CHAPTER 3 Chemical Dynamics – I 147

 Ionic Reactions: Single and Double Sphere Models

It is a quite well-known fact that the rate of ionic reactions is generally small, which is obviously due
to the larger magnitude of activation energies arising from the very strong nature of electrostatic interactions.
The magnitude of the frequency factor in ionic reactions is a function of ionic charges. The frequency factors
have larger values if the charges on the participating ions are opposite, while smaller values are obtained in
the case of like-charged ions. This behavior can be explained in terms of the kinetic theory of gases; which
suggests that oppositely charged ions are more prone to collision due to attraction than the ions colliding with
same charges (repulsive forces). Besides the collision theory, the activated complex theory also provides an
alternate explanation for the ionic reactions. In this section, we will discuss the rationalization of ionic reactions
on the basis of the single-sphere model and the double-sphere model in detail.
 Double Sphere Model
Before we discuss the double sphere model of the ionic reactions, a simplified surrounding must be
assumed. Although it would be an oversimplification of the actual situation, it is highly beneficial as far as
conceptual and quantitative understanding is concerned. To do so, the solvent is considered as continuous
surrounding with a ε as the dielectric constant.
According to this model, two ions, which can same or opposite charges, combine together to form an
activated complex. In the initial state, the ions are considered as discrete; while in the final state, they assumed
to form a dumbbell like coordination with ʻrʼ as the distance of separation between their centers.

Figure 12. The pictorial depiction of the double-sphere model of ionic reactions.

Now, if ZA and ZB are the charge numbers of the participating ions and x as the distance of separation, the force
of electrostatic interaction (FAB) between them can be given from the Coulomb’s law as:

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 148 A Textbook of Physical Chemistry – Volume I

𝑍𝐴 𝑍𝐵 𝑒 2 (206)
𝐹𝐴𝐵 =
4𝜋𝜀0 𝜀𝑥 2

Where ε0 and ε are permittivities of the vacuum (8.854 × 10−12 C2 N−1 m−2) and the dielectric constant of the
solvent used, respectively. The symbol e represents the elementary charge and has a value equal to 1.6 × 10−19
C. The value of parameter varies from ∞ to r with the mutual approach of two ions. The amount of work done
in moving the two ions closer by an extant dx will be

𝑤𝑜𝑟𝑘 = 𝑓𝑜𝑟𝑐𝑒 × 𝑑𝑖𝑠𝑝𝑙𝑎𝑐𝑒𝑚𝑒𝑛𝑡 (207)

𝑑𝑤 = 𝐹𝐴𝐵 × 𝑑𝑥 (208)

𝑍𝐴 𝑍𝐵 𝑒 2 (209)
𝑑𝑤 = − 𝑑𝑥
4𝜋𝜀0 𝜀𝑥 2

The negative sign is an indicator of decreasing separation i.e. distance is reduced by dx. The total amount of
work done in moving the two ions from x = ∞ to x = r will be
𝑟
𝑍𝐴 𝑍𝐵 𝑒 2 (210)
𝑤=−∫ 𝑑𝑥
4𝜋𝜀0 𝜀𝑥 2
∞

𝑍𝐴 𝑍𝐵 𝑒 2 (211)
𝑤=
4𝜋𝜀0 𝜀 𝑟

The work given the above equation is actually the potential energy of the system which would have a negative
sign for oppositely charged ions and positive sign if the ions have same charges. Furthermore, we can also say
that this work is the free energy change due to electrostatic interactions, therefore, multiplying it by Avogadro
number (N) would give the value of the corresponding molar free energy change (𝛥𝐺𝐸𝐼 ∗
) i.e.

∗
𝑁𝑍𝐴 𝑍𝐵 𝑒 2 (212)
𝛥𝐺𝐸𝐼 =
4𝜋𝜀0 𝜀 𝑟

Correcting the above equation for non-electrostatic contribution 𝛥𝐺𝑁𝐸𝐼

∗
, the total molar free energy change for
the whole process can be given by the following relation.

