Browse
Submit Data
Databases
API
Help

Dataset Information

29 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Evolving contact mechanics and microstructure formation dynamics of the lithium metal-Li7La3Zr2O12 interface

ABSTRACT: The dynamic behavior of the interface between the lithium metal electrode and a solid-state electrolyte plays a critical role in all-solid-state battery performance. The evolution of this interface throughout cycling involves multiscale mechanical and chemical heterogeneity at the micro- and nano-scale. These features are dependent on operating conditions such as current density and stack pressure. Here we report the coupling of operando acoustic transmission measurements with nuclear magnetic resonance spectroscopy and magnetic resonance imaging to correlate changes in interfacial mechanics (such as contact loss and crack formation) with the growth of lithium microstructures during cell cycling. Together, the techniques reveal the chemo-mechanical behavior that governs lithium metal and Li7La3Zr2O12 interfacial dynamics at various stack pressure regimes and with voltage polarization. All-solid-state batteries are promising alternatives to Li-ion batteries. Here, the authors investigate the chemo-mechanical changes at the lithium metal/solid electrolyte interface via operando acoustic transmission and magnetic resonance imaging.

SUBMITTER: Chang W

PROVIDER: S-EPMC8569160 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Cross-Linked Composite Solid Polymer Electrolyte Doped with Li6.4La3Zr1.4Ta0.6O12 for High Voltage Lithium Metal Batteries.

Project description:Composite solid polymer electrolytes (CSPEs) are safer alternatives to liquid electrolytes and excellent candidates for high-voltage solid-state batteries. However, interfacial instabilities between the electrodes and CSPEs are one of the bottlenecks in pursuing these systems. In this study, a cross-linked CSPE was synthesized based on polypropylene carbonate, polyethylene glycol methyl ether acrylate, polyethylene glycol diacrylate with additives including lithium bis(trifluoromethane)sulfonimide salt, and tantalum-doped lithium lanthanum zirconium oxide (LLZTO). Mass fractions of 10, 20, and 40% LLZTO were added to the CSPE matrix. In a symmetric cell, lithium plating and stripping revealed that the interface between the lithium metal anode and CSPE with 10% of the LLZTO (CSPE-10LLZTO) shows the most stable interface. The CSPE-10LLZTO sample demonstrated high flexibility and showed no degradation over 800 h of cycling at varying current densities. The ionic conductivity for the CSPE-10LLZTO sample at 40 °C was 6.4 × 10-4 S/cm. An all-solid-state full cell was fabricated with LiNi0.5Mn0.3Co0.2O2 as the cathode, CSPE-10LLZTO as the electrolyte and separator, and Li metal as the anode, delivering approximately 140 mAh/g of capacity. Differential scanning calorimetry measurements on CSPE-xLLZTO showed high miscibility and the elimination of crystallinity. Raman spectroscopy revealed uniformity in the structure. These findings demonstrate the capability of the CSPEs to develop high-voltage solid-state lithium metal batteries.

| S-EPMC11367574 | biostudies-literature

Data mining of molecular dynamics data reveals Li diffusion characteristics in garnet Li7La3Zr2O12.

Project description:Understanding Li diffusion in solid conductors is essential for the next generation Li batteries. Here we show that density-based clustering of the trajectories computed using molecular dynamics simulations helps elucidate the Li diffusion mechanism within the Li7La3Zr2O12 (LLZO) crystal lattice. This unsupervised learning method recognizes lattice sites, is able to give the site type, and can identify Li hopping events. Results show that, while the cubic LLZO has a much higher hopping rate compared to its tetragonal counterpart, most of the Li hops in the cubic LLZO do not contribute to the diffusivity due to the dominance of back-and-forth type jumps. The hopping analysis and local Li configuration statistics give evidence that Li diffusivity in cubic LLZO is limited by the low vacancy concentration. The hopping statistics also shows uncorrelated Poisson-like diffusion for Li in the cubic LLZO, and correlated diffusion for Li in the tetragonal LLZO in the temporal scale. Further analysis of the spatio-temporal correlation using site-to-site mutual information confirms the weak site dependence of Li diffusion in the cubic LLZO as the origin for the uncorrelated diffusion. This work puts forward a perspective on combining machine learning and information theory to interpret results of molecular dynamics simulations.

| S-EPMC5240091 | biostudies-literature

Bilayer Dense-Porous Li7 La3 Zr2 O12 Membranes for High-Performance Li-Garnet Solid-State Batteries.

