DFT design of polyguanidine – a unique two-dimensional material with high-energy density

ABSTRACT

We report herein a theoretical prediction and characterisation of a new two-dimensional (2D) material based on energetic polyguanidine. The structure represents a hexagonal type lattice of the P6/m space group. The material is dynamically and mechanically stable. Highly accurate band structure calculation with hybrid functional HSE06 reveals a tiny direct band gap being equal to 0.181 eV. We provide an additional spectral characterisation of the 2D polyguanidine substance including UV-vis, nuclear magnetic resonance and nuclear quadrupolar resonance parameters. The electron transport properties of a 26.6 Å wide polyguanidine ribbon are calculated in terms of tight-binding density functional theory approach. The predicted 2D material is also analysed by means of Quantum Theory of Atoms in Molecules and the aromatic character of the formed rings is estimated using nucleus-independent chemical shifts quantities.

KEYWORDS:

• 2D materials
• polyguanidine
• nitrogen-rich compounds
• high-energy density materials

Acknowledgments

This work was supported by the Ministry of Education and Science of Ukraine, Research Fund (Grant No. 0113U001694). We thank Professor Hans Ågren (KTH, Stockholm) for the PDC supercomputer use. The computations were performed on resources provided by the Swedish National Infrastructure for Computing (SNIC) at the Parallel Computer Center (PDC) through the project ‘Multiphysics Modeling of Molecular Materials’, SNIC 020/11-23.

Disclosure statement

No potential conflict of interest was reported by the authors.

Additional information

Funding

Ministry of Education and Science of Ukraine, Research Fund [grant number 0113U001694].