Multiwalled carbon nanotubes as hard templates to yield advanced geopolymer-based self-assembled nanostructured ceramics

Novel multifunctional construction materials are needed to promote resilient infrastructure in the face of climate change and extreme weather. Nanostructured materials such as geopolymer reinforced with carbon-based nanomaterials are a promising way to reach that goal. In recent years, several studies have investigated the influence of nanomaterials on the physical properties of geopolymer composites such as compressive strength and fracture toughness. Yet, a fundamental understanding of the influence of nanomaterials on the nanoscale and micron-scale structure has been elusive so far. Our research objective is to understand how multiwalled carbon nanotubes (MWCNT) can help tailor the microstructure of geopolymers to yield architected multifunctional nanocomposites. We synthesized geopolymer nanocomposites reinforced with 50-nm thick multiwalled carbon nanotubes with mass fractions in the range of 0.1 wt%, 0.2 wt%, and 0.5 wt%. Our major finding is that MWCNTs act as hard templates that promote geopolymer formation via self-assembly. Geopolymer nanoparticle growth is observed along the walls of MWCNTs. A refinement in grain size is observed: increasing the fraction of MWCNTs by 0.5 wt% leads to a reduction in grain size by 54%. Similarly, increasing the mass fraction of MWCNTs leads to a densification of the geopolymer matrix as demonstrated by the Fourier transform infrared spectroscopy results and the statistical deconvolution analysis. Mercury intrusion porosimetry shows a nanoscale tailoring of the pore size distribution: a 26% decrease in porosity is observed as the fraction of MWCNTs is increased to 0.5 wt%. As a result of these nanoscale structural changes, a greater resistance to long-term deformation is observed for MWCNT-reinforced geopolymers, as the creep modulus increases both locally and macroscopically. At the macroscopic level, a 42% increase in the macroscopic logarithmic creep modulus is observed as the fraction of MWCNTs is increased to 0.5 wt%. These findings and the supporting methodology are important to understand how to manipulate matter below 100 nm. This research also paves the way for the design of resilient infrastructure materials with tailored microstructure and mechanical properties.