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Due to global environmental concerns related to climate change, the need to improve the service life of structures and infrastructures is imminently urgent. Structural elements typically suffer service life reductions, leading to poor environmental sustainability and high maintenance costs. Graphene oxide nanosheets (GONSs) effectively dispersed in a cement matrix can promote hydration, refine the microstructure and improve interfacial bonding, leading to enhanced building materials’ performance, including mechanical strength and transport properties. Cement-based nanocomposites engineered with GONSs were obtained using two commercial nanofillers, a GO water suspension and a free-flowing GO nanopowder, characterized by fully comparable morphology, size and aspect ratio and different oxidation degrees (i.e., oxygen-to-carbon molar ratio), 0.55 and 0.45, respectively. The dosage of the 2D-nanofiller ranged between 0.01% and 0.2% by weight of cement. The electrical and thermal properties were assessed through electrochemical impedance spectroscopy (EIS) and a heat flow meter, respectively. The results were discussed and linked to micrometric porosity investigated by micro-computed tomography (μ-CT) and transport properties as determined by initial surface absorption test (ISAT), boil-water saturation method (BWS) and chloride ion penetration test. Extra-low dosage mortars, especially those loaded with a lower oxidation degree (i.e., 0.45GO), showed decreased permeability and improved barrier to chloride ion transport combined with enhanced thermal and electrical conductivity with respect to that of the control samples.

The impact of extra-low dosage (0.01% by weight of cement) Graphene Oxide (GO) on the properties of fresh and hardened nanocomposites was assessed. The use of a minimum amount of 2-D nanofiller would minimize costs and sustainability issues, therefore encouraging the market uptake of nanoengineered cement-based materials. GO was characterized by X-ray Photoelectron Spectroscopy (XPS), Fourier-transform infrared spectroscopy (FTIR), Atomic Force Microscopy (AFM), X-ray Diffraction (XRD), and Raman spectroscopy. GO consisted of stacked sheets up to 600 nm × 800 nm wide and 2 nm thick, oxygen content 31 at%. The impact of GO on the fresh admixtures was evaluated by rheology, flowability, and workability measurements. GO-modified samples were characterized by density measurements, Scanning Electron Microscopy (SEM) analysis, and compression and bending tests. Permeability was investigated using the boiling-water saturation technique, salt ponding test, and Initial Surface Absorption Test (ISAT). At 28 days, GO-nanocomposite exhibited increased density (+14%), improved compressive and flexural strength (+29% and +13%, respectively), and decreased permeability compared to the control sample. The strengthening effect dominated over the adverse effects associated with the worsening of the fresh properties; reduced permeability was mainly attributed to the refining of the pore network induced by the presence of GO.