Two-dimensional polymers made of carbonyl-bridged heterotriangulenes are promising anode materials for Li-ion batteries

Abstract

The development of effective electrode materials is essential to realizing high- performance lithium ion batteries (LIBs), which play an important role in powering modern society. By means of first-principles calculations, we have herein explored the potential of two-dimensional (2D) polymers made of carbonyl-bridged triphenylamine (CTPA) and carbonyl-bridged triphenylborane (CTPB) as electrode materials for LIBs. Our investigations demonstrate that the carbonyl groups of 2D CTPB and CTPA are rather active to accommodate Li. Both 2D CTPA and CTPB show the transition from semiconductor to metal after combining with Li. The migration of Li through the pore space of 2D CTPB and CTPA is facilitated with the diffusion barrier of 0.76 and 0.79 eV, respectively. 2D CTPB exhibits a high theoretical capacity of 760.86 mAh g-1 because it can accommodate Li at both the carbonyl sites and the surface sites of the skeleton, which is ascribed to the promotion of the electron-deficient B center. As a comparison, 2D CTPA can only combine with Li at the carbonyl sites and shows a capacity of 251.09 mAh g-1. With fast Li-diffusion ability, high capacity and low average operating voltage, 2D CTPA and CTPB are predicted to be promising non-metal anode materials for LIBs.

Storage of Na in 2D SnS for Na ion batteries: a DFT prediction

“…The determined diffusion barrier is much lower than earlier DFT results, such as for Na x MoN 2 (0.56 eV), Na x B 3 C (0.23 eV), Na x MoC 2 (0.23 eV), 2D carbonylbridged triphenylamine (0.76 eV) and Na x CP 3 (0.356 eV). [62][63][64][65] A comparison of the diffusion barrier, voltage, and storage capacity with other 2D materials is given in Table 2.…”

Computational insights into the rational design of organic electrode materials for metal ion batteries

“…67 Thus, hybrid functional for example HSE06 and PBE0 are suggested to well describe the electronic structure of organic semiconductors, but is certainly expensive to be used. Fortunately, PBE can predict identical trend (e.g., band structure variation caused by redox reaction with metal ions) with that of the high-accuracy hybrid functional, 68 thus is widely used for qualitative calculations.…”

On-Surface Two-Dimensional Polymerization: Advances, Challenges, and Prospects

“…1−3 Different from 2D supramolecular assembled structures sustained by noncovalent bonds, 2DPs exhibit good thermal stability and exotic physicochemical properties. 4−6 These properties make 2DPs promising materials for a wide range of applications in the fields of catalysis, 7 chemical sensing, 8,9 proton and ion conduction, 10,11 molecular separations, 12,13 and organic electronic devices. 14,15 The construction of high-quality 2DPs with specific structures and properties is one of the most important subjects in 2DPs research.…”

“…Two-dimensional polymers (2DPs) are molecularly thin networks entirely linked through covalent bonds within a plane. − Different from 2D supramolecular assembled structures sustained by noncovalent bonds, 2DPs exhibit good thermal stability and exotic physicochemical properties. − These properties make 2DPs promising materials for a wide range of applications in the fields of catalysis, chemical sensing, , proton and ion conduction, , molecular separations, , and organic electronic devices. , …”