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In last years, the requirements for materials and devices have increased exponentially. Greater competitiveness; cost and weight reduction for structural materials; greater power density for electronic devices; higher design versatility; materials customizing and tailoring; lower energy consumption during the manufacturing, transport, and use; among others, are some of the most common market demands. A higher operational efficiency together with long service life claimed. Particularly, high thermally conductive in epoxy resins is an important requirement for numerous applications, including energy and electrical and electronic industry. Over time, these materials have evolved from traditional single-function to multifunctional materials to satisfy the increasing demands of applications. Considering the complex application contexts, this review aims to provide insight into the present state of the art and future challenges of thermally conductive epoxy composites with various functionalities. Firstly, the basic theory of thermally conductive epoxy composites is summarized. Secondly, the review provides a comprehensive description of five types of multifunctional thermally conductive epoxy composites, including their fabrication methods and specific behavior. Furthermore, the key technical problems are proposed, and the major challenges to developing multifunctional thermally conductive epoxy composites are presented. Ultimately, the purpose of this review is to provide guidance and inspiration for the development of multifunctional thermally conductive epoxy composites to meet the increasing demands of the next generation of materials.

Self-healing materials have attracted great interest in recent years. Particularly, the use of thermoset/thermoplastics blends has emerged as a good option with relatively low activation temperatures and potential infinite healing cycles. Nevertheless, a methodical study of healing conditions and evaluation is still required for further industrial development. The effect of activation temperature and crack morphology in polycaprolactone (PCL)/epoxy blends are explored. For this purpose, PCL content was varied (5, 10, and 15 wt %) with contents lower than critical composition. Therefore, the morphology of all studied blends is the epoxy matrix with a separated PCL phase. In this sense, an increase in PCL content leads to a reduction in the Tg, due to the partial PCL miscibility, and the presence of larger PCL domains. It was observed that a higher temperature (150 °C) and PCL content led to a more efficient self-healing process because of both the lower viscosity of the melted PCL at higher temperatures and the presence of larger PCL reservoirs when increasing the PCL content. Crack morphology influence was studied by inducing cracks with different tools: a custom crack machine with a cutting blade, a scalpel, and a pin. The results show that the recovery was better when the cracks were smaller and shallower, that is, with the pin. In addition, the healing efficiency by means of both parameters, crack volume and depth change, showed more similar results in slimmer cracks, due to a lower crack width-to-depth ratio.

A new manufacturing method of thermosetting resins reinforced with dense particles is developed in the present work. A rotary mold is used, avoiding the natural sedimentation of particles through applying centrifuge forces. A deep study of the sedimentation phenomenon is carried out in order to evaluate the main experimental parameters which influence the manufacturing of composite. The used reinforcement is zinc oxide (ZnO) obtained by a new recycling method from spent alkaline batteries. In order to compare the benefits, commercial ZnO nanoparticles are also analyzed. Recycled ZnO particles enhance the interaction of the epoxy matrix due to their inner moisture, allowing the manufacture of composites with relatively high ceramic content. Moreover, an increment in the glass transition temperature of the epoxy matrix and in the mechanical properties, such as its stiffness and hardness, is achieved.

The influence of the average surface area of different graphene nanoplatelets (GNP) on the thermo-electrical behaviour, associated with Joule heating, and the attenuation of electromagnetic signals of epoxy composites has been studied, analysing the effect of the morphology obtained as a function of the dispersion time by ultrasonication and the GNP content added. Gravity moulding was used as the first stage in the scaling-up, oriented to the industrial manufacture of multilayer coatings, observing a preferential self-orientation of nanoparticles and, in several conditions, a self-stratification too. The increase of sonication time during the GNP dispersion provides a decrease in the electrical conductivity, due to the GNP fragmentation. Instead, the thermal conductivity is enhanced due to the higher homogeneous distribution of GNPs into the epoxy matrix. Finally, the lower surface area of GNPs reduces the thermal and electrical conductivity due to a greater separation between nanosheets. Regarding the study of the attenuation of electromagnetic waves, it has been discovered that in the frequency range from 100 Hz to 20 MHz, this attenuation is independent of the direction of analysis, the type of graphene, the sonication time, and the state of dispersion of the nano-reinforcement in the matrix. Furthermore, it has also been observed that the conservation of the constant shielding values for the three types of GNPs are in a range of average frequencies between 0.3 and 3 MHz.