Insights into Formation and Li-Storage Mechanisms of Hierarchical Accordion-Shape Orthorhombic CuNb₂O₆ toward Lithium-Ion Capacitors as an Anode-Active Material

Abstract

The orthorhombic CuNb₂O₆ (O-CNO) is established as a competitive anode for lithium-ion capacitors (LICs) owing to its attractive compositional/structural merits. However, the high-temperature synthesis (>900 ℃) and controversial charge-storage mechanism always limit its applications. Herein, we develop a low-temperature strategy to fabricate a nano-blocks-constructed hierarchical accordional O-CNO framework by employing multilayered Nb₂CT_x as the niobium source. The intrinsic stress-induced formation/transformation mechanism of the monoclinic CuNb₂O₆ to O-CNO is tentatively put forward. Furthermore, the integrated phase conversion and solid solution lithium-storage mechanism is reasonably unveiled with comprehensive in(ex) situ characterizations. Thanks to its unique structural merits and lithium-storage process, the resulted O-CNO anode is endowed with a large capacity of 150.3 mAh g^-1 at 2.0 A g^-1, along with long-duration cycling behaviors. Furthermore, the constructed O-CNO-based LICs exhibit a high energy (138.9 Wh kg^-1) and power (4.0 kW kg^-1) densities with a modest cycling stability (15.8% capacity degradation after 3000 consecutive cycles). More meaningfully, the in-depth insights into the formation and charge-storage process here can promote the extensive development of binary metal Nb-based oxides for advanced LICs.

Keywords

high-rate anodes / lithium-ion capacitors / lithium-storage mechanisms / orthorhombic CuNb ₂O ₆ / phase transform

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