∗ ∗ ∗
𝑁𝑍𝐴 𝑍𝐵 𝑒 2 (213)
𝛥𝐺 ∗ = 𝛥𝐺𝑁𝐸𝐼 + 𝛥𝐺𝐸𝐼 = 𝛥𝐺𝑁𝐸𝐼 +
4𝜋𝜀0 𝜀 𝑟

Also, from the activated complex theory, we know that

𝑅𝑇 −𝛥𝐺∗ (214)
𝑘= 𝑒 𝑅𝑇
𝑁ℎ
After putting the value of ΔG* from equation (213) into equation (214), we get

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 CHAPTER 3 Chemical Dynamics – I 149

(215)
∗ 2
𝑅𝑇 −(𝛥𝐺𝑅𝑇
𝑁𝐸𝐼 + 𝑁𝑍𝐴 𝑍𝐵 𝑒 )
𝑅𝑇4𝜋𝜀0 𝜀 𝑟
𝑘= 𝑒
𝑁ℎ
∗
𝑅𝑇 −𝛥𝐺𝑁𝐸𝐼 −
𝑁𝑍𝐴 𝑍𝐵 𝑒 2
(216)
𝑘= 𝑒 𝑅𝑇 . 𝑒 𝑅𝑇4𝜋𝜀0 𝜀 𝑟
𝑁ℎ
Taking natural logarithm both side of equation (216), we get

𝑅𝑇 ∗
𝛥𝐺𝑁𝐸𝐼 −
𝑁𝑍𝐴 𝑍𝐵 𝑒 2
(217)
ln 𝑘 = ln + ln 𝑒 − 𝑅𝑇 + ln 𝑒 𝑅𝑇4𝜋𝜀0 𝜀 𝑟
𝑁ℎ
or
∗
𝑅𝑇 𝛥𝐺𝑁𝐸𝐼 𝑁𝑍𝐴 𝑍𝐵 𝑒 2 (218)
ln 𝑘 = ln − −
𝑁ℎ 𝑅𝑇 𝑅𝑇4𝜋𝜀0 𝜀 𝑟

Which can also be expressed as

𝑁𝑍𝐴 𝑍𝐵 𝑒 2 (219)
ln 𝑘 = ln 𝑘0 −
𝑅𝑇4𝜋𝜀0 𝜀 𝑟

Where k0 represents the magnitude of the rate constant for the ionic reaction carried out in a solvent of infinite
dielectric constant so that the electrostatic interactions become zero.
 Single Sphere Model
Besides the double-sphere model, another theoretical model that is quite rationalizing is a single-
sphere model. Just like the double-sphere model, the solvent is also considered as a continuum with a ε as the
dielectric constant. However, the primary differentiating aspect of this model is that it considers the two ions,
which can same or opposite charges, to form a single-sphere activated complex.

Figure 12. The pictorial depiction of the single-sphere model of ionic reactions.

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 150 A Textbook of Physical Chemistry – Volume I

In the initial state, the ions are considered as discrete; while in the final state, they assumed to form a single-
sphere activated complex with ʻr*ʼ as the overall radius. The rate law for this case was derived by Born by
considering the energy required to charge an ion in solution. Now suppose that we need to charge a conducting
sphere of radius r from an initial value of zero to the final value Ze. This can be visualized as a process in
which a very small charge is e.dλ (λ = 0 − Z) is carried from infinite to this sphere.
Now, if ZA and ZB are the charge numbers of the participating ions and x as the distance of separation
between the sphere and the “increment” at any time, the force of electrostatic interaction (dF) between them
can be given from the Coulomb’s law as:

𝜆𝑒 2 𝑑𝜆 (220)
𝑑𝐹 =
4𝜋𝜀0 𝜀𝑥 2

Where ε0 and ε are permittivities of the vacuum (8.854 × 10−12 C2 N−1 m−2) and the dielectric constant of the
solvent used, respectively. The symbol e represents the elementary charge and has a value equal to 1.6 × 10−19
C. The amount of work done in moving the “increment” closer by an extant dx will be

𝑑𝑤 = 𝑑𝐹 × 𝑑𝑥 (221)

𝜆𝑒 2 𝑑𝜆 (222)
𝑑𝑤 = 𝑑𝑥
4𝜋𝜀0 𝜀𝑥 2

The total amount of work done can be obtained by carrying out the double integration with respect to x = ∞ –
r and λ = 0 – Z i.e.
𝑍 𝑟 (223)
𝑒2 𝜆
𝑤= ∫ ∫ 2 𝑑𝜆 𝑑𝑥
4𝜋𝜀0 𝜀 𝑥
0 ∞

𝑍2𝑒2 (224)
𝑤=
8𝜋𝜀0 𝜀 𝑟

The work given the above equation is actually the contribution of the electrostatic interactions to the Gibbs
energy of the ion i.e.

