Sulfur-rich Graphdiyne-Containing Electrochemical Active Tetrathiafulvalene for Highly Efficient Lithium Storage Application.

A sulfur-rich graphdiyne (TTF-GDY) material containing electrochemically active unit of tetrathiafulvalene was successfully synthesized at the liquid/liquid interface under mild conditions. The extended two-dimensional (2D) π-conjugated framework contains large in-plane cavities to accommodate defined sulfur elements and precise sulfur content. Transmission electron microscopy (TEM), scanning electron microscopy (SEM), and atomic force microscopy (AFM) characterizations demonstrated that the TTF-GDY adopted the layered structures. X-ray photoelectron spectroscopy (XPS), Raman spectrum, selected area electron diffraction (SAED), crystal modeling, and molecular-mechanics-based calculation further confirmed the proposed framework structure and the expected chemical compositions. Considering the unique structure and sulfur-rich characteristic, we then applied this material as an electrode in lithium battery applications. Due to the unique 2D framework structure, the TTF-GDY exhibited a high specific capacity of 837.6 mAh/g, particularly having a robust long-term stability under the high current density. These results demonstrated that such a sulfur-rich TTF-GDY, as a novel electrochemical material would have great application potential in energy fields.