Cricondentherm & Cricondenbar Pressures | Gases | Physical Sciences

The Cricondentherm and Cricondenbar Pressures of Multicomponent Hydrocarbon Mixtures

R O B E R T B. G R I E V E S * GEORGE THODOS

1

NORTHWESTERN V. E V A N S T O N , ILL.

ABSTRACT

A method i s presented for the accurate calculation of the cricondentherm and cricondenbar pressures of multicon~ponenthydrocarbon mixtures of known composition. T h e mixtures may contain s i x and quite possibly any number of components including isopamffins, olefirzs, acetylenes, paraffins, naphthenes and aromatics. T h e approach i s similur t o that used for calculating critical pressures and cricondentherm and cricondenbar temperatures. T h e critical pressure, the normal boiling point and the approximate vapor pressure behavior of each component are all that art required. il stepuiise culculation procedure i s necessary for mixtures containing more than two components. Frorri a n a n a l y s i s of 2 2 binary s y s t e m s and 118 mixtures, the average de~iiatiorz of calculuted cricondentherm pressures from reported values i s 2.4 pvr cent. For nine multicomponent mixtures the average deviation i s 1 per cent. Considering 19 binary s y s t e m s and 108 mixtures, t h e average deviation of calculated cricorzdenbar pressurts from reported v a l u e s i s 1.7 per cent. For 15 multicomponent mixtures, the average deviation i s 2.2 per cent.
INTRODUCTION A knowledge of the p h a s e behavior in the critical region of multicomponent hydrocarbon mixtures i s of value both in industrial processing operations and for the optimum operation of g a s condensate r e s e r voirs. Accurate methods of calculating the critical nd temperatures a n d critical p r e s s u r e s 4 . 6 ~ 7 ~ 8 . 9 ~a2 3 criconden therm and cricondenbar temperatures6p 10 of multicomponent hydrocarbon mixtures a r e a v a i l a b l e in the literamre. If the cricondentherm a n d cricondenbar p r e s s u r e s could b e calculated with equal accuracy, the entire p h a s e diagram of a multicomponent hydrocarbon mixture could b e well approximated. T h e work of E t t e r and Kay6 i s limited to s y s t e m s containing the normal paraffins a n d h a s not been t e s t e d on s y s t e m s
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Original manuscript r e c e i v e d i n S o c i e t y of P e t r o l e u m E n g i n e e r s o f f i c e J a n . 2 7 , 1964. R e v i s e d manuscript r e c e i v e d J u l y 6. 1964. * P r e s e n t a d d r e s s : I l l i n o i s I n s t i t u t e of T e c h n o l o g y , C h i c a g o . 4 ~ e f e r e n c e s i v e n a t e n d of p a p e r . g
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containing a heavier component than heptane. In addition, the development of their multicomponent equations i s b a s e d upon a limited number of mixtures containing from three to s i x components. Silverman a n d tho do^^^ have considered s y s t e m s containing both paraffinic a n d non-paraffinic hydrocarbons, but their correlation i s limited to binary s y s t e m s a n d i s highly inaccurate for methane s y s t e m s . E i l e r t s 5 h a s done e x t e n s i v e work on the cricondenbar p r e s s u r e ; h e h a s produced an excellent correlation for binary s y s t e m s . However, h i s procedure for multicomponent mixtures i s chiefly useful for highly complex mixtures requiring a knowledge of the vapor-liquid equilibrium behavior of the mixtures; h e h a s not considered the cricondentherm pressure. The objective of t h i s study w a s the development of a n a c c u r a t e a n d rapid method for the calculation of the cricondentherm a n d cricondenbar p r e s s u r e s of multicomponent mixtures containing a l l types of hydrocarbons a n d having a wide volatility range. T h e approach t h a t w a s adopted i s similar to that u s e d by Grieves a n d Thodos for cricondentherm a n d cricondenbar temperatures l o and for critical p r e s s u r e s . 