CN108801860B - Method for measuring diffusion coefficient of carbon dioxide in crude oil - Google Patents
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Abstract
The invention belongs to the technical field of oil and gas field development and discloses a method for measuring diffusion coefficient of carbon dioxide in crude oil. The method comprises the following steps: 1) to volume of VCIs filled into the closed container0A volume of crude oil; 2) keeping the temperature of the closed container filled with the crude oil in the step 1) constant at a measured temperature T; 3) filling carbon dioxide gas into the constant-temperature closed container in the step 2), and starting from the initial time t0Beginning to measure the pressure of carbon dioxide gas p (t) at intervals of Δ t until an equilibrium pressure is reached; 4) the expansion coefficient beta of the crude oil dissolved with the carbon dioxide is combined with the relation between the diffusion time t and the pressure P (t) to obtain the diffusion coefficient D of the carbon dioxide in the crude oilAB(ii) a The formula according to step 4) is:
the method considers the volume expansion of the crude oil after the carbon dioxide is diffused into the crude oil, and can more accurately measure the diffusion coefficient of the carbon dioxide in the crude oil.
Description
Technical Field
The invention belongs to the technical field of oil and gas field development, and particularly relates to a method for measuring diffusion coefficient of carbon dioxide in crude oil.
Background
In the development of oil and gas fields, the recovery ratio of crude oil can be improved by adopting carbon dioxide to drive oil, so that the carbon dioxide oil recovery technology is widely applied. The steps of using carbon dioxide to recover oil are as follows: firstly, injecting a certain amount of carbon dioxide gas into an oil layer, then closing a well to ensure that the diffusion of the carbon dioxide in crude oil reaches balance, and finally opening the well to recover oil. In order to predict the time for carbon dioxide to reach equilibrium in crude oil, the diffusion coefficient of carbon dioxide in crude oil needs to be known, and if the diffusion coefficient is not accurate, the equilibrium time cannot be accurately determined, which brings adverse effects to oil recovery.
In the prior art, methods for determining the diffusion coefficient of carbon dioxide in a liquid can be divided into two categories: direct and indirect processes. Wherein the direct process comprises: the fluid is sampled at different time and different diffusion distances, and then the samples are analyzed to obtain the concentration data of the carbon dioxide, and then the diffusion coefficient of the carbon dioxide in the fluid is deduced. However, the sampling process can interfere with the flow field in the system, causing experimental error. The indirect method does not require sampling, and among them, the NMR (nuclear magnetic resonance) method and the PVT (pressure-volume-temperature) method are the two most widely used methods. The NMR method can directly measure the concentration of carbon dioxide in a closed system through nuclear magnetic resonance spectroscopy, but the NMR method is expensive and high in cost. The PVT method is a relatively conventional method, and takes a pressure collapse method as an example, which measures a pressure change of a gas-liquid diffusion system, and then calculates a diffusion coefficient from a pressure change curve with time.
Literature CO2Measurement of diffusion coefficient in porous media (proceedings of higher schools of petrochemical industry, 2009, 22(4)), CO was developed2Measuring diffusion coefficient in porous medium of saturated simulated salt water, recording CO diffused into porous medium at different time in the experimental process2Substituting the amount into corresponding mathematical model to calculate CO2Diffusion coefficient in porous media saturated with fluid. The process does not take into account CO2After diffusion into the porous medium, the resulting expansion of the water in the porous medium, and the use of a pump to meter the CO injection2The measurement accuracy of the quantity of (2) is far less than the accuracy of the measurement pressure.
The document Measurement of gas diffusion in the gravity oils (Journal of Petroleum Science and Engineering, 2000, 25: 37-47) establishes a one-dimensional mathematical model for calculating the diffusion coefficient, and the diffusion coefficient is obtained by experimentally measuring the change rule of the system pressure along with time and substituting the change rule into the diffusion mathematical model. However, the expansion of the liquid phase volume caused by the diffusion of carbon dioxide is not considered in the modeling process.
