Abstract

The development of lithium (Li)-metal anode is high priority research to initiate next-generation Li batteries. Applying Li-metal in practical applications as anode still has many hurdles to clear away, such as low Coulombic efficiency and capacity degradation by the continuous formation of dead Li. We demonstrate that cobalt (Co) nanoparticle incorporation in a porous carbon host anode can play a critical role in the formation of a thick lithium fluoride dominated solid-electrolyte interphase in ether-based electrolyte. As a result, the host anode containing Co nanoparticles shows excellent electrochemical performance with high Li-metal reversible capacity and even stable long-term cyclability with no dead Li formation.

Highlights

  • For the past few decades, lithium (Li) secondary batteries have played a crucial role in facilitating more rapid growth of portable electrical devices and the electric vehicle market, because their energy density and operating voltage are considerably higher than those of previous secondary batteries [1,2,3,4]

  • We have reported that the physical properties of nanoporous zeolitic imidazolate framework (ZIF)-derived carbons can be controlled by different ratios of zinc (Zn) to cobalt (Co)-ion metallic precursors [19,20,21]

  • According to the density functional theory calculations, Co-assisted nitrogen (N)-doped graphite structures can facilitate delocalization of transferred electrons from Li atoms near Co–N. This indicates that the strong binding and interaction between carbon and Li can be affected by the delocalized electrons over a wide range of area on the graphite surface, it still remains elusive as to how Co nanoparticles affect the interphase between ether-based electrolyte and the ZIF-derived carbon electrode

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Summary

Introduction

For the past few decades, lithium (Li) secondary batteries have played a crucial role in facilitating more rapid growth of portable electrical devices and the electric vehicle market, because their energy density and operating voltage are considerably higher than those of previous secondary batteries [1,2,3,4]. We have reported that the physical properties of nanoporous zeolitic imidazolate framework (ZIF)-derived carbons can be controlled by different ratios of zinc (Zn) to cobalt (Co)-ion metallic precursors [19,20,21] This approach was designed to achieve tailored ZIF-derived carbons with different pore volumes, pore sizes, surface areas, and even degrees of graphitization. According to the density functional theory calculations, Co-assisted nitrogen (N)-doped graphite structures can facilitate delocalization of transferred electrons from Li atoms near Co–N This indicates that the strong binding and interaction between carbon and Li can be affected by the delocalized electrons over a wide range of area on the graphite surface, it still remains elusive as to how Co nanoparticles affect the interphase between ether-based electrolyte and the ZIF-derived carbon electrode. Once the LiF-SEI is firmly established on the electrode surface, induced by the synergetic interaction between the Co nanoparticle-containing medium and the ether-based electrolyte, the anode shows excellent electrochemical performance with high Li-metal reversible capacity and even stable long-term cyclability with no dead Li formation

Experimental
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