9 However, methane s y s t e m s had to b e considered separately a n d a modified s t e p w i s e calculation procedure w a s utilized for the cricondertherm pressure. T h e correlations were developed in a manner similar to t h o s e for critical p r e s s u r e s a n d cricondentherm and cricondenbar temperatures. B a s e d upon binary data reported in the literature i t w a s observed that the r a t i o s of cricondentherm and cricondenbar pressure to the pseudocritical pressure (molar average), pL / p p c and pp / p p c , respectively, in twocomponent s y s t e m s depended upon the mole fraction of the low-boiling component a n d upon the diversity in properties o f t h e two components. A dimensionless boiling-point parameter T i, / T b w a s chosen to represent the diversity in properties of the components. For a binary s y s t e m , T i , ' i s the molar average of the normal boiling points of the two components involved. For a multicomponent system i t i s either the molar average of the normal boiling points of a l l of t h e components involved or the molar average of the normal boiling point of the pure low-boiling component a n d of the atmospheric boiling point of the low-boiling-free mixture of
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no correction i s needed. in which the parameters are the mole fraction of methane.7 per cent.25 per cent. 1 and 2. 1. For systems containing an acetylene. /Tb i s presented a s Fig. For the 10 systems and 53 mixtures the average deviation of cricondentherm pressures calculated with Fig. the normal boiling point and perhaps one additional point are all that are required. Tb i s the boiling point of the mixture a t atmospheric pressure. naphthenes and aromatics. For five systems and 30 mixtures containing acetylenes.1 . pp/ppc. 2 . The parameters are the mole fraction of the lowboiling component in the mixture. the average deviation of calculated values from reported values i s 2. a naphthene. / FIG. the vapor pressures and mole fractions are then substituted into Eq. 1 and 2 should be multiplied by the factors in Table 1 to give the correct value to be used in finding pl. 1 .RELATIONSHIP BETWEEN pt/ppc AND Tb FOR METHANE SYSTEMS. a stepwise calculation procedure i s necessary for p t and P p reducing all of the high-boiling components to pseudo-component. For values of ze outside of the ranges indicated.73 per cent. the relationship between the cricondentherm pressure ratio pt /ppc and the boiling-point parameter T i . and the upper limit on T i / T b i s established by the ethane-ndecane system. or an aromatic hydrocarbon a s a component. the critical point. where n i s the number of components. The approximate straight line given by a plot of the logarithm of the vapor pressure of each pure component vs the reciprocal of the absolute temperature i s sufficiently accurate for the evaluation of T b . For multicomponent mixtures.the system. CRICONDENBAR PRESSURE Figs. For the seven available systems and 35 mixtures the average deviation of calculated values from reported values i s 3. and T i /Tb Tb FIG. T / SEPTEMBER.RELATIONSHIP BETWEEN pt /ppc AND T Tb FOR NON-METHANE SYSTEMS. 2. T b i s chosen and the vapor pressures of the components determined. / T b i s established by the methane-n-heptane system. 1 from reported values i s 1. The value of p t / p P c obtained by the normal procedure from Figs. Tb i s arrived a t by a trial-and-error procedure. The maximum deviation for each system i s a l s o included. a correction factor must be applied for u s e with Figs. 196. 1 to s e e if the equality holds. The results for a l l 22 binary systems considered a r e presented a s part of Table 2. BINARY SYSTEMS CRICONDENTHERM PRESSURE Based upon data available in the literature for 10 non-methane binary systems containing paraffins. isoparaffins and olefins. The limit on T i . For such systems the behavior of the cricondentherm pressure ratio does not vary with the difference in boiling point properties of the components in the same manner a s it does for paraffin and olefin systems. A similar relationship for methane systems i s presented a s Fig. calculated from the relation. 3 and 4 present the relationships between the cricondenbar pressure ratio. The procedure i s fully a s~ngle described and example calculations are included in the sections that follow.

