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4

Physical transformations

of pure substances

Answers to discussion questions

D4.1 Consider two phases of a system, labeled and . The phase with the lower chemical potential under

the given set of conditions is the more stable phase. First consider the variation of with temperature

at a xed pressure. We have

_

T

_

p

= S

and

_

T

_

p

= S

.

Therefore, if S

increases because its chemical potential decreases more rapidly with temperature than for the phase.

We also have

_

P

_

T

= V

m,

and

_

P

_

T

= V

m,

.

Therefore, if V

m,

is larger than V

m,

the phase will be favored over the phase as pressure increases

because the chemical potential of the phase will not increase as rapidly with pressure as that of the

phase. See Example 4.1.

D4.3 Refer to Fig. 4.1 above and Fig. 4.5 in the text. Starting at point A and continuing clockwise on path

p(T) toward point B, we see a gaseous phase only within the container with water at pressures and

temperatures p(T). Upon reaching point B on the vapor pressure curve, liquid appears on the bottom of

the container and a phase boundary or meniscus is evident between the liquid and less dense gas above

it. The liquid and gaseous phases are at equilibrium at this point. Proceeding clockwise away from the

vapor pressure curve the meniscus disappears and the system becomes wholly liquid. Continuing along

p(T) to point C at the critical temperature no abrupt changes are observed in the isotropic uid. Before

point C is reached, it is possible to return to the vapor pressure curve and a liquidgas equilibrium by

reducing the pressure isothermally. Continuing clockwise from point C along path p(T) back to point A,

no phase boundary is observed even though we now consider the water to have returned to the gaseous

state. Additionally, if the pressure is isothermally reduced at any point after point C, it is impossible to

return to a liquidgas equilibrium.

When the path p(T) is chosen to be very close to the critical point, the water appears opaque. At near

critical conditions, densities and refractive indices of both the liquid and gas phases are nearly identical.

Furthermore, molecular uctuations cause spatial variations of densities and refractive indices on a scale

large enough to strongly scatter visible light. This is called critical opalescence.

TRAPP: CHAP04 2006/3/8 17:05 PAGE 82 #2

82 SOLUTIONS MANUAL

A

B

C

Critical point

Exploration

Path p(T)

Vapor pressure curve of water

221.2 bar

647.4 K

p

T

Figure 4.1 Vapor pressure curve of water

D4.5 The supercritical uid extractor consists of a pump to pressurize the solvent (e.g. CO

2

), an oven with

extractionvessel, anda trappingvessel. Extractions are performeddynamicallyor statically. Supercritical

uid ows continuously through the sample within the extraction vessel when operating in dynamic

mode. Analytes extracted into the uid are released through a pressure-maintaining restrictor into a

trapping vessel. In static mode the supercritical uid circulates repetitively through the extraction vessel

until being released into the trapping vessel after a period of time. Supercritical carbon dioxide volatilizes

when decompression occurs upon release into the trapping vessel.

Advantages Disadvantages Current uses

Dissolving power of SCF can

be adjusted with selection of T

and p

Elevated pressures are required

and the necessary apparatus

expensive

Extraction of caffeine, fatty

acids, spices, aromas, avors,

and biological materials from

natural sources

Select SCFs are inexpensive

and non-toxic. They reduce

pollution

Cost may prohibit large scale

applications

Extraction of toxic salts (with

a suitable chelation agent) and

organics from contaminated

water

Thermally unstable analytes

may be extracted at low

temperature

Modiers like methanol (110%)

may be required to increase

solvent polarity

Extraction of herbicides from

soil

The volatility of scCO

2

makes

it easy to isolate analyte

scCO

2

is toxic to whole cells in

biological applications (CO

2

is not

toxic to the environment)

scH

2

O oxidation of toxic,

intractable organic waste

during water treatment

SCFs have high diffusion rates,

low viscosity, and low surface

tension

Synthetic chemistry, polymer

synthesis and crystallization,

textile processing

O

2

and H

2

are completely

miscible with scCO

2

. This

reduces multi-phase reaction

problems

Heterogeneous catalysis for

green chemistry processes

TRAPP: CHAP04 2006/3/8 17:05 PAGE 83 #3

PHYSICAL TRANSFORMATIONS OF PURE SUBSTANCES 83

D4.7 First-order phase transitions showdiscontinuities in the rst derivative of the Gibbs energy with respect to

