Issue 11, 2023

Manipulating charge-transfer kinetics and a flow-domain LiF-rich interphase to enable high-performance microsized silicon–silver–carbon composite anodes for solid-state batteries

Abstract

A silicon (Si) anode with a high theoretical specific capacity (3579 mA h g−1) offers great promise for realizing high-energy solid-state batteries (SSBs). However, given Si's huge volume variations during cycling, sluggish kinetics and unfavorable interface stability with a solid-state electrolyte (SSE), its practical potential in SSBs has not been fully exploited. Herein, we propose a design of highly dense Ag nanoparticles decorated with porous microsized Si, which is coated by thin-layer carbon (PS–Ag–C) working as a high-performance anode for boosting SSB performance. Specifically, the mechanical stress at the interface, originating from a large volume change of Si, can be alleviated by the highly porous architecture. Meanwhile, continuous charge transfer within Si can be achieved by the introduction of Ag nanoparticles, a thin carbon layer and the as-formed Ag–Li alloys, which contribute to high-rate capability and stable cycling performance. Furthermore, coupled with a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)/Li1.3Al0.3Ti1.7(PO4)3 (LATP) SSE with low mobility, a flow-domain LiF-rich solid–electrolyte-interphase (SEI) is formed, ensuring desirable interfacial and mechanical stability. Accordingly, the as-fabricated PS–Ag–C anode achieves high reversible capacities of 3030.3 mA h g−1 at 0.2 A g−1 with an initial Coulombic efficiency of 90% and 1600 mA h g−1 over 500 cycles at 1 A g−1, respectively. In particular, we observed that the highest areal capacity reaches 4.0 mA h cm−2 over 100 cycles at 0.5 A g−1 in Si-based SSBs with organic–inorganic composite SSEs. Moreover, a solid-state full cell assembled with the as-obtained PS–Ag–C anode and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode demonstrates high capacity and desirable cycling stability. This work provides new insights into developing a high-capacity and durable Si anode for high-performance SSBs.

Graphical abstract: Manipulating charge-transfer kinetics and a flow-domain LiF-rich interphase to enable high-performance microsized silicon–silver–carbon composite anodes for solid-state batteries

Supplementary files

Article information

Article type
Paper
Submitted
26 May 2023
Accepted
21 Sep 2023
First published
27 Sep 2023

Energy Environ. Sci., 2023,16, 5395-5408

Manipulating charge-transfer kinetics and a flow-domain LiF-rich interphase to enable high-performance microsized silicon–silver–carbon composite anodes for solid-state batteries

X. Han, L. Gu, Z. Sun, M. Chen, Y. Zhang, L. Luo, M. Xu, S. Chen, H. Liu, J. Wan, Y. He, J. Chen and Q. Zhang, Energy Environ. Sci., 2023, 16, 5395 DOI: 10.1039/D3EE01696J

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