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SPE-129517-STU Comparative PVT Simulation: An Application to Australasian Fluid Samples

D.I. OReilly, SPE, Australian School of Petroleum, U. of Adelaide


This paper was prepared for presentation at the 2009 SPE International Student Paper Contest at the SPE Annual Technical Conference and Exhibition held in New Orleans, Louisiana, USA, 47 October 2009. This paper was selected for presentation by merit of placement in a regional student paper contest held in the program year preceding the International Student Paper Contest. Contents of the paper, as presented, have not been reviewed by the Society of Petroleum Engineers and are subject to correction by the author(s). The material, as presented, does not necessarily reflect any position of the Society of Petroleum Engineers, its officers, or members.

Abstract This paper investigates the effectiveness of Equations of State (EOS) when used to simulate Pressure-Volume-Temperature (PVT) experiments. The phase behaviour and volumetrics of six EOS and three EOS modifications (9 models in total) has been examined using a newly developed package inside the MATLAB software. The simulator is an expandable system designed to compare different EOS and fluid characterisation schemes. Comparison will be made between the Soave-Redlich-Kwong (SRK), Peng-Robinson (PR), Adachi-Lu (AL), Patel-Teja (PT), Schmidt-Wenzel (SW) and Esmaeilzadeh-Roshanfekr (ER) EOS, for which the SRK, PR and ER equations optionally include published volumetric shift parameters. Local Australasian fluid samples are studied to illustrate strengths and weaknesses of different EOS, using several fluid types. It was found that the Esmaeilzadeh-Roshanfekr EOS is most accurate for predicting gas-condensate properties, while the original SRK and PR equations remain reliable for oil samples. The purpose of the study is twofold: (1) Increasingly companies are optimising experimental PVT studies by simulating subsequent experiments using EOS1,2, or they are using preliminary simulation to evaluate the need for further experiments. This is particularly true for multi-contact miscibility experiments such as the Rising Bubble Apparatus or slim-tube test, which are timeconsuming and costly. Furthermore, (2) there is reason to believe that thermodynamic models which provide better representation of PVT experiments without matching will perform best after complete matching has occurred. Matching EOS simulation with experiment, known as tuning or regression, is used in industry before application in compositional simulation. Obviously, this is only possible if PVT studies are available. Introduction Some work has been done previously on EOS comparison. Recently, Bonyadi and Esmaeilzadeh3 compared the EsmaeilzadehRoshanfekr EOS against the popular Peng-Robinson EOS for gas-condensates. This was done in a purely predictive manner, i.e. no EOS tuning took place before simulation begun. It was reported that the ER equation was superior for saturation pressure predictions and had lower average deviation on PVT experiment simulation. Ahmed4 compared 8 EOS in a semi-predictive fashion; each EOS was matched to a known saturation pressure before the simulation of PVT experiments started. Again, gas-condensates were chosen for the study. It was reported that certain EOS were advantageous in different areas: compressibility factors were best represented by the PT and SW equations of state, phase compositions were best predicted by the PR equation and the volumetric behaviour of condensates was best predicted by the SW equation. Martin5 considered pure petroleum components and compared EOS. From the Australian School of Petroleum, Beinke6 compared different EOS in the compositional simulation of CO2 sequestration. There are many more examples in the literature7-9 where EOS are compared. The findings all highlight the fact that there is currently no all in one EOS that will favourably predict all thermodynamic properties. It seems that some EOS can outperform others only for certain reservoir fluid types, and some EOS are advantageous for particular properties, e.g. the PR EOS for superior phase compositions. This may also lead to entire PVT experiments being better represented by particular EOS, as is suspected. These are all subtle points for the engineer to consider when modelling fluids under either limited data or laboratory PVT experiment appraisal. Often the peculiarity of phase behaviour (e.g. in the near-critical area, for oil-CO2 systems under asphaltene precipitation or for oil with significant non-hydrocarbon components3,15,36) can encourage the development of EOS which are hoped to increase this accuracy of predictive simulation. The objective of this study is thus to compare the new and old EOS, using a larger and more comprehensive set of samples than those already present in the literature. There will be 7 case studies, comprising of six new samples from South Australian oil companies and one previously published oil sample. A spectrum of fluids is studied: Oil, volatile oil, gas condensates and gas. These will provide a small survey of Australian fluid types from currently producing fields. In some instances, practical applications of EOS are also considered in addition to the comparison aspect, according to which company provided the sample and their interests.

