CN107063935A - One kind measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase - Google Patents
One kind measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase Download PDFInfo
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Abstract
CO is measured the present invention relates to one kind2Single 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 determined according to drop of pressure method2Diffusion coefficient in single liquid phase, CO can be directly obtained by extending Modeling The Concentration Profiles2Concentration distribution in two liquid phases, and then obtain CO2Diffusion coefficient between water-oil phase.Present method avoids direct measurement CO2Pressure when being spread to Two Liquid Phases, improves computational accuracy during subsequent experimental data processing, and computing is more succinct;Meanwhile, method of the invention more conforms to the diffusion characteristic under HTHP, it is to avoid the problem of there is pressure fluctuation under the conditions of Two Liquid Phases diffusion pressure drop is less so that result of calculation more conforms to the actual conditions spread under HTHP.
Description
Technical field
CO is measured the present invention relates to one kind2Diffusion 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 is increased 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 are by the important object as 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
Ask and be widely used.
Note CO2Production technique mainly includes CO2Drive, CO2Handle up and CO2Water-air two-phase flow drive etc..Applied in these technologies
During, the CO of injection2Can be with stratum water, injection water and crude oil formation three-phase system, CO2Can be in single liquid phase and oil
Mass transfer is diffused between water two-phase.CO2Diffusion can reduce oil water interfacial tension, viscosity of crude and enable to
Crude oil expands, so as 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, improve nontraditional reservoir ultimate recovery and finally realize 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.
At present, CO is determined2The method of diffusion coefficient in oil phase or aqueous phase is generally 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 ripe.The method is surveyed due to only needing to
Determine the pressure change in diffusion process, it is not necessary to directly determine the concentration in diffusion process, measure efficient and convenient, so that extensive
Using.However, such a method can only be used as determining CO2Diffusion coefficient when being spread to single liquid phase, is not suitable for determining CO2To two
Diffusion coefficient during alternate diffusion, if such a method is used to determine CO2During diffusion process between water-oil phase, CO2In list
The amount for the material for diffusing into another liquid phase in the time of position is smaller, causes pressure drop smaller, and conventional pressure manometers are difficult to accurate seizure,
The continuous mode duration is longer and balances pressure and is difficult to determine.In addition, the CO under HTHP2In above-critical state and pole not
It is stable, cause the pressure measured in experimentation big ups and downs occur so that pressure curve is difficult to accurate acquisition.
Chinese patent literature CN104237079A discloses a kind of measurement CO2The experimental method and dress of diffusion coefficient in water
Put.Experimental provision is using fixed diffusion length, mainly including data collecting system, constant-temperature heating system, pH meter probe, diffusion
Kettle, pressure sensor, temp probe etc., pH meter probe are arranged on the bottom end cover of diffusion kettle, and pressure sensor is arranged on upper end cover,
Heating coil outside temp probe one end connection diffusion kettle, the other end is connected with constant-temperature heating system.Carried out in diffusion kettle real
When testing, diffusion kettle it is mounted on bearings, Rotational diffusion kettle simulation tilted stratum, according to The Ideal-Gas Equation using pressure come
Calculate CO2Initial concentration, the pH value gathered according to data collecting system calculates CO2Amount of hydrolysis, draw CO2Amount of hydrolysis with
Time subduplicate matched curve, obtains slope k, diffusion coefficient D is tried to achieve according to computation model, and the device and method is to determine
CO2The diffusion coefficient in water, it is impossible to determine 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 aqueous phase
The method of number and equilibrium concentration.This method is by U-tube bottom aqueous phase saturation CO2, form saturated carbon sour water, the injection of U-tube upper end
CO2, lower end injection crude oil, according to improved PVT pressure decline methods, by determining CO2The pressure caused is spread to saturated carbon sour water to become
Change, CO can be obtained with reference to drop formula2CO after diffusion coefficient from aqueous 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 aqueous phase into oil phase diffusion process, but experiment is obtained
The falloff curve fluctuation obtained is larger, and the processing to subsequent experimental result brings great error, and measurement process is complicated.
Therefore, how CO is tested using the method for simple and fast2Diffusion process and diffusion coefficient turn between water-oil phase
There is technical problem to be solved at present.