temperature. They are recognized by nite discontinuities in plots of H, U, S, and V against temperature

and by an innite discontinuity in C

p

. Second-order phase transitions show discontinuities in the second

derivatives of the Gibbs energy with respect to temperature, but the rst derivatives are continuous. The

second-order transitions are recognized by kinks in plots of H, U, S, and V against temperature, but most

easily by a nite discontinuity in a plot of C

p

against temperature. A -transition shows characteristics

of both rst- and second-order transitions and, hence, is difcult to classify by the Ehrenfest scheme. It

resembles a rst-order transition in a plot of C

p

against T, but appears to be a higher-order transition

with respect to other properties.

At the molecular level rst-order transitions are associated with discontinuous changes in the interaction

energies between the atoms or molecules constituting the systemand in the volume they occupy. One kind

of second-order transition may involve only a continuous change in the arrangement of the atoms from

one crystal structure (symmetry) to another while preserving their orderly arrangement. In one kind of

8-transition, called an orderdisorder transition, randomness is introduced into the atomic arrangement.

See Figs. 4.18 and 4.19 of the text.

Solutions to exercises

E4.1(a) On the assumption that the vapor is a perfect gas and that

vap

H is independent of temperature, we

may write

p = p

, =

_

vap

H

R

_

_

1

T

1

T

_

[4.12], ln

p

p

= .

1

T

=

1

T

+

R

vap

H

ln

p

p

=

1

297.25 K

+

_

8.314 J K

1

mol

1

28.7 10

3

J mol

1

_

ln

53.3 kPa

70.0 kPa

= 3.285 10

3

K

1

.

Hence, T = 304 K = 31

C .

E4.2(a)

dp

dT

=

trs

S

trs

V

[4.6].

fus

S =

fus

V

_

dp

dT

_

fus

V

p

T

[

fus

S and

fus

V assumed independent of temperature].

fus

S = [(163.3 161.0) 10

6

m

3

mol

1

]

_

(100 1) (1.013 10

5

Pa)

(351.26 350.75) K

_

= +45.23 J K

1

mol

1

.

fus

H = T

f

S = (350.75 K) (45.23 J K

1

mol

1

) = +16 kJ mol

1

.

TRAPP: CHAP04 2006/3/8 17:05 PAGE 84 #4

84 SOLUTIONS MANUAL

E4.3(a) The expression for ln p is the indenite integral of eqn 4.11,

_

d ln p =

_

vap

H

RT

2

dT; ln p = constant

vap

H

RT

.

Therefore,

vap

H = (2501.8 K) R = (2501.8 K) (8.314 J K

1

mol

1

) = +20.80 kJ mol

1

.

E4.4(a) (a) The indenitely integrated form of eqn 4.11 is used as in Exercise 4.3(a).

ln p = constant

vap

H

RT

, or log p = constant

vap

H

2.303RT

.

Therefore,

vap

H = (2.303) (1780 K) R = (2.303) (1780 K) (8.314 J K

1

mol

1

)

= +34.08 kJ mol

1

.

(b) The boiling point corresponds to p = 1.000 atm = 760 Torr.

log 760 = 7.960

1780 K

T

b

, T

b

= 350.5 K .

E4.5(a)

T

fus

V

fus

S

p [4.6, and Exercise 4.2(a)]

T

f

fus

V

fus

H

p =

T

f

pM

fus

H

=

_

1

_

[V

m

= M/]

_

(278.6 K) (999) (1.013 10

5

Pa) (78.12 10

3

kg mol

1

)

10.59 10

3

J mol

1

_

_

1

879 kg m

3

1

891 kg m

3

_

3.18 K.

Therefore, at 1000 atm, T

f

(278.6 +3.18) K = 281.8 K [8.7

C].

E4.6(a) The rate of loss of mass of water may be expressed as

dm

dt

=

dn

dt

M

H

2

O

; n =

q

vap

H

.

dn

dt

=

(dq/dt)

vap

H

=

(1.2 10

3

Wm

2

) (50 m

2

)

44.0 10

3

J mol

1

= 1.4 mols

1

.

dm

dt

= (1.4 mols

1

) (18.02 g mol

1

) = 25 g s

1

.

