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Dedicated to my wife Ghashang
and to my mother Azra
About the Author
Abbas Firoozabadi is the director of the Reservoir Engineering Research Institute
(RERI) and a professor at Yale University. He is the author of Thermodynamics of
Hydrocarbon Reservoirs and has published some 200 papers. More than 70 of the
papers have appeared in Society of Petroleum Engineers (SPE) journals. Firoozabadi
is a member of the National Academy of Engineering (USA).
 Contents

Preface
Acknowledgments
Notation

1 Review of Basic Concepts in Bulk Phase Equilibrium Thermodynamics

1.1 Conditions for Equilibrium
1.1.1 Thermal Equilibrium
1.1.2 Mechanical Equilibrium
1.1.3 Chemical Equilibrium
1.2 Mathematical Properties of U and S
1.3 Gibbs-Duhem Equation
1.4 Other Fundamental Equations
1.5 Internal Energy Minimum Principle
1.5.1 Relation between Partial Derivatives of Implicit Functions
1.5.2 Reciprocity Relation
1.6 Chemical Potential of a Component in a Mixture
1.7 Partial Molar Quantities
1.8 Fugacity
1.9 Ideal and Nonideal Fluids
1.9.1 Ideal Gas
1.9.2 Ideal Solution
1.9.3 Nonideal Solution
1.10 Activity Coefficient
1.11 Relation between γi and GE
1.11.1 Pressure and Temperature Derivative of γi
1.12 Activity Coefficient Models
1.12.1 Margules Activity Coefficient Equations
1.12.2 Van Laar Activity Coefficient Equations
1.12.3 Scatchard-Hildebrand Regular-Solution Activity Coefficients
1.12.4 Flory-Huggins Polymer-Solution Activity Coefficients
1.13 Legendre Transformation
1.14 Jacobian Transformation
1.15 Maxwell’s Relations
1.16 Examples and Theory Extension
 1.17 Problems
1.18 References

2 General Theory of Bulk Phase Equilibria

2.1 Equilibrium Condition under the Influence of Gravity
2.1.1 Conditions for Pronounced Compositional Variation
2.2 Equilibrium Condition for Curved Interfaces
2.2.1 Effect of Curvature on Saturation Pressure: Condensation and
Vaporization in Porous Media
2.3 Equilibrium Condition for Charged Systems
2.3.1 Electrostatic Energy of a Sphere with Uniform Charge
2.3.2 Criteria of Equilibrium for a Charged System
2.4 Examples and Theory Extension
2.5 Problems
2.6 References

3 Equation-of-State Representation of Fluid Phase Behavior and Properties

3.1 EOS Representation of Volumetric and Phase Behavior
3.1.1 Algebraic Form of Cubic Equations
3.1.2 Peng-Robinson Equation of State (PR-EOS)
3.1.3 Phase Behavior of Mixtures with Well-Defined Components
3.1.4 Reservoir Fluid Phase Behavior and Volumetric Properties
3.1.5 CO2 Dissolution in Petroleum Fluids and Property Changes
3.2 Associating Species
3.3 Cubic-Plus-Association Equation of State
3.3.1 CPA-EOS
3.3.2 Water-Containing Mixtures
3.3.3 Asphaltene Precipitation Modeling
3.4 Two-Phase Isothermal Compressibility
3.5 Two-Phase Isentropic Compressibility and Two-Phase Sonic Velocity
3.6 Single-Phase Sonic Velocity and Temperature Change due to Expansion
3.6.1 Heating and Cooling due to Expansion
3.7 Examples and Theory Extension
3.8 Problems
3.9 References

4 Stability and Criticality

4.1 Stability Analysis and Stability Limit
4.1.1 Stability Analysis for a Single-Component
 4.1.2 Stability Analysis in a Two-Component System
4.1.3 Stability Analysis for Multicomponent Mixtures
4.2 Criticality Analysis
4.2.1 Single-Component Fluid
4.2.2 Two-Component Fluid
4.2.3 Multicomponent Fluid
4.3 Alternative Approach for Critical-Point Calculation
4.3.1 Single-Component Fluids
4.3.2 Two-Component Fluids
4.3.3 Three-Component Fluids
4.4 Examples and Theory Extension
4.5 Problems
4.6 References

