In this work, the consolidation of calcium carbonate (CaCO3) by polyacrylamide (PAM) of different molecular weights, charge densities, and functional groups was investigated via oscillatory rheology and unconfined compressive strength (UCS) analysis. Oscillatory rheology showed that the storage modulus G′ was approximately 10 times higher than the loss modulus G″, indicating a highly elastic CaCO3 sample upon consolidation via PAM. Both oscillatory rheology and UCS analysis exhibited similar trends, wherein the mechanical values (G′, G″, and UCS) first increased with increasing polymer dosage, until they reached a peak value (typically at 3 mgpol/gCaCO3), followed by a decrease in the mechanical values. This indicates that there is an optimum polymer dosage for the different PAM-CaCO3 colloidal systems, and that exceeding this value induces the re-stabilisation of the colloidal system, leading to a decreased degree of consolidation. Regarding the effect of the PAM molecular weight, the peak G’ and UCS values of CaCO3 consolidated by hydrolysed PAM (HPAM) of different molecular weights are very similar. This is likely due to the contour length of the HPAMs being either almost the same or longer than the average distance between two CaCO3 particles. The effect of the PAM charge density revealed that the peak G′ and UCS values decreased as the charge density of the PAM increased, while the optimum PAM dosage increased with decreasing PAM charge density. The higher likelihood of lower-charge PAM bridging between the particles contributes to higher elastic energy and mechanical strength. Finally, regarding the PAM functional group, CaCO3 consolidated by sulfonated polyacrylamide (SPAM) typically offers lower mechanical strength than that consolidated with HPAM. The bulky sulfonate side groups of SPAM interfere with the surface packing, reducing the number of polymers able to adsorb onto the surface and, eventually, reducing the degree of consolidation of CaCO3. The zeta potential of the PAM-CaCO3 samples became more negative with increasing PAM concentration due to the saturation of the particle surface. Good agreement between oscillatory rheology and UCS analysis could accelerate PAM screening for optimum CaCO3 consolidation.