E4.7(a) Assume perfect gas behavior.

n =

pV

RT

, n =

m

M

, V = 75 m

3

.

m =

pVM

RT

.

TRAPP: CHAP04 2006/3/8 17:05 PAGE 85 #5

PHYSICAL TRANSFORMATIONS OF PURE SUBSTANCES 85

(a) m =

(3.2 kPa) (75 m

3

) (18.02 10

3

kg mol

1

)

(8.314 10

3

kPa K

1

mol

1

) (298.15 K)

= 1.7 kg .

(b) m =

(13.1 kPa) (75 m

3

) (78.11 10

3

kg mol

1

)

(8.314 10

3

kPa K

1

mol

1

) (298.15 K)

= 31 kg .

(c) m =

(0.23 Pa) (75 m

3

) (200.59 g mol

1

)

(8.314 Pa m

3

K

1

mol

1

) (298.15 K)

= 1.4 g .

Question. Assuming all the mercury vapor breathed remains in the body, how long would it take to

accumulate 1.4 g? Make reasonable assumptions about the volume and frequency of a breath.

E4.8(a) The ClausiusClapeyron equation [4.11] integrates to the form [4.12] which may be rewritten as

ln

_

p

2

p

1

_

=

vap

H

R

_

1

T

1

1

T

2

_

.

(a)

ln

_

40 kPa

10 kPa

_

=

_

vap

H

8.314 J K

1

mol

1

_

_

1

359.0 K

1

392.5 K

_

,

1.405 =

vap

H (2.86 10

5

J

1

mol),

vap

H = 49.1 kJ mol

1

.

(b) The normal boiling point corresponds to a vapor pressure of 760 Torr. Using the data at 119.3

C

ln

_

101.3 kPa

5.3 kPa

_

=

_

49.1 10

3

J mol

1

8.314 J K

1

mol

1

_

_

1

392.5 K

1

T

b

_

,

2.950 = 15.04

5905 K

T

b

; T

b

= 488 K = 215

C .

[The accepted value is 218

C.]

(c)

vap

S(T

b

) =

vap

H(T

b

)

T

b

49.1 10

3

J mol

1

488 K

= 101 J K

1

mol

1

.

E4.9(a)

T = T

f

(50 bar) T

f

(1 bar)

T

f

pM

fus

H

_

1

_

[Exercise 4.5(a)],

fus

H = 6.01 kJ mol

1

[Table 2.3],

T =

_

(273.15 K) (49 10

5

Pa) (18 10

3

kg mol

1

)

6.01 10

3

J mol

1

_

_

1

1.00 10

3

kg m

3

1

9.2 10

2

kg m

3

_

= 0.35 K.

T

f

(50 bar) = (273.15 K) (0.35 K) = 272.80 K .

TRAPP: CHAP04 2006/3/8 17:05 PAGE 86 #6

86 SOLUTIONS MANUAL

E4.10(a)

vap

H =

vap

U +

vap

(pV) = 40.656 kJ mol

1

[Table 2.3]

vap

(pV) = p

vap

V = p(V

gas

V

liq

) pV

gas

= RT [per mole, perfect gas]

= (8.314 J K

1

mol

1

) (373.2 K) = 3.102 10

3

kJ mol

1

Fraction =

vap

(pV)

vap

H

=

3.102 10

3

kJ mol

1

40.656 kJ mol

1

= 0.07630 7.6 per cent

Solutions to problems

Solutions to numerical problems

P4.1 At the triple point, T

3

, the vapor pressures of liquid and solid are equal; hence

10.5916

1871.2 K

T

3

= 8.3186

1425.7 K

T

3

; T

3

= 196.0 K .

log(p

3

/Torr) =

1871.2 K

196.0 K

+10.5916 = 1.0447; p

3

= 11.1 Torr .

P4.3 (a)

dp

dT

=

vap

S

vap

V

=

vap

H

T

b

vap

V

[4.6, Clapeyron equation]

=

14.4 10

3

J mol

1

(180 K)

_

14.5 10

3

1.15 10

4

_

m

3

mol

1

= +5.56 kPa K

1

.