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Details of Simulator This section will provide an overview of the new simulator programme and algorithms used to solve phase-behaviour problems. It will then review the studied EOS and their modifications. Selected methods for plus fraction (e.g. C7+) characterisation will be outlined at the end of the section. Comments are as brief as possible, as the purpose of this paper is not to review phase behaviour mathematics but rather summarise results of simulation using the new programme. A screen capture of a running script in an early version of the programme is seen in Fig. 1. Part 1 Phase behaviour algorithms The last 30 years have seen immense improvement in phase behaviour modelling using EOS. Through experience, reliable methods now exist for the prediction of phase equilibrium under even the most complex of conditions, e.g. close to the phase boundary or nearcritical conditions. These established methods have been coded into the current package. For two-phase flash calculations, a combined tangent plane stability analysis method10 is used to initialise the traditional flash calculation strategy11. For saturation pressure or temperature, stability analysis is further utilised to solve for points on the phase boundary12. Phase envelopes (either for PressureTemperature or Pressure-Composition/Swelling) are solved iteratively using extrapolated initial guesses from previous points13. This method also allows for an interpolated calculation of the critical point of a mixture. To ensure rapid convergence it was necessary to use a combination of numerical methods: first Quasi Newton Successive Substitution (QNSS)14, and under slow convergence a switch can be made to the full Newton-Raphson non-linear equation solver. Fig. 2 presents an example case where the automated switch is necessary a near-critical flash on a petroleum mixture. Use of successive substitution alone would have seen inadequate convergence nearby the critical point. Michelsen and Mollerup15 have provided an excellent reference on all of these topics. Table 1 summarises core functions of the programme. The simulation of PVT experiments is a logical step after the foundation of a simulator has been developed. Inbuilt are the following experiments: Constant Composition Expansion (CCE) Differential Liberation (DL) Constant Volume Depletion (CVD) Swelling Test (ST) Minimum Miscibility Pressure16 (MMP) Phase envelope/critical point calculation

(There are currently more accurate simulation methods for MMP prediction using EOS but these lie outside the scope of this work.) MATLAB is a particularly useful environment to code the algorithms because of its native vector and matrix handling. This allows easy manipulation of composition vectors, property vectors and Jacobian matrices. It does, however, suffer from slower run-times than properly compiled code using an established language such as C or Fortran (most PVT simulators are written in the latter). The ease of coding and inbuilt matrix handling far outweighed this problem, however. Furthermore, several non-linear regression algorithms are packaged with the product and these become particularly useful for regression of laboratory PVT data using EOS. The least-squares non-linear equation minimisation tool (lsqnonlin) was used for this purpose. Validation of the programme was a continual process. This involved comparison with textbook examples, commercial simulators (CMG WinProp, Schlumberger PVTi and Tie-Line Tech MI-PVT), historically published data and new reservoir fluid data from the literature. One particular validation tool was the methane-ethane mixtures of Bloomer et al17. Fig. 3 presents the comparison between SRK calculated phase envelopes and experimental data for these mixtures. They are in good agreement, as should be expected. Some more validation will be discussed in the following sections. Part 2 Examined Equations of State Six cubic EOS have been studied, three of which include volume-shift modifications. The unmodified two-parameter equations are: Soave-Redlich-Kwong18 (SRK) 1972 Peng-Robinson19,20 (PR) 1978 Adachi-Lu21 (AL) 1984

and the unmodified three-parameter equations are: Schmidt-Wenzel22 (SW) 1980 Patel-Teja23 (PT) 1982 Esmaeilzadeh- Roshanfekr24 (ER) 2006

