Fracture toughness is generally considered as the main properties of a polymer or a polymer adhesive system for measuring the material resistance to the extension of cracks. Epoxy adhesives are generally brittle in nature; however, the addition of a second dispersed phase could induce a remarkable increase of damage tolerance performance by an enhancement of the material fracture toughness. The fracture behavior of a filled epoxy resin is strongly affected by the dimensions, the shape, and the chemical nature of the considered filler. The chapter describes the different toughening mechanisms for polymer adhesives with special attention toward innovative nanofiller such as graphene nanoplatelets and hyperbranched polymer nanoparticles.

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The effects of the addition of an aromatic hyperbranched polyester (AHBP) on thermal, mechanical, and fracture toughness properties of a thermosetting resin system were investigated. AHBP filler, synthesized by using a bulk poly-condensation reaction, reveals a glassy state at room temperature. Indeed, according to differential scanning calorimetry measurements, the glass transition temperature (Tg) of AHBP is 95 °C. Three different adduct weight percentages were employed to manufacture the AHBP/epoxy samples, respectively, 0.1, 1, and 5 wt%. Dynamical Mechanical Analysis tests revealed that the addition of AHBP induces a negligible variation in terms of conservative modulus, whereas a slight Tg reduction of about 4 °C was observed at 5 wt% of filler content. Fracture toughness results showed an improvement of both critical stress intensity factor (+18%) and critical strain energy release rate (+83%) by adding 5 wt% of AHBP compared to the neat epoxy matrix. Static and dynamic compression tests covering strain rates ranging from 0.0008 to 1000 s−1 revealed a pronounced strain rate sensitivity for all AHBP/epoxy systems. The AHBP composites all showed an increase of the true peak yield compressive strength with the best improvement associated with the sample with 0.1 wt% of AHBP.

The effects of temperature and moisture on flexural and thermomechanical properties of neat and filled epoxy with both multiwall carbon nanotubes (CNT), carbon nanofibers (CNF), and their hybrid components were investigated. Two regimes of environmental aging were applied: Water absorption at 70 °C until equilibrium moisture content and thermal heating at 70 °C for the same time period. Three-point bending and dynamic mechanical tests were carried out for all samples before and after conditioning. The property prediction model (PPM) was successfully applied for the prediction of the modulus of elasticity in bending of manufactured specimens subjected to both water absorption and thermal aging. It was experimentally confirmed that, due to addition of carbon nanofillers to the epoxy resin, the sorption, flexural, and thermomechanical characteristics were slightly improved compared to the neat system. Considering experimental and theoretical results, most of the epoxy composites filled with hybrid carbon nanofiller revealed the lowest effect of temperature and moisture on material properties, along with the lowest sorption characteristics.

Synthesized silicon oxide (silica) nanoparticles were functionalized with a hyperbranched polymer (HBP) achieving a core/shell nanoparticles (CSNPs) morphology. CSNPs were characterized by Fourier Transform Infrared (FTIR) spectroscopy, Transmission Electron Microscopy (TEM), and Thermogravimetric Analysis (TGA). A core diameter of about 250 nm with a 15 nm thick shell was revealed using TEM images. An aeronautical epoxy resin was loaded with the synthesized CSNPs at different percentages and thermal properties, such as thermal stability and dynamic mechanical properties, were investigated with the use of different techniques. Although the incorporation of 2.5 wt% of CSNPs induces a ~4 °C reduction of the hosting matrix glass transition temperature, a slight increase of the storage modulus of about ~10% was also measured. The Kissinger Method was employed in order to study the thermal stability of the nanocomposites; the degradation activation energies that resulted were higher for the sample loaded with low filler content with a maximum increase of both degradation step energies of about ~77% and ~20%, respectively. Finally, fracture toughness analysis revealed that both the critical stress intensity factor (KIC) and critical strain energy release rate (GIC) increased with the CSNPs content, reporting an increase of about 32% and 74%, respectively, for the higher filler loading.

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Synthesized silica nanoparticles (SiO2) were coated with a thin polydopamine (PDA) shell by a modified one-step procedure leading to PDA coated silica nanoparticles (SiO2@PDA). Core-shell (CSNPs) characterization revealed 15 nm thickness of PDA shell surrounding the SiO2 core (~270 nm in diameter). Different weight percentages of CSNPs were employed as filler to enhance the final properties of an aeronautical epoxy resin (RTM6) commonly used as matrix to manufacture structural composites. RTM6/SiO2@PDA nanocomposites were experimentally characterized in terms of thermal stability and mechanical performances to assess the induced effects by the synthesized CSNPs on pristine matrix. Thermal stability was investigated by thermogravimetry and data were modelled by the Doyle model and Kissinger methods. An overall enhancement in thermal stability was achieved and clearly highlighted by modelling results. Dynamic Mechanical Analysis has revealed an improvement in the nanocomposite performances compared to the neat matrix, with an increase in the glassy (+9.5%) and rubbery moduli (+32%) as well as glass transition temperature (+10 °C). Fracture Toughness tests confirmed the positive effect in damage resistance compared to unloaded resin with an impressive variation in critical stress intensity factor (KIC) and critical strain energy (GIC) of about 60% and 138%, respectively, with the highest SiO2@PDA content.