Computational Investigation on the Electronic Structure and Functionalities of a Thiophene-Based Covalent Triazine Framework

Using the state-of-the-art theoretical method, we have investigated the electronic and optical properties of a thiophene-based covalent triazine framework (TBCTF). We have found that TBCTF is a direct band gap semiconductor. Our calculations reveal that constitutional isomerism is a tool for band gap tuning. The variation of band gap can be achieved by the bilayer TBCTF formation and further can be tuned by the z-axial strain. We have designed a new two-dimensional van der Waals heterostructure g-ZnO/TBCTF, which shows type-II band alignment, ensuring effective separation of photogenerated electron–hole pairs. This composite system also exhibits enhanced absorption in the visible range compared to that of individual g-ZnO and TBCTF monolayers. Therefore, this composite system may find potential application in photovoltaic devices. We have also investigated the hydrogen adsorption ability of TBCTF through Li atom doping. Our results indicate that the calculated hydrogen adsorption energies lie in the range, which is suitable for reversible hydrogen storage under ambient conditions. Therefore, the lithium-doped TBCTF may be a potential candidate for the hydrogen storage material.