The content of the invention
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 wide variety of single liquid phase drop of pressure method and the present invention are extended concentration by the measuring method of the present invention
Distributed model is combined, the CO determined 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 try to achieve CO2Diffusion coefficient between water-oil phase.
This method avoid direct measurement CO2Pressure when being spread to Two Liquid Phases, improves calculating essence during subsequent experimental data processing
Degree;Meanwhile, this method more conforms to the diffusion characteristic under HTHP, it is to avoid drop less condition in Two Liquid Phases diffusion pressures
Under the problem of there is pressure fluctuation so that result of calculation more conforms to the actual conditions spread under HTHP.
Technical scheme is as follows:
One kind measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase, including step are as follows:
(1) CO determined respectively using drop of pressure method2To the diffusion coefficient D of aqueous phase1And CO2To the diffusion coefficient of oil phase
D2;
(2) according to Fick's law, use formula 2. to test out diffusion coefficient D and advised for the concentration distribution of the one-dimensional diffusion of constant
Rule:
Formula 2. in, C is CO2Concentration in the liquid phase, mol/m3;T is diffusion time, s;A is normal for the amount determination of material
Number;X is the distance to liquid phase surface, m.
(3) concentration C is integrated to x, and set3. diffused into according to formula
The amount for entering the total material of liquid phase is:
(4) 2. the formula that 3. formula is transformed to constant A substitutes into formula, obtains formula 4.:
(5) 4. write formula as integrated form, obtain formula
(6) standard error function is formula
Using standard error function by formulaRepresent, obtain formula
FormulaIn, C0For CO under experiment condition2Maximum meltage in current liquid phase, mol/m3;
(7) use formula is 5., 6. model obtains CO to formula2Concentration distribution in oil phase, aqueous phase:
Formula 5. in, C1It is t in aqueous phase away from CO at liquid level x position2Concentration, mol/m3;x1For the lower boundary position of aqueous phase
Put, m;Formula 6. in, C2It is t 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 is integrated for x, t 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, P1For diffusion initial pressure, Pa;P2Carried out for diffusion to pressure during t, 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 material 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. obtained according to formula2, obtain pressure P2With root after time t change curve
According to fitting formulaIt is fitted, by formulaCalculating obtains CO2In water-oil phase
Between diffusion coefficient;Formula 10. middle z1For liquid phase height, m;k1For pressure P2- time t fitting parameter.
According to currently preferred, CO2To the diffusion coefficient D of aqueous phase1Determine and obtain as follows:
(a) determine the cross-sectional area A of diffusion container and spread the volume V of container1, cleaning, drying is carried out to diffusion container
And vacuumize;
(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) temperature is injected for T pure water with 15~25mL/min speed from diffusion lower vessel portion, it is pure that record injects
Water volume V2, injection process connects back pressure, to keep diffusion containment system pressure constant, wherein aqueous phase heightThe V2
Span 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 collectiont- time t relation data and balance pressure PeqHandled, be converted to pressure difference logarithm Ln
(Pt-Peq)-time t curves carry out linear fit, and calculating obtains CO2To the diffusion coefficient D of aqueous phase1:
Formula 1. in, k be pressure difference logarithm-linearly matched curve slope;D1For CO2The diffusion system spread into aqueous phase
Number, m2/s。
According to currently preferred, CO2To the diffusion coefficient D of oil phase2Assay method and step and CO2To the expansion of aqueous phase
Dissipate coefficient D1Assay method it is identical.
According to currently preferred, in step (b), the P1Span is 1MPa-20MPa.
According to currently preferred, in step (c), the span of the T is 293.15K-353.15K, the V2Take
Value scope is 50mL-150mL.
The advantage of the invention is that:
1st, the CO that method of the invention can be determined according to drop of pressure method2Diffusion coefficient in single liquid phase, by expanding
Exhibition Modeling The Concentration Profiles, which are calculated, obtains CO2The diffusion coefficient spread between water-oil phase, efficiently solves CO2In water-oil phase
Between diffusion coefficient computational methods the problem of lack.And in CO2To Two Liquid Phases diffusion pressures drop it is less under the conditions of, it is to avoid pressure
There is the error that fluctuation is brought in power measurement result, improve computational accuracy during subsequent experimental data processing.
