Coating of flexible substrates is crucial to prepare versatile, multifunctional materials. However, exploration of effective fabrication approaches is still a challenging issue, since the pathways generally proposed require time-consuming, multi-step protocols. Here, we developed a one-pot process for decorating either pearl necklace-like or fibrous fluffy-like structures of polycaprolactone (PCL) with graphene oxide (GO) skin. PCL solutions were dry jet-wet electrosprayed or electrospun into a stirred liquid collector constituted by ethanol containing GO nanoparticles. The stirred liquid collector enables the formation of 3D-structures, whose microarchitecture can be designed by controlling the rheological behaviour of PCL solutions. Two molecular weights of PCL were used (45 or 80 kDa), with ensuing different viscosity, which determines the prevalent formation of beads or fibres. The presence of GO in the coagulation bath allows the polymeric structures to be rapidly wrapped by those nanoparticles. Graphenic coating endows these materials with the intriguing peculiarities of GO: PCL/GO nanocomposites displayed increments of elastic modulus ranging from 1250% (beads) to 3300% (fibres) with respect to the neat matrices and a change from hydrophobic to amphiphilic character. A potential application of such devices in water treatment was assessed in phenol removal. The results pointed out that PCL/GO scaffolds retain the same sorption capacity of GO nanoparticles, while bringing several advantages in terms of handling, robustness, recyclability. The ease of control of the process, as well as its fastness and cost-effectiveness could open a wide range of scenarios, including sensors, energy, catalysis, biomedicine.

Platelet-like and fibrous lignocellulosic fillers were achieved from the leaves of Chamaerops humilis (CHL) and Posidonia oceanica (POL) and used as a hybrid reinforcement for a polylactic acid (PLA) matrix at three different loading levels (from 5 to 20%). The materials were fully characterized from a morphological, physicochemical, mechanical, and dynamic-thermomechanical point of view. When compared to their counterpart containing either CHL or POL only, the resulting hybrid biocomposites showed the highest mechanical properties, with strengthening and stiffening effects respectively up to 120% and 50% higher than those expected from the linear combination of the two, and higher dynamic-mechanical performance, with storage moduli in the rubbery region 10 times higher than those of composites containing solely CHL or POL. Such synergistic efficiency is likely due to the formation of a strong and extensive interphase region, promoted by the balanced effect of morphological features of the hybrid network and physicochemical characteristics of the components. These green materials could find applications as panels for furniture or in the automotive industry. Graphical Abstract

Growing environmental concerns are stimulating researchers to develop more and more efficient materials for environmental remediation. Among them, polymer-based hierarchical structures, attained by properly combining certain starting components and processing techniques, represent an emerging trend in materials science and technology. In this work, graphene oxide (GO) and/or carbon nanotubes (CNTs) were integrated at different loading levels into poly (vinyl fluoride-co-hexafluoropropylene) (PVDF-co-HFP) and then electrospun to construct mats capable of treating water that is contaminated by methylene blue (MB). The materials, fully characterized from a morphological, physicochemical, and mechanical point of view, were proved to serve as membranes for vacuum-assisted dead-end membrane processes, relying on the synergy of two mechanisms, namely, pore sieving and adsorption. In particular, the nanocomposites containing 2 wt % of GO and CNTs gave the best performance, showing high flux (800 L × m⁻² h⁻¹) and excellent rejection (99%) and flux recovery ratios (93.3%), along with antifouling properties (irreversible and reversible fouling below 6% and 25%, respectively), and reusability. These outstanding outcomes were ascribed to the particular microstructure employed, which endowed polymeric membranes with high roughness, wettability, and mechanical robustness, these capabilities being imparted by the peculiar self-assembled network of GO and CNTs.