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DE-SC0024528: Uncovering the mechano-electro-chemo mechanism of fresh Li in sulfide based all solid-state batteries through operando studies

Award Status: Active
  • Institution: Northeastern University, Boston, MA
  • DUNS: 001423631
  • Most Recent Award Date: 09/20/2023
  • Number of Support Periods: 1
  • PM: Henderson, Craig
  • Current Budget Period: 08/01/2023 - 07/31/2024
  • Current Project Period: 08/01/2023 - 07/31/2026
  • PI: Zhu, Hongli
  • Supplement Budget Period: N/A

Public Abstract

Lithium (Li) metal is a desirable anode material for all-solid-state batteries due to its low electrochemical potential, high capacity, and lightweight properties. However, the utilization of Li metal faces challenges, particularly dendritic growth. All-solid-state Li metal batteries (ASLMBs) have been proposed as a solution to suppress dendrites by leveraging their high mechanical strength. However, ASLMBs encounter additional hurdles such as significant volume changes, mechanical creeping, deformation, and interface contact issues. Furthermore, the "soft-short" mechanism in ASLMBs remains complex and poorly understood. During the charging and discharging process, Li metal exists in two distinct forms: the initial bulky Li metal and the Li that departs from the cathode. Understanding the differences in chemical, electrochemical, and mechanical properties between these two forms is critical. 
This project aims to gain fundamental insights into the atomic, crystalline, chemical, and mechanical distinctions between the as-plated Li metal (referred to as fresh Li) and the original bulky Li, leading to a better understanding of the metallic Li anode and the realization of safe Li metal batteries with higher energy density. The research objective is to study the real-time mechano-electro-chemo behavior of fresh Li metal during various plating and stripping processes in ASLMBs using operando studies and mechanical modeling. The goal is to develop principles of Li plating and stripping in ASLMBs that can inform the design of Li metal anodes through structure and interface engineering, ensuring long-term stability in all-solid-state batteries. This project specifically emphasizes investigating the mechanical properties of fresh Li metal during the early plating stages, a crucial factor in maintaining Li metal stability within the battery.

To achieve the main objectives of this project, a multifaceted and integrated approach, combining operando characterization, experimentation, and computation, will be employed. The material chemistry of fresh Li will be investigated experimentally and theoretically, analyzing its atomic structure, interatomic bonding, and crystalline structure, and comparing the results to those of bulky Li. The mechano-electro-chemo behavior of Li metal in ASLMBs will be evaluated through operando techniques, characterizing its mechanical properties, and observing Li behaviors such as nucleation, plating/stripping, deformation, propagation, creeping, and vacancy/void formation. These findings will guide the designs of stable Li metal anodes. Various strategies will be employed to address dendrite formation in ASLMBs, aiming to achieve high cell-level energy density, extended cycling life, and superior rate performance. 

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