289.9 Fig.6 707.7R T b (from Eq.06) = 1.B I N A R Y SYSTEMS I N V E S T I G A T E D A N D C R I C O N D E N T H E R M A N D CRICONDENBAR PRESSURE D E V I A T I O N S Cricondenbar Pressure.22 1.06) = 1. Pc/Ppc = 1.8 (494. EXAMPLE CALCULATION 2 Determine the cricondentherm and cricondenbar pressures of a mixture having the following composition: Mole Fraction Tbi (%) pCj (psia) Ethane Cyclohexane 0. p t No. P t = 1-42 (649.1) + 0.8) = 1. % Mixtures Average Maximum Methane-cyclohexane(27) Ethane-cyclohexone(l6) Ethane -benzene(l7) % = calculated valve reported v a l u e reported value - 100 SOCIETY O F PETROLEUM ENGINEERS J O U R N A L .502 0. of Deviations.2 (707. Reamer. of Deviations. the average deviation for the 46 mixtures i s 1.92 per.79.1 494. 1 and vapor pressure data) = 397R Ppc = 0.6) = 922.Component ocety lene no~hthene arornat ic Range of ze O < z p < 0.502 and TL /Tb = 1. For acetylene.1 591.65 0.2 0.2 and T i / T b = 1. p.zp<0. the average deviation for 32 mixtures i s 1.08 Fig.34(1.34.5) = 649. 1 and 3 a t z e 1. EXAMPLE CALCULATION 1 Determine the cricondentherm and cricondenbar pressures of a mixture having the following c o n position: Mole Fraction T b i (OR) p C j (psia) .4 psia.8) - = 628. together with maximum deviations. naphthene and aromatic systems and 30 mixtures. isoparaffins and olefins. Sage and Lacey28 report values of 632 and 677 psia for this mixture. 665. 1 and 3 a t ze = 0.2<.8 TABLE 2 331.7 637 707./ppc = 1.42.2 i p < 0. The results are included a s part of Table 2.24(536. 1.9.1 p s i a .7) + 0.2) = = 536. the correction factors and ranges of ze presented in the preceding section again apply. P c / p p c = 1. for non-methane and methane systems.17(536. naphthene. % Mixtures Average Maximum System Cricondentherrn Pressure.5 T = 0.1 1. pp/ppc = 1. p p / p p c = 0.498(591. For eight non-methane binary systems containing paraffins.06 1. The parameters are the mole fractions of the lowboiling component and of methane. 1 1.354. and the upper limits on T i / T b are established by the ethane-ndecane and by the methane-n-heptane systems.i) + 0.7 556. Using the correction actors.17. for five acetylene.2 .6 psia From Figs.8 psia From Figs. respectively.2 Tb (from Eq.17 1.C Pn No.79 (1. 1 and vapor pressure data) = 356R Ppc = 0.56 per cent. p p / p p c = 1.498(637) = 483.- Pt Pp = 1. For six methane systems.502(331. 2 1.24. Ethane n-Pentane 0.502(707. respectively.6 p s i a . and aromatic-containing systems.cent .9 z 0.498 331.73 per cent.

