Elsevier

Polymer

Volume 47, Issue 4, 8 February 2006, Pages 1357-1363
Polymer

Effect of crystallinity and loading-rate on mode I fracture behavior of poly(lactic acid)

https://doi.org/10.1016/j.polymer.2005.12.046Get rights and content

Abstract

The aim of this study is to characterize the fracture behavior of biodegradable poly(lactic acid) (PLA). Especially, the effects of crystallinity and loading-rate on the fracture behavior are emphasized. Annealing was performed to control the crystallinity of the PLA samples prepared, and then their fracture toughness values were measured under quasi-static and impact loading conditions. The results showed that the quasi-static fracture toughness of PLA decreases with increase of crystallinity; on the other hand, the impact fracture toughness tends to increase with crystallinity. The crack growth behaviors of the PLA specimens having different crystallinity were also observed by polarizing and scanning electron microscopies. The microscopic results exhibited that under quasi-static loading, disappearance of multiple crazes in the crack-tip region results in the decrease of the fracture toughness with crystallinity. On the contrary, under impact loading, the increase of the fracture toughness with crystallinity is considered to be related to the increase of fibril formation.

Introduction

Poly(lactic acid) (PLA), a biodegradable polymer, has widely been used in industrial applications such as interior parts of automobiles, exterior parts of electric devices and food packages. Recently, PLA is also considered to be used as a biomaterial mainly due to its bioabsorbability and biocompatibility. For example, it has been used for bone fixation devices in orthopedic and oral surgeries. Since bioabsorbability is one of the key factors for PLA medical devices, some of the studies have mainly focused on the degradation behavior in vivo and in vitro [1], [2], [3], [4], [5]. Some fundamental studies were also performed to characterize the crystallization behavior and mechanical properties of thin PLA films [6], [7], [8], [9]. Although such PLA implants are in bulk forms such as plate, rod and screw, a few studies have been performed to characterize the mechanical behavior of PLA solids [10], [11]. In addition, it is reported that fracture of PLA implants sometimes occurs in medical application, while the fracture behavior of PLA has not sufficiently been understood yet.

The aim of this study is to characterize the effects of crystallization and loading-rate on the mode I fracture toughness and mechanism of PLA. Annealing was performed to control the microstructure of the PLA samples. Microstructures were then observed using a polarizing microscope (POM). Thermal and dynamic mechanical properties were measured by a differential scanning calorimetry (DSC) and a dynamic mechanical analyser (DMA), respectively. Mode I fracture tests were performed to measure the critical strain energy release rate as a mode I fracture toughness under static and impact loading-rates. Crack growth behaviors and fracture surfaces were also observed using POM and a scanning electron microscope (SEM) to characterize the fracture mechanisms, and the macroscopic fracture toughness values were then correlated with the microscopic mechanisms.

Section snippets

Material and specimen

PLA pellets (Lacty#9030) were supplied by Shimadzu Co., Ltd as test sample. The content of L-form and the weight average molecular weight are 95% and 140,000 g mol−1, respectively. Thermal properties of the pellets such as the glass transition, the melting and the crystallization temperature are 64, 167 and 123 °C, respectively. Plates of 5 mm thick were fabricated using a hot press installed with a water cooling system. Those Pellets were heated and melted at 180 °C, pressed for 30 min at 30 MPa and

Crystallinity and spherulite size

Effects of annealing conditions, temperature and time, on the crystallinity, Xc, evaluated using Eq. (1) are shown in Fig. 2. The lowest value of Xc is about 2.7% for the quenched sample, and Xc of the annealed samples increases with increase of annealing time and temperature. The highest Xc is about 56% for the 100 °C–24 h sample.

POM microphotographs of the microstructures are shown in Fig. 3. It is clearly observed that the density and size of spherulites increase with increase of annealing

Conclusions

PLA samples were annealed under several conditions to obtain different microstructures with varying spherulite size and density. Dynamic mechanical analysis was then performed to assess the effect of crystallization on dynamic viscoelastic properties. Mode I fracture testing of the PLA specimens was carried out to measure the critical strain energy release rate GIC as the mode I fracture toughness. Polarizing and scanning electron microscopies were also conducted to characterize the fracture

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