5 Phase Equilibrium Computations

5.1 Gibbs Free Energy Surface Analysis
5.2 Tangent-Plane Distance (TPD) Analysis
5.3 Stability Testing
5.3.1 SSI Method
5.3.2 Newton Method
5.4 Two-Phase Split Computations
5.4.1 SSI Method
5.4.2 Newton Method
5.5 Three-Phase Split Calculations
5.5.1 SSI Method
5.5.2 Newton Method
5.6 Direct Minimization of Gibbs Free Energy in Multiphase Split Calculation
5.7 Phase-Split Calculations in Reduced Space
5.7.1 Zero Interaction Coefficients
5.7.2 Nonzero Interaction Coefficients
5.8 Critical-Point Calculation
5.8.1 Numerical Solution
5.8.2 One-D Search
5.8.3 Initial Guess
5.9 Examples and Theory Extension
5.10 Problems
5.11 References

6 Theory of Irreversibility and Diffusion in Multicomponent Mixtures

 6.1 Irreversibility in a Closed System
6.1.1 Entropy Production Strength
6.2 Derivation of Diffusion Flux and Diffusion Coefficients in Multicomponent
Mixtures
6.2.1 Phenomenological Laws of Irreversible Thermodynamics
6.2.2 Diffusion Mass Flux
6.2.3 Thermal Convection
6.2.4 Natural Convection and Diffusion in Porous Media
6.2.5 Compositional Variation in Hydrocarbon Reservoirs
6.3 Prediction of Past Climate Changes from Irreversible Thermodynamics
6.3.1 Ice Core Data
6.3.2 Sampling
6.3.3 Ice Dating
6.3.4 Trapped Air Dating
6.3.5 Temperature Modeling
6.4 Examples and Theory Extension
6.5 Problems
6.6 Appendix
6.6.1 Scalars, Vectors, Tensors, and their Products
6.6.2 Multiplication of a Vector by a Scalar
6.6.3 Scalar Product or Dot Product (·) of Two Vectors
6.7 References

7 Interfacial Thermodynamics
7.1 Plane Interface
7.2 Curved Interface
7.3 Thermodynamic Functions
7.4 Effect of Curvature on Interfacial Tension
7.5 Work of Cluster Formation: Single-Component Systems
7.5.1 Spherical Clusters
7.5.2 Incompressible Clusters
7.5.3 Gas Clusters
7.6 Cap-Shaped Clusters
7.7 Derivation of the Young Equation
7.8 Driving Force (Δµ)
7.8.1 Condensation from Vapor at Constant T
7.8.2 Evaporation from Liquid at Constant T
7.9 Thermodynamic Functions and Gibbs Adsorption Equation without
Chemical Equilibrium
7.10 Helmholtz Free Energy of an Open System
 7.11 Relation between and
7.12 Fundamental Equation of the Interface
7.12.1 Adsorption at the Interface
7.12.2 Work of Cluster Formation in a Multicomponent Mixture
7.13 Examples and Theory Extension
7.14 Problems
7.15 References

8 Thermodynamics of Thin Liquid Films

8.1 Pressure Anisotropy in the Film
8.2 Thin Liquid Film Work and Energy
8.3 Equilibrium Conditions
8.3.1 Mechanical Equilibrium
8.3.2 Augmented Young Equation
8.4 Film Tension
8.5 Thermodynamic Functions of the Thin Liquid Film
8.6 Relations between Disjoining Pressure and Contact Angle
8.7 Example and Theory Extension
8.8 Problems
8.9 References

Index
 Preface

A theory is the more impressive the greater the simplicity of its premises,
the more different kinds of things it relates, and the more extended its area
of applicability. Therefore, the deep impression that classical
thermodynamics made upon me. It is the only physical theory of universal
content which I am convinced will never be overthrown, within the
framework of applicability of its basic concepts.—ALBERT EINSTEIN