The standard for measuring the diffusion coefficient of hydrocarbon gas in rock (the oil and gas industry standard of the people's republic of China, SY/T6129-: firstly, the method is difficult to realize under the condition of lacking gas chromatography; secondly, the gas sampling of the diffusion chambers at the two ends can destroy the diffusion balance to cause larger experimental error.
According to the research on the molecular diffusion coefficient of the multi-component gas-crude oil in the porous medium at high temperature and high pressure (lithologic hydrocarbon reservoir, 2012, 24 (5): 111-2Recording the change of inlet pressure and corresponding time until oil-gas balance is reachedAnd (4) substituting the recorded data into a mathematical model to obtain the molecular diffusion coefficient of each component in the multi-component gas-crude oil. However, the method still does not consider the liquid phase volume expansion caused by the diffusion process, and the initial value of the diffusion coefficient must be given through an empirical formula when the model is calculated, and the model in the document is relatively complex.
The literature Molecular differentiation coefficients of the multicomponent gas-reactant systems under high temperature and pressure&Engineering Chemistry Research, 2009, 48: 9023-2Rich gas-crude oil, CO2Rich gas-crude oil, CH4Gas-rich-crude oil diffusion coefficients for the three systems. They use the PVT device to mix gas with crude oil, then record the pressure of the whole system until the gas-liquid reaches equilibrium, bring it into a mathematical model, and calculate and obtain the diffusion coefficient. However, the method still does not consider the liquid phase volume expansion caused by the diffusion process, and the initial value of the diffusion coefficient must be given through an empirical formula when the model is calculated, and the model in the document is relatively complex.
Literature supercritical CO2In the determination of the diffusion coefficient in the saturated water porous medium (application basis and engineering science bulletin, 2014, 22 (4): 733-2Diffusion in a saturated water porous medium, and the supercritical CO is obtained by applying Fick diffusion law on the basis of the model2And (3) calculating the diffusion coefficient by combining a diffusion equation in a saturated water porous medium and an indoor diffusion experiment. But the model ignores the effect of the volume expansion of the liquid phase due to the dissolution of gas in the liquid phase.
As can be seen from the above, the diffusion coefficient of carbon dioxide gas cannot be directly measured by either direct or indirect measurement. In addition, these measurement methods cannot obtain an accurate diffusion coefficient of carbon dioxide gas, and thus cannot accurately confirm the equilibrium time of carbon dioxide gas in crude oil, thereby adversely affecting oil recovery.
Disclosure of Invention
In order to solve the above problems in the prior art, the present invention provides a method for determining the diffusion coefficient of carbon dioxide in crude oil, which considers the volume expansion of crude oil after carbon dioxide diffuses into crude oil and can accurately determine the diffusion coefficient of carbon dioxide in crude oil.
The invention provides a method for measuring diffusion coefficient of carbon dioxide in crude oil, which comprises the following steps:
1) to volume of VCIs filled into the closed container0A volume of crude oil of which V0＜VC；
2) Keeping the temperature of the closed container filled with the crude oil in the step 1) constant at a measured temperature T;
3) filling carbon dioxide gas into the constant-temperature closed container in the step 2), and starting from the initial time t0Measuring the pressure P (t) of carbon dioxide gas at a time interval of Δ t until an equilibrium pressure is reached, wherein at an initial time t0Has a pressure of P (t) as carbon dioxide gas0)；
4) The expansion coefficient beta of the crude oil dissolved with the carbon dioxide is combined with the relation between the diffusion time t and the pressure P (t) to obtain the diffusion coefficient D of the carbon dioxide in the crude oilAB；
The formula of the basis in the step 4) is as follows:
wherein Z isgIs the compression factor of carbon dioxide, R is the universal gas constant, xeqThe equilibrium interface concentration of carbon dioxide at the oil-gas interface is shown, and A is the sectional area of the rock core.
The method can accurately measure the diffusion coefficient of the carbon dioxide in the crude oil, thereby more accurately predicting the balance time in the carbon dioxide oil extraction and being beneficial to the oil extraction; in addition, the method of the invention adopts uniform time intervals to measure the pressure, which is beneficial to realizing automatic control and convenient for operation.
