Can Liao,Yanbei Hou,Longfei Han,Yulu Zhu,Huijuan Wang,Na Wu,Yuan Hu,Yongchun Kan,Lei Song
Eco-friendly carbon-based anodes are highly attractive for use as anode materials in lithium-ion batteries because of their accessibility, high conductivity, and satisfactory storage capacity. However, to date, the carbon anodes reported in literature exhibit low capacity, poor cycling stability, and cannot meet the current increasing demands for materials that possess high energy density . Herein, highly nitrogen-doped expandable carbon-based anodes are developed using the zeolitic imidazolate frameworks (ZIFs) ZIF-67 and ZIF-8 as self-sacrificial templates. Compared with pure carbon anodes, such as graphene oxide (GO) and carbon nanotubes (CNTs), the expandable N-doped with small size CNTs decorated GO (NC-GO) and CNTs (NC-CNTs) anodes developed in this work exhibit gradually increasing reversible specific capacities, as well as high capacities of 790 and 800 mA h g −1 , respectively, which can be sustained even after 500 cycles at 100 mA g −1 . Moreover, the anodes show ultralong cycling lives with extremely low capacity loss rates in each cycle of 0.0042% for NC-GO over 7000 cycles and 0.0035% for NC-CNTs over 10,000 cycles, which are superior to those in the current literature. This work details a new vision and direction for the development of high-capacity ultralong cycling life carbon-based anodes for use in next generation rechargeable energy storage systems .
Non-aqueous sodium-ion batteries (SiBs) are a viable electrochemical energy storage system for grid storage. However, the practical development of SiBs is hindered mainly by the sluggish kinetics and interfacial instability of positive-electrode active materials, such as polyanion-type iron-based sulfates, at high voltage. Here, to circumvent these issues, we proposed the multiscale interface engineering of Na 2.26 Fe 1.87 (SO 4 ) 3 , where bulk heterostructure and exposed crystal plane were tuned to improve the Na-ion storage performance. Physicochemical characterizations and theoretical calculations suggested that the heterostructure of Na 6 Fe(SO 4 ) 4 phase facilitated ionic kinetics by densifying Na-ion migration channels and lowering energy barriers. The (11-2) plane of Na 2.26 Fe 1.87 (SO 4 ) 3 promoted the adsorption of the electrolyte solution ClO 4 − anions and fluoroethylene carbonate molecules, which formed an inorganic-rich Na-ion conductive interphase at the positive electrode. When tested in combination with a presodiated FeS/carbon-based negative electrode in laboratory- scale single-layer pouch cell configuration, the Na 2.26 Fe 1.87 (SO 4 ) 3 -based positive electrode enables an initial discharge capacity of about 83.9 mAh g −1 , an average cell discharge voltage of 2.35 V and a specific capacity retention of around 97% after 40 cycles at 24 mA g −1 and 25 °C.
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