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2014 | OriginalPaper | Buchkapitel

3. Crystallization, Micro- and Nano-structure, and Melting Behavior of Polymer Blends

verfasst von : G. Groeninckx, C. Harrats, M. Vanneste, V. Everaert

Erschienen in: Polymer Blends Handbook

Verlag: Springer Netherlands

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Abstract

When the melt of a crystalline polymer is cooled to a temperature between the glass transition and the equilibrium melting point, the thermodynamic requirement for crystallization is fulfilled.
In a crystallizable miscible blend, however, the presence of an amorphous component, either thermoplastic or thermosetting, can either increase or decrease the tendency to crystallize depending on the effect of the composition of the blend on its glass transition and on the equilibrium melting point of the crystallizable component and also on the curing extent and conditions in case of thermosetting amorphous component. The type of segregation of the amorphous component, influenced by parameters such as crystallization conditions, chain microstructure, molecular weight, blend composition, and curing extent, determines to a large extent the crystalline morphology of a crystallizable binary blend. Separate crystallization, concurrent crystallization, or cocrystallization can occur in a blend of two crystallizable components. The spherulite growth of the crystallizable component in miscible blends is influenced by the type and molecular weight of the amorphous component, the former affecting the intermolecular interactions between both components and the latter the diffusion of the amorphous component. The blend composition, the crystallization conditions, the degree of miscibility and the mobility of both blend components, and the nucleation activity of the amorphous component are important factors with respect to the crystallization kinetics. The melting behavior of crystallizable miscible blends often reveals multiple DSC endotherms, which can be ascribed to recrystallization, secondary crystallization, or liquid-liquid phase separation. Complex crystallization behavior develops in miscible blends containing a crystallizable thermoplastic and a curable thermosetting component. That depends on the temperature and time of curing the thermosetting and also on whether crystallization is initiated before, during, or after the curing process.
For the discussion of the crystallization and melting behavior in immiscible polymer blends, a division into three main classes is proposed.
In blends with a crystallizable matrix and an amorphous dispersed phase, both the nucleation behavior and the spherulite growth rate of the matrix can be affected. Nucleation of the matrix always remains heterogeneous; however, the amount of nuclei can be altered due to migration of heterogeneous nuclei during melt-mixing. Blending can also influence the spherulite growth rate of the matrix. During their growth, the spherulites can have to reject, occlude, or deform the dispersed droplets. In general, the major influence of blending is a change in the spherulite size and semicrystalline morphology of the matrix.
A completely different behavior is reported for blends in which the crystallizable phase is dispersed. Fractionated crystallization of the dispersed droplets, associated with different degrees of undercooling and types of nuclei, is the rule. The most important reason is a lack of primary heterogeneous nuclei within each crystallizable droplet. An important consequence of fractionated crystallization may be a drastic reduction in the degree of crystallinity.
When two crystallizable components are blended, a more complex behavior due to the influence of both phases on each other is expected. In general, the discussion for matrix crystallization and droplet crystallization can be combined. However, crystallization of one of the phases can sometimes directly induce crystallization in the second phase. As a consequence, the discussion of blends of this type has been subdivided with respect to the physical state of the second phase during crystallization. The special case of “coincident crystallization,” in which the two phases crystallize at the same time, is discussed. Finally, the effect of compatibilization of crystalline/crystalline polymer blends is briefly reviewed.
A new section has been added, introduced to deal with crystallization phenomena in immiscible polymer blends containing nanoparticles. Recent reports, although few, discuss the effect of nanoparticles on crystallization and melting in immiscible polymer blends.