Thermodynamics shapes the understanding and formulation of diverse groups of

problems in energy production, hard materials, soft matter, nanoparticles, climate
change, Alzheimer’s disease, stars, black holes, and many others. In thermodynamics,
one examines bulk phases and the interface between the bulk phases as well as
heterogeneous state in confinement. This book offers a unified approach to bulk-
phase equilibrium thermodynamics, bulk-phase irreversible thermodynamics, and
interfacial thermodynamics and thermodynamics of thin films in the framework of
classical thermodynamics. Concepts of stability, criticality, and the effects of
curvature, gravity, and electrical charge on equilibrium are covered in
multicomponent systems. The choice of the Gibbs free energy function covers
applications to a broad range of problems in chemical, environmental, biomedical,
and petroleum engineering. The grand potential is also introduced to study
equilibrium in open systems and in inhomogeneous nanopore domains. A number of
concepts and problems related to phase change and interface energy, thin liquid
films, and premelting and nonequilibrium effects are discussed in different chapters.
Molecular dynamics simulations, based on concepts from statistical
thermodynamics, are being used increasingly in the study of molecular structures in
complex fluid and other states of matter. Molecular dynamics and other molecular
simulation techniques can also provide prediction and understanding of both complex
and simple fluids. In molecular simulations, use of concepts from classical
thermodynamics can greatly facilitate computations and guide simulations. An
example is provided in Chap. 4 on the use of stability and criticality in molecular
dynamics simulations.
No comprehensive thermodynamics text is available that covers bulk-phase
equilibrium thermodynamics, bulk-phase irreversible thermodynamics, and
interfacial and thin-film thermodynamics. This book presents a unified approach in
the study of various problems in the domains of equilibrium, nonequilibrium, and the
interfaces.
Chapter 1 covers basic concepts of bulk-phase equilibrium thermodynamics.
Thermodynamic functions such as Gibbs free energy and grand potential are
introduced. Many examples including thermodynamics of atmosphere and reverse
melting are included to demonstrate the wide range of problems that can be solved
from simple concepts.
Chapter 2 presents a general theory for bulk-phase equilibrium when gravity,
interface curvature, and electric fields are accounted for. Examples help with clear
understanding of topics. The effect of interface curvature on equilibrium both in
single components and mixtures in ideal and nonideal systems is covered. Some of
the examples relate to shale gas.
Chapter 3 provides the basic expressions for computation of the relation between
pressure, temperature, and volume and presents with clarity how to account for
association of polar molecules. The working equations allow for engineering
computations in all the chapters. This chapter also contains examples for shale gas.
Chapter 4 provides a deep but simple mathematical approach to thermodynamic
stability and criticality for both pure components and mixtures. One of the examples
is devoted to derivations related to complete miscibility of solvents and polymers.
Another example demonstrates the usefulness of classical thermodynamics in
decreasing the computational time of molecular dynamics simulations of hydrate
nucleation by orders of magnitude.
Chapter 5 offers efficient numerical solution of algebraic expressions of
multicomponent and multiphase bulk mixtures. This chapter is self-contained for
those who are interested in efficient and robust code development in fluid-phase
equilbria.
Chapter 6 presents a new perspective on diffusion of multicomponents based on
rigorous derivations of entropy production. Past climate change computations and
species distributions in hydrocarbon reservoirs are covered in the Examples and
Theory Extension section. Explanation is provided for unusual cases in which a
heavy fluid can float on top of a light fluid in a hydrocarbon reservoir.
Chapter 7 covers thermodynamics of interfaces in a unified approach. There is no
comparable material in current thermodynamics texts in English to the level and
depth of this chapter. One of the examples relates to the effect of electric charge on
vaporization of droplets and the unique features of Gibbs free energy change.
Interestingly, Lord Kelvin solved the same problem in a different approach. Another
example covers thermodynamics of the weightless state. The concept of line tension
is presented in the last example of Chap. 7. Basics of classical nucleation are
covered in this chapter.
Chapter 8 covers thermodynamics of thin liquid films. This is the shortest chapter
of the book with only one example and several problems. Concepts, such as
disjoining pressure, are clearly introduced. The key example of this chapter is
calculation of the melting point of gold nanoparticles in relation to consideration of
thin liquid films. This chapter is partly based on examination of thin-film
thermodynamics and consistent thermodynamics derivations.
Abbas Firoozabadi
 Acknowledgments

