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The Thermophysical Properties of Methane, from 90 to 500 K At I Ho Bora .*> IkJ-*, .</*>-* MS 'y-- > NBS TECHNICAL NOTE 653 »«" "' "o. % in \ *"*C A U O* * NATIONAL BUREAU OF STANDARDS The National Bureau of Standards 1 was established by an act of Congress March 3, 1901. The Bureau's overall goal is to strengthen and advance the Nation's science and technology and facilitate their effective application for public benefit. To this end, the Bureau conducts research and provides: (I) a basis for the Nation's physical measurement system, (2) scientific and technological services for industry and government, (3 ) a technical basis for equity in trade, and (4) technical services to promote public safety. The Bureau consists of the Institute for Basic Standards, the Institute for Materials Research, the Institute for Applied Technology, the Institute for Computer Sciences and Technology, and the Office for Information Programs. THE INSTITUTE FOR BASIC STANDARDS provides the central basis within the United States of a complete and consistent system of physical measurement; coordinates that system with measurement systems of other nations; and furnishes essential services leading to accurate and uniform physical measurements throughout the Nation's scientific community, industry, and commerce. The Institute consists of a Center for Radiation Research, an Office of Meas- urement Services and the following divisions: Applied Mathematics — Electricity — Mechanics — Heat — Optical Physics — Nuclear Sciences 2 — Applied Radiation s — Quantum Electronics 3 — Electromagnetics 3 — Time n 3 and Frequency — Laboratory Astrophysics — Cryogenics ". THE INSTITUTE FOR MATERIALS RESEARCH conducts materials research leading to improved methods of measurement, standards, and data on the properties of well-characterized materials needed by industry, commerce, educational institutions, and Government; provides advisory and research services to other Government agencies; and develops, produces, and distributes standard reference materials. The Institute consists of the Office of Standard Reference Materials and the following divisions: Analytical Chemistry — Polymers — Metallurgy — Inorganic Materials — Reactor Radiation — Physical Chemistry. THE INSTITUTE FOR APPLIED TECHNOLOGY provides technical services to promote the use of available technology and to facilitate technological innovation in industry and Government; cooperates with public and private organizations leading to the development of technological standards (including mandatory safety standards), codes and methods of test; and provides technical advice and services to Government agencies upon request. The Institute consists of a Center for Building Technology and the following divisions and offices: Engineering and Product Standards — Weights and Measures — Invention and Innova- tion — Product Evaluation Technology — Electronic Technology — Technical Analysis — Measurement Engineering — Structures, Materials, and Life Safety * — Building * Environment ' — Technical Evaluation and Application — Fire Technology. THE INSTITUTE FOR COMPUTER SCIENCES AND TECHNOLOGY conducts research and provides technical services designed to aid Government agencies in improving cost effec- tiveness in the conduct of their programs through the selection, acquisition, and effective utilization of automatic data processing equipment; and serves as the principal focus within the executive branch for the development of Federal standards for automatic data processing equipment, techniques, and computer languages. The Institute consists of the following divisions: Computer Services — Systems and Software — Computer Systems Engineering — Informa- tion Technology. THE OFFICE FOR INFORMATION PROGRAMS promotes optimum dissemination and accessibility of scientific information generated within NBS and other agencies of the Federal Government; promotes the development of the National Standard Reference Data System and a system of information analysis centers dealing with the broader aspects of the National Measurement System; provides appropriate services to ensure that the NBS staff has optimum accessibility to the scientific information of the world. The Office consists of the following organizational units: Office of Standard Reference Data — Office of Information Activities — Office of Technical Publications — Library — Office of International Relations. 1 Headquarters and Laboratories at Gaithersburg, Maryland, unless otherwise noted; mailing address Washington, D.C. 20234. 3 Part of the Center for Radiation Research. 