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Volumetric shift modification is optionally applied to the SRK, PR and ER equations25-27, adding an extra parameter to the original EOS. It will be of interest to see whether the newer EOS provide many benefits over the older established SRK and PR equations, used most commonly in industry calculations. At this stage it should be noted that the Adachi-Lu EOS is mostly included for interests sake and is only a minor modification of the original van der Waals EOS. Accurate behaviour of complex reservoir fluids is not expected. Part 3 Heavy end characterisation and tuning An important first step in EOS simulation is the characterisation of the pseudocomponent, Cn+, fraction. This fraction is the last temperature cut from which distillation ceases. The input data for EOS models is usually the critical temperature and pressure (Tc and pc) and acentric factor () of each component, along with other properties for more complicated EOS. Usually these properties are known for pure components (<C6), but will not be known for heavier fractions and must be estimated using correlations. There are many different strategies available in the literature. For components of unknown properties, these case studies will use the correlations of Sreide28 for boiling temperature Tb, Twu29 for Tc and pc and Lee-Kesler30 for . Input parameters for the correlations are usually the molecular weight (MW), and specific gravity (S.G.) of the fraction, and it is assumed that these are available from laboratory data. The correlations are known to provide reasonable accuracy. Depending upon fluid type, this work may use one of several approaches to describe the heavy end. One approach is to simply represent the Cn+ fraction as a single component using the correlations described above. Another method is to hypothetically split the Cn+ fraction into multiple Single Carbon Number (SCN) groups and assign each SCN critical properties as described above. A third approach is to split the pseudocomponent into SCNs and later recombine these SCNs into a few Multiple Carbon Number (MCN) groups, reducing the number of components used. These different methods are powerful for different fluid types and their use will be highlighted as seen necessary. The last step in characterisation is to refine the critical properties of the extended fractions. This is often done through EOS matching (tuning or regression). If sufficient data is available for the sample fluid, this work will extend on the semi-predictive4 methodology discussed in the introduction, by matching an entire CCE experiment before subsequent PVT experiments are simulated. Often Tc and pc of the extended components will be selected as regression variables to match the density measurements and saturation pressure of the CCE experiment. Each example fluid, however, will vary slightly in regression strategy. It will be possible to ascertain how each EOS performs for subsequent experiments after tuning to the first experiment. This characterisation methodology may be summarised as: 1. 2. 3. 4. 5. Using composition data for pure components, assign pure component properties from the literature Keep the pesudocomponent as one fraction or split, depending upon fluid type. Split SCNs may then be recombined into MCNs. Assign properties to these fraction/s using the discussed correlations28-30 Match a CCE experiment (density and saturation pressure) if possible by refining the values of these extended fractions through regression Simulate subsequent experiments

Some extra validation was necessary to ensure appropriate coding of the simulator and these extended fraction correlations. The recently published fluids of Jaubert, Avaullee and Souvay31 were all tested during early stages of simulator development. Fig. 4 and Fig. 5 display simulation results for two oil samples. Fluid F2 only contained CCE and MMP data, whereas F3 was much more comprehensive. In each case the fluids were modeled using 3 MCNs representing the C7+ fraction and Tc and pc of these MCNs were set as regression variables for CCE experiment matching. Comparison of EOS emerges through simulation of subsequent experiments. In F2 it is interesting to see that different EOS can be matched to the same data but can result in vastly different phase envelopes. We must exercise caution when observing new simulation from a tuned EOS. Case Studies Six case studies have been undertaken using samples provided by oil companies (Beach Petroleum Ltd and Santos Ltd) and a PVT service company (Petrolab Pty Ltd). A seventh published miscibility study is also considered. This section employs the use of absolute average deviations (AAD) for quantitative comparison of EOS simulation and PVT experiment. Each case study is accompanied by an AAD table. In one case, the use of EOS is compared with a newly published correlation. In other cases, EOS are used to check the quality of fluid samples. In all cases EOS are compared with each other.

