Direct observation of microstructural fracture dynamics in carbon fiber reinforced plastics via in situ transmission electron microscopy

https://doi.org/10.1016/j.compscitech.2020.108264Get rights and content

Abstract

The tensile deformation process of carbon fiber reinforced plastics (CFRPs) was in situ observed by high-resolution transmission electron microscopy (TEM). CFRPs were prepared with sizing and unsizing treatment on the fiber surfaces. The microstructural evolution of crack propagation along fiber/resin interfaces and inside resin matrices was examined. Fine resin fragments remained on the fiber surfaces after fracture. From the differences in the shape of the residual resin fragments between the two types of CFRPs, the influence of the sizing treatment on fracture was quantitatively evaluated. We demonstrated a new method on the basis of in situ TEM to evaluate the microstructural fracture dynamics and the influence of the sizing treatment on fracture.

Introduction

Remarkable mechanical properties of carbon fiber reinforced plastics (CFRPs) have been demonstrated by various strength and fracture tests to obtain relating various physical quantities, such as specific strength, specific stiffness, and fracture length [[1], [2], [3], [4], [5], [6], [7], [8]]. The fracture of CFRPs, which represents the reliability of CFRPs as structural materials, has been investigated using various methods, and the obtained results have been utilized in their material designs [5,[9], [10], [11], [12], [13], [14], [15], [16], [17], [18], [19]]. The examples of the methods are X-ray computer tomography [[20], [21], [22]], the digital image correlation [23], and scanning electron microscopy [16]. In these studies, observations were performed before and after fracture with spatial resolutions on the micrometer order of magnitude; the fracture dynamics was not directly observed. As a result, the fracture processes and mechanisms have been speculated on the basis of the observed results before and after fracture. One of the most effective methods to evaluate fracture in CFRPs is to observe in situ the localized microstructural dynamics in crack generation and propagation, although the method is a state-of-the-art technology. In situ transmission electron microscopy (TEM) allows us to observe such fracture dynamics, as demonstrated for that in isolated carbon fibers [24]. In particular, the atomic resolution of TEM provides a clue to the elucidation of the atomistic fracture processes in CFRPs [25]. Since the fracture and the other mechanical properties of CFRPs are affected by the adhesive strength of fiber/resin interfaces, the fiber surfaces are coated by sizing agents [1,15,16,[26], [27], [28], [29], [30], [31], [32], [33], [34], [35], [36], [37], [38], [39], [40], [41], [42], [43], [44], [45], [46]]. Thus, it is important to clarify the relationship between fracture features and the variations in the interface structures by sizing treatments. In this study, the fracture of CFRPs during off-axis tensile deformation tests was directly observed by in situ TEM. This observation resulted in the quantitative analyses of the influence of a sizing treatment on fracture.

Section snippets

Materials and sample preparation for TEM

The original materials of CFRPs used in this study were provided by NIPPON STEEL Chemical & Material Co., Ltd. The CFRPs were prepared along with following processes. A mixed solution of bisphenol A (BPA) type epoxy and cyclohexylamine was used as the resin matrix. The carbon fibers produced by the combustion of polyacrylonitrile fibers (TORAY T700SC-12000-50C), in which graphitic layered structures align along the fiber direction, were used for reinforcement. Two types of CFRPs were prepared:

Unsized CFRPs

  • (1)

    Crack propagation along the fiber/resin interfaces

Fig. 2 shows a TEM image of an unsized CFRP before a tensile test. Parts of the fiber/resin interfaces were sufficiently thinned and could be successfully observed by TEM. Fig. 3 shows a time-sequence series of the TEM images of the region indicated by the broken-line red frame in Fig. 2 during the tensile test (see Movie 1 in Supplementary materials). As shown in Fig. 3(a–c), a crack propagated along a fiber/resin interface by application of a

The crack propagation paths

In both unsized and sized CFRPs, the resin matrix was exfoliated from the fibers during tensile deformation, and the resin fragments remained discretely on fiber surfaces. The external shape of the residual resin fragments corresponds to the trajectory of the crack propagation path inside the resin matrix. Based on the observation of the change in the crack propagation path (Fig. 7), the propagation processes are explained as shown in Fig. 14. A crack propagates at a fiber/resin interface when

Conclusions

The microscopic fracture process in CFRPs, i.e., the crack propagation and relating structural variation, was observed in situ by TEM. The crack propagated alternatively along the fiber/resin interfaces and inside the resin matrix, regardless of the sizing treatment. The sizing treatment leads to the increase in the average size of the residual resin fragments and to the decrease in the coverage factor on the fiber surfaces after tensile fracture.

The results of this study revealed

CRediT authorship contribution statement

Tatsuhiro Ishikawa: Investigation, Formal analysis, Visualization, Writing - original draft. Manabu Tezura: Investigation, Writing - review & editing. Tokushi Kizuka: Conceptualization, Methodology, Investigation, Visualization, Writing - original draft, Supervision, Project administration, Funding acquisition.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

We thank NIPPON STEEL Chemical & Material Co., Ltd. for providing CFRP samples and their information. The authors acknowledge the members within their laboratory for cooperation with a part of the experiment, especially, TEM observation. This study was partly supported by Cross-Ministerial Strategic Innovation Promotion Program (Unit D66, Innovative Measurement and Analysis for Structural Materials).

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