Unveiling the Mechanical and Electrochemical Evolution of Nanosilicon Composite Anodes in Sulfide-Based All-Solid-State Batteries

Daxian Cao, Tongtai Ji, Avtar Singh, Seongmin Bak, Yonghua Du, Xianghui Xiao, Hongyi Xu, Juner Zhu, Hongli Zhu

Research output: Contribution to journalArticlepeer-review

Abstract

The utilization of silicon anodes in all-solid-state lithium batteries provides good prospects for facilitating high energy density. However, the compatibility of sulfide solid-state electrolytes (SEs) with Si and carbon is often questioned due to potential decomposition. Herein, operando X-ray absorption near-edge structure (XANES) spectroscopy, ex situ scanning electron microscopy (SEM), and ex situ X-ray nanotomography (XnT) are utilized to investigate the chemistry and structure evolution of nano-Si composite anodes. Results from XANES demonstrate a partial decomposition of SEs during the first lithiation stage, which is intensified by the presence of carbon. Nevertheless, the performances of first three cycles in Si–SE–C are stable, which proves that the generated media is ionically conductive. XnT and SEM results show that the addition of SEs and carbon improves the structural stability of the anode, with fewer pores and voids. A chemo-elasto-plastic model reveals that SEs and carbon buffer the volume expansion of Si, thus enhancing mechanical stability. The balance between the pros and cons of SEs and carbon in enhancing reaction kinetics and structural stability enables the Si composite anode to demonstrate the highest Si utilization with higher specific capacities and a better rate than pure Si and Si composite anodes with only SEs.

Original languageEnglish
JournalAdvanced Energy Materials
DOIs
Publication statusAccepted/In press - 2023

Bibliographical note

Funding Information:
D.C., T.J., and A.S. contributed equally to this work. H.Z. acknowledges the financial support from National Science Foundation under Award No. CBET‐ES‐1924534. A.S. and J.Z. are grateful to the financial support of NASA 19‐TTT‐0103 project (Award No. 80NSSC21M0114). This research used 8‐BM of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. This research used resources 18‐ID (FXI) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE‐SC0012704. The authors acknowledge the Boston Electron Microscopy Center at Northeastern University for the use of SEM facility. The authors would like to acknowledge the Northeastern University Center for Renewable Energy Technology for the use of XRD facility.

Publisher Copyright:
© 2023 Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

  • Renewable Energy, Sustainability and the Environment
  • Materials Science(all)

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