Drawings
FIG. 1: a schematic diagram of a test apparatus employed in one embodiment of the invention;
FIG. 2: example 1 plot of volume expansion versus pressure for crude oil with dissolved carbon dioxide;
FIG. 3: graph of pressure correction term versus square root of diffusion time in example 1;
FIG. 4: comparative example 1 is a plot of pressure term as a function of square root of diffusion time.
Detailed Description
In order that the present invention may be more readily understood, the following detailed description of the invention is given with reference to the accompanying embodiments, which are given by way of illustration only and are not intended to limit the invention.
The invention provides a method for measuring diffusion coefficient of carbon dioxide in crude oil, which comprises the following steps:
1) to volume of VCIs filled into the closed container0A volume of crude oil of which V0＜VC；
2) Keeping the temperature of the closed container filled with the crude oil in the step 1) constant at a measured temperature T;
3) filling carbon dioxide gas into the constant-temperature closed container in the step 2), and starting from the initial time t0Measuring the pressure P (t) of carbon dioxide gas at a time interval of Δ t until an equilibrium pressure is reached, wherein at an initial time t0Has a pressure of P (t) as carbon dioxide gas0)；
4) The expansion coefficient beta of the crude oil dissolved with the carbon dioxide is combined with the relation between the diffusion time t and the pressure P (t) to obtain the diffusion coefficient D of the carbon dioxide in the crude oilAB；
The formula according to step 4) is:
wherein Z isgIs the compression factor of carbon dioxide, R is the universal gas constant, xeqThe equilibrium interface concentration of carbon dioxide at the oil-gas interface is shown, and A is the sectional area of the rock core.
According to the invention, said initial time t0The diffusion time of carbon dioxide gas when measurement is started is referred to; p (t) is the pressure corresponding to the diffusion time t of carbon dioxide.
Preferably, the method for measuring the expansion coefficient β includes:
1) determining the volume V of the liquid phase at the bubble point pressure P of crude oils containing different amounts of carbon dioxideL；
2) By the formula VL/Vdβ P +1, where V gives the expansion coefficient βdIs the volume of crude oil without carbon dioxide.
Specifically, carbon dioxide with different amounts is respectively dissolved in crude oil, and corresponding bubble point pressure P and liquid phase volume V are measuredLWith VL/VdAnd (3) drawing by taking the bubble point pressure P as an abscissa, fitting to obtain a relation straight line of the bubble point pressure P and the abscissa, wherein the slope of the obtained straight line is the expansion coefficient beta.
The expansion coefficient beta measured by the method can accurately reflect the volume expansion of the crude oil caused by dissolving the carbon dioxide, and further obtain the accurate diffusion coefficient D of the carbon dioxide in the crude oilAB。
Preferably, the compression factor ZgThe PVT sample kettle is adopted for measurement, and the state equation P is obtainedgV＝ZgCalculating nRT.
In particular, the compression factor ZgThe determination of (a) comprises the steps of:
1) adding V into PVT sample kettle1Volume of carbon dioxide, pressure 0.1MPa (normal pressure), and Z at this pressure when carbon dioxide is considered as an ideal gas at normal pressure g1 according to equation of state PgV＝ZgnrT, calculating the amount of carbon dioxide substance n1；
2) Raising the pressure to the initial pressure P of filling carbon dioxide in the closed container2Recording volume V of carbon dioxide2And in combination with the amount of substance n thereof1Calculated at a pressure P2Compression factor Z of carbon dioxide at temperature Tg。
In the invention, R is a general gas constant, and the specific value is 8.314cm3·MPa·mol-1·K-1。
According to the invention, said xeqIn particular to P in a closed container under the balanced stateeqThe amount of carbon dioxide per unit volume under pressure, which can be calculated according to the following formula:
In the invention, the core sectional area A is selected according to the actual situation of the crude oil to be measured.
