Issue 9, 2024

Polymer configuration conversion mechanism in dynamically stable interface of silicon anodes

Abstract

Silicon oxide nanospheres (SiOC) have been considered one of the key candidates for the next generation of high-energy-density anode materials. Nevertheless, the intrinsic limitations of their design impede their large-scale commercial deployment, including large volume expansion, poor electrical conductivity, and low initial coulombic efficiency (ICE). The application of a polymer coating represents a beneficial modification. Herein, a composite SiOC anode is synthesized by constructing poly(hexaazatrinaphthalene) (PHATN) on the surface of boron doping-induced self-assembled SiOC nanospheres. The SiOC nanospheres change from a monodisperse structure to a regular and ordered arrangement by self-assembly, which improves the structural stability. A special polymer, PHATN, is selected for its unique structure, which introduces a dynamic conversion mechanism to the material. During the lithium intercalation process, –C[double bond, length as m-dash]N– groups in the PHATN coordinate with Li+ to form –C–N–Li– bonds on the PHATN molecule layer. The dynamic volume change of the PHATN molecule allows room for the volume expansion of SiOC, thus providing excellent protection against structural collapse. After 1000 deep cycles, the capacity of the composite anode can be maintained at 623.7 mA h g−1, showing considerable stability and superior specific capacity. PHATN simultaneously repairs the surface defects of the SiOC assemblies and enhances the performance of the SEI membrane, increasing the ICE from 40% to 50%, which exhibits better electrochemical performance.

Graphical abstract: Polymer configuration conversion mechanism in dynamically stable interface of silicon anodes

Supplementary files

Article information

Article type
Paper
Submitted
15 mar 2024
Accepted
30 mai 2024
First published
07 jun 2024

Mol. Syst. Des. Eng., 2024,9, 937-946

Polymer configuration conversion mechanism in dynamically stable interface of silicon anodes

Q. Ye, M. Jiang, Y. Zhang, L. Chen, Y. Ma and J. Yang, Mol. Syst. Des. Eng., 2024, 9, 937 DOI: 10.1039/D4ME00049H

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