Theoretical investigation of electronic, energetic, and mechanical properties of polyvinyl alcohol/cellulose composite hydrogel electrolyte

Abstract

Hydrogels are a new class of electrolytic materials employed in zinc-air batteries due to their significant on the battery's performance. However, the effectiveness of electrolytic hydrogel is affected by factors such as water content, temperature, additives, etc. Using DMol³ and molecular dynamics modeling techniques, this research aimed at investigating the electronic properties, effect of water content, and temperature on the binding energy, cohesive energy, and the mechanical properties of polyvinyl alcohol/cellulose-based composite hydrogel at the molecular level. The electronic optimized structures of the polymeric materials and parameters such as frontier molecular orbitals, band gap and electron density were analyzed. The results revealed that the binding energies of hydrogel polymer composite increased as the number of water molecules in the composite increased up to 60 % after which the binding energy decreased. In addition, the temperature increase led to a decrease in the binding energy of the composite. The cohesive energy density of the composite was highest at 40 % water content while higher temperatures decreased the cohesive energy density of the hydrogel. As the number of water molecules increased from 29 to 256, the tensile modulus increased from 0.707 × 10⁻³ to 2.821 × 10⁻³ Gpa; while the bulk modulus (K) increased in the order of K 40 > 50 > 30 > 20 > 10 respectively. These results serve as a theoretical enlightenment and a guide for experimental works in the field of energy conversion and storage devices.