2nd, the CO that method of the invention is determined respectively according to drop of pressure method2Diffusion coefficient into single liquid phase, by expanding
Exhibition Modeling The Concentration Profiles can directly obtain CO2Concentration distribution in two liquid phases, and then try to achieve CO2Between water-oil phase
Diffusion coefficient.This method avoid direct measurement CO2Pressure when being spread to Two Liquid Phases, when improving subsequent experimental data processing
Computational accuracy;Meanwhile, this method more conforms to the diffusion characteristic under HTHP, it is to avoid Two Liquid Phases diffusion pressures drop compared with
The problem of there is pressure fluctuation under conditions of small so that result of calculation more conforms to the actual feelings spread under HTHP
Condition.
Brief description of the drawings
Fig. 1 is CO2Pressure difference logarithm-time curve and matched curve into aqueous 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;2nd, aqueous phase;3rd, oil phase.
Fig. 4 is CO2Pressure time histories and matched curve into aqueous phase diffusion process by oil phase.
Embodiment
With reference to embodiment and Figure of description, the present invention is described further, but not limited to this.
Embodiment 1
One kind prediction CO2By oil phase to aqueous phase diffusion process and the method for diffusion coefficient, implementation steps are as follows:
(1) cross-sectional area for determining diffusion container is 20cm2And the volume V of diffusion container1For 250mL, to diffusion container
Carry out cleaning, drying and vacuumize;
(2) by CO2Full of spreading container and raising pressure to experimental pressure 14.60MPa, the external back pressure of container is spread, is returned
Pressure is equal with experimental pressure;
(3) 92mL temperature is injected for 323.15K pure water with 20mL/min speed from diffusion lower vessel portion, injected
Cheng Liantong back pressure, to keep diffusion containment system pressure constant, wherein aqueous phase height z0For 1.3cm;
(4) after pure water injection, closing diffusion container, the pressure change recorded using pressure acquisition system in diffusion container is straight
The fall of pressure is no more than 1KPa in 30min, and experiment terminates;
(5) the pressure P of collectiont- time t relation data and balance pressure PeqHandled, be converted to pressure difference logarithm Ln
(Pt-Peq)-time t curves carry out linear fit, and CO is obtained as shown in figure 1, calculating2To the diffusion coefficient D of aqueous phase1:
Formula 1. in, k be pressure difference logarithm-time graph slope;D1For CO2The diffusion coefficient spread into aqueous phase, m2/s。
(6) repeat step (1)-step (5), determines pressure difference logarithm-time progress linear fit, as shown in Fig. 2 calculating
CO2To the diffusion coefficient of oil phase
(7) for the one-dimensional diffusion that diffusion coefficient D is constant, according to Fick's law, its concentration distribution rule can be write out:
Formula 2. in, C is CO2Concentration in the liquid phase, mol/m3;T is diffusion time, s;A is normal for the amount determination of material
Number;X is the distance to liquid phase surface, m.
(8) concentration C is integrated to x, and setIt can obtain diffusing into liquid
The amount of the total material of phase is:
(9) 2. the formula that 3. formula is transformed to constant A substitutes into formula, obtains formula 4.:
(10) 4. write formula as integrated form, obtain formula
(11) standard error function is formula
Using standard error function by formulaRepresent, obtain formula
FormulaIn, C0For experiment condition 323.15K, CO under 14.60MPa2Maximum meltage in oil phase, be
6957.38mol/m3。
(12) as shown in figure 3, according to formula 5., 6. model obtains CO to formula2Concentration distribution in oil phase, aqueous phase:
Formula 5. in, C1It is t in aqueous phase away from CO at liquid level x position2Concentration, mol/m3;x1For the lower boundary position of aqueous phase
Put, m;Formula 6. in, C2It is t 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 is integrated for x, total thing that t spreads in aqueous phase and oil phase can be obtained
The amount of matter:
(13) it can be obtained by state equation:
It can draw:
Wherein, P1For diffusion initial pressure 1.46*107Pa;P2Carried out for diffusion to pressure during t;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 material 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 obtained according to formula2, obtain pressure P2It is bent with time t change
According to fitting formula after lineFitting parameter k1, as shown in figure 4, according to fitting parameter k1Calculate
Diffusion coefficient
Embodiment 2
One kind measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase, shown in be the same as Example 1, difference
Be in:
By the oil phase and aqueous phase location swap that spread in container, diffusion process is CO2By diffusion from aqueous phase to oil phase,
Diffusion coefficient can be obtained using this method measurement.
