Abstract

Bicontinuous hierarchically porous Mn2O3 single crystals (BHP-Mn2O3-SCs) with uniform parallelepiped geometry and tunable sizes have been synthesized and used as anode materials for lithium-ion batteries (LIBs). The monodispersed BHP-Mn2O3-SCs exhibit high specific surface area and three dimensional interconnected bimodal mesoporosity throughout the entire crystal. Such hierarchical interpenetrating porous framework can not only provide a large number of active sites for Li ion insertion, but also good conductivity and short diffusion length for Li ions, leading to a high lithium storage capacity and enhanced rate capability. Furthermore, owing to their specific porosity, these BHP-Mn2O3-SCs as anode materials can accommodate the volume expansion/contraction that occurs with lithium insertion/extraction during discharge/charge processes, resulting in their good cycling performance. Our synthesized BHP-Mn2O3-SCs with a size of ~700 nm display the best electrochemical performance, with a large reversible capacity (845 mA h g−1 at 100 mA g−1 after 50 cycles), high coulombic efficiency (>95%), excellent cycling stability and superior rate capability (410 mA h g−1 at 1 Ag−1). These values are among the highest reported for Mn2O3-based bulk solids and nanostructures. Also, electrochemical impedance spectroscopy study demonstrates that the BHP-Mn2O3-SCs are suitable for charge transfer at the electrode/electrolyte interface.

Highlights

  • Porous micro/nanostructures have been demonstrated as ideal candidates to overcome the major limitations in developing high-performance lithium-ion batteries (LIBs)

  • The TG profile demonstrates that the decomposition starts at ~300 °C and terminates at ~500 °C, indicating 550 °C is an appropriate annealing temperature to obtain Mn2O3

  • BHP-Mn2O3-single crystals (SCs) with uniform parallelepiped geometry have been successfully synthesized via the thermal decomposition of MnCO3 SCs

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Summary

Introduction

Porous micro/nanostructures have been demonstrated as ideal candidates to overcome the major limitations in developing high-performance LIBs. The electrochemical properties show that the BHP-Mn2O3-SCs deliver an excellent reversible capacity even at high current density and exceptional rate capability with high specific capacity Such high lithium storage capacity and rate capability are among the highest values obtained for BHP-Mn2O3-SCs. Such high lithium storage capacity and rate capability are among the highest values obtained for BHP-Mn2O3-SCs We attribute these to the bicontinuous interpenetrating framework of the Mn2O3-SCs with bimodal mesoporous structure, offering higher conductivities for charge transfer, large specific surface areas, short transport distances for the lithium-ion insertion reaction at the interface and freedom for volume change during the charge/discharge cycles

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