Boosting Electron Transfer with Heterointerface Effect for High-Performance Lithium-Ion Storage

Abstract Although metal silicates are considered as the promising electrode materials for lithium-ion batteries, metal silicate-based materials suffer from inadequate cycling performance and dimensional unreliability evoked by the large volume changes during cycling, which hinders their practical applications. In principle, the poor electrochemical kinetics during the redox reactions of metal silicates is originated from the instinct structure. Hence, the precise and delicate ability to construct hetero-layers to tailor intercalation reaction remains elusive. Herein, a facile strategy of designing and constructing heterostructure in a cobalt-copper silicates nano-architecture (CNT@CoCuSiOx) with synergistic interaction between cobalt silicate (Co2SiO4) with copper silicate (CuSiO3) on the surface of carbon nanotubes (CNTs). Moreover, Co2SiO4/CuSiO3 heterojunction with unbalanced charge distributions that rooted from in-situ generation on CNTs by a facile one-step hydrothermal process, can efficiently tailor the electrochemical activities of Cu3+/Cu2+ and Co3+/Co2+ redox reactions by elevating transfer of electrons and delivering the heterointerface effect. The tough and conductive nanostructure of CNTs basement facilitate the ion diffusion and improve the rate capability. The heterostructure-incorporated CNT@CoCuSiOx-(2/1) exhibits not only outstanding electrochemical capacity (545 mAh g−1 at 0.1 A g−1), superior ion/electron transmission efficiency but also robust cycling performance (516 mAh g−1 after 900 cycles at 0.5 A g−1 and an excellent capacity retention rate of 95%). Beyond energy storage, our delicate methodology in manipulating the electrochemical behavior of metal silicates opens up a critical insight into rational fabrication of next-generation anodes for lithium-ion battery.