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Case 1 Petrolab black oil We begin with a black oil sample taken from a New Zealand reservoir, supplied by Petrolab Pty Ltd. A CCE and DL experiment were available. Distillation data was available until C20+, and this component was extended until C80. All components were included as SCNs until C10, and SCN11-80 were grouped into 5 MCNs. Each EOS was tuned to the entire CCE experiment using grouped multipliers for Tc and pc of all components larger than nC5. Results of simulation follow in Fig. 6. AADs appear in Table 2. All six EOS are included in this simulation, the SRK and PR including shift factors (labelled SRK3 and PR3). From the figures and AAD table it is seen that the PR3 equation performs best for every simulated property, both in CCE and DL experiments. Global density in the CCE and liquid densities in the DL experiment are well represented by the SW equation, although there is less accuracy in gas Z-factors. The ER equation is very strong in this area, most likely because this EOS has been designed for the very purpose of gas reservoirs. The unmodified three-parameter EOS (PT, ER, SW), in general, do not perform as well as the PR3 or SRK3 equations for this black oil. Case 2 Petrolab gas-condensate This case study tests the use of unmodified 3-parameter EOS in condensate fluids. The gas-condensate sample is CO2-rich and has been taken from a South Australian reservoir. Composition data is available until C12+, which is left as a single pseudocomponent in the EOS model. SCNs from C6 onwards are assigned standard properties for the temperature cuts. Critical temperatures of extended components in the mixture, C6-C12+, were selected as regression variables for matching of the original CCE experiment. It was initially thought that BICs (Binary Interaction Coefficients) between heavier components and CO2 may need adjustment but erroneous results and high regression multipliers resulted in the change of methodology. The CCE experiment was then adequately matched. A subsequent CVD experiment has been simulated and compared with experimental data. Fig. 7 and Table 3 present simulation and AADs respectively. All six EOS are compared in this example. For the original CCE experiment, the unmodified SRK equation fits liquid densities best. Equations predict cumulative gas production in the CVD test very well. The ER4 and PT equations are considerably better for liquid dropout although the SRK equation follows Z-factor data (single and two-phase) more closely. This sample may have been complicated by the high proportion of CO2, but the ER4 and other 3-paramater EOS begin to show strong promise for condensate studies. Case 3 Bon, Emera and Sarma32 oil data Oil A from a South Australian reservoir has been sampled to investigate the effect of normal-pentane (nC5) on MMP. PVT data on the original oil was not included and therefore these calculations are purely predictive, unlike others seen in this paper. MMPs for the oil combined with several different gases at different temperatures were provided. A correlation for MMP was also proposed by the authors. The plus fraction for this example remained as one pseudocomponent and the standard correlations were assigned. A plot of the miscibility criterion used is shown in Fig. 8 for one case, using the SRK EOS. The calculated MMP for different gases and temperatures is tabulated in Table 4. In this case the 2-parameter equations (PR and SRK) strongly outperformed 3-parameter equations (PT, SW and ER). The 3-parameter equations were over 500psia in error in most cases, and thus only the PT EOS has been tabulated. It is suspected that these problems may arise from either the predictive nature of this problem, inaccurate BICs used in the model (ER equation currently has none published), or general troubles these EOS seem to have with heavier oils. 3-parameter equations are not always poor for MMP however, as it has been recently reported that the ER equation outperforms others for condensate miscibility studies33. It is interesting to note that the unmatched PR and SRK EOS are not as accurate as the published correlation, particularly at higher temperatures. Matching the EOS to saturation pressure at each temperature would have been beneficial. In conclusion, it seems that the PR and SRK equations work best for this oil sample. Case 4 Beach Petroleum crude oil The first sample from Beach Petroleum is a low bubble point oil sampled from a Permian formation in a South Australian reservoir, rich in intermediate components. The fluid was withdrawn from a DST apparatus and the company is interested in testing the integrity of their sample through the use of EOS (the PVT studies are done on the DST sample only). Sample quality will thus be tested in addition to EOS comparison. Fortunately, detailed distillation information was available and the crude was characterised using SCNs until SCN33. These were not combined into MCNs, although if a sufficient number of groups were used, accuracy would not have been affected. It will be of interest to test how the unmatched EOS simulate reservoir bubble point pressure using two composition models: (1) The original DST composition and (2) a recombined surface sample composition. The only experimental saturation pressure available is from the DST sample (Pb=212.7psia) and this is compared against the both unmatched EOS models in Table 5. One immediate conclusion is that all EOS are quite close to DST bubble point pressure when considering the EOS modeled using original DST sample composition. The second conclusion is that the recombined surface samples simulate bubble point pressure only slightly lower than the DST PVT experiment. This is pertinent to quality assurance of the DST sample.

