We performed an extensive study on the most stable structures, the electronic
properties, and the thermal stability of the 2D biphenylene sheet decorated with Li atoms.
Our structural results show that the Li storage capacity of biphenylene is much higher than
that recently reported, which increases the interest in this 2D material as a promising anode
material for Li-ion batteries, although Li diffusion is not expected at room temperature.
Moreover, we found striking phenomena that had not been detected yet, such as the
formation of Li zigzag wires and metallic Li monolayers on the biphenylene sheet beyond
a certain coverage threshold. In our calculations, we use high-level density-functional
theory, quantum chemical topology analysis, and ab initio molecular dynamics simulations.
In particular, the latter methodology allows for confirming the stability of the predicted
Li-decorated biphenylene structures at room-temperature conditions.
