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VAPOR-LIQUID K-VALUES,FOR APPLICATION of the INTEGRAL I TECHNIQUE to PETROLEUM VAPORIZATION CALCULATIONS

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VAPOR-LIQUID K-VALUES,FOR APPLICATION of the INTEGRAL I TECHNIQUE to PETROLEUM VAPORIZATION CALCULATIONS VAPOR-LIQUID K-VALUES,FOR APPLICATION OF THE INTEGRAL i TECHNIQUE TO PETROLEUM VAPORIZATION CALCULATIONS By CHARLES LINFRED HENDERSON,, Bachelor of Science Oklahoma State University Stillwater, Oklahoma 1961 Submitted to the faculty of the Graduate School of the Oklahoma State University in partial fulfillment of the requirements for the degree of Master of Science Mayt 1964 ,... 8KLAHQMA J.fATJUNt~ L~~ JJ.,~ § l9o5 VAPOR-LIQUID K-VALUES FOR APPLICATION OF THE INTEGRAL TECHNIQUE TO PETROLEUM VAPORIZATION CALCULATIONS Thesis Approved: De~hool 569598 ii PREFACE With the advance of technology in today's petroleum industry, greater accuracy and reliability are needed in methods for pre­ dicting heavy hydrocarbon vapor-liquid phenomena. Equilibrium vapor-liquid distribution ratios, or K-values as they are fre­ quently called, are used in the petroleum industry for making distillation design calculations. This thesis is concerned with improving our knowledge of the vaporization phenomena of petroleum fractions. I am indebted to all of my fellow gra duate s tudents who offered advice and assistance whenever needed. I also wish to thank Dr. A. Amir-Yeganeh and Mr. C. B. Woodward who preceded me and Mr. R. M. Walston who worked with me, f or the unselfish sharing of their knowledge and experience. I owe special thanks to Professor R. N. Maddox for his encouragement throughout my graduate study and to my adviser, Professor Wayne C. Edmister, for his many helpful sugge stions and comments without which this wo r k could not have been accom­ plished. I also wish to express my thank s to, Esso Research and Engineering Company for their grant wh ich ma de this wo r k possible. Thanks should also be give n the Continental Oil Com pany for their help in the development of the molecular weight device, and to the ilumb le Oil and Refining Com pany for the oils with wh ich this work W8~ ~ccomplished. iii TABLE OF CONTENTS Chapter Page I. INTRODUCTION. • • . • . • . • . • . • . • . 1 II. EXPERIMENTAL EQUIPMENT AND PROCEDURES............. 5 Equilibrium Flow Still....................... 5 Oldershaw Column •... :........................ 11 Molecular Weight Determinations .. ·....•..••••• 15 Other Analyticc\l Equipment .........•• ~...... 24 III. EXPERIMENTAL RESULTS AND DISCUSSION •.• ~. ··......... 26 e quilibrium Flash Vaporization............... 26 Volumetric True Boiling Point Distillations.. 27 Specific Gravities ......................•... ,. 29 Molecular Weights.. • . • 31 Molar True Boiling Point Pl.ots ....•.•...... ~ . 31 IV. EVALUATION OF VAPOR-LIQUID EQUILIBRIUM FUNCTIONS •. (. Liquid Activity Coefficient from Regular Solution Theory ......... .............. ... 37 Derived Liquid Activity Coefficients ....... 39 Comparison of Vapor-Liquid Distribution Ratios ..... ... ··. • . • •. • • . • 41" Correlation of K-Values ..•...•....•• !•······· 41 V. RECOMMENDATIONS AND CONCLUSIONS..... ............. 54 BIBLIOGRAPHY..........• ~ •... • . .. ·. , ... ...... ........ ·. • • • 57 APPENDIX \ - NOMENCLATURE . • . • . 59 APPENDIX D - COMPUTER PROGRAMS .. ..• . .. ........•... .•••• . 62 Program l. • . • • . • . • . •. 62 Critical Values ...•...... •.• . ·•..•. ... .. 62 Acentric ·Factor... .. ... ......••. .. .. .. 64 Vapor Pressure ........... .. ...... .. ....· 64 Imperfection Pressure Correcti o~ Factor.......................... ... 65 Scatchard-Hildebrand Liquid Activity Coefficient. ........................ 67 Data Input f or Program 1......... .. ..... 68 i v Chapter Page Program 2 ....... o••••••••IP"O···•·•••oiil•• 69 Fortran Statements for Program 1 •••.••• 72 Fortran Statements for Program 2 •.••.•• 75 APPENDIX C - PHYSICAL PROPERTIES OF OILS •.•••...••••••••• 78 APPENDIX D - EXPERIMENTAL FLASH VAPORIZATION DATA AND EQUILIBRIUM FLASH VAPORIZATION CALCULATIONS .......................... 89 APPENDIX E - SMOOTHED KA-VALUES ......................... 120 APPENDIX F - COMPARISON OF EQUILIBRIUM FUNCTIONS DERIVED FROM PETROLEUM FRACTIONS ANALYSED BY THE CHROMATOGRAPH AND THE OLDERSHAW COLUMN •• 130 V LIST 0.1" TAilLES Table Page I. Hydrocarb on Molecular We i ghts Comparing Those Obtainsd from Vapor Density with Th ose Known from Atomic Mass...... • • . • . • •. • • • • • • • 33 II. Characteristics of Oils Obtained from Amir- Yeganeh (1).................................. 36 III. Liquid Activity Coefficient as Calculated by the Scatchard-Hildebrand Equation as~ Fu.ncti-0n of Normal Boiling Point. • • . • . • • • 38 IV . K = y / x for Hypothetical Components by Different ~·i0 t.l1ods ••• ••• ·• •• • •••• • • •· ••••••• o • •• ~ •••• • • • • • 42 V. Constants for Equatio·n ( IV~l) • ••.• .... .• . •. .•• ·.... 48 VI. Constants for Equation (IV-2) ................. ·••• 53 VII. C'onsta:n:ts for Equations of T and P • • • • . • • . • • . 63 C C · VIII. Comparison of Vap@r l: 'r t~,;; sure by Correlation and by Maxwell and.. Bon r:. ell (12). ........ ..... 66 IX. Output from Program 1. .. ......................... 71 X. Physical Propert_i es of Light Crude Naphtha: - Fe eds tock . ~ . o • o • • • o • • • • • • • • • • • • • • 7 9 XI. Physical Properties of Light Crude Naphtha - Equilibrium Li q-...i id No. 4 .. • . • . • . • . • 80 XII. Physical Properties of Light Crude Naphtha - Equilibrium Li quid No. 6..... ........ .. .. 81 XIII. Physical Properties of Light Crude Naphtha - Equilibrium Li c;,uid No. 9... .... ............. 83 XIV. Physical Properties of Heavy Crude Naphtha - Feedstock . ....... .. ........ .... o • • • • • • • • • • 85 XV. Physical Properties of Kerosene - Feedstock...... 86 vi Table Page XVI. Physical Properties of Trade Gas Oil - Feedstock................... ... .. ............ 87 XVII. Physical Properties of Heavy Gas Oil - Feedstock..................................... 88 XVIII. Equilibrium Flash Vaporization Data - Light Crude Naphtha........................... 90 XIX. Equilibrium Flash Vaporization Data - Heavy Crude Naphtha........................... 91 XX. Equilibrium Flash Vapprization Data - Kerosene. • . 92 XXI. Equilibrium Flash Vaporization Data - Trade Gas Oi 1. • . • • . 93 XXII. Equilibrium Flash Vaporization Data - Heavy Gas Oil................................. 94 XXIII. Equilibrium Flash Calculations (Oil A - Run lOU... 95 XXIV. Equilibrium Flash Calculations (Oil A - Run 10~... 