Claims (5)
1. one kind measurement CO2Diffusion process and the method for diffusion coefficient between water-oil phase, including step are as follows:
(1) CO determined respectively using drop of pressure method2To the diffusion coefficient D of aqueous phase1And CO2To the diffusion coefficient D of oil phase2;
(2) according to Fick's law, formula is used 2. to test out concentration distribution rule of the diffusion coefficient D for the one-dimensional diffusion of constant:
Formula 2. in, C is CO2Concentration in the liquid phase, mol/m3;T is diffusion time, s;A is the constant of the amount determination of material, and x is
To the distance on liquid phase surface, m.
(3) concentration C is integrated to x, and set3. obtained diffusing into liquid according to formula
The amount of the total material of phase is:
(4) 2. the formula that 3. formula is transformed to constant A substitutes into formula, obtains formula 4.:
(5) 4. write formula as integrated form, obtain formula
(6) standard error function is formula
Using standard error function by formulaRepresent, obtain formula
FormulaIn, C0For CO under experiment condition2Maximum meltage in current liquid phase, mol/m3;
(7) use formula is 5., 6. model obtains CO to formula2Concentration distribution in oil phase, aqueous phase:
Formula 5. in, C1It is t in aqueous phase away from CO at liquid level x position2Concentration, mol/m3;x1For the lower boundary position of aqueous phase, m;Formula
6. in, C2It is t 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 is integrated for x, t is 7. obtained according to formula and diffuses into CO in two kinds of liquid phases2Total thing
The amount n of matter:
(8) 8. formula is obtained by state equation:
Formula 8. in, P1For diffusion initial pressure, Pa;P2Carried out for diffusion to pressure during t, 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 expansion
Dissipate the amount for the material for entering two liquid phases, mol;R is universal gas constant, Pa*m3/(mol*K);T is Kelvin, K;Do 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. obtained according to formula2, obtain pressure P2With after time t change curve according to plan
It is box-likeIt is fitted, by formulaCalculating obtains CO2Between water-oil phase
Diffusion coefficient;Formula 10. middle z1For liquid phase height, m;k1For pressure P2- time t fitting parameter.
2. measurement CO according to claim 12Diffusion process and the method for diffusion coefficient between water-oil phase, its feature exist
In CO2To the diffusion coefficient D of aqueous phase1Determine and obtain as follows:
(a) determine the cross-sectional area A of diffusion container and spread the volume V of container1, cleaning, drying is carried out to diffusion container and 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) temperature is injected for T pure water with 15~25mL/min speed from diffusion lower vessel portion, records the pure water body of injection
Product V2, injection process connects back pressure, to keep diffusion containment system pressure constant, wherein aqueous phase heightThe V2Value
Scope 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 collectiont- time t relation data and balance pressure PeqHandled, be converted to pressure difference logarithm Ln (Pt-
Peq)-time t curves carry out linear fit, and calculating obtains CO2To the diffusion coefficient D of aqueous phase1:
Formula 1. in, k be pressure difference logarithm-linearly matched curve slope;D1For CO2The diffusion coefficient spread into aqueous phase,
m2/s。
3. measurement CO according to claim 12Diffusion process and the method for diffusion coefficient between water-oil phase, its feature exist
In CO2To the diffusion coefficient D of oil phase2Assay method and step and CO2To the diffusion coefficient D of aqueous 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 P1Span 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 span of the T is 293.15K-353.15K, the V2Span is 50mL-150mL.
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CN109522672A (en) * | 2018-11-30 | 2019-03-26 | 华南理工大学 | A kind of continuous flow upstream two-phase mass transport process stable state solute concentration distribution model |
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CN109443995A (en) * | 2018-11-29 | 2019-03-08 | 朗缪环保科技(天津)有限公司 | A method of measurement porous material diffusion coefficient and prediction adsorbance |
CN109522672A (en) * | 2018-11-30 | 2019-03-26 | 华南理工大学 | A kind of continuous flow upstream two-phase mass transport process stable state solute concentration distribution model |
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