2023/06/25

Kwame Nkrumah University of

Science & Technology, Kumasi, Ghana

CHE 254
Chemical Engineering Thermodynamics II

(2 Credits)

Instructor:
Eunice Sefakor Dogbe

LESSON 2 - THERMODYNAMIC PROPERTIES OF

FLUID MIXTURES - I

Aim and objectives

Aim: To lay the theoretical foundation for applications of thermodynamics to gas mixtures and liquid
solutions.
Objectives:
▪ Develop a fundamental property relation that is applicable to open phases of variable composition.
▪ Introduce partial properties, a class of thermodynamic properties defined mathematically to
distribute total mixture properties among individual species as they exist in a mixture. These are
composition-dependent and distinct from the molar properties of pure species.
▪ Define the chemical potential, a fundamental new property that facilitates treatment of phase and
chemical-reaction equilibria.
▪ Develop property relations for the ideal-gas-state mixture, which provide the basis for treatment of
real-gas mixtures.
▪ Define yet another useful property, the fugacity. Related to the chemical potential, it lends itself to
mathematical formulation of both phase- and chemical-reaction-equilibrium problems (continued).
▪ Introduce a useful class of solution properties, known as excess properties, in conjunction with an
idealization of solution behaviour called the ideal-solution model, which serves as a reference for
real-solution behaviour.

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Reference materials
• J.M. Smith, Hendrick Van Ness, Michael Abbot, Mark Swihart (2015).
Introduction to Chemical Engineering Thermodynamics, 8th Edition. Chapter 10
• Kevin D. Dahm and Donald P. Visco, Jr. (2015). Fundamentals of Chemical
Engineering Thermodynamics. Chapter 9
• Green, W. Don and Perry, H. Robert (2008). Perry’s Chemical Engineer’s
Handbook. New York, McGraw-Hill. Section 4

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Introduction
Measures of composition are essential variables (along with temperature and pressure already
discussed in Lesson 1) because multicomponent fluid mixtures processed in chemical industries
undergo composition changes due to mixing and separation processes, the transfer of species
from one phase to another, and chemical reaction.
The composition of mixtures can be measured in three common ways;
▪ Mole fraction: the ratio of the number of moles of a particular
chemical species, 𝑛𝑖 , in a mixture to the total number of moles of
mixture, 𝑛. Used for both reacting and nonreacting systems. For flow
or open
▪ Mass fraction: the ratio of the mass of a particular chemical species,
𝑚𝑖 , in a mixture to the total mass of mixture, 𝑚. Not suitable for processes
reacting systems but can be used for nonreacting systems.
▪ Molar concentration: the ratio of the mole fraction of a particular
chemical species, 𝑥𝑖 , in a mixture or solution to the molar volume of
the mixture or solution, 𝑉.
The molar mass of a mixture or solution is the mole-fraction-weighted
sum of the molar masses of all species present:
mሶ i and nሶ i are mass and molar flow rate of species i, respectively and q is volumetric flow rate
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Partial properties
▪ Chemical species in solution do not have their individual properties, rather an arbitrary
solution properties are assigned to the individual species.
▪ Notations for the three kinds of molar (or unit-mass) thermodynamic properties of mixtures:

Note that for a pure

fluid of specie i,
𝑀𝑖 = 𝑀 ഥ𝑖 = 𝑀

▪ For a homogenous PVT system with a total system property 𝑛𝑀 (denoted 𝑀𝑡 ) such that

▪ The total differential is

(2.1)

▪ Subscript 𝑛𝑗 indicates that all mole numbers are held constant except that of the 𝑖𝑡ℎ species.
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Eq. (2.1) can also be written in a simpler form as

(2.2)