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A second approach for quality assurance involves matching an entire CCE experiment for the DST sample (using the DST sample composition, of course) and flashing the mixture to surface conditions. The flashed composition may then be compared against surface samples. This approach appears in Fig. 9. The tuned CCE experiment is first shown above a plot of flashed liquid compositions. Firstly, we note that all EOS flash to similar compositions. Secondly, we note there are some minor differences between EOS and surface composition, but the trend is quite close. For the crude it was seen that different EOS present extremely similar simulations and that there is most likely a reasonable representation of reservoir fluid by the DST sample. Case 5 Beach Petroleum gas A gas sample from a South Australian Permian formation is now analysed using six EOS. The gas is CO2-rich and has only slight liquid-dropout during depletion. Much like Case 2, characterisation will use SCNs until C12+, where all unknown fractions are assigned properties using the standard correlations. CCE and CVD experiments were available. It was decided that the entire CCE experiment would be matched by the adjustment of Tc of each higher fraction using a single multiplier. Resultant simulations are seen in Fig. 10, with AADs in Table 6. The phase envelope verifies the small liquid dropout. A separator flash simulation at the marked point also confirmed phase compositions within reasonable accuracy. All six EOS (apart from Adachi-Lu) deliver similar results for the subsequent CVD simulation in all properties. Again, the cumulative gas curve is simulated well but problems arise for densities and Z-factors. Unfortunately none of the EOS seem to simulate gas Z-factor data appropriately. Regression of the CCE saturation pressure and densities must not have described this area adequately. The modified PR3 equation performs best on average but these differences are only minor and not particularly conclusive. Case 6 Santos volatile oil A high-temperature, volatile oil from the Cooper basin was supplied by Santos. Composition data was available until C11+, which was extended and grouped into 3 MCNs. SCN6-SCN10 were left as single components. Critical temperature and pressure of each component above nC5 were selected as regression variables for the entire CCE experiment. Two experiments were available: CCE and CVD. The six EOS are compared in Fig. 11, with deviations reported in Table 7. It was easiest to tune the CCE experiment using the SRK3 equation, but the Esmaeilzadeh-Roshanfekr-4 EOS best predicted the CVD liquid volume afterwards. The PR3 equation best represents CVD gas Z-factors (although all EOS exhibit problems in this area), while the PT equation simulates cumulative gas volume well. The Schmidt-Wenzel EOS seems to, on average, capture all of the behaviour. This fluid is an interesting example as each EOS has shown strengths and weaknesses. Because the sample is a volatile oil combining liquid and gas properties, its behaviour has been similarly represented by many equations. Case 7 Santos gas-condensate The last case study is a CO2-rich condensate from the Cooper Basin, South Australia. Much like Case 2 and 5, the sample was characterised using SCNs until C12+ and components were assigned properties from the standard correlations. A CCE and CVD test were available; the CCE was matched through the adjustment of Tc for each component from SCN6-C12+. All six EOS were used in this study, results appearing in Fig. 12. The success of the modified 4-parameter Esmaeilzadeh-Roshanfekr EOS is confirmed again for gas-condensates, with close reproduction of the liquid dropout curve. The other unmodified 3-parameter equations (PT and SW) also perform well for this sample. The SRK3 and PR3 equations are slightly better in density and Z-factors, but fail to reproduce liquid dropout as well as other equations. The trend has emerged that the unmodified 3-parameter equations (and modified 4-parameter Esmaeilzadeh-Roshanfekr EOS) are best for condensate studies. Discussion The study has shown that there is value in using newer EOS along with those available in commercial packages, such as Schlumberger Eclipse, CMG WinProp or Tie-Line Technologies MI-PVT. Computer programming of phase equilibrium problems in MATLAB is not time consuming and allows engineers to take advantage of more precise PVT predictions in several practically important cases. It has been shown that, particularly in the case of gas condensates, several EOS are superior when compared to the most common industry equations (SRK and PR). The developed software could be applied in reservoir studies where the recovery and exploitation strategy is highly related to PVT predictions, e.g. partly miscible gasflooding34,35, CO2 injection under asphaltenes precipitation34-36, non-isothermal waterflooding with paraffin deposition36,37, etc. Phase behaviour properties, as represented by Equations of State, are most important to the economics of these projects.

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Conclusion Mathematical modelling of phase behaviour and volumetrics using six different equations of state and comparison with laboratory PVT data led to the following conclusions: 1. Gas-condensates are best represented using the unmodified 3-parameter equations studied: Patel-Teja, Schmidt-Wenzel and Esmaeilzadeh-Roshanfekr. The new Esmaeilzadeh-Roshanfekr EOS showed minimum deviation from laboratory data for gas-condensate studies. 2. Conventional oil phase behaviour is most reliably predicted using the original Soave-Redlich-Kwong or Peng-Robinson equations. For volatile oils, the unmodified 3-parameter equations also predict well. 3. Low bubble point oils rich in intermediate components, in general, seem relatively insensitive to the type of EOS used. Nomenclature AAD = Absolute Average Deviation AL = Adachi-Lu EOS BIC = Binary Interaction Coefficient CCE = Constant Composition Expansion CVD = Constant Volume Depletion DL = Differential Liberation DST = Drill Stem Test ER = Esmaeilzadeh-Roshanfekr EOS ER4 = Esmaeilzadeh-Roshanfekr w/ volume shift MCN = Multiple Carbon Number MMP = Minimum Miscibility Pressure MW = Molecular Weight PR = Peng-Robinson EOS PR3 = Peng-Robinson EOS w/ volume shift PT = Patel-Teja EOS PVT = Pressure-Volume-Temperature SCN = Single Carbon Number SG = Specific Gravity SRK = Soave-Redlich-Kwong EOS SRK3 = Soave-Redlich-Kwong EOS w/ volume shift ST = Swelling Test SW = Schmidt-Wenzel EOS Cn+ pc psat Tb Tc Vrel x y z Z2phase Zg l = = = = = = = = = = = = = = Last pseudocomponent from distillation Critical pressure (mixture or component) Saturation pressure (bubble or dew) Boiling temperature Critical temperature (mixture or component) Relative volume (Vrel=V/Vsat) Liquid composition vector Gas composition vector Total composition vector Z-factor of gas and liquid phases Z-factor of gas phase Total density Liquid density Acentric factor

Acknowledgements Many thanks are due to Prof. Hemanta Sarma, Dr. Mofazzal Hossain and Prof. Pavel Bedrikovetsky (U. of Adelaide) for their encouragement and useful discussions. I also thank Jan Bon and Jan G. Bon (Petrolab), Mark Pitkin (Beach Petroleum), Paul Lyford and Peter Clark (Santos) for the contribution of fluid samples.

