Academic Journal
Li+ concentration and morphological changes at the anode and cathode interphases inside solid-state lithium metal batteries
| Title: | Li+ concentration and morphological changes at the anode and cathode interphases inside solid-state lithium metal batteries |
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| Authors: | Chun Huang, Matthew D Wilson, Ben Cline, Abeiram Sivarajah, Wiebe Stolp, Matthieu N Boone, Thomas Connolley, Chu Lun Alex Leung |
| Source: | JPhys Energy, Vol 7, Iss 2, p 025009 (2025) |
| Publisher Information: | IOP Publishing, 2025. |
| Publication Year: | 2025 |
| Collection: | LCC:Production of electric energy or power. Powerplants. Central stations LCC:Renewable energy sources |
| Subject Terms: | solid-state batteries, correlative imaging, lithium ion concentration, microstructure, x-ray Compton scattering, mass transport, Production of electric energy or power. Powerplants. Central stations, TK1001-1841, Renewable energy sources, TJ807-830 |
| More Details: | Irregular Li heterostructure growth at the interphase between the solid electrolyte and anode reduces solid-state Li metal battery (SSLMB) performance, but the fundamental cause is still elusive. Measuring and imaging Li ^+ ion diffusion in operando inside an SSLMB using a commercially standard cell configuration are extremely challenging because the ultra-light Li element exhibits a minute signal-to-noise ratio using most x-ray-related characterization methods, and the weak x-ray signals of Li ^+ are buried by strong signals of other heavy transition metal elements in the cathode and battery enclosure. Here, we pioneer novel operando correlative imaging of coupling x-ray Compton scattering with computed tomography (XCS-CT), which is able to quantify the interplay between spatially resolved Li ^+ ion diffusion kinetics and Li ^0 metal structure growth at the interphases of both the anode and cathode sides inside a full-cell SSLMB using a solid polymer electrolyte (SPE) and commercially standard cell configuration during (dis)charging. We show a 61% increase in the efficiency of extracting Li ^+ ions from the cathode LiNi _0.6 Mn _0.2 Co _0.2 O _2 to the anode during charging at 0.1 C compared with at 1 C due to restricted Li ^+ ion diffusion at the higher rate inside SSLMB. However, this led to the formation of a more irregular interfacial morphology, consisting not only of Li ^0 dendrites, but also sub-surface pore formation at the anode/SPE interphase. We find that surprisingly, the irregular Li ^0 structure initiation and growth are accelerated during the first Li stripping step, not the Li plating step, and the root cause is the onset imbalance of Li ^+ ion diffusion and redox reactions between the anode and cathode. These insights highlight the benefits of asymmetric charging and discharging rates as a promising solution to improving SSLMB performance with SPEs. The operando correlative XCS-CT imaging technique has the potential to study the relationship between active ion concentrations and buried morphological changes for a variety of battery chemistries. |
| Document Type: | article |
| File Description: | electronic resource |
| Language: | English |
| ISSN: | 2515-7655 |
| Relation: | https://doaj.org/toc/2515-7655 |
| DOI: | 10.1088/2515-7655/adafda |
| Access URL: | https://doaj.org/article/59cc3719a6534d95b3003e9b23e913fe |
| Accession Number: | edsdoj.59cc3719a6534d95b3003e9b23e913fe |
| Database: | Directory of Open Access Journals |
| ISSN: | 25157655 |
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| DOI: | 10.1088/2515-7655/adafda |
| Published in: | JPhys Energy |
| Language: | English |