved at present.
Invention content
In view of the shortcomings of the prior art, the present invention provides a kind of measurement CO2Diffusion process and diffusion coefficient between water-oil phase
Method.
Summary of the invention：
The Two Liquid Phases of widely applied single liquid phase drop of pressure method and the present invention are extended concentration by the measurement method of the present invention
Distributed model is combined, the CO measured respectively according to drop of pressure method2Diffusion coefficient into single liquid phase, by extending concentration point
Cloth model can directly obtain CO2Concentration distribution in two liquid phases, and then acquire CO2Diffusion coefficient between water-oil phase.
This method avoid directly measure CO2Pressure when being spread to Two Liquid Phases improves calculating essence when subsequent experimental data processing
Degree；Meanwhile this method is more in line with the diffusion characteristic under high temperature and pressure, avoids and drops smaller condition in Two Liquid Phases diffusion pressure
Under there are problems that pressure fluctuation so that result of calculation is more in line with the actual conditions spread under high temperature and pressure.
Technical scheme is as follows：
A kind of measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase, including steps are as follows：
(1) CO for using drop of pressure method to measure respectively2To the diffusion coefficient D of water phase1And CO2To the diffusion coefficient of oil phase
D2；
(2) it according to Fick's law, uses formula 2. to test out diffusion coefficient D and is advised for the concentration distribution of the one-dimensional diffusion of constant
Rule：
Formula 2. in, C CO2Concentration in the liquid phase, mol/m3；T is diffusion time, s；A is the normal of the amount determination of substance
Number；X is the distance to liquid phase surface, m.
(3) concentration C integrates x, and setsIt is 3. diffused into according to formula
The amount for entering the total material of liquid phase is：
(4) 2. 3. formula that formula is transformed to constant A substitutes into formula, obtain formula 4.：
(5) it is 4. write formula as integrated form, obtains formula
(6) standard error function is formula
Using standard error function by formulaIt indicates, obtains formula
FormulaIn, C0For CO under experiment condition2Maximum meltage in current liquid phase, mol/m3；
(7) use formula 5., 6. model obtains CO to formula2Concentration distribution in oil phase, water phase：
Formula 5. in, C1It is t moment in water phase away from CO at liquid level x position2Concentration, mol/m3；x1For the lower boundary position of water phase
It sets, m；Formula 6. in, C2It is t moment in oil phase away from CO at liquid level x position2Concentration, mol/m3；x2For the lower boundary position of oil phase 2,
m；
The concentration distribution of t moment integrates x, t moment is 7. obtained according to formula and diffuses into CO in two kinds of liquid phases2
The amount n of total material：
(8) 8. formula is obtained by state equation：
Formula 8. in, P1To spread initial pressure, Pa；P2Pressure when being carried out to t moment for diffusion, Pa；V is gas volume,
m3；Z1For original state gas compressibility factor；Z2For final state gas compressibility factor；n1To spread the amount of parent material, mol；
N is the amount for the substance for diffusing into two liquid phases, mol；R is universal gas constant, Pa*m3/(mol*K)；T is Kelvin,
K；The influence that liquid phase volume expands in diffusion process is not considered；
And then obtain formula 9.：
(9) the pressure P under different diffusion time t is 9. found out according to formula2, obtain pressure P2Root after the change curve of t at any time
According to fitting formulaIt is fitted, by formulaCO is calculated2In water-oil phase
Between diffusion coefficient；Formula 10. in z1For liquid phase height, m；k1For pressure P2Time t fitting parameter.
