The objective of this research is to examine the viability of a 2D-polyaramid monolayer for sensing and delivering the anticancer drug gemcitabine. Our results indicate that the energy gap of polyaramid (2.48 eV) is reduced by 16.35% once gemcitabine anticancer drugs are adsorbed, suggesting that the 2D-polyaramid monolayer exhibits an electrical response by detection of this drug. The most energetically favorable configuration of the gemcitabine/2D-polyaramid complex exhibits adsorption energies of −1.5 eV in the gas phase and −0.75 eV in aqueous solution. To further assess the system’s behavior in biological conditions, we evaluate the solubility profiles of the drug, the polymeric surface, and their hybrid complexes in water. Upon adsorption onto the 2D-polyaramid monolayer, a slight increase in the net charge of the drug molecule has been observed, indicating charge transfer from the monolayer to gemcitabine. In the most stable complex, this charge transfer amounts to 0.06 electrons. Structural stability at ambient temperature has verified through ab initio molecular dynamics (AIMD) simulations conducted under the NVT ensemble. Additionally, we model the drug release mechanism in a mildly acidic microenvironment, representative of conditions near target cells. In conclusion, the pristine 2D-polyaramid substrate shows promise as a carrier and sensor for the gemcitabine anticancer drug.
