Silicon-based all-solid-state batteries operating free from external pressure

Zhiyong Zhang, Xiuli Zhang, Yan Liu, Chaofei Lan, Xiang Han (hanxiang@njfu.edu.cn), Shanpeng Pei, Linshan Luo, Pengfei Su, Ziqi Zhang, Jingjing Liu, Zhengliang Gong, Cheng Li, Guangyang Lin, Cheng Li, Wei Huang, Ming-Sheng Wang (mswang@xmu.edu.cn) and Songyan Chen (sychen@xmu.edu.cn)
Additional contact information
Zhiyong Zhang: Xiamen University
Xiuli Zhang: Xiamen University
Yan Liu: South China Normal University
Chaofei Lan: Xiamen University
Xiang Han: Nanjing Forestry University
Shanpeng Pei: Xiamen University
Linshan Luo: Xiamen University
Pengfei Su: Xiamen University
Ziqi Zhang: Science and Technology on Analog Integrated Circuit Laboratory
Jingjing Liu: Microsoft Corporation, One Microsoft Way
Zhengliang Gong: Xiamen University
Cheng Li: Xiamen University
Guangyang Lin: Xiamen University
Cheng Li: Xiamen University
Wei Huang: Xiamen University
Ming-Sheng Wang: Xiamen University
Songyan Chen: Xiamen University

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: Abstract Silicon-based all-solid-state batteries offer high energy density and safety but face significant application challenges due to the requirement of high external pressure. In this study, a Li21Si5/Si–Li21Si5 double-layered anode is developed for all-solid-state batteries operating free from external pressure. Under the cold-pressed sintering of Li21Si5 alloys, the anode forms a top layer (Li21Si5 layer) with mixed ionic/electronic conduction and a bottom layer (Si–Li21Si5 layer) containing a three-dimensional continuous conductive network. The resultant uniform electric field at the anode|SSE interface eliminates the need for high external pressure and simultaneously enables a twofold enhancement of the lithium-ion flux at the anode interface. Such an efficient ionic/electronic transport system also facilitates the uniform release of cycling expansion stresses from the Si particles and stabilizes bulk-phase and interfacial structure of anode. Consequently, the Li21Si5/Si–Li21Si5 anode exhibited a critical current density of 10 mA cm−2 at 45 °C with a capacity of 10 mAh cm−2. And the Li21Si5/Si–Li21Si5|Li6PS5Cl|Li3InCl6|LCO cell achieve an high initial Coulombic efficiency of (97 ± 0.7)% with areal capacity of 2.8 mAh cm−2 at 0.25 mA cm−2, as well as a low expansion rate of 14.5% after 1000 cycles at 2.5 mA cm−2.

Date: 2025
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DOI: 10.1038/s41467-025-56366-z

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