Abstract

Silicon (Si) based materials are highly desirable to replace currently used graphite anode for lithium ion batteries. Nevertheless, its usage is still a big challenge due to poor battery performance and scale-up issue. In addition, two-dimensional (2D) architectures, which remain unresolved so far, would give them more interesting and unexpected properties. Herein, we report a facile, cost-effective, and scalable approach to synthesize Si nanocrystals embedded 2D SiOx nanofoils for next-generation lithium ion batteries through a solution-evaporation-induced interfacial sol-gel reaction of hydrogen silsesquioxane (HSiO1.5, HSQ). The unique nature of the thus-prepared centimeter scale 2D nanofoil with a large surface area enables ultrafast Li+ insertion and extraction, with a reversible capacity of more than 650 mAh g−1, even at a high current density of 50 C (50 A g−1). Moreover, the 2D nanostructured Si/SiOx nanofoils show excellent cycling performance up to 200 cycles and maintain their initial dimensional stability. This superior performance stems from the peculiar nanoarchitecture of 2D Si/SiOx nanofoils, which provides short diffusion paths for lithium ions and abundant free space to effectively accommodate the huge volume changes of Si during cycling.

Highlights

  • Despite these outstanding advantages of 2D morphology, the synthesis of 2D nanostructured materials has been very limited and applied to only a few materials via chemical vapor deposition (CVD) or self-assembly[21,22,23,24,25,26,27,28,29,30]

  • We expect that unique 2D Si/SiOx nanofoils can effectively minimize the inevitable mechanical strain induced by Li+ insertion, thereby promoting strong enhancement in Li+ storage capability

  • The process was deliberately designed after careful consideration of various synthetic parameters, such as the vapor pressure of precursor and the reaction temperature

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Summary

Introduction

Despite these outstanding advantages of 2D morphology, the synthesis of 2D nanostructured materials has been very limited and applied to only a few materials via chemical vapor deposition (CVD) or self-assembly[21,22,23,24,25,26,27,28,29,30]. We have developed a highly reliable Si/SiOx nanocomposite via a sol-gel reaction, which exhibited a high reversible capacity In a continuing effort to exploit advanced Si/SiOx nanocomposite using this synthetic approach, we here propose a facile and scalable synthesis of large-area Si/SiOx 2D nanofoils with a thickness of about 8 nm as a potential Li+ storage material for lithium ion batteries (LIBs) via a solution evaporation induced interfacial sol-gel reaction. We expect that unique 2D Si/SiOx nanofoils can effectively minimize the inevitable mechanical strain induced by Li+ insertion, thereby promoting strong enhancement in Li+ storage capability. Our newly developed approach presented here allows the synthesis of facile, cost-effective, and scalable 2D Si/SiOx nanofoils in an aqueous solution by promoting lateral growth of hydrogen silsesquioxane (HSiO1.5, HSQ) nanofoils at the interface between water and air

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