Abstract

Lithium metal has been regarded as the future anode material for high-energy-density rechargeable batteries due to its favorable combination of negative electrochemical potential and high theoretical capacity. However, uncontrolled lithium deposition during lithium plating/stripping results in low Coulombic efficiency and severe safety hazards. Herein, we report that nanodiamonds work as an electrolyte additive to co-deposit with lithium ions and produce dendrite-free lithium deposits. First-principles calculations indicate that lithium prefers to adsorb onto nanodiamond surfaces with a low diffusion energy barrier, leading to uniformly deposited lithium arrays. The uniform lithium deposition morphology renders enhanced electrochemical cycling performance. The nanodiamond-modified electrolyte can lead to a stable cycling of lithium | lithium symmetrical cells up to 150 and 200 h at 2.0 and 1.0 mA cm–2, respectively. The nanodiamond co-deposition can significantly alter the lithium plating behavior, affording a promising route to suppress lithium dendrite growth in lithium metal-based batteries.

Highlights

  • Lithium metal has been regarded as the future anode material for high-energy-density rechargeable batteries due to its favorable combination of negative electrochemical potential and high theoretical capacity

  • Inspired by this co-deposition strategy, we propose the use of nanodiamond additives in a conventional Li ion batteries (LIBs) electrolyte, lithium hexafluorophosphate (LiPF6)-ethylene carbonate (EC)/diethyl carbonate (DEC) electrolyte, to suppress Li dendrite growth

  • The interplanar crystal spacing in lattice-fringe transmission electron microscopy (TEM) images was measured to be ~ 0.21 nm, which corresponds to diamond (111) planes (0.206 nm, PDF#65-0537)

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Summary

Introduction

Lithium metal has been regarded as the future anode material for high-energy-density rechargeable batteries due to its favorable combination of negative electrochemical potential and high theoretical capacity. The Li+/Li redox couple provides the most negative potential of −3.04 V (vs standard hydrogen electrode), rendering a high working voltage in a full cell These features deliver a high-energy density when the Li metal anode is paired with the high-capacity cathode material to form a full cell. A major improvement in properties can be achieved with minimal capture of nanodiamond particles, due to modification of the deposition conditions with nanoparticles at the solid-electrolyte interface[36] Inspired by this co-deposition strategy, we propose the use of nanodiamond additives in a conventional LIB electrolyte, lithium hexafluorophosphate (LiPF6)-ethylene carbonate (EC)/diethyl carbonate (DEC) electrolyte, to suppress Li dendrite growth. After adding nanodiamonds to the electrolyte, Li ions co-deposit with nanodiamond particles onto the substrate, producing uniform and dendrite-free Li deposits, and, resulting in stable electrochemical cycling (Fig. 1b)

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