Bio-based epoxy adhesives face significant challenges due to their relatively poor mechanical properties compared to their petroleum-based competitors, including low fracture toughness and abrupt failure. By mimicking the molecular structure of spider silk, which is one of the toughest materials in nature, 3D-printed polymer overlapping curls consisting of coiling fibers with sacrificial bonds and hidden lengths, were impregnated into a bio-based epoxy adhesive to improve its mode I fracture toughness. Such bio-inspired structures were designed specifically to toughen and improve the crack resistance of adhesive joints. These overlapping curls were embedded in the bio-based epoxy bondline with various adhesion patterning strategies, aiming to architect the fracture scenario and increase mode I energy dissipation. Double cantilever beam test results show that an extrinsic bridging is triggered by the embedded curls that promote progressive failure and delay crack growth, which improved the mean energy release rate by 133% and enhanced the mean peak energy release rate up to 313%. The proposed 3D-printed coiling fibers successfully improved the mechanical performance of the bio-based epoxy and retarded the crack growth within the bondline, opening new horizons for their use as carriers of bondlines in structural applications to control crack growth in adhesively bonded joints.

Four specimens were prepared from one continuous Carbon Fiber Reinforced Thermoplastic Polymer (CFRP) tape and nondestructively tested using 2D X-ray micrographs and 3D X-ray Computed Tomography (CT). They were each polished on one front side and imaged by optical microscopy using a Keyence VK-X1000 confocal scanning microscope. These two-dimensional micrographs provided high-resolution reference data of the polished tape surfaces. CT was performed on the same specimens with a Zeiss Xradia 520 Versa at voxel sizes of 0.8, 2.0, and 3.5 µm each. The field of view was adjusted to include the polished front side, and the rotation axis was kept constant in between scans of one specimen. This configuration enabled the CT datasets to be registered into a common coordinate system. The registered stacks were subsequently cropped to the tape volume to optimize memory usage. The 3D CT datasets were segmented using structure tensor analysis and Trainable Weka Segmentation to extract fiber, matrix and pore regions in the CFRP tapes’ microstructure. The 2D microscopy images were used as complementary benchmarks to evaluate the required spatial resolution. The overall aim was to determine whether reliable microstructural characterization demands full fiber-level resolution, or whether coarser CT scans provide sufficient information.

In this study, a 3D-printed biomimetic overlapping curl structure inspired by spider silk molecular structure, containing sacrificial bonds and hidden lengths, is studied as a toughening mechanism for a bio-based epoxy. Experimental results of the fracture phenomena of the overlapping curl-reinforced bio-based epoxy identify three toughening mechanisms triggered by the overlapping curl: (1) crack re-initiation, (2) overlapping curl bridging, and (3) epoxy ligament. First, the integrated overlapping curl creates a void within the epoxy matrix. As the crack tip reaches the end of this void, the crack re-initiates. Then, as the hidden length of overlapping curl unfolds, it leads to a bridging effect in resisting crack growth. In addition, for the smallest hidden length, an epoxy ligament is formed due to crack branching, significantly improving the energy release rate. The epoxy fracture energy release rate increased by 13 %. The overall modest improvement is attributed to the large plastic dissipation energy of the epoxy and the relatively low overlapping curl load-capacity. However, when expanding the design space numerically, it was shown that as the failure load of the overlapping curl increases, the bridging effect increases progressively. The introduction of the bio-inspired overlapping curl structure into bio-based epoxy proves the concept of a toughening strategy for developing high-performance sustainable composite materials.

Adhesive bonded composite joints with an embedded insert consisting of an interfacial hybrid thermoset–thermoplastic bondline could activate an extrinsic toughening mechanism that quadruples the mode I fracture toughness. However, the mechanisms of extrinsic toughening (anchoring, debonding, stretching, detachment), their associated energy dissipation, and the role of bondline parameters (wavelength, porosity, ductility) have not been detailed thus far. Here, we developed double cantilever beam (DCB) finite element models consisting of two rigid composite adherends and an elastoplastic bondline. We prescribed a spatially arranged interfacial/cohesive pattern to simulate the extrinsic toughening and evaluate the increase in fracture toughness. DCB tests were performed to validate the load–displacement curves, fracture toughness, and extrinsic toughening mechanisms obtained from the finite element models. The elastic–plastic energy dissipation during the crack-bridging process was also evaluated using the models. Despite the two-dimensional nature, the modeling results are in reasonable agreement with the experiments, providing an option for further developing a new heterogeneous bondline concept.