(b)

dp

dT

=

vap

H

RT

2

p

_

4.11, with d ln p =

dp

p

_

=

_

14.4 10

3

J mol

1

_

_

1.013 10

5

Pa

_

_

8.314 J K

1

mol

1

_

(180 K)

2

= +5.42 kPa K

1

.

The percentage error is 2.5 per cent .

P4.5 (a)

_

(1)

p

_

T

_

(s)

p

_

T

= V

m

(l) V

m

(s)[4.13] = M

_

1

_

=

_

18.02 g mol

1

_

_

1

1.000 g cm

3

1

0.917 g cm

3

_

= 1.63 cm

3

mol

1

.

(b)

_

(g)

p

_

T

_

(l)

p

_

T

= V

m

(g) V

m

(l)

=

_

18.02 g mol

1

_

_

1

0.598 g dm

3

1

0.958 10

3

g dm

3

_

= +3.01 dm

3

mol

1

.

TRAPP: CHAP04 2006/3/8 17:05 PAGE 87 #7

PHYSICAL TRANSFORMATIONS OF PURE SUBSTANCES 87

At 1.0 atm and 100

C, (g) (1) V

vap

p =

(as in Problem 4.4)

(30.1 10

3

m

3

mol

1

) (0.2) (1.013 10

5

Pa) + 0.6 kJ mol

1

.

Since (g) > (l), the gas tends to condense into a liquid.

P4.7 The amount (moles) of water evaporated is n

g

=

p

H

2

O

V

RT

.

The heat leaving the water is q = n

vap

H.

The temperature change of the water is T =

q

nC

p,m

, n =amount of liquid water.

Therefore, T =

p

H

o

2

V

vap

H

RTnC

p,m

=

(3.17 kPa)

_

50.0 dm

3

_

_

44.0 10

3

J mol

1

_

_

8.314 kPa dm

3

K

1

mol

1

_

(298.15 K)

_

75.5 J K

1

mol

1

_

(250 g/18.02 g mol

1

)

= 2.7K.

The nal temperature will be about 22

C .

P4.9 (a) Follow the procedure in Problem 4.8, but note that T

b

= 227.5

(b) Draw up the following table. The points are plotted in Fig. 4.2. The slope is

/

T/K 330.6 373.6 406.2 430.5 476.7 500.7

1000 K/T 3.02 2.68 2.46 2.32 2.10 2.00

ln p/Torr 0.00 2.30 3.69 4.61 5.99 6.63

6.4 10

3

K, so

vap

H

R

= 6.4 10

3

K,

implying that

vap

H = +53 kJ mol

1

.

P4.11 (a) The phase diagram is shown in Fig. 4.3.

(b) The standard melting point is the temperature at which solid and liquid are in equilibrium at 1 bar.

That temperature can be found by solving the equation of the solidliquid coexistence curve for the

temperature

1 = p

3

/bar +1000(5.60 +11.727x)x.

So 11727x

2

+5600x +

_

4.362 10

7

1

_

= 0.

TRAPP: CHAP04 2006/3/8 17:05 PAGE 88 #8

88 SOLUTIONS MANUAL

Figure 4.2

Figure 4.3

The quadratic formula yields

x =

5600

_

(5600)

2

4 (11 727) (1)

_

1/2

2 (11 727)

=

1

_

1 +(4(11 727))/5600

2

_

1/2

2 ((11 727)/5600)

.

The square root is rewritten to make it clear that the square root is of the form {1 +a}

1/2

, with

a 1; thus the numerator is approximately 1 +

_

1 +

1

2

a

_

=

1

2

a, and the whole expression

reduces to

x 1/5600 = 1.79 10

4

.

Thus, the melting point is

T = (1 +x) T

3

= (1.000179) (178.15 K) = 178.18 K .

(c) The standard boiling point is the temperature at which the liquid and vapor are in equilibrium at

1 bar. That temperature can be found by solving the equation of the liquidvapor coexistence curve

for the temperature. This equation is too complicated to solve analytically, but not difcult to solve

numerically with a spreadsheet. The calculated answer is T = 383.6 K .