𝑍2𝑒 2 (225)
𝐺𝐸𝐼 =
8𝜋𝜀0 𝜀 𝑟

In the light of the above correlation, the electrostatic contribution to the Gibbs free energy of discrete ions and
activated complex can be written as

𝑍𝐴2 𝑒 2 (225)
𝐺𝐸𝐼 (𝐴) =
8𝜋𝜀0 𝜀 𝑟𝐴

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 CHAPTER 3 Chemical Dynamics – I 151

𝑍𝐵2 𝑒 2 (226)
𝐺𝐸𝐼 (𝐵) =
8𝜋𝜀0 𝜀 𝑟𝐵

∗
(𝑍𝐵 + 𝑍𝐵 )2 𝑒 2 (227)
𝐺𝐸𝐼 =
8𝜋𝜀0 𝜀 𝑟 ∗

Hence, the change in electrostatic contribution can be obtained simply by subtracting the sum of individual
contributions from the overall contribution i.e.

∗
(𝑍𝐵 + 𝑍𝐵 )2 𝑒 2 𝑍𝐴2 𝑒 2 𝑍𝐵2 𝑒 2 (228)
𝛥𝐺𝐸𝐼 = − −
8𝜋𝜀0 𝜀 𝑟 ∗ 8𝜋𝜀0 𝜀 𝑟𝐴 8𝜋𝜀0 𝜀 𝑟𝐵

or

∗
𝑒 2 (𝑍𝐵 + 𝑍𝐵 )2 𝑍𝐴2 𝑍𝐵2 (229)
𝛥𝐺𝐸𝐼 = [ − − ]
8𝜋𝜀0 𝜀 𝑟∗ 𝑟𝐴 𝑟𝐵

Correcting the above equation for non-electrostatic contribution 𝛥𝐺𝑁𝐸𝐼

∗
, the total molar free energy change for
the whole process can be given by the following relation.

∗ ∗ ∗
𝑁𝑒 2 (𝑍𝐵 + 𝑍𝐵 )2 𝑍𝐴2 𝑍𝐵2 (230)
𝛥𝐺 ∗ = 𝛥𝐺𝑁𝐸𝐼 + 𝛥𝐺𝐸𝐼 = 𝛥𝐺𝑁𝐸𝐼 + [ − − ]
8𝜋𝜀0 𝜀 𝑟∗ 𝑟𝐴 𝑟𝐵

Also, from the activated complex theory, we know that

𝑅𝑇 −𝛥𝐺∗ (231)
𝑘= 𝑒 𝑅𝑇
𝑁ℎ
After putting the value of ΔG* from equation (230) into equation (231), we get

𝑅𝑇 −(
∗
𝛥𝐺𝑁𝐸𝐼
+
𝑁𝑒 2 2
(𝑍𝐵 +𝑍𝐵 )2 𝑍𝐴 𝑍2
− − 𝐵 ]) (232)
𝑅𝑇 𝑅𝑇8𝜋𝜀0 𝜀 [ 𝑟∗ 𝑟𝐴 𝑟𝐵
𝑘= 𝑒
𝑁ℎ
Taking natural logarithm both side of equation (232) and rearranging, we get
∗
𝑅𝑇 𝛥𝐺𝑁𝐸𝐼 𝑁𝑒 2 (𝑍𝐵 + 𝑍𝐵 )2 𝑍𝐴2 𝑍𝐵2 (233)
ln 𝑘 = ln − − [ − − ]
𝑁ℎ 𝑅𝑇 𝑅𝑇8𝜋𝜀0 𝜀 𝑟∗ 𝑟𝐴 𝑟𝐵

Which can also be expressed as

𝑁𝑒 2 (𝑍𝐵 + 𝑍𝐵 )2 𝑍𝐴2 𝑍𝐵2 (234)

ln 𝑘 = ln 𝑘0 − [ − − ]
𝑅𝑇8𝜋𝜀0 𝜀 𝑟∗ 𝑟𝐴 𝑟𝐵

Where k0 represents the magnitude of the rate constant for the ionic reaction carried out in a solvent of infinite
dielectric constant so that the electrostatic interactions become zero.

