Stabilizing the Bulk-Phase and Solid Electrolyte Interphase of Silicon Microparticle Anode by Constructing Gradient-Hierarchically Ordered Conductive Networks

Liang Ma; Youyou Fang; Ni Yang; Ning Li; Lai Chen; Duanyun Cao; Yun Lu; Qing Huang; Tinglu Song; Yuefeng Su; Feng Wu

doi:10.1002/adma.202404360

Stabilizing the Bulk-Phase and Solid Electrolyte Interphase of Silicon Microparticle Anode by Constructing Gradient-Hierarchically Ordered Conductive Networks

Adv Mater. 2024 Apr 24:e2404360. doi: 10.1002/adma.202404360. Online ahead of print.

Authors

Liang Ma^{1

2}, Youyou Fang^{1

2}, Ni Yang², Ning Li^{1

2}, Lai Chen^{1

2}, Duanyun Cao^{1

2}, Yun Lu^{1

2}, Qing Huang^{1

2}, Tinglu Song³, Yuefeng Su^{1

2}, Feng Wu^{1

2}

Affiliations

¹ School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
² Innovation Center, Beijing Institute of Technology, Beijing, 100081, China.
³ Experimental Center of Advanced Materials School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081, China.

PMID: 38657134
DOI: 10.1002/adma.202404360

Abstract

The poor bulk-phase and interphase stability, attributable to adverse internal stress, impede the cycling performance of silicon microparticles (µSi) anodes and the commercial application for high-energy-density lithium-ion batteries. In this work, a groundbreaking gradient-hierarchically ordered conductive (GHOC) network structure, ingeniously engineered to enhance the stability of both bulk-phase and the solid electrolyte interphase (SEI) configurations of µSi, is proposed. Within the GHOC network architecture, two-dimensional (2D) transition metal carbides (Ti₃C₂T_x) act as a conductive "brick", establishing a highly conductive inner layer on µSi, while the porous outer layer, composed of one-dimensional (1D) Tempo-oxidized cellulose nanofibers (TCNF) and polyacrylic acid (PAA) macromolecule, functions akin to structural "rebar" and "concrete", effectively preserves the tightly interconnected conductive framework through multiple bonding mechanisms, including covalent and hydrogen bonds. Additionally, Ti₃C₂T_x enhances the development of a LiF-enriched SEI. Consequently, the µSi-MTCNF-PAA anode presents a high discharge capacity of 1413.7 mAh g^-1 even after 500 cycles at 1.0 C. Moreover, a full cell, integrating LiNi_0.8Mn_0.1Co_0.1O₂ with µSi-MTCNF-PAA, exhibits a capacity retention rate of 92.0% following 50 cycles. This GHOC network structure can offer an efficacious pathway for stabilizing both the bulk-phase and interphase structure of anode materials with high volumetric strain.

Keywords: LiF‐enriched sei; bulk‐phase and interphase structure; gradient‐hierarchically ordered conductive networks; tempo‐cnf; ti3c2tx.

Abstract

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