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Glossar
Notations and Abbreviations
AN
Acrylonitrile
aPMMA
Atactic poly(methyl methacrylate)
aPS
Atactic polystyrene
BR
Butyl rubber
CPE
Chlorinated polyethylene
DDS
4,4′-diaminodiphenylsulfone
DGEBA
Diglycidyl ether of bisphenol A
DHDPE
Deuterated high-density polyethylene
EBA
Ethylene butylacrylate
EEA
Elastomeric copolymer from ethylene and ethyl acrylate
EGMA
Ethylene glycidyl methacrylate
EPDM
Elastomeric terpolymer from ethylene, propylene, and a non-conjugated diene
EPR
Elastomeric ethylene-propylene copolymer
EPR-g-SA
Elastomeric ethylene-propylene copolymer grafted with styrene acrylonitrile
ER
Epoxy resin
EVAc
Poly(ethylene-co-vinyl acetate) (random)
FVA
Poly(vinyl acetate-co-di-n-tetradecyl fumarate) (alternating)
GMA
Glycidyl methacrylate copolymer
HDPE
High-density polyethylene
iP(p-Me-S)
Isotactic copolymer of styrene and p-methyl styrene
iPEMA
Isotactic poly(ethyl methacrylate)
iPMMA
Isotactic poly(methyl methacrylate)
iPS
Isotactic polystyrene
LDPE
Low-density polyethylene
LLDPE
Linear low-density polyethylene
MA or MAH
Maleic anhydride
MCDEA
4,4′-methylenebis(3-chloro-2,6-diethylaniline
P(4-Me-pentene)
Poly(4-methyl pentene)
P(E)0.43(K)0.57
Random copolymer of phenyl ether and phenyl ketone
P(iPr-vinyl ether)
Poly(isopropyl-vinyl ether)
P(sec-But-vinyl ether)
Poly(sec-butyl vinyl ether)
PA-11
Polyamide 11
PA-12
Polyamide 12
PA-6
Polyamide 6
PA-66
Polyamide 66
PAr
Polyarylate
PBA
Poly(1,4.butylene adipate)
PBT
Polybutyleneterephthalate
PC
Bisphenol-A polycarbonate
PCDS
Poly(1,4-cyclohexane-dimethylene succinate)
PCL
Poly-e-caprolactone
PDPA
Poly(2,2-dimethyl-1,3-propylene adipate)
PDPS
Poly(2,2-dimethyl-1,3-propylene succinate)
PE
Polyethylene
PEA
Poly(ethylene adipate)
PECH
Poly(epichlorohydrin)
PED
n-Dodecyl ester terminated poly(ethylene glycol)
PEE
Poly(ester-ether) segmented block copolymers
PEEEK
Poly(ether ether ether ketone)
PEEK
Poly(ether ether ketone)
PEEKK
Poly(ether ether ketone ketone)
PEG
Polyethylene glycol (also PEO)
PEI
Poly(ether imide)
PEK
Poly(ether ketone)
PEKK
Poly(ether ketone ketone)
PEMA
Polyethylmethacrylate
Penton
Poly[3,3-bis(chloromethyl)oxetane]
PET
Polyethyleneterephthalate
PET-b-PS
Block copolymer of PET and PS segments
Phenoxy
Poly(hydroxy ether of bisphenol A)
PI
Di-n-octadecyl ester of itaconic acid
PI
Polyisoprene
PIB
Polyisobutene
PMMA
Polymethylmethacrylate
POM
Polyoxymethylene
PP
Isotactic polypropylene
PPE, PPO
Poly(2,6-dimethyl 1,4-phenylene ether), GE Co. trade name
PPG
Poly(propylene glycol)
PPS
Poly(phenylene sulfide)
PS
Atactic polystyrene
PSMA
Poly(styrene-co-maleic anhydride)
PVAc
Poly(vinyl acetate)
PVC
Polyvinyl chloride
PVDF
Poly(vinylidene fluoride) (sometimes expressed as PVF2)
PVF
Poly(vinyl fluoride)
PVME
Polyvinylmethylether
RIPS
Reaction-induced phase separation
SAN
Poly(styrene-co-acrylonitrile)
SARAN
P(VCl2-VC), P(VCl2-VA), or P(VCl2-AN) random copolymers of vinylidene chloride (VCl2) with vinyl chloride (VC), vinyl acetate (VA), and acrylonitrile (AN), respectively
SBS
Elastomeric styrene-butadiene-styrene triblock polymer (also TR)
SD
Spinodal decomposition
SEBS
Styrene-ethylene/butylene-styrene triblock polymer
SMA
Poly(styrene-co-maleic anhydride)
sPMMA
Syndiotactic poly(methyl methacrylate)
sPS
Syndiotactic polystyrene
TR
Thermoplastic rubber (also SBS)
UHMWPE
Ultra-high-molecular-weight polyethylene
VDF-HFA
Copolymer of vinylidene fluoride and hexafluoro acetone
VDF-TFE
Copolymer of vinylidene fluoride and tetrafluoro ethylene
VLDPE
Very low-density polyethylene
compat.
Compatibilization, compatibilized, etc.
conc.
Concentration
cryst.
Crystallization, crystalline, crystallize
cte
Constant
DSC
Differential scanning calorimetry
etc.
Et cetera
exp.
Exponent
HM
High molecular weight
LCST
Lower critical solution temperature
O. M.
Optical microscopy (also OM)
phr.
Parts per hundred
[(polymer)]
Amount/concentration of the cited polymer
SALS
