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Research Article

Synergistic protection of Si anode based on multi-dimensional graphitic carbon skeletons

Qitao Shi1,§Haiming Wang1,§Junhua Zhou1Huy Quang Ta1,2Jiaqi Wang1Xueyu Lian1Klaudia Kurtyka3Barbara Trzebicka3Thomas Gemming4Mark H. Rümmeli1,2,3,4( )
Soochow Institute for Energy and Materials Innovation, College of Energy, Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou 215006, China
Institute for Complex Materials, IFW Dresden, 20 Helmholtz Strasse, Dresden 01069, Germany
Centre of Polymer and Carbon Materials, Polish Academy of Sciences, M. Curie-Sklodowskiej 34, Zabrze 41-819, Poland
Thomas Gemming - Institute of Environmental Technology, VSB-Technical University of Ostrava, 17. Listopadu 15, Ostrava 70833, Czech Republic

§ Qitao Shi and Haiming Wang contributed equally to this work.

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Graphical Abstract

This work proposes a bottom-up method synthesized hollow graphene shell as an elastic skeleton and employs graphene as an extra armor to synergistically prepare advanced corn-like Si@hollow graphene shell@graphene (Si@GS@G) anode. Improved conductivity and structural stability are harvested attributed to the porous and rigid conductive network.

Abstract

Inspired by the natural corn structure, a Si@hollow graphene shell@graphene (Si@GS@G) anode material was prepared in which silicon nanoparticles were preliminarily anchored onto the surface of an elastic graphene shell and further constrained using graphene sheets. Hollow graphene oxide shells with abundant surficial hydrogen bonds, which were synthesized using a novel bottom-up method, were used as an intermediate material to anchor positively charged silicon nanoparticles via electrostatic attraction and achieve a rational spatial distribution. The inner hollow graphene shell anchorage and outer graphene constraint synergistically constituted a porous and robust conductive corn-like structure. The as-fabricated Si@GS@G anode afforded efficient electron and ion transport pathways and improved structural stability, thereby enhancing Li+ storage capability (505 mAh·g−1 at 10 A·g−1) and extending the lifespan compared to the single hollow graphene shell or graphene sheet-protected Si anode (72% capacity retention after 500 cycles). The improved kinetics of the Si@GS@G anode were investigated using electro impedance spectroscopy, galvanostatic intermittent titration, and pseudocapacitance contribution rate analysis, and the structural evolution was analyzed using ex situ electron microscopy. This study proposes a novel hollow graphene oxide shell as an activated intermediate material for designing a porous electrode structure that facilitates an enhanced electrochemical performance.

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Nano Research
Pages 8146-8155
Cite this article:
Shi Q, Wang H, Zhou J, et al. Synergistic protection of Si anode based on multi-dimensional graphitic carbon skeletons. Nano Research, 2022, 15(9): 8146-8155. https://doi.org/10.1007/s12274-022-4518-9
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Received: 18 March 2022
Revised: 25 April 2022
Accepted: 09 May 2022
Published: 22 June 2022
© Tsinghua University Press 2022
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