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Journal article
In-Operando FTIR Spectroscopy Study on Rapid Polysulfide Binding via Caffeine in Lithium-Sulfur Batteries
The journal of physical chemistry letters, pp 12164-12170
02 Dec 2024
PMID: 39620945
Featured in Collection : Research Supported by Drexel Libraries' OA Programs
Abstract
Lithium-sulfur batteries are limited by the high mobility of polysulfides in the electrolyte, which allows them to migrate from the cathode to the lithium anode. This is known as polysulfide shuttling and simultaneously diminishes the active material and poisons the anode. Various cathode additives have been shown empirically to mitigate this problem, although the mechanism is not often ascertained experimentally. Herein, we demonstrate for the first time that the small molecule additive caffeine reduces the polysulfide shuttling current in a lithium-sulfur battery and decreases the capacity fade in galvanostatic cycling experiments. Using in-operando Fourier transform infrared (FTIR) spectroscopy, we identify reversible shifts in the carbonyl stretching frequencies of caffeine that are strongly correlated with the onset of polysulfide formation during both discharging and charging. These spectroscopic shifts are consistent with a polar-polar interaction between polysulfides and the carbonyl groups of caffeine, leading to the observed decrease in polysulfide mobility.Lithium-sulfur batteries are limited by the high mobility of polysulfides in the electrolyte, which allows them to migrate from the cathode to the lithium anode. This is known as polysulfide shuttling and simultaneously diminishes the active material and poisons the anode. Various cathode additives have been shown empirically to mitigate this problem, although the mechanism is not often ascertained experimentally. Herein, we demonstrate for the first time that the small molecule additive caffeine reduces the polysulfide shuttling current in a lithium-sulfur battery and decreases the capacity fade in galvanostatic cycling experiments. Using in-operando Fourier transform infrared (FTIR) spectroscopy, we identify reversible shifts in the carbonyl stretching frequencies of caffeine that are strongly correlated with the onset of polysulfide formation during both discharging and charging. These spectroscopic shifts are consistent with a polar-polar interaction between polysulfides and the carbonyl groups of caffeine, leading to the observed decrease in polysulfide mobility.
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Details
- Title
- In-Operando FTIR Spectroscopy Study on Rapid Polysulfide Binding via Caffeine in Lithium-Sulfur Batteries
- Creators
- Taber Yim - Drexel UniversityRhyz Pereira - Drexel UniversityJantakan Nedsaengtip - Cornell UniversityAaron T Fafarman (Corresponding Author) - Drexel UniversityVibha Kalra - Drexel University
- Publication Details
- The journal of physical chemistry letters, pp 12164-12170
- Publisher
- ACS Publications
- Number of pages
- 7
- Grant note
This work was financially supported by the National Science Foundation, NSF grant 1804374. The authors would also like to acknowledge the Materials Characterization Core (MCC) at Drexel University for use of the Apreo 2S SEM (NSF-MRI Award 2117602) and the Cornell Center for Materials Research (CCMR) for the use of the Nexsa G2 XPS.
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemical and Biological Engineering; Chemistry; Materials Characterization Core
- Web of Science ID
- WOS:001368385500001
- Scopus ID
- 2-s2.0-85210943945
- Other Identifier
- 991021970099504721
InCites Highlights
Data related to this publication, from InCites Benchmarking & Analytics tool:
- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Chemistry, Physical
- Materials Science, Multidisciplinary
- Nanoscience & Nanotechnology
- Physics, Atomic, Molecular & Chemical