April 7 - 11, 2025
Seattle, Washington
Symposium Supporters
2025 MRS Spring Meeting & Exhibit
CH01.10.01

Dehydrogenation-Driven Li Metal-Free Prelithiation for High Performance SiO-Based Lithium Storage Materials

When and Where

Apr 10, 2025
1:30pm - 2:00pm
Summit, Level 3, Room 342

Presenter(s)

Co-Author(s)

Hansu Kim1

Hanyang University1

Abstract

Hansu Kim1

Hanyang University1
Silicon monoxide (SiO)-based anode materials are one of the most intensively investigated class of materials for use as high-capacity anodes in lithium-ion batteries. However, their low initial Coulombic efficiency (ICE), resulting from the irreversible electrochemical reaction of the amorphous SiO2 (a-SiO2) phase in the SiO, restricts the wide-spread adoption of SiO-based anode materials in lithium-ion batteries. In this work, we deomonstrate Si/M-silicate(M: Li, Mg, Ca) nanocomposite materials based on the dehydorgenation reaction of metal hydrides to improve the electrochemical performance of SiO. The resulting Si/M-silicate nanocomposite materials showed much improved electrochemical performance compared to pristine SiO. Laser-assisted atom probe tomography(LA-APT) combined with high resolution transmission microscopy(HR-TEM) clearly revealed that two exothermic reactions during prelihitation process related to microstructural evolution are key in optimizing the domain size of Si active phase and metal silicate buffer phase, and their topological arrangements in prelithiated SiO materials. We also report that the pre-emptive formation of irreversible phase combined with high-energy mechanical milling (HEMM) process can simultaneously improve both the ICE and long-term cycle performance by effectivley mitigating the volume expansion of Si during cycling, resulting in improved long-term cycle stability.

Keywords

composite | Li | Si

Symposium Organizers

Kejie Zhao, Purdue University
Jungwon Park, Seoul National University
Luxi Li, Argonne National Laboratory
Yijin Liu, University of Texas at Austin

Session Chairs

Tongchao Liu
Weilai Yu

In this Session