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PVD Customized 2D Porous Amorphous Silicon Nanoflakes Percolated with Carbon Nanotubes for High Areal Capacity Lithium Ion Batteries

Abstract

Integrating nanostructured Si materials into a freestanding membrane with high mechanical strength and continuous conductive network is a promising but challenging route to achieve high energy density lithium ion batteries (LIBs). Herein, we demonstrate that physical vapor deposition (PVD) customized two-dimensional (2D) porous amorphous Si nanoflakes, reinforced with ultralong multiwalled carbon nanotubes (MWCNTs), can be integrated into freestanding film electrode with high volumetric/areal capacity and energy density. Owing to the special 1D/2D nanotube/nanoflake entangled architecture, the freestanding Si-MWCNT film is highly porous, electrically conductive, and mechanically robust. Moreover, the interconnected MWCNT network functions as a spacer to prevent adjacent Si nanoflakes from restacking, and the 2D porous Si nanoflakes provide large electrode/electrolyte contact area, both of which enable fast Li+ transportation. Due to the existence of abundant pores in both amorphous Si nanoflakes (mesopores) and Si-MWCNT electrode (macropores), the volume change is significantly suppressed, resulting in stable electrodes with tunable mass loadings from 1.7 to 5.4 mg cm-2. When directly used as the anode electrode, the Si-MWCNT film with mass loading of 2.9 mg cm-2 exhibits a high specific capacity of 1556 mAh g-1 and areal capacity of 4.5 mAh cm-2. Remarkably, when coupling this freestanding anode with a commercial LiNi1/3Co1/3Mn1/3O2 (NCM) cathode, the full battery delivers a high gravimetric energy density of ~484.7 Wh kg-1. This study offers a promising and general route to design the freestanding electrodes by percolating CNTs with PVD generated 2D porous nanoflakes and provides significant insights for developing high energy battery systems.

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Supplementary files

Article information


Submitted
25 Nov 2019
Accepted
30 Jan 2020
First published
31 Jan 2020

J. Mater. Chem. A, 2020, Accepted Manuscript
Article type
Paper

PVD Customized 2D Porous Amorphous Silicon Nanoflakes Percolated with Carbon Nanotubes for High Areal Capacity Lithium Ion Batteries

S. Huang, Z. Wang, Y. Li, L. Liu, Y. Wang, J. Jin, D. Kong, L. Zhang and O. G. Schmidt, J. Mater. Chem. A, 2020, Accepted Manuscript , DOI: 10.1039/C9TA12923E

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