Heteroatom-bridged pillar[4]quinone: evolutionary active cathode material for lithium-ion battery using density functional theory

Quinone-based macrocyclic compounds have been proposed as promising electrode materials for rechargeable lithium-ion batteries (LIBs). To improve the electrochemical performance, in this paper, two heteroatom-bridged pillar[4]quinones (namely, oxa- and thia-pillar[4]quinones) are presented as active cathode materials for LIBs. The geometry structures, electronic structural properties, and electrochemical properties of these new species are calculated by Density Functional Theory (DFT) at the M06-2X/6-31G(d,p) level of theory. Two heteroatom-bridged pillar[4]quinones possess higher theoretical specific capacity (659 mA h g −1 and 582 mA h g −1 for oxa- and thia- pillar[4]quinones, respectively) than that of parental pillar[4]quinone (446 mA h g −1 ). The electrochemical performances of oxa- and thia-pillar[4]quinones are predicted theoretically to be superior to those of pillar[4]quinone as cathode material for LIBs. Compared with oxa-pillar[4]quinone, thia-pillar[4]quinone is predicted to be slightly more suitable as cathode electrode material. These results may provide fresh ideas and guidelines for enhancing the performance of quinones organic electrode materials for LIBs. Graphic Abstract Two heteroatom-bridged pillar[4]quinones, Oxapillar[4]quinone and Thiapillar[4]quinone, are proposed as the electrode active molecules. The lithium storage mechanisms and electrochemical properties are investigated by using DFT calculations. The results show that the heteroatom-bridged pillar[4]quinones are predicted theoretically to exihibit a better electrode material performance than the parent pillar[4]quinone.