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Table of Contents
CHAPTER 1 ................................................................................................................................................ 11
Quantum Mechanics – I ........................................................................................................................ 11
 Postulates of Quantum Mechanics .................................................................................................. 11
 Derivation of Schrodinger Wave Equation...................................................................................... 16
 Max-Born Interpretation of Wave Functions .................................................................................. 21
 The Heisenberg’s Uncertainty Principle.......................................................................................... 24
 Quantum Mechanical Operators and Their Commutation Relations............................................... 29
 Hermitian Operators – Elementary Ideas, Quantum Mechanical Operator for Linear Momentum,
Angular Momentum and Energy as Hermitian Operator ................................................................. 52
 The Average Value of the Square of Hermitian Operators ............................................................. 62
 Commuting Operators and Uncertainty Principle (x & p; E & t) .................................................... 63
 Schrodinger Wave Equation for a Particle in One Dimensional Box.............................................. 65
 Evaluation of Average Position, Average Momentum and Determination of Uncertainty in Position
and Momentum and Hence Heisenberg’s Uncertainty Principle..................................................... 70
 Pictorial Representation of the Wave Equation of a Particle in One Dimensional Box and Its
Influence on the Kinetic Energy of the Particle in Each Successive Quantum Level ..................... 75
 Lowest Energy of the Particle ......................................................................................................... 80
 Problems .......................................................................................................................................... 82
 Bibliography .................................................................................................................................... 83
CHAPTER 2 ................................................................................................................................................ 84
Thermodynamics – I .............................................................................................................................. 84
 Brief Resume of First and Second Law of Thermodynamics .......................................................... 84
 Entropy Changes in Reversible and Irreversible Processes ............................................................. 87
 Variation of Entropy with Temperature, Pressure and Volume ...................................................... 92
 Entropy Concept as a Measure of Unavailable Energy and Criteria for the Spontaneity of Reaction
...........................................................................................................................................................94
 Free Energy, Enthalpy Functions and Their Significance, Criteria for Spontaneity of a Process ... 98
 Partial Molar Quantities (Free Energy, Volume, Heat Concept) ................................................... 104
 Gibb’s-Duhem Equation ................................................................................................................ 108
 Problems ........................................................................................................................................ 111
 Bibliography .................................................................................................................................. 112
CHAPTER 3 .............................................................................................................................................. 113
Chemical Dynamics – I ........................................................................................................................ 113
 Effect of Temperature on Reaction Rates ...................................................................................... 113
 Rate Law for Opposing Reactions of Ist Order and IInd Order..................................................... 119
 Rate Law for Consecutive & Parallel Reactions of Ist Order Reactions ....................................... 127
 Collision Theory of Reaction Rates and Its Limitations ............................................................... 135
 Steric Factor................................................................................................................................... 141
 Activated Complex Theory ........................................................................................................... 143
 Ionic Reactions: Single and Double Sphere Models ..................................................................... 147
 Influence of Solvent and Ionic Strength ........................................................................................ 152
 The Comparison of Collision and Activated Complex Theory ..................................................... 157
 Problems ........................................................................................................................................ 158
 Bibliography .................................................................................................................................. 159
CHAPTER 4 .............................................................................................................................................. 160
Electrochemistry – I: Ion-Ion Interactions ..................................................................................... 160
 The Debye-Huckel Theory of Ion-Ion Interactions ....................................................................... 160
 Potential and Excess Charge Density as a Function of Distance from the Central Ion ................. 168
 Debye-Huckel Reciprocal Length ................................................................................................. 173
 Ionic Cloud and Its Contribution to the Total Potential ................................................................ 176
 Debye-Huckel Limiting Law of Activity Coefficients and Its Limitations ................................... 178
 Ion-Size Effect on Potential ........................................................................................................... 185
 Ion-Size Parameter and the Theoretical Mean - Activity Coefficient in the Case of Ionic Clouds with
Finite-Sized Ions ............................................................................................................................ 187
 Debye-Huckel-Onsager Treatment for Aqueous Solutions and Its Limitations ............................ 190
 Debye-Huckel-Onsager Theory for Non-Aqueous Solutions........................................................ 195
 The Solvent Effect on the Mobility at Infinite Dilution ................................................................ 196
 Equivalent Conductivity (Λ) vs Concentration C1/2 as a Function of the Solvent ......................... 198
 Effect of Ion Association Upon Conductivity (Debye-Huckel-Bjerrum Equation) ...................... 200
 Problems ........................................................................................................................................ 209
 Bibliography .................................................................................................................................. 210
CHAPTER 5 .............................................................................................................................................. 211
Quantum Mechanics – II .................................................................................................................... 211
 Schrodinger Wave Equation for a Particle in a Three Dimensional Box ...................................... 211
  The Concept of Degeneracy Among Energy Levels for a Particle in Three Dimensional Box .... 215
 Schrodinger Wave Equation for a Linear Harmonic Oscillator & Its Solution by Polynomial Method
.........................................................................................................................................................217
 Zero Point Energy of a Particle Possessing Harmonic Motion and Its Consequence ................... 229
 Schrodinger Wave Equation for Three Dimensional Rigid Rotator .............................................. 231
 Energy of Rigid Rotator ................................................................................................................ 241
 Space Quantization ........................................................................................................................ 243
 Schrodinger Wave Equation for Hydrogen Atom: Separation of Variable in Polar Spherical
Coordinates and Its Solution ......................................................................................................... 247
 Principal, Azimuthal and Magnetic Quantum Numbers and the Magnitude of Their Values ....... 268
 Probability Distribution Function .................................................................................................. 276
 Radial Distribution Function ......................................................................................................... 278
 Shape of Atomic Orbitals (s, p & d) .............................................................................................. 281
 Problems ........................................................................................................................................ 287
 Bibliography .................................................................................................................................. 288
CHAPTER 6 .............................................................................................................................................. 289
Thermodynamics – II ........................................................................................................................... 289
 Clausius-Clapeyron Equation ........................................................................................................ 289
 Law of Mass Action and Its Thermodynamic Derivation ............................................................. 293
 Third Law of Thermodynamics (Nernst Heat Theorem, Determination of Absolute Entropy,
Unattainability of Absolute Zero) And Its Limitation ................................................................... 296
 Phase Diagram for Two Completely Miscible Components Systems ........................................... 304
 Eutectic Systems (Calculation of Eutectic Point) .......................................................................... 311
 Systems Forming Solid Compounds AxBy with Congruent and Incongruent Melting Points ....... 321
 Phase Diagram and Thermodynamic Treatment of Solid Solutions.............................................. 332
 Problems ........................................................................................................................................ 342
 Bibliography .................................................................................................................................. 343
CHAPTER 7 .............................................................................................................................................. 344
Chemical Dynamics – II ...................................................................................................................... 344
 Chain Reactions: Hydrogen-Bromine Reaction, Pyrolysis of Acetaldehyde, Decomposition of
Ethane ............................................................................................................................................ 344
 Photochemical Reactions (Hydrogen-Bromine & Hydrogen-Chlorine Reactions) ....................... 352
 General Treatment of Chain Reactions (Ortho-Para Hydrogen Conversion and Hydrogen-Bromine
Reactions) ....................................................................................................................................... 358
  Apparent Activation Energy of Chain Reactions .......................................................................... 362
 Chain Length ................................................................................................................................. 364
 Rice-Herzfeld Mechanism of Organic Molecules Decomposition (Acetaldehyde) ...................... 366
 Branching Chain Reactions and Explosions (H2-O2 Reaction) ..................................................... 368
 Kinetics of (One Intermediate) Enzymatic Reaction: Michaelis-Menten Treatment .................... 371
 Evaluation of Michaelis's Constant for Enzyme-Substrate Binding by Lineweaver-Burk Plot and
Eadie-Hofstee Methods ................................................................................................................. 375
 Competitive and Non-Competitive Inhibition ............................................................................... 378
 Problems ........................................................................................................................................ 388
 Bibliography .................................................................................................................................. 389
CHAPTER 8 .............................................................................................................................................. 390
Electrochemistry – II: Ion Transport in Solutions ....................................................................... 390
 Ionic Movement Under the Influence of an Electric Field ............................................................ 390
 Mobility of Ions ............................................................................................................................. 393
 Ionic Drift Velocity and Its Relation with Current Density .......................................................... 394
 Einstein Relation Between the Absolute Mobility and Diffusion Coefficient .............................. 398
 The Stokes-Einstein Relation ........................................................................................................ 401
 The Nernst-Einstein Equation ....................................................................................................... 403
 Walden’s Rule ............................................................................................................................... 404
 The Rate-Process Approach to Ionic Migration ............................................................................ 406
 The Rate-Process Equation for Equivalent Conductivity .............................................................. 410
 Total Driving Force for Ionic Transport: Nernst-Planck Flux Equation ....................................... 412
 Ionic Drift and Diffusion Potential ................................................................................................ 416
 The Onsager Phenomenological Equations ................................................................................... 418
 The Basic Equation for the Diffusion ............................................................................................ 419
 Planck-Henderson Equation for the Diffusion Potential ............................................................... 422
 Problems ........................................................................................................................................ 425
 Bibliography .................................................................................................................................. 426
INDEX ......................................................................................................................................................... 427