6) = 1234. 1 may a l s o b e u s e d for the calculation of p i of a non-methane hydrocarbon mixture containing three or more constituents. . Fig. 196.~FOR METHANE SYSTEMS. Next t h e ternary i s considered and T b i s calculated with Eq. 1 : when ze becomes zero. A s t e p w i s e calculation procedure must be adopted. T h e cricondentherm p r e s s u r e of the binary i s c a l c u l a t e d u s i n g t h e r e l a t i v e (lowboiling-free b a s i s ) mole fractions of the two components to e s t a b l i s h the binary composition. 1. low-boiling component and of the determined cricondentherm p r e s s u r e of t h e heavy binary. the procedure i s the s a m e a s for non-methane s y s t e m s . P a s t h e molar a v e r a g e of t h e CriticafCpressure of the pure. the procedure i s identical to that presented by Grieves and T h o d o s l o for cricondentherm a n d cricondenbar temperatures. a r e c a l c u l a t e d a n d P I determined. T h e r e s u l t s a r e included in T a b l e 3. a n d p i of the ternary for ppc of the quaternary. then. For s y s t e m s containing more than two components. Then. F o r a four component system. 3 . . F o r a ternary s y s t e m . T h e only difference from that given for pi i s in the calculation of T i . ternary. e t c . T b a n d T i .2 psia. FIG. FIG. e x c e p t for the final s t e p in the calculation. e t c . the h e a v i e s t binary i s again considered first.pp = 1. which is somewhat different than t h a t developed by Grieves and T h o d o s 10 for cricondentherm a n d cricondenbar temperatures. .96 per c e n t for both rnethane a n d non-methane mixtures. then the h e a v i e s t ternary and finally the quaternary.244 p s i a for this mixture.1 243 . For multicomponent mixtures containing methane.9 (649. T P b is computed a s the molar a v e r a g e of the normal boiling point of t h e pure low-boiling component a n d of the atmospheric boiling point of t h e high-boiling binary (composition is c a l c u l a t e d b a s e d on low-boiling-free b a s i s ) . Fig.RELATIONSHIP BETWEEN p / p AND T : / Tb FOR NON-METHANE S Y S ~ E ~ S . T h e procedure h a s been t e s t e d on nine synthetic a n d naturally-occurring mixtures containing from three to s i x components. may b e termed a pseudocricondentherm pressure. In e a c h s t e p of the calculation. MULTICOMPONENT MIXTLJRES CRICONDENTHERM PRESSURE Fig. must become t h e a c t u a l cricondentherm p r e s s u r e of t h e mixture of the remaining high-boiling components. ternary. 2 is used. determining p 1 of the binary for p p c of the ternary. T h e criconden therm p r e s s u r e i s then e s t a b l i s h e d from Fig. p I / p p c becomes unity ( a s d o e s T i / T b ) .' / S E P T E M B E R . and p p . T i i s evaluated a s t h e molar average of the normal boiling points of a l l the components involved. for t h e calculation of pi of the required mixture. ' I . p p . 1.RELATIONSHIP BETWEEN p p / p . 1 is used to c a l c u l a t e the cricondentherm p r e s s u r e of the h e a v i e s t binary. AND T. 4 . T b for e a c h s t e p is computed using T b of the h e a v i e s t binary. T h e average deviation i s 0. CRICONDENBAR PRESSURE A slightly modified s t e p w i s e procedure should be employed for the computation of p p for multicomponent mixtures. T h e n e c e s s i t y of a s t e p w i s e procedure i s obvious from Fig. p p . the binary portion c o n s i s t i n g of t h e two high-boiling components is considered first. Kay l 6 r e p o r t s v a l u e s of 950 a n d 1.