TRAPP: CHAP04 2006/3/8 17:05 PAGE 89 #9

PHYSICAL TRANSFORMATIONS OF PURE SUBSTANCES 89

(d) The slope of the liquidvapor coexistence curve is given by

dp

dT

=

vap

H

T

vap

V

so

vap

H

= T

vap

V

dp

dT

.

The slope can be obtained by differentiating the equation for the coexistence curve.

dp

dT

= p

dlnp

dT

= p

dlnp

dy

dy

dT

,

dp

dT

=

_

10.413

y

2

15.996 +2(14.015)y 3(5.0120)y

2

(1.70) (4.7224) (1 y)

0.70

_

_

p

T

c

_

.

At the boiling point, y = 0.6458, so

dp

dT

= 2.851 10

2

bar K

1

= 2.851 kPa K

1

and

vap

H

= (383.6 K)

_

(30.3 0.12) dm

3

mol

1

1000 dm

3

m

3

_

_

2.851 kPa K

1

_

= 33.0 kJ mol

1

.

Solutions to theoretical problems

P4.13

_

G

p

_

T

=

_

G

p

_

T

_

G

p

_

T

= V

.

Therefore, if V

= V

= V

, so that G is nonzero,

though small, since V

is small.

P4.15 Amount of gas bubbled through liquid =

pV

RT

(p = initial pressure of gas and emerging gaseous mixture).

Amount of vapor carried away =

m

M

.

Mole fraction of vapor in gaseous mixture =

m/M

(m/M) +(pV/RT)

.

Partial pressure of vapor = p =

m/M

(m/M) +(pV/RT)

p =

p (mRT/PVM)

(mRT/PVM) +1

=

mPA

mA +1

, A =

RT

PVM

.

For geraniol, M = 154.2 g mol

1

, T = 383 K, V = 5.00 dm

3

, p = 1.00 atm, and m = 0.32 g, so

A =

_

8.206 10

2

dm

3

atm K

1

mol

1

_

(383 K)

(1.00 atm)

_

5.00 dm

3

_

_

154.2 10

3

kg mol

1

_ = 40.76 kg

1

.

TRAPP: CHAP04 2006/3/8 17:05 PAGE 90 #10

90 SOLUTIONS MANUAL

Therefore

p =

_

0.32 10

3

kg

_

(760 Torr)

_

40.76 kg

1

_

_

0.32 10

3

kg

_

_

40.76 kg

1

_

+1

= 9.8 Torr .

P4.17 In each phase the slopes are given by

_

T

_

p

= S

m

[4.1].

The curvatures of the graphs of

.

against T are given by

_

T

2

_

p

=

_

S

m

T

_

p

=

1

T

C

p,m

[Problem 3.26].

Since C

p,m

is necessarily positive, the curvatures in all states of matter are necessarily negative. C

p,m

is often largest for the liquid state, though not always, but it is the ratio C

p,m

/T that determines the

magnitude of the curvature, so no precise answer can be given for the state with the greatest curvature.

It depends upon the substance.

P4.19 S

m

= S

m

(T, p).

dS

m

=

_

S

m

T

_

p

dT +

_

S

m

p

_

T

dp.

_

S

m

T

_

p

=

C

p,m

T

[Problem 3.26] ,

_

S

m

p

_

T

=

_

V

m

T

_

p

[Maxwell relation] .

dq

rev

= T dS

m

= C

p,m

dT T

_

V

m

T

_

p

dp.

C

S

=

_

q

T

_

s

= C

p,m

TV

m

_

p

T

_

s

= C

p,m

V

m

H

m

V

m

[4.7] .

Solutions to applications

P4.21 (a) The Dieterici equation of state is purported to have good accuracy near the critical point. It does fail

badly at high densities where V

m

begins to approach the value of the Dieterici coefcient b. We will

use it to derive a practical equation for the computations.

p

r

=

e

2

T

r

e

2/T

r

V

r

2V

r

1

[Table 1.7].

Substitution of the Dieterici equation of state derivative (p

r

/T

r

)

V

r

= (2 +T

r

V

r

)p

r

/T

2

r

V

r

into the

reduced form of eqn 3.48 gives

_

U

r

V

r

_

T

r

= T

r

_

p

r

T

r

_

V

r

p

r

=

2p

r

T

r

V

r

(U

r

= U/p

c

V

c

).