According to currently preferred, CO2To the diffusion coefficient D of water phase1It measures and obtains as follows：
(a) it measures the cross-sectional area A of diffusion container and spreads the volume V of container1, cleaning, drying is carried out to diffusion container
And it vacuumizes；
(b) by CO2Full of diffusion container and boost to experimental pressure P1, spread the external back pressure of container, back pressure and experimental pressure
P1It is equal；
(c) pure water that temperature is T is injected with the speed of 15~25mL/min from diffusion lower vessel portion, records the pure of injection
Water volume V2, injection process is connected to back pressure, constant to keep spreading containment system pressure, wherein water phase heightIt is described
V2Value range is
(d) after pure water injection, closing diffusion container records the pressure change in diffusion container using pressure acquisition system,
Until the fall of pressure is no more than 1KPa in 30min；
(e) the pressure P of acquisitiontTime t relation data and balance pressure PeqIt is handled, is converted to pressure difference logarithm Ln
(Pt-Peq)-time t curves carry out linear fit, and CO is calculated2To the diffusion coefficient D of water phase1：
Formula 1. in, k be pressure difference logarithm-linearly matched curve slope；D1For CO2The diffusion system spread into water phase
Number, m2/s。
According to currently preferred, CO2To the diffusion coefficient D of oil phase2Assay method and step and CO2Expansion to water phase
Dissipate coefficient D1Assay method it is identical.
According to currently preferred, in step (b), the P1Value range is 1MPa-20MPa.
According to currently preferred, in step (c), the value range of the T is 293.15K-353.15K, the V2It takes
It is worth ranging from 50mL-150mL.
The advantage of the invention is that：
1, the CO that method of the invention can be measured according to drop of pressure method2Diffusion coefficient in single liquid phase passes through expansion
CO is calculated in exhibition Modeling The Concentration Profiles2The diffusion coefficient spread between water-oil phase, efficiently solves CO2In water-oil phase
Between diffusion coefficient computational methods lack the problem of.And in CO2To Two Liquid Phases diffusion pressure drop it is smaller under conditions of, avoid pressure
There are the errors that fluctuation is brought for power measurement result, improve computational accuracy when subsequent experimental data processing.
2, the CO that method of the invention measures respectively according to drop of pressure method2Diffusion coefficient into single liquid phase passes through expansion
Exhibition Modeling The Concentration Profiles can directly obtain CO2Concentration distribution in two liquid phases, and then acquire CO2Between water-oil phase
Diffusion coefficient.This method avoid directly measure CO2Pressure when being spread to Two Liquid Phases, when improving subsequent experimental data processing
Computational accuracy；Meanwhile this method is more in line with the diffusion characteristic under high temperature and pressure, avoid Two Liquid Phases diffusion pressure drop compared with
There are problems that pressure fluctuation under conditions of small so that result of calculation is more in line with the practical feelings spread under high temperature and pressure
Condition.
Description of the drawings
Fig. 1 is CO2Pressure difference logarithm-time curve and matched curve into water phase diffusion process；
Fig. 2 is CO2Pressure difference logarithm-time curve and matched curve into oil phase diffusion process；
Fig. 3 is CO2The schematic diagram of concentration distribution physical model is extended in Two Liquid Phases；
In figure, 1, CO2；2, water phase；3, oil phase.
Fig. 4 is CO2Pressure time histories and matched curve into water phase diffusion process by oil phase.
Specific implementation mode
With reference to embodiment and Figure of description, the present invention is described further, but not limited to this.
Embodiment 1
A kind of prediction CO2It is as follows to water phase diffusion process and the method for diffusion coefficient, implementation steps by oil phase：
(1) cross-sectional area for measuring diffusion container is 20cm2And the volume V of diffusion container1For 250mL, to spreading container
It carries out cleaning, drying and vacuumizes；
(2) by CO2Full of diffusion container and pressure is increased to experimental pressure 14.60MPa, is spread the external back pressure of container, is returned
Pressure is equal with experimental pressure；
(3) pure water that 92mL temperature is 323.15K is injected with the speed of 20mL/min from diffusion lower vessel portion, was injected
Cheng Liantong back pressure, to keep diffusion containment system pressure constant, wherein water phase height z0For 1.3cm；
(4) after pure water injection, it is straight to record the pressure change in diffusion container using pressure acquisition system for closing diffusion container
The fall of pressure is no more than 1KPa in 30min, and experiment terminates；
(5) the pressure P of acquisitiontTime t relation data and balance pressure PeqIt is handled, is converted to pressure difference logarithm Ln
(Pt-Peq)-time t curves carry out linear fit, as shown in Figure 1, CO is calculated2To the diffusion coefficient D of water phase1：
Formula 1. in, k be pressure difference logarithm-time graph slope；D1For CO2The diffusion coefficient spread into water phase, m2/s。
(6) step (1)-step (5) is repeated, pressure difference logarithm-time progress linear fit is measured, as shown in Fig. 2, calculating
CO2To the diffusion coefficient of oil phase
(7) its concentration distribution rule can be write out according to Fick's law for the one-dimensional diffusion that diffusion coefficient D is constant：
Formula 2. in, C CO2Concentration in the liquid phase, mol/m3；T is diffusion time, s；A is the normal of the amount determination of substance
Number；X is the distance to liquid phase surface, m.