pp/pp.6) .665 0.2 p s i a .6 p s i a = + (0.332 508 = 463.03. a n d p p of t h e required quaternary Tb (from Eq.119) = (483.1 491.027. Ternary compositicn: n-butane: . Pp = 1.9) = 474.(%) l - - Pci(psia) = 0.04(526.486(416.4R (Note the u s e of T b c a l c u l a t e d in Section A) PPC Mole Fraction _ ?' b.ll) Methane-ethane-propme n-pentane-n-hexane(1 1) Ethane-propane-n-butane- n-pentane-n-hexane(6) Methane-ethane-propanen-butane -n-pentanen-hexane(6) S O C I E T Y OF P E T R O L E U M E N G I N E E R S JOIJRNAI.1 494.6) + 0.646 and T L / T b = 521.332 0. 3 i s used for non-methane s y s t e m s .665 (494. Fig.646 (491. .p p c . i s calculated in the s a m e manner a s given for cricondentherm p r e s s u r e s .121 + 0. + 416. 1 and vapor p r e s s u r e d a t a ) = 570R p p c = 0. 3 a t z e 0. E s t a b l i s h p i and p binary. n-pentane = 0.121 +0.2) + 0.6R p .3R + 0.235 (556.2) = 559.5 p s i a .2 psia.011.5) 519.03(474) = = 483. Binary composition: n-pentane: .06. p p Number of Average Mixtures Deviation.02.646 (550.4 550.7 1 Propane -n-butane-n-pentane(6) n-B~tane-n-~entane-n-hexane(6) Methane-ethane-propane-n- 1 1 1 2.2) = 528.235 + 0. 3 and 4 for methane s y s t e m s with Fig.9 p s i a .646 0.0 p s i a = Ti. = T.1) + (0.3K T b (from Eq.19 butane(l8) Ethane-propane--n-butane -n- pentane(6) Propane-n-butanen-hexane(6) n-pentane- Methane-ethane-propane n-butane-n-pentane(6.43 3.4 617. pt Number of Average Mixtures Deviation. % 1 System Methane-ethane-n-butane(3) Ethane-propane-n-pentane(6) Cricondenbar Pressure.6 556. EXAMPLE CALCULATION 3 Determine the cricondentherm and cricondenbar p r e s s u r e s of a mixture having the following composition: _ Pt = .0.061 A. a n d pp of the n-butane-n-pentanen-hexane ternary.02(474) 1. a pseudocricondenbar pressure. /Tb 1.332 +0. B. pt/ppc = of the n-pentane-whexane 7. = = = From Fig. Pt/ppc = 1. E s t a b l i s h p. 1 and vapor p r e s s u r e d a t a ) Pt: T i = 0.4 /508 Propane n-Butane n-Pentane n-Hexane 0.332 = 0.6) = 547.7 psia.9 From Fig. 1 and 3 a t z~ = 0. pp/'ppc = 1. 4 u s e d in the l a s t s t e p of the cnlculation.55 1.119 (615.119) (570) = 519.665 (556.45 0.bp = 1. 1 and vapor p r e s s u r e d a t a ) = 442R Pt: From F i g s .6) + 0.235 + 0.M U L T I C O M P O N E N T SYSTEMS I N V E S T I G A T E D A N D C R I C O N D E N T H E R M A N D C R I C O N D E N B A R PRESSURE D E V I A T I O N S Cricondentherm Pressure.4) = 576.121 + 0.04 1.119 508R T b (from Eq. Pt Pp: = 0.335 (433.335 (615.335 = 1. n-hexane = = 0.022. 488.t 0.665 and 7'.84 0.235. For 15 synthetic and naturallyoccurring multicomponen t mixtures t h e a v e r a g e deviation of calculated cricondenbar p r e s s u r e s from reported values i s 2.65 0.486 0. C. % 1 1 1 1 1. E s t a b l i s h p .121 0.121 0.44 3.1) + (0./Tb 1. = 0.2 433.061 Similarly. 0. 0.6/508 n-hexane: ----- 0.646(550.646 (491.121 0.24 per cent.061 0. e x c e p t cricondenbar p r e s s u r e s a r e used for e a c h s t e p following the binary.061 0.1) = 526.061 - = 0. and F i g s .235 + 0. T h e r e s u l t s a r e given in T a b l e 3. 1 a t ZJ = 1.119) (488.061) TABLE 3 .6 61 5.4) 521. = 1.646 and T E. = 0. .6) + (0.06(528.

