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Mesoporous Silicon Hollow Nanocubes Derived from Metal–Organic Framework Template for Advanced Lithium-Ion Battery Anode

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Center for Superfunctional Materials, Department of Chemistry and §Department of Energy Engineering, School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulsan 44919, Republic of Korea
Cite this: ACS Nano 2017, 11, 5, 4808–4815
Publication Date (Web):May 3, 2017
Copyright © 2017 American Chemical Society

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    Controlling the morphology of nanostructured silicon is critical to improving the structural stability and electrochemical performance in lithium-ion batteries. The use of removable or sacrificial templates is an effective and easy route to synthesize hollow materials. Herein, we demonstrate the synthesis of mesoporous silicon hollow nanocubes (m-Si HCs) derived from a metal–organic framework (MOF) as an anode material with outstanding electrochemical properties. The m-Si HC architecture with the mesoporous external shell (∼15 nm) and internal void (∼60 nm) can effectively accommodate volume variations and relieve diffusion-induced stress/strain during repeated cycling. In addition, this cube architecture provides a high electrolyte contact area because of the exposed active site, which can promote the transportation of Li ions. The well-designed m-Si HC with carbon coating delivers a high reversible capacity of 1728 mAhg–1 with an initial Coulombic efficiency of 80.1% after the first cycle and an excellent rate capability of >1050 mAhg–1 even at a 15 C-rate. In particular, the m-Si HC anode effectively suppresses electrode swelling to ∼47% after 100 cycles and exhibits outstanding cycle stability of 850 mAhg–1 after 800 cycles at a 1 C-rate. Moreover, a full cell (2.9 mAhcm–2) comprising a m-Si HC-graphite anode and LiCoO2 cathode exhibits remarkable cycle retention of 72% after 100 cycles at a 0.2 C-rate.

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