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References 1. Toulekima, S.B., Clark, P.B. and Sarma, H.K.: A Miscibility Scoping Study for Gas Injection into a High-Temperature Volatile Oil Reservoir in the Cooper Basin, Australia, SPE paper 116782 to be presented at APOGCE held in Perth, Australia, October 20-22, 2008. 2. Williams, C.A., Zana, E.N. and Humphrys, G.E.: Use of the Peng-Robinson Equation of State to Predict Hydrocarbon Phase Behavior and Miscibility for Fluid Displacement, SPE paper 8817 presented at First Joint SPE/DOE Symposium on Enhanced Oil Recovery held in Tulsa, Oklahoma, April 20-23, 1980. 3. Bonyadi, M. and Esmaeilzadeh, F.: Prediction of gas condensate properties by Esmaeilzadeh-Roshanfekr equation of state, Fluid Phase Equilibria, pp326-334, August 2007. 4. Ahmed, T.: Comparative Study of Eight Equations of State for Predicting Hydrocarbon Volumetric Phase Behavior, SPE Reservoir Engineering, pp337-348, February 1988. 5. Martin, J. J.: Cubic Equations of State Which?, Ind. Eng. Chem. Fundam., 18(2), pp81-97, 1979. 6. Beinke, J.: A Code Comparison of Numerical Simulators for CO2 Geo-Sequestration, Honours Thesis, Australian School of Petroleum, October 2007. 7. Weng, W.L. and Lee, M.J.: Vapor-liquid equilibria for nitrogen with 2-methyl-1-pentanol, 1-octanol, or 1-decanol binary systems, Fluid Phase Equilibria, Vol. 122, pp243-253, 1996. 8. Sing, B.P.: A comparison of equations of state including the generalized Rydberg EOS, Physica B, Vol. 369 , pp111-116, 2005. 9. Coats, K.H. and Smart, G.T.: Application of a Regression-Based EOS PVT Program to Laboratory Data, SPE Reservoir Engineering, pp277-299, May 1986. 10. Michelsen, M.L.: The isothermal flash problem. Part I. Stability, Fluid Phase Equilibria, Vol. 9, pp1-19, 1982. 11. Michelsen, M.L.: The isothermal flash problem. Part II. Phase-split calculation, Fluid Phase Equilibria, Vol. 9, pp21-40, 1982. 12. Nghiem, L.X., Li, Y.-K., and Heidemann, R.A.: "Application of the Tangent Plane Criterion to Saturation Pressure and Temperature Computations," Fluid Phase Equil., Vol. 21, pp39-50, 1985. 13. Michelsen, M.L., "Calculation of Phase Envelopes and Critical Points for Multicomponent Mixtures," Fluid Phase Equilibria, Vol. 4, pp1-10, 1980. 14. Nghiem, L.X., and Heidemann, R.A.: "General Acceleration Procedure for Multiphase Flash Calculation With Application to Oil-Gas-Water Systems," paper presented at the 2nd European Symposium on Enhanced Oil Recovery, Paris, France, November 8-10, 1982. 15. Michelsen, M.L. and Mollerup, J.M., Thermodynamic Models: Fundamentals & Computational Aspects, Tie-Line Publications, 2nd edition, Denmark, 2007. 16. Ahmed, T.: A Generalized Methodology for Minimum Miscibility Pressure, SPE paper 39034 presented at the 5th Latin American and Caribbean Petroleum Engineering Conference and Exhibition, Rio de Janeiro, Brazil, August 30-September , 1997. 17. Bloomer, et al., Institute of Gas Technology Research Bulletin 22, Institute of Gas Technology, Chicago, 1953. 18. Soave, G.: "Equilibrium Constants from a Modified Redlich-Kwong Equation of State," Chem. Eng. Sci., Vol. 27, pp11971203, 1972. 19. Peng, D.Y. and Robinson, D.B.: A New Two-Constant Equation of State, Ind. Eng. Chem. Fundam., 15(1), pp59-64, 1976. 20. Robinson, D.B, and Peng, D.Y.: "The Characterization of the Heptanes and Heavier Fractions for the GPA Peng-Robinson Programs," Gas Processors Association, Research Report RR-28, March 1978. 21. Adachi, Y. and Lu, B.: Simplest Equation of State for Vapor-Liquid Equilibrium Calculations: A Modification of the van der Waals Equation, AIChE J., Vol. 30(6), pp991-993, Novemeber 1984. 22. Schmidt, G. and Wenzel, H.: A Modified van der Waals Type Equation of State, Chem. Eng. Sci., Vol. 135, pp1503-1512, 1980. 23. Patel, N. C. and Teja, A. S.: A New Cubic Equation of State for Fluids and Fluid Mixtures, Chem. Eng. Sci., Vol. 37(3), pp462-473, 1982. 24. Esmaeilzadeh, F. and Roshanfekr, M.: A new cubic equation of state for reservoir fluids, Fluid Phase Equilibria, Vol. 239, pp83-90, 2006. 25. Peneloux, A., Rauzy, E. And Freze, R.: A Conistent Correction for Redlich-Kwong-Soave Volumes, Fluid Phase Equilibria, Vol. 8, pp7-23, 1982. 26. Jhaveri, B. S., and Youngren, G.K.: Three-Parameter Modification of the Peng-Robinson Equation of Sate to Improve Volumetric Predictions. SPE paper 13118, presented at the SPE Annual Technical Conference, Houston, September 1619, 1984. 27. Esmaeilzadeh, F. and Samadi, F.: Modification of Esmaeilzadeh-Roshanfekr equation of state to improve volumetric predictions of gas condensate reservoir, Fluid Phase Equilibria, Vol. 267, pp113-118, 2008.