96 XXV. Equilibrium Flash Calculations (Oil A - Run 103).. 97 XXVI. Equilibrium Flash Calculations (Oil A - Run 104).. 98 XXVII. Equilibrium Flash Calculations (Oil B - Run 105).. 99 XXVIII. Equilibrium Flash Calculations (Oil B - Run 106) .. 100 XXIX. Equilibrium Flash Calculations (Oil B - Run 107) .. 101 XXX. Equilibrium Flash Calculations (Oil G - Run 110) •• 102 XXXI. Equilibrium Flash Calculations (Oil G - Run 111) .. 103 XXXII. Equilibrium Flash Calculations (Oil G - Run 112) •. 104 XXXIII. Equilibrium Flash Calculations (Light Crude Naphtha - Run 34)........... ................ 105 XXXIV. Equilibrium Flash Calculations (Light Crude Naphtha - Run 36).......... ................. 106 XXXV. Equilibrium Flash Calculations (Light Crude Naphtha - Run 39)............................ 107 vii Table Page XXXVI. Equilibrium Flash Calculations (Heavy Crude Naphtha - Run 4032-l)..................... 108 XXXVII. Equilibrium Flash Calculations (Heavy Crude Naphtha - Run 4032-2)..................... 109 XXXVIII. Equilibrium Flash Calculations (Heavy Crude Naphtha - Run 4032-3).... ............. .... 110 XXXIX. Equilibrium Flash Calculations (Kerosene - Run 4033-1)............................... 111 XL. Equilibrium Flash Calculations (Kerosene - Run 4033-2)........... • 112 XLI. Equilibrium Flash Calculations (Kerosene - Run 4033-2........ .. .. .. ................ 113 XLII. Equilibrium Flash Calculations (Trade Gas Oil - Run 4034-1) .................•......• 114 XLIII. Equilibrium Flash Calculations (Trade Gas Oil - Run 4034-2)......................... 115 XLIV. Equilibrium Flash Calculations (Trade Gas Oil - Run 4034-3)......................... 116 XLV. Equilibrium Flash Calculations (Trade Gas Oil - Run 4034-4)......................... 117 XLVI. Equilibrium Flash Calculations (Heavy Gas Oil - Run 4035-1)........................ 118 XLVII • . Equilibrium Flash Calculations (Heavy Gas Oil - Run 4035-2)......................... 119 XLVIII. Smoothed KA-Values Derived for Oil A• •••• • •••• • 121 XLIX. Smoothed KA-Values Derived for Oil B • • ... • • • • • 122 L. Smoothed KA-Values Derived for Oil G • ••• • •••• • • 124 LI. Smoothed KA-Values Derived for Light Crude Naphtha ..•.......•....... ....•..........• 125 LIL Smoothed ~A-Values Derived for Heavy Crude Naphtha..... .... .......................... 126· Lill. Smoothed KA-Values Derived for Kerosene .••••••• 127 viii Table Page LIV. Smoothed KA-Values Derived for Trade Gas Oil. •.• 128 LV. Smoothed KA-Values Derived for Heavy Gas Oil •••• 129 LVI. Comparison of Imperfection Pressure Correction 0 0 • .• 0 • 0 0 • O O • • o O e O O o O O O O ·G O O • 0 0 e O O O O O c,. O 1 132 ix LIST OF FIGURES Figure Page 1. Equilibrium Flow Still "B".......................... 6 2. Schematic Flow Diagram of Equilibrium Still 11 B"..... 8 3. Oldershaw Column . .......... o ••••• e •••••••••••••• o " • • 12 4 ... Schematic Diagram of Molecular Weight Device ••••.••• 16 5. Mercury Orifice . .................... l!I •••••• o ••••• o o • 20 6. Magnified Mercury Orifice with Ground Glass Sections. G ••••••• o •••••••••••• o ......... o •••• o o •• o • 21 7. Volumetric True Boiling Point Curve of Light Crude Naphtha and Equilibrium Liquids ••••••••••••• 28 8. Specific Gravity Versus Normal Boiling Point for Light
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