193(673. 111. 1 0 .471. Technology Center.(Note the u s e of Tb calculated in Section B) Pp: T PPC = 0. psia = critical pressure of pure jth component. George: Jour. H .205 (642) = 773.418 (550. Establish pt and p p of the ethane-n-butane binary.134. = B. OR = molar average boiling point of mixture (method of calculation depends on number of components and whether p t or p p i s being computed). 2.1 psia.11. olefins.486 (617.063.6) + 0. Binary composition: ethane: 0. Bloomer. 22.337 Tbi('%) p p / p p c = 1.4R 351R 0. 62.7 491. T . 65.07 ppc + (0.6) = 360. e l al. 6. Johnson. Institute of -.337) (773.17 p l = 1. 0.6) + 0. E.332(491.193 (200. OR = mole fraction of jth component = mole fraction of low-boiling component = total pressure. Cota. 2 a t zb 0.7 = 587.9 psia. p s i a = cricondentherm pressure of mixture.35 P p = 1.061) 559.337 = 0. psia.332 547.193 and T / T b = 1. Tbi zi Z& From Figs.332 + 0. W.486 and T i / T b = 1. B. C. acetylenes. 1964 = 881. No. F. From Fig.1) = 642 psia. .47 + 0. = 1.1) + 0. Chem.7 331.337) (841) 807. p s i a = atmospheric boiling point of mixture.193 0. PP c = 0. R e s e a r c h B u l l e t i n No. = 1. and Thodos. 1953).6) = 622.121 (556.337 (491. -pseudocricondentherm. E n g . From Fig.582 pci pi pp pt Tb n-butane = 0. 3 a t z e = 0. Etter and ~a~ 6 report values of 635 and 654 psia for this mixture. Prog+.121 + 0. NOMENCLATURE pci(psia) 673.3) = 1092 psia. 3.418 (491. These mixtures may contain normal and isoparaffins.2R p p c = 0.1) + 0. 1.07 (581.3R = 0.ll(587. 4. M. p p / p P c = 1-31.582 and T i /Tb = 1.418 Ti T i Tb = = ppc= 0.47 0.470 0. Amick.6 ppc A. or pseudocricondenbar pressure of mixture (method of calculation depends on number of components).6 psia.4) = 470.7) + 0.6 psia.048. p p / p p c = 1. USBM (1957) Vol.9 psia From Fig.: . EXAMPLE CALCULATION 4 Determine the cricondentherm and cricondenbar pressures of a mixture having the following composition: Mole Fraction Methane Ethane n-Butane 0. Eng. and Parent.6) = 398. psia = cricondenbar pressure of mixture. p t / p p C = 1.4) + (0.: Chem. SUMMARY A rather accurate method h a s been developed for the prediction of the cricondentherm and cricondenbar pressures of multicomponent hydrocarbon mixtures of known composition.4) + (0. H. B. 1 and 3 a t ze = 0. and Dodge. Cota and Thodos3 report values of 905 and 1108 psia for this mixture.. 101. C.7) + 0.1) + (0.1 550.193 (673. = 1.316. Establish p and p p of the required ternary REFERENCES 1. Eilerts.6) = = 753. T i = 0.47(331. D.1 707. 3. Monograph No. (Symposium Series) (1952) Vol.582 (331.486(617.121 + 0. "Physical -Chemical Properties of Methane-Ethane Mixtures".6 p s i a .47 + 0.9) = 652.486 and T i / T b = 1.7 = 581.3 psia pt P p: = 1. (July. Gami.47 + 0.31 (642) = 841 psia n pseudocritical.17(753.061 (615.7) + 0.061) - 0.582 (707. 1 a t zp = 0. Chicago. and their cricondentherm and cricondenbar pressures may be computed from a knowledge of the pure component critical properties and vapor pressure behavior. psia = vapor pressure of pure jth component. 4 a t z~ = 0. . naphthenes and aromatics. J. pt p. + 0.9) SEPTEMBER.486(416.1 200. K.193 and T i / T b = 1. p p = l. D a t a (1962) Vol.3 psia. A / p p .35 (809. D. 7.205. p t / p p c = 1. OR = normal boiling point of pure jth component.1) = From Fig. Gas Technology.: "Phase Relations of GasCondensate Fluids".

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