Spider silk is known for its excellent strength and fracture resistance properties due to its molecular design structure, characterized by sacrificial bonds and hidden lengths. These structures have inspired reinforcements of synthetic polymer materials to enhance toughness. In this study, we mimic these natural toughening mechanisms by designing and manufacturing 3D-printed polymeric structures incorporating overlapping curls consisting of coiling fiber with sacrificial bonds and hidden lengths. Utilizing the liquid rope coiling effect, we manufactured overlapping curls using three polymers: polylactic acid (PLA), liquid crystal polymer (LCP), and polyamide 6 (PA6). Uniaxial tensile tests were performed to characterize the mechanical properties of overlapping curl as a function of geometries, post-treatments, and material constitutive parameters. Our results show that single-sided overlapping curls can fully unfold while double-sided curls are prone to premature failure. Heat-pressure post-treatment was found to significantly increase the load-capacity of the sacrificial bonds by up to [Formula presented] due to increased contact area. However, the defects introduced in the fibre after the break of the sacrificial bonds, make the structure more susceptible to premature failure, limit the complete unfolding of the hidden length, and lead to a decrease up to [Formula presented] of the toughness. To guarantee the complete unfolding of the hidden lengths and improve the toughness, we demonstrate that selecting a polymer material with either high fracture strength (e.g., LCP, [Formula presented]) or high fracture strain (e.g., PA6, >2) is crucial, and increase toughness up to [Formula presented] and [Formula presented], respectively.

Interfaces play a critical role in modern structures, where integrating multiple materials and components is essential to achieve specific functions. Enhancing the mechanical performance of these interfaces, particularly their resistance to delamination, is essential to enable extremely lightweight designs and improve energy efficiency. Improving toughness (or increasing energy dissipation during delamination) has traditionally involved modifying materials to navigate the well-known strength-toughness trade-off. However, a more effective strategy involves promoting non-local or extrinsic energy dissipation. This approach encompasses complex degradation phenomena that extend beyond the crack tip, such as long-range bridging, crack fragmentation, and ligament formation. This work explores this innovative strategy within the arena of laminated structures, with a particular focus on fiber-reinforced polymers. This review highlights the substantial potential for improvement by presenting various strategies, from basic principles to proof-of-concept applications. This approach represents a significant design direction for integrating materials and structures, especially relevant in the emerging era of additive manufacturing. However, it also comes with new challenges in predictive modeling of such mechanisms at the structural scale, and here the latest development in this direction is highlighted. Through this perspective, greater durability and performance in advanced structural applications can be achieved.

This study uses the acoustic emission structural health monitoring method to identify fracture mechanisms in composite bonded joints when varying the substrate stacking sequence. Quasi-static mode I loading tests were performed on secondary adhesively bonded multidirectional composite substrates (0, 90, 45, −45, 60 and −60° fibre orientations). An unsupervised artificial neural network combined with the visual fracture evaluation of the specimens and the Morlet continuous wavelet transform was used to cluster and give the acoustic emission signals a physical meaning. Different fracture mechanisms could be identified within the adhesive layer (i.e., cohesive failure) and in the composite substrates, including non-visible damage mechanisms (matrix micro-cracking, fibre/matrix debonding, fibre pull-out and fibre breakage). Using the Morlet continuous wavelet transform, it was possible to recognise that the highest peak frequency does not always represent the most relevant signature of the fracture mechanism. Moreover, multiple peak frequencies can be associated with multiple fracture mechanisms, such as the fibre pull-out that occurs in the combination of matrix cracking and fibre breakage. Furthermore, no differences were observed in mode I loading conditions between the acoustic emission signatures from the cohesive failure in the adhesive layer and the matrix cracking within the composite substrate. The findings of this study present a great opportunity to gain more insight into the fracture behaviour of polymer materials and fibre-reinforced polymer materials and to improve the quality of adhesively bonded joints.

Aiming to increase damage tolerance of adhesively bonded joints, this work explores the influence of CFRP layup of the adherends on the crack onset and crack propagation of composite bonded joints under mode I loading. Quasi-static Double Cantilever Beam tests were performed using four different CFRP layups bonded with two adhesives. Parallel to the experimental program, finite element analyses were performed to aid in understanding and identifying the various damage mechanisms in each specimen type. The results show that the CFRP layup and adhesive fracture toughness significantly influence the joint fracture phenomena at crack onset and further crack propagation. An enhancement of the joint's mode I fracture toughness values at crack onset was observed in the specimens where a crack competition between the propagation within the bondline and the composite's layers was triggered. During crack propagation, the fracture toughness of the joint increases at crack deflections between the different plies of the CFRP layup until reaching the 0° ply, where sudden delamination occurs. It has been shown that CFRP layup tailoring is a promising toughening method that, when carefully designed, has the potential to increase the maximum effective fracture toughness up to 100% when compared to pure cohesive failure.