According to one embodiment of the present invention, the method employs a testing device, as shown in fig. 1, the testing device includes: a test closed container 15, a carbon dioxide closed container 14, a crude oil closed container 29, a vacuum pump 21, an incubator 16, a pressure sensor 17 and a data processing device 24,
the carbon dioxide closed container 14 and the crude oil closed container 29 are respectively connected to the testing closed container 15, the carbon dioxide closed container 14 and the testing closed container 15 are arranged in the incubator 16, the vacuum pump 21 is used for vacuumizing the testing closed container 15, and the pressure sensor 17 is used for measuring the pressure of the testing closed container 15 and transmitting a pressure signal to the data processing device 24.
Preferably, the carbon dioxide containment vessel 14 is attached to the top of the test containment vessel 15 and the crude oil containment vessel 29 is attached to the bottom of the test containment vessel 15.
In the present invention, the pressure sensor 17 is used to determine the pressure of the carbon dioxide-crude system within the test enclosure 15.
According to the invention, the testing device also comprises a carbon dioxide supply pump 22 and a crude oil supply pump 23, which are connected to the carbon dioxide closed vessel 14 and the crude oil closed vessel 29, respectively.
According to the invention, the testing device also comprises a temperature sensor 18, arranged on the oven 16, which ensures a constant measured temperature.
As shown in FIG. 1, the testing device further comprises other components such as valves and the like, so as to realize the measurement of the diffusion coefficient of carbon dioxide in crude oil by the flow control device of crude oil and carbon dioxide gas.
The present invention will be described in detail below with reference to examples and application examples.
Example 1
This example illustrates the method of the present invention for determining the diffusion coefficient of carbon dioxide in crude oil.
As shown in fig. 1, the test apparatus used for measurement includes: the device comprises a testing closed container 15, a carbon dioxide closed container 14 connected to the top of the testing closed container 15, a crude oil closed container 29 connected to the bottom of the testing closed container 15, a vacuum pump 21, an incubator 16 provided with a temperature sensor 18, a pressure sensor 17, a data processing device 24, a carbon dioxide supply pump 22 connected to the carbon dioxide closed container 14 and a crude oil supply pump 23 connected to the crude oil closed container 29, wherein the carbon dioxide closed container 14 and the testing closed container 15 are arranged in the incubator 16, the vacuum pump 21 is connected to a pipeline 19 through a pipeline 25, and the pressure sensor 17 is connected to the pipeline 19 and transmits a pressure signal to the data processing device 24.
A valve 26 is provided between the junction of the pipe 25 and the pipe 19 and the outlet of the carbon dioxide closed vessel 14, a valve 27 is provided on a line connecting the bottom of the test closed vessel 15 and the crude oil closed vessel 29, and after the valves 26 and 27 are closed, the vacuum pump 21 is actually communicated only with the test closed vessel 15, thereby achieving evacuation of the test closed vessel 15.
The specific determination method comprises the following steps: after the devices are connected, the devices are cleaned by petroleum ether, dried by hot air, and then the air tightness of the whole device is checked to ensure that the devices are airtight. Valve 26 and valve 27 are closed and vacuum pump 21 is activated to evacuate test capsule 15 for 16 hours. After the completion of the gas extraction, the valve 27 is opened and the crude oil is supplied to the test closed vessel 15 by the crude oil supply pump 23 (V)C174 ml) was fed inV0The valve 27 was closed and the crude oil density was 0.87g/cm for 100 ml of crude oil3The viscosity was 20.1 mPas. The test capsule 15 and the carbon dioxide capsule 14 were thermostatted to an experimental temperature (T) of 97.53 ℃. The valve 26 is opened, and the test closed vessel 15 is filled with carbon dioxide gas by the carbon dioxide supply pump 22 until the pressure sensor 17 indicates 7MPa, and the valve 26 is closed. The pressure p (t) indicated by the pressure sensor 17 is recorded every 1 minute until an equilibrium pressure is reached. The results are shown in Table 1.