ഥ𝑖 is the partial molar property given as

where 𝑀

ഥ𝑖 of species 𝑖 is a measure of the response of total

▪ Partial molar property, 𝑀
property 𝑛𝑀 to the addition of an infinitesimal amount of species 𝑖 to a finite
amount of solution, at constant 𝑇 and 𝑃. It is also known as a response function.
Note that 𝑀ഥ𝑖 may also be expressed on unit-mass basis instead of molar basis.
Since
𝑑𝑛𝑖 = 𝑑 𝑥𝑖 𝑛 = 𝑥𝑖 𝑑𝑛 + 𝑛𝑑𝑥𝑖 and 𝑑 𝑛𝑀 = 𝑛𝑑𝑀 + 𝑀𝑑𝑛
Replacing 𝑑𝑛𝑖 and 𝑑 𝑛𝑀 in Eq. (2.2) and grouping like terms gives
(2.3)

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Equating each bracket term in Eq. (2.3) to zero because 𝑛 and d𝑛 are independent and arbitrary gives

(2.4)

and (2.5) or

This Summability Equation (Eq. 2.5) relates the solution molar property to the partial molar property.
▪ Differentiating Eq. 2.5 gives
(2.6)

▪ Combining Eqs. 2.4 and 2.6 gives the Gibbs-Duhem Equation:

The Gibbs/Duhem Equation imposes a constraint on
how the partial molar properties of any phase may
vary with temperature, pressure, and composition.
▪ A special case of the Gibbs-Duhem equation where T and P are constant is
This equation shows that the partial molar properties cannot all vary
independently because they must add up to the total solution property.

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Partial Molar Gibbs Energy - Chemical

potential
▪ The fundamental property relation for total Gibbs energy of any closed system is

▪ For a system constant composition - a single-phase fluid in a closed system with no

chemical reactions - the partial differentials of nG with respect to T and to P are;

▪ For a more general case of a single-phase, open system, nG is a function of T and P

as well as the numbers of moles of the chemical species present; Chemical potential

▪ Therefore,
(2.7)
By definition, 𝜇𝑖 = 𝐺ҧ𝑖 , the Partial Molar Gibbs Energy
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▪ Replacing all the partial derivatives in Eq. (2.7) gives ,

The fundamental property relation for single-phase
fluid systems of variable mass and composition –
the basis for Solution Thermodynamics
▪ For one mole of solution, 𝑛 = 1 and 𝑛𝑖 = 𝑥𝑖 , therefore:
Implying that

▪ Since , 𝑥𝑖 s are all not independent variable even though 𝑛𝑖 s are.

By constraints, the following equations can be written:
and

The Gibbs energy expressed as a function of its canonical variables (natural or special pair of
independent variables), serves as a generating function, providing the means for the
calculation of all other thermodynamic properties (using their definitions) by simple
mathematical operations and it implicitly represents complete property information.
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Exercise 2.1
Write the Gibbs-Duhem Equation for the Gibb’s energy of a binary solution.

Solution
Given that a binary system is made up of two component 1 and 2 and that
𝑛𝐺 = 𝑔(𝑇, 𝑃, 𝑥1 , 𝑥2 )
The Gibbs-Duhem equation is given as
𝜕𝐺 𝜕𝐺
𝑑𝑃 + 𝑑𝑇 − (𝑥1 𝑑𝐺1ҧ ) 𝑇,𝑃,𝑥2 + (𝑥2 𝑑𝐺ҧ2 ) 𝑇,𝑃,𝑥1 = 0
𝜕𝑃 𝑇,𝑥 𝜕𝑇 𝑃,𝑥
Simplified in terms of chemical potential as

𝜕𝐺 𝜕𝐺
𝑑𝑃 + 𝑑𝑇 − (𝑥1 𝑑𝜇1 ) 𝑇,𝑃,𝑥2 + (𝑥2 𝑑𝜇2 ) 𝑇,𝑃,𝑥1 = 0
𝜕𝑃 𝑇,𝑥
𝜕𝑇 𝑃,𝑥

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Partial Properties in Binary Solutions

▪ Recall that the partial molar property is generally defined as

▪ For a binary solution (i.e. a solution made up of two species), an alternative

method is useful. Recall the equation that relates the solution molar property to
the partial molar property is

which can be expressed for binary solutions as

(2.8)
▪ The total derivative gives
(2.9)