(8) concentration C integrates x, and setsIt can obtain diffusing into liquid
The amount of the total material of phase is：
(9) 2. 3. formula that formula is transformed to constant A substitutes into formula, obtain formula 4.：
(10) it is 4. write formula as integrated form, obtains formula
(11) standard error function is formula
Using standard error function by formulaIt indicates, obtains formula
FormulaIn, C0For experiment condition 323.15K, CO under 14.60MPa2Maximum meltage in oil phase is
6957.38mol/m3。
(12) as shown in figure 3, according to formula 5., 6. model obtains CO to formula2Concentration distribution in oil phase, water phase：
Formula 5. in, C1It is t moment in water phase away from CO at liquid level x position2Concentration, mol/m3；x1For the lower boundary position of water phase
It sets, m；Formula 6. in, C2It is t moment in oil phase away from CO at liquid level x position2Concentration, mol/m3；x2For the lower boundary position of oil phase,
m。
The concentration distribution of t moment integrates x, total object that t moment is spread in water phase and oil phase can be obtained
The amount of matter：
(13) it can be obtained by state equation：
It can obtain：
Wherein, P1To spread initial pressure 1.46*107Pa；P2Pressure when being carried out to t moment for diffusion；V is gas body
Product, 8.6*10-5m3；Z1It is 0.3486 for original state gas compressibility factor；Z2For final state gas compressibility factor, it is
0.3431；N is the amount for the substance for diffusing into liquid phase, 2.2081mol；R is universal gas constant, 8.314Pa*m3/(mol*
K)；T is Kelvin, 323.15K；The influence that liquid phase volume expands in diffusion process is not considered.
(14) the pressure P under different diffusion time t 9. can be found out according to formula2, obtain pressure P2The variation of t is bent at any time
According to fitting formula after lineFitting parameter k1, as shown in figure 4, according to fitting parameter k1It calculates
Diffusion coefficient
Embodiment 2
A kind of measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase, shown in embodiment 1, difference
Be in：
The oil phase in container and water phase location swap, diffusion process CO will be spread2Diffusion by from water phase to oil phase,
This method measurement may be used and obtain diffusion coefficient.
Claims (5)
1. a kind of measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase, including steps are as follows：
(1) CO for using drop of pressure method to measure respectively2To the diffusion coefficient D of water phase1And CO2To the diffusion coefficient D of oil phase2；
(2) according to Fick's law, formula is used 2. to test out diffusion coefficient D as the concentration distribution rule of the one-dimensional diffusion of constant：
Formula 2. in, C CO2Concentration in the liquid phase, mol/m3；T is diffusion time, s；A is the constant that the amount of substance determines, x is
To the distance on liquid phase surface, m；
(3) concentration C integrates x, and setsIt is 3. obtained diffusing into liquid according to formula
The amount of the total material of phase is：
(4) 2. 3. formula that formula is transformed to constant A substitutes into formula, obtain formula 4.：
(5) it is 4. write formula as integrated form, obtains formula
(6) standard error function is formula
Using standard error function by formulaIt indicates, obtains formula
FormulaIn, C0For CO under experiment condition2Maximum meltage in current liquid phase, mol/m3；
(7) use formula 5., 6. model obtains CO to formula2Concentration distribution in oil phase, water phase：
Formula 5. in, C1It is t moment in water phase away from CO at liquid level x position2Concentration, mol/m3；x1For the lower boundary position of water phase, m；Formula
In 6., C2It is t moment in oil phase away from CO at liquid level x position2Concentration, mol/m3；x2For the lower boundary position of oil phase, m；
The concentration distribution of t moment integrates x, t moment is 7. obtained according to formula and diffuses into CO in two kinds of liquid phases2Total object
The amount n of matter：
(8) 8. formula is obtained by state equation：
