Electrochemical Performance and Microstructure Evolution of a Quasi-Solid-State Lithium Battery Prepared by Spark Plasma Sintering
Bibliographic record
Abstract
Solid-state lithium batteries are promising next-generation energy storage systems for electric vehicles due to their high energy density and high safety and require achieving and maintaining intimate solid–solid interfaces for lithium-ion and electron transport. However, the solid–solid interfaces may evolve over cycling, disrupting the ion and electron diffusion pathways and leading to rapid performance degradation. The development of solid-state lithium batteries has been hindered by the lack of fundamental understanding of the interfacial microstructure change over cycling and its relation to electrochemical properties. Herein, we prepared a quasi-solid-state lithium battery, 30%LiFePO 4 -55%Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 -15%C| Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 |Li, by spark plasma sintering, and employed it as a model system to reveal the microstructure evolution at the solid–solid interfaces with electrochemical performance of the batteries. The electrochemical assessment showed that the quasi-solid-state lithium battery exhibited a discharge specific capacity of about 150 mAh g –1 in the first 80 cycles and then experienced severe capacity attenuation afterward, accompanied by a gradual internal resistance increase. Scanning electron microscopy observation showed that more cracks were formed inside the solid-state electrolyte and at the solid–solid interfaces as the battery cycled from 10 to 67 and 157 cycles. Detailed microstructure and phase analysis by high-resolution transmission electron microscopy and selected area electron diffraction discovered that the crack formation and performance decay were mainly caused by (1) the volume change of the LiFePO 4 composite cathode during cycling, (2) the grain expansion of the Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 solid-state electrolyte at its interface with lithium anode, and (3) the formation of a solid electrolyte interphase layer, comprising Li 2 CO 3, LiF, and LiTFSI, at the cathode–solid-state electrolyte interface. These microstructure changes built up over repeated battery cycling, ultimately causing the structure collapse and battery failure. The microstructure evolution information is expected to guide the design of better structures and interfaces for solid-state lithium batteries.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".