Li Decorated Graphdiyne Nanosheets: A Theoretical Study for an Electrode Material for Nonaqueous Lithium Batteries

In this work, Density Functional Theory (DFT) is used to study pristine and defective GDY. We investigate the effect of Li atom adsorption on the electronic and structural properties of this 2D material. In both cases, the Li atom is located at the corner of the triangular‐like pore (H1), but with a slight shift for the defective system. In the perfect system, the Li−C bond distances range from 2.289 Å to 2.461 Å, while in the defective case, they range from 2.237 Å to 3.184 Å. In the perfect case, the GDY−Li system becomes metallic and the Li 2 s states are stabilized. Charge transfer to the surfaces occurs near the vicinity of the Li atom. The C vacancy generates new C=C bonds similar to double bonds, enhancing the interaction with Li through strong conjugation. After Li adsorption, the sum of bond order for all the C atoms increases in both structures, from 0.4 % to 6 %. The Li storage capacity without significant restructuring is six Li atoms. When the atom concentration increases, the OCV values for Li decrease from 0.93 V to 0.23 V. For defective GDY, the specific capacity is 788 mAhg−1, which is slightly higher than for pristine case. We conducted Density Functional Theory simulations for pristine and defective GDY to study the Li atoms adsorption effect on the electronic and structural properties of this 2D material. We modeled the structures and examined their stability. The electronic properties and the possible adsorption sites are studied. The OCV and the specific capacities for an increased atom concentration are calculated.