Composition and Molecule Weight Dependences of Thermal Transition Temperatures o f Dihydroxy-Telechelic Poly(LLA-co-GA) and Poly(CL-co-GA) Crystalline Polymers
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Research Bulletin|更新时间:2021-03-19
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Composition and Molecule Weight Dependences of Thermal Transition Temperatures o f Dihydroxy-Telechelic Poly(LLA-co-GA) and Poly(CL-co-GA) Crystalline Polymers
JI Bin, WU Linbo. Composition and Molecule Weight Dependences of Thermal Transition Temperatures o f Dihydroxy-Telechelic Poly(LLA-co-GA) and Poly(CL-co-GA) Crystalline Polymers. [J]. Acta Polymerica Sinica (3):297-302(2008)
DOI:
JI Bin, WU Linbo. Composition and Molecule Weight Dependences of Thermal Transition Temperatures o f Dihydroxy-Telechelic Poly(LLA-co-GA) and Poly(CL-co-GA) Crystalline Polymers. [J]. Acta Polymerica Sinica (3):297-302(2008) DOI: 10.3724/SP.J.1105.2008.00297.
Composition and Molecule Weight Dependences of Thermal Transition Temperatures o f Dihydroxy-Telechelic Poly(LLA-co-GA) and Poly(CL-co-GA) Crystalline Polymers
Hydroxy-telechelic aliphatic (co)polyesters are important building blocks of biodegradable multiblock copolymers which can be used as biodegradable elastomers and biodegradable shape memory polymers (BSMPs).For BSMPs
the transition or switch temperature at which the shape memory effect takes place is determined by the thermal trasition temperature of the reversible phase or soft segments
and the shape memory properties and mechanical properties are maily affected by the condensed state of the fixed phase or hard segments.Therefore
the thermal transition temperatures of hydroxy-telechelic aliphatic (co)polyesters are critical parameters for successful design of BSMPs.This article aims to report the relationship among the thermal transition temperature of two important hydroxy-telechelic aliphatic copolyesters
poly(L-lactide-co-glycolide) (PLLGA) and poly(ε-caprolactone-co-glycolide) (PCG)
and their molecular weight and copolymer composition. Hydroxy-telechelic PLLGA and PCG are synthesized via ringopening copolymerization of L-lactide and glycolide (LLA/GA) and ε-caprolactone and glycolide (CL/GA) using 1
4-butanediol as initiator and stannous octoate as catalyst at 140℃.After dissolving in chloroform
precipitated from methanol and drying under vacuum at 75℃ for 48 h
purified PLLGA and PCG were obtained and characterized by FTIR
1H-NMR
GPC and DSC. The polymerization took place in a living/controlled manner
and the molecular weight was adjusted by the monomer/initiator ratio in the range of 2000~14000.The polydispersity index ranged from 1.1 to 1.3.The GA content in the copolymers is of 0~0.22 for PLLGA and 0~0.32 for PCG and can be adjusted by the GA content in monomer feed (GA
0~0.2).The contents of GA in copolymers are higher than GA because of higher reactivity ratio of GA than LLA and CL.For convenience,GA was used to denote the copolymer composition.The FTIR and 1H-NMR spectra indicate that the copolymers are hydroxy-telechelic. The DSC results indicate that the copolymers with above mentioned copolymer composition and molecular weight are all semicrystalline polymers.The melt temperatures (Tm) of both PLLGA and PCG were determined from the second scan.The Tm ranged from 37℃ to 58℃ for PCG and from 80℃ to 162℃ for PLLA.They increased with increasing the molecular weight but decreased with increasing the copolymer composition.The glass transition temperature (Tg) of PLLGA was obtained from the second scan and ranged from 35℃ to 54℃.It also increased with increasing the molecular weight but decreased with increasing the copolymer composition.By ploting Tg and Tms with the reciprocal of number average molecular weight (Mn)
linear relationships
Tg=Tg(∞)-K/Mn and Tm=Tm(∞)-K′/Mn
are observed.For Tm
the interceptions Tm(∞) are linearly decreased with increasing GA
but the slope K′ is independent of GA.Therefore
experiential linear equations Tm=Tm(H)-AGA-K′/Mn have been established to describe their relationship
in which Tm(H) is the melt temperature of PLLA and PCL homopolymers.For PLLGA
the values of Tm(H)
A and K′ are 166.9
129.5 and 1.48×105
respectively.For PCG
they are 60.4
82.0 and 2.92×104
respectively.From these results
one can design and synthesize hydroxytelechelic PLLGA and PCG copolymers and corresponding shape memory multiblock copolymers with desired transition temperatures.