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Schematic representation of the degradation mechanism at the LCO-LPS interface

Reactivity and potential profile across the electrified LiCoO2-Li3PS4 interface probed by operando X-ray photoelectron spectroscopy

All-solid-state lithium batteries are a promising alternative for next generation of safe energy storage devices, provided that parasitic side reactions and the resulting hindrances in ionic transport at the electrolyte-electrode interface can be overcome. Motivated by the need for a fundamental understanding of such interface, we present here real-time measurements of the (electro-)chemical reactivity and local surface potential at the electrified interface Li3PS4 and LiCoO2 using operando X-ray photoelectron spectroscopy.

 

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Structural formula of (a) EMIM+ cation, (b) TFSI- and (c) FSI- anions.

Li-ion solvation in TFSI and FSI - based ionic liquid electrolytes probed by X-ray photoelectron spectroscopy

We demonstrate the capability of conventional laboratory XPS to determine the anions solvation shell of Li+ cation within 1M of LiTFSI and 1M of LiFSI salts dissolved in (EMIM+-FSI-) and (EMIM+-TFSI-) ionic liquids. The binding energy difference between the N1s components originating from the EMIM+ cation and from TFSI- or FSI- anions, solvating the Li+, confirms that both TFSI- and FSI- contribute simultaneously to the Li+ solvation. Additionally, the degradation of the TFSI and FSI -based electrolytes under X-ray exposure is proved.   

 

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High quality 90 nm and 50 nm Li4Ti5O12 films integrated on silicon substrates

Integration of Li4Ti5O12 crystalline films on silicon towards high-rate performance lithionic devices

The growth of crystalline Li-based oxide thin films on silicon substrates is essential for the integration of next-generation solid-state lithionic and electronic devices. In this work, we employ a 2 nm γ-Al2O3 buffer layer on Si substrates in order to grow high quality crystalline thin films Li4Ti5O12 (LTO). Long-term galvanostatic cycling of 50 nm LTO demonstrates exceptional electrochemical performance, specific capacity of 175 mAh g-1 and 56 mAh g-1 at 100C and 5000C respectively, with a capacity retention of 91% after 5000 cycles.

 

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Operando XAS and XRD

Understanding the (de-)lithiation mechanism of nano-sized LiMn2O4 allows achieving long-term cycling stability

We report an in-depth investigation of the local atomic geometry, electronic and crystallographic structure evolution of nano-sized LiMn2O4 using operando XAS and XRD to shed light on (de-)lithiation mechanism when cycled in wide voltage range of 2.0 to 4.3 V vs Li+/Li. Leveraging on these findings, a novel electrochemical cycling protocol, with periodic deep discharge, yields superior electrochemical performance cycled in the range of 3.3 to 4.3 V exhibiting an excellent structure cyclability and an unprecedented increase in the specific capacity upon long cycling.

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