TRAPP: CHAP04 2006/3/8 17:05 PAGE 91 #11

PHYSICAL TRANSFORMATIONS OF PURE SUBSTANCES 91

Integration along the isotherm T

r

from an innite volume to V

r

yields the practical computational

equation.

U

r

(T

r

, V

r

) =

_

T

r

constant

2p

r

(T

r

, V

r

)

T

r

V

r

dV

r

.

The integration is performed with mathematical software.

(c) (T

r

, V

r

) =

p

c

U

r

/V

r

where p

c

= 72.9 atm.

Carbon dioxide should have solvent properties similar to liquid carbon tetrachloride (8 9)

when the reduced pressure is in the approximate range

0.85 to 0.90 when T

r

= 1

2 (a)

(b)

3

4

5

6

7

0.5 1 1.5 2 2.5 3 3.5 4

T

r

=1.5

T

r

=1.2

p

r

U

r

T

r

=1

4.5

T

r

=1.5

p

r

T

r

=1

0.95 0.9 1 0.85 0.8 0.75

5

10

15

atm

20

Solubility parameter of carbon dioxide

Figure 4.4

TRAPP: CHAP04 2006/3/8 17:05 PAGE 92 #12

92 SOLUTIONS MANUAL

P4.23 C(graphite) C(diamond) ,

r

G

= 2.8678 kJ mol

1

at Tc . Tc = 25

C.

We want the pressure at which

r

G = 0; above that pressure the reaction will be spontaneous. Equation

3.50 determines the rate of change of

r

G with p at constant T.

(1)

_

r

G

p

_

T

=

r

V = (V

D

V

G

)M

where M is the molar mass of carbon; V

D

and V

G

are the specic volumes of diamond and graphite,

respectively.

r

G( Tc , p) may be expanded in a Taylor series around the pressure p

= 100 kPa at Tc .

(2)

r

G( Tc , p) =

r

G

_

Tc , p

_

+

_

r

G

_

Tc , p

_

p

_

T

_

p p

_

+

1

2

_

r

G

(T, p

)

p

2

_

T

_

p p

_

2

+

_

p p

_

3

.

We will neglect the third- and higher-order terms; the derivative of the rst-order term can be

calculated with eqn 1. An expression for the derivative of the second-order term can be derived with

eqn 1.

(3)

_

r

G

p

2

_

T

=

__

V

D

p

_

T

_

V

G

p

_

T

_

M = {V

G

T

(G) V

D

T

(D)} M [2.52 with 2.22].

Calculating the derivatives of eqns 1 and 2 at Tc and p

,

(4)

_

r

G

_

Tc , p

_

p

_

T

= (0.284 0.444)

_

cm

3

g

_

_

12.01 g

mol

_

= 1.92 cm

3

mol

1

,

(5)

_

r

G

_

Tc , p

_

p

2

_

T

= {0.444(3.04 10

8

) 0.284(0.187 10

8

)}

_

cm

3

kPa

1

g

_

_

12.01 g

mol

_

= 1.56 10

7

cm

3

(kPa)

1

mol

1

.

It is convenient to convert the value of

r

G

to the units cm

3

kPa mol

1

,

AQ: Kindly

provide closing

bracket

r

G

= 2.8678 kJ mol

1

_

8.315 10

2

dm

3

bar K

1

mol

1

8.315J K

1

mol

1

_

10

3

cm

3

dm

3

_

_

10

5

Pa

bar

_

.

(6)

r

G

= 2.8678 10

6

cm

3

kPa mol

1

.

Setting = p p

2.8678 10

6

cm

3

kPa mol

1

(1.92 cm

3

mol

1

) +(7.80 10

8

cm

3

kPa

1

mol

1

)

2

= 0

TRAPP: CHAP04 2006/3/8 17:05 PAGE 93 #13

PHYSICAL TRANSFORMATIONS OF PURE SUBSTANCES 93

when

r

G( Tc , p) = 0. One real root of this equation is

= 1.60 10

6

kPa = p p

or

p = 1.60 10

6

kPa 10

2

kPa

= 1.60 10

6

kPa = 1.60 10

4

bar .

Above this pressure the reaction is spontaneous. The other real root is much higher: 2.3 10

7

kPa.

Question. What interpretation might you give to the other real root?

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