Project description:Li dendrites form in Li7 La3 Zr2 O12 (LLZO) solid electrolytes due to intrinsic volume changes of Li and the appearance of voids at the Li metal/LLZO interface. Bilayer dense-porous LLZO membranes make for a compelling solution of this pertinent challenge in the field of Li-garnet solid-state batteries (SSB). Lithium is thus stored in the pores of the LLZO, thereby avoiding i) dynamic changes of the anode volume and ii) the formation of voids during Li stripping due to increased surface area of the Li/LLZO interface. The dense layer then additionally reduces the probability of short circuits during cell charging. In this work, a method for producing such bilayer membranes utilizing sequential tape-casting of porous and dense layers is reported. The minimum attainable thicknesses are 8-10 µm for dense and 32-35 µm for porous layers, enabling gravimetric and volumetric energy densities of Li-garnet SSBs of 279 Wh kg-1 and 1003 Wh L-1 , respectively. Bilayer LLZO membranes in symmetrical cell configuration exhibit high critical current density up to 6 mA cm-2 and cycling stability of over 160 cycles at a current density of 0.5 mA cm-2 at an areal capacity limitation of 0.25 mAh cm-2 .

| S-EPMC10015908 | biostudies-literature

Self-diffusion in garnet-type Li7La3Zr2O12 solid electrolytes.

Project description:Tetragonal garnet-type Li7La3Zr2O12 is an important candidate solid electrolyte for all-solid-state lithium ion batteries because of its high ionic conductivity and large electrochemical potential window. Here we employ atomistic simulation methods to show that the most favourable disorder process in Li7La3Zr2O12 involves loss of Li2O resulting in lithium and oxygen vacancies, which promote vacancy mediated self-diffusion. The activation energy for lithium migration (0.45 eV) is much lower than that for oxygen (1.65 eV). Furthermore, the oxygen migration activation energy reveals that the oxygen diffusion in this material can be facilitated at higher temperatures once oxygen vacancies form.

| S-EPMC7801511 | biostudies-literature

Synergetic Effect of Li-Ion Concentration and Triple Doping on Ionic Conductivity of Li7La3Zr2O12 Solid Electrolyte.

Project description:Li7La3Zr2O12 (LLZO) is a promising and safe solid electrolyte for all-solid-state batteries. To achieve high ionic conductivity of LLZO, stabilizing the cubic phase and reducing Li loss during the sintering process is essential. Therefore, reducing the sintering temperature, which increases the sintering time for high-density pellets, is necessary. Herein, we investigate the change in the crystal structure, morphology, and Li ionic conductivity of LLZO pellets by triple doping with Al, Ga, and Ta and modulating the variation in initial Li concentrations. Interestingly, the proportion of the conductive cubic phase increased with increasing Li stoichiometry by 1.1 times, and this tendency was further accelerated by triple doping. The synergetic effects of triple doping and Li concentration also minimized Li loss during sintering. Accordingly, it provided a high-quality LLZO pellet with good ionic conductivity (3.6 × 10-4 S cm-1) and high relative density (97.8%). Notably, the LLZO pellet was obtained using a very short sintering process (40 min). Considering that the most time-consuming step is the sintering process for LLZO, this study can provide guidelines for the fast production and commercialization of LLZO electrolytes with high ionic conductivity.

| S-EPMC9457903 | biostudies-literature

Cold Sintering of Li6.4La3Zr1.4Ta0.6O12/PEO Composite Solid Electrolytes.

Project description:Ceramic/polymer composite solid electrolytes integrate the high ionic conductivity of in ceramics and the flexibility of organic polymers. In practice, ceramic/polymer composite solid electrolytes are generally made into thin films rather than sintered into bulk due to processing temperature limitations. In this work, Li6.4La3Zr1.4Ta0.6O12 (LLZTO)/polyethylene-oxide (PEO) electrolyte containing bis(trifluoromethanesulfonyl)imide (LiTFSI) as the lithium salt was successfully fabricated into bulk pellets via the cold sintering process (CSP). Using CSP, above 80% dense composite electrolyte pellets were obtained, and a high Li-ion conductivity of 2.4 × 10-4 S cm-1 was achieved at room temperature. This work focuses on the conductivity contributions and microstructural development within the CSP process of composite solid electrolytes. Cold sintering provides an approach for bridging the gap in processing temperatures of ceramics and polymers, thereby enabling high-performance composites for electrochemical systems.

| S-EPMC9572155 | biostudies-literature

Li7La3Zr2O12-co-LiNbO3 Surface Modification Improves the Interface Stability between Cathode and Sulfide Solid-State Electrolyte in All-Solid-State Batteries.

Project description:With the rapid development of energy storage and electric vehicles, thiophosphate-based all-solid-state batteries (ASSBs) are considered the most promising power source. In order to commercialize ASSBs, the interfacial problem between high-voltage cathode active materials and thiophosphate-based solid-state electrolytes needs to be solved in a simple, effective way. Surface coatings are considered the most promising approach to solving the interfacial problem because surface coatings could prevent direct physical contact between cathode active materials and thiophosphate-based solid-state electrolytes. In this work, Li7La3Zr2O12 (LLZO) and LiNbO3 (LNO) coatings for LiCoO2 (LCO) were fabricated by in-situ interfacial growth of two high-Li+ conductive oxide electrolytes on the LCO surface and tested for thiophosphate-based ASSBs. The coatings were obtained from a two-step traditional sol-gel coatings process, the inner coatings were LNO, and the surface coatings were LLZO. Electrochemical evaluations confirmed that the two-layer coatings are beneficial for ASSBs. ASSBs containing LLZO-co-LNO coatings LiCoO2 (LLZO&LNO@LCO) significantly improved long-term cycling performance and discharge capacity compared with those assembled from uncoated LCO. LLZO&LNO@LCO||Li6PS5Cl (LPSC)||Li-In delivered discharge capacities of 138.8 mAh/g, 101.8 mAh/g, 60.2 mAh/g, and 40.2 mAh/g at 0.05 C, 0.1 C, 0.2 C, and 0.5 C under room temperature, respectively, and better capacity retentions of 98% after 300 cycles at 0.05 C. The results highlighted promising low-cost and scalable cathode material coatings for ASSBs.

| S-EPMC9967944 | biostudies-literature

Zr- and Ce-doped Li6Y(BO3)3 electrolyte for all-solid-state lithium-ion battery.

Project description:The ionic conductivity of Li6Y(BO3)3 (LYBO) was enhanced by the substitution of tetravalent ions (Zr4+ and Ce4+) for Y3+ sites through the formation of vacancies at the Li sites, an increase in compact densification, and an increase in the Li+-ion conduction pathways in the LYBO phase. As a result, the ionic conductivity of Li5.875Y0.875Zr0.1Ce0.025(BO3)3 (ZC-LYBO) reached 1.7 × 10-5 S cm-1 at 27 °C, which was about 5 orders of magnitude higher than that of undoped Li6Y(BO3)3. ZC-LYBO possessed a large electrochemical window and was thermally stable after cosintering with a LiNi1/3Mn1/3Co1/3O2 (NMC) positive electrode. These characteristics facilitated good reversible capacities in all-solid-state batteries for both NMC positive electrodes and graphite negative electrodes via a simple cosintering process.

| S-EPMC9031198 | biostudies-literature

Investigating the electrochemical stability of Li7La3Zr2O12 solid electrolytes using field stress experiments.

Project description:Cubic Li7La3Zr2O12 (LLZO) garnets are among the most promising solid electrolytes for solid-state batteries with the potential to exceed conventional battery concepts in terms of energy density and safety. The electrochemical stability of LLZO is crucial for its application, however, controversial reports in the literature show that it is still an unsettled matter. Here, we investigate the electrochemical stability of LLZO single crystals by applying electric field stress via macro- and microscopic ionically blocking Au electrodes in ambient air. Induced material changes are subsequently probed using various locally resolved analysis techniques, including microelectrode electrochemical impedance spectroscopy (EIS), laser induced breakdown spectroscopy (LIBS), laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS), and microfocus X-ray diffraction (XRD). Our experiments indicate that LLZO decomposes at 4.1-4.3 V vs. Li+/Li, leading to the formation of Li-poor phases like La2Zr2O7 beneath the positively polarized electrode. The reaction is still on-going even after several days of polarization, indicating that no blocking interfacial layer is formed. The decomposition can be observed at elevated as well as room temperature and suggests that LLZO is truly not compatible with high voltage cathode materials.

| S-EPMC8279110 | biostudies-literature

Li7La3Zr2O12 Garnet Solid Polymer Electrolyte for Highly Stable All-Solid-State Batteries.

Project description:All-solid-state batteries have gained significant attention as promising candidates to replace liquid electrolytes in lithium-ion batteries for high safety, energy storage performance, and stability under elevated temperature conditions. However, the low ionic conductivity and unsuitability of lithium metal in solid polymer electrolytes is a critical problem. To resolve this, we used a cubic garnet oxide electrolyte (Li7La3Zr2O12 - LLZO) and ionic liquid in combination with a polymer electrolyte to produce a composite electrolyte membrane. By applying a solid polymer electrolyte on symmetric stainless steel, the composite electrolyte membrane shows high ionic conductivity at elevated temperatures. The effect of LLZO in suppressing lithium dendrite growth within the composite electrolyte was confirmed through symmetric lithium stripping/plating tests under various current densities showing small polarization voltages. The full cell with lithium iron phosphate as the cathode active material achieved a highest specific capacity of 137.4 mAh g-1 and a high capacity retention of 98.47% after 100 cycles at a current density of 50 mA g-1 and a temperature of 60°C. Moreover, the specific discharge capacities were 137 and 100.8 mAh g-1 at current densities of 100 and 200 mA g-1, respectively. This research highlights the capability of solid polymer electrolytes to suppress the evolution of lithium dendrites and enhance the performance of all-solid-state batteries.

| S-EPMC7847977 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data