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Hybrid 2D/3D carbon framework confined Si with optimized reaction kinetics for highly stable Li-Ion storage.

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Title:	Hybrid 2D/3D carbon framework confined Si with optimized reaction kinetics for highly stable Li-Ion storage.
Authors:	Lin, LiLin¹ (AUTHOR), Zhou, Peijun¹ (AUTHOR), Xiong, Wen¹ (AUTHOR), Zhao, Tingting² (AUTHOR), Li, Shengsong¹ (AUTHOR), Yang, Liangui¹ (AUTHOR), Meng, Tao¹ (AUTHOR) mengt@scnu.edu.cn, Zhong, Junhao¹ (AUTHOR), Cui, Zhibiao¹ (AUTHOR), Shu, Dong^1,3 (AUTHOR) dshu@scnu.edu.cn
Source:	Chemical Engineering Journal. Nov2024, Vol. 499, pN.PAG-N.PAG. 1p.
Subjects:	Chemical kinetics, Structural stability, Electrode reactions, Carbon nanotubes, Silicon surfaces
Abstract:	Building 2D/3D carbon hierarchical structures on the surface of silicon particles to optimize the electron/Li-ion reaction kinetics and alleviate the stress accumulation in silicon-based anode for stable Li-ion storage. [Display omitted] • Constructing 2D/3D hybrid structure within the Si anode show stable Li-ion storage. • Theoretical simulations analyze the physicochemical properties of the composites. • The fabricated Si-based anode exhibits superior electrochemical performance. • The electrode reaction and stress dissipation mechanisms are well demonstrated. Three-dimensional (3D) conductive skeletons can optimize electron/Li-ion migration kinetics and alleviate stress accumulation for silicon (Si)-based electrodes. In this study, the modified carbon nanotubes (MCNs) are used as a stress-buffering and high-speed conducting framework, and a hierarchical structure of 3D MCNs interspersed with flour-derived 2D N-doped C layer is designed for Si anode via molecular self-assembly and in-situ carbonization strategies. Experimental and theoretical calculations show that the charge redistribution occurred in the fabricated SiO x and N-doped C interfaces, which induced an electric field response and increased the interfacial electron/Li-ion transfer rate. Multiphysics simulations show that the 2D/3D hierarchical structures of carbon can optimize the physicochemical properties, such as a favorable local electronic environment, flexible stress dissipation mechanisms and good thermal stability. The prepared electrode with 77.1 wt% Si@SiO x shows a low volume expansion rate of 23 % and has an excellent Li-ion storage capability (972.1 mAh g−1 at 4000 mA g−1). Moreover, the structural stability of fabricated Si-based electrodes is enhanced, achieving 0.04 % per cycle capacity decay for 500 cycles at 2000 mA g−1. Such integrating the 2D/3D carbon framework to manipulate Si interfacial properties provides fundamental research for other electrodes plagued by significant volume expansion. [ABSTRACT FROM AUTHOR]
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Database:	Engineering Source

Description
Abstract:	Building 2D/3D carbon hierarchical structures on the surface of silicon particles to optimize the electron/Li-ion reaction kinetics and alleviate the stress accumulation in silicon-based anode for stable Li-ion storage. [Display omitted] • Constructing 2D/3D hybrid structure within the Si anode show stable Li-ion storage. • Theoretical simulations analyze the physicochemical properties of the composites. • The fabricated Si-based anode exhibits superior electrochemical performance. • The electrode reaction and stress dissipation mechanisms are well demonstrated. Three-dimensional (3D) conductive skeletons can optimize electron/Li-ion migration kinetics and alleviate stress accumulation for silicon (Si)-based electrodes. In this study, the modified carbon nanotubes (MCNs) are used as a stress-buffering and high-speed conducting framework, and a hierarchical structure of 3D MCNs interspersed with flour-derived 2D N-doped C layer is designed for Si anode via molecular self-assembly and in-situ carbonization strategies. Experimental and theoretical calculations show that the charge redistribution occurred in the fabricated SiO x and N-doped C interfaces, which induced an electric field response and increased the interfacial electron/Li-ion transfer rate. Multiphysics simulations show that the 2D/3D hierarchical structures of carbon can optimize the physicochemical properties, such as a favorable local electronic environment, flexible stress dissipation mechanisms and good thermal stability. The prepared electrode with 77.1 wt% Si@SiO x shows a low volume expansion rate of 23 % and has an excellent Li-ion storage capability (972.1 mAh g−1 at 4000 mA g−1). Moreover, the structural stability of fabricated Si-based electrodes is enhanced, achieving 0.04 % per cycle capacity decay for 500 cycles at 2000 mA g−1. Such integrating the 2D/3D carbon framework to manipulate Si interfacial properties provides fundamental research for other electrodes plagued by significant volume expansion. [ABSTRACT FROM AUTHOR]
ISSN:	13858947
DOI:	10.1016/j.cej.2024.156266