Formula 8. in, P1To spread initial pressure, Pa；P2Pressure when being carried out to t moment for diffusion, Pa；V is gas volume, m3；Z1
For original state gas compressibility factor；Z2For final state gas compressibility factor；n1To spread the amount of parent material, mol；N is to expand
Dissipate the amount into the substance of two liquid phases, mol；R is universal gas constant, Pa*m3/(mol*K)；T is Kelvin, K；It does not examine
Consider the influence that liquid phase volume expands in diffusion process；
And then obtain formula 9.：
(9) the pressure P under different diffusion time t is 9. found out according to formula2, obtain pressure P2At any time according to quasi- after the change curve of t
It is box-likeIt is fitted, k in formula1, k2, m1, m2It is pressure P2Time t fitting parameter；
Peq' it is pressure P2Time t fitting balance pressure, Pa；By formulaCO is calculated2Diffusion between water-oil phase
Coefficient；Formula 10. in z1For liquid phase height, m；k1For pressure P2Time t fitting parameter.
2. measurement CO according to claim 12Diffusion process and the method for diffusion coefficient, feature exist between water-oil phase
In CO2To the diffusion coefficient D of water phase1It measures and obtains as follows：
(a) it measures the cross-sectional area A of diffusion container and spreads the volume V of container1, cleaning, drying is carried out to diffusion container and is taken out
Vacuum；
(b) by CO2Full of diffusion container and boost to experimental pressure P1, spread the external back pressure of container, back pressure and experimental pressure phase
Deng,
(c) pure water that temperature is T is injected with the speed of 15~25mL/min from diffusion lower vessel portion, records the pure water body of injection
Product V2, injection process is connected to back pressure, constant to keep spreading containment system pressure, wherein water phase heightThe V2Value
Ranging from
(d) after pure water injection, closing diffusion container records the pressure change in diffusion container using pressure acquisition system, until
The fall of pressure is no more than 1KPa in 30min；
(e) the pressure P of acquisitiontTime t relation data and balance pressure PeqIt is handled, is converted to pressure difference logarithm Ln (Pt-
Peq)-time t curves carry out linear fit, and CO is calculated2To the diffusion coefficient D of water phase1：
Formula 1. in, k be pressure difference logarithm-linearly matched curve slope；D1For CO2The diffusion coefficient spread into water phase,
m2/s。
3. measurement CO according to claim 12Diffusion process and the method for diffusion coefficient, feature exist between water-oil phase
In CO2To the diffusion coefficient D of oil phase2Assay method and step and CO2To the diffusion coefficient D of water phase1Assay method it is identical.
4. measurement CO according to claim 22Diffusion process and the method for diffusion coefficient, step (b) between water-oil phase
In, the P1Value range is 1MPa-20MPa.
5. measurement CO according to claim 22Diffusion process and the method for diffusion coefficient, step (c) between water-oil phase
In, the value range of the T is 293.15K-353.15K, the V2Value range is 50mL-150mL.
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| CN108362614B (en) * | 2018-01-19 | 2020-03-27 | 中国石油大学(华东) | Device and method for measuring diffusion coefficient in huff and puff process of shale oil carbon dioxide |
| CN109443995B (en) * | 2018-11-29 | 2021-09-03 | 朗缪环保科技(天津)有限公司 | Method for measuring diffusion coefficient and predicting adsorption capacity of porous material |
| CN109522672B (en) * | 2018-11-30 | 2020-11-24 | 华南理工大学 | Steady-state solute concentration distribution model in continuous countercurrent two-phase mass transfer process |
| CN110186815B (en) * | 2019-06-27 | 2024-02-23 | 西南石油大学 | High-temperature high-pressure phase-change-preventing gas-liquid interfacial tension measuring device and measuring method |
| CN112730157B (en) * | 2020-12-30 | 2022-03-18 | 湖南大学 | Method for measuring diffusion coefficient of solute substance in solution |
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