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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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96 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Petaloid-shaped ZnO coated carbon felt as a controllable host to construct hierarchical Li composite anode

Prestoring Li metal into the 3D host via thermal infusion strategy has been considered as an effective approach on suppressing Li dendrites growth of Li-metal anode during cycling. However, the fast Li infusing process generally induces uncontrollable and undesirable structures during the formation of composite Li metal anode. It is widely accepted that both physical and chemical interactions between the molten Li and the hosts provide driving forces for Li infusing into the host, but which one plays the dominant role has not been explored clearly. In this work, a 3D carbon felt coated by petaloid zinc oxide (CFZO) is designed as a controllable host for prestoring Li metal via thermal infusion method. It is revealed that the morphology induced physical driving force plays a more important role than the chemical reaction between ZnO and molten Li in the thermal infusion process. The physical driving force originates from the capillarity effect, depending on the roughness of the host according to Wenzel's model. An adjustable Li infusing process can be controlled to fabricate the Li composite electrode with a hierarchical structure (with dense Li-rich layer and porous Li-poor layer). The unique structure of the CFZO-Li not only provides enough spaces for Li deposition, but also disperses local current density to induce a uniform Li deposition behavior, thus Li dendrites can be suppressed effectively. As a result, CFZO-Li anode exhibits promising cycle stability when coupled with both Li-containing (LiNi 0.8 Co 0.15 Al 0.05 O 2 ) and Li-free (sulfur) cathodes.

25 ENERGY STORAGE↗
DOE OSTI2025

Atomic Structural Features of Stacking Faults and Domain Connections in the Li- and Mn-Rich Cathode

Li- and Mn-rich layered oxides (LMRs), a class of earth-abundant materials for rechargeable Li-ion battery cathodes, crystallize into layered structures of two different symmetries: C2/m represented by Li 2 MnO 3 and R$\overline{3}$m represented by LiMn 0.5 Ni 0.5 O 2 . Fundamental questions about how the C2/m and R$\overline{3}$m domains spatially correlate within the same oxide grain and how the C2/m stacking faults arrange themselves when this happens still remain. Here, by using integrated differential phase contrast imaging in scanning transmission electron microscopy (STEM-iDPC), we probe the structural and compositional details of a prototypical, cobalt-free LMR material, 0.3Li 2 MnO 3 •0.7LiMn 0.5 Ni 0.5 O 2 (Li 1.13 Mn 0.57 Ni 0.3 O 2 ). The connection between the C2/m and R$\overline{3}$m domains is found to be abrupt, facilitated by the small lattice mismatch between the two structures. Stacking faults in the C2/m domains feature atomic plane shifting that accommodates stacking sequence changes, which explains why the stacking faults form in a random manner. Furthermore, a local disordering mechanism was identified to correlate with the C2/m stacking faults. Chemically, it is found that Ni coexists with Mn at the transition metal sites within the nominal Li 2 MnO 3 domain. As a result, this study demonstrates that STEM-iDPC is a very useful tool for capturing all the elements in a single image, revealing atomic details on domain connections and stacking faults in the LMRs.

Li-rich and Mn-rich oxides↗
DOE OSTI2020

Impact of surface coating on electrochemical and thermal behaviors of a Li-rich Li 1.2 Ni 0.16 Mn 0.56 Co 0.08 O 2 cathode

Lithium-rich layered oxide materials are considered as potential cathode materials for future high-performance lithium-ion batteries (LIBs) owing to their high operating voltage and relatively high specific capacity. However, perceptible issues such as poor rate performance, poor capacity retention, and voltage degradation during cycling need to be improved before the successful commercialization of the material. In this report, zirconia coated Li 1.2 Ni 0.16 Mn 0.56 Co 0.08 O 2 2 = 1.0, 1.5 and 2.0 wt%) materials are synthesized using a sol–gel assisted ball milling approach. A comparison of structural, morphological and electrochemical properties is examined to elucidate the promising role of ZrO 2 coating on the performance of the NMC cathode. A uniform and homogeneous ZrO 2 coating is observed on the surface of NMC particles as evident by TEM elemental mapping images. The ZrO 2 coated NMCs exhibit significantly improved electrochemical performance at a higher C-rate as compared to pristine material. 1.5% ZrO 2 coated NMC demonstrates better cycling stability (95% capacity retention) than pristine NMC (77% capacity retention) after 50 cycles. All ZrO 2 coated NMC materials demonstrated improved thermal stability compared to pristine material. The difference in onset temperature of 2 wt% ZrO 2 coated and pristine NMC is 20 °C. The improved electrochemical performance of ZrO 2 coated NMC can be attributed to the stabilization of its surface structure due to the presence of ZrO 2 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Understanding cation-disordered rocksalt oxyfluoride cathodes

Partial fluorine (F) substitution into the oxygen (O) sublattice has been shown to improve cycling stability of cation-disordered Li-excess rocksalt oxide (DRX) cathodes. Detailed understanding on failure mechanisms and key optimization knowledge of fluorinated-DRX (F-DRX), however, are lacking. In the present study, we incorporate different amounts of F into a baseline DRX system, Li 1.2 Ti 0.4 Mn 0.4 O 2 (LTMO3.0, 3.0 denotes nominal Li/Mn ratio), and synthesize two oxyfluoride compounds, Li-rich Li 1.3 Ti 0.3 Mn 0.4 O 1.7 F 0.3 (LTMOF3.25) and Mn-rich Li 1.2 Ti 0.2 Mn 0.6 O 1.8 F 0.2 (LTMOF2.0) with an increased and reduced Li/Mn ratio of 3.25 and 2.0, respectively. Through careful monitoring of chemical and structural evolution, we show that cycling-induced changes are manifested not only by Mn reduction and degradation of its local coordination environment, but also by F enrichment and formation of LiF-type of domains on the surface. A “concerted-densification” based failure mechanism, involving atomic-level changes in both transition-metal cationic sublattice and oxygen/fluorine anionic sublattice, is proposed for the degradation in F-DRX cathode materials. The study reveals that increasing F content accompanied by reduced Li/Mn ratio mitigates the degradation process, offering key design strategies in achieving balanced cathode capacity and stability.

25 ENERGY STORAGE↗
DOE OSTI2022

Highly reversible Li 2 RuO 3 cathodes in sulfide-based all solid-state lithium batteries

The practical application of high-capacity lithium-rich cathode materials in lithium-ion batteries has been largely restricted by severe side reactions with electrolytes. Herein, we report a highly stable lithium-rich Li 2 RuO 3 cathode by forming a passivating solid electrolyte interphase at the interface with a sulfide solid electrolyte such as Li 6 PS 5 Cl in all-solid-state lithium batteries (ASSLBs), which efficiently suppresses serious parasitic interfacial reactions and fast-increasing interfacial impedance normally observed in liquid electrolytes. The exceptionally high interfacial stability of the Li 2 RuO 3 /sulfide electrolyte interface contributes to a high reversible capacity of 257 mA h g –1 of Li 2 RuO 3 at 0.05C rate, and unprecedented cycling stability with 90% capacity retention after 1000 cycles at 1C rate. Iin this work, comprehensive experimental characterizations and first-principles calculations disclose that electronically insulating interfacial reaction products forming at the interface between the Li 2 RuO 3 cathode and Li 6 PS 5 Cl facilitate the formation of a stable and passivating interphase and block the continuous side reactions. Importantly, reversible oxygen redox activity of Li 2 RuO 3 is well-maintained in this configuration of ASSLBs even after 600 cycles, thus the common voltage decay of the Li-rich material is also significantly reduced. These new discoveries demonstrate the critical role of interface design for achieving prolonged cycling stability of lithium-rich cathode materials.

25 ENERGY STORAGE↗