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▪ Also recall the special case of the Gibbs-Duhem equation (simplified form) where T and P
are constant;

which can be expressed for binary solutions as

(2.10)
▪ Because 𝑥1 + 𝑥2 = 1, it implies that 𝑑𝑥1 = −𝑑𝑥2 . Eliminating 𝑑𝑥2 in Eq. (2.9) and
combining the result with Eq. (2.10) gives:
(2.11)

▪ Note that Eq. (2.8) can also be written in two other forms as (in terms of either 𝑥1 or 𝑥2 ):
and
▪ Combining these with Eq. (2.11) gives:
The equations for calculating the partial
properties of a binary system from an
(2.12) (2.13) expression for the solution property as a
function of composition at constant T and P
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Example 1
The need arises in a laboratory for 2000 cm3 of an antifreeze solution consisting of
30 mol-% methanol in water. What volumes of pure methanol and of pure water at
25°C must be mixed to form the 2000 cm3 of antifreeze, also at 25°C? Partial
molar volumes for methanol and water in a 30 mol-% methanol solution and their
pure-species molar volumes, both at 25°C, are:
Methanol (1) :
𝑉ത1= 38.632 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1
𝑉1 = 40.727 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1
Water (2) :
𝑉ത2 = 17.765 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1
𝑉2 = 18.068 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1

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Solution
Data given:

Methanol (1) : Water (2) : Solution (mixture):

𝑥1 = 0.3 𝑉ത2 = 17.765 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1 𝑉 𝑡 = 2000𝑐𝑚3
𝑉ത1= 38.632 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1 𝑉2 = 18.068 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1
𝑉1 = 40.727 𝑐𝑚3 ⋅ 𝑚𝑜𝑙 −1
Other information: Temperature is constant.
What to find: 𝑉1𝑡 and 𝑉2𝑡
By definition,
𝑉1𝑡 = 𝑛1 𝑉1 and 𝑉2𝑡 = 𝑛2 𝑉2 , where 𝑛1 + 𝑛2 = 𝑛
Also,
𝑉𝑡
𝑉 𝑡 = 𝑛𝑉, therefore, 𝑛 = 𝑉

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From the summability relation,

𝑉 = 𝑥1 𝑉ത1 + 𝑥2 𝑉ത2 = 0.3 × 38.632 + (1− 0.3) × 17.765 =24.025 𝑐𝑚3 ⋅ 𝑚𝑜𝑙−1
2000
𝑛= = 83.246 𝑚𝑜𝑙
24.025
𝑛1 = 𝑥1 𝑛 = 0.3 × 83.246 = 24.974 𝑚𝑜𝑙
𝑛2 = 𝑛 − 𝑛1 = 83.246 − 24.974 = 58.272 𝑚𝑜𝑙

Finally,
𝑽𝒕𝟏 = 𝑛1 𝑉1 = 24.974 × 40.727 = 𝟏𝟎𝟏𝟕 𝒄𝒎𝟑
And
𝑽𝒕𝟐 = 𝑛2 𝑉2 = 58.272 × 18.068 = 𝟏𝟎𝟓𝟑 𝒄𝒎𝟑

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Example 2
The enthalpy of a binary liquid system of species 1 and 2 at fixed T and P is
represented by the equation:
𝐻 = 400𝑥1 + 600𝑥2 + 𝑥1 𝑥2 ( 40𝑥1 + 20𝑥2 )
where H is in J.𝑚𝑜𝑙 −1 . Determine expressions for 𝐻 ഥ1 and 𝐻
ഥ2 as functions of 𝑥1 ,
numerical values for the pure-species enthalpies 𝐻1 and 𝐻2 , and numerical values
ഥ1∞ and 𝐻
for the partial enthalpies at infinite dilution 𝐻 ഥ2∞ .