Small-angle light scattering (also SALLS)
SAXS
Small-angle X-ray scattering
SEM
Scanning electron microscopy
temp.
Temperature
UCST
Upper critical solution temperature
WAXS
Wide-angle X-ray scattering
WLF
Williams, Landel, and Ferry
C 1, C 2, C 3
WLF constants
C-2
Carbon chain with 2 C-atoms; i.e., ethylene
C-3
Carbon chain with 3 C-atoms; i.e., propylene
C p
Heat capacity under constant pressure
E 1
Energy dissipated for rejection of droplets during spherulite growth
E 2
Energy to overcome the inertia of droplets during spherulite growth
E 3
Energy required to form new interfaces when droplets are engulfed
E 4
Energy dissipated for deformation of occluded particles during spherulite growth
F 12
Spreading coefficient
f z (1)
Fraction of dispersed droplets of volume VD that contain z heterogeneities of type 1
G
Isothermal spherulite growth rate
G o
Theoretical spherulite growth rate
G 1
Undisturbed spherulite growth rate of the homopolymer described by the Turnbull-Fisher equation
M (1)
Concentration of heterogeneities of type 1
MW
Molecular weight
n
Avrami exponent
N
Nucleation density
N/S
Nucleation density normalized per unit area
K
Overall crystallization rate
t 0.5
Halftime of crystallization at a fixed T c,iso
T c
Bulk crystallization temperature upon cooling from the melt
T c o
Crystallization temperature of the bulk homopolymer
T c,cold
Cold crystallization temperature
T c,hom
Homogeneous crystallization temperature
T c,i
Crystallization temperature at which heterogeneities of type i become active
T c,iso
Isothermal crystallization temperature
T c,max
Optimal isothermal crystallization temperature which yields the highest overall crystallization
T g
Glass-transition temperature
T m
Measured melting temperature of the crystalline phase
T m o
Theoretical melting temperature for crystalline lamellae of infinite thickness
T m ′
Observed melting temperature of the crystalline phase in blends
T melt
Premelting temperature
t melt
Time the polymer is kept in the melt
V D
Average volume of dispersed polymer droplets
Vol%
Volume percentage
wt%
Weight percentage
X c
Total degree of crystallinity
y p (m, c)
Lateral surface free energy between the crystal and its own melt
y pn (m)
Interfacial energy between the nucleating species and the polymer melt
y pn (c)
Interfacial energy between the nucleating species and the polymer crystal
z
Number of heterogeneities of type 1, inducing crystallization in the bulk polymer at T c o
Symbols: Greek Letters
ΔE
Activation free energy for the transport of chains through the liquid–solid interface
ΔF
Difference of interfacial energies; driving force for rejection, engulfing, and/or deformation of dispersed droplets during spherulite growth
ΔF *
Free energy for the formation of a nucleus of critical size
ΔH m
Total melting enthalpy of the crystalline polymer fraction
ΔT c,hom
Degree of undercooling required for homogeneous crystallization
ΔT c,i
Degree of undercooling required before a heterogeneity of type i can become active
Δy i
Specific interfacial energy difference between a nucleating species of type i and the polymer
Δy pn
Specific interfacial energy difference between a nucleating species and the polymer
γ PS
Interfacial free energy between the crystallizing solid and the inclusions
γ PL
Interfacial free energy between the liquid polymer melt and the inclusions
σ ο
Surface free energy of folding
σ 1,2
Interfacial free energy between two phases of a blend in the melt
σ i,1
Interfacial free energy of an impurity with respect to melt phase 1
σ i,2
Interfacial free energy of an impurity with respect to melt phase 2
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Metadaten
Titel
Crystallization, Micro- and Nano-structure, and Melting Behavior of Polymer Blends
verfasst von
G. Groeninckx
C. Harrats
M. Vanneste
V. Everaert
Copyright-Jahr
2014
Verlag
Springer Netherlands
DOI
https://doi.org/10.1007/978-94-007-6064-6_5

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