Chemistry Reference
In-Depth Information
entropy losses due to the uniform swelling of a randomly branched polymer, up to
the size R , can be accounted for as [ 99 , 100 ] :
R 2
k B T =
F conf /
(24)
(
Nn
)
1
/
2 a 2
where R ideal =
1 / 4 is the unperturbed, Gaussian, size of an ideal, randomly
branched polymer [ 101 ] . Balancing the entropic elastic force with the intramolecu-
lar Coulomb repulsions and/or the osmotic pressure of counterions leads to:
a
(
Nn
)
aN 5 / 6
2 l B
1
/
3 n 1 / 6
2
) 2
( α
/
a
)
,
N
/
n
( α (
l B
/
a
)
R random =
(25)
aN 3 / 4
1
/
2 n 1 / 4
2
) 2
α
,
N
/
n
( α (
l B /
a
)
An interesting feature of ( 25 ) is the fractal dimension, specifying how the mass
N
of a randomly branched PE depends on its size R . For small clusters that release
many counterions into the bulk solution, d f
=
/
6
5, whereas for large (osmotic) clus-
=
/
ters, d f
3. Again, the counterion localization threshold is set by the increase in
the electrostatic potential, =
4
N 1 / 6 in
the regime of free counterions (small clusters). Another remarkable feature of ( 25 )
is, that the counterion condensation threshold occurs when the number of branching
points N
l B Q
/
R which grows upon an increase in N as
n reaches the characteristic value = α 2
) 4 , which again is indepen-
/
(
l B /
a
dent of the spacer length n .
These results have been generalized further in [ 31 ], for charged polymeric frac-
tals with arbitrary connectivity characterized by spectral dimension, d s , (the latter
relates the longest path in the fractal, R max =
aN 1 / d s , to its mass
N ) and arbitrary
fractal dimension d f (in the absence of ionic charges) in d -dimensional space. For
ideal (Gaussian) fractals d f =
2 d s / (
2
d s )
. For charged fractals:
d s
d s d f +( d 2 )( d f d s )
2 d f
d s
d s d f +( d 2 )( d f d s )
d f
2 l B /
N
aN
( α
a
)
,
N
R fractal =
(26)
d f
d s
d s d f
aN 1 / d s
N
α
,
N
Here, the threshold value for the number of monomers, corresponding to the onset
of charge renormalization, is specified as:
d s d f (
d
2
)(
d f
d s )
d s
N = α
(
l B /
a
)
(27)
d f ( d 2 d s )
(
d
2
d s )
As follows from ( 26 ) charge renormalization effects occur only when d
<
d s +
2.
4.3
Polyelectrolyte Cylindrical (Molecular) Brushes
Molecular brushes are polymers composed of a long main chain (backbone), onto
which side chains (grafts) are attached at regular intervals. See Fig. 4 c for a graphic
illustration. The graft-copolymers are classified as molecular brushes, provided the
 
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