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28. Sreide, I.: Improved Phase Behavior Predictions of Petroleum Reservoir Fluids From a Cubic Equation of State, Dr.Ing. dissertation, Norway Inst. Of Technology, Trondheim, Norway, 1989. 29. Twu, C.H.: "An Internally Consistent Correlation for Predicting the Critical Properties and Molecular Weights of Petroleum and Coal-Tar Liquids," Fluid Phase Equilibria, Vol. 16, pp137-150, 1984. 30. Lee, B.I., and Kesler, M.G.: "A Generalized Thermodynamic Correlation Based on Three-Parameter Corresponding States," AIChE J., Vol. 21, pp510-527, May 1975. 31. Jaubert, J., Avaullee, L. and Souvary, J.: A crude oil data bank containing more than 5000 PVT and gas injection data, Journal of Petroleum Science and Engineering, Vol. 34, pp65-107, 2002. 32. Bon, J., Emera, M.K. and Sarma, H.K.: An Experimental Study and Genetic Algorithm (GA) Correlation to Explore the Effect of nC5 on Impure CO2 Minimum Miscibility Pressure (MMP), SPE paper 101036 presented at APOGCE held in Adelaide, Australia, 11-13 September, 2006. 33. Esmaeilzadeh, F. and Roshanfekr, M.: Calculation of minimum miscibility pressure for gas condensate reservoirs, Fluid Phase Equilibria, Vol. 249, pp75-81, 2006. 34. Lake, L.W., Enhanced Oil Recovery, Prentice Hall, New Jersey, 1996 35. Bedrikovetsky P.G., Mathematical Theory of Oil & Gas Recovery (With applications to ex-USSR oil & gas condensate fields), Kluwer Academic Publishers, London-Boston-Dordrecht, 1993. 36. Danesh, A., PVT and Phase Behaviour of Petroleum Reservoir Fluids, Elsevier Science, The Netherlands, 1998. 37. Green, D.W. and Willhite, G.P., Enhanced Oil Recovery, SPE series, Texas, 1998.

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Figure 1: EOS programme running in MATLAB

Figure 2: Near-critical flash simulation for petroleum mixture (PR EOS)

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Function name eosroot stabilitytest flashpt saturation_p saturation_t diag_pt diag_pz QNSS newton regression CCE CVD DL Swell MMP

Input z, p, T z, p, T z, p, T z, T z, p z z1, z2, T 0 0 PVT data z, p, T z, p, T z, p, T z1, z2, T z1, z2, T

Output , Z Stability, K0 x, y, F, Z Pb or Pd Tb or Td Phase diagram Phase diagram Tuned EOS All properties All properties All properties Sat pressures pmulti-contact-miscible

Comment Solve EOS at specified p & T Stability test Two-phase flash Saturation pressure Saturation temperature P-T phase diagram P-z phase diagram QNSS solver Newton-Raphson solver Non-linear regression on PVT data Constant Composition Expansion Constant Volume Depletion Differential Liberation Swelling Test Minimum Miscibility Pressure

High-level PVT expt

Low-level

Table 1: Function summary list of custom script system10-16


(Nomenclature: z overall composition vector, x and y liquid and vapour composition vectors, p pressure, T temperature, K equilibrium ratio vector, fugacity coeff. vector, Z compressibility factor, F vapour mole fraction, Pb bubble point pressure, Pd dew point pressure, solution vector, etc.)

