Scalable Production of Freestanding Few-Layer β₁₂-Borophene Single Crystalline Sheets as Efficient Electrocatalysts for Lithium–Sulfur Batteries

Abstract

Two-dimensional (2D) borophene has attracted tremendous interest due to its fascinating properties, which have potential applications in catalysts, energy storage devices, and high-speed transistors. In the past few years, borophene was theoretically predicted as an ideal electrode material for lithium–sulfur (Li–S) batteries because of its low-density, metallic conductivity, high Li-ion surface mobility, and strong interface bonding energy to polysulfide. But until now, borophene-based Li–S batteries have not yet been achieved in experiments due to the absence of a large-scale synthetic method of freestanding borophene nanostructures with a high enough structural stability, conductivity, and uniformity. Herein, we developed a low-temperature liquid exfoliation (LTLE) method to synthesize freestanding few-layer β12-borophene single-crystalline sheets with a P6¯m2 symmetry in tens of milligrams. The as-synthesized 2D sheets were used as the polysulfide immobilizers and electrocatalysts of Li–S batteries. The resulting borophene-based Li–S battery delivered an extralarge areal capacity of 5.2 mAh cm–2 at a high sulfur loading of 7.8 mg cm–2, an excellent rate performance of 8 C (@721 mAh g–1), and an ultralow capacity fading rate of 0.039% in 1000 cycles, outperforming commercial Li-ion batteries and many other 2D material-based Li–S batteries. Based on the density functional theory model, the excellent electrochemical performances of the borophene-based Li–S batteries should originate from the enormous enhancement of β12-borophene sheets for both the surface migration of the Li-ions and the adsorption energy of Li2Sn clusters. Our results thus demonstrate a great potential for scalable production of freestanding β12-borophene single-crystalline sheets in future high-performance Li–S batteries.

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