Nano electrochemical reactors of Fe2O3 nanoparticles embedded in shells of nitrogen-doped hollow carbon spheres as high-performance anodes for lithium-ion batteries

Abstract

Iron oxides are extensively investigated as anode materials for lithium-ion batteries (LIBs) because of their large specific capacities. However, they undergo huge volume changes during cycling that result in anode pulverization and loss of electrical connectivity. As a result, the capacity retention of the iron oxide anodes is poor and should be improved for commercial applications. Herein, we report the preparation of ultrasmall Fe₂O₃ nanoparticles embedded in nitrogen-doped hollow carbon sphere shells (Fe₂O₃@N-C) by the direct pyrolysis of Fe-based zeolitic imidazolate frameworks (Fe-ZIF) at 620 °C in air. As an anode material for LIBs, the capacity retained was 1573 mA h g⁻¹ after 50 cycles at a current density of 0.1 C (1 C = 1000 mA g⁻¹). Even undergoing the high-rate capability test twice, it can still deliver a remarkably reversible and stable capacity of 1142 mA h g⁻¹ after 100 cycles at a current density of 1 C. The excellent electrochemical performance is attributed to the unique structure of ultrasmall Fe₂O₃ nanoparticles uniformly distributed in the shell of nitrogen-doped carbon spheres, which simultaneously solve the major problems of pulverization, facilitate rapid electrochemical kinetics, and effectively avoid the aggregation of Fe₂O₃ nanoparticles during de/lithiation. The novel method developed in this work for the synthesis of functional hybrid materials can be extended to the preparation of various MOFs-derived functional nanocomposites owing to the versatility of links and metal centers in MOFs.