eScience (Dec 2023)
Ultra-thick, dense dual-encapsulated Sb anode architecture with conductively elastic networks promises potassium-ion batteries with high areal and volumetric capacities
Abstract
Ultra-thick, dense alloy-type anodes are promising for achieving large areal and volumetric performance in potassium-ion batteries (PIBs), but severe volume expansion as well as sluggish ion and electron diffusion kinetics heavily impede their widespread application. Herein, we design highly dense (3.1 g cm−3) Ti3C2Tx MXene and graphene dual-encapsulated nano-Sb monolith architectures (HD-Sb@Ti3C2Tx-G) with high-conductivity elastic networks (1560 S m−1) and compact dually encapsulated structures, which exhibit a large volumetric capacity of 1780.2 mAh cm−3 (gravimetric capacity: 565.0 mAh g−1), a long-term stable lifespan of 500 cycles with 82% retention, and a large areal capacity of 8.6 mAh cm−2 (loading: 31 mg cm−2) in PIBs. Using ex-situ SEM, in-situ TEM, kinetic investigations, and theoretical calculations, we reveal that the excellent areal and volumetric performance mechanism stems from the three dimensional (3D) high-conductivity elastic networks and the dual-encapsulated Sb architecture of Ti3C2Tx and graphene; these effectively mitigate against volume expansion and the pulverization of Sb, offering good electrolyte penetration and rapid ionic/electronic transmission. Ti3C2Tx also decreases the K+ diffusion energy barrier, and the ultra-thick compact electrode ensures volumetric and areal performance. These findings provide a feasible strategy for fabricating ultra-thick, dense alloy-type electrodes to achieve high areal and volumetric capacity energy storage via highly-dense, dual-encapsulated architectures with conductive elastic networks.