Unveiling the potential of a BCN-biphenylene monolayer as a high-performance anode material for alkali metal ion batteries: a first-principles study

Abstract

Inspired by a freshly synthesized two-dimensional biphenylene carbon network, which features a captivating combination of hexagonal, square, and octagonal rings, we explored a similar biphenylene network composed of boron, carbon, and nitrogen (bpn-BCN) using first-principles calculations. There are six possible phases of borocarbonitrides, which are isoelectronic to biphenylene carbon networks with a stoichiometric ratio of 1 : 1 : 1 for boron (B), carbon (C), and nitrogen (N) atoms. All possible isoelectronic structures of the BCN combination of biphenylene networks are found to be stable, according to first-principles calculations. However, the geometry has a relatively large number of robust C–C and B–N bonds and strong partially ionic–covalent B–C and C–N bonds inside these bpn-BCN monolayers are effectively more stable. Furthermore, we employed first-principles calculations to investigate the electrochemical properties of the most stable geometry of BCN biphenylene as a potential anode material for alkali metal (AM) ion batteries. A global search has been made to find the most favourable alkali metal ion adsorption sites. The biphenylene monolayer has octagonal, square, and hexagonal motifs with different adsorption strengths. Furthermore, the partially ionic bond of B–N (due to the electronegativity difference) also supports the alkali metal ions for adsorption. The electronic properties of the stable phase of bpn-BCN reveal its narrow bandgap semiconductor nature. The ion diffusion calculations show a low activation barrier for Li, Na, and K of 0.65 eV, 0.26 eV, and 0.23 eV, respectively, indicating a fast charge/discharge rate. Furthermore, the theoretical capacities of the BCN biphenylene monolayer for Li (1057.33 mA h g⁻¹), Na (647.27 mA h g⁻¹), and K (465.98 mA h g⁻¹) are found to be greater than those of commercial graphite. The average open-circuit voltage for AM decreases with increasing metal ion concentrations. It falls within a reasonable range of 0.34–1.89 V. Our results show that the BCN biphenylene monolayer could be a promising anode material in alkali metal ion rechargeable batteries.