Figure 3: Comparison of PVT experiments by Bloomer et al.17 with EOS prediction

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Figure 4: Simulation of Jaubert, Avaullee and Souvay31 F2 (210oF). Note phase envelopes vary considerably.

Figure 5: Simulation of Jaubert, Avaullee and Souvay31 F3 (236.7oF)

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Figure 6: Petrolab black oil (143oF)

Figure 7: Petrolab condensate (254oF)

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AAD for PVT properties CCE DL l Zg global 0.68% 0.71% 1.44% SRK3 0.41% 0.53% 0.13% PR3 1.92% 2.81% 4.12% AL 0.85% 1.02% 0.44% PT 1.05% 1.43% 0.14% ER 0.62% 0.67% 1.05% SW Table 2: Petrolab black oil property deviation

SRK PR AL PT ER4 SW

AAD for PVT properties CVD Liquid Cumulative Z2phase global Dropout Zg gas % 1.71% 1.38% 4.44% 2.14% 3.02% 8.97% 1.71% 4.03% 7.26% 7.73% 13.47% 2.54% 5.76% 9.81% 12.76% 5.60% 1.25% 1.71% 4.77% 5.13% 5.28% 1.17% 0.81% 4.44% 4.85% 5.40% 1.28% 2.47% 4.55% 5.23% Table 3: Petrolab condensate property deviation CCE

Figure 8: Bon, Emera and Sarma32 Oil A-Gas#2 miscibility (60oC) (unmatched)

Table 4: Bon, Emera and Sarma32 Oil A miscibility comparison (EOS not matched with any PVT data)

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Sample (1) DST sample composition (2) Recombined surface sample composition

SRK 192.32 psia

PR 193.35 psia

PT 209.53 psia

ER 214.41 psia

Experiment
212.7psia

175.19 psia

176.04 psia

190.16 psia

194.46 psia

Not done

Table 5: Beach Petroleum oil bubble point pressure from EOS, using either (1) DST sample or (2) recombined surface sample (unmatched with PVT data)
Note: Experimental Pb=212.7psia, from DST sample PVT study

Figure 9: Beach Petroleum oil (213oF): Matched CCE experiment (top) and surface flash using DST sample (bottom)

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Figure 10: Beach Petroleum gas (271oF): PVT experiments (top) and phase envelope simulation after matching, red line indicates CCE expt (bottom) AAD for PVT properties CVD Cumulative Liquid Zg global gas Dropout % 7.23% 0.50% 0.11% 5.46% 6.40% 0.45% 0.12% 4.31% 14.46% 1.64% 0.19% 10.83% 6.83% 0.49% 0.08% 4.87% 7.26% 0.63% 0.08% 5.14% 7.05% 0.50% 0.08% 5.07% Table 6: Beach Petroleum gas property deviation CCE

Z2phase 6.73% 5.58% 12.17% 6.22% 6.50% 6.41%

SRK3 PR3 AL PT ER SW

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Figure 11: Santos volatile oil (285oF)

Figure 12: Santos gas-condensate (250oF)

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AAD for PVT properties CVD Cumulative Liquid Zg global gas Volume % 1.55% 11.16% 3.65% SRK3 0.66% 1.26% 8.96% 2.52% PR3 0.90% 1.00% 0.45% 3.69% 2.76% PT 0.65% 1.93% 2.74% ER4 1.16% 0.70% 0.64% 7.47% 2.81% SW Table 7: Santos volatile oil property deviation CCE

AAD for PVT properties CVD Liquid Cumulative global Dropout Zg gas % 0.60% 0.42% 0.44% SRK3 0.73% 0.63% 0.41% 0.71% PR3 1.07% 3.79% 1.30% 1.09% 11.14% AL 1.02% 0.48% 0.04% 0.92% PT 0.48% 0.03% 1.17% ER4 1.13% 1.07% 0.51% 0.10% 0.92% SW Table 8: Santos gas-condensate property deviation CCE

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