ABSTRACT
Recent advancements in two-dimensional (2D) allotropes of carbon materials and their usage as superior CO2 adsorbents can decrease the detrimental impact of CO2 on climate change. With the use of quantum chemical calculations, the effect of metal clusters (Agn = 1-4 and Pdn = 1-4) on the structural and electrical characteristics of 55-77 2D graphene sheet is examined in the current work with an aim towards enhancing CO2 capture capacity. The findings revealed that the binding energy (Eb) of the 55-77 sheet decoration with Pdn = 1-4 metal clusters are greater owing to chemisorption by 1.17 eV, 1.69 eV, 0.27 eV, and 1.58 eV than the decoration with Agn = 1-4 clusters. Moreover, CO2 molecules adsorb on the Pdn = 1-4 cluster decorated systems having -0.35 eV, 0.83 eV, 1.53 eV, and -0.98 eV greater adsorption energies than on the Agn = 1-4 decorated 55-77 sheet due to a stronger charge transfer. Further, the findings of an atoms in molecules (AIM) study show that the interaction between CO2 and Pdn = 1-4 decorated 55-77 sheet is partially covalent and non-covalent, confirming the greater charge transfer between the CO2 molecule and Pdn = 1-4 decorated 55-77 systems. Moreover, the CO2 adsorption on Pdn = 1-4 decorated 55-77 systems is clearly demonstrated by non-covalent interaction (NCI) analysis to be a strong electrostatic interaction at sign(λ2)ρ = -0.05 a.u, and this is further supported by an electron localization function (ELF) map. The highest CO2 adsorption capacity is obtained for 55-77/Pd1+CO2 with the value of 6.27 wt % which concludes 55-77 sheet with Pdn decoration is a more suitable structure for CO2 adsorption than the Agn decorated system.