TABLE 1
Measurement of expansion coefficient β of crude oil dissolved with carbon dioxide:
first, the volume V of the liquid phase was measured at the bubble point pressure of crude oil in which carbon dioxide was dissolved in various amountsLThe measurements were carried out at molar ratios of carbon dioxide to crude oil of 0.412, 1.813, 3.057, 3.806, respectively. Then according to VL/VdObtaining the expansion coefficient beta, V as beta P +1dIs the volume of crude oil that does not contain carbon dioxide. The measurement results are shown in table 2.
TABLE 2
| Molar ratio of 0.412 | Molar ratio of 1.813 | The molar ratio is 3.057 | The molar ratio is 3.806 | |
| P/MPa | 4.169 | 11.790 | 18.507 | 24.995 |
| Vd/mL | 97.929 | 96.657 | 95.852 | 95.201 |
| VL/mL | 102.283 | 105.199 | 112.961 | 116.243 |
According to VL/Vdβ P +1, with pressure P as abscissa and VL/VdPlotted as the ordinate in a planar rectangular coordinate system, as shown in fig. 2. Fitting to obtain
This gives an expansion coefficient β equal to 0.0089.
The data in table 1 were processed based on the expansion coefficient β measured above. By pressure correction terms
As ordinate, the square root of diffusion time
Plotted for the abscissa in a rectangular plane coordinate system, as shown in fig. 3. The fit results in y being 0.8457x-26.512, where y represents the pressure correction term, x represents the square root of the diffusion time, and the formula
Slope of
Comparing the fitted straight line with the formula to obtain the slope k which is 0.8457, and calculating the diffusion coefficient D of the carbon dioxide in the crude oilABEqual to 0.000772233cm2/s。
In this embodiment, the parameters used in calculating the diffusion coefficient are as follows:
Zgthe compression factor of the carbon dioxide is measured to be 0.81774, and the specific measurement steps comprise: (1) according to equation of state PgV＝ZgnRT, CO at atmospheric pressure2Considered to be an ideal gas, when Z isgPut a known volume V into a PVT sample kettle1CO of2The gas, the pressure of which is 0.1MPa and the temperature of which is 97.53 ℃, can be calculated to obtain the mole number n of the gas1(ii) a (2) The pressure was raised to 7MPa for the experiment of this example, and the volume V of the PVT sample vessel at this time was recorded2Substituting the data into the equation of state can calculate and obtain the Z under the pressure and temperature conditions of the implementationg。
R is a general gas constant of 8.314cm3·MPa·mol-1·K-1。
T is the experimental temperature 97.53 ℃.
xeqTesting P in the closed container 15 under equilibriumeqAmount of carbon dioxide per unit volume under pressure, wherein
A is the core cross-sectional area, which in this example is 4.71cm2。
In the present embodiment, t0＝0。
Application example 1
In the actual oil recovery process, the diffusion coefficient D calculated by using the method of embodiment 1 of the inventionAB＝0.000772233cm2The time to carbon dioxide equilibrium in crude oil is predicted to be 450 days/s, while in actual cases the time to carbon dioxide equilibrium in crude oil is 465 days.
Comparative example 1
The apparatus and assay procedure used was the same as in example 1, except that the formula according to which the diffusion coefficient was calculated was different, and the data in table 1 were processed using the formula in the prior art.
In the prior art, the formula is as follows:
wherein, P (t)0)、t、t0、Zg、R、T、xeqThe meaning of A is the same as that of example 1, and the description thereof is omitted.
By the square root of the diffusion time
As abscissa, by pressure difference P (t)0) -P (t) is the ordinate, plotted in a planar rectangular coordinate system, as shown in FIG. 4. The fit yields y ═ 0.0124x-0.3833, where y represents the pressure term, x represents the square root of the diffusion time, and the slope k' is equal to 0.0124. According to the above formula
The diffusion coefficient D 'of the carbon dioxide in the crude oil is calculated'ABEqual to 0.001033cm2/s。
Application comparative example 1
In the actual oil production process, pairs are usedDiffusion coefficient D 'obtained from proportion 1'AB0.001033, the time to carbon dioxide equilibrium in crude oil is predicted to be 352 days, whereas in practice carbon dioxide equilibrium in crude oil is predicted to be 465 days.
