Abstract

With increasing demand for high-capacity and rapidly rechargeable anodes, problems associated with unstable evolution of a solid-electrolyte interphase on the active anode surface become more detrimental. Here, we report the near fatigue-free, ultrafast, and high-power operations of lithium-ion battery anodes employing silicide nanowires anchored selectively to the inner surface of graphene-based micro-tubular conducting electrodes. This design electrically shields the electrolyte inside the electrode from an external potential load, eliminating the driving force that generates the solid-electrolyte interphase on the nanowire surface. Owing to this electric control, a solid-electrolyte interphase develops firmly on the outer surface of the graphene, while solid-electrolyte interphase-free nanowires enable fast electronic and ionic transport, as well as strain relaxation over 2000 cycles, with 84% capacity retention even at ultrafast cycling (>20C). Moreover, these anodes exhibit unprecedentedly high rate capabilities with capacity retention higher than 88% at 80C (vs. the capacity at 1C).

Highlights

  • With increasing demand for high-capacity and rapidly rechargeable anodes, problems associated with unstable evolution of a solid-electrolyte interphase on the active anode surface become more detrimental

  • SEM images of the nickel silicide nanowires (NiSiNWs)@GrμT taken after cycling confirmed that the NiSiNWs maintained most of their original shape and size, they did show a roughened surface (Fig. 4a, b)

  • The selective formation of an solid-electrolyte interphase (SEI) layer on the outer surface of the GrμT, which agrees with our hypothesis, was confirmed (Fig. 4a, right panel)

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Summary

Introduction

With increasing demand for high-capacity and rapidly rechargeable anodes, problems associated with unstable evolution of a solid-electrolyte interphase on the active anode surface become more detrimental. We report the near fatigue-free, ultrafast, and highpower operations of lithium-ion battery anodes employing silicide nanowires anchored selectively to the inner surface of graphene-based micro-tubular conducting electrodes This design electrically shields the electrolyte inside the electrode from an external potential load, eliminating the driving force that generates the solid-electrolyte interphase on the nanowire surface. As a proofof-concept for the proposed strategy, we explore anodes with a high density of nickel silicide nanowires (NiSiNWs) anchored selectively to the inner surfaces of graphene-based micro-tubes (GrμTs) (hereinafter referred to as NiSiNWs@GrμT) In this anode design, the electrolyte inside the GrμTs is electrically separated from an external potential load, eliminating the buildup of potential difference that drives SEI formation on the surface of the NiSiNW anode during lithiation. The capacity fade is markedly reduced with a capacity of 780 mAh g–1 at 80C, retaining more than 88% of the capacity at 1C

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