3 Located at Boulder, Colorado 80302. • Part of the Center for Building Technology. :'~ :,:-'' , Gut;;;.! t;-f -^# ?4^ Wk The Thermophysical Properties (6C of Methane, from 90 to 500 K at Pressures to 700 Bar R. D. Goodwin Cryogenics Division Institute tor Basic Standards US. National Bureau of Standards Boulder, Colorado 80302 •'•tAU O* * U.S. DEPARTMENT OF COMMERCE, Frederick B. Dent. Secretary NATIONAL BUREAU OF STANDARDS. Richard W Roberts. Director National Bureau of Standards Technical Note 653 Nat. Bur. Sland. (U.S.). Tech. !Nole 640, 280 pages (April 1974) CODEN: !NBT!\AK For sale by ihe Superintendent of Documents, U.S. Government Printing Office, Washington, D.C. 20402 (Order by SI) Catalogue No.C 13.46:653). 82.25 CONTENTS Page 1. INTRODUCTION 1 2. PHYSICAL PROPERTIES AND THEIR REPRESENTATION 3 2. 1 Fixed -Point Constants 3 2. 2 Melting Line and Vapor Pressures 3 2.3 The Orthobaric Densities 4 2.4 The Virial Equation 6 2. 5 The Equation of State 6 2.6 Representation of C (T) at 18.5 mol/t 8 3. COMPUTATIONAL METHODS 9 3.1 The Homogeneous Domain 9 3. 2 The Vapor-Liquid Transition 10 3.3 Representation of E (T) and S (T) 11 a a 3.4 Circumventing the Critical Domain 12 4. COMPARISON OF DERIVED AND EXPERIMENTAL PROPERTIES 12 4. 1 Heats of Vaporization 12 4.2 Specific Heats C (T), C (p , T), C (p , T) 13 4.3 Speeds of Sound W (T), W(p,T) 13 a 5. TABLES OF PHYSICAL AND THERMODYNAMIC PROPERTIES 13 5. 1 Calculated P-p-T Isochores and Isotherms 13 5. 2 The Joule -Thomson Inversion Locus 14 5.3 Thermophysical Properties of the Saturated Liquid 14 5.4 Thermophysical Properties Along Selected Isobars 14 6. TABLES IN BRITISH ENGINEERING UNITS 14 7. COMMENTS ON UNCERTAINTIES 14 8. ACKNOWLEDGMENTS 15 9. REFERENCES 1& . CONTENTS (continued) Appendix A, Symbols and Units 21 Appendix B, Fixed-Point Values 22 Appendix C. Conversion of Units 23 Appendix D, List of new Data 24 Appendix E. Computer Programs 25 LIST OF FIGURES Figure 1 Density-temperature phase diagram 42 LIST OF TABLES Table 1-A The saturated vapor densities 43 Table 1-B The saturated liquid densities 45 Table 1-C The vapor-liquid saturation temperatures 46 Table 2-A The second virial coefficient 49 Table 2-B The third virial coefficient 50 Table 3. Summary of P-P-T data 51 Table 4. Comparison of experimental and calculated P-p-T values 52 Table 5. Comparison of specific heats for saturated liquid .... 79 Table 6. Comparison of specific heats, C (P,T) 80 Table 7. Comparison of specific heats, C (P,T) 85 ir Table 8. Comparison of speeds of sound for saturated liquid . 87 Table 9. Comparison of speeds of sound, W(p, T) 88 Table 10 Calculated P(T) isochores 90 Table 11 Calculated P(p) isotherms 117 Table 12 The Joule-Thomson inversion locus 134 Table 13 Thermophysical properties of the saturated liquid .... 135 Table 14 Thermophysical properties along isobars 137 Table 15 The Joule-Thomson inversion locus 205 Table 16 Thermophysical properties of the saturated liquid .... 206 Table 17 Thermophysical properties along isobars 209 : Tables in British engineering units . ABSTRACT Thermophysical properties of methane are tabulated at uniform tempera- tures from 90.68 to 500 K along isobars to 700 bar. A novel equation of state is employed for the first time, having origin on the vapor-liquid coexistence boundary. Computations are based almost entirely on ideal gas specific heats and experi- mental P- p-T data via the equation of state, without weighting to data for derived properties. Good agreement with such data confirms validity of the equation and method. New P- P-T data are reported at 0.3 to 1.7 times the critical density. Key words: Densities; enthalpies; entropies; equation of state; internal energies; isobars; isochores; isotherms; Joule-Thomson inversion; latent heats of vaporiza- tion; melting line; orthobaric densities; PVT data; specific heats; speeds of sound; vapor pressures 1. INTRODUCTION Methane is the major component of natural gas, and hence of great economic importance. For the processes of liquefaction, separation, storage, pumping, transport and custodial transfer there is required a knowledge of physical and thermodynamic prop- erties. For mixtures, some properties can be approximated by those of pure methane. For computations on the properties of LNG mixtures, the dominant thermodynamic data required again are those of methane . In the following work it is possible to test the thermo- dynamic computations against experimental data for specific heats, heats of vaporization, and speeds of sound available over wider ranges than for other components of LNG . Some of the experimental data obtained here on methane, for example the saturated liquid densities, also have been useful to others for calibrating experimental apparatus. Extreme accuracy is needed in physical and thermodynamic properties data for engineering plant design, as demonstrated recently by Zudkevitch [73] . Two monographs on methane [61, 72] show, however, that low temperature data necessary for thermal computations either are
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