Comparing the data of application example 1 and application comparative example 1, the diffusion coefficient measured by the method of the invention is more accurate, the predicted time for carbon dioxide to reach the equilibrium in crude oil is closer to the actual equilibrium time, and compared with the measurement method in the prior art, the method of the invention can provide more accurate theoretical basis for oil recovery.
Having described embodiments of the present invention, the foregoing description is intended to be exemplary, not exhaustive, and not limited to the disclosed embodiments. Many modifications and variations will be apparent to those of ordinary skill in the art without departing from the scope and spirit of the illustrated embodiments.
Claims (7)
1. A method for determining the diffusion coefficient of carbon dioxide in crude oil, comprising the steps of:
1) to volume of VCIs filled into the closed container0A volume of crude oil of which V0＜VC；
2) Keeping the temperature of the closed container filled with the crude oil in the step 1) constant at a measured temperature T;
3) filling carbon dioxide gas into the constant-temperature closed container in the step 2), and starting from the initial time t0Measuring the pressure P (t) of carbon dioxide gas at a time interval of Δ t until an equilibrium pressure is reached, wherein at an initial time t0Has a pressure of P (t) as carbon dioxide gas0)；
4) The expansion coefficient beta of the crude oil dissolved with the carbon dioxide is combined with the relation between the diffusion time t and the pressure P (t) to obtain the diffusion coefficient D of the carbon dioxide in the crude oilAB；
The formula according to step 4) is:
wherein Z isgIs the compression factor of carbon dioxide, R is the universal gas constant, xeqThe equilibrium interface concentration of carbon dioxide at the oil-gas interface is shown, and A is the sectional area of the rock core.
2. The method of claim 1, wherein the method of measuring the coefficient of expansion β comprises:
1) determining the volume V of the liquid phase at the bubble point pressure P of crude oils containing different amounts of carbon dioxideL；
2) By the formula VL/Vdβ P +1, where V gives the expansion coefficient βdIs the volume of crude oil without carbon dioxide.
3. The method of claim 1, wherein the compression factor ZgThe PVT sample kettle is adopted for measurement, and the state equation P is obtainedgV＝ZgCalculating nRT.
4. The method of claim 1, wherein x iseqAccording to the formula
Is calculated to obtaineqThe pressure in the closed vessel is in an equilibrium state.
5. The method according to any one of claims 1 to 4, wherein the method employs a testing device comprising: a test closed container (15), a carbon dioxide closed container (14), a crude oil closed container (29), a vacuum pump (21), a constant temperature box (16), a pressure sensor (17) and a data processing device (24),
the carbon dioxide closed container (14) and the crude oil closed container (29) are respectively connected to the testing closed container (15), the carbon dioxide closed container (14) and the testing closed container (15) are arranged in the constant temperature box (16), the vacuum pump (21) is used for vacuumizing the testing closed container (15), and the pressure sensor (17) is used for measuring the pressure of the testing closed container (15) and transmitting a pressure signal to the data processing device (24).
6. The method according to claim 5, wherein the testing device further comprises a carbon dioxide feed pump (22) and a crude oil feed pump (23) connected to the carbon dioxide containment vessel (14) and crude oil containment vessel (29), respectively.
7. The method according to claim 5, wherein said testing device further comprises a temperature sensor (18) arranged on said oven (16).
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| CN111879666B (en) * | 2020-07-31 | 2022-07-15 | 西南石油大学 | High-temperature ultrahigh-pressure oil-gas reservoir fluid interfacial tension and contact angle testing device |
| CN112198093B (en) * | 2020-10-09 | 2022-08-12 | 中国石油大学(华东) | Device and method for testing diffusion coefficient of gas in saturated live oil core |
| CN112630090B (en) * | 2020-12-08 | 2022-09-06 | 中国石油大学(华东) | Method for calculating diffusion coefficient of methane-carbon dioxide-propane mixed gas by considering volume expansion of thickened oil |
| CN113008739B (en) * | 2021-03-23 | 2022-06-21 | 中国石油大学(华东) | Method for determining gas diffusion coefficient under heavy oil thermal recovery condition |
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