Effect of Microstructure and Elemental Composition on Electrode Interfacial Impedance of Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub>-based Batteries
Notice bibliographique
Résumé
Introduction Solid state batteries offer increased safety, high voltage stability, and simpler electrolyte chemistry than organic electrolytes. Their inherent protection from dendrite growth gives the capability to use metallic lithium anodes. Recent advances have improved conductivity to within an order of magnitude of organic electrolytes at room temperature. However, interfacial resistance between electrodes and the electrolyte remains a pressing concern. In a typical planar battery, this high resistance per area is magnified by low interfacial surface area. Elemental composition has a significant effect on the conductivity of a garnet electrolyte. The conductivity of the garnet fluctuates an order of magnitude based on a lithium stoichiometry of 6 to 7 in the Li7-xLa3Zr2-xTaxO12series. It has also been demonstrated that aluminium composition at the grain boundaries associated with higher temperature sintering increases conductivity. It stands to reason lithium activity extremes at the electrode interfaces effects would cause local variations in electrolyte composition and affect the conductivity. This study aims to address some of these concerns using a systematic study of the anode-electrolyte interface and the cathode-electrolyte interface. We investigate the elemental composition of the interface, as well as the effect of greatly increased surface area through a highly microporous electrolyte scaffold containing the cathode and anode material. Experimental Procedure Li7La3Zr2O12 garnet was produced in a conventional solid state method. 10% excess LiOH-H2O and stoichiometric amounts of La2O3 and ZrO2were ball milled in ethanol for 24 hours. The milled materials were added to an alumina crucible, calcined at 900 ºC for 4 hours, and milled again. A colloidal deposition of this slurry is prepared with polyvinyl butyral (PVB), benzyl butyl phthalate (BBP), and Solsperse dispersant in ethanol. Calcined powder is added to toluene and ethanol solvents with a binder system containing PVB, BBP, and menhaden fish oil as a dispersant. This preparation is milled for two days, then degassed in preparation for tape-casting. After tape-casting, tapes are drop-coated with the colloidal slurry and another tape is applied on top. This structure is held at 500ºC for 1 hour to burn off binders then heated to 1100 ºC for 1 hour. This produces a three layer porous-dense-porous scaffold of electrolyte that will maintain electronic isolation between electrodes. Symmetric cells with two cathodes are produced by infiltrating a glycine/metal-nitrate solution into the pores of each side and combusting. For two-anode symmetric cells, lithium is lightly pressed into both sides at 350 ºC. Electrochemical impedance spectroscopy was performed between room temperature and 300 ºC using a 10 mV amplitude between 10 MHz and 100 mHz. Electron energy loss spectroscopy was performed on a 2100F TEM equipped with a Gatan Tridiem post-it column energy filter. Results Figure 1 shows a cross section of a lithium-penetrated Li-garnet scaffold showing the fracture plane of the garnet(light) fully coated by the lithium (dark). Figure 2 shows the Nyquist plot of a full cell made with a lithium-penetrated scaffold. The bulk conductivity shown in the inset is fairly low at 20 Ω compared to the 1000 Ω overall cell impedance.
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Comment cette classification a été obtenuedéplier
Prédiction machine sur la base complète
Imitation des enseignantsNi prévalence calibrée, ni vérité terrain. Validation humaine à venir. Le volet Gemma est une étiquette directe du modèle pour chaque travail de la base, lue sur la notice réduite au titre. Le volet Codex est un classifieur appris des 10 348 étiquettes directes de Codex et calibré sur les taux pondérés de l'échantillon; les champs sans appui suffisant ne portent aucun appel Codex. Le mode candidate est l'union des deux volets; le consensus est leur intersection. Ces sorties portent le statut machine_predicted_unvalidated et ne sont pas des étiquettes humaines.
Scores du classifieur distillé par catégorie (deux têtes)
| Catégorie | Codex | Gemma |
|---|---|---|
| Métarecherche | 0,000 | 0,000 |
| Méta-épidémiologie (sens strict) | 0,000 | 0,000 |
| Méta-épidémiologie (sens large) | 0,000 | 0,000 |
| Bibliométrie | 0,000 | 0,000 |
| Études des sciences et des technologies | 0,000 | 0,000 |
| Communication savante | 0,000 | 0,000 |
| Science ouverte | 0,000 | 0,000 |
| Intégrité de la recherche | 0,000 | 0,000 |
| Charge utile insuffisante (le modèle a refusé de juger) | 0,001 | 0,000 |
Scores machine (provisoires)
Les deux têtes enseignantes du modèle étudiant, lues sur ce travail. Un score ordonne la base pour la relecture; il n'affirme jamais une catégorie, et le statut de validation accompagne chaque rangée tel quel.
Scores de référence d'un modèle non mature (critères de maturité non atteints, 7 itérations). Un score ordonne; il n'affirme jamais une catégorie.
score_only:v0-immature-baseline · tel quel depuis la passe de notation : score_only signifie que le nombre peut ordonner les travaux, et qu'aucune étiquette de catégorie n'en découleClassification
machine, non validéePrédiction automatique; un appel candidat d’une seule source (Gemma direct ou Codex distillé), pas un consensus.
Le détail, modèle par modèle et score par score, se trouve en fin de page sous « Comment cette classification a été obtenue ».