T hermodynamics and Applications in Hydrocarbon Energy Production has

evolved from 10 years of teaching graduate thermodynamics in the Department
of Chemical and Environmental Engineering at Yale University from 2003 to
2012. The material from my teaching and some parts of my earlier book,
Thermodynamics of Hydrocarbon Reservoirs, constitute the new book.
The 10 years of teaching at Yale have been the most pleasant experience. I could
not have enjoyed myself more and had more fun than teaching thermodynamics to
eager graduate students. One of my most fond memories was correcting students’
assignments as I, too, learned from their smart approaches to solving problems.
I would like to thank the following former graduate students who were my
teaching assistants in the last 4 years of teaching and helped me with class duties: Dr.
Livia Moreira (Max Planck Institute), Dr. Xiaokai Li (Apple), Dr. Xiaoming Wang
(BASF), and Dr. Seyla Azoz (Yale University).
Three colleagues at Yale provided the opportunity for my teaching graduate
thermodynamics. Prof. Daniel Rosner set the stage for my teaching, as I co-taught a
special graduate course on Advanced Topics in Transport and Thermodynamics in
2002. Dan has more of a fascination with the Soret effect in flames and the
thermodynamics of irreversible processes than anyone else I know in the United
States. The common interest in the Soret effect evolved into a friendship and a
genuine interest in graduate teaching at Yale. Profs. Menachem (Meny) Elimelech
and Lisa Pfefferle provided much support to my teaching during their respective
tenures as department chairs. Meny also facilitated the pleasant work with my Ph.D.
students and postdocs.
Much of the material in Chaps. 5 through 8 is based on the research work
performed by my Ph.D. students and postdocs at the Reservoir Engineering Research
Institute (RERI), which was further refined by my interest in these special topics. The
material in these chapters is based on the work of Dr. Hussein Hoteit (Chevron), Dr.
Kjetil Haugen (Exxon-Mobil), Dr. Alana Leahy-Dios (ExxonMobil), Dr. Kassem
Ghorayeb (Schlumberger), Dr. Wambui Mutoru (ConocoPhillips), Dr. Joachim
Moortgat (Ohio State University), Dr. Hadi Nasrabadi (Texas A&M University), Dr.
Philip Myint (Lawrence Livermore National Laboratory), Dr. Erick Santiso (North
Carolina State University), Dr. Jiri Mikyska (Czech Technical University in Prague),
and Dr. Boris Lukanov (RERI). Specific contributions to the book were also made by
the following coworkers: Hussein read Chaps. 4 through 6; Philip read Chaps. 3 and
8, and I would like to acknowledge his work on the examples on invariant
eigenvalues of the Fickian diffusion coefficients in multicomponent mixtures in Chap.
6 and the weightless state in Chap. 7; Erick solved the partial differential equations
that lead to the augmented Young-Laplace equation of capillarity in Chap. 7; Dr.
Seyma Aslan prepared two of the figures in Chap. 3; Kjetil prepared two examples
on past climate changes from irreversible thermodynamics in Chap. 6; Alana read
Chap. 1; Dr. Atefeh Khoshnood (RERI) read Chaps. 1, 2, 4, and 6 and helped with
one example in Chap. 6; Wambui helped with reading Chap. 3; Hadi perused the
notes of this book before the final stage of preparation and also read Chaps. 2 and 3;
Dr. Zhehui Jin (RERI) helped with an example in Chap. 3; Dr. Nima Rezai (Kuwait
University) did some early derivations in the CPA equation of state; Joachim read
Chaps. 2 and 6; Jiri provided one example for Chap. 1 and also read a few chapters
and gave me his suggestions; and Boris read Chap. 7 and helped with the climate
change description in Chap. 6, and also solved many problems of different chapters
(these solutions will be made available when this book is finalized).
Mrs. Sirma Pandev, the former RERI office manager, did most of the typing and
some of the illustrations. Miss Anna Rowland, the former RERI assistant, enhanced
most of the figures. Miss Sasha Rojas, the former RERI office manager, helped with
final typing.
Dr. L. Kent Thomas, a RERI board member, helped with reading Chap. 7. He,
along with Dr. Bret Beckner (ExxonMobil), Prof. Clay Radke (University of
California, Berkeley), and other board members of RERI, has played a key role in
advising and counseling the institute in order to allow me the opportunity to write the
book.
My sincere thanks and gratitude go to all my colleagues at RERI and Yale
University; and to my family—my wife Ghashang, my son Reza, my daughter Rozie,
and my daughter-in-law Suzette—who created the atmosphere of love and support
that allowed me the endless hours I needed to write the book. I will try to compensate
for what I have missed.
 Notation

All the terms and symbols used in the book are listed here, except for those that
appear infrequently, or only in one section.

Terms
Superscripts

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