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

Zhiyong Zhang; Xiuli Zhang; Yan Liu; Chaofei Lan; Xiang Han; Shanpeng Pei; Linshan Luo; Pengfei Su; Ziqi Zhang; Jingjing Liu; Zhengliang Gong; Cheng Li; Guangyang Lin; Cheng Li; Wei Huang; Ming-Sheng Wang; Songyan Chen

doi:10.1038/s41467-025-56366-z

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

Nat Commun. 2025 Jan 25;16(1):1013. doi: 10.1038/s41467-025-56366-z.

Authors

Zhiyong Zhang^#¹, Xiuli Zhang^#², Yan Liu^#³, Chaofei Lan^#¹, Xiang Han⁴, Shanpeng Pei^{1

5}, Linshan Luo¹, Pengfei Su¹, Ziqi Zhang⁶, Jingjing Liu⁷, Zhengliang Gong⁸, Cheng Li⁸, Guangyang Lin¹, Cheng Li¹, Wei Huang¹, Ming-Sheng Wang^{9

10}, Songyan Chen¹¹

Affiliations

¹ Department of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen University, Xiamen, China.
² State Key Lab of Physical Chemistry of Solid Surfaces, College of Materials, Xiamen University, Xiamen, China.
³ School of Semiconductor Science and Technology, South China Normal University, Foshan, China.
⁴ College of Materials Science and Engineering, Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Nanjing Forestry University, Nanjing, China. hanxiang@njfu.edu.cn.
⁵ Shandong Electric Power Engineering Consulting Institute Corporation, Jinan, China.
⁶ Science and Technology on Analog Integrated Circuit Laboratory, Chongqing, China.
⁷ Microsoft Corporation, One Microsoft Way, Redmond, WA, USA.
⁸ College of Energy, Xiamen University, Xiamen, China.
⁹ Department of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen University, Xiamen, China. mswang@xmu.edu.cn.
¹⁰ State Key Lab of Physical Chemistry of Solid Surfaces, College of Materials, Xiamen University, Xiamen, China. mswang@xmu.edu.cn.
¹¹ Department of Physics, Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Key Laboratory of Low Dimensional Condensed Matter Physics (Department of Education of Fujian Province), Jiujiang Research Institute, Xiamen University, Xiamen, China. sychen@xmu.edu.cn.

^# Contributed equally.

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.