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Solution (From Smith et al, 2015)

(2.5),

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(2.6),

Alternative
solution

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Ideal gas mixture – Partial molar properties

▪ The partial pressure of a component i in an ideal gas mixture is
𝑦𝑖 𝑅𝑇
𝑝𝑖 = 𝑦𝑖 𝑃 = 𝑖𝑔 (𝑖 = 1, 2, … . , 𝑁)
𝑉
where 𝑦𝑖 is the mole fraction of (gas) species i and note that the sum of the partial pressures
equals the total pressure.
▪ An ideal gas is a model gas comprising imaginary molecules of no size (zero volume) and no
interactions.
▪ Therefore, each chemical species in an ideal gas mixture has its own private properties,
uninfluenced by the presence of other species, giving rise to the Gibbs theorem stated as
A partial molar property (other than volume) of a constituent species in an ideal gas mixture is
equal to the corresponding molar property of the species in the pure ideal-gas state at the
mixture temperature but at a pressure equal to its partial pressure in the mixture.
▪ Mathematically, the partial molar property of species i in an ideal gas mixture is defined as
ഥ𝑖𝑖𝑔 𝑇, 𝑃 = 𝑀𝑖𝑖𝑔 𝑇, 𝑝𝑖 ;
𝑀 ഥ𝑖𝑖𝑔 ≠ 𝑉ത𝑖𝑖𝑔
𝑀
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ഥ 𝑖𝑔 can be defined for 𝐻, 𝑈, 𝑆 𝑎𝑛𝑑 𝐺 (and not for V)

▪𝑀𝑖
▪ Enthalpy and internal energy of an ideal gas are independent of pressure. Thus, it
doesn’t matter what pressure (𝑝𝑖 , P, or any other pressure) is used to model them
in the ideal gas state. Therefore,
ഥ𝑖𝑖𝑔 𝑇, 𝑃 = 𝐻𝑖𝑖𝑔 𝑇, 𝑝𝑖 = 𝐻𝑖𝑖𝑔 𝑇, 𝑃
𝐻

ഥ 𝑖𝑔 𝑇, 𝑃 = 𝑈 𝑖𝑔 𝑇, 𝑝𝑖 = 𝑈 𝑖𝑔 𝑇, 𝑃
𝑈𝑖 𝑖 𝑖

These can be simplified as

ഥ𝑖𝑖𝑔 = 𝐻𝑖𝑖𝑔
𝐻 and ഥ𝑖𝑖𝑔 = 𝑈𝑖𝑖𝑔
𝑈
▪ Entropy of an ideal gas depends on pressure as expressed by
𝐶𝑃 𝑅 𝑅
𝑑𝑆 𝑖𝑔 = 𝑇
𝑑𝑇 − 𝑃 𝑑𝑃 or 𝑑𝑆 𝑖𝑔 = − 𝑃 𝑑𝑃 (constant T)
▪ Taking the entropy difference between a component gas at its partial pressure in the
mixture and at the total pressure of the mixture and integration from 𝑝𝑖 to 𝑃 gives:
𝑖𝑔 𝑖𝑔 𝑃 𝑃
𝑆𝑖 𝑇, 𝑃 − 𝑆𝑖 𝑇, 𝑝𝑖 = −𝑅 ln = −𝑅 ln = 𝑅 ln 𝑦𝑖
𝑝𝑖 𝑦𝑖 𝑃
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▪ Rearranging the previous equation gives:

𝑖𝑔 𝑖𝑔
𝑆𝑖 𝑇, 𝑝𝑖 = 𝑆𝑖 𝑇, 𝑃 − 𝑅 ln 𝑦𝑖
▪ Applying the definition of partial molar property of an ideal gas mixture gives:
𝑖𝑔 𝑖𝑔
𝑆𝑖ҧ 𝑇, 𝑃 = 𝑆𝑖 𝑇, 𝑃 − 𝑅 ln 𝑦𝑖
𝑖𝑔 𝑖𝑔
or simply, 𝑆𝑖ҧ = 𝑆𝑖 − 𝑅 ln 𝑦𝑖
▪ From the definition of Gibb’s free energy, the following equation can be written
for an ideal gas state:
𝑖𝑔 ഥ𝑖𝑖𝑔 − T𝑆𝑖ҧ 𝑖𝑔
𝐺𝑖ҧ = 𝐻
ഥ 𝑖𝑔 and 𝑆ҧ 𝑖𝑔 gives:
▪ Substituting the derived expressions for 𝐻𝑖 𝑖
𝑖𝑔 𝑖𝑔 𝑖𝑔
𝐺𝑖ҧ = 𝐻𝑖 − T𝑆𝑖 + 𝑅𝑇 ln 𝑦𝑖
𝑖𝑔 𝑖𝑔 𝑖𝑔
or 𝜇𝑖 = 𝐺𝑖ҧ = 𝐺𝑖 + 𝑅𝑇 ln 𝑦𝑖
Note that the Gibbs theorem does not apply to volume and a different approach is
used to model the volume of ideal gas mixtures.

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▪ Molar volumes in the ideal-gas state are

𝑅𝑇
𝑉 𝑖𝑔 =
𝑃
▪ Thus, for the ideal-gas state, regardless of the nature of the gas (whether of pure or
mixed gases), the molar volume is the same for given T and P.
▪ The partial molar volume of species i in the ideal-gas-state mixture is found from the
general definition of partial molar properties, using the superscript ig to denote the
ideal-gas state:

which implies that

This result means that for the ideal-gas state at given T and P the partial molar volume,
the pure-species molar volume, and the mixture molar volume are identical.

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Summability relations for ideal gas mixture

▪ From the summability relation, the following general equation can be written for
ideal gas mixtures: 𝑀𝑖𝑔 = σ𝑖 𝑦𝑖 𝑀 ഥ𝑖𝑖𝑔
▪ The summability relations for the molar properties of ideal gas mixtures are given as:
𝑖𝑔
𝐻 𝑖𝑔 = σ𝑖 𝑦𝑖 𝐻𝑖
𝑖𝑔
𝑈 𝑖𝑔 = σ𝑖 𝑦𝑖 𝑈𝑖
𝑖𝑔
𝑆 𝑖𝑔 = σ𝑖 𝑦𝑖 𝑆𝑖 − 𝑅 σ𝑖 𝑦𝑖 ln 𝑦𝑖
𝑖𝑔
𝐺 𝑖𝑔 = σ𝑖 𝑦𝑖 𝐺𝑖 + 𝑅𝑇 σ𝑖 𝑦𝑖 ln 𝑦𝑖

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Mixing properties of ideal gas mixture

▪ Property change of mixing is defined as the property change associated with a process
in which appropriate amounts of the pure species at T and P are mixed to form one
mole of mixture at the same T and P. For the ideal-gas state, this is given as:
𝑖𝑔 𝑖𝑔
∆𝑀𝑚𝑖𝑥 = 𝑀𝑖𝑔 − σ𝑖 𝑦𝑖 𝑀𝑖
▪ These can be obtained from the ideal gas state summability relations given in the
previous slide (23) as:
𝑖𝑔 𝑖𝑔
∆𝐻𝑚𝑖𝑥 = 𝐻 𝑖𝑔 − σ𝑖 𝑦𝑖 𝐻𝑖 = 0
and
𝑖𝑔 𝑖𝑔
∆𝑈𝑚𝑖𝑥 = 𝑈 𝑖𝑔 − σ𝑖 𝑦𝑖 𝑈𝑖 = 0
For the ideal-gas state, the enthalpy change of mixing and internal energy change of
mixing are zero. For ideal-gas-state mixing at constant T and P, no heat transfer will
occur between the system and surroundings.

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▪ Entropy change of mixing for the ideal-gas state is given as:

𝑖𝑔 𝑖𝑔
∆𝑆𝑚𝑖𝑥 = 𝑆 𝑖𝑔 − ෍ 𝑦𝑖 𝑆𝑖 = −𝑅 ෍ 𝑦𝑖 ln 𝑦𝑖
𝑖 𝑖
or
𝑖𝑔 𝑖𝑔 1
∆𝑆𝑚𝑖𝑥 = 𝑆 𝑖𝑔 − ෍ 𝑦𝑖 𝑆𝑖 = 𝑅 ෍ 𝑦𝑖 ln
𝑦𝑖
𝑖 𝑖
1
In agreement with the second law this quantity is always positive since 𝑦 > 1 and
𝑖
1
(ln 𝑦 ) is positive. The mixing process is inherently irreversible, so the mixing process
𝑖
must increase the total entropy of the system and surroundings together. Since for
ideal-gas-state mixing at constant T and P, there is no heat transfer between the system
and surroundings (as seen earlier), the total entropy change of system plus
surroundings is only the entropy change of mixing.

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EXAMPLE 1 (ideal gas entropy of mixing)

What is the entropy change when you mix one mole of butane gas with one mole of
propane gas, modeled as an ideal gas mixture? Assume the pressure and temperature
of the system are constant during the process.
SOLUTION:
▪ Step 1 Identify what the problem is asking
We are looking for the ideal gas entropy change of mixing.
▪ Step 2 Utilize the given equation for ideal gas entropy change of mixing
Since we have one mole of each substance, we have an equimolar mixture, so 𝑦1 =
𝑦2 = 0.5.

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▪ Step 3 Convert to an extensive value, per problem statement.

The problem provided extensive values (moles) and asked for the entropy change,
not the molar entropy change. Thus, we need to multiply our answer by the number
of moles in the system.

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EXAMPLE 2 (ideal gas entropy of mixing)

What is the change in entropy when 0.7 𝑚3 of 𝐶𝑂2 and 0.3 𝑚3 of 𝑁2 , each at 1 bar and
25°C, blend to form a gas mixture at the same conditions? Assume ideal gases.
SOLUTION:
Let the molar entropy change of mixing be ∆𝑆 𝑖𝑔 , the entropy change of mixing
(required) be ∆𝑆 𝑖𝑔 , 𝐶𝑂2 be component 1 and 𝑁2 be component 2.
Data given:
𝑉1 = 0.7 𝑚3 𝑉2 = 0.3 𝑚3
P = 1 bar = 105 Pa
T= 25°C = 298.15 K
The molar entropy change of mixing for a binary mixture can be written as
∆𝑆 𝑖𝑔 = −𝑅 𝑦1 ln 𝑦1 + 𝑦2 ln 𝑦2
From the ideal gas law,
𝑃𝑉1 105 Pa × 0.7 𝑚3
𝑛1 = = = 28.239 𝑚𝑜𝑙𝑒𝑠
𝑅𝑇 8.314 𝐽
× 298.15 𝐾
𝑚𝑜𝑙. 𝐾
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𝑃𝑉2 105 Pa × 0.3 𝑚3

𝑛2 = = = 12.103 𝑚𝑜𝑙𝑒𝑠
𝑅𝑇 8.314 𝐽
× 298.15 𝐾
𝑚𝑜𝑙. 𝐾

𝑛 = 𝑛2 + 𝑛2 = 28.239 + 12.103 = 40.342 𝑚𝑜𝑙𝑒𝑠

𝑛1 28.239
𝑦1 = 𝑛
= 40.342 = 0.7 and 𝑦2 = 1 − 𝑦1 = 1 − 0.7 = 0.3

𝐽 𝐽
∆𝑆 𝑖𝑔 = −8.314 0.7 ln 0.7 + 0.3 ln 0.3 = 5.0787
𝑚𝑜𝑙. 𝐾 𝑚𝑜𝑙
The entropy change of mixing is
∆𝑆 𝑖𝑔 = 𝑛 × ∆𝑆 𝑖𝑔 = 40.342 × 5.0787 = 𝟐𝟎𝟒. 𝟖𝟖 𝑱

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Alternative solution to Example 2 (if you interested) :

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Step 3 of 3 (cont’d)

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Thank you

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