Regulating Lithium Plating and Stripping by Using Vertically Aligned Graphene/CNT Channels Decorated with ZnO Particles

Graphical A Li host material that features vertically aligned channels composed of graphene, carbon nanotubes (CNTs), and decorated ZnO particles (designated ZnO@G-CNT-C) has been prepared by using an ice-template method through oriented freezing. The Li host material not only suppresses the formation of Li dendrites but also reduces the overpotential of Li nucleation. The usability of ZnO@G-CNT-C as Li host was confirmed in full cells with a LiFePO 4 cathode. Lithium (Li) metal is regarded as the ultimate anode material for use in Li batteries due to its high theoretical capacity (3860 mA h g −1 ). However, the Li dendrites that are generated during iterative Li plating/stripping cycles cause poor cycling stability and even present safety risks, and thus severely handicap the commercial utility of Li metal anodes. Herein, we describe a graphene and carbon nanotube (CNT)-based Li host material that features vertically aligned channels with attached ZnO particles (designated ZnO@G-CNT-C) and show that the material effectively regulates Li plating and stripping. ZnO@G-CNT-C is prepared from an aqueous suspension of Zn(OAc) 2 , CNTs, and graphene oxide by using ice to template channel growth. ZnO@G-CNT-C was found to be mechanically robust and capable of guiding Li deposition on the inner walls of the channels without the formation of Li dendrites. When used as an electrode, the material exhibits relatively low polarization for Li plating, fast Li-ion diffusion, and high Coulombic efficiency, even over hundreds of Li plating/stripping cycles. Moreover, full cells prepared with ZnO@G-CNT-C as Li host and LiFePO 4 as cathode exhibit outstanding performance in terms of specific capacity (155.9 mA h g −1 at 0.5 C), rate performance (91.8 mA h g −1 at 4 C), cycling stability (109.4 mA h g −1 at 0.5 C after 800 cycles). The methodology described can be readily adapted to enable the use of carbon-based electrodes with well-defined channels in a wide range of contemporary applications that pertain to energy storage and delivery.