scholarly journals Probing Lithium-Ion Battery Electrolytes with Laboratory Near-Ambient Pressure XPS

Crystals ◽  
2020 ◽  
Vol 10 (11) ◽  
pp. 1056
Author(s):  
Paul M. Dietrich ◽  
Lydia Gehrlein ◽  
Julia Maibach ◽  
Andreas Thissen

In this article, we present Near Ambient Pressure (NAP)-X-ray Photoelectron Spectroscopy (XPS) results from model and commercial liquid electrolytes for lithium-ion battery production using an automated laboratory NAP-XPS system. The electrolyte solutions were (i) LiPF6 in EC/DMC (LP30) as a typical commercial battery electrolyte and (ii) LiTFSI in PC as a model electrolyte. We analyzed the LP30 electrolyte solution, first in its vapor and liquid phase to compare individual core-level spectra. In a second step, we immersed a V2O5 crystal as a model cathode material in this LiPF6 solution. Additionally, the LiTFSI electrolyte model system was studied to compare and verify our findings with previous NAP-XPS data. Photoelectron spectra recorded at pressures of 2–10 mbar show significant chemical differences for the different lithium-based electrolytes. We show the enormous potential of laboratory NAP-XPS instruments for investigations of solid-liquid interfaces in electrochemical energy storage systems at elevated pressures and illustrate the simplicity and ease of the used experimental setup (EnviroESCA).

2021 ◽  
Author(s):  
David Starr ◽  
Marco Favaro ◽  
Pip Clark ◽  
Rossella Yivlialin ◽  
Maryline Ralaiarisoa ◽  
...  

2020 ◽  
Vol 118 ◽  
pp. 106790
Author(s):  
Hisao Kiuchi ◽  
Kazuhiro Hikima ◽  
Keisuke Shimizu ◽  
Ryoji Kanno ◽  
Fukunaga Toshiharu ◽  
...  

Surfaces ◽  
2020 ◽  
Vol 3 (3) ◽  
pp. 392-407
Author(s):  
Marco Favaro

Molecular-level understanding of electrified solid/liquid interfaces has recently been enabled thanks to the development of novel in situ/operando spectroscopic tools. Among those, ambient pressure photoelectron spectroscopy performed in the tender/hard X-ray region and coupled with the “dip and pull” method makes it possible to simultaneously interrogate the chemical composition of the interface and built-in electrical potentials. On the other hand, only thin liquid films (on the order of tens of nanometers at most) can be investigated, since the photo-emitted electrons must travel through the electrolyte layer to reach the photoelectron analyzer. Due to the challenging control and stability of nm-thick liquid films, a detailed experimental electrochemical investigation of such thin electrolyte layers is still lacking. This work therefore aims at characterizing the electrochemical behavior of solid/liquid interfaces when confined in nanometer-sized regions using a stochastic simulation approach. The investigation was performed by modeling (i) the electron transfer between a solid surface and a one-electron redox couple and (ii) its diffusion in solution. Our findings show that the well-known thin-layer voltammetry theory elaborated by Hubbard can be successfully applied to describe the voltammetric behavior of such nanometer-sized interfaces. We also provide an estimation of the current densities developed in these confined interfaces, resulting in values on the order of few hundreds of nA·cm−2. We believe that our results can contribute to the comprehension of the physical/chemical properties of nano-interfaces, thereby aiding to a